Effect of catalyst for the decomposition of VOCs in a NTP reactor

International Nuclear Information System (INIS)

Mohanty, Suchitra; Das, Smrutiprava; Paikaray, Rita; Sahoo, Gourishankar; Samantaray, Subrata

2015-01-01

Air pollution has become a major cause of human distress both directly and indirectly. VOCs are becoming the major air pollutants. So the decomposition of VOCs is present need of our society. Non-thermal plasma reactor (NTP) is proven to be effective for low concentration VOCs decomposition. For safe and effective application of DBD, optimization of treatment process requires different plasma parameter characterization. So electron temperature and electron density parameters of VOCs show the decomposition path ways. In this piece of work by taking the emission spectra and comparing the line intensity ratios, the electron temperature and density were determined. Also the decomposition rate in terms of the deposited products on the dielectric surface was studied. Decomposition rate increases in presence of catalyst as compared to the pure compound in presence of a carrier gas. Decomposition process was studied by UV-VIS, FTIR, OES Spectroscopic methods and by GCMS. Deposited products are analyzed by UV-VIS and FTIR spectroscopy. Plasma parameters like electron temperature, density are studied with OES. And gaseous products are studied by GCMS showing the peaks for the by products. (author)

Direct NO decomposition over conventional and mesoporous Cu-ZSM-5 and Cu-ZSM-11 catalysts

DEFF Research Database (Denmark)

Kustova, Marina; Rasmussen, Søren Birk; Kustov, Arkadii

2006-01-01

Conventional Cu-ZSM-5 has for many years been recognized as a unique catalyst for direct NO decomposition. Zeolite-based catalysts have a crystallographically well-defined microporous structure. In such microporous catalysts, the creation and accessibility of the active sites is often influenced...... that ZSM-11 has only straight microporous channels, while ZSNI-5 has both straight and sinusoidal channels. Apparently, there is a preferential formation of active sites and/or improved accessibility in the straight channels compared to the sinusoidal channels, which make the ZSM-11 material a better...

Patched bimetallic surfaces are active catalysts for ammonia decomposition.

Science.gov (United States)

Guo, Wei; Vlachos, Dionisios G

2015-10-07

Ammonia decomposition is often used as an archetypical reaction for predicting new catalytic materials and understanding the very reason of why some reactions are sensitive on material's structure. Core-shell or surface-segregated bimetallic nanoparticles expose outstanding activity for many heterogeneously catalysed reactions but the reasons remain elusive owing to the difficulties in experimentally characterizing active sites. Here by performing multiscale simulations in ammonia decomposition on various nickel loadings on platinum (111), we show that the very high activity of core-shell structures requires patches of the guest metal to create and sustain dual active sites: nickel terraces catalyse N-H bond breaking and nickel edge sites drive atomic nitrogen association. The structure sensitivity on these active catalysts depends profoundly on reaction conditions due to kinetically competing relevant elementary reaction steps. We expose a remarkable difference in active sites between transient and steady-state studies and provide insights into optimal material design.

Catalytic decomposition of tar derived from wood waste pyrolysis using Indonesian low grade iron ore as catalyst

Energy Technology Data Exchange (ETDEWEB)

Wicakso, Doni Rahmat [Chemical Engineering Department, Faculty of Engineering, Lambung Mangkurat University, Jalan A. Yani KM. 36 Banjarbaru, 70714, South Kalimantan (Indonesia); Chemical Engineering Department, Faculty of Engineering, Gadjah Mada University, Jalan Grafika No. 2 Bulaksumur, Yogyakarta, 55281 (Indonesia); Sutijan; Rochmadi [Chemical Engineering Department, Faculty of Engineering, Gadjah Mada University, Jalan Grafika No. 2 Bulaksumur, Yogyakarta, 55281 (Indonesia); Budiman, Arief, E-mail: abudiman@ugm.ac.id [Chemical Engineering Department, Faculty of Engineering, Gadjah Mada University, Jalan Grafika No. 2 Bulaksumur, Yogyakarta, 55281 (Indonesia); Center for Energy Studies, Gadjah Mada University, Sekip K1A, Yogyakarta, 55281 (Indonesia)

2016-06-03

Low grade iron ore can be used as an alternative catalyst for bio-tar decomposition. Compared to other catalysts, such as Ni, Rd, Ru, Pd and Pt, iron ore is cheaper. The objective of this research was to investigate the effect of using low grade iron ore as catalyst for tar catalytic decomposition in fixed bed reactor. Tar used in this experiment was pyrolysis product of wood waste while the catalyst was Indonesian low grade iron ore. The variables studied were temperatures between 500 – 600 °C and catalyst weight between 0 – 40 gram. The first step, tar was evaporated at 450 °C to produce tar vapor. Then, tar vapor was flowed to fixed bed reactor filled low grade iron ore. Gas and tar vapor from reactor was cooled, then the liquid and uncondensable gas were analyzed by GC/MS. The catalyst, after experiment, was weighed to calculate total carbon deposited into catalyst pores. The results showed that the tar components that were heavy and light hydrocarbon were decomposed and cracked within the iron ore pores to from gases, light hydrocarbon (bio-oil) and carbon, thus decreasing content tar in bio-oil and increasing the total gas product. In conclusion, the more low grade iron ore used as catalyst, the tar content in the liquid decrease, the H{sup 2} productivity increased and calorimetric value of bio-oil increased.

Catalytic decomposition of trichloroethylene over Pt-/Ni-catalyst under microwave heating

Energy Technology Data Exchange (ETDEWEB)

Takashima, Hideaki; Karches, Martin [Chemiace Laboratory, 36-13 Hon-cho, Hachioji 192-0066 (Japan); Kanno, Yoshinori [Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi, 4-3-11 Takeda, Kofu 400-8511 (Japan)], E-mail: kanno@yamanashi.ac.jp

2008-01-30

Microwave (MW)-activated catalytic reactor system was studied and the results were compared with that of a conventional system based on the thermal activation method. Trichloroethylene (TCE) was decomposed under various MW-powers supply. Results showed that there is an optimum film thickness that was loaded on supports in MW heating system. The threshold may be within 1-3 {mu}m. Lower temperature cannot activate the catalyst, while higher temperature results in carbon deposition and catalyst deactivation. This means that the dechlorination reaction needs to fix an optimum film MW-power supply in order to avoid the deposition of carbon on the surface of the active phase. MW-activated system is also worth compensating the conventional system in VOCs decomposition reaction.

Effect of hydrogen and propylene on the hydrogen peroxide decomposition over Pt, PtO and Au catalysts

NARCIS (Netherlands)

Kertalli, E.; Schouten, J.C.; Nijhuis, T.A.

2017-01-01

The decomposition of hydrogen peroxide (H2O2) on Pt, PtO and Au catalysts has been investigated in the presence of nitrogen, propylene and hydrogen. H2O2 formation on the catalyst is known to be a key intermediate step for the direct synthesis of propylene oxide (PO) from hydrogen, propylene and

Ozone decomposition

Directory of Open Access Journals (Sweden)

Batakliev Todor

2014-06-01

Full Text Available Catalytic ozone decomposition is of great significance because ozone is a toxic substance commonly found or generated in human environments (aircraft cabins, offices with photocopiers, laser printers, sterilizers. Considerable work has been done on ozone decomposition reported in the literature. This review provides a comprehensive summary of the literature, concentrating on analysis of the physico-chemical properties, synthesis and catalytic decomposition of ozone. This is supplemented by a review on kinetics and catalyst characterization which ties together the previously reported results. Noble metals and oxides of transition metals have been found to be the most active substances for ozone decomposition. The high price of precious metals stimulated the use of metal oxide catalysts and particularly the catalysts based on manganese oxide. It has been determined that the kinetics of ozone decomposition is of first order importance. A mechanism of the reaction of catalytic ozone decomposition is discussed, based on detailed spectroscopic investigations of the catalytic surface, showing the existence of peroxide and superoxide surface intermediates

Session 4: Combinatorial research of methane catalytic decomposition on supported nitride catalysts for CO-free hydrogen

Energy Technology Data Exchange (ETDEWEB)

Jianghan, Shen; Hua, Wang; Zhongmin, Liu; Hongchao, Liu [Natural Gas Utilization and Applied Catalysis Lab., Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian P. R. (China)

2004-07-01

CO-free Hydrogen production is needed for proton exchange membrane fuel cells (PEMs) because CO strongly poisons the anode-electrocatalysts. Methane directly catalytic decomposition is an attractive way to produce CO-free hydrogen for the large abundance of methane and its high H/C ratio. It is more effective to employ high-throughput screening (HTS) technology in heterogeneous catalysis. In this paper, a combinatorial multi-stream reaction system with online multi-stream mass spectrometer screening (MSMSS) detection technique was applied to study the decomposition of methane over supported MoN{sub x}O{sub y} catalysts (supports = Al{sub 2}O{sub 3}, SiO{sub 2}, SBA-15, ZSM-5,13X, and NaY), which is a catalyst system seldom reported recently. (authors)

Cobalt Oxide Catalysts on Commercial Supports for N2O Decomposition.

Czech Academy of Sciences Publication Activity Database

Klegová, A.; Pacultová, K.; Fridrichová, D.; Volodarskaja, A.; Kovanda, J.; Jirátová, Květa

2017-01-01

Roč. 40, č. 5 (2017), s. 981-990 ISSN 0930-7516. [International Congress of Chemical and Process Engineering CHISA 2016 /22./ and the 19th Conference PRES 2016. Prague, 27.08.2016-31.08.2016] R&D Projects: GA ČR GA14-13750S Institutional support: RVO:67985858 Keywords : N2O decomposition * cobalt oxide * shaped catalyst Subject RIV: CI - Industrial Chemistry, Chemical Engineering OBOR OECD: Chemical process engineering Impact factor: 2.051, year: 2016

Fe(III)-loaded collagen fiber as a heterogeneous catalyst for the photo-assisted decomposition of Malachite Green

International Nuclear Information System (INIS)

Liu Xiaohu; Tang Rui; He Qiang; Liao Xuepin; Shi Bi

2010-01-01

A heterogeneous catalyst for Fenton reaction was prepared by immobilizing Fe(III) onto collagen fiber and its catalytic activity for the photo-assisted decomposition of Malachite Green (MG) was investigated. The results indicated that this Fe(III)-immobilized collagen fiber (Fe-CF) can effectively catalyse the decoloration and decomposition/mineralization of MG in aqueous solution. Catalysed by Fe-CF, MG solution was completely decolorized in 30 min, while 55.0% of TOC was removed from the dye solution within 120 min in the presence of H 2 O 2 and UVA irradiation (365 nm, 10 W). Fe-CF was recycled for seven times with certain activity loss (32.6% in decoloration, 18.5% in TOC removal), and its catalytic activity can be easily recovered by re-immobilization of Fe(III). Therefore, Fe-CF could act as an efficient and cost-effective catalyst for the photo-assisted decomposition of MG, and shows potential applications in practice.

Iron ore catalysts for methane decomposition to make CO x free hydrogen and carbon nano material

KAUST Repository

Zhou, Lu

2018-03-27

In this work, for the first time, iron ores with 91.7%–96.2% FeO, 1.3%–2.3% AlO, 1.2%–4.5% SiO, 1.3%–3.9% NaO, were studied directly as bulk catalysts for methane decomposition. By hydrogen pre-reduction at 850 °C, FeO species on iron ores were gradually reduced into FeO, FeO and then finally into Fe species. After reduction of 1.6 g of iron ore catalysts of 50 µm particle size with 100 mL/min pure H for 3.5 h at 850 °C, CMD life testing was conducted at 850 °C and GHSV of 3.75 L/g h and the catalyst showed a stable methane conversion for 5 h. When methane decomposition proceeded on Fe sites, FeC species would be formed to deposit graphite around themselves to finally form carbon nano onions. This carbon nano onions material showed excellent application for wastewater purification. All samples were fully characterized with XRF, XRD, H-TPR, TEM and Raman.

Using first principles to predict bimetallic catalysts for the ammonia decomposition reaction.

Science.gov (United States)

Hansgen, Danielle A; Vlachos, Dionisios G; Chen, Jingguang G

2010-06-01

The facile decomposition of ammonia to produce hydrogen is critical to its use as a hydrogen storage medium in a hydrogen economy, and although ruthenium shows good activity for catalysing this process, its expense and scarcity are prohibitive to large-scale commercialization. The need to develop alternative catalysts has been addressed here, using microkinetic modelling combined with density functional studies to identify suitable monolayer bimetallic (surface or subsurface) catalysts based on nitrogen binding energies. The Ni-Pt-Pt(111) surface, with one monolayer of Ni atoms residing on a Pt(111) substrate, was predicted to be a catalytically active surface. This was verified using temperature-programmed desorption and high-resolution electron energy loss spectroscopy experiments. The results reported here provide a framework for complex catalyst discovery. They also demonstrate the critical importance of combining theoretical and experimental approaches for identifying desirable monolayer bimetallic systems when the surface properties are not a linear function of the parent metals.

Activity of iridium-ruthenium and iridium-rhodium adsorption catalysts in decomposition of hydrogen peroxide

Energy Technology Data Exchange (ETDEWEB)

Zubovich, I A; Mikhaylov, V A; Migulina, N N [Yaroslavskij Politekhnicheskij Inst. (USSR)

1976-06-01

Experimental data for the activities of iridium-ruthenium and iridium-rhodium adsorption catalysts in the decomposition of hydrogen peroxide are considered and the results of magnetic susceptibility measurements are presented. It is concluded that surface structures (complexes) may be formed and that micro-electronic feaures play a role in heterogeneous catalysis.

Oblate hemispheroidal Large Ruthenium Particles Supported on Calcium Amide as Efficient Catalysts for Ammonia Decomposition.

Science.gov (United States)

Kishida, Kazuhisa; Kitano, Masaaki; Inoue, Yasunori; Sasase, Masato; Nakao, Takuya; Tada, Tomofumi; Abe, Hitoshi; Niwa, Yasuhiro; Yokoyama, Toshiharu; Hara, Michikazu; Hosono, Hideo

2018-03-30

Ammonia decomposition is positioned as an important technology for abstracting hydrogen from ammonia toward the realization of a hydrogen economy. Here, we report that oblate hemispheroidal large Ru particles on Ca(NH₂)₂ function as efficient catalysts for ammonia decomposition. The turnover frequency (TOF) of Ru/Ca(NH₂)₂ increased by two orders of magnitude as the Ru particle size was increased from 1.5 to 8.4 nm. More than 90% ammonia decomposition was achieved over Ru/Ca(NH₂)₂ with oblate hemispheroidal large Ru particles at 360 ºC, which is comparable to that of alkali-promoted Ru catalysts with small Ru particle sizes. XAFS analyses revealed that Ru particles are immobilized on Ca(NH₂)₂ by Ru-N bonding formed at the metal-support interface, which leads to oblate hemispheroidal Ru particles. Such a strong metal-support interaction in the Ru/Ca(NH₂)₂ is also substantiated by density functional theory calculations. The high activity of Ru/Ca(NH₂)₂ with large Ru particles primarily originates from the shape and appropriate size of Ru particles with a high density of active sites rather than the electron-donating ability of Ca(NH₂)₂. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and characterization of Fe–Ni/ɣ-Al2O3 egg-shell catalyst for H2 generation by ammonia decomposition

DEFF Research Database (Denmark)

Silva, Hugo José Lopes; Nielsen, Morten Godtfred; Fiordaliso, Elisabetta Maria

2015-01-01

The Fe–Ni alloyed nanoparticles are a promising alternative to expensive ruthenium-based catalysts for a real-scale application of hydrogen generation by ammonia decomposition. In practical applications, millimeter-sized extrudates are used as catalyst supports, where the spatial distribution...... of the active phase should match with the type of reaction. In this work, a novel synthesis route was developed for the preparation of a Fe–Ni/ɣ-Al2O3 egg-shell catalyst. Egg-shell is a preferred profile considering the highly endothermic nature of ammonia decomposition reaction. The high viscosity of glycerol...... using focused ion bean (FIB) milling allowed to acquire high resolution images of the Ni and Fe nanoparticles on ɣ-Al2O3, which is particularly challenging due to the crystalline nature of this support. Distinct regions of the egg-shell catalyst were analyzed through scanning TEM (STEM) and TEM...

Effects of catalyst-bed’s structure parameters on decomposition and combustion characteristics of an ammonium dinitramide (ADN)-based thruster

International Nuclear Information System (INIS)

Yu, Yu-Song; Li, Guo-Xiu; Zhang, Tao; Chen, Jun; Wang, Meng

2015-01-01

Highlights: • The decomposition and combustion process is investigated by numerical method. • Heat transfer in catalyst bed is modeled using non-isothermal and radiation model. • The wall heat transfer can impact on the distribution of temperature and species. • The value of catalyst bed length, diameter and wall thickness are optimized. - Abstract: The present investigation numerically studies the evolutions of decomposition and combustion within an ADN-based thruster, and the effects of the catalyst-bed’s three structure parameters (length, diameter, and wall thickness) on the general performance of ADN-based thruster have been systematically investigated. Based upon the calculated results, it can be known that the distribution of temperature gives a Gaussian manner at the exits of the catalyst-bed and the combustion chamber, and the temperature can be obviously effected by each the three structure parameters of the catalyst-bed. With the rise of each the three structure parameter, the temperature will first increases and decreases, and there exists an optimal design value making the temperature be the highest. Via the comparison on the maximal temperature at combustion chamber’s exit and the specific impulse, it can be obtained that the wall thickness plays an important role in the influences on the general performance of ADN-based thruster while the catalyst-bed’s length has the weak effects on the general performance among the three structure parameters.

Polymer-modified copper catalysts on carbon-containing support for reactions of H2O2 decomposition and cyclohexane oxidation

Directory of Open Access Journals (Sweden)

S. Auezkhanova

2012-12-01

Full Text Available Polymer-copper catalysts supported on a carbon-containing sorbent(CS, obtained by rice husk pyrolysis have been studied in the reactions of hydrogen peroxide decomposition and cyclohexane oxidation by hydrogen peroxide at 40°C and atmospheric pressure. The effect of the polymer nature on the activity of the developed catalysts have been shown. Polyhexamethyleneguanidine (PHMG was an optimal modifier for the developed catalysts. The calculated number of catalytic cycles (TON for 7% Cu-PGMG/CS was 450.

Cu-ZSM-5, Cu-ZSM-11, and Cu-ZSM-12 Catalysts for Direct NO Decomposition

DEFF Research Database (Denmark)

Kustova, Marina; Kustov, Arkadii; Christiansen, Sofie E.

2006-01-01

Cu-ZSM-5 has for many years been recognized as a unique catalyst for direct NO decomposition. Here, it is discovered that both Cu-ZSM-11 and Cu-ZSM-12 are about twice as active as Cu-ZSM-5. This difference is attributed to the active sites located almost exclusively in the straight zeolite pores...

Ozone decomposition on Ag/SiO2 and Ag/clinoptilolite catalysts at ambient temperature

International Nuclear Information System (INIS)

Nikolov, Penko; Genov, Krassimir; Konova, Petya; Milenova, Katya; Batakliev, Todor; Georgiev, Vladimir; Kumar, Narendra; Sarker, Dipak K.; Pishev, Dimitar; Rakovsky, Slavcho

2010-01-01

Silver modified zeolite (Bulgarian natural clinoptilolite) and Ag/silica catalysts were synthesized by ion exchange and incipient wet impregnation method respectively and characterized by different techniques. DC arc-AES was used for Ag detection. XRD spectra show that Ag is loaded over the surface of the SiO 2 sample and that after the ion-exchange process the HEU type structure of clinoptilolite is retained. UV-VIS (specific reflection at 310 nm) and IR (band at 695 cm -1 ) spectroscopy analysis proved that silver is loaded as a T-atom into zeolite channels as Ag + , instead of Na + , Ca 2+ , or K + ions, existing in the natural clinoptilolite form. The samples Ag/SiO 2 and Ag-clinoptilolite were tested as catalysts for decomposition of gas phase ozone. Very high catalytic activity (up to 99%) was observed and at the same time the catalysts remained active over time at room temperature.

Decomposition of hydrogen peroxide on nickel oxide - vanadium pentoxide catalysts and the effect of ionizing radiation on them

International Nuclear Information System (INIS)

Mucka, V.

1984-01-01

Some physico-chemical and catalytic properties of nickel oxide-vanadium pentoxide two-component catalysts were studied over the entire concentration range of the components, using the decomposition of hydrogen peroxide in an aqueous solution as the test reaction. The two oxides were found to affect each other; this was shown by the dependences of the specific surface area, the V 4+ ion concentration, and the catalyst activity on the system composition. At low vanadium pentoxide concentrations (up to 15 mol%) the reaction took place on nickel oxide modified with vanadium pentoxide, whereas in the region of higher vanadium pentoxide concentrations the decomposition of the peroxide was catalyzed primarily in the homogeneous phase by vanadium(V) peroxide ions; in a sample with 30 mol% V 2 O 5 , trivalent vanadium also played a part. With catalysts obtained by mere mechanical mixing of the two oxides, a modified activity was observed in the region of high excess of nickel oxide. The activity of catalyst, particularly pure nickel oxide, was increased by its partial reduction and decreased by its exposure to gamma radiation if the dose was higher than 10 5 Gy. The effects observed are interpreted in terms of the concept of bivalent catalytic centres. (author)

The role of catalysts in the decomposition of phenoxy compounds in coal: A density functional theory study

Science.gov (United States)

Liu, Jiang-Tao; Wang, Ming-Fei; Gao, Zhi-Hua; Zuo, Zhi-Jun; Huang, Wei

2018-01-01

The pyrolysis mechanisms of anisole (C6H5OCH3), as a coal-based model compound, on CaO, ZnO and γ-Al2O3 catalysts were studied using density functional theory (DFT). In contrast to the products of pyrolysis (C6H6, H2 and CO), the products of catalytic pyrolysis on CaO, ZnO, and γ-Al2O3 are C6H5OH and C2H4; CO, C5H6 and C2H4; and C6H5OH and C2H4, respectively. Our results indicate that CaO, ZnO and γ-Al2O3 catalysts not only decrease the energy barrier of C6H5OCH3 decomposition but also alter the pyrolysis process and the products. It is also found that the pyrolysis gas H2 alters the products on CaO (C6H5OH and CH4), but it does not affect the products on ZnO and γ-Al2O3. In sum, these catalysts are beneficial for phenoxy compound decomposition.

Comparative study of activated carbon, natural zeolite, and green sand supports for CuOX and ZnO sites as ozone decomposition catalyst

Science.gov (United States)

Azhariyah, A. S.; Pradyasti, A.; Dianty, A. G.; Bismo, S.

2018-03-01

This research was based on ozone decomposition in industrial environment. Ozone is harmful to human. Therefore, catalysts were made as a mask filter to decompose ozone. Comparison studies of catalyst supports were done using Granular Activated Carbon (GAC), Natural Zeolite (NZ), and Green Sand (GS). GAC showed the highest catalytic activity compared to other supports with conversion of 98%. Meanwhile, the conversion using NZ was only 77% and GS had been just 27%. GAC had the highest catalytic activity because it had the largest pore volume, which is 0.478 cm3/g. So GAC was used as catalyst supports. To have a higher conversion in ozone decomposition, GAC was impregnated with metal oxide as the active site of the catalyst. Active site comparison was made using CuOX and ZnO as the active site. Morphology, composition, and crystal phase were analyzed using SEM-EDX, XRF, and XRD methods. Mask filter, which contained catalysts for ozone decomposition, was tested using a fixed bed reactor at room temperature and atmospheric pressure. The result of conversion was analyzed using iodometric method. CuOX/GAC and ZnO/GAC 2%-w showed the highest catalytic activity and conversion reached 100%. From the durability test, CuOX/GAC 2%-w was better than ZnO/GAC 2%-w because the conversion of ozone to oxygen reached 100% with the lowest conversion was 70% for over eight hours.

Uranium sesqui nitride synthesis and its use as catalyst for the thermo decomposition of ammonia

International Nuclear Information System (INIS)

Rocha, Soraya Maria Rizzo da

1996-01-01

The preoccupation to have a secure destination for metallic uranium scraps and wastes and to search new non-nuclear uses for the huge amount of depleted metal uranium accumulated at the nuclear industry encouraged the study of the uranium sesqui nitride synthesis and its use. The use of uranium sesqui nitride as a catalyst for the thermo decomposition of ammonia for the hydrogen production has enormous significance. One of the most important nuclear cycle step is the reduction of the higher uranium oxides for the production of uranium dioxide and its conversion to uranium tetrafluoride. The reduction of the UO 3 and U 3 O 8 oxides is accomplished by the gas-solid reaction with elementary hydrogen. For economical purposes and for the safety concern the nuclear industry prefers to manufacture the hydrogen gas at the local and at the moment of use, exploring the catalytic decomposition of ammonia vapor. Using metallic uranium scraps as the raw material the obtention of its nitride was achieved by the reaction with ammonia. The results of the chemical and physical characterization of the prepared uranium sesqui nitride and its behavior as a catalyst for the cracking of ammonia are commented. A lower ammonia cracking temperature (550 deg C) using the uranium sesqui nitride compared with recommended industrial catalysts iron nitride (650 deg C) and manganese nitride (700 deg C) sounds reliable and economically advantageous. (author)

Effect of oxygen on decomposition of nitrous oxide over various metal oxide catalysts

International Nuclear Information System (INIS)

Satsuma, Atsushi; Maeshima, Hajime; Watanabe, Kiyoshi; Hattori, Tadashi

2001-01-01

The inhibitory effect of oxygen on decomposition of nitrous oxide over various metal oxide catalysts was investigated. The activity of nitrous oxide decomposition significantly decreased over CuO, Co 3 O 4 , NiO, Fe 2 O 3 , SnO 2 , In 2 O 3 and Cr 2 O 3 by reversible adsorption of oxygen onto the active sites. On the contrary to this, there was no or small change in the activity of TiO 2 , Al 2 O 3 , MgO, La 2 O 3 and CaO. A good correlation was observed between the degree of inhibition and the heat of formation of metal oxides. On the basis of kinetic model, the reduction of catalytic activity in the presence of oxygen was rationalized with the strength of oxygen adsorption on the metal oxide surface. (author)

Decomposition of methane over alumina supported Fe and Ni–Fe bimetallic catalyst: Effect of preparation procedure and calcination temperature

Directory of Open Access Journals (Sweden)

A.S. Al-Fatesh

2018-02-01

Full Text Available Catalytic decomposition of methane has been studied extensively as the production of hydrogen and formation of carbon nanotube is proven crucial from the scientific and technological point of view. In that context, variation of catalyst preparation procedure, calcination temperature and use of promoters could significantly alter the methane conversion, hydrogen yield and morphology of carbon nanotubes formed after the reaction. In this work, Ni promoted and unpromoted Fe/Al2O3 catalysts have been prepared by impregnation, sol–gel and co-precipitation method with calcination at two different temperatures. The catalysts were characterized by X-ray diffraction (XRD, N2 physisorption, temperature programmed reduction (TPR and thermogravimetric analysis (TGA techniques. The catalytic activity was tested for methane decomposition reaction. The catalytic activity was high when calcined at 500 °C temperature irrespective of the preparation method. However while calcined at high temperature the catalyst prepared by impregnation method showed a high activity. It is found from XRD and TPR characterization that disordered iron oxides supported on alumina play an important role for dissociative chemisorptions of methane generating molecular hydrogen. The transmission electron microscope technique results of the spent catalysts showed the formation of carbon nanotube which is having length of 32–34 nm. The Fe nanoparticles are present on the tip of the carbon nanotube and nanotube grows by contraction–elongation mechanism. Among three different methodologies impregnation method was more effective to generate adequate active sites in the catalyst surface. The Ni promotion enhances the reducibility of Fe/Al2O3 oxides showing a higher catalytic activity. The catalyst is stable up to six hours on stream as observed in the activity results.

Ozone decomposition on Ag/SiO{sub 2} and Ag/clinoptilolite catalysts at ambient temperature

Energy Technology Data Exchange (ETDEWEB)

Nikolov, Penko, E-mail: penmail@mail.bg [Institute of Catalysis, Bulgarian Academy of Sciences, 1113 Sofia (Bulgaria); Genov, Krassimir; Konova, Petya [Institute of General and Inorganic Chemistry, Bulgarian Academy of Sciences, 1113 Sofia (Bulgaria); Milenova, Katya; Batakliev, Todor; Georgiev, Vladimir [Institute of Catalysis, Bulgarian Academy of Sciences, 1113 Sofia (Bulgaria); Kumar, Narendra [Laboratory of Industrial Chemistry, Process Chemistry Centre, Abo Akademi University, Biskopsgatan 8, 20500 Abo/Turku (Finland); Sarker, Dipak K. [School of Pharmacy and Biomolecular Sciences, University of Brighton, Lewes Road, Brighton BN2 4GJ (United Kingdom); Pishev, Dimitar [University of Chemical Technology and Metallurgy, 1756 Sofia (Bulgaria); Rakovsky, Slavcho [Institute of Catalysis, Bulgarian Academy of Sciences, 1113 Sofia (Bulgaria)

2010-12-15

Silver modified zeolite (Bulgarian natural clinoptilolite) and Ag/silica catalysts were synthesized by ion exchange and incipient wet impregnation method respectively and characterized by different techniques. DC arc-AES was used for Ag detection. XRD spectra show that Ag is loaded over the surface of the SiO{sub 2} sample and that after the ion-exchange process the HEU type structure of clinoptilolite is retained. UV-VIS (specific reflection at 310 nm) and IR (band at 695 cm{sup -1}) spectroscopy analysis proved that silver is loaded as a T-atom into zeolite channels as Ag{sup +}, instead of Na{sup +}, Ca{sup 2+}, or K{sup +} ions, existing in the natural clinoptilolite form. The samples Ag/SiO{sub 2} and Ag-clinoptilolite were tested as catalysts for decomposition of gas phase ozone. Very high catalytic activity (up to 99%) was observed and at the same time the catalysts remained active over time at room temperature.

Spatially and size selective synthesis of Fe-based nanoparticles on ordered mesoporous supports as highly active and stable catalysts for ammonia decomposition.

Science.gov (United States)

Lu, An-Hui; Nitz, Joerg-Joachim; Comotti, Massimiliano; Weidenthaler, Claudia; Schlichte, Klaus; Lehmann, Christian W; Terasaki, Osamu; Schüth, Ferdi

2010-10-13

Uniform and highly dispersed γ-Fe(2)O(3) nanoparticles with a diameter of ∼6 nm supported on CMK-5 carbons and C/SBA-15 composites were prepared via simple impregnation and thermal treatment. The nanostructures of these materials were characterized by XRD, Mössbauer spectroscopy, XPS, SEM, TEM, and nitrogen sorption. Due to the confinement effect of the mesoporous ordered matrices, γ-Fe(2)O(3) nanoparticles were fully immobilized within the channels of the supports. Even at high Fe-loadings (up to about 12 wt %) on CMK-5 carbon no iron species were detected on the external surface of the carbon support by XPS analysis and electron microscopy. Fe(2)O(3)/CMK-5 showed the highest ammonia decomposition activity of all previously described Fe-based catalysts in this reaction. Complete ammonia decomposition was achieved at 700 °C and space velocities as high as 60,000 cm(3) g(cat)(-1) h(-1). At a space velocity of 7500 cm(3) g(cat)(-1) h(-1), complete ammonia conversion was maintained at 600 °C for 20 h. After the reaction, the immobilized γ-Fe(2)O(3) nanoparticles were found to be converted to much smaller nanoparticles (γ-Fe(2)O(3) and a small fraction of nitride), which were still embedded within the carbon matrix. The Fe(2)O(3)/CMK-5 catalyst is much more active than the benchmark NiO/Al(2)O(3) catalyst at high space velocity, due to its highly developed mesoporosity. γ-Fe(2)O(3) nanoparticles supported on carbon-silica composites are structurally much more stable over extended periods of time but less active than those supported on carbon. TEM observation reveals that iron-based nanoparticles penetrate through the carbon layer and then are anchored on the silica walls, thus preventing them from moving and sintering. In this way, the stability of the carbon-silica catalyst is improved. Comparison with the silica supported iron oxide catalyst reveals that the presence of a thin layer of carbon is essential for increased catalytic activity.

Iron ore catalysts for methane decomposition to make CO x free hydrogen and carbon nano material

KAUST Repository

Zhou, Lu; Enakonda, Linga Reddy; Li, Sheng; Gary, Daniel; Del-Gallo, Pascal; Mennemann, Christina; Basset, Jean-Marie

2018-01-01

In this work, for the first time, iron ores with 91.7%–96.2% FeO, 1.3%–2.3% AlO, 1.2%–4.5% SiO, 1.3%–3.9% NaO, were studied directly as bulk catalysts for methane decomposition. By hydrogen pre-reduction at 850 °C, FeO species on iron ores were

Reaction mechanism of ethylene glycol decomposition on Pt model catalysts: A density functional theory study

International Nuclear Information System (INIS)

Lv, Cun-Qin; Yang, Bo; Pang, Xian-Yong; Wang, Gui-Chang

2016-01-01

Highlights: • DFT calculations were performed to study the ethylene glycol decomposition on Pt. • The final products are CO and H_2 on Pt(111), (100) and (211). • Ethylene glycol decomposition on Pt(111) undergoes via initial O−H bond scission and followed by C−H bond cleavage. • Ethylene glycol decomposition proceeds via initial O−H bond scission and followed by O−H bond cleavage on Pt(100)/(211). - Abstract: Understanding and controlling bond beak sequence is important in catalytic processes. The DFT-GGA method combined with slab model was performed to study the ethylene glycol decomposition on various Pt model catalysts such as close-packed Pt(111), stepped Pt(211) and a more open one, Pt(100). Calculation results show that the adsorption energies of ethylene glycol and other decomposition species depend on the coordination number of surface atom, that is, low coordination number correspond to high adsorption energy. Moreover, it was found that final products of ethylene glycol decomposition are CO and H_2 on all model catalysts, but the reaction mechanism varies: On Pt(111), the first step is O−H bond scission, followed by C−H bond cleavage, namely C_2H_6O_2 → HOCH_2CH_2O + H → HOCH_2CHO + 2H→ HOCH_2CO +3H → OCH_2CO + 4H → OCHCO + 5H → CO + HCO + 5H → 2CO + 6H→ 2CO + 3H_2; On Pt(211) and Pt(100), however, it is a second O−H bond cleavage that follows the initial O−H bond scission, that is, C_2H_6O_2 → HOCH_2CH_2O + H → OCH_2CH_2O + 2H → OCHCH_2O + 3H → OCHCHO + 4H → 2HCO + 4H → 2CO + 6H → 2CO + 3H_2  on Pt(211), and C_2H_6O_2 →HOCH_2CH_2O+ H → OCH_2CH_2O + 2H→OCHCH_2O+3H→OCCH_2O+4H→CO+H_2CO+4H→CO+HCO+5H→2CO+6H→2CO+3H_2 on Pt(100) For the catalytic order of ethylene glycol to form H_2, it may be determined based on the rate-controlling step, and it is Pt(111) > Pt(211) > Pt(100).

Catalyst for Decomposition of Nitrogen Oxides

Science.gov (United States)

Schryer, David R. (Inventor); Jordan, Jeffrey D. (Inventor); Akyurtlu, Ates (Inventor); Akyurtlu, Jale (Inventor)

2015-01-01

This invention relates generally to a platinized tin oxide-based catalyst. It relates particularly to an improved platinized tin oxide-based catalyst able to decompose nitric oxide to nitrogen and oxygen without the necessity of a reducing gas.

Comparison of sol-gel prepared catalysts for CO oxidation and N2O decomposition reactions.

OpenAIRE

Euesden, Claire

2002-01-01

This thesis comprises analysis for two types of catalysis: CO oxidation and N2O decomposition; related by their research in sol-gel catalysis. The CO oxidation work was undertaken on behalf of Servomex plc in order to understand how their catalyst-based sensor (Tfx 1750) worked and why it failed when exposed to coal power station flue streams within its two-year guarantee period. This research will show, by means of many analytical techniques and catalytic tests: 1. A comparison of the Servom...

Kinetics of methane decomposition to CO{sub x}-free hydrogen and carbon nanofiber over Ni-Cu/MgO catalyst

Energy Technology Data Exchange (ETDEWEB)

Borghei, Maryam; Karimzadeh, Ramin [Chemical Engineering Department, Tarbiat Modares University, Tehran (Iran); Rashidi, Alimorad; Izadi, Nosrat [Research Center of Nanotechnology, Research Institute of Petroleum Industry, Tehran (Iran)

2010-09-15

Kinetic modeling of methane decomposition to CO{sub x}-free hydrogen and carbon nanofiber has been carried out in the temperature range 550-650 C over Ni-Cu/MgO catalyst from CH{sub 4}-H{sub 2} mixtures at atmospheric pressure. Assuming the different mechanisms of the reaction, several kinetic models were derived based on Langmuir-Hinshelwood type. The optimum value of kinetic parameters has been obtained by Genetic Algorithm and statistical analysis has been used for the model discrimination. The suggested kinetic model relates to the mechanism when the dissociative adsorption of methane molecule is the rate-determining stage and the estimated activation energy is 50.4 kJ/mol in agreement with the literature. The catalyst deactivation was found to be dependent on the time, reaction temperature, and partial pressures of methane and hydrogen. Inspection of the behavior of the catalyst activity in relation to time, led to a model of second order for catalyst deactivation. (author)

Influence of ionizing radiation on the catalytic properties of oxide catalysts tested by hydrogen peroxide decomposition

International Nuclear Information System (INIS)

Mucka, V.

1987-01-01

Results of a study of some physical and catalytic properties of different oxide catalysts as affected by ionizing radiation (γ, n, e - ) and tested by the decomposition of hydrogen peroxide in aqueous solution are presented in this paper. The oxidation state of the active component present on the catalyst surface was found to be one of the most sensitive properties to the ionizing radiation. Changes of this state induced by γ-irradiation were found to be positive in most cases; electron pre-irradiation of the oxides leads, as a rule, to negative effects and the effects of neutron irradiation may be positive or negative. On the other hand, changes in the catalytic activity of the oxides after γ-or electron-irradiation seem to be mostly negative and positive, respectively; the effects of fast neutrons seem to vary here. Neither quantitative or qualitative correlation was found between the radiation-induced changes in these two quantities. The results give evidence that ionizing radiation principally affects the surface concentration of the catalytic sites. Both the character and magnitude of the changes in surface oxidation abilities and in catalytic activities of the oxide catalysts seem to be dependent upon the actual state of the catalyst surface. (author)

Methamphetamine generates peroxynitrite and produces dopaminergic neurotoxicity in mice: protective effects of peroxynitrite decomposition catalyst.

Science.gov (United States)

Imam, S Z; Crow, J P; Newport, G D; Islam, F; Slikker, W; Ali, S F

1999-08-07

Methamphetamine (METH)-induced dopaminergic neurotoxicity is believed to be produced by oxidative stress and free radical generation. The present study was undertaken to investigate if METH generates peroxynitrite and produces dopaminergic neurotoxicity. We also investigated if this generation of peroxynitrite can be blocked by a selective peroxynitrite decomposition catalyst, 5, 10,15, 20-tetrakis(N-methyl-4'-pyridyl)porphyrinato iron III (FeTMPyP) and protect against METH-induced dopaminergic neurotoxicity. Administration of METH resulted in the significant formation of 3-nitrotyrosine (3-NT), an in vivo marker of peroxynitrite generation, in the striatum and also caused a significant increase in the body temperature. METH injection also caused a significant decrease in the concentration of dopamine (DA), 3, 4-dihydroxyphenylacetic acid (DOPAC), and homovanillic acid (HVA) by 76%, 53% and 40%, respectively, in the striatum compared with the control group. Treatment with FeTMPyP blocked the formation of 3-NT by 66% when compared with the METH group. FeTMPyP treatment also provided significant protection against the METH-induced hyperthermia and depletion of DA, DOPAC and HVA. Administration of FeTMPyP alone neither resulted in 3-NT formation nor had any significant effect on DA or its metabolite concentrations. These findings indicate that peroxynitrite plays a role in METH-induced dopaminergic neurotoxicity and also suggests that peroxynitrite decomposition catalysts may be beneficial for the management of psychostimulant abuse. Copyright 1999 Published by Elsevier Science B.V.

Thermal decomposition of supported lithium nitrate catalysts

Energy Technology Data Exchange (ETDEWEB)

Ruiz, Maria Lucia [INTEQUI (CONICET-UNSL), 25 de Mayo 384, V. Mercedes, 5730, San Luis (Argentina); Lick, Ileana Daniela [CINDECA (CONICET-UNLP), Calle 47 No 257, La Plata, 1900, Buenos Aires (Argentina); Ponzi, Marta Isabel [INTEQUI (CONICET-UNSL), 25 de Mayo 384, V. Mercedes, 5730, San Luis (Argentina); Castellon, Enrique Rodriguez; Jimenez-Lopez, Antonio [Departamento de Quimica Inorganica, Cristalografia y Mineralogia. Facultad de Ciencias, Universidad de Malaga, Campus de Teatinos, 29071 Malaga (Spain); Ponzi, Esther Natalia, E-mail: eponzi@quimica.unlp.edu.ar [CINDECA (CONICET-UNLP), Calle 47 No 257, La Plata, 1900, Buenos Aires (Argentina)

2010-02-20

New catalysts for soot combustion were prepared by impregnation of different supports (SiO{sub 2}, ZrO{sub 2} and ZrO{sub 2}.nH{sub 2}O) with a LiNO{sub 3} solution and then characterized by means of FTIR, XPS, TGA and UV-vis spectroscopy, whereby the presence of lithium nitrate in the prepared catalysts was identified and quantified. The soot combustion rate using this series of catalysts (LiNO{sub 3}/support) was compared with the activity of a series of impregnated catalysts prepared using LiOH (Li{sub 2}O/supports). Catalysts prepared using LiNO{sub 3} are found to be more active than those prepared using LiOH. The catalytic performance was also studied with a NO/O{sub 2} mixture in the feed, demonstrating that NO increases the combustion rate of soot, probably as a consequence of lithium oxide forming an 'in situ' nitrate ion.

Formic acid decomposition on Pt1/Cu (111) single platinum atom catalyst: Insights from DFT calculations and energetic span model analysis

Science.gov (United States)

Wang, Ying-Fan; Li, Kun; Wang, Gui-Chang

2018-04-01

Inspired by the recent surface experimental results that the monatomic Pt catalysts has more excellent hydrogen production that Cu(111) surface, the mechanism of decomposition of formic acid on Cu(111) and single atom Pt1/Cu(111) surface was studied by periodic density functional theory calculations in the present work. The results show that the formic acid tends to undergo dehydrogenation on both surfaces to obtain the hydrogen product of the target product, and the selectivity and catalytic activity of Pt1/Cu (111) surface for formic acid dehydrogenation are better. The reason is that the single atom Pt1/Cu(111) catalyst reduces the reaction energy barrier (i.e., HCOO → CO2 + H) of the critical step of the dehydrogenation reaction due to the fact that the single atom Pt1/Cu(111) catalyst binds formate weakly compared to that of Cu (111) one. Moreover, it was found that the Pt1/Cu (111) binds CO more strongly than that of Cu (111) one and thus leading to the difficult for the formation of CO. These two factors would make the single Pt atom catalyst had the high selectivity for the H2 production. It is hoped that the present work may help people to design the efficient H2 production from HCOOH decomposition by reduce the surface binding strength of HCOO species, for example, using the low coordination number active site like single atom or other related catalytic system.

IN SITU INFRARED STUDY OF CATALYTIC DECOMPOSITION OF NITRIC OXIDE (NO); FINAL

International Nuclear Information System (INIS)

Unknown

1999-01-01

The growing concerns for the environment and increasingly stringent standards for NO emission have presented a major challenge to control NO emissions from electric utility plants and automobiles. Catalytic decomposition of NO is the most attractive approach for the control of NO emission for its simplicity. Successful development of an effective catalyst for NO decomposition will greatly decrease the equipment and operation cost of NO control. Due to lack of understanding of the mechanism of NO decomposition, efforts on the search of an effective catalyst have been unsuccessful. Scientific development of an effective catalyst requires fundamental understanding of the nature of active site, the rate-limiting step, and an approach to prolong the life of the catalyst. The authors have investigated the feasibility of two novel approaches for improving catalyst activity and resistance to sintering. The first approach is the use of silanation to stabilize metal crystallites and supports for Cu-ZSM-5 and promoted Pt catalysts; the second is utilization of oxygen spillover and desorption to enhance NO decomposition activity. The silanation approach failed to stabilize Cu-ZSM-5 activity under hydrothermal condition. Silanation blocked the oxygen migration and inhibited oxygen desorption. Oxygen spillover was found to be an effective approach for promoting NO decomposition activity on Pt-based catalysts. Detailed mechanistic study revealed the oxygen inhibition in NO decomposition and reduction as the most critical issue in developing an effective catalytic approach for controlling NO emission

Catalyst study for the plasma exhaust purification process

International Nuclear Information System (INIS)

Chabot, J.; Sannier, J.

1990-01-01

Several catalysts available from commercial sources have been screened to find out specific catalysts which allow complete methane oxidation and ammonia decomposition at temperature as low as possible in order to minimize tritium loss by permeation through processing equipment walls. Afterwards, an extended kinetic investigation has been performed on the best catalysts to achieve the data necessary to unit calculations. For methane oxidation, a palladium on alumina catalyst shows a very satisfactory low-temperature efficiency while a non-precious metal catalyst made of nickel oxide and alumina was found to be the more efficient for ammonia decomposition

Ni/Ce-MCM-41 mesostructured catalysts for simultaneous production of hydrogen and nanocarbon via methane decomposition

Energy Technology Data Exchange (ETDEWEB)

Guevara, J.C.; Wang, J.A.; Chen, L.F.; Valenzuela, M.A. [ESIQIE, Instituto Politecnico Nacional, Col. Zacatenco, Av. Politecnico s/n, 07738 Mexico D. F. (Mexico); Salas, P. [Centro de Fisica Aplicada y Tecnologia Avanzada, Universidad Nacional Autonoma de Mexico, Apartado Postal 1-1010, Queretaro 76000 (Mexico); Garcia-Ruiz, A. [UPIICSA, Instituto Politecnico Nacional, Te 950 Col. Granjas-Mexico, 08400 Mexico D.F. (Mexico); Toledo, J.A.; Cortes-Jacome, M.A.; Angeles-Chavez, C. [Programa de Molecular Ingenieria, Instituto Mexicano del Petroleo, Eje Lazaro Cardenas 152, 07730 Mexico D. F. (Mexico); Novaro, O. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, A. P. 20-364, 01000 Mexico D.F. (Mexico)

2010-04-15

For the first time, simultaneous production of hydrogen and nanocarbon via catalytic decomposition of methane over Ni-loaded mesoporous Ce-MCM-41 catalysts was investigated. The catalytic performance of the Ni/Ce-MCM-41 catalysts is very stable and the reaction activity remained almost unchanged during 1400 min steam on time at temperatures 540, 560 and 580 C, respectively. The methane conversion level over these catalysts reached 60-75% with a 100% selectivity towards hydrogen. TEM observations revealed that most of the Ni particles located on the tip of the carbon nanofibers/nanotubes in the used catalysts, keeping their exposed surface clean during the test and thus remaining active for continuous reaction without obvious deactivation. Two kinds of carbon materials, graphitic carbon (C{sub g}) as major and amorphous carbon (C{sub A}) as minor were produced in the reaction, as confirmed by XRD analysis and TEM observations. Carbon nanofibers/nanotubes had an average diameter of approximately 30-50 nm and tens micrometers in length, depending on the reaction temperature, reaction time and Ni particle diameter. Four types of carbon nanofibers/nanotubes were detected and their formations greatly depend on the reaction temperature, time on steam and degree of the interaction between the metallic Ni and support. The respective mechanisms of the formation of nanocarbons were postulated and discussed. (author)

CATALYSTS NHI Thermochemical Systems FY 2009 Year-End Report

International Nuclear Information System (INIS)

Ginosar, Daniel M.

2009-01-01

Fiscal Year 2009 work in the Catalysts project focused on advanced catalysts for the decomposition of sulfuric acid, a reaction common to both the Sulfur-Iodine (S-I) cycle and the Hybrid Sulfur cycle. Prior years effort in this project has found that although platinum supported on titanium oxide will be an acceptable catalyst for sulfuric acid decomposition in the integrated laboratory scale (ILS) project, the material has short comings, including significant cost and high deactivation rates due to sintering and platinum evaporation. For pilot and larger scale systems, the catalyst stability needs to be improved significantly. In Fiscal Year 2008 it was found that at atmospheric pressure, deactivation rates of a 1 wt% platinum catalyst could be reduced by 300% by adding either 0.3 wt% iridium (Ir) or 0.3 wt% ruthenium (Ru) to the catalyst. In Fiscal Year 2009, work focused on examining the platinum group metal catalysts activity and stability at elevated pressures. In addition, simple and complex metal oxides are known to catalyze the sulfuric acid decomposition reaction. These metal oxides could offer activities comparable to platinum but at significantly reduced cost. Thus a second focus for Fiscal Year 2009 was to explore metal oxide catalysts for the sulfuric acid decomposition reaction. In Fiscal Year 2007 several commercial activated carbons had been identified for the HI decomposition reaction; a reaction specific to the S-I cycle. Those materials should be acceptable for the pilot scale project. The activated carbon catalysts have some disadvantages including low activity at the lower range of reactor operating temperature (350 to 400 C) and a propensity to generate carbon monoxide in the presence of water that could contaminate the hydrogen product, but due to limited funding, this area had low priority in Fiscal Year 2009. Fiscal Year 2009 catalyst work included five tasks: development, and testing of stabilized platinum based H2SO4 catalysts

Application of sodium carbonate prevents sulphur poisoning of catalysts in automated total mercury analysis

Science.gov (United States)

McLagan, David S.; Huang, Haiyong; Lei, Ying D.; Wania, Frank; Mitchell, Carl P. J.

2017-07-01

Analysis of high sulphur-containing samples for total mercury content using automated thermal decomposition, amalgamation, and atomic absorption spectroscopy instruments (USEPA Method 7473) leads to rapid and costly SO2 poisoning of catalysts. In an effort to overcome this issue, we tested whether the addition of powdered sodium carbonate (Na2CO3) to the catalyst and/or directly on top of sample material increases throughput of sulphur-impregnated (8-15 wt%) activated carbon samples per catalyst tube. Adding 5 g of Na2CO3 to the catalyst alone only marginally increases the functional lifetime of the catalyst (31 ± 4 g of activated carbon analyzed per catalyst tube) in relation to unaltered catalyst of the AMA254 total mercury analyzer (17 ± 4 g of activated carbon). Adding ≈ 0.2 g of Na2CO3 to samples substantially increases (81 ± 17 g of activated carbon) catalyst life over the unaltered catalyst. The greatest improvement is achieved by adding Na2CO3 to both catalyst and samples (200 ± 70 g of activated carbon), which significantly increases catalyst performance over all other treatments and enables an order of magnitude greater sample throughput than the unaltered samples and catalyst. It is likely that Na2CO3 efficiently sequesters SO2, even at high furnace temperatures to produce Na2SO4 and CO2, largely negating the poisonous impact of SO2 on the catalyst material. Increased corrosion of nickel sampling boats resulting from this methodological variation is easily resolved by substituting quartz boats. Overall, this variation enables an efficient and significantly more affordable means of employing automated atomic absorption spectrometry instruments for total mercury analysis of high-sulphur matrices.

Catalytic N 2O decomposition on Pr 0.8Ba 0.2MnO 3 type perovskite catalyst for industrial emission control

Czech Academy of Sciences Publication Activity Database

Kumar, S.; Vinu, A.; Šubrt, Jan; Bakardjieva, Snejana; Rayalu, S.; Teraoka, Y.; Labhsetwar, N.

2012-01-01

Roč. 198, 1-SI (2012), s. 125-132 ISSN 0920-5861 R&D Projects: GA MŠk LC523 Institutional support: RVO:61388980 Keywords : Ba substituted perovskite * catalyst * honeycomb * N 2O decomposition * perovskite * praseodymium manganate Subject RIV: CA - Inorganic Chemistry Impact factor: 2.980, year: 2012

Investigatons on the local structure of AG+/ZSM-5 catalysts and their photocatalytic reactivities for the decomposition of N2O at 298 κ

International Nuclear Information System (INIS)

Matsuoka, Masaya; Ju, Woo-Sung; Yamashita, Hiromi; Anpo, Masakazu

2001-01-01

Ag + /ZSM-5 catalysts were prepared by an ion-exchange method and UV-irradiation of the catalysts in the presence of N 2 O led to the photo-catalytic decomposition of N 2 O into N 2 and O 2 at 298 κ. Investigations on the effective wavelength of irradiated UV-light for the reaction as well as the in-situ characterization of the catalysts by means of XAFS, UV-Vis, photoluminescence and FT-IR spectroscopies revealed that the photoexcitation of the Ag + -N 2 O complexes formed between gaseous N 2 O and the isolated Ag + ions play a significant role in this reaction. (au)

Ir catalysts: Preventing CH3COOH formation in ethanol oxidation

Science.gov (United States)

Miao, Bei; Wu, Zhipeng; Xu, Han; Zhang, Minhua; Chen, Yifei; Wang, Lichang

2017-11-01

Current catalysts used for ethanol oxidation reaction (EOR) cannot effectively prevent CH3COOH formation, and thus become a major hindrance for direct ethanol fuel cell applications. We report an Ir catalyst that shows great promise for a complete EOR based on density functional theory calculations using PBE functional. The reaction barrier on Ir(1 0 0) was found to be 2.10 eV for CH3COOH formation, which is much higher than currently used Pd and Pt, and 0.57 eV for Csbnd C bond cleavage in CHCO species, which are comparable to Pd and Pt. The result suggests future directions for studying optimal complete EOR catalysts.

A Nanomesoporous Catalyst from Modified Red Mud and Its Application for Methane Decomposition to Hydrogen Production

Directory of Open Access Journals (Sweden)

Xiaoke Fang

2016-01-01

Full Text Available A type of nanomesoporous modified red mud (MRM catalyst was prepared and utilized for catalytic methane decomposition (CMD to produce hydrogen. The modification process significantly simplified the mineral composition of the red mud (RM; in the meantime, the physical and chemical structure of RM was changed. TEM images suggested that MRM was a kind of nanomesoporous material assembled by a number of uniformly nanoscale particles, BET results showed that the pore size distributions of MRM were ranged from 3 to 12 nm, and the specific surface area and total pore volumes of red mud improved from 8.00 m2/g and 0.08 cm3/g to 190.61 m2/g and 0.39 cm3/g, respectively. The catalytic performance of the catalysts has been tested at 800°C; the results showed that MRM exhibited much higher activity and stability than RM for CMD.

Decomposition of ammonium nitrate in homogeneous and catalytic denitration

International Nuclear Information System (INIS)

Anan'ev, A. V.; Tananaev, I. G.; Shilov, V. P.

2005-01-01

Ammonium nitrate is one of potentially explosive by-products of spent fuel reprocessing. Decomposition of ammonium nitrate in the HNO 3 -HCOOH system was studied in the presence or absence of Pt/SiO 2 catalyst. It was found that decomposition of ammonium nitrate is due to homogeneous noncatalytic oxidation of ammonium ion with nitrous acid generated in the HNO 3 -HCOOH system during denitration. The platinum catalyst initiates the reaction of HNO 3 with HCOOH to form HNO 2 . The regular trends were revealed and the optimal conditions of decomposition of ammonium nitrate in nitric acid solutions were found [ru

Catalysis mechanism of Pd-promoted γ-alumina in the thermal decomposition of methane to hydrogen: A density functional theory study

Energy Technology Data Exchange (ETDEWEB)

Salam, M. Abdus; Abdullah, Bawadi, E-mail: bawadi_abdullah@utp.edu.my

2017-02-15

Thermo-catalytic methane decomposition to elemental hydrogen mechanism in transitional metals (Pd, Ni & Mo) promoted Al{sub 2}O{sub 3} (001) catalyst have been studied using the density functional theory (DFT). Decomposition reactions are spontaneous and favourable above 775 K for all promoter. Pd-promoted Al{sub 2}O{sub 3} (001) catalyst demonstrates a breakthrough decomposition activity in hydrogen production as compared to Ni− and Mo-promoted Al{sub 2}O{sub 3} (001) catalysts. The activation energy (E{sub a}) range of the catalysis for Pd promoted Al{sub 2}O{sub 3} (001) catalysts is 0.003–0.34 eV. Whereas, Ni and Mo promoted Al{sub 2}O{sub 3} (001) catalysts display activation energy E{sub a} in the range of 0.63–1.15 eV and 0.04–5.98 eV, respectively. Pd-promoted catalyst also shows a higher adsorption energy (−0.68 eV) and reactivity than that of Ni and Mo promoted Al{sub 2}O{sub 3} (001) catalysts. The rates of successive decomposition of methane are found to be 16.15 × 10{sup 12}, 15.95 × 10{sup 12} and 16.09 × 10{sup 12} s{sup −1} for the promoter of Pd, Ni and Mo, respectively. Pd promoted Al{sub 2}O{sub 3} (001) catalyst reduces the methane decomposition temperature (775 K) and deactivation rate significantly. The catalytic conditions and catalyst is promising in producing hydrogen to support hydrogen economy. - Highlights: • Transition metals (Pd, Ni & Mo) promoted γ-alumina catalysts are designed successfully. • Pd-promoted catalyst showed breakthrough activity in methane decomposition to hydrogen. • DFT study explored the catalysis mechanism of methane decomposition at atomic level. • Pd-promoted catalyst reduced temperature and activation barrier of methane decomposition reaction significantly.

Catalysis mechanism of Pd-promoted γ-alumina in the thermal decomposition of methane to hydrogen: A density functional theory study

International Nuclear Information System (INIS)

Salam, M. Abdus; Abdullah, Bawadi

2017-01-01

Thermo-catalytic methane decomposition to elemental hydrogen mechanism in transitional metals (Pd, Ni & Mo) promoted Al_2O_3 (001) catalyst have been studied using the density functional theory (DFT). Decomposition reactions are spontaneous and favourable above 775 K for all promoter. Pd-promoted Al_2O_3 (001) catalyst demonstrates a breakthrough decomposition activity in hydrogen production as compared to Ni− and Mo-promoted Al_2O_3 (001) catalysts. The activation energy (E_a) range of the catalysis for Pd promoted Al_2O_3 (001) catalysts is 0.003–0.34 eV. Whereas, Ni and Mo promoted Al_2O_3 (001) catalysts display activation energy E_a in the range of 0.63–1.15 eV and 0.04–5.98 eV, respectively. Pd-promoted catalyst also shows a higher adsorption energy (−0.68 eV) and reactivity than that of Ni and Mo promoted Al_2O_3 (001) catalysts. The rates of successive decomposition of methane are found to be 16.15 × 10"1"2, 15.95 × 10"1"2 and 16.09 × 10"1"2 s"−"1 for the promoter of Pd, Ni and Mo, respectively. Pd promoted Al_2O_3 (001) catalyst reduces the methane decomposition temperature (775 K) and deactivation rate significantly. The catalytic conditions and catalyst is promising in producing hydrogen to support hydrogen economy. - Highlights: • Transition metals (Pd, Ni & Mo) promoted γ-alumina catalysts are designed successfully. • Pd-promoted catalyst showed breakthrough activity in methane decomposition to hydrogen. • DFT study explored the catalysis mechanism of methane decomposition at atomic level. • Pd-promoted catalyst reduced temperature and activation barrier of methane decomposition reaction significantly.

Facile and large-scale synthesis of high quality few-layered graphene nano-platelets via methane decomposition over unsupported iron family catalysts

Energy Technology Data Exchange (ETDEWEB)

Awadallah, Ahmed E., E-mail: ahmedelsayed_epri@yahoo.com [Process Development Division, Egyptian Petroleum Research Institute, 11727 Cairo (Egypt); Aboul-Enein, Ateyya A. [Process Development Division, Egyptian Petroleum Research Institute, 11727 Cairo (Egypt); Kandil, Usama F. [Petroleum Application Department, Egyptian Petroleum Research Institute, 11727 Cairo (Egypt); Taha, Mahmoud Reda [Department of Civil Engineering, University of New Mexico, Albuquerque, NM 87131 (United States)

2017-04-15

High quality few-layered graphene nano-platelets (GNPs) were successfully prepared via catalytic chemical vapor deposition of methane under ambient pressure using substrate-free unsupported iron, cobalt, and nickel metallic sheets as catalysts. The bulk catalysts were prepared via combustion method using citric acid as a fuel. Various analytical techniques, including high-resolution transmission electron microscopy (TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), temperature programmed reduction (TPR) and Raman spectroscopy were employed to characterize the fresh and reduced catalysts and to identify the morphological structure of the as-grown GNPs. TEM images of the reduced metal catalysts showed that polycrystalline metallic sheets were easily produced after complete reduction of unsupported metal oxides. The data demonstrated that the formation of zero-valent metallic sheets could effectively promote the growth of GNPs on their surfaces. The unsupported Ni catalyst exhibits higher catalytic growth activity in terms of GNPs yield (254 wt%) compared with all other catalysts. Raman spectra and TEM results established that a few layers of GNPs with high crystallinity and good graphitization were produced. TGA results further demonstrated that the as-grown GNPs exhibit significantly higher thermal stability in air atmosphere compared with other synthesis methods. - Highlights: • Few-layered graphene nanoplatelets were prepared via methane catalytic decomposition. • Metallic sheets of iron group metals were used as novel catalysts. • The surfaces of metallic sheets were found to be very effective for GNPs growth. • The number of layers is dependent on the morphological structure of the catalysts. • The unsupported metallic Ni catalyst exhibited higher catalytic growth activity.

Study on Endurance and Performance of Impregnated Ruthenium Catalyst for Thruster System.

Science.gov (United States)

Kim, Jincheol; Kim, Taegyu

2018-02-01

Performance and endurance of the Ru catalyst were studied for nitrous oxide monopropellant thruster system. The thermal decomposition of N2O requires a considerably high temperature, which make it difficult to be utilized as a thruster propellant, while the propellant decomposition temperature can be reduced by using the catalyst through the decomposition reaction with the propellant. However, the catalyst used for the thruster was frequently exposed to high temperature and high-pressure environment. Therefore, the state change of the catalyst according to the thruster operation was analyzed. Characterization of catalyst used in the operation condition of the thruster was performed using FE-SEM and EDS. As a result, performance degradation was occurred due to the volatilization of Ru catalyst and reduction of the specific surface area according to the phase change of Al2O3.

Cobalt Oxide Catalysts Supported on CeO2–TiO2 for Ethanol Oxidation and N2O Decomposition.

Czech Academy of Sciences Publication Activity Database

Jirátová, Květa; Kovanda, F.; Balabánová, Jana; Koloušek, D.; Klegová, A.; Pacultová, K.; Obalová, L.

2017-01-01

Roč. 12, č. 1 (2017), s. 121-139 ISSN 1878-5190. [Pannonian Symposium on Catalysis. Siófok, 19.09.2016-23.09.2016] R&D Projects: GA ČR GA14-13750S Institutional support: RVO:67985858 Keywords : cobalt oxide catalysts * ethanol total oxidation * N2O decomposition Subject RIV: CI - Industrial Chemistry, Chemical Engineering OBOR OECD: Chemical process engineering Impact factor: 1.264, year: 2016

The platinum catalysed decomposition of hydrazine in acidic media

International Nuclear Information System (INIS)

Ananiev, A.V.; Tananaev, I.G.; Brossard, Ph.; Broudic, J.C.

2000-01-01

Kinetic study of the hydrazine decomposition in the solutions of HClO 4 , H 2 SO 4 and HNO 3 in the presence of Pt/SiO 2 catalyst has been undertaken. It was shown that the kinetics of the hydrazine catalytic decomposition in HClO 4 and H 2 SO 4 are identical. The process is determined by the heterogeneous catalytic auto-decomposition of N 2 H 4 on the catalyst's surface. The platinum catalysed hydrazine decomposition in the nitric acid solutions is a complex process, including heterogeneous catalytic auto-decomposition of N 2 H 4 , reaction of hydrazine with catalytically generated nitrous acid and the catalytic oxidation of hydrazine by nitric acid. The kinetic parameters of these reactions have been determined. The contribution of each reaction in the total process is determined by the liquid phase composition and by the temperature. (authors)

Bifunctional Characteristics of Al2O3 supported Ni in the HI Decomposition of Sulfur-Iodine Process

Directory of Open Access Journals (Sweden)

Park Chu-Sik

2016-01-01

Full Text Available The Sulfur-Iodine process is in need of catalytic reactor for HI decomposition because the HI decomposition reaction rate is very slow. Nickel as an alternative catalyst for platinum was investigated in this study. Al2O3 supported Ni catalysts were prepared by impregnation method. Ni amounts loaded over Al2O3 were in the range of 0.1~20 wt. %. HI decompositions were carried out in the temperature range of 573 ~ 773 K using the fixed-bed quartz reactor. The difference of catalysts before and after the reaction was analyzed using BET, CO/H2 chemisorption, XRD, XRF and SEM. It was confirmed by XRD and SEM-EDX analysis that Ni was converted to NiI2 during the HI decomposition. Catalyst deactivation due to the formation of NiI2 leads to a reduction of HI conversion. Although Ni of catalyst converted to NiI2, HI decomposition with low loading (up to 3 wt. % catalyst showed a little decrease of HI conversion. However, with more than 5 wt. % catalyst, the initial HI conversion was considerably decreased. In the particular case of 20 wt. %, the initial conversion was increased close to 60 %, which is higher than 20 % as an equilibrium conversion at 723 K. These results showed that Ni had not only a catalytic function for HI decomposition, but also function as a sorbent to absorb I2 produced from HI.

Silver-palladium catalysts for the direct synthesis of hydrogen peroxide

Science.gov (United States)

Khan, Zainab; Dummer, Nicholas F.; Edwards, Jennifer K.

2017-11-01

A series of bimetallic silver-palladium catalysts supported on titania were prepared by wet impregnation and assessed for the direct synthesis of hydrogen peroxide, and its subsequent side reactions. The addition of silver to a palladium catalyst was found to significantly decrease hydrogen peroxide productivity and hydrogenation, but crucially increase the rate of decomposition. The decomposition product, which is predominantly hydroxyl radicals, can be used to decrease bacterial colonies. The interaction between silver and palladium was characterized using scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy (XPS) and temperature programmed reduction (TPR). The results of the TPR and XPS indicated the formation of a silver-palladium alloy. The optimal 1% Ag-4% Pd/TiO2 bimetallic catalyst was able to produce approximately 200 ppm of H2O2 in 30 min. The findings demonstrate that AgPd/TiO2 catalysts are active for the synthesis of hydrogen peroxide and its subsequent decomposition to reactive oxygen species. The catalysts are promising for use in wastewater treatment as they combine the disinfectant properties of silver, hydrogen peroxide production and subsequent decomposition. This article is part of a discussion meeting issue 'Providing sustainable catalytic solutions for a rapidly changing world'.

Decomposition of environmentally persistent perfluorooctanoic acid in water by photochemical approaches.

Science.gov (United States)

Hori, Hisao; Hayakawa, Etsuko; Einaga, Hisahiro; Kutsuna, Shuzo; Koike, Kazuhide; Ibusuki, Takashi; Kiatagawa, Hiroshi; Arakawa, Ryuichi

2004-11-15

The decomposition of persistent and bioaccumulative perfluorooctanoic acid (PFOA) in water by UV-visible light irradiation, by H202 with UV-visible light irradiation, and by a tungstic heteropolyacid photocatalyst was examined to develop a technique to counteract stationary sources of PFOA. Direct photolysis proceeded slowly to produce CO2, F-, and short-chain perfluorocarboxylic acids. Compared to the direct photolysis, H2O2 was less effective in PFOA decomposition. On the other hand, the heteropolyacid photocatalyst led to efficient PFOA decomposition and the production of F- ions and CO2. The photocatalyst also suppressed the accumulation of short-chain perfluorocarboxylic acids in the reaction solution. PFOA in the concentrations of 0.34-3.35 mM, typical of those in wastewaters after an emulsifying process in fluoropolymer manufacture, was completely decomposed by the catalyst within 24 h of irradiation from a 200-W xenon-mercury lamp, with no accompanying catalyst degradation, permitting the catalyst to be reused in consecutive runs. Gas chromatography/mass spectrometry (GC/MS) measurements showed no trace of environmentally undesirable species such as CF4, which has a very high global-warming potential. When the (initial PFOA)/(initial catalyst) molar ratio was 10: 1, the turnover number for PFOA decomposition reached 4.33 over 24 h of irradiation.

Methane-induced Activation Mechanism of Fused Ferric Oxide-Alumina Catalysts during Methane Decomposition

KAUST Repository

Reddy Enakonda, Linga

2016-06-27

Activation of Fe2O3-Al2O3 with CH4 (instead of H2) is a meaningful method to achieve catalytic methane decomposition (CMD). This reaction of CMD is more economic and simple against commercial methane steam reforming (MSR) as it produces COx-free H2. In this study, for the first time, structure changes of the catalyst were screened during CH4 reduction with time on stream. The aim was to optimize the pretreatment conditions through understanding the activation mechanism. Based on results from various characterization techniques, reduction of Fe2O3 by CH4 proceeds in three steps: Fe2O3→Fe3O4→FeO→Fe0. Once Fe0 is formed, it decomposes CH4 with formation of Fe3C, which is the crucial initiation step in the CMD process to initiate formation of multiwall carbon nanotubes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Research on catalysts for long-life closed-cycle CO2 laser oaperation

Science.gov (United States)

Sidney, Barry D.; Schryer, David R.; Upchurch, Billy T.; Hess, Robert V.; Wood, George M.

1987-01-01

Long-life, closed-cycle operation of pulsed CO2 lasers requires catalytic CO-O2 recombination both to remove O2, which is formed by discharge-induced CO2 decomposition, and to regenerate CO2. Platinum metal on a tin-oxide substrate (Pt/SnO2) has been found to be an effective catalyst for such recombination in the desired temperature range of 25 to 100 C. This paper presents a description of ongoing research at NASA-Langley on Pt/SnO2 catalyzed CO-O2 recombination. Included are studies with rare-isotope gases since rare-isotope CO2 is desirable as a laser gas for enhanced atmospheric transmission. Results presented include: (1) the effects of various catalyst pretreatment techniques on catalyst efficiency; (2) development of a technique, verified in a 30-hour test, to prevent isotopic scrambling when C(O-18) and (O-18)2 are reacted in the presence of a common-isotope Pt/Sn(O-16)2 catalyst; and (3) development of a mathematical model of a laser discharge prior to catalyst introduction.

Prevention of dopaminergic neurotoxicity by targeting nitric oxide and peroxynitrite: implications for the prevention of methamphetamine-induced neurotoxic damage.

Science.gov (United States)

Imam, S Z; Islam, F; Itzhak, Y; Slikker, W; Ali, S F

2000-09-01

Methamphetamine (METH) is a neurotoxic psychostimulant that produces catecholaminergic brain damage by producing oxidative stress and free radical generation. The role of oxygen and nitrogen radicals is well documented as a cause of METH-induced neurotoxic damage. In this study, we have obtained evidence that METH-induced neurotoxicity is the resultant of interaction between oxygen and nitrogen radicals, and it is mediated by the production of peroxynitrite. We have also assessed the effects of inhibitors of neuronal nitric oxide synthase (nNOS) as well as scavenger of nitric oxide and a peroxynitrite decomposition catalyst. Significant protective effects were observed with the inhibitor of nNOS, 7-nitroindazole (7-NI), as well as by the selective peroxynitrite scavenger or decomposition catalyst, 5,10,15,20-tetrakis(2,4,6-trimethyl-3,5-sulfonatophenyl)porphyrinato iron III (FeTPPS). However, the use of a nitric oxide scavenger, 2-phenyl-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide (c-PTIO), did not provide any significant protection against METH-induced hyperthermia or peroxynitrite generation and the resulting dopaminergic neurotoxicity. In particular, treatment with FeTPPS completely prevented METH-induced hyperthermia, peroxynitrite production, and METH-induced dopaminergic depletion. Together, these data demonstrate that METH-induced dopaminergic neurotoxicity is mediated by the generation of peroxynitrite, which can be selectively protected by nNOS inhibitors or peroxynitrite scavenger or decomposition catalysts.

A New Bioinspired Perchlorate Reduction Catalyst with Significantly Enhanced Stability via Rational Tuning of Rhenium Coordination Chemistry and Heterogeneous Reaction Pathway.

Science.gov (United States)

Liu, Jinyong; Han, Mengwei; Wu, Dimao; Chen, Xi; Choe, Jong Kwon; Werth, Charles J; Strathmann, Timothy J

2016-06-07

Rapid reduction of aqueous ClO4(-) to Cl(-) by H2 has been realized by a heterogeneous Re(hoz)2-Pd/C catalyst integrating Re(O)(hoz)2Cl complex (hoz = oxazolinyl-phenolato bidentate ligand) and Pd nanoparticles on carbon support, but ClOx(-) intermediates formed during reactions with concentrated ClO4(-) promote irreversible Re complex decomposition and catalyst deactivation. The original catalyst design mimics the microbial ClO4(-) reductase, which integrates Mo(MGD)2 complex (MGD = molybdopterin guanine dinucleotide) for oxygen atom transfer (OAT). Perchlorate-reducing microorganisms employ a separate enzyme, chlorite dismutase, to prevent accumulation of the destructive ClO2(-) intermediate. The structural intricacy of MGD ligand and the two-enzyme mechanism for microbial ClO4(-) reduction inspired us to improve catalyst stability by rationally tuning Re ligand structure and adding a ClOx(-) scavenger. Two new Re complexes, Re(O)(htz)2Cl and Re(O)(hoz)(htz)Cl (htz = thiazolinyl-phenolato bidentate ligand), significantly mitigate Re complex decomposition by slightly lowering the OAT activity when immobilized in Pd/C. Further stability enhancement is then obtained by switching the nanoparticles from Pd to Rh, which exhibits high reactivity with ClOx(-) intermediates and thus prevents their deactivating reaction with the Re complex. Compared to Re(hoz)2-Pd/C, the new Re(hoz)(htz)-Rh/C catalyst exhibits similar ClO4(-) reduction activity but superior stability, evidenced by a decrease of Re leaching from 37% to 0.25% and stability of surface Re speciation following the treatment of a concentrated "challenge" solution containing 1000 ppm of ClO4(-). This work demonstrates the pivotal roles of coordination chemistry control and tuning of individual catalyst components for achieving both high activity and stability in environmental catalyst applications.

Urea thermolysis and NOx reduction with and without SCR catalysts

International Nuclear Information System (INIS)

Fang, Howard L.; DaCosta, Herbert F.M.

2003-01-01

Urea-selective catalytic reduction (SCR) has been a leading contender for removal of nitrogen oxides (deNO x ) from diesel engine emissions. Despite its advantages, the SCR technology faces some critical detriments to its catalytic performance such as catalyst surface passivation (caused by deposit formation) and consequent stoichiometric imbalance of the urea consumption. Deposit formation deactivates catalytic performance by not only consuming part of the ammonia produced during urea decomposition but also degrading the structural and thermal properties of the catalyst surface. We have characterized the urea thermolysis with and without the urea-SCR catalyst using both spectroscopic (DRIFTS and Raman) and thermal techniques (thermal gravimetric analysis (TGA) and differential scanning calorimetry (DSC)) to identify the deposit components and their corresponding thermal properties. Urea thermolysis exhibits two decomposition stages, involving ammonia generation and consumption, respectively. The decomposition after the second stage leads to the product of melamine complexes, (HNC=NH) x (HNCO) y , that hinder catalytic performance. The presence of catalyst accompanied with a good spray of the urea solution helps to eliminate the second stage. In this work, kinetics of the direct reduction of NO x by urea is determined and the possibility of using additives to the urea solution in order to rejuvenate the catalyst surface and improve its performance will be discussed

Catalytic performance and durability of Ni/AC for HI decomposition in sulfur–iodine thermochemical cycle for hydrogen production

International Nuclear Information System (INIS)

Fu, Guangshi; He, Yong; Zhang, Yanwei; Zhu, Yanqun; Wang, Zhihua; Cen, Kefa

2016-01-01

Highlights: • The relation between Ni content and Ni particle dispersion were disclosed. • The effect of Ni content on the catalytic activity of Ni/AC catalyst was revealed. • The optimal content of Ni for Ni/AC catalysts in HI decomposition was found. - Abstract: This work reports the Ni content effect on the Ni/AC catalytic performance in the HI decomposition reaction of the sulfur–iodine (SI) thermochemical cycle for hydrogen production and the Ni/AC catalyst durability in a long-term test. Accordingly, five catalysts with the Ni content ranging from 5% to 15% were prepared by an incipient-wetness impregnation method. The activity of all catalysts was examined under the temperature range of 573–773 K. The catalytic performance evaluation suggests that Ni content plays a significant role in the Ni dispersion, Ni particle size, and eventually the catalytic activity in HI decomposition. 12% is the optimal Ni content for Ni/AC catalysts in HI decomposition which is balanced between poor dispersion of Ni particles and increasing active center. The results of 24 h durability test, which incorporated with BET and TEM investigations of the 12%Ni/AC catalyst before and after the reaction, indicate that establishing a better Ni particle dispersion pattern and improving the stability of Ni particles on the support should be considered in the future.

Catalytic Combustion of Low Concentration Methane over Catalysts Prepared from Co/Mg-Mn Layered Double Hydroxides

Directory of Open Access Journals (Sweden)

Hongfeng Liu

2014-01-01

Full Text Available A series of Co/Mg-Mn mixed oxides were synthesized through thermal decomposition of layered double hydroxides (LDHs precursors. The resulted catalysts were then subjected for catalytic combustion of methane. Experimental results revealed that the Co4.5Mg1.5Mn2LDO catalyst possessed the best performance with the T90=485°C. After being analyzed via XRD, BET-BJH, SEM, H2-TPR, and XPS techniques, it was observed that the addition of cobalt had significantly improved the redox ability of the catalysts whilst certain amount of magnesium was essential to guarantee the catalytic activity. The presence of Mg was helpful to enhance the oxygen mobility and, meanwhile, improved the dispersion of Co and Mn oxides, preventing the surface area loss after calcination.

Catalyst for hydrogen-amine D exchange

International Nuclear Information System (INIS)

Holtslander, W.J.; Johnson, R.E.

1976-01-01

A process is claimed for deuterium isotopic enrichment (suitable for use in heavy water production) by amine-hydrogen exchange in which the exchange catalyst comprises a mixture of alkyl amides of two metals selected from the group consisting of the alkali metals. Catalyst mixtures comprising at least one of the alkali amides of lithium and potassium are preferred. At least one of the following benefits are obtained: decreased hydride formation, decreased thermal decomposition of alkyl amide, increased catalyst solubility in the amine phase, and increased exchange efficiency. 11 claims

Catalysts for Efficient Production of Carbon Nanotubes

Science.gov (United States)

Sun, Ted X.; Dong, Yi

2009-01-01

Several metal alloys have shown promise as improved catalysts for catalytic thermal decomposition of hydrocarbon gases to produce carbon nanotubes (CNTs). Heretofore almost every experiment on the production of carbon nanotubes by this method has involved the use of iron, nickel, or cobalt as the catalyst. However, the catalytic-conversion efficiencies of these metals have been observed to be limited. The identification of better catalysts is part of a continuing program to develop means of mass production of high-quality carbon nanotubes at costs lower than those achieved thus far (as much as $100/g for purified multi-wall CNTs or $1,000/g for single-wall CNTs in year 2002). The main effort thus far in this program has been the design and implementation of a process tailored specifically for high-throughput screening of alloys for catalyzing the growth of CNTs. The process includes an integral combination of (1) formulation of libraries of catalysts, (2) synthesis of CNTs from decomposition of ethylene on powders of the alloys in a pyrolytic chemical-vapor-decomposition reactor, and (3) scanning- electron-microscope screening of the CNTs thus synthesized to evaluate the catalytic efficiencies of the alloys. Information gained in this process is put into a database and analyzed to identify promising alloy compositions, which are to be subjected to further evaluation in a subsequent round of testing. Some of these alloys have been found to catalyze the formation of carbon nano tubes from ethylene at temperatures as low as 350 to 400 C. In contrast, the temperatures typically required for prior catalysts range from 550 to 750 C.

Cu–Co–O nano-catalysts as a burn rate modifier for composite solid propellants

Directory of Open Access Journals (Sweden)

D. Chaitanya Kumar Rao

2016-08-01

Full Text Available Nano-catalysts containing copper–cobalt oxides (Cu–Co–O have been synthesized by the citric acid (CA complexing method. Copper (II nitrate and Cobalt (II nitrate were employed in different molar ratios as the starting reactants to prepare three types of nano-catalysts. Well crystalline nano-catalysts were produced after a period of 3 hours by the calcination of CA–Cu–Co–O precursors at 550 °C. The phase morphologies and crystal composition of synthesized nano-catalysts were examined using Scanning Electron Microscope (SEM, Energy Dispersive Spectroscopy (EDS and Fourier Transform Infrared Spectroscopy (FTIR methods. The particle size of nano-catalysts was observed in the range of 90 nm–200 nm. The prepared nano-catalysts were used to formulate propellant samples of various compositions which showed high reactivity toward the combustion of HTPB/AP-based composite solid propellants. The catalytic effects on the decomposition of propellant samples were found to be significant at higher temperatures. The combustion characteristics of composite solid propellants were significantly improved by the incorporation of nano-catalysts. Out of the three catalysts studied in the present work, CuCo-I was found to be the better catalyst in regard to thermal decomposition and burning nature of composite solid propellants. The improved performance of composite solid propellant can be attributed to the high crystallinity, low agglomeration and lowering the decomposition temperature of oxidizer by the addition of CuCo-I nano-catalyst.

Effect of Gas Flowrate on Nucleation Mechanism of MWCNTs for a Compound Catalyst

Directory of Open Access Journals (Sweden)

S. Shukrullah

2017-01-01

Full Text Available Activation of the catalyst particles during a CVD process can be anticipated from the carbon feeding rate. In this study, Fe2O3/Al2O3 catalyst was synthesized with uniformly dispersed iron over alumina support for onward production of multiwalled carbon nanotubes (MWCNTs in a fluidized bed chemical CVD reactor. The effect of the ethylene flowrate on catalytic activity of the compound catalyst and morphology of the as-grown MWCNTs was also investigated in this study. The dispersed active phases of the catalyst and optimized gas flowrate helped in improving the tube morphology and prevented the aggregation of the as-grown MWCNTs. The flowrates, below 100 sccm, did not provide sufficient reactants to interact with the catalyst for production of defect-free CNT structures. Above 100 sccm, concentration of the carbon precursor did not show notable influence on decomposition rate of the gas molecules. The most promising results on growth and structural properties of MWCNTs were gained at ethylene flowrate of 100 sccm. At this flowrate, the ratio of G and D intensity peaks (IG/ID was deliberated about 1.40, which indicates the growth of graphitic structures of MWCNTs.

The influence of water vapor and sulfur dioxide on the catalytic decomposition of nitrous oxide

Energy Technology Data Exchange (ETDEWEB)

Yalamas, C.; Heinisch, R.; Barz, M. [Technische Univ. Berlin (Germany). Inst. fuer Energietechnik; Cournil, M. [Ecole Nationale Superieure des Mines, 42 - Saint-Etienne (France)

2001-03-01

For the nitrous oxide decomposition three groups of catalysts such as metals on support, hydrotalcites, and perovskites were studied relating to their activity in the presence of vapor or sulfur dioxide, in the temperature range from 200 to 500 C. It was found that the water vapor strongly inhibates the nitrous oxide decomposition at T=200-400 C. The sulfur dioxide poisons the catalysts, in particular the perovskites. (orig.)

Sustainable fuel production by thermocatalytic decomposition of methane – A review

Directory of Open Access Journals (Sweden)

K. Srilatha

2017-12-01

Full Text Available Thermocatalytic Decomposition of Methane (TCD is a completely green single step technology for producing hydrogen and carbon nanomaterials. This paper review about the research in laboratory-scale on TCD, specifically the recent advances like co-feeding effect and regeneration of catalyst for enhancing the productivity of the entire process. Although a remarkable success on the laboratory-scale has been fulfilled, TCD for free greenhouse gas (GHG hydrogen production is still in its infancy. The necessity for commercialization of TCD is more than ever in the present-day condition of massive GHG emission. TCD generally studied over several types of catalysts, for example mono, bi, trimetallic, combination of metal–metal oxide, carbon and metal doped carbon catalysts. Catalyst Deactivation is the main problem found in TCD process. Regeneration of catalyst and co-feeding of methane with other hydrocarbon are the two main solutions placed helped in accordance to overcome deactivation problem. Higher amount of co-feed hydrocarbon in situ produce more amount of highly active carbon deposits which support further methane decomposition to produce extra hydrogen. The conversion rate of methane increases with increasing temperature and decreases with the flow rate in the co-feeding process in a comparable manner as observed in normal TCD. The presence of co-components in the post-reaction stream is an important challenge attempted in the co-feeding and regeneration. Keywords: Hydrogen, Catalysts, Thermocatalytic decomposition

Catalysts for long-life closed-cycle CO2 lasers

Science.gov (United States)

Schryer, David R.; Sidney, Barry D.; Miller, Irvin M.; Hess, Robert V.; Wood, George M.; Batten, Carmen E.; Burney, Lewis G.; Hoyt, Ronald F.; Paulin, Patricia A.; Brown, Kenneth G.

1987-01-01

Long-life, closed-cycle operation of pulsed CO2 lasers requires catalytic CO-O2 recombination both to remove O2, which is formed by discharge-induced CO2 decomposition, and to regenerate CO2. Platinum metal on a tin (IV) oxide substrate (Pt/SnO2) has been found to be an effective catalyst for such recombination in the desired temperature range of 25 to 100 C. This paper presents a description of ongoing research at NASA-LaRC on Pt/SnO2 catalyzed CO-O2 recombination. Included are studies with rare-isotope gases since rare-isotope CO2 is desirable as a laser gas for enhanced atmospheric transmission. Results presented include: (1) achievement of 98% to 100% conversion of a stoichiometric mixture of CO and O2 to CO2 for 318 hours (greater than 1 x 10 to the 6th power seconds), continuous, at a catalyst temperature of 60 C, and (2) development of a technique verified in a 30-hour test, to prevent isotopic scrambling when CO-18 and O-18(2) are reacted in the presence of a common-isotope Pt/Sn O-16(2) catalyst.

Application of microscopy technology in thermo-catalytic methane decomposition to hydrogen

Energy Technology Data Exchange (ETDEWEB)

Mei, Irene Lock Sow, E-mail: irene.sowmei@gmail.com; Lock, S. S. M., E-mail: serenelock168@gmail.com; Abdullah, Bawadi, E-mail: bawadi-abdullah@petronas.com.my [Chemical Engineering Department, Universiti Teknologi PETRONAS, Bandar Sri Iskandar, 31750, Perak (Malaysia)

2015-07-22

Hydrogen production from the direct thermo-catalytic decomposition of methane is a promising alternative for clean fuel production because it produces pure hydrogen without any CO{sub x} emissions. However, thermal decomposition of methane can hardly be of any practical and empirical interest in the industry unless highly efficient and effective catalysts, in terms of both specific activity and operational lifetime have been developed. In this work, bimetallic Ni-Pd on gamma alumina support have been developed for methane cracking process by using co-precipitation and incipient wetness impregnation method. The calcined catalysts were characterized to determine their morphologies and physico-chemical properties by using Brunauer-Emmett-Teller method, Field Emission Scanning Electron Microscopy, Energy-dispersive X-ray spectroscopy and Thermogravimetric Analysis. The results suggested that that the catalyst which is prepared by the co-precipitation method exhibits homogeneous morphology, higher surface area, have uniform nickel and palladium dispersion and higher thermal stability as compared to the catalyst which is prepared by wet impregnation method. This characteristics are significant to avoid deactivation of the catalysts due to sintering and carbon deposition during methane cracking process.

Nanoparticle-assisted photo-Fenton reaction for photo-decomposition of humic acid

Science.gov (United States)

Banik, Jhuma; Basumallick, Srijita

2017-11-01

We report here the synthesis of CuO-doped ZnO composite nanomaterials (NMs) by chemical route and demonstrated for the first time that these NMs are efficient catalysts for H2O2-assisted photo-decomposition (photo-Fenton type catalyst) of humic acid, a natural pollutant of surface water by solar irradiation. This has been explained by faster electron transfer to OH radical at the p-n hetero-junction of this composite catalyst. Application of this composite catalyst in decomposing humus substances of local pond water by solar energy has been demonstrated.

SO2 influence on the K/La2O3 soot combustion catalyst deactivation

International Nuclear Information System (INIS)

Peralta, M.A.; Ulla, M.A.; Querini, C.A.

2008-01-01

In the present work, K/La 2 O 3 was prepared and tested as a potential catalyst to be used in a diesel engine exhaust. The soot combustion activity was evaluated by temperature-programmed-oxidation (TPO), and the NO x -catalyst interaction was studied using a microbalance experiment. The SO 2 poisoning process and the regeneration of a poisoned K/La 2 O 3 catalyst were analyzed. The fresh catalyst presented a good soot combustion activity. After being treated with a 1000 ppm SO 2 stream, the catalyst was poisoned due to lanthanum sulfate and potassium sulfate formation. The NO x treatment contributed to the K 2 (SO 4 ) decomposition at the expense of extra La 2 (SO 4 ) 3 formation and the H 2 treatment contributed to the La 2 (SO 4 ) 3 decomposition. (author)

Alkaline leaching for synthesis of improved Fe-ZSM5 catalysts

NARCIS (Netherlands)

Espinosa, S; Mentruit, C; Kapteijn, F; Moulijn, JA; Melián-Cabrera, I.

Fe-ZSM5 catalysts were fully Fe-exchanged by pretreating the parent zeolite with base a solution prior to the Fe-exchange. The catalysts prepared in this way showed very low amount of inactive FeOx and improved performance in N2O decomposition. Alkaline leaching breaks down the zeolite crystals -

Iridium-catalyst-based autonomous bubble-propelled graphene micromotors with ultralow catalyst loading.

Science.gov (United States)

Wang, Hong; Sofer, Zdeněk; Eng, Alex Yong Sheng; Pumera, Martin

2014-11-10

A novel concept of an iridium-based bubble-propelled Janus-particle-type graphene micromotor with very high surface area and with very low catalyst loading is described. The low loading of Ir catalyst (0.54 at %) allows for fast motion of graphene microparticles with high surface area of 316.2 m(2)  g(-1). The micromotor was prepared with a simple and scalable method by thermal exfoliation of iridium-doped graphite oxide precursor composite in hydrogen atmosphere. Oxygen bubbles generated from the decomposition of hydrogen peroxide at the iridium catalytic sites provide robust propulsion thrust for the graphene micromotor. The high surface area and low iridium catalyst loading of the bubble-propelled graphene motors offer great possibilities for dramatically enhanced cargo delivery. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Pretreatment of Platinum/Tin Oxide-Catalyst

Science.gov (United States)

Hess, Robert V.; Paulin, Patricia A.; Miller, Irvin M.; Schryer, David R.; Sidney, Barry D.; Wood, George M.; Upchurch, Billy T.; Brown, Kenneth G.

1987-01-01

Addition of CO to He pretreatment doubles catalytic activity. In sealed, high-energy, pulsed CO2 laser, CO and O2 form as decomposition products of CO2 in laser discharge zone. Products must be recombined, because oxygen concentration of more than few tenths of percent causes rapid deterioration of power, ending in unstable operation. Promising low-temperature catalyst for combining CO and O2 is platinum on tin oxide. New development increases activity of catalyst so less needed for recombination process.

Catalytic activity of γ-irradiated transition metal ions in the decomposition of hydrogen peroxide

International Nuclear Information System (INIS)

Arnikar, H.J.; Kapadi, A.H.; Gohad, A.S.; Bhosale, S.B.

1988-01-01

The catalystic decomposition of hydrogen peroxide by transition metal ions, Fe 2+ , Fe 3+ , Co 2+ and Cu 2+ , adsorbed on neutral α-alumina was studied over the temperature range of 295-313 K. γ-irradiation of the catalysts to a dose of 0.12 MGy enhanced markedly the first order decomposition rate. Negligible in the case of Cu 2+ , the radiation effect increased roughly in the order of the number of unpaired d electrons in these ions: Cu(II), Fe(II), Co(II) and Fe(III). Results are explained on the basis of Kremer's mechanism of electron induced heterogeneous decomposition of H 2 O 2 . The radiation effect is attributed to the initial excess of electrons released from traps in the beginning of the reaction

Trends in catalytic NO decomposition over transition metal surfaces

DEFF Research Database (Denmark)

Falsig, Hanne; Bligaard, Thomas; Rass-Hansen, Jeppe

2007-01-01

The formation of NOx from combustion of fossil and renewable fuels continues to be a dominant environmental issue. We take one step towards rationalizing trends in catalytic activity of transition metal catalysts for NO decomposition by combining microkinetic modelling with density functional...... theory calculations. We show specifically why the key problem in using transition metal surfaces to catalyze direct NO decomposition is their significant relative overbinding of atomic oxygen compared to atomic nitrogen....

Catalytic Oxidation of Phenol over Zeolite Based Cu/Y-5 Catalyst: Part 1: Catalyst Preparation and Characterization

Directory of Open Access Journals (Sweden)

K. Maduna Valkaj

2015-01-01

Full Text Available The necessity to remove organic pollutants from the industrial wastewater streams has forced the development of new technologies that can produce better results in terms of pollutant removal and process efficiency in combination with low investment and operating costs. One of the new emerging processes with a potential to fulfil these demands is catalytic wet peroxide oxidation, commonly known as the CWPO process. The oxidative effect of the hydrogen peroxide is intensified by the addition of a heterogeneous catalyst that can reduce the operating conditions to atmospheric pressure and temperatures below 383 K. Zeolites, among others, are especially appealing as catalysts for selective oxidation processes due to their unique characteristics such as shape selectivity, thermal and chemical stability, and benign effect on nature and the living world. In this work, catalytic activity, selectivity and stability of Cu/Y-5 zeolite in phenol oxidation with hydrogen peroxide was examined. Catalyst samples were prepared by ion exchange method of the protonic form of commercial zeolite. The catalysts were characterized with powder X-ray diffraction (XRD, scanning electron microscopy (SEM, and AAS elemental analysis, while the adsorption techniques were used for the measurement of the specific surface area. The catalytic tests were carried out in a stainless steel Parr reactor in batch operation mode at the atmospheric pressure and in the temperature range from 323 to 353 K. The catalyst was prepared in powdered form and the mass fraction of the active metal component on the zeolite was 3.46 %. The initial concentration of phenol solution was equal to 0.01 mol dm−3 and the concentration of hydrogen peroxide ranged from 0.01 to 0.10 mol dm−3. The obtained experimental data was tested to a proposed kinetic model for phenol oxidation r = k1 cF cVP and hydrogen peroxide decomposition rHP = k2 cHP. The kinetic parameters were estimated using the Nelder

A Review of Study on Thermal Energy Transport System by Synthesis and Decomposition Reactions of Methanol

Science.gov (United States)

Liu, Qiusheng; Yabe, Akira; Kajiyama, Shiro; Fukuda, Katsuya

The study on thermal energy transport system by synthesis and decomposition reactions of methanol was reviewed. To promote energy conservation and global environment protection, a two-step liquid-phase methanol synthesis process, which starts with carbonylation of methanol to methyl formate, then followed by the hydrogenolysis of the formate, was studied to recover wasted or unused discharged heat from industrial sources for the thermal energy demands of residential and commercial areas by chemical reactions. The research and development of the system were focused on the following three points. (1) Development of low-temperature decomposition and synthetic catalysts, (2) Development of liquid phase reactor (heat exchanger accompanying chemical reaction), (3) Simulation of the energy transport efficiency of entire system which contains heat recovery and supply sections. As the result of the development of catalyst, promising catalysts which agree with the development purposes for the methyl formate decomposition reaction and the synthetic reaction are being developed though some studies remain for the methanol decomposition and synthetic reactions. In the fundamental development of liquid phase reactor, the solubilities of CO and H2 gases in methanol and methyl formate were measured by the method of total pressure decrease due to absorption under pressures up to 1500kPa and temperatures up to 140°C. The diffusivity of CO gas in methanol was determined by measuring the diameter and solution time of single CO bubbles in methanol. The chemical reaction rate of methanol synthesis by hydrogenolysis of methyl formate was measured using a plate-type of Raney copper catalyst in a reactor with rectangular channel and in an autoclave reactor. The reaction characteristics were investigated by carrying out the experiments at various temperatures, flow rates and at various catalyst development conditions. We focused on the effect of Raney copper catalyst thickness on the liquid

Catalytic activity of metal borides in the reaction of decomposition

International Nuclear Information System (INIS)

Labodi, I.; Korablev, L.I.; Tavadyan, L.A.; Blyumberg, Eh.A.

1982-01-01

Catalytic effect of CoB, MoB 2 , ZrB 2 and NbB 2 , prepared by the method of self-propagating high-temperature synthesis, on decomposition of tertiary butyl hydroperoxide has been studied. A technigue of determination of action mechanism of heterogeneous catalysts in liquid-phase process is suggested. It is established that CoB in contrast to other metal borides catalyzes only hydroperoxide decomposition into radicals

Reactivity of nanoaggregations of platinum on supports of different nature in reactions of catalytic decomposition of hydrazine in acid media

International Nuclear Information System (INIS)

Anan'ev, A.V.; Boltoeva, M.Yu.; Grigor'ev, M.S.; Shilov, V.P.; Sharygin, L.M.

2006-01-01

Platinized catalysts on the basis of supports of different chemical nature are tested in reactions of catalytic hydrazine decomposition in perchloric and nitric acid solutions. In perchloric acid catalytic activity of catalysts on the basis of ceramic materials of Termoksid brand is higher of activity of catalysts on the basis of amorphous silica gel. In nitric acid solutions opposite dependence is observed. Tendency of ceramic supports to peptization in acid solutions is pointed out. Results obtained are interpreted using conceptions of energetic heterogeneity of surface atoms and hydrazine catalytic decomposition mechanisms in different media [ru

Synthesis of multi-layer graphene and multi-wall carbon nanotubes from direct decomposition of ethanol by microwave plasma without using metal catalysts

International Nuclear Information System (INIS)

Rincón, R; Melero, C; Jiménez, M; Calzada, M D

2015-01-01

The synthesis of nanostructured carbon materials by using microwave plasmas at atmospheric pressure is presented. This technique involves only one step and without any other supplementary chemical process or metal catalyst. Multi-layer graphene, multi-wall carbon nananotubes and H 2 were obtained by the plasma after ethanol decomposition. Strong emissions of both C 2 molecular bands and C carbon were emitted by the plasma during the process. Futhermore, plasma parameters were studied. Our research shows that both C 2 radicals and high gas temperatures (>3000 K) are required for the synthesis of these materials, which contribute to the understanding of materials synthesis by plasma processes. (fast track communication)

ETHANOL OXIDATION OVER AU/TIO2 CATALYSTS

African Journals Online (AJOL)

DR. AMINU

The adsorption and reaction of ethanol over Au/TiO2 catalysts was investigated using pulse ... the surface disappears, so the mechanism reverts to a decomposition pathway, producing methane, ... allowed to flow at a rate of 30 ml per minutes.

Catalytic N{sub 2}O decomposition in a model tail gas from nitric acid plants; Decomposition catalytique du protoxyde d'azote dans un modele de gaz de queue produits par un atelier d'acide nitrique

Energy Technology Data Exchange (ETDEWEB)

Mul, G.; Xu, X.; Perez Ramirez, J.; Vaccaro, A.R.; Kapteijn, F.; Moulijn, J.A. [Delft University of Technology, Faculty of Chemical Technology and Materials Sciences, Delft (Netherlands)

2001-07-01

In this study direct catalytic decomposition of N{sub 2}O in simulated tail-gas from nitric acid plants, containing water, oxygen, NO{sub x}, was investigated. Three groups of catalysts were prepared: oxide-supported catalysts; zeolite-based catalysts; mixed oxides derived from hydrotalcites-like (HTLc) materials. The activity of these types of catalysts was tested in an advanced automated six-flow reactor system. Nobel metal (Ru, Rh) based catalysts, either supported on zeolites or ex-hydrotalcite compositions (Mg-Al or Co-Al mixed oxides), and Fe-ZSM-5 effectively decompose N{sub 2}O in tail-gas conditions at temperatures of about 400-450 deg C, typical for certain nitric acid plants. Catalysts active for tail gas temperatures of 230-250 deg C, typical for other nitric acid plants, were not found. This is mainly due to the dramatic negative effect of especially water and NO{sub x} on the conversion of N{sub 2}O. The negative effect of NO{sub x} observed for many catalysts might be related to the formation of surface nitrites and nitrates, blocking active sites for N{sub 2}O decomposition in the 200-300 deg C temperature range. (authors)

Catalytic Ammonia Decomposition over High-Performance Ru/Graphene Nanocomposites for Efficient COx-Free Hydrogen Production

Directory of Open Access Journals (Sweden)

Gang Li

2017-01-01

Full Text Available Highly-dispersed Ru nanoparticles were grown on graphene nanosheets by simultaneously reducing graphene oxide and Ru ions using ethylene glycol (EG, and the resultant Ru/graphene nanocomposites were applied as a catalyst to ammonia decomposition for COx-free hydrogen production. Tuning the microstructures of Ru/graphene nanocomposites was easily accomplished in terms of Ru particle size, morphology, and loading by adjusting the preparation conditions. This was the key to excellent catalytic activity, because ammonia decomposition over Ru catalysts is structure-sensitive. Our results demonstrated that Ru/graphene prepared using water as a co-solvent greatly enhanced the catalytic performance for ammonia decomposition, due to the significantly improved nano architectures of the composites. The long-term stability of Ru/graphene catalysts was evaluated for COx-free hydrogen production from ammonia at high temperatures, and the structural evolution of the catalysts was investigated during the catalytic reactions. Although there were no obvious changes in the catalytic activities at 450 °C over a duration of 80 h, an aggregation of the Ru nanoparticles was still observed in the nanocomposites, which was ascribed mainly to a sintering effect. However, the performance of the Ru/graphene catalyst was decreased gradually at 500 °C within 20 h, which was ascribed mainly to both the effect of the methanation of the graphene nanosheet under a H2 atmosphere and to enhanced sintering under high temperatures.

The effect of peroxynitrite decomposition catalyst MnTBAP on aldehyde dehydrogenase-2 nitration by organic nitrates: role in nitrate tolerance.

Science.gov (United States)

Mollace, Vincenzo; Muscoli, Carolina; Dagostino, Concetta; Giancotti, Luigino Antonio; Gliozzi, Micaela; Sacco, Iolanda; Visalli, Valeria; Gratteri, Santo; Palma, Ernesto; Malara, Natalia; Musolino, Vincenzo; Carresi, Cristina; Muscoli, Saverio; Vitale, Cristiana; Salvemini, Daniela; Romeo, Francesco

2014-11-01

Bioconversion of glyceryl trinitrate (GTN) into nitric oxide (NO) by aldehyde dehydrogenase-2 (ALDH-2) is a crucial mechanism which drives vasodilatory and antiplatelet effect of organic nitrates in vitro and in vivo. Oxidative stress generated by overproduction of free radical species, mostly superoxide anions and NO-derived peroxynitrite, has been suggested to play a pivotal role in the development of nitrate tolerance, though the mechanism still remains unclear. Here we studied the free radical-dependent impairment of ALDH-2 in platelets as well as vascular tissues undergoing organic nitrate ester tolerance and potential benefit when using the selective peroxynitrite decomposition catalyst Mn(III) tetrakis (4-Benzoic acid) porphyrin (MnTBAP). Washed human platelets were made tolerant to nitrates via incubation with GTN for 4h. This was expressed by attenuation of platelet aggregation induced by thrombin (40U/mL), an effect accompanied by GTN-related induction of cGMP levels in platelets undergoing thrombin-induced aggregation. Both effects were associated to attenuated GTN-induced nitrite formation in platelets supernatants and to prominent nitration of ALDH-2, the GTN to NO metabolizing enzyme, suggesting that GTN tolerance was associated to reduced NO formation via impairment of ALDH-2. These effects were all antagonized by co-incubation of platelets with MnTBAP, which restored GTN-induced responses in tolerant platelets. Comparable effect was found under in in vivo settings. Indeed, MnTBAP (10mg/kg, i.p.) significantly restored the hypotensive effect of bolus injection of GTN in rats made tolerants to organic nitrates via chronic administration of isosorbide-5-mononitrate (IS-5-MN), thus confirming the role of peroxynitrite overproduction in the development of tolerance to vascular responses induced by organic nitrates. In conclusion, oxidative stress subsequent to prolonged use of organic nitrates, which occurs via nitration of ALDH-2, represents a key event

Catalytic activity of laminated compounds of graphite with transitions metals in decomposition of alcohols and formic acid

International Nuclear Information System (INIS)

Novikov, Yu.N.; Lapkina, N.D.; Vol'pin, M.E.

1976-01-01

The catalytic activity is studied of laminated graphite compounds with Fe, Co, Ni, Cu, Mo, W and Mn both in the reduced and oxidized forms in gas phase decomposition reactions of isopropyl, n-butyl, cyclohexyl, and 4-tret-butylcyclohexyl alcohols, and also formic acid. All the catalysts are shown to be active in the reactions where isopropyl and n-butyl alcohols undergo decomposition. The laminated compounds of graphite with Co and Ni both in the oxidized and reduction form are the most active catalysts of the selective decomposition of alcohols to aldehydes and ketones, and also formic acid to CO 2 and H 2 . The kinetics of a number of reactions is found to obey the second order equation with allowance made for the system volume

Thermal decomposition behaviors of magnesium borohydride doped with metal fluoride additives

International Nuclear Information System (INIS)

Zhang, Z.G.; Wang, H.; Liu, J.W.; Zhu, M.

2013-01-01

Highlights: • The decomposition proceeded through several distinct steps. • The mixed materials show a dramatically low initial hydrogen release temperature. • The additives react with the Mg–B–H compounds rather than acting as catalysts. • The reaction process was studied using an in situ TEM. - Abstract: The thermal decomposition behaviors of Magnesium borohydride [Mg(BH 4 ) 2 ] and metal fluoride doped mixtures were studied by temperature programmed desorption measurement/mass spectrometry (TPD/MS), differential scanning calorimetry (DSC) and in situ transmission electron microscope (TEM) observations. The decomposition and release of hydrogen proceeded through several distinct steps, including two polymorphic transitions, ionic Mg(BH 4 ) 2 melting with solid Mg–B–H amorphous phase formation and Mg–B–H decomposition. The addition of additives such as CaF 2 , ZnF 2 and TiF 3 resulted in a decrease in the hydrogen release temperature. ZnF 2 and TiF 3 reduced the initial hydrogen release temperature to ca. 50 °C. However, hydrogen release during the transformation from γ-Mg(BH 4 ) 2 to the amorphous Mg–B–H compounds at ca. 300 °C was only 4.5 wt.% in contrast to 9.8 wt.% for the direct decomposition of pure Mg(BH 4 ) 2 . TEM observations confirmed that ZnF 2 and TiF 3 reacted with amorphous Mg–B–H compounds rather than acting as catalysts

Phosgene-free synthesis of hexamethylene-1,6-diisocyanate by the catalytic decomposition of dimethylhexane-1,6-dicarbamate over zinc-incorporated berlinite (ZnAlPO{sub 4})

Energy Technology Data Exchange (ETDEWEB)

Sun, Da-Lei [Department of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006 (China); College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082 (China); Luo, Jun-Yin; Wen, Ru-Yu [Department of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006 (China); Deng, Jian-Ru [College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082 (China); Chao, Zi-Sheng, E-mail: zschao@yahoo.com [College of Chemistry and Chemical Engineering, State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082 (China)

2014-02-15

Highlights: • Synthesis of HDI via HDU decomposition over ZnAlPO{sub 4} heterogeneous catalyst. • Employment of self-designed reliable fixed bed reactor for HDU decomposition to HDI. • As high as 89.4% yield of HDI over ZnAlPO{sub 4} catalyst. • High stability and large ability for repeating usage of ZnAlPO{sub 4} catalyst. -- Abstract: The phosgene-free synthesis of hexamethylene-1,6-diisocyanate (HDI) by the decomposition of dimethylhexane-1,6-dicarbamate (HDU) was carried out on a self-designed fixed-bed catalytic reactor, using zinc-incorporated berlinite (ZnAlPO{sub 4}) as catalyst, dioctyl phthalate (DOP) as solvent and N{sub 2} as carrier gas. Factors influencing the yield of HDI, including the Zn/Al molar ratio, HDU concentration and liquid space velocity (LHSV), were investigated. Under the optimized reaction conditions, i.e., 4.8 wt.% concentration of HDU in DOP, 100 ml/min N{sub 2} flow rate, 0.09 MPa vacuum, 623 K reaction temperature, 1.2 h{sup −1} LHSV and catalyst usage 2.0 g, a 89.4% yield of HDI had been achieved over the ZnAlPO{sub 4} (molar ratio Zn/Al = 0.04) catalyst. The ZnAlPO{sub 4} catalyst was found to exhibit a considerable large on-stream stability and could be repeatedly used in the decomposition of HDU to HDI, after its regeneration.

Behaviors of glucose decomposition during acid-catalyzed hydrothermal hydrolysis of pretreated Gelidium amansii.

Science.gov (United States)

Jeong, Tae Su; Choi, Chang Ho; Lee, Ji Ye; Oh, Kyeong Keun

2012-07-01

Acid-catalyzed hydrothermal hydrolysis is one path to cellulosic glucose and subsequently to its dehydration end products such as hydroxymethyl furfural (HMF), formic acid and levulinic acid. The effect of sugar decomposition not only lowers the yield of fermentable sugars but also forms decomposition products that inhibit subsequent fermentation. The present experiments were conducted with four different acid catalysts (H(2)SO(4), HNO(3), HCl, and H(3)PO(4)) at various acid normalities (0.5-2.1N) in batch reactors at 180-210 °C. From the results, H(2)SO(4) was the most suitable catalyst for glucose production, but glucose decomposition occurred during the hydrolysis. The glucose production was maximized at 160.7 °C, 2.0% (w/v) H(2)SO(4), and 40 min, but resulted in a low glucan yield of 33.05% due to the decomposition reactions, which generated formic acid and levulinic acid. The highest concentration of levulinic acid, 7.82 g/L, was obtained at 181.2 °C, 2.0% (w/v) H(2)SO(4), and 40 min. Copyright © 2012 Elsevier Ltd. All rights reserved.

Nanocrystalline transition metal oxides as catalysts in the thermal decomposition of ammonium perchlorate

Energy Technology Data Exchange (ETDEWEB)

Kapoor, Inder Pal Singh; Srivastava, Pratibha; Singh, Gurdip [Department of Chemistry, DDU Gorakhpur University, Gorakhpur (India)

2009-08-15

Nanocrystalline transition metal oxides (NTMOs) have been successfully prepared by three different methods: novel quick precipitation method (Cr{sub 2}O{sub 3} and Fe{sub 2}O{sub 3}); surfactant mediated method (CuO), and reduction of metal complexes with hydrazine as reducing agent (Mn{sub 2}O{sub 3}). The nano particles have been characterized by X-ray diffraction (XRD) which shows an average particle diameter of 35-54 nm. Their catalytic activity was measured in the thermal decomposition of ammonium perchlorate (AP). AP decomposition undergoes a two step process where the addition of metal oxide nanocrystals led to a shifting of the high temperature decomposition peak toward lower temperature. The kinetics of the thermal decomposition of AP and catalyzed AP has also been evaluated using model fitting and isoconversional method. (Abstract Copyright [2009], Wiley Periodicals, Inc.)

Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide

KAUST Repository

Bourlinos, Athanasios B.

2017-03-21

We present the first bottom-up approach to synthesize Fe(III)-functionalized carbon dots (CDs) from molecular precursors without the need of conventional thermal or microwave treatment and additional reagents. Specifically, sonication of xylene in the presence of anhydrous FeCl3 results in oxidative coupling of the aromatic substrate towards Fe(III)-functionalized CDs. The as-prepared CDs are spherical in shape with a size of 3–8 nm, highly dispersible in organic solvents and display wavelength-dependent photoluminescence (PL). The iron ions attached to the surface endow the CDs with superior catalytic activity for olefin hydrogenation with excellent conversion and selectivity (up to 100%). The Fe(III)-CDs are more effective in the hydrogenation of a series of electron donating or withdrawing olefin substrates compared to conventional homogeneous or heterogeneous Fe(III)-based catalysts. The as-prepared heterogeneous nanocatalyst can be used repeatedly without any loss of catalytic activity. Importantly, the stability of the new catalysts can be easily monitored by PL intensity or quantum yield measurements, which certainly opens the doors for real time monitoring in a range of applications. Additionally, to the best of our knowledge, for the first time, the oxidative property of Fe-CDs was also explored in decomposition of hydrogen peroxide in water with the first order rate constant of 0.7 × 10−2 min−1, proving the versatile catalytic properties of such hybrid systems.

Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide

KAUST Repository

Bourlinos, Athanasios B.; Rathi, Anuj K.; Gawande, Manoj B.; Hola, Katerina; Goswami, Anandarup; Kalytchuk, Sergii; Karakassides, Michael A.; Kouloumpis, Antonios; Gournis, Dimitrios; Deligiannakis, Yannis; Giannelis, Emmanuel P.; Zboril, Radek

2017-01-01

We present the first bottom-up approach to synthesize Fe(III)-functionalized carbon dots (CDs) from molecular precursors without the need of conventional thermal or microwave treatment and additional reagents. Specifically, sonication of xylene in the presence of anhydrous FeCl3 results in oxidative coupling of the aromatic substrate towards Fe(III)-functionalized CDs. The as-prepared CDs are spherical in shape with a size of 3–8 nm, highly dispersible in organic solvents and display wavelength-dependent photoluminescence (PL). The iron ions attached to the surface endow the CDs with superior catalytic activity for olefin hydrogenation with excellent conversion and selectivity (up to 100%). The Fe(III)-CDs are more effective in the hydrogenation of a series of electron donating or withdrawing olefin substrates compared to conventional homogeneous or heterogeneous Fe(III)-based catalysts. The as-prepared heterogeneous nanocatalyst can be used repeatedly without any loss of catalytic activity. Importantly, the stability of the new catalysts can be easily monitored by PL intensity or quantum yield measurements, which certainly opens the doors for real time monitoring in a range of applications. Additionally, to the best of our knowledge, for the first time, the oxidative property of Fe-CDs was also explored in decomposition of hydrogen peroxide in water with the first order rate constant of 0.7 × 10−2 min−1, proving the versatile catalytic properties of such hybrid systems.

Co-Assembled Supported Catalysts: Synthesis of Nano-Structured Supported Catalysts with Hierarchic Pores through Combined Flow and Radiation Induced Co-Assembled Nano-Reactors

Directory of Open Access Journals (Sweden)

Galip Akay

2016-05-01

Full Text Available A novel generic method of silica supported catalyst system generation from a fluid state is presented. The technique is based on the combined flow and radiation (such as microwave, thermal or UV induced co-assembly of the support and catalyst precursors forming nano-reactors, followed by catalyst precursor decomposition. The transformation from the precursor to supported catalyst oxide state can be controlled from a few seconds to several minutes. The resulting nano-structured micro-porous silica supported catalyst system has a surface area approaching 300 m2/g and X-ray Diffraction (XRD-based catalyst size controlled in the range of 1–10 nm in which the catalyst structure appears as lamellar sheets sandwiched between the catalyst support. These catalyst characteristics are dependent primarily on the processing history as well as the catalyst (Fe, Co and Ni studied when the catalyst/support molar ratio is typically 0.1–2. In addition, Ca, Mn and Cu were used as co-catalysts with Fe and Co in the evaluation of the mechanism of catalyst generation. Based on extensive XRD, Scanning Electron Microscopy (SEM and Transmission Electron Microscopy (TEM studies, the micro- and nano-structure of the catalyst system were evaluated. It was found that the catalyst and silica support form extensive 0.6–2 nm thick lamellar sheets of 10–100 nm planar dimensions. In these lamellae, the alternate silica support and catalyst layer appear in the form of a bar-code structure. When these lamellae structures pack, they form the walls of a micro-porous catalyst system which typically has a density of 0.2 g/cm3. A tentative mechanism of catalyst nano-structure formation is provided based on the rheology and fluid mechanics of the catalyst/support precursor fluid as well as co-assembly nano-reactor formation during processing. In order to achieve these structures and characteristics, catalyst support must be in the form of silane coated silica nano

Hydrogen generation from decomposition of hydrous hydrazine over Ni-Ir/CeO2 catalyst

Directory of Open Access Journals (Sweden)

Hongbin Dai

2017-02-01

Full Text Available The synthesis of highly active and selective catalysts is the central issue in the development of hydrous hydrazine (N2H4·H2O as a viable hydrogen carrier. Herein, we report the synthesis of bimetallic Ni-Ir nanocatalyts supported on CeO2 using a one-pot coprecipitation method. A combination of XRD, HRTEM and XPS analyses indicate that the Ni-Ir/CeO2 catalyst is composed of tiny Ni-Ir alloy nanoparticles with an average size of around 4 nm and crystalline CeO2 matrix. The Ni-Ir/CeO2 catalyst exhibits high catalytic activity and excellent selectivity towards hydrogen generation from N2H4·H2O at mild temperatures. Furthermore, in contrast to previously reported Ni-Pt catalysts, the Ni-Ir/CeO2 catalyst shows an alleviated requirement on alkali promoter to achieve its optimal catalytic performance.

Efficient Method for the Determination of the Activation Energy of the Iodide-Catalyzed Decomposition of Hydrogen Peroxide

Science.gov (United States)

Sweeney, William; Lee, James; Abid, Nauman; DeMeo, Stephen

2014-01-01

An experiment is described that determines the activation energy (E[subscript a]) of the iodide-catalyzed decomposition reaction of hydrogen peroxide in a much more efficient manner than previously reported in the literature. Hydrogen peroxide, spontaneously or with a catalyst, decomposes to oxygen and water. Because the decomposition reaction is…

Thermal degradation of Shredded Oil Palm Empty Fruit Bunches (SOPEFB) embedded with Cobalt catalyst by Thermogravimetric Analysis (TGA)

Science.gov (United States)

Alias, R.; Hamid, N. H.; Jaapar, J.; Musa, M.; Alwi, H.; Halim, K. H. Ku

2018-03-01

Thermal behavior and decomposition kinetics of shredded oil palm empty fruit bunches (SOPEFB) were investigated in this study by using thermogravimetric analysis (TGA). The SOPEFB were analyzed under conditions of temperature 30 °C to 900 °C with nitrogen gas flow at 50 ml/min. The SOPEFB were embedded with cobalt (II) nitrate solution with concentration 5%, 10%, 15% and 20%. The TG/DTG curves shows the degradation behavior of SOPEFB following with char production for each heating rate and each concentration of cobalt catalyst. Thermal degradation occurred in three phases, water drying phase, decomposition of hemicellulose and cellulose phase, and lignin decomposition phase. The kinetic equation with relevant parameters described the activation energy required for thermal degradation at the temperature regions of 200 °C to 350 °C. Activation energy (E) for different heating rate with SOPEFB embedded with different concentration of cobalt catalyst showing that the lowest E required was at SOPEFB with 20% concentration of cobalt catalyst..

Contribution to the study of the oxidation reaction of the carbon oxide in contact with catalysts issued from the decomposition of nickel hydro-aluminates at various temperatures

International Nuclear Information System (INIS)

Samaane, Mikhail

1966-01-01

Addressing the study of the oxidation reaction of carbon oxide which produces carbon dioxide, this research thesis reports the study of this reaction in presence of catalysts (2NiO + Al 2 O 3 , NiAl 2 O 4 and NiO + NiAl 2 O 4 ) issued from the decomposition of nickel hydro-aluminates at different temperatures. The first part describes experimental techniques and the nature of materials used in this study. The second part reports the study of the catalytic activity of the 2NiO+Al 2 O 3 catalyst during the oxidation of CO. Preliminary studies are also reported: structure and texture of nickel hydro-aluminate which is the raw material used to produce catalysts, activation of this compound to develop the catalytic activity in CO oxidation, chemisorption of CO, O 2 and CO 2 on the 2NiO+Al 2 O 3 solid, interaction of adsorbed gases at the solid surface, and kinetic study of the oxidation reaction. The third part reports the study of the catalytic activity in the oxidation reaction of CO of spinel catalysts (NiAl 2 O 4 and NiO+NiAl 2 O 4 ) obtained by calcination of nickel hydro-aluminates at high temperature. The formation of the spinel phase, the chemisorption of CO, O 2 and CO 2 on NiAl 2 O 4 , and the kinetic of the oxidation reaction are herein studied

Utilization of a by-product produced from oxidative desulfurization process over Cs-mesoporous silica catalysts.

Science.gov (United States)

Kim, Hyeonjoo; Jeong, Kwang-Eun; Jeong, Soon-Yong; Park, Young-Kwon; Kim, Do Heui; Jeon, Jong-Ki

2011-02-01

We investigated the use of Cs-mesoporous silica catalysts to upgrade a by-product of oxidative desulfurization (ODS). Cs-mesoporous silica catalysts were characterized through N2 adsorption, XRD, CO2-temperature-programmed desorption, and XRF. Cs-mesoporous silica prepared by the direct incorporation method showed higher catalytic performance than a Cs/MCM-41 catalyst by impregnation method for the catalytic decomposition of sulfone compounds produced from ODS process.

Location of adsorbed species in NO-reduction catalysts by high resolution neutron powder diffraction

International Nuclear Information System (INIS)

Fowkes, A.J.; Rosseinsky, M.J.

1999-01-01

Complete text of publication follows. Catalysts containing copper ion exchanged into zeolites are attracting considerable attention due to their efficiency for both NO decomposition and the selective catalytic reduction of NO x in so-called lean-burn conditions in automotive exhausts. This presentation will describe the application of in-situ high resolution neutron powder diffraction to study active sites in a Cu-zeolite Y catalyst active for NO decomposition. The study under NO pressure reveals the location of two distinct copper sites for sorption. The influence of copper oxidation state on the structure of both the pristine and NO-loaded zeolites will be discussed. (author)

METHANOL OXIDATION OVER AU/ γ -AL 2O3 CATALYSTS 149

African Journals Online (AJOL)

DR. AMINU

catalysts were used to catalyze the oxidation of methanol and characterised using X-ray ... As the concentration of methoxy diminishes, so the mechanism reverts to a decomposition pathway ..... Catalysis Reviews: Science and Engineering 41.

Catalytic wet air oxidation of 2-chlorophenol over sewage sludge-derived carbon-based catalysts

Energy Technology Data Exchange (ETDEWEB)

Tu, Yuting [Institut de recherches sur la catalyse et l’environnement de Lyon (IRCELYON), CNRS – Université Claude Bernard Lyon 1, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex (France); School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Xiong, Ya; Tian, Shuanghong [School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou 510275 (China); Kong, Lingjun [School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 (China); Descorme, Claude, E-mail: claude.descorme@ircelyon.univ-lyon1.fr [Institut de recherches sur la catalyse et l’environnement de Lyon (IRCELYON), CNRS – Université Claude Bernard Lyon 1, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex (France)

2014-07-15

Highlights: • A sewage sludge derived carbon-supported iron oxide catalyst (FeSC) was prepared. • FeSC exhibited high catalytic activity in the wet air oxidation of 2-chlorophenol. • A strong correlation was observed between the 2-CP conversion, the iron leaching and the pH. • Using an acetate buffer, the iron leaching was suppressed while keeping some catalytic activity. • A simplified reaction pathway was proposed for the CWAO of 2-CP over the FeSC catalyst. - Abstract: A sewage sludge derived carbon-supported iron oxide catalyst (FeSC) was prepared and used in the Catalytic Wet Air Oxidation (CWAO) of 2-chlorophenol (2-CP). The catalysts were characterized in terms of elemental composition, surface area, pH{sub PZC}, XRD and SEM. The performances of the FeSC catalyst in the CWAO of 2-CP was assessed in a batch reactor operated at 120 °C under 0.9 MPa oxygen partial pressure. Complete decomposition of 2-CP was achieved within 5 h and 90% Total Organic Carbon (TOC) was removed after 24 h of reaction. Quite a straight correlation was observed between the 2-CP conversion, the amount of iron leached in solution and the pH of the reaction mixture at a given reaction time, indicating a strong predominance of the homogeneous catalysis contribution. The iron leaching could be efficiently prevented when the pH of the solution was maintained at values higher than 4.5, while the catalytic activity was only slightly reduced. Upon four successive batch CWAO experiments, using the same FeSC catalyst recovered by filtration after pH adjustment, only a very minor catalyst deactivation was observed. Finally, based on all the identified intermediates, a simplified reaction pathway was proposed for the CWAO of 2-CP over the FeSC catalyst.

Survey of the energy use rationalization freon decomposition technology (public use); Energy shiyo gorika freon bunkai gijutsu chosa. (kokaiyo)

Energy Technology Data Exchange (ETDEWEB)

NONE

1996-03-01

The paper made a research survey of a technology to decompose the recovered CFC (specified freon) in which energy efficiency is high and no hazardous materials such as dioxin are generated. As to the technology to decompose specified freon, the high frequency plasma method, the cement kiln method and the combustion method are at the stage of the demonstration test and close to the commercialization. The catalyst method has finished the basic test and is at the stage of a pilot plant. Besides, there are the supercritical water decomposition method, the ultraviolet decomposition method, etc., but they are at the stage of the fundamental research. Mechanisms of the dioxin generation and the suppression of dioxin generation in case of incinerating waste mixed with halide have been made clear. In the fundamental test, conditions were obtained under which the freon decomposition rate of more than 99.99% is attained by the combustion of a mixture of industrial waste and freon using the combustion method, and measures for reduction in hazardous materials such as dioxin were expected to be taken. In the catalyst method, the result obtained was the decomposition rate of more than 99.99% and the catalyst life of more than 1000 years, and its practicality was confirmed. 43 refs., 97 figs., 29 tabs.

Catalytic non-thermal plasma reactor for the decomposition of a ...

Indian Academy of Sciences (India)

2016-08-26

Aug 26, 2016 ... Among the catalytic study, MnOx/SMF (manganese oxide on sintered metal fibres electrode) shows better performance, probably due to the formation of active oxygen species by in situ decomposition of ozone on the catalyst surface. Water vapour further enhanced the performance due to the in situ ...

Solar production of catalytic filamentous carbon by thermal decomposition of hydrocarbons and carbon monoxide

Energy Technology Data Exchange (ETDEWEB)

Kirillov, V A; Kuvshinov, G G; Mogilnykh, Yu I [Boreskov Institute of Catalysis, Novosibirsk (Russian Federation); Reller, A [University of Hamburg (Germany); Steinfeld, A; Weidenkaff, A; Meier, A [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1999-08-01

Concentrated solar radiation was used as the clean source of process heat for the production of Catalytic Filamentous Carbon (CFC) by thermal decomposition of gaseous hydrocarbons and by CO disproportionation in the presence of small metal catalyst particles. Depending on the catalyst, two different types of CFC, namely nano tubes and nano fibers, were obtained in solar experiments at the PSI solar furnace. (author) 2 figs., 1 tab., 7 refs.

Catalytic Methane Decomposition over Fe-Al2O3

KAUST Repository

Zhou, Lu; Enakonda, Linga Reddy; Saih, Youssef; Loptain, Sergei; Gary, Daniel; Del-Gallo, Pascal; Basset, Jean-Marie

2016-01-01

The presence of a Fe-FeAl2O4 structure over an Fe-Al2O3 catalysts is demonstrated to be vital for the catalytic methane decomposition (CMD) activity. After H2 reduction at 750°C, Fe-Al2O3 prepared by means of a fusion method, containing 86.5wt% Fe

Stable hydrogen production from ethanol through steam reforming reaction over nickel-containing smectite-derived catalyst.

Science.gov (United States)

Yoshida, Hiroshi; Yamaoka, Ryohei; Arai, Masahiko

2014-12-25

Hydrogen production through steam reforming of ethanol was investigated with conventional supported nickel catalysts and a Ni-containing smectite-derived catalyst. The former is initially active, but significant catalyst deactivation occurs during the reaction due to carbon deposition. Side reactions of the decomposition of CO and CH4 are the main reason for the catalyst deactivation, and these reactions can relatively be suppressed by the use of the Ni-containing smectite. The Ni-containing smectite-derived catalyst contains, after H2 reduction, stable and active Ni nanocrystallites, and as a result, it shows a stable and high catalytic performance for the steam reforming of ethanol, producing H2.

Comparison of the decomposition characteristics of aromatic VOCs using an electron beam hybrid system

International Nuclear Information System (INIS)

Son, Youn-Suk; Kim, Ki-Joon; Kim, Ji-Yong; Kim, Jo-Chun

2010-01-01

We applied a hybrid technique to assess the decomposition characteristics of ethylbenzene and toluene that annexed the catalyst technique with existing electron beam (EB) technology. The removal efficiency of ethylbenzene in the EB-catalyst hybrid turned out to be 30% greater than that of EB-only treatment. We concluded that ethylbenzene was decomposed more easily than toluene by EB irradiation. We compared the independent effects of the EB-catalyst hybrid and catalyst-only methods, and observed that the efficiency of the EB-catalyst hybrid demonstrated approximately 6% improvement for decomposing toluene and 20% improvement for decomposing ethylbenzene. The G-values for ethylbenzene increased with initial concentration and reactor type: for example, the G-values by reactor type at 2800 ppmC were 7.5-10.9 (EB-only) and 12.9-25.7 (EB-catalyst hybrid). We also observed a significant decrease in by-products as well as in the removal efficiencies associated with the EB-catalyst hybrid technique.

Comparison of the decomposition characteristics of aromatic VOCs using an electron beam hybrid system

Science.gov (United States)

Son, Youn-Suk; Kim, Ki-Joon; Kim, Ji-Yong; Kim, Jo-Chun

2010-12-01

We applied a hybrid technique to assess the decomposition characteristics of ethylbenzene and toluene that annexed the catalyst technique with existing electron beam (EB) technology. The removal efficiency of ethylbenzene in the EB-catalyst hybrid turned out to be 30% greater than that of EB-only treatment. We concluded that ethylbenzene was decomposed more easily than toluene by EB irradiation. We compared the independent effects of the EB-catalyst hybrid and catalyst-only methods, and observed that the efficiency of the EB-catalyst hybrid demonstrated approximately 6% improvement for decomposing toluene and 20% improvement for decomposing ethylbenzene. The G-values for ethylbenzene increased with initial concentration and reactor type: for example, the G-values by reactor type at 2800 ppmC were 7.5-10.9 (EB-only) and 12.9-25.7 (EB-catalyst hybrid). We also observed a significant decrease in by-products as well as in the removal efficiencies associated with the EB-catalyst hybrid technique.

Decomposition mechanism of trichloroethylene based on by-product distribution in the hybrid barrier discharge plasma process

Energy Technology Data Exchange (ETDEWEB)

Han, Sang-Bo [Industry Applications Research Laboratory, Korea Electrotechnology Research Institute, Changwon, Kyeongnam (Korea, Republic of); Oda, Tetsuji [Department of Electrical Engineering, The University of Tokyo, Tokyo 113-8656 (Japan)

2007-05-15

The hybrid barrier discharge plasma process combined with ozone decomposition catalysts was studied experimentally for decomposing dilute trichloroethylene (TCE). Based on the fundamental experiment for catalytic activities on ozone decomposition, MnO{sub 2} was selected for application in the main experiments for its higher catalytic abilities than other metal oxides. A lower initial TCE concentration existed in the working gas; the larger ozone concentration was generated from the barrier discharge plasma treatment. Near complete decomposition of dichloro-acetylchloride (DCAC) into Cl{sub 2} and CO{sub x} was observed for an initial TCE concentration of less than 250 ppm. C=C {pi} bond cleavage in TCE gave a carbon single bond of DCAC through oxidation reaction during the barrier discharge plasma treatment. Those DCAC were easily broken in the subsequent catalytic reaction. While changing oxygen concentration in working gas, oxygen radicals in the plasma space strongly reacted with precursors of DCAC compared with those of trichloro-acetaldehyde. A chlorine radical chain reaction is considered as a plausible decomposition mechanism in the barrier discharge plasma treatment. The potential energy of oxygen radicals at the surface of the catalyst is considered as an important factor in causing reactive chemical reactions.

Comparison of the Effects of Fluidized-Bed and Fixed-Bed Reactors in Microwave-Assisted Catalytic Decomposition of TCE by Hydrogen

Directory of Open Access Journals (Sweden)

Lili Ren

2012-01-01

Full Text Available Trichloroethylene (TCE decomposition by hydrogen with microwave heating under different reaction systems was investigated. The activities of a series of catalysts for microwave-assisted TCE hydrodechlorination were tested through the fixed-bed and the fluidized-bed reactor systems. This study found that the different reaction system is suitable for different catalyst type. And there is an interactive relationship between the catalyst type and the reaction bed type.

Sodium Tetraphenylborate Catalyst Identification: Preliminary Studies Set 2

International Nuclear Information System (INIS)

Barnes, M.J.

1997-05-01

This document details the results of these tests and represents the second report of the task designed to identify soluble NaTPB decomposition catalysts. This task, performed as part of the DNFSB Recommendation 96-1 Implementation Plan, partially fulfills the request by High Level Waste Engineering and the ITP Flow Sheet Team in task Technical Request HLW-TTR-97008

Catalytic Ammonia Decomposition Over Ruthenium Nanoparticles Supported on Nano-Titanates

DEFF Research Database (Denmark)

Klerke, Asbjørn; Klitgaard, Søren Kegnæs; Fehrmann, Rasmus

2009-01-01

Nanosized Na2Ti3O7, K2Ti6O13 and Cs2Ti6O13 materials were prepared and used as supports of ruthenium nanoparticles for catalytic ammonia decomposition. It is shown that these catalysts exhibit higher catalytic activity than ruthenium supported on TiO2 nanoparticles promoted with cesium. The diffe...

The effect of diluting ruthenium by iron in RuxSey catalyst for oxygen reduction

International Nuclear Information System (INIS)

Delacote, Cyril; Lewera, Adam; Pisarek, Marcin; Kulesza, Pawel J.; Zelenay, Piotr; Alonso-Vante, Nicolas

2010-01-01

This study has focused on the synthesis of novel oxygen reduction reaction (ORR) chalcogenide catalysts, with Ru partially replaced by Fe in a cluster-type Ru x Se y . The catalysts were obtained by thermal decomposition of Ru 3 (CO) 12 and Fe(CO) 5 in the presence of Se. As indicated by the XPS data, the composition of catalyst nanoparticles depends on the solvent used (either p-xylene or dichlorobenzene). The presence of iron in synthesized catalysts has been confirmed by both EDAX and XPS. Voltammetric activation of the catalysts results in a partial removal of iron and unreacted selenium from the surface. The ORR performance of electrochemically pre-treated catalysts was evaluated using rotating disk and ring-disk electrodes in a sulfuric acid solution. No major change in the ORR mechanism relative to the Se/Ru catalyst has been observed with Fe-containing catalysts.

In-situ and self-distributed: A new understanding on catalyzed thermal decomposition process of ammonium perchlorate over Nd{sub 2}O{sub 3}

Energy Technology Data Exchange (ETDEWEB)

Zou, Min, E-mail: zoumin3362765@163.com; Wang, Xin, E-mail: wangx@mail.njust.edu.cn; Jiang, Xiaohong, E-mail: jxh0668@sina.com; Lu, Lude, E-mail: lulude17@yahoo.com

2014-05-01

Catalyzed thermal decomposition process of ammonium perchlorate (AP) over neodymium oxide (Nd{sub 2}O{sub 3}) was investigated. Catalytic performances of nanometer-sized Nd{sub 2}O{sub 3} and micrometer-sized Nd{sub 2}O{sub 3} were evaluated by differential scanning calorimetry (DSC). In contrast to universal concepts, catalysts in different sizes have nearly similar catalytic activities. Based on structural and morphological variation of the catalysts during the reaction, combined with mass spectrum analyses and studies of unmixed style, a new understanding of this catalytic process was proposed. We believed that the newly formed chloride neodymium oxide (NdOCl) was the real catalytic species in the overall thermal decomposition of AP over Nd{sub 2}O{sub 3}. Meanwhile, it was the “self-distributed” procedure which occurred within the reaction that also worked for the improvement of overall catalytic activities. This work is of great value in understanding the roles of micrometer-sized catalysts used in heterogeneous reactions, especially the solid–solid reactions which could generate a large quantity of gaseous species. - Graphical abstract: In-situ and self-distributed reaction process in thermal decomposition of AP catalyzed by Nd{sub 2}O{sub 3}. - Highlights: • Micro- and nano-Nd{sub 2}O{sub 3} for catalytic thermal decomposition of AP. • No essential differences on their catalytic performances. • Structural and morphological variation of catalysts digs out catalytic mechanism. • This catalytic process is “in-situ and self-distributed” one.

Synthesis and Electrocatalytic Activity of Ammonium Nickel Phosphate, [NH4]NiPO4·6H2O, and β-Nickel Pyrophosphate, β-Ni2P2O7: Catalysts for Electrocatalytic Decomposition of Urea.

Science.gov (United States)

Meguerdichian, Andrew G; Jafari, Tahereh; Shakil, Md R; Miao, Ran; Achola, Laura A; Macharia, John; Shirazi-Amin, Alireza; Suib, Steven L

2018-02-19

Electrocatalytic decomposition of urea for the production of hydrogen, H 2, for clean energy applications, such as in fuel cells, has several potential advantages such as reducing carbon emissions in the energy sector and environmental applications to remove urea from animal and human waste facilities. The study and development of new catalyst materials containing nickel metal, the active site for urea decomposition, is a critical aspect of research in inorganic and materials chemistry. We report the synthesis and application of [NH 4 ]NiPO 4 ·6H 2 O and β-Ni 2 P 2 O 7 using in situ prepared [NH 4 ] 2 HPO 4 . The [NH 4 ]NiPO 4 ·6H 2 O is calcined at varying temperatures and tested for electrocatalytic decomposition of urea. Our results indicate that [NH 4 ]NiPO 4 ·6H 2 O calcined at 300 °C with an amorphous crystal structure and, for the first time applied for urea electrocatalytic decomposition, had the greatest reported electroactive surface area (ESA) of 142 cm 2 /mg and an onset potential of 0.33 V (SCE) and was stable over a 24-h test period.

Controlled metal nitrate decomposition for the preparation of supported metal Catalysts

NARCIS (Netherlands)

Wolters, M.

2010-01-01

High surface area supported metal (oxide) catalysts are essential for the production of fuels, chemicals, pharmaceuticals and the abatement of environmental pollution. Impregnation of high surface area supports, often silica or alumina, followed by drying, calcination and reduction is one of the

Propan-1-ol Oxidation Reaction on Au/TiO2 Catalysts

African Journals Online (AJOL)

MBI

2014-11-27

Nov 27, 2014 ... a decomposition pathway, producing CO2 and H2O. However, the presence of gold ... complete oxidation reaction of propan-1-ol on the catalysts. Keywords: Gold Catalysis ... flowed at a rate of 30 mL min-1. Propan- o-l was.

Mechanistic approach for the kinetics of the decomposition of nitrous oxide over calcined hydrotalcites

Energy Technology Data Exchange (ETDEWEB)

Dandl, H.; Emig, G. [Lehrstuhl fuer Technische Chemie I, Erlangen (Germany)

1998-03-27

A highly active catalyst for the decomposition of N{sub 2}O was prepared by the thermal treatment of CoLaAl-hydrotalcite. For this catalyst the reaction rate was determined at various partial pressures of N{sub 2}O, O{sub 2} and H{sub 2}O in a temperature range from 573K to 823K. The kinetic simulation resulted in a mechanistic model. The energies of activation and rate coefficients are estimated for the main steps of the reaction

Experimental investigation of the catalytic decomposition and combustion characteristics of a non-toxic ammonium dinitramide (ADN)-based monopropellant thruster

Science.gov (United States)

Chen, Jun; Li, Guoxiu; Zhang, Tao; Wang, Meng; Yu, Yusong

2016-12-01

Low toxicity ammonium dinitramide (ADN)-based aerospace propulsion systems currently show promise with regard to applications such as controlling satellite attitude. In the present work, the decomposition and combustion processes of an ADN-based monopropellant thruster were systematically studied, using a thermally stable catalyst to promote the decomposition reaction. The performance of the ADN propulsion system was investigated using a ground test system under vacuum, and the physical properties of the ADN-based propellant were also examined. Using this system, the effects of the preheating temperature and feed pressure on the combustion characteristics and thruster performance during steady state operation were observed. The results indicate that the propellant and catalyst employed during this work, as well as the design and manufacture of the thruster, met performance requirements. Moreover, the 1 N ADN thruster generated a specific impulse of 223 s, demonstrating the efficacy of the new catalyst. The thruster operational parameters (specifically, the preheating temperature and feed pressure) were found to have a significant effect on the decomposition and combustion processes within the thruster, and the performance of the thruster was demonstrated to improve at higher feed pressures and elevated preheating temperatures. A lower temperature of 140 °C was determined to activate the catalytic decomposition and combustion processes more effectively compared with the results obtained using other conditions. The data obtained in this study should be beneficial to future systematic and in-depth investigations of the combustion mechanism and characteristics within an ADN thruster.

Zeolite ZSM5 catalysts for abatement of nitrogen oxide

Energy Technology Data Exchange (ETDEWEB)

Ganemi, Bager

1999-07-01

Airborne pollutants from the combustion of fossil fuels are a global problem. Emission of nitrogen oxides (NO{sub x}) is increasing with the worldwide increase in the use of energy. Atmospheric and photochemical reactions link nitrogen oxides to hydrocarbons and tropospheric ozone. The emission of NO{sub x} has to be tackled urgently in order to limit the harmful effects of anthropogenic activity on the environment. The subject of this thesis is catalytic nitrogen oxide abatement through direct decomposition and reduction by methane over ion-exchanged zeolite ZSM5. The work covers catalytic conversion and surface intermediates, including correlations with the level of exchanged Cu{sup 2+} cations and Ni{sup 2+} or Pd{sup 2+} co-cations. Special attention is given to the aluminium content of the support and changes in structural parameters. It was found that NO{sub x} conversion over cation-exchanged ZSM5 is strongly influenced by the ion-exchange procedure and by the above material parameters. Characterization of Cu-ZSM5 reveals that approximately two molecules of water per Cu{sup 2+} ion desorb at temperatures between 150 and 350 Deg C, in addition to the conventional dehydration at lower temperatures. The desorbed water comes from the decomposition of Cu(OH){sub 2}. Decomposition of hydroxylated copper ions results in the formation Of Cu{sup 2+}-O-Cu{sup 2+} dimers, which are suggested to be the active sites for catalytic decomposition of NO. Acid sites are important for the dispersion of copper ions on the catalyst surface. Acid sites are also important for the interaction between copper species and the zeolite. Increased acidity leads to a stronger interaction between the exchanged cation and the framework, i.e. the exchanged cations become more resistant to mobility. The stronger bond between the exchanged cations and lattice oxygen also prevents dealumination of the catalyst and decreases the thermal expansion at higher temperatures. The temperature of

Ruthenium–Platinum Catalysts and Direct Methanol Fuel Cells (DMFC: A Review of Theoretical and Experimental Breakthroughs

Directory of Open Access Journals (Sweden)

Ana S. Moura

2017-02-01

Full Text Available The increasing miniaturization of devices creates the need for adequate power sources and direct methanol fuel cells (DMFC are a strong option in the various possibilities under current development. DMFC catalysts are mostly based on platinum, for its outperformance in three key areas (activity, selectivity and stability within methanol oxidation framework. However, platinum poisoning with products of methanol oxidation led to the use of alloys. Ruthenium–platinum alloys are preferred catalysts active phases for methanol oxidation from an industrial point of view and, indeed, ruthenium itself is a viable catalyst for this reaction. In addition, the route of methanol decomposition is crucial in the goal of producing H2 from water reaction with methanol. However, the reaction pathway remains elusive and new approaches, namely in computational methods, have been ensued to determine it. This article reviews the various recent theoretical approaches for determining the pathway of methanol decomposition, and systematizes their validation with experimental data, within methodological context.

Preparation and application of granular ZnO/Al2O3 catalyst for the removal of hazardous trichloroethylene

International Nuclear Information System (INIS)

Chen, J.-C.; Tang, C.-T.

2007-01-01

Trichloroethylene (TCE) is a volatile and nerve-toxic liquid, which is widely used in many industries as an organic solvent. Without proper treatment, it will be volatilized into the atmosphere easily and hazardous to the human health and the environment. This study tries to prepare granular ZnO/Al 2 O 3 catalyst by a modified oil-drop sol-gel process incorporated the incipient wetness impregnation method and estimates its performance on the catalytic decomposition of TCE. The effects of different preparation and operation conditions are also investigated. Experimental results show that the granular ZnO/Al 2 O 3 catalyst has good catalytic performance on TCE decomposition and the conversion of TCE is 98%. ZnO/Al 2 O 3 (N) catalyst has better performance than ZnO/Al 2 O 3 (O) at high temperature. Five percent of active metal concentration and 550 deg. C calcination temperature are the better and economic preparation conditions, and the optimum operation temperature and space velocity are 450 deg. C and 18,000 h -1 , respectively. The conversions of TCE are similar and all higher than 90% as the oxygen concentration in feed gas is higher than 5%. By Fourier transform infrared spectrography (FT-IR) analyses, the major reaction products in the catalytic decomposition of TCE are HCl and CO 2 . The Brunauer-Emmett-Teller (BET) surface areas of catalysts are significantly decreased as the calcination temperature is higher than 550 deg. C due to the sintering of catalyst materials, as well as the reaction temperature is higher than 150 deg. C due to the accumulations of reaction residues on the surfaces of catalysts. These results are also demonstrated by the results of scanning electron micrography (SEM) and energy disperse spectrography (EDS)

NOx Direct Decomposition: Potentially Enhanced Thermodynamics and Kinetics on Chemically Modified Ferroelectric Surfaces

Science.gov (United States)

Kakekhani, Arvin; Ismail-Beigi, Sohrab

2014-03-01

NOx are regulated pollutants produced during automotive combustion. As part of an effort to design catalysts for NOx decomposition that operate in oxygen rich environment and permit greater fuel efficiency, we study chemistry of NOx on (001) ferroelectric surfaces. Changing the polarization at such surfaces modifies electronic properties and leads to switchable surface chemistry. Using first principles theory, our previous work has shown that addition of catalytic RuO2 monolayer on ferroelectric PbTiO3 surface makes direct decomposition of NO thermodynamically favorable for one polarization. Furthermore, the usual problem of blockage of catalytic sites by strong oxygen binding is overcome by flipping polarization that helps desorb the oxygen. We describe a thermodynamic cycle for direct NO decomposition followed by desorption of N2 and O2. We provide energy barriers and transition states for key steps of the cycle as well as describing their dependence on polarization direction. We end by pointing out how a switchable order parameter of substrate,in this case ferroelectric polarization, allows us to break away from some standard compromises for catalyst design(e.g. the Sabatier principle). This enlarges the set of potentially catalytic metals. Primary support from Toyota Motor Engineering and Manufacturing, North America, Inc.

Catalytic hydroprocessing of simulated coal tars. 2. Effect of acid catalysts on the hydroconversion of model compounds on a sulphided Ni-Mo/Al/sub 2/O/sub 3/ catalyst

Energy Technology Data Exchange (ETDEWEB)

Lemberton, J.L.; Touzeyidio, M.; Guisnet, M. (Laboratoire de Catalyse en Chimie Organique CNRS, Poitiers (France))

1989-09-15

Acid catalysts were added to sulphided Ni-Mo/Al/sub 2/O/sub 3/ catalyst in order to obtain a higher hydrocracking activity. The hydroconversion of phenanthrene, alone or in the presence of carbazole and/or 1-naphthol, was chosen as a model reaction. The presence of acid catalysts greatly increases the conversion of phenanthrene and allows significant amounts of light products to be obtained. In the presence of carbazole or of 1-naphthol, acid catalysts create a small increase in phenanthrene conversion, but light products are no longer obtained as the acid sites are poisoned either by adsorption of ammonia from carbazole decomposition, or by extensive coke deposition generated from 1-naphthol. In the presence of carbazole and 1-naphthol, there is no longer any effect of the acid catalysts on the hydroconversion of phenanthrene, owing to complete inhibition of the acid sites. 12 refs., 5 tabs.

Decomposição catalítica de óxidos de nitrogênio Catalytic decomposition of nitrogen oxides

Directory of Open Access Journals (Sweden)

Julia María Díaz Cónsul

2004-06-01

Full Text Available Contaminant gases in the atmosphere constitute an important problem to be solved in the world. The NOx gases produced as a consequence of engine high temperatures are deleterious to environment and human health, as they promote acid rain and can act in the same way as freons in the destruction of the ozone layer in the stratosphere. In this review, three way and selective reduction catalysts for decomposition of these contaminant gases are described. Details about conditions and problems, such as catalyst poisoning, and the search for new catalysts are shown.

Efficient Production of Hydrogen from Decomposition of Formic Acid over Zeolite Incorporated Gold Nanoparticles

DEFF Research Database (Denmark)

Gallas-Hulin, Agata; Mielby, Jerrik Jørgen; Kegnæs, Søren

2016-01-01

Formic acid has a great potential as a safe and convenient source of hydrogen for sustainable chemical synthesis and renewable energy storage. Here, we report a heterogeneous gold nanoparticles catalyst for efficient production of hydrogen from vapor phase decomposition of formic acid using zeolite...... incorporated gold nanoparticles. The catalyst is prepared by pressure assisted impregnation and reduction (PAIR), which results in a uniform distribution of small gold nanoparticles that are incorporated into zeolite silicalite-1 crystals. Consequently, the incorporated nanoparticles exhibit increased...... sintering stability. Based on these results, we believe that incorporation of metal nanoparticles in zeolites may find use as highly active and selective heterogeneous catalysts for the production of hydrogen in future renewable energy applications....

Sulfur deactivation of fatty ester hydrogenolysis catalysts

Energy Technology Data Exchange (ETDEWEB)

Brands, D.S.; U-A-Sai, G.; Poels, E.K.; Bliek, A. [Univ. of Amsterdam (Netherlands). Dept. of Chemical Engineering

1999-08-15

Trace organosulfur compounds present as natural impurities in oleochemical feedstocks may lead to activation of copper-containing catalysts applied for hydrogenolysis of esters toward fatty alcohols. In this paper, the sulfur deactivation of Cu/SiO{sub 2} and Cu/ZnO/SiO{sub 2} catalysts was studied in the liquid-phase hydrogenolysis of methyl palmitate. The rate of deactivation is fast and increases as a function of the sulfur-containing compound present: octadecanethiol {approx} dihexadecyl disulfide < benzyl isothiocyanate < methyl p-toluene sulfonate < dihexadecyl sulfide < dibenzothiophene. The rapid deactivation is caused by the fact that sulfur is quantitatively removed from the reaction mixture and because mainly surface sulfides are formed under hydrogenolysis conditions. The life time of a zinc-promoted catalyst is up to two times higher than that of the Cu/SiO{sub 2} catalyst, most likely due to zinc surface sulfide formation. The maximum sulfur coverage obtained after full catalyst deactivation with dibenzothiophene and dihexadecyl sulfide--the sulfur compounds that cause the fastest deactivation--may be as low as 0.07. This is due to the fact that decomposition of these compounds as well as the hydrogenolysis reaction itself proceeds on ensembles of copper atoms. Catalyst regeneration studies reveal that activity cannot be regained by reduction or combined oxidation/reduction treatments. XRD, TPR, and TPO results confirm that no distinct bulk copper or zinc sulfide or sulfate phases are present.

Design and implementation of mixing chambers to improve thermal decomposition of urea for NOX abatement

KAUST Repository

Lee, Junggil

2012-10-01

Urea-selective catalytic reduction (SCR) has been reported as the most promising technique for adherence to NOX emissions regulations. In the urea-SCR process, NH3 is generated by urea thermal decomposition and hydrolysis and is then used as a reductant of NOX in the SCR catalyst. Therefore, improving the NOX conversion efficiency of urea-SCR requires enhancement of thermal decomposition upstream of the SCR catalyst. In the present work, two types of mixing chambers were designed and fabricated to improve urea thermal decomposition, and experiments with and without a mixing chamber were carried out to analyze thermal-decomposition characteristics of urea in the exhaust pipe with respect to inlet velocity (4-12μm/s) and temperature (350°C-500°C). Urea thermal decomposition is greatly enhanced at higher gas temperatures. At an inlet velocity of 6μm/s in the A-type mixing chamber, NH3 concentrations generated along the exhaust pipe were about 171% and 157% greater than those without the mixing chamber for inlet temperatures of 400°C and 500°C, respectively. In the case of the B-type mixing chamber, NH3 concentrations generated at inlet temperatures of 400°C and 500°C were about 147% and 179% greater than those without the mixing chamber, respectively. Note that the implementation of mixing chambers significantly enhanced conversion of urea to NH3 because it increased the residence time of urea in the exhaust pipe and improved mixing between urea and exhaust gas. © 2012, Mary Ann Liebert, Inc.

Activity of ruthenium, rhodium, iridium-ruthenium and iridium-rhodium adsorbed catalysts in dehydrogenation of formic acid

Energy Technology Data Exchange (ETDEWEB)

Mikhailov, V A; Zubovich, I A [Yaroslavskij Politekhnicheskij Inst. (USSR)

1977-04-01

The activity of Ru-, Rh- (Ir+nRu)- and (Ir+nRn) catalysts on sugar carbon and silicon dioxide in decomposition of HCOOH was studied. The catalyst activity increases in the series Ircatalysts on silicon dioxide. The results obtained point to activity of single centres (Ru)/sub 1/ and (Rh)/sub 1/ in the reaction of dehydration of HCOOH. It is shown that in the course of preparation of (Ir+nRh)- and (Ir+nRu)-catalysts the Ir atoms interact with Ru(Rh), and variable-composition structures are formed.

Decomposition and reduction of N2O over Limestone under FBC Conditions

DEFF Research Database (Denmark)

Johnsson, Jan Erik; Jensen, Anker; Vaaben, Rikke

1997-01-01

The addition of limestone for sulfur retention in FBC has in many cases been observed to influence the emission of N2O. The catalytic activity of N2O over calcined Stevns Chalk for decomposition of N2O in a laboratory fixed bed quartz reactor was measured. It was found that calcined Stevns Chalk...... is a very active catalyst for N2O decomposition in an inert atmosphere, and the presence of 3 vol% CO increased the rate of N2O destruction by a factor of 5 due to the catalytic reduction of N2O by CO. The activity decreased with increasing CO2 concentration, and uncalcined or recarbonated limestone had...... negligible activity. Sulfation of the calcined limestone under oxidizing conditions lowered the activity, however sulfidation under reducing conditions showed that CaS is an active catalyst for the reduction of N2O by CO. Without CO present a gas solid reaction between N2O and CaS takes place and SO2...

Moessbauer and EXAFS studies of amorphous iron produced by thermal decomposition of carbonyl iron in liquid phase

International Nuclear Information System (INIS)

Nomura, Kiyoshi; Tanaka, Junichi; Ujihira, Yusuke; Takahashi, Tamotu; Uchida, Yasuzo

1990-01-01

Decomposition of iron carbonyl Fe(CO) 5 and Fe 2 (CO) 9 in liquid phase gave amorphous and crystalline iron powders in the absence and presence of catalyst, respectively. The hyperfine fields were large in amorphous phases prepared from Fe(CO) 5 than from Fe 2 (CO) 9 . Crystalline iron, iron carbide and a trace amount of Fe 3 O 4 were detected in the decomposition products of the amorphous phase prepared from Fe(CO) 5 , and iron carbide was mainly included in the decomposition products of the amorphous phase prepared from Fe 2 (CO) 9 . (orig.)

Steam reforming of methanol over oxide decorated nanoporous gold catalysts: a combined in situ FTIR and flow reactor study.

Science.gov (United States)

Shi, J; Mahr, C; Murshed, M M; Gesing, T M; Rosenauer, A; Bäumer, M; Wittstock, A

2017-03-29

Methanol as a green and renewable resource can be used to generate hydrogen by reforming, i.e., its catalytic oxidation with water. In combination with a fuel cell this hydrogen can be converted into electrical energy, a favorable concept, in particular for mobile applications. Its realization requires the development of novel types of structured catalysts, applicable in small scale reactor designs. Here, three different types of such catalysts were investigated for the steam reforming of methanol (SRM). Oxides such as TiO 2 and CeO 2 and mixtures thereof (Ce 1 Ti 2 O x ) were deposited inside a bulk nanoporous gold (npAu) material using wet chemical impregnation procedures. Transmission electron and scanning electron microscopy reveal oxide nanoparticles (1-2 nm in size) abundantly covering the strongly curved surface of the nanoporous gold host (ligaments and pores on the order of 40 nm in size). These catalysts were investigated in a laboratory scaled flow reactor. First conversion of methanol was detected at 200 °C. The measured turn over frequency at 300 °C of the CeO x /npAu catalyst was 0.06 s -1 . Parallel investigation by in situ infrared spectroscopy (DRIFTS) reveals that the activation of water and the formation of OH ads are the key to the activity/selectivity of the catalysts. While all catalysts generate sufficient OH ads to prevent complete dehydrogenation of methanol to CO, only the most active catalysts (e.g., CeO x /npAu) show direct reaction with formic acid and its decomposition to CO 2 and H 2 . The combination of flow reactor studies and in operando DRIFTS, thus, opens the door to further development of this type of catalyst.

Industrial wastewater advanced treatment via catalytic ozonation with an Fe-based catalyst.

Science.gov (United States)

Li, Xufang; Chen, Weiyu; Ma, Luming; Wang, Hongwu; Fan, Jinhong

2018-03-01

An Fe-based catalyst was used as a heterogeneous catalyst for the ozonation of industrial wastewater, and key operational parameters (pH and catalyst dosage) were studied. The results indicated that the Fe-based catalyst significantly improved the mineralization of organic pollutants in wastewater. TOC (total organic carbon) removal was high, at 78.7%, with a catalyst concentration of 200 g/L, but only 31.6% with ozonation alone. The Fe-based catalyst significantly promoted ozone decomposition by 70% in aqueous solution. Hydroxyl radicals (·OH) were confirmed to be existed directly via EPR (electron paramagnetic resonance) experiments, and ·OH were verified to account for about 34.4% of TOC removal with NaHCO 3 as a radical scavenger. Through characterization by SEM-EDS (field emission scanning electron microscope with energy-dispersive spectrometer), XRD (X-ray powder diffraction) and XPS (X-ray photoelectron spectroscopy), it was deduced that FeOOH on the surface of the catalyst was the dominant contributor to the catalytic efficiency. The catalyst was certified as having good stability and excellent reusability based on 50 successive operations and could be used as a filler simultaneously. Thereby, it is a promising catalyst for practical industrial wastewater advanced treatment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Advanced Oxidation: Oxalate Decomposition Testing With Ozone

International Nuclear Information System (INIS)

Ketusky, E.; Subramanian, K.

2012-01-01

At the Savannah River Site (SRS), oxalic acid is currently considered the preferred agent for chemically cleaning the large underground Liquid Radioactive Waste Tanks. It is applied only in the final stages of emptying a tank when generally less than 5,000 kg of waste solids remain, and slurrying based removal methods are no-longer effective. The use of oxalic acid is preferred because of its combined dissolution and chelating properties, as well as the fact that corrosion to the carbon steel tank walls can be controlled. Although oxalic acid is the preferred agent, there are significant potential downstream impacts. Impacts include: (1) Degraded evaporator operation; (2) Resultant oxalate precipitates taking away critically needed operating volume; and (3) Eventual creation of significant volumes of additional feed to salt processing. As an alternative to dealing with the downstream impacts, oxalate decomposition using variations of ozone based Advanced Oxidation Process (AOP) were investigated. In general AOPs use ozone or peroxide and a catalyst to create hydroxyl radicals. Hydroxyl radicals have among the highest oxidation potentials, and are commonly used to decompose organics. Although oxalate is considered among the most difficult organic to decompose, the ability of hydroxyl radicals to decompose oxalate is considered to be well demonstrated. In addition, as AOPs are considered to be 'green' their use enables any net chemical additions to the waste to be minimized. In order to test the ability to decompose the oxalate and determine the decomposition rates, a test rig was designed, where 10 vol% ozone would be educted into a spent oxalic acid decomposition loop, with the loop maintained at 70 C and recirculated at 40L/min. Each of the spent oxalic acid streams would be created from three oxalic acid strikes of an F-area simulant (i.e., Purex = high Fe/Al concentration) and H-area simulant (i.e., H area modified Purex = high Al/Fe concentration) after nearing

ADVANCED OXIDATION: OXALATE DECOMPOSITION TESTING WITH OZONE

Energy Technology Data Exchange (ETDEWEB)

Ketusky, E.; Subramanian, K.

2012-02-29

At the Savannah River Site (SRS), oxalic acid is currently considered the preferred agent for chemically cleaning the large underground Liquid Radioactive Waste Tanks. It is applied only in the final stages of emptying a tank when generally less than 5,000 kg of waste solids remain, and slurrying based removal methods are no-longer effective. The use of oxalic acid is preferred because of its combined dissolution and chelating properties, as well as the fact that corrosion to the carbon steel tank walls can be controlled. Although oxalic acid is the preferred agent, there are significant potential downstream impacts. Impacts include: (1) Degraded evaporator operation; (2) Resultant oxalate precipitates taking away critically needed operating volume; and (3) Eventual creation of significant volumes of additional feed to salt processing. As an alternative to dealing with the downstream impacts, oxalate decomposition using variations of ozone based Advanced Oxidation Process (AOP) were investigated. In general AOPs use ozone or peroxide and a catalyst to create hydroxyl radicals. Hydroxyl radicals have among the highest oxidation potentials, and are commonly used to decompose organics. Although oxalate is considered among the most difficult organic to decompose, the ability of hydroxyl radicals to decompose oxalate is considered to be well demonstrated. In addition, as AOPs are considered to be 'green' their use enables any net chemical additions to the waste to be minimized. In order to test the ability to decompose the oxalate and determine the decomposition rates, a test rig was designed, where 10 vol% ozone would be educted into a spent oxalic acid decomposition loop, with the loop maintained at 70 C and recirculated at 40L/min. Each of the spent oxalic acid streams would be created from three oxalic acid strikes of an F-area simulant (i.e., Purex = high Fe/Al concentration) and H-area simulant (i.e., H area modified Purex = high Al/Fe concentration

Characterization of Co and Fe-MCM-56 catalysts for NH3-SCR and N2O decomposition: An in situ FTIR study

Science.gov (United States)

Grzybek, Justyna; Gil, Barbara; Roth, Wieslaw J.; Skoczek, Monika; Kowalczyk, Andrzej; Chmielarz, Lucjan

2018-05-01

Two-step preparation of iron and cobalt-containing MCM-56 zeolites has been undertaken to evaluate the influence of their physicochemical properties in the selective catalytic reduction (NH3-SCR or DeNOx) of NO using NH3 as a reductant. Zeolites were prepared by the selective leaching of the framework cations by concentrated HNO3 solution and NH4F/HF mixture and consecutively, introduction of Co and Fe heteroatoms, in quantities below 1 wt%. Further calcination allowed to obtain highly dispersed active species. Their evaluation and speciation was realized by adsorption of pyridine and NO, followed by FTIR spectroscopy. Both Fe-MCM-56 zeolites showed excellent activities (maximum NO conversion 92%) with high selectivity to dinitrogen (above 99%) in the high temperature NH3-SCR process. High catalytic activity of Fe-MCM-56 zeolites was assigned to the formation of stable nitrates, delivering NO to react with NH3 at higher temperatures and suppressing the direct NO oxidation. It was found that more nitrates was formed in Fe-MCM-56 (HNO3) than in Fe-MCM-56 (HF/NH4F) and that could compensate for the lower Fe loading, resulting in very similar catalytic activity of both catalysts. At the same time both Co-and Fe-MCM-56 zeolites were moderately active in direct N2O decomposition, with maximum N2O conversion not higher than 80% and activity window starting at 500 °C. This phenomenon was expected since both types of catalysts contained well dispersed active centers, not beneficial for this reaction.

Catalytic reduction of NOx in gasoline engine exhaust over copper- and nickel-exchanged X-zeolite catalysts

International Nuclear Information System (INIS)

Bhattacharyya, S.; Das, R.K.

2001-01-01

Catalytic removal of NO x in engine exhaust gases can be accomplished by non-selective reduction, selective reduction and decomposition. Noble metals are extensively used for non-selective reduction of NO x and up to 90% of engine NO x emissions can be reduced in a stoichiometric exhaust. This requirement of having the stoichiometric fuel-air ratio acts against efficiency improvement of engines. Selective NO x reduction in the presence of different reductants such as, NH 3 , urea or hydrocarbons, requires close control of the amount of reductant being injected which otherwise may be emitted as a pollutant. Catalytic decomposition is the best option for NO x removal. Nevertheless, catalysts which are durable, economic and active for NO x reduction at normal engine exhaust temperature ranges are still being investigated. Three catalysts based on X-zeolite have been developed by exchanging the Na+ ion with copper, nickel and copper-nickel metal ions and applied to the exhaust of a stationary gasoline engine to explore their potential for catalytic reduction of NO x under a wide range of engine and exhaust conditions. Some encouraging results have been obtained. The catalyst Cu-X exhibits much better NO x reduction performance at any temperature in comparison to Cu-Ni-X and Ni-X; while Cu-Ni-X catalyst exhibits slightly better performance than Ni-X catalyst. Maximum NO x efficiency achieved with Cu-X catalyst is 59.2% at a space velocity (sv) of 31 000 h -1 ; while for Cu-Ni-X and Ni-X catalysts the equivalent numbers are 60.4% and 56% respectively at a sv of 22 000 h -1 . Unlike noble metals, the doped X-zeolite catalysts exhibit significant NO x reduction capability for a wide range of air/fuel ratio and with a slower rate of decline as well with increase in air/fuel ratio. (author)

Preparation and application of granular ZnO/Al{sub 2}O{sub 3} catalyst for the removal of hazardous trichloroethylene

Energy Technology Data Exchange (ETDEWEB)

Chen, J.-C. [Department of Environmental Engineering, Hung-Kuang University, No. 34, Chung-Chie Road, Shalu, Taichung County, Taiwan 43302 (China)]. E-mail: jcchen@sunrise.hk.edu.tw; Tang, C.-T. [Department of Environmental Engineering, Hung-Kuang University, No. 34, Chung-Chie Road, Shalu, Taichung County, Taiwan 43302 (China)

2007-04-02

Trichloroethylene (TCE) is a volatile and nerve-toxic liquid, which is widely used in many industries as an organic solvent. Without proper treatment, it will be volatilized into the atmosphere easily and hazardous to the human health and the environment. This study tries to prepare granular ZnO/Al{sub 2}O{sub 3} catalyst by a modified oil-drop sol-gel process incorporated the incipient wetness impregnation method and estimates its performance on the catalytic decomposition of TCE. The effects of different preparation and operation conditions are also investigated. Experimental results show that the granular ZnO/Al{sub 2}O{sub 3} catalyst has good catalytic performance on TCE decomposition and the conversion of TCE is 98%. ZnO/Al{sub 2}O{sub 3}(N) catalyst has better performance than ZnO/Al{sub 2}O{sub 3}(O) at high temperature. Five percent of active metal concentration and 550 deg. C calcination temperature are the better and economic preparation conditions, and the optimum operation temperature and space velocity are 450 deg. C and 18,000 h{sup -1}, respectively. The conversions of TCE are similar and all higher than 90% as the oxygen concentration in feed gas is higher than 5%. By Fourier transform infrared spectrography (FT-IR) analyses, the major reaction products in the catalytic decomposition of TCE are HCl and CO{sub 2}. The Brunauer-Emmett-Teller (BET) surface areas of catalysts are significantly decreased as the calcination temperature is higher than 550 deg. C due to the sintering of catalyst materials, as well as the reaction temperature is higher than 150 deg. C due to the accumulations of reaction residues on the surfaces of catalysts. These results are also demonstrated by the results of scanning electron micrography (SEM) and energy disperse spectrography (EDS)

Characterization, non-isothermal decomposition kinetics and photocatalytic water splitting of green chemically synthesized polyoxoanions of molybdenum containing phosphorus as hetero atom

International Nuclear Information System (INIS)

D’Cruz, Bessy; Samuel, Jadu; George, Leena

2014-01-01

Highlights: • CPM nanorods were synthesized by applying the principles of green chemistry. • The isoconversional method was used to analyze the effective activation energy. • The appropriate reaction models of the two decomposition stages were determined. • Photocatalytic water splitting was investigated in the presence of platinum co-catalyst. - Abstract: In here, the green synthesis and thermal characterization of a novel polyoxoanions of molybdenum containing phosphorus as hetero atom are reported. The composition and morphology of the nanorods were established by fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA) and inductively coupled plasma atomic emission spectroscopic (ICP-AES) techniques. Thermal properties of the nanoparticles were investigated by non-isothermal analysis under nitrogen atmosphere. The values activation energy of each stage of thermal decomposition for all heating rates was calculated by Flynn–Wall–Ozawa (FWO) and Kissinger–Akahira–Sunnose (KAS) methods. Invariant kinetic parameter (IKP) method and master plot method were also used to evaluate the kinetic parameters and mechanism for the thermal decomposition of cetylpyridinium phosphomolybdate (CPM). Photocatalytic water oxidation mechanism using CPM catalyst in the presence of platinum (Pt) co-catalyst enhances the H 2 evolution and was found to be 1.514 mmol/g/h

Characterization, non-isothermal decomposition kinetics and photocatalytic water splitting of green chemically synthesized polyoxoanions of molybdenum containing phosphorus as hetero atom

Energy Technology Data Exchange (ETDEWEB)

D’Cruz, Bessy [Department of Chemistry, Mar Ivanios College, Thiruvananthapuram 695015 (India); Samuel, Jadu, E-mail: jadu_samuel@yahoo.co.in [Department of Chemistry, Mar Ivanios College, Thiruvananthapuram 695015 (India); George, Leena [Catalysis and Inorganic Chemistry Division, National Chemical Laboratory, Pune 411008 (India)

2014-11-20

Highlights: • CPM nanorods were synthesized by applying the principles of green chemistry. • The isoconversional method was used to analyze the effective activation energy. • The appropriate reaction models of the two decomposition stages were determined. • Photocatalytic water splitting was investigated in the presence of platinum co-catalyst. - Abstract: In here, the green synthesis and thermal characterization of a novel polyoxoanions of molybdenum containing phosphorus as hetero atom are reported. The composition and morphology of the nanorods were established by fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA) and inductively coupled plasma atomic emission spectroscopic (ICP-AES) techniques. Thermal properties of the nanoparticles were investigated by non-isothermal analysis under nitrogen atmosphere. The values activation energy of each stage of thermal decomposition for all heating rates was calculated by Flynn–Wall–Ozawa (FWO) and Kissinger–Akahira–Sunnose (KAS) methods. Invariant kinetic parameter (IKP) method and master plot method were also used to evaluate the kinetic parameters and mechanism for the thermal decomposition of cetylpyridinium phosphomolybdate (CPM). Photocatalytic water oxidation mechanism using CPM catalyst in the presence of platinum (Pt) co-catalyst enhances the H{sub 2} evolution and was found to be 1.514 mmol/g/h.

Co, Fe and Ni catalysts supported on coke for direct coal liquefaction

International Nuclear Information System (INIS)

Jimenez, Jose A; Villalba, Oscar A; Rodriguez, Luis I; Hernandez, Orlando; Agamez, Yasmin Y; Dias Jose de Jesus

2008-01-01

Transition metal catalysts supported on coke were prepared by impregnation with a solution of complex of metal-thiourea, that is produced from salt precursors of cobalt chloride, Nickel chloride or iron sulfate and ammonium. sulphide formation on the support surface was generated by decomposition of the metal complex. The catalysts obtained were used in direct coal liquefaction of a medium volatile bituminous coal (Yerbabuena N 1) from Cundinamarca using a 250 Ml, Parr reactor at 723 K and a hydrogen-donor solvent. The catalytic results show, for all samples, both a good coal conversion and an enhancement of the yield of oils, this indicates that the proposed preparation method of catalyst is effective and that eventually the H 2 S sulphidation conventional process could be replaced

Ruthenium-catalysed decomposition of formic acid: Fuel cell and catalytic applications

KAUST Repository

Piola, Lorenzo

2017-08-08

The decomposition of formic acid into H2 and CO2 was successfully performed using a ruthenium hydride catalyst, without any concomitant CO evolution. The reaction mechanism is investigated by means of density functional theory calculations (DFT). The generated H2 was further exploited in a fuel cell to produce electricity. The catalytic hydrogenation of conjugated olefins, using this dihydrogen generation procedure, is also reported.

Ruthenium-catalysed decomposition of formic acid: Fuel cell and catalytic applications

KAUST Repository

Piola, Lorenzo; Ferná ndez-Salas, José A.; Nahra, Fady; Poater, Albert; Cavallo, Luigi; Nolan, Steven P.

2017-01-01

The decomposition of formic acid into H2 and CO2 was successfully performed using a ruthenium hydride catalyst, without any concomitant CO evolution. The reaction mechanism is investigated by means of density functional theory calculations (DFT). The generated H2 was further exploited in a fuel cell to produce electricity. The catalytic hydrogenation of conjugated olefins, using this dihydrogen generation procedure, is also reported.

Conversion of hot coke oven gas into light fuel gas over Ni/Al{sub 2}O{sub 3} catalyst

Energy Technology Data Exchange (ETDEWEB)

Li, L.Y.; Morishita, K.; Takarada, T. [Gunma University, Gunma (Japan). Dept. of Biology & Chemical Engineering

2006-04-15

Conversion of hot coke oven gas (COG, containing tarry material) into light fuel gas over a Ni/Al{sub 2}O{sub 3} catalyst was studied. Laboratory scale tests were carried out in a two-stage fixed-bed reactor at ambient pressure. The nickel catalyst promoted the hydropyrolysis reaction of tarry materials. High yields of total product gas and methane were obtained at high hydrogen concentrations. If the hydrogen supply was adequate for hydropyrolysis of the tarry material, conversion of coal volatiles was high, at more than 95% on carbon balance, even with a gas residence time as short as 0.15 s in the catalyst bed. The product gas yield depended on catalytic temperature. At 923 K, the maximum conversion of coal volatiles into the light gas was achieved at 95.0% on carbon balance, with methane 86.7 vol% of the carbonaceous gas product. Although carbon deposits deactivated the catalyst after a long period of use, the catalyst could be regenerated by treatment with oxygen at 800 K, providing high activity in subsequent decomposition of tarry material. The influence of sulphide on the tarry material decomposition reaction was small even in a 2000 ppm H{sub 2}S atmosphere.

Passivation of bimetallic catalysts used in water treatment: prevention and reactivation.

Science.gov (United States)

Chen, Jianming; Gillham, Robert W; Gui, Lai

2013-01-01

With respect to degradation rates and the range in contaminants treated, bimetals such as Ni-Fe or Pd-Fe generally outperform unamended granular iron. However, the catalytic enhancement is generally short-lived, lasting from a few days to months. To take advantage of the significant benefits of bimetals, this study aims at developing an effective method for the rejuvenation of passivated bimetals and alternatively, the prevention of rapid reactivity loss of bimetals. Because the most likely cause of Ni-Fe and Pd-Fe passivation is the deposition of iron oxide films over the catalyst sites, it is hypothesized that removal of the iron oxide films will restore the lost reactivity or avoiding the deposition of iron oxide films will prevent passivation. Two organic ligands (ethylenediaminetetraacetic acid (EDTA), and [s,s]-ethylenediaminedisuccinate acid ([s,s]-EDDS)) and two acids (citric acid and sulphuric acid) were tested as possible chemical reagents for both passivation rejuvenation and prevention. Trichloroethene (TCE) and Ni-Fe were chosen as probes for chlorinated solvents and bimetals respectively. The test was carried out using small glass columns packed with Ni-Fe. TCE solution containing a single reagent at various concentrations was pumped through the Ni-Fe columns with a residence time in the Ni-Fe of about 6.6 min. TCE concentrations in the influent and effluent were measured to evaluate the performance of each chemical reagent. The results show that (i) for passivated Ni-Fe, flushing with a low concentration of acid or ligand solution without mechanical mixing can fully restore the lost reactivity; and (ii) for passivation prevention, adding a small amount of a ligand or an acid to the feed solution can successfully prevent or at least substantially reduce Ni-Fe passivation. All four chemicals tested are effective in both rejuvenation and prevention, but sulphuric acid and citric acid are considered to be the most practical reagents due to their

Treatment of off-gas evolved from thermal decomposition of sludge waste

International Nuclear Information System (INIS)

Doo-Seong Hwang; Yun-Dong Choi; Gyeong-Hwan Jeong; Jei-Kwon Moon

2013-01-01

Korea Atomic Energy Research Institute (KAERI) started a decommissioning program of a uranium conversion plant. The treatment of the sludge waste, which was generated during the operation of the plant, is one of the most important tasks in the decommissioning program of the plant. The major compounds of sludge waste are nitrate salts and uranium. The sludge waste is denitrated by thermal decomposition. The treatment of off-gas evolved from the thermal decomposition of nitrate salts in the sludge waste is investigated. The nitrate salts in the sludge were decomposed in two steps: the first decomposition is due to the ammonium nitrate, and the second is due to the sodium and calcium nitrate and calcium carbonate. The components of off-gas from the decomposition of ammonium nitrate at low temperature are NH 3 , N 2 O, NO 2 , and NO. In addition, the components from the decomposition of sodium and calcium nitrate at high temperature are NO 2 and NO. Off-gas from the thermal decomposition is treated by the catalytic oxidation of ammonia and selective catalytic reduction (SCR). Ammonia is converted into nitrogen oxides through the oxidation catalyst and all nitrogen oxides are removed by SCR treatment besides nitrous oxide, which is greenhouse gas. An additional process is needed to remove nitrous oxide, and the feeding rate of ammonia in SCR should be controlled properly for evolved nitrogen oxides. (author)

Local structure of Pb2 ion catalysts anchored within zeolite cavities and their photo-catalytic reactivity for the elimination of N2O

International Nuclear Information System (INIS)

Ju, Woo-Sung; Matsuoka, Masaya; Yamashita, Hiromi; Anpo, Masakazu

2001-01-01

The Pb 2+ /ZSM-5 catalyst was prepared by an ion-exchange method and its photo-catalytic activity for the decomposition of N 2 O under UV irradiation was investigated. In-situ UV-Vis absorption spectroscopy and XAFS (XANES and FT-EXAFS) investigations revealed that the Pb 2+ ions exist in a highly dispersed state within the pores of the zeolites. UV irradiation of the catalysts in the presence of N 2 O led to the photo-catalytic decomposition of N 2 O into N 2 at temperatures as low as 298κ. The effective wavelength of the irradiated UV light indicated that the excited state of the Pb 2+ ions included within the zeolite cavities plays a significant role in the photo-catalytic decomposition of N 2 O molecules. (au)

The effect of diluting ruthenium by iron in Ru{sub x}Se{sub y} catalyst for oxygen reduction

Energy Technology Data Exchange (ETDEWEB)

Delacote, Cyril [Laboratory of Electrocatalysis, CNRS, University of Poitiers, F-86022 Poitiers Cedex (France); CEISAM, CNRS, University of Nantes, F-44322 Nantes Cedex 3 (France); Lewera, Adam [University of Warsaw, Department of Chemistry, ul. Pasteura 1, 02-093 Warsaw (Poland); Pisarek, Marcin [Institute of Physical Chemistry, Polish Academy of Sciences, ul. Kasprzaka 44/52, 01-224 Warsaw (Poland); Kulesza, Pawel J. [University of Warsaw, Department of Chemistry, ul. Pasteura 1, 02-093 Warsaw (Poland); Zelenay, Piotr [Materials Physics and Applications, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Alonso-Vante, Nicolas, E-mail: nicolas.alonso.vante@univ-poitiers.f [Laboratory of Electrocatalysis, CNRS, University of Poitiers, F-86022 Poitiers Cedex (France)

2010-11-01

This study has focused on the synthesis of novel oxygen reduction reaction (ORR) chalcogenide catalysts, with Ru partially replaced by Fe in a cluster-type Ru{sub x}Se{sub y}. The catalysts were obtained by thermal decomposition of Ru{sub 3}(CO){sub 12} and Fe(CO){sub 5} in the presence of Se. As indicated by the XPS data, the composition of catalyst nanoparticles depends on the solvent used (either p-xylene or dichlorobenzene). The presence of iron in synthesized catalysts has been confirmed by both EDAX and XPS. Voltammetric activation of the catalysts results in a partial removal of iron and unreacted selenium from the surface. The ORR performance of electrochemically pre-treated catalysts was evaluated using rotating disk and ring-disk electrodes in a sulfuric acid solution. No major change in the ORR mechanism relative to the Se/Ru catalyst has been observed with Fe-containing catalysts.

Low-temperature conversion of ammonia to nitrogen in water with ozone over composite metal oxide catalyst.

Science.gov (United States)

Chen, Yunnen; Wu, Ye; Liu, Chen; Guo, Lin; Nie, Jinxia; Chen, Yu; Qiu, Tingsheng

2018-04-01

As one of the most important water pollutants, ammonia nitrogen emissions have increased year by year, which has attracted people's attention. Catalytic ozonation technology, which involves production of ·OH radical with strong oxidation ability, is widely used in the treatment of organic-containing wastewater. In this work, MgO-Co 3 O 4 composite metal oxide catalysts prepared with different fabrication conditions have been systematically evaluated and compared in the catalytic ozonation of ammonia (50mg/L) in water. In terms of high catalytic activity in ammonia decomposition and high selectivity for gaseous nitrogen, the catalyst with MgO-Co 3 O 4 molar ratio 8:2, calcined at 500°C for 3hr, was the best one among the catalysts we tested, with an ammonia nitrogen removal rate of 85.2% and gaseous nitrogen selectivity of 44.8%. In addition, the reaction mechanism of ozonation oxidative decomposition of ammonia nitrogen in water with the metal oxide catalysts was discussed. Moreover, the effect of coexisting anions on the degradation of ammonia was studied, finding that SO 4 2- and HCO 3 - could inhibit the catalytic activity while CO 3 2- and Br - could promote it. The presence of coexisting cations had very little effect on the catalytic ozonation of ammonia nitrogen. After five successive reuses, the catalyst remained stable in the catalytic ozonation of ammonia. Copyright © 2017. Published by Elsevier B.V.

Preparation and photocatalytic activity of B, Y co-doped nanosized TiO_2 catalyst

Institute of Scientific and Technical Information of China (English)

石中亮; 刘富梅; 姚淑华

2010-01-01

The catalysts of un-doped, single-doped and co-doped titanium dioxide (TiO2) powders were prepared by sol-gel method with Ti(OC4H9)4 as a raw material. The photocatalytic decomposition of phenol in aqueous solution under UV light was used as a probe reaction to evaluate their photocatalytic activities. The effects of B, Y co-doping on the crystallite sizes, crystal pattern, surface composition, and optical property of the catalyst were investigated by thermogravimetric differential thermal analysis, X-ray d...

An optimization study of PtSn/C catalysts applied to direct ethanol fuel cell: Effect of the preparation method on the electrocatalytic activity of the catalysts

Science.gov (United States)

Almeida, T. S.; Palma, L. M.; Leonello, P. H.; Morais, C.; Kokoh, K. B.; De Andrade, A. R.

2012-10-01

The aim of this work was to perform a systematic study of the parameters that can influence the composition, morphology, and catalytic activity of PtSn/C nanoparticles and compare two different methods of nanocatalyst preparation, namely microwave-assisted heating (MW) and thermal decomposition of polymeric precursors (DPP). An investigation of the effects of the reducing and stabilizing agents on the catalytic activity and morphology of Pt75Sn25/C catalysts prepared by microwave-assisted heating was undertaken for optimization purposes. The effect of short-chain alcohols such as ethanol, ethylene glycol, and propylene glycol as reducing agents was evaluated, and the use of sodium acetate and citric acid as stabilizing agents for the MW procedure was examined. Catalysts obtained from propylene glycol displayed higher catalytic activity compared with catalysts prepared in ethylene glycol. Introduction of sodium acetate enhanced the catalytic activity, but this beneficial effect was observed until a critical acetate concentration was reached. Optimization of the MW synthesis allowed for the preparation of highly dispersed catalysts with average sizes lying between 2.0 and 5.0 nm. Comparison of the best catalyst prepared by MW with a catalyst of similar composition prepared by the polymeric precursors method showed that the catalytic activity of the material can be improved when a proper condition for catalyst preparation is achieved.

Active sites in Fe/ZSM-5 for nitrous oxide decomposition and benzene hydroxylation with nitrous oxide

NARCIS (Netherlands)

Sun, K.; Xia, H.; Feng, Z.; Santen, van R.A.; Hensen, E.J.M.; Li, Can

2008-01-01

The effect of the iron content and the pretreatment conditions of Fe/ZSM-5 catalysts on the Fe speciation and the catalytic activities in nitrous oxide decomposition and benzene hydroxylation with nitrous oxide has been investigated. Iron-containing ZSM-5 zeolites with varying iron content (Fe/Al =

Vibration measurements of automobile catalyst

Science.gov (United States)

Aatola, Seppo

1994-09-01

Vibration of catalyst cell, which is inside the casing of the catalyst, is difficult to measure with usual measuring instrumentation. When catalyst is in use, there is hot exhaust gas flow though the catalyst cell and temperature of the cell is approximately +900 degree(s)C. Therefore non-contact Laser- Doppler-Vibrometer was used to measure vibration velocity of the catalyst cell. The laser beam was directed towards the cell through pipe which was put through and welded to the casing of the catalyst. The outer end of the pipe was screw down with a tempered class to prevent exhaust gas flow from the pipe. The inner end of the pipe was open and few millimeters away from the measuring point. Catalyst was attached to the engine with two ways, rigidly close to the engine and flexible under the engine. The engine was running in test bench under controlled conditions. Vibration measurements were carried out during constant running speeds of the engine. Vibration signals were captured and analyzed with FFT-analyzer. Vibration of catalyst cell was strongest at running speed of 5000 rpm, from 10 to 20 g (1 g equals 9.81 ms-2), when catalyst was attached rigidly close to the engine. At running speed of 3000 rpm, vibration of catalyst cell was from 2 to 3 g in most cases, when catalyst was attached either rigidly or flexible to the engine. It is estimated that in real life, i.e. when catalyst is attached to car with same engine, vibration of catalyst cell at running speed of 5000 rpm is somewhere between 1 and 10 g. At running speed of 3000 rpm, which may be more often used when driving car (car speed approximately 100 kmh-1), vibration of catalyst cell is probably few g's.

Preparation of Fischer-Tropsch catalysts from cobalt/iron hydrotalcites

Energy Technology Data Exchange (ETDEWEB)

Howard, B.H.; Boff, J.J.; Zarochak, M.F. [Pittsburgh Energy Technology Center, PA (United States)] [and others

1995-12-31

Compounds with the (hydrotalcites) have properties that make them attractive as precursors for Fischer-Tropsch catalysts. A series of single-phase hydrotalcites with cobalt/iron atom ratios ranging from 75/25 to 25/75 has been synthesized. Mixed cobalt/iron oxides have been prepared from these hydrotalcites by controlled thermal decomposition. Thermal decomposition at temperatures below 600 {degrees}C typically produced a single-phase mixed metal oxide with a spinel structure. The BET surface areas of the spinal samples have been found to be as high as about 150 m{sup 2}/g. Appropriate reducing pretreatments have been developed for several of these spinels and their activity, selectivity, and activity and selectivity maintenance have been examined at 13 MPa in a fixed-bed microreactor.

Nanostructured Co3O4 grown on nickel foam: An efficient and readily recyclable 3D catalyst for heterogeneous peroxymonosulfate activation.

Science.gov (United States)

Yuan, Ruixia; Hu, Lin; Yu, Peng; Wang, Huaiyuan; Wang, Zhaohui; Fang, Jingyun

2018-05-01

Cobalt-based heterogeneous catalyst has been recognized as one of most efficient activators for peroxymonosulfate (PMS) decomposition, but usually suffers from the poor stability and difficulty to recover and reuse. Here easily recyclable cobalt oxide (Co 3 O 4 ) nanowires and nanoflowers grown on nickel foam (NF) are fabricated by a hydrothermal and calcination method. The prepared 3D Co 3 O 4 /NF catalyst is characterized and applied as a heterogeneous catalyst for PMS activation to generate sulfate radicals for decomposition of Acid Orange 7 (AO7). The results show that the AO7 degradation rate increases with cobalt loading and PMS dosage, but decreases with the increase of solution pH. The Co 3 O 4 /NF catalyst using 2 mM Co(NO 3 ) 2 ·6H 2 O as cobalt source exhibits highest activity, and almost complete decolorization could be achieved within 30 min. The diverse effects of coexisting anions (SO 4 2- , HCO 3 - , NO 3 - and Cl - ) on AO7 degradation are observed and explained. After 10 consecutive runs, excellent catalytic reactivity of the catalyst remains while the level of leached cobalt during the catalyst usage is much lower than the maximum allowable concentration in drinking and natural water. More importantly, the macroscopic Co 3 O 4 /NF catalyst shows advantage of easy recycling after application compared to traditional catalysts. It is believed that the as-prepared Co 3 O 4 /NF is promising to be an effective and green heterogeneous catalyst for PMS activation to degrade organic pollutants for environmental application. Copyright © 2018 Elsevier Ltd. All rights reserved.

Nanosized spinel oxide catalysts for CO-oxidation prepared via CoMnMgAl quaternary hydrotalcite route

Energy Technology Data Exchange (ETDEWEB)

Mokhtar, M., E-mail: mmoustafa@kau.edu.s [Chemistry Department, Faculty of Science, King Abdulaziz University, 21589 Jeddah, P.O. Box 80203 (Saudi Arabia); Basahel, S.N.; Al-Angary, Y.O. [Chemistry Department, Faculty of Science, King Abdulaziz University, 21589 Jeddah, P.O. Box 80203 (Saudi Arabia)

2010-03-18

Catalytic activity of the Co-Mn-Mg-Al mixed oxide spinel catalysts was examined in CO oxidation by O{sub 2}. The prepared catalysts were characterized by chemical analysis (ICP), infrared spectroscopy (FTIR), thermal analysis (TG, DTG), powder X-ray diffraction (XRD), surface area measurements, and scanning electron microscopy (SEM).The calcined hydrotalcite-like precursor was composed of spinel-like Co-Mn-Mg-Al mixed oxide as the only XRD crystalline phases. The nanosized spinel oxide catalysts produced by calcination of hydrotalcites showed higher S{sub BET} than CoMn-hydrotalcite samples as calcination led to dehydroxylation and carbonate decomposition of anions in interlayer spaces. All the catalysts showed 100% CO conversion at high temperature even those calcined at 800 {sup o}C. A catalyst with Co/Mn = 4 and calcined at 500 {sup o}C showed 100% CO conversion at 160 {sup o}C. Moreover, this catalyst exhibited quite good durability without deactivation in 60 h stability test.

Adsorption and Deactivation Characteristics of Cu/ZnO-Based Catalysts for Methanol Synthesis from Carbon Dioxide

Energy Technology Data Exchange (ETDEWEB)

Natesakhawat, Sittichai; Ohodnicki, Paul R; Howard, Bret H; Lekse, Jonathan W; Baltrus, John P; Matranga, Christopher

2013-07-09

The adsorption and deactivation characteristics of coprecipitated Cu/ZnO-based catalysts were examined and correlated to their performance in methanol synthesis from CO₂ hydrogenation. The addition of Ga₂O₃ and Y₂O₃ promoters is shown to increase the Cu surface area and CO₂/H₂ adsorption capacities of the catalysts and enhance methanol synthesis activity. Infrared studies showed that CO₂ adsorbs spontaneously on these catalysts at room temperature as both monoand bi-dentate carbonate species. These weakly bound species desorb completely from the catalyst surface by 200 °C while other carbonate species persist up to 500 °C. Characterization using N₂O decomposition, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM) with energy-dispersive X-ray spectroscopy (EDX) analysis clearly indicated that Cu sintering is the main cause of catalyst deactivation. Ga and Y promotion improves the catalyst stability by suppressing the agglomeration of Cu and ZnO particles under pretreatment and reaction conditions.

The removal of VOC from air using EB, MW and catalyst - Laboratory plant results

International Nuclear Information System (INIS)

Calinescu, I.; Ighigeanu, D.; Martin, D.

2011-01-01

A new hybrid technique for the VOCs removal from gases, based on the combined use of EB induced NTP (non-thermal plasma), MW induced NTP and catalytic oxidation, named “EB+MW-plasma catalysis”, is presented. The main goal of our research was to combine the features of each known technique used in gas pollution control, i.e. the very high efficiency of EB in converting VOCs to intermediate products, the ability of MW to produce and sustain NTP in large electrodeless reactors, and the important role of catalysts in the complete conversion to CO 2 and H 2 O. Our experiences shown that the two means of treating the gases are complementary: the catalytic oxidation in the presence of MW is efficient for high VOC initial concentrations and low flow rates while the exclusive use of the EB irradiation determines high decomposition efficiencies only in the case of very low concentrations of VOC but for large flow rates. Real synergistic effects between NTP and catalysis were obtained by introducing the catalyst into the irradiation zone. The main conclusion of this work is that the combined treatment EB+MW+catalyst improves both decomposition efficiency and oxidation efficiency. The EB+MW+Catalysis method demonstrated good results on a wide range of concentrations and flow rates. (author)

Selective Transformation of Various Nitrogen-Containing Exhaust Gases toward N2 over Zeolite Catalysts.

Science.gov (United States)

Zhang, Runduo; Liu, Ning; Lei, Zhigang; Chen, Biaohua

2016-03-23

In this review we focus on the catalytic removal of a series of N-containing exhaust gases with various valences, including nitriles (HCN, CH3CN, and C2H3CN), ammonia (NH3), nitrous oxide (N2O), and nitric oxides (NO(x)), which can cause some serious environmental problems, such as acid rain, haze weather, global warming, and even death. The zeolite catalysts with high internal surface areas, uniform pore systems, considerable ion-exchange capabilities, and satisfactory thermal stabilities are herein addressed for the corresponding depollution processes. The sources and toxicities of these pollutants are introduced. The important physicochemical properties of zeolite catalysts, including shape selectivity, surface area, acidity, and redox ability, are described in detail. The catalytic combustion of nitriles and ammonia, the direct catalytic decomposition of N2O, and the selective catalytic reduction and direct catalytic decomposition of NO are systematically discussed, involving the catalytic behaviors as well as mechanism studies based on spectroscopic and kinetic approaches and molecular simulations. Finally, concluding remarks and perspectives are given. In the present work, emphasis is placed on the structure-performance relationship with an aim to design an ideal zeolite-based catalyst for the effective elimination of harmful N-containing compounds.

Current status and prospect on photo-catalyst application in environmental problems; Kankyo mondai ni okeru hikari shokubai oyo no ganjo to tenbo

Energy Technology Data Exchange (ETDEWEB)

Watanabe, T. [Toto Ltd., Kitakyushu (Japan)

1995-09-30

This paper summarizes application of photo-catalysts in environmental problems. The paper lists examples of the application in residential environments. Photo-catalytic decomposition is possible by using ultraviolet rays contained in room illumination if the bacterial presence is sparse. The examples thereof may be cited as follows: if colon bacilli are suspended on a tile with TiO2 photo-catalyst sintered in it and exposed to room illumination, the bacteria are disinfected; using photo-catalysts in a bathroom suppresses deposition of Pseudomonas aeruginosa; a photo-catalyst tile (TiO2 loaded with Cu) and light irradiation reduce intensity of tobacco smoke odor; and adsorbents may be used simultaneously if intermediate products are odor generating substances. The examples of applying photo-catalysts to regional environments may be quoted as follows: growth of algae in a Petri dish is suppressed by presence of Cu loaded TiO2 under room illumination; this leads to an expectation on its effect in a relatively clean water environment; glass beads loaded with a TiO2 photo-catalyst placed in a gold fish breeding tank reduces turbidity, the number of colon bacilluses, and COD value; and the mortality in gold fish shows no change. With an objective of application to exterior building materials, photo-catalyst applied tiles were left outdoors for 160 days. Nitric acid ions were detected that are thought to have been generated by decomposition of microorganisms that have deposited on the tiles. 6 refs., 5 figs., 3 tabs.

Structural/surface characterization and catalytic evaluation of rare-earth (Y, Sm and La) doped ceria composite oxides for CH{sub 3}SH catalytic decomposition

Energy Technology Data Exchange (ETDEWEB)

He, Dedong; Chen, Dingkai; Hao, Husheng; Yu, Jie; Liu, Jiangping; Lu, Jichang; Liu, Feng [Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500 (China); Wan, Gengping [Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500 (China); Research Center for Analysis and Measurement, Hainan University, Haikou, 570228 (China); He, Sufang [Research Center for Analysis and Measurement, Kunming University of Science and Technology, Kunming, 650093 (China); Luo, Yongming, E-mail: environcatalysis222@yahoo.com [Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500 (China)

2016-12-30

Highlights: • Ce{sub 0.75}RE{sub 0.25}O{sub 2-δ} (RE = Y, Sm and La) were synthesized by citrate complexation method. • Ce{sub 0.75}Y{sub 0.25}O{sub 2-δ} exhibited the best stability for the decomposition of CH{sub 3}SH. • Cation radius played a key role in determining structure and surface characteristics. • Catalytic behavior depended on synergistic role of oxygen vacancies and basic sites. • Ce{sub 2}S{sub 3} accumulation on the surface was responsible for the deactivation of catalyst. - Abstract: A series of rare earth (Y, Sm and La) doped ceria composite oxides and pure CeO{sub 2} were synthesized and evaluated by conducting CH{sub 3}SH catalytic decomposition test. Several characterization studies, including XRD, BET, Raman, H{sub 2}-TPR, XPS, FT-IR, CO{sub 2}-TPD and CH{sub 3}SH-TPD, were undertaken to correlate structural and surface properties of the obtained ceria-based catalysts with their catalytic performance for CH{sub 3}SH decomposition. More oxygen vacancies and increased basic sites exhibited in the rare earth doped ceria catalysts. Y doped ceria sample (Ce{sub 0.75}Y{sub 0.25}O{sub 2-δ}), with a moderate increase in basic sites, contained more oxygen vacancies. More structural defects and active sites could be provided, and a relatively small amount of sulfur would accumulate, which resulted in better catalytic performance. The developed catalyst presented good catalytic behavior with stability very similar to that of typical zeolite-based catalysts reported previously. However, La doped ceria catalyst (Ce{sub 0.75}La{sub 0.25}O{sub 2-δ}) with the highest alkalinity was not the most active one. More sulfur species would be adsorbed and a large amount of cerium sulfide species (Ce{sub 2}S{sub 3}) would accumulate, which caused deactivation of the catalysts. The combined effect of increased oxygen vacancies and alkalinity led to the catalytic stability of Ce{sub 0.75}Sm{sub 0.25}O{sub 2-δ} sample was comparable to that of pure Ce

Decomposition of toluene in a steady-state atmospheric-pressure glow discharge

International Nuclear Information System (INIS)

Trushkin, A. N.; Grushin, M. E.; Kochetov, I. V.; Trushkin, N. I.; Akishev, Yu. S.

2013-01-01

Results are presented from experimental studies of decomposition of toluene (C 6 H 5 CH 3 ) in a polluted air flow by means of a steady-state atmospheric pressure glow discharge at different water vapor contents in the working gas. The experimental results on the degree of C 6 H 5 CH 3 removal are compared with the results of computer simulations conducted in the framework of the developed kinetic model of plasma chemical decomposition of toluene in the N 2 : O 2 : H 2 O gas mixture. A substantial influence of the gas flow humidity on toluene decomposition in the atmospheric pressure glow discharge is demonstrated. The main mechanisms of the influence of humidity on C 6 H 5 CH 3 decomposition are determined. The existence of two stages in the process of toluene removal, which differ in their duration and the intensity of plasma chemical decomposition of C 6 H 5 CH 3 is established. Based on the results of computer simulations, the composition of the products of plasma chemical reactions at the output of the reactor is analyzed as a function of the specific energy deposition and gas flow humidity. The existence of a catalytic cycle in which hydroxyl radical OH acts a catalyst and which substantially accelerates the recombination of oxygen atoms and suppression of ozone generation when the plasma-forming gas contains water vapor is established.

Decomposition of toluene in a steady-state atmospheric-pressure glow discharge

Science.gov (United States)

Trushkin, A. N.; Grushin, M. E.; Kochetov, I. V.; Trushkin, N. I.; Akishev, Yu. S.

2013-02-01

Results are presented from experimental studies of decomposition of toluene (C6H5CH3) in a polluted air flow by means of a steady-state atmospheric pressure glow discharge at different water vapor contents in the working gas. The experimental results on the degree of C6H5CH3 removal are compared with the results of computer simulations conducted in the framework of the developed kinetic model of plasma chemical decomposition of toluene in the N2: O2: H2O gas mixture. A substantial influence of the gas flow humidity on toluene decomposition in the atmospheric pressure glow discharge is demonstrated. The main mechanisms of the influence of humidity on C6H5CH3 decomposition are determined. The existence of two stages in the process of toluene removal, which differ in their duration and the intensity of plasma chemical decomposition of C6H5CH3 is established. Based on the results of computer simulations, the composition of the products of plasma chemical reactions at the output of the reactor is analyzed as a function of the specific energy deposition and gas flow humidity. The existence of a catalytic cycle in which hydroxyl radical OH acts a catalyst and which substantially accelerates the recombination of oxygen atoms and suppression of ozone generation when the plasma-forming gas contains water vapor is established.

Exploring electronic and steric effects on the insertion and polymerization reactivity of phosphinesulfonato pdii catalysts

KAUST Repository

Neuwald, Boris

2013-11-21

Thirteen different symmetric and asymmetric phosphinesulfonato palladium complexes ([{(X1-Cl)-μ-M}n], M=Na, Li, 1= X(P^O)PdMe) were prepared (see Figure 1). The solid-state structures of the corresponding pyridine or lutidine complexes were determined for (MeO)21-py, (iPrO)21-lut, (MeO,Me2)1-lut, (MeO)31-lut, CF31-lut, and Ph1-lut. The reactivities of the catalysts X1, obtained after chloride abstraction with AgBF4, toward methyl acrylate (MA) were quantified through determination of the rate constants for the first and the consecutive MA insertion and the analysis of β-H and other decomposition products through NMR spectroscopy. Differences in the homo- and copolymerization of ethylene and MA regarding catalyst activity and stability over time, polymer molecular weight, and polar co-monomer incorporation were investigated. DFT calculations were performed on the main insertion steps for both monomers to rationalize the effect of the ligand substitution patterns on the polymerization behaviors of the complexes. Full analysis of the data revealed that: 1) electron-deficient catalysts polymerize with higher activity, but fast deactivation is also observed; 2) the double ortho-substituted catalysts (MeO)21 and (MeO)31 allow very high degrees of MA incorporation at low MA concentrations in the copolymerization; and 3) steric shielding leads to a pronounced increase in polymer molecular weight in the copolymerization. The catalyst properties induced by a given P-aryl (alkyl) moiety were combined effectively in catalysts with two different non-chelating aryl moieties, such as cHexO/(MeO)21, which led to copolymers with significantly increased molecular weights compared to the prototypical MeO1. Catalyst control: The influence of steric and electronic effects on the reactivity of phosphinesulfonato PdII catalysts in polymerization and copolymerization is explored through experimental and DFT methods. A comparison of thirteen different X(P O)PdMe catalysts ((P O)= κ2-P

Reduction of nanowire diameter beyond lithography limits by controlled catalyst dewetting

Science.gov (United States)

Calahorra, Yonatan; Kerlich, Alexander; Amram, Dor; Gavrilov, Arkady; Cohen, Shimon; Ritter, Dan

2016-04-01

Catalyst assisted vapour-liquid-solid is the most common method to realize bottom-up nanowire growth; establishing a parallel process for obtaining nanoscale catalysts at pre-defined locations is paramount for further advancement towards commercial nanowire applications. Herein, the effect of a selective area mask on the dewetting of metallic nanowire catalysts, deposited within lithography-defined mask pinholes, is reported. It was found that thin disc-like catalysts, with diameters of 120-450 nm, were transformed through dewetting into hemisphere-like catalysts, having diameters 2-3 fold smaller; the process was optimized to about 95% yield in preventing catalyst splitting, as would otherwise be expected due to their thickness-to-diameter ratio, which was as low as 1/60. The catalysts subsequently facilitated InP and InAs nanowire growth. We suggest that the mask edges prevent surface migration mediated spreading of the dewetted metal, and therefore induce its agglomeration into a single particle. This result presents a general strategy to diminish lithography-set dimensions for NW growth, and may answer a fundamental challenge faced by bottom-up nanowire technology.

Influence of Gold on Ce-Zr-Co Fluorite-Type Mixed Oxide Catalysts for Ethanol Steam Reforming

Directory of Open Access Journals (Sweden)

Véronique Pitchon

2012-02-01

Full Text Available The effect of gold presence on carbon monoxide oxidation and ethanol steam reforming catalytic behavior of two Ce-Zr-Co mixed oxides catalysts with a constant Co charge and different Ce/Zr ratios was investigated. The Ce-Zr-Co mixed oxides were obtained by the pseudo sol-gel like method, based on metallic propionates polymerization and thermal decomposition, whereas the gold-supported Ce-Zr-Co mixed oxides catalysts were prepared using the direct anionic exchange. The catalysts were characterized using XRD, TPR, and EDXS-TEM. The presence of Au in doped Ce-Zr-Co oxide catalyst decreases the temperature necessary to reduce the cobalt and the cerium loaded in the catalyst and favors a different reaction pathway, improving the acetaldehyde route by ethanol dehydrogenation, instead of the ethylene route by ethanol dehydration or methane re-adsorption, thus increasing the catalytic activity and selectivity into hydrogen.

Development of Coke-tolerant Transition Metal Catalysts for Dry Reforming of Methane

KAUST Repository

Al-Sabban, Bedour E.

2016-11-07

Dry reforming of methane (DRM) is an attractive and promising process for the conversion of methane and carbon dioxide which are the most abundant carbon sources into valuable syngas. The produced syngas, which is a mixture of hydrogen and carbon monoxide, can be used as intermediates in the manufacture of numerous chemicals. To achieve high conversion, DRM reaction is operated at high temperatures (700-900 °C) that can cause major drawbacks of catalyst deactivation by carbon deposition, metal sintering or metal oxidation. Therefore, the primary goal is to develop a metal based catalyst for DRM that can completely suppress carbon formation by designing the catalyst composition. The strategy of this work was to synthesize Ni-based catalysts all of which prepared by homogeneous deposition precipitation method (HDP) to produce nanoparticles with narrow size distribution. In addition, control the reactivity of the metal by finely tuning the bimetallic composition and the reaction conditions in terms of reaction temperature and pressure. The highly endothermic dry reforming of methane proceeds via CH4 decomposition to leave surface carbon species, followed by removal of C with CO2-derived species to give CO. Tuning the reactivity of the active metal towards these reactions during DRM allows in principle the catalyst surface to remain active and clean without carbon deposition for a long-term. The initial attempt was to improve the resistance of Ni catalyst towards carbon deposition, therefore, a series of 5 wt.% bimetallic Ni9Pt1 were supported on various metal oxides (Al2O3, CeO2, and ZrO2). The addition of small amount of noble metal improved the stability of the catalyst compared to their monometallic Ni and Pt catalysts, but still high amount of carbon (> 0.1 wt.%) was formed after 24 h of the reaction. The obtained results showed that the catalytic performance, particle size and amount of deposited carbon depends on the nature of support. Among the tested

Catalytic decomposition of nitrous oxide from nitric acid production tail gases. Investigation of inhibition effects. Executive summary

International Nuclear Information System (INIS)

Mul, G.; Perez-Ramirez, J.; Xu, Xiaoding; Oonk, H.; Yakovlev, A.

2001-06-01

Nitric acid production is an important source of nitrous oxide, one of the green-house gases. Catalytic decomposition of N2O in nitric acid tail-gases might be a possibility for emission reduction, but technology is not yet available. As a part of development of suitable catalytic systems, research was performed, aiming at: gaining an improved understanding of catalytic decomposition of N2O and the inhibiting effects of NO, NO2, H2O and O2; and preparing a 'go-no go' decision whether or not to proceed with subsequent re-search and development and if yes, to indicate what technology further development should aim for. Due to the presence of NOx and water in the nitric acid tail gases, catalytic decomposition proves not to be feasible at temperatures below 350C. At higher temperatures possibilities do exist and a number of promising catalysts are identified. These are active (80 - 100 % conversion) in the temperature range of 400 - 500C and under simulated tail gas conditions. Considering process conditions only (temperatures and composition of the tail-gases), the catalysts studied (pref. the Rh/Al2O3 types) could be in principle applied successfully in all Dutch nitric acid plants

Dynamical properties of nano-structured catalysts for methane conversion: an in situ scattering study

DEFF Research Database (Denmark)

Kehres, Jan

/NiO particles in a fresh catalyst sample showed a Ni/NiO core shell structure. The Ni lattice parameter decreased during the reduction due to the release of stress between the Ni core and the NiO shell. Ni particles sintered during heating in hydrogen after the reduction of the NiO shell. Dry reforming......The reactivity of catalyst particles can be radically enhanced by decreasing their size down to the nanometer range. The nanostructure of a catalyst can have an enormous and positive influence on the reaction rate, for example strong structure sensitivity was observed for methane reforming...... range from 298 - 1023 K. Correlated crystallite and particle growth due to sintering were observed after the decomposition of the surfactant. Furthermore transformations from rod to spherical particle shape were observed. In situ reduction experiments of a Ni/MgAl2O4 catalyst were performed. The Ni...

Conversion of glycerol to polyglycerol over waste duck-bones as a catalyst in solvent free etherification process

Science.gov (United States)

Ayoub, Muhammad; Sufian, Suriati; Mekuria Hailegiorgis, Sintayehu; Ullah, Sami; Uemura, Yoshimitsu

2017-08-01

The alkaline catalyst derived from the duck-bones was used for conversion of glycerol to polyglycerol via solvent free etherification process. The physicochemical properties of prepared materials were duck-bones were systematically investigated as a catalyst by latest techniques of Thermo gravimetric analysis (TGA), X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) surface properties. TGA showed different trends of duck-bones decomposition from room temperature to 1000C. XRD pattern showed a clear and sharp peaks of a crystalline phase of CaO. The activity of the catalysts was in line with the basic amount of the strong base sites, surface area, and crystalline phase in the catalysts. The prepared catalyst derived from duck-bones provided high activity (99 %) for glycerol conversion and around 68 % yield for polyglycerol production. These ample wastes of duck-bones have good potential to be used as polyglycerol production catalysts due to have high quantity of Ca compare to other types of bones like cow, chicken and fish bones.

Kinetic Model of Resin－Catalyzed Decomposition of Acetone Cyanohydrin in Organic Solvent

Institute of Scientific and Technical Information of China (English)

章亭洲; 杨立荣; 朱自强; 吴坚平

2003-01-01

Decomposition of acetone cyanohydrin is the first-step reaction for preparing (S)-α-cyano-3-phenoxybenzyl alcohol (CPBA) by the one-pot method in organic media. Considering the compatibility of biocatalysts with chemical catalysts and the successive operation in the bioreactor, anion exchange resin (D301) was used as catalyst for this reaction. External diffusion limitation was excluded by raising rotational speed to higher than 190r·min-1 in both solvents. Internal diffusion limitation was verified to be insignificant in this reaction system. The effect of acetone cyanohydrin concentration on the reaction was also investigated. An intrinsic kinetic model was proposed when the mass transfer limitation was excluded, and the average deviation of the model is 10.5%.

Catalytic Methane Decomposition over Fe-Al2O3

KAUST Repository

Zhou, Lu

2016-05-09

The presence of a Fe-FeAl2O4 structure over an Fe-Al2O3 catalysts is demonstrated to be vital for the catalytic methane decomposition (CMD) activity. After H2 reduction at 750°C, Fe-Al2O3 prepared by means of a fusion method, containing 86.5wt% FeAl2O4 and 13.5wt% Fe0, showed a stable CMD activity at 750°C for as long as 10h. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Development of new heterogeneous catalysts for the decomposition of methanol into hydrogen and carbon monoxide applying high throughput methods; Entwicklung neuer heterogener Katalysatoren zur Spaltung von Methanol in Wasserstoff und Kohlenmonoxid mittels Hochdurchsatz-Methoden

Energy Technology Data Exchange (ETDEWEB)

Weiss, Torsten

2008-07-11

The topic of this thesis has been the development of new heterogeneous catalysts for the decomposition of methanol into hydrogen and carbon monoxide. As an important constraint here, the content of noble metals of the catalysts should be as low as possible. High-throughput-methods were applied in some of the syntheses and experiments to accelerate the development, as, for example, the use of liquid based sol-gel syntheses and the examination of catalyst libraries by spatial resolution gas chromatography. This screening technique allowed to test up to 207 different substances during one single experiment. Then, different combinatorial strategies were applied. First, these methods led to a highly active and stable catalyst in the ternary system of Cu-Ni-Zn, which showed high conversion and selectivity comparable to an industrial reference catalyst. Its activity during an 18 hour long term run was constant in contrast to the reference. Second, an additional approach starting from a broader variety of elements led to a Ce- Ru- and to a Cr-Ru-catalyst. Both of them were highly active in short term experiments, but lost their outstanding performances during long term runs. (orig.) [German] Die vorliegende Arbeit befasste sich mit der Entwicklung neuer heterogener Katalysatoren fuer die Spaltung von Methanol zu Wasserstoff und Kohlenmonoxid, die einen moeglichst geringen Gehalt an Edelmetallen aufweisen sollten. Um diesen Prozess zu beschleunigen, wurden in einem Teil der Synthesen und Experimente Hochdurchsatzmethoden verwendet. Neben der Roboter gestuetzten Sol-Gel-Synthese umfasste dies die Untersuchung von Katalysatorbibliotheken mittels ortsaufgeloester Gaschromatographie, die es ermoeglichte, in einem Experiment bis zu 207 verschiedene Substanzen auf ihre katalytische Aktivitaet zu testen. Unter Anwendung verschiedener kombinatorischer Strategien wurde zunaechst ein sehr aktiver und stabiler Katalysator im ternaeren Cu-Ni-Zn-System entdeckt. Neben Umsaetzen und

Methane-induced Activation Mechanism of Fused Ferric Oxide-Alumina Catalysts during Methane Decomposition

KAUST Repository

Reddy Enakonda, Linga; Zhou, Lu; Saih, Youssef; Ould-Chikh, Samy; Lopatin, Sergei; Gary, Daniel; Del-Gallo, Pascal; Basset, Jean-Marie

2016-01-01

Activation of Fe2O3-Al2O3 with CH4 (instead of H2) is a meaningful method to achieve catalytic methane decomposition (CMD). This reaction of CMD is more economic and simple against commercial methane steam reforming (MSR) as it produces COx-free H2

Soot oxidation over NOx storage catalysts. Activity and deactivation

International Nuclear Information System (INIS)

Krishna, K.; Makkee, M.

2006-01-01

Soot oxidation activity and deactivation of NO x storage and reduction (NSR) catalysts containing Pt, K, and Ba supported on Al 2 O 3 , are studied under a variety of reaction conditions. K-containing catalysts decrease soot oxidation temperature with O 2 alone and the presence of Pt further enhance the activity due to synergetic effect. The active species responsible for synergism on Pt/K-Al 2 O 3 are unstable and cannot be regenerated. Soot oxidation temperature decreases by about 150 o C with NO+O 2 exhaust feed gas and under lean conditions NSR system acts as catalysed soot filter (CSF). The reactions that are mainly responsible for decreasing soot oxidation temperature are: (1) soot oxidation with NO 2 followed by NO recycles to NO 2 , and (2) soot oxidation with O 2 assisted by NO 2 . Only a part of the stored NO x that is decomposed at high temperatures under lean conditions is found to be useful for soot oxidation. NO x storage capacity of NSR catalysts decreases upon ageing under soot oxidising conditions. This will lead to a decreased soot oxidation activity on stored nitrate decomposition. Pt/K-Al 2 O 3 catalyst is more active, but least stable compared with Pt/Ba-Al 2 O 3 . (author)

Fructose decomposition kinetics in organic acids-enriched high temperature liquid water

Energy Technology Data Exchange (ETDEWEB)

Li, Yinghua; Lu, Xiuyang; Yuan, Lei; Liu, Xin [Department of Chemical and Biochemical Engineering, Zhejiang University, Zheda Road 38, Hangzhou 310027, Zhejiang (China)

2009-09-15

Biomass continues to be an important candidate as a renewable resource for energy, chemicals, and feedstock. Decomposition of biomass in high temperature liquid water is a promising technique for producing industrially important chemicals such as 5-hydroxymethylfurfural (5-HMF), furfural, levulinic acid with high efficiency. Hexose, which is the hydrolysis product of cellulose, will be one of the most important starting chemicals in the coming society that is highly dependent on biomass. Taking fructose as a model compound, its decomposition kinetics in organic acids-enriched high temperature liquid water was studied in the temperature range from 180 C to 220 C under the pressure of 10 MPa to further improve reaction rate and selectivity of the decomposition reactions. The results showed that the reaction rate is greatly enhanced with the addition of organic acids, especially formic acid. The effects of temperature, residence time, organic acids and their concentrations on the conversion of fructose and yield of 5-HMF were investigated. The evaluated apparent activation energies of fructose decomposition are 126.8 {+-} 3.3 kJ mol{sup -1} without any catalyst, 112.0 {+-} 13.7 kJ mol{sup -1} catalyzed with formic acid, and 125.6 {+-} 3.8 kJ mol{sup -1} catalyzed with acetic acid, respectively, which shows no significant difference. (author)

Reduction of nanowire diameter beyond lithography limits by controlled catalyst dewetting

International Nuclear Information System (INIS)

Calahorra, Yonatan; Kerlich, Alexander; Gavrilov, Arkady; Cohen, Shimon; Ritter, Dan; Amram, Dor

2016-01-01

Catalyst assisted vapour-liquid–solid is the most common method to realize bottom-up nanowire growth; establishing a parallel process for obtaining nanoscale catalysts at pre-defined locations is paramount for further advancement towards commercial nanowire applications. Herein, the effect of a selective area mask on the dewetting of metallic nanowire catalysts, deposited within lithography-defined mask pinholes, is reported. It was found that thin disc-like catalysts, with diameters of 120–450 nm, were transformed through dewetting into hemisphere-like catalysts, having diameters 2–3 fold smaller; the process was optimized to about 95% yield in preventing catalyst splitting, as would otherwise be expected due to their thickness-to-diameter ratio, which was as low as 1/60. The catalysts subsequently facilitated InP and InAs nanowire growth. We suggest that the mask edges prevent surface migration mediated spreading of the dewetted metal, and therefore induce its agglomeration into a single particle. This result presents a general strategy to diminish lithography-set dimensions for NW growth, and may answer a fundamental challenge faced by bottom-up nanowire technology. (paper)

Pyrolysis of aseptic packages (tetrapak) in a laboratory screw type reactor and secondary thermal/catalytic tar decomposition

Energy Technology Data Exchange (ETDEWEB)

Haydary, J., E-mail: juma.haydary@stuba.sk [Institute of Chemical and Environmental Engineering, Faculty of Chemical and Food Technology, Slovak University of Technology, Radlinského 9, 812 37 Bratislava (Slovakia); Susa, D.; Dudáš, J. [Institute of Chemical and Environmental Engineering, Faculty of Chemical and Food Technology, Slovak University of Technology, Radlinského 9, 812 37 Bratislava (Slovakia)

2013-05-15

Highlights: ► Pyrolysis of aseptic packages was carried out in a laboratory flow reactor. ► Distribution of tetrapak into the product yields was obtained. ► Composition of the pyrolysis products was estimated. ► Secondary thermal and catalytic decomposition of tars was studied. ► Two types of catalysts (dolomite and red clay marked AFRC) were used. - Abstract: Pyrolysis of aseptic packages (tetrapak cartons) in a laboratory apparatus using a flow screw type reactor and a secondary catalytic reactor for tar cracking was studied. The pyrolysis experiments were realized at temperatures ranging from 650 °C to 850 °C aimed at maximizing of the amount of the gas product and reducing its tar content. Distribution of tetrapak into the product yields at different conditions was obtained. The presence of H{sub 2}, CO, CH{sub 4}, CO{sub 2} and light hydrocarbons, HCx, in the gas product was observed. The Aluminum foil was easily separated from the solid product. The rest part of char was characterized by proximate and elemental analysis and calorimetric measurements. The total organic carbon in the tar product was estimated by elemental analysis of tars. Two types of catalysts (dolomite and red clay marked AFRC) were used for catalytic thermal tar decomposition. Three series of experiments (without catalyst in a secondary cracking reactor, with dolomite and with AFRC) at temperatures of 650, 700, 750, 800 and 850 °C were carried out. Both types of catalysts have significantly affected the content of tars and other components in pyrolytic gases. The effect of catalyst on the tetrapack distribution into the product yield on the composition of gas and on the total organic carbon in the tar product is presented in this work.

Characterization and Utilization of Calcium Oxide (CaO) Thermally Decomposed from Fish Bones as a Catalyst in the Production of Biodiesel from Waste Cooking Oil

OpenAIRE

Aldes Lesbani; Sabat Okta Ceria Sitompul; Risfidian Mohadi; Nurlisa Hidayati

2016-01-01

Thermal decomposition of fish bones to obtain calcium oxide (CaO) was conducted at various temperatures of 400, 500, 800, 900, 1000, and 1100 °C. The calcium oxide was then characterized using X-ray diffractometer, FTIR spectrophotometer, and SEM analysis. The calcium oxide obtained from the decomposition at 1000 °C was then used as a catalyst in the production of biodiesel from waste cooking oil. Diffraction pattern of the calcium oxide produced from decomposition at 1000...

The removal of VOC from air using EB, MW and catalyst - Laboratory plant results

Energy Technology Data Exchange (ETDEWEB)

Calinescu, I. [Polytechnic University, Bucharest (Romania); Ighigeanu, D.; Martin, D. [National Institute for Lasers, Plasma and Radiation Physics, Bucharest (Romania)

2011-07-01

A new hybrid technique for the VOCs removal from gases, based on the combined use of EB induced NTP (non-thermal plasma), MW induced NTP and catalytic oxidation, named “EB+MW-plasma catalysis”, is presented. The main goal of our research was to combine the features of each known technique used in gas pollution control, i.e. the very high efficiency of EB in converting VOCs to intermediate products, the ability of MW to produce and sustain NTP in large electrodeless reactors, and the important role of catalysts in the complete conversion to CO{sub 2} and H{sub 2}O. Our experiences shown that the two means of treating the gases are complementary: the catalytic oxidation in the presence of MW is efficient for high VOC initial concentrations and low flow rates while the exclusive use of the EB irradiation determines high decomposition efficiencies only in the case of very low concentrations of VOC but for large flow rates. Real synergistic effects between NTP and catalysis were obtained by introducing the catalyst into the irradiation zone. The main conclusion of this work is that the combined treatment EB+MW+catalyst improves both decomposition efficiency and oxidation efficiency. The EB+MW+Catalysis method demonstrated good results on a wide range of concentrations and flow rates. (author)

Report on surveys in fiscal 1999 on research and development of the environment harmonizing catalyst technology; 1999 nendo kankyo chowagata shokubai gijutsu no kenkyu kaihatsu chosa hokokusho

Energy Technology Data Exchange (ETDEWEB)

NONE

2000-03-01

This paper reports the surveys in fiscal 1999 on research and development of the environment harmonizing catalyst technology. The discussion subjects taken up included suppression of discharge of carbon dioxide, catalysts used when manufacturing hydrogen and technology thereof, and environment purifying catalysts to decompose harmful substances, and technology thereof. The roles of catalysts and their technologies are expected in reducing the reforming temperatures, achieving energy saving, and reducing decomposition energy. Furthermore, the catalysts are expected of high activity, long life and low cost. Three themes were selected from the emergency and importance points of view. The themes are, in the consumer field, research and development of efficiency improvement in membrane reactors for reforming low-grade hydrocarbons to structure a technology to manufacture hydrogen for small-size portable fuel cells; and in the industrial field, development of hydrogen and carbon product manufacturing technologies with which CO2 generation is suppressed by means of the catalytic decomposition process. In practice, for such discharged harmful substances as dioxins, PCB and volatile organic compounds (VOC), treating them is the urgent environmental problem, and therefore, the fundamental research was taken up for practical application of the second-generation catalysts of the ultra-violet light and visible light responding type. (NEDO)

Synergistic effect of catalyst for oxidation removal of toluene

International Nuclear Information System (INIS)

Zhu Tao; Li Jian; Liang Wenjun; Jin Yuquan

2009-01-01

A series of experiments was performed for toluene removal from a gaseous influent at the normal temperature and atmospheric pressure by decomposition due to dielectric barrier discharge generated non-thermal plasma, by using MnO 2 /γ-Al 2 O 3 as catalyst. The removal efficiency of toluene was significantly increased by combining MnO 2 /γ-Al 2 O 3 with NTP. At the same time, the goal of improving energy efficiency and decreasing O 3 from exhaust gas treatment was accomplished.

Synergistic effect of catalyst for oxidation removal of toluene.

Science.gov (United States)

Zhu, Tao; Li, Jian; Liang, Wenjun; Jin, Yuquan

2009-06-15

A series of experiments was performed for toluene removal from a gaseous influent at the normal temperature and atmospheric pressure by decomposition due to dielectric barrier discharge generated non-thermal plasma, by using MnO(2)/gamma-Al(2)O(3) as catalyst. The removal efficiency of toluene was significantly increased by combining MnO(2)/gamma-Al(2)O(3) with NTP. At the same time, the goal of improving energy efficiency and decreasing O(3) from exhaust gas treatment was accomplished.

Fabrication of aligned carbon nanotubes on Cu catalyst by dc plasma-enhanced catalytic decomposition

Energy Technology Data Exchange (ETDEWEB)

Zhang Zhejuan [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China); Shakerzadeh, Maziar; Tay, Beng Kang; Li Xiaocheng; Tan Chongwei [School of Electrical and Electronic Engineering, Nanyang Technological University, Nanyang Avenue 50, 639798 Singapore (Singapore); Lin Lifeng; Guo Pingsheng; Feng Tao [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China); Sun Zhuo, E-mail: zsun@phy.ecnu.edu.cn [Department of Physics, Engineering Research Center for Nanophotonics and Advanced Instrument, East China Normal University, North Zhongshan Road 3663, 200062 Shanghai (China)

2009-04-01

Aligned multi-walled carbon nanotubes (ACNTs) are deposited using copper (Cu) catalyst on Chromium (Cr)-coated substrate by plasma-enhanced chemical vapor deposition at temperature of 700 deg. C. Acetylene gas has been used as the carbon source while ammonia is used for diluting and etching. The thicknesses of Cu films on Cr-coated Si (100) substrates are controlled by deposition time of magnetron sputtering. The growth behaviors and quality of ACNTs are investigated by scanning electron microscopy (SEM) and transmission electron microscopy. The different performance of ACNTs on various Cu films is explained by referring to the graphitic order as detected by Raman spectroscopy. The results indicate that the ACNTs are formed in tip-growth model where Cu is used as a novel catalyst, and the thickness of Cu films is responsible to the diameter and quality of synthesized CNTs.

Catalytic reduction of NO{sub x} in gasoline engine exhaust over copper- and nickel-exchanged X-zeolite catalysts

Energy Technology Data Exchange (ETDEWEB)

Bhattacharyya, S. [Indian Inst. of Technology, Kharagpur (India). Dept. of Mechanical Engineering; Das, R.K. [Indian School of Mines, Dhanbad (India). Dept. of Engineering and Mining Machinery

2001-10-11

Catalytic removal of NO{sub x} in engine exhaust gases can be accomplished by non-selective reduction, selective reduction and decomposition. Noble metals are extensively used for non-selective reduction of NO{sub x} and up to 90% of engine NO{sub x} emissions can be reduced in a stoichiometric exhaust. This requirement of having the stoichiometric fuel-air ratio acts against efficiency improvement of engines. Selective NO{sub x} reduction in the presence of different reductants such as, NH{sub 3}, urea or hydrocarbons, requires close control of the amount of reductant being injected which otherwise may be emitted as a pollutant. Catalytic decomposition is the best option for NO{sub x} removal. Nevertheless, catalysts which are durable, economic and active for NO{sub x} reduction at normal engine exhaust temperature ranges are still being investigated. Three catalysts based on X-zeolite have been developed by exchanging the Na+ ion with copper, nickel and copper-nickel metal ions and applied to the exhaust of a stationary gasoline engine to explore their potential for catalytic reduction of NO{sub x} under a wide range of engine and exhaust conditions. Some encouraging results have been obtained. The catalyst Cu-X exhibits much better NO{sub x} reduction performance at any temperature in comparison to Cu-Ni-X and Ni-X; while Cu-Ni-X catalyst exhibits slightly better performance than Ni-X catalyst. Maximum NO{sub x} efficiency achieved with Cu-X catalyst is 59.2% at a space velocity (sv) of 31 000 h{sup -1}; while for Cu-Ni-X and Ni-X catalysts the equivalent numbers are 60.4% and 56% respectively at a sv of 22 000 h{sup -1}. Unlike noble metals, the doped X-zeolite catalysts exhibit significant NO{sub x} reduction capability for a wide range of air/fuel ratio and with a slower rate of decline as well with increase in air/fuel ratio. (author)

Permanganate oxidation of sulfur compounds to prevent poisoning of Pd catalysts in water treatment processes.

Science.gov (United States)

Angeles-Wedler, Dalia; Mackenzie, Katrin; Kopinke, Frank-Dieter

2008-08-01

The practical application of Pd-catalyzed water treatment processes is impeded by catalyst poisoning by reduced sulfur compounds (RSCs). In this study, the potential of permanganate as a selective oxidant for the removal of microbially generated RSCs in water and as a regeneration agent for S-poisoned catalysts was evaluated. Hydrodechlorination using Pd/Al2O3 was carried out as a probe reaction in permanganate-pretreated water. The activity of the Pd catalysts in the successfully pretreated reaction medium was similar to that in deionized water. The catalyst showed no deactivation behavior in the presence of permanganate at a concentration level or = 0.08 mM, a significant but temporary inhibition of the catalytic dechlorination was observed. Unprotected Pd/Al2O3, which had been completely poisoned by sulfide, was reactivated by a combined treatment with permanganate and hydrazine. However, the anthropogenic water pollutants thiophene and carbon disulfide were resistant against permanganate. Together with the preoxidation of catalyst poisons, hydrophobic protection of the catalysts was studied. Pd/zeolite and various hydrophobically coated catalysts showed a higher stability against ionic poisons and permanganate than the uncoated catalyst. By means of a combination of oxidative water pretreatment and hydrophobic catalyst protection, we provide a new tool to harness the potential of Pd-catalyzed hydrodehalogenation for the treatment of real waters.

Solid state synthesis, characterization, surface and catalytic properties of Pr2CoO4 and Pr2NiO4 catalyst

International Nuclear Information System (INIS)

Sinha, K.K.; Indu, N.K.; Sinha, S.K.; Pankaj, A.K.

2008-01-01

Full text: The most interesting non-stoichiometric oxides are found in transition metal and rare earth oxides at higher temperatures. The role of Solid State properties in the catalysis using mixed metal oxide as catalyst have wide applications in fertilizer, Petro-chemical, Pharmaceutical, cosmetic, paint detergents, plastics and food-stuff industries and these are also resistive towards acids and alkalies. The use of catalyst has opened up new process routes or revolutioned the existing process in terms of economics and efficiency and has radically changed the industrial scenario. The use of catalyst is so pervasive today that nearly 70 % of modern chemical processes are based on it at some stage or other and 90% new processes developed are catalytic nature. A series of non-stoichiometric spinel type of oxide catalyst of Praseodymium with cobalt and nickel were synthesized by their oxalates through Solid State reaction technique at different activation temperatures i.e. 600, 700, 800 and 900 deg C. The characterization of catalyst was done by XRD, FTIR and ESR methods. X-ray powder diffraction study shows that catalysts are made up of well grown crystallinities mostly in single phase crystal and system is of orthorhombic structure. FTIR is related to inadequate decomposition of oxalate ion from the Catalyst. The kinetic decomposition of Urea was employed as a model reaction to study the catalytic potentiality of different catalysts. Surface and Catalytic Properties of catalysts were measured. A relation between activation temperature and surface properties like excess surface oxygen (E.S.O.), surface acidity and surface area was observed. A linear relationship between the surface area of the catalyst and the amount of ammonia gas evolved per gm of the sample was observed also. Nickel containing catalysts were found a bit more catalytic active in comparison to cobalt oxide catalysts. Transition metal ions (i.e. Ni 2+ and Co 2+ ions) are mainly responsible for

Lithium chemistry of lithium doped magnesium oxide catalysts used in the oxidative coupling of methane

NARCIS (Netherlands)

Korf, S.J.; Roos, J.A.; de Bruijn, N.A.; van Ommen, J.G.; Ross, J.R.H.

1990-01-01

Active sites are created on the surface of a Li/MgO catalyst used for the selective oxidation of methane by the gradual loss of carbon dioxide from surface carbonate species in the presence of oxygen. Decomposition of the carbonate species in the absence of oxygen is detrimental to the activity of

Catalytic activity of cobalt and cerium catalysts supported on calcium hydroxyapatite in ethanol steam reforming

Directory of Open Access Journals (Sweden)

Dobosz Justyna

2016-09-01

Full Text Available In this paper, Co,Ce/Ca10(PO46(OH2 catalysts with various cobalt loadings for steam reforming of ethanol (SRE were prepared by microwave-assisted hydrothermal and sol-gel methods, and characterized by XRD, TEM, TPR-H2, N2 adsorption-desorption measurements and cyclohexanol (CHOL decomposition tests. High ethanol conversion (close to 100% was obtained for the catalysts prepared by both methods but these ones prepared under hydrothermal conditions (HAp-H ensured higher hydrogen yield (3.49 mol H2/mol C2H5OH as well as higher amount of hydrogen formed (up to 70% under reaction conditions. The superior performance of 5Co,10Ce/HAp-H catalyst is thought to be due to a combination of factors, including increased reducibility and oxygen mobility, higher density of basic sites on its surface, and improved textural properties. The results also show a significant effect of cobalt loading on catalysts efficiency in hydrogen production: the higher H2 yield exhibit catalysts with lower cobalt content, regardless of the used synthesis method.

Possible use of ferrocyanide as a redox additive for prevention of electrolyte decomposition in overcharged nickel batteries

Energy Technology Data Exchange (ETDEWEB)

Xiaoming Zhu [Wuhan University (China). Dept. of Chemistry; College of Xianning (China). Dept. of Chemistry; Hanxi Yang; Xingping Ai [Wuhan University (China). Dept. of Chemistry

2003-11-30

The redox reaction of ferrocyanide was investigated for possible use as a redox additive for the prevention of the electrolyte decomposition of aqueous secondary Ni-NH batteries in the overcharged condition. It was found that with the presence of ferrocyanide, the charging voltage can be leveled off just above the complete oxidation of the positive nickel electrode. As a result, the oxygen evolution was greatly suppressed and the internal pressure of the batteries was kept at low level even at prolonged overcharging. In addition, no detrimental effects of the redox additive were observed on the normal charge-discharge performance of Ni-MH batteries. (author)

Effect of Ni-Co Ternary Molten Salt Catalysts on Coal Catalytic Pyrolysis Process

Science.gov (United States)

Cui, Xin; Qi, Cong; Li, Liang; Li, Yimin; Li, Song

2017-08-01

In order to facilitate efficient and clean utilization of coal, a series of Ni-Co ternary molten salt crystals are explored and the catalytic pyrolysis mechanism of Datong coal is investigated. The reaction mechanisms of coal are achieved by thermal gravimetric analyzer (TGA), and a reactive kinetic model is constructed. The microcosmic structure and macerals are observed by scanning electron microscope (SEM). The catalytic effects of ternary molten salt crystals at different stages of pyrolysis are analyzed. The experimental results show that Ni-Co ternary molten salt catalysts have the capability to bring down activation energy required by pyrolytic reactions at its initial phase. Also, the catalysts exert a preferable catalytic action on macromolecular structure decomposition and free radical polycondensation reactions. Furthermore, the high-temperature condensation polymerization is driven to decompose further with a faster reaction rate by the additions of Ni-Co ternary molten salt crystal catalysts. According to pyrolysis kinetic research, the addition of catalysts can effectively decrease the activation energy needed in each phase of pyrolysis reaction.

Comparison of Preparation Methods of Copper Based PGMFree Diesel-Soot Oxidation Catalysts

Directory of Open Access Journals (Sweden)

R. Prasad

2011-05-01

Full Text Available CuO-CeO2 systems have been proposed as a promising catalyst for low temperature diesel-soot oxidation. CuO-CeO2 catalysts prepared by various methods were examined for air oxidation of the soot in a semi batch tubular flow reactor. The air oxidation of soot was carried out under tight contact with soot/catalyst ratio of 1/10. Air flow rate was 150 ml/min, soot-catalyst mixture was 110 mg, heating rate was 5 0C/min. Prepared catalysts were calcined at 500 0C and their stability was examined by further heating to 800 0C for 4 hours. It was found that the selectivity of all the catalysts was nearly 100% to CO2 production. It was observed that the activity and stability of the catalysts greatly influenced by the preparation methods. The strong interaction between CuO and CeO2 is closely related to the preparation route that plays a crucial role in the soot oxidation over the CuO-CeO2 catalysts. The ranking order of the preparation methods of the catalysts in the soot oxidation performance is as follows: sol-gel > urea nitrate combustion > Urea gelation method > thermal decomposition > co-precipitation. Copyright © 2011 BCREC UNDIP. All rights reserved.(Received: 27th June 2010, Revised: 7th August 2010; Accepted: 13rd October 2010[How to Cite: R. Prasad, V.R. Bella. (2011. Comparison of Preparation Methods of Copper Based PGMFree Diesel-Soot Oxidation Catalysts. Bulletin of Chemical Reaction Engineering and Catalysis, 6(1: 15-21. doi:10.9767/bcrec.6.1.822.15-21][How to Link / DOI: http://dx.doi.org/10.9767/bcrec.6.1.822.15-21 || or local: http://ejournal.undip.ac.id/index.php/bcrec/article/view/822 | View in 

Nanosized ruthenium particles decorated carbon nanofibers as active catalysts for the oxidation of p-cymene by molecular oxygen

CSIR Research Space (South Africa)

Makgwane, PR

2013-07-01

Full Text Available demonstrated that the direct participation of the catalyst in p-cymene C-H bond activation occurred via catalytic decomposition of tertiary-butyl hydroperoxide (TBHP), which was added as an initiator, into a free-radical chain initiator rather than the direct H...

Contribution to the study of the oxidation reaction of the carbon oxide in contact with catalysts issued from the decomposition of nickel hydro-aluminates at various temperatures; Contribution a l'etude de la reaction d'oxydation de l'oxyde de carbone au contact des catalyseurs issus de la decomposition a diverses temperatures des hydroaluminates de nickel

Energy Technology Data Exchange (ETDEWEB)

Samaane, Mikhail

1966-09-26

Addressing the study of the oxidation reaction of carbon oxide which produces carbon dioxide, this research thesis reports the study of this reaction in presence of catalysts (2NiO + Al{sub 2}O{sub 3}, NiAl{sub 2}O{sub 4} and NiO + NiAl{sub 2}O{sub 4}) issued from the decomposition of nickel hydro-aluminates at different temperatures. The first part describes experimental techniques and the nature of materials used in this study. The second part reports the study of the catalytic activity of the 2NiO+Al{sub 2}O{sub 3} catalyst during the oxidation of CO. Preliminary studies are also reported: structure and texture of nickel hydro-aluminate which is the raw material used to produce catalysts, activation of this compound to develop the catalytic activity in CO oxidation, chemisorption of CO, O{sub 2} and CO{sub 2} on the 2NiO+Al{sub 2}O{sub 3} solid, interaction of adsorbed gases at the solid surface, and kinetic study of the oxidation reaction. The third part reports the study of the catalytic activity in the oxidation reaction of CO of spinel catalysts (NiAl{sub 2}O{sub 4} and NiO+NiAl{sub 2}O{sub 4}) obtained by calcination of nickel hydro-aluminates at high temperature. The formation of the spinel phase, the chemisorption of CO, O{sub 2} and CO{sub 2} on NiAl{sub 2}O{sub 4}, and the kinetic of the oxidation reaction are herein studied.

Effect of thermal treatment conditions on properties of vanadium molybdenum oxide catalyst in acrolein oxidation reaction to acrylic acid

International Nuclear Information System (INIS)

Gorshkova, T.P.; Tarasova, D.V.; Olen'kova, I.P.; Andrushkevich, T.V.; Nikoro, T.A.

1984-01-01

The effect of thermal treatment conditions (temperature and gas medium) on properties of vanadium molybdenum oxide catalyst in acrolein oxidation reaction to acrylic acid is investigated. It is shown that active and selective catalysts are formed in the course of thermal decomposition of the drying product of ammonium metavanadate and paramolybdate under the conditions ensuring the vanadium ion reduction up to tetravalent state with conservation of molybdenum oxidation degree equal to 6. It is possible to realize it either by treatment of the catalyst calcinated in the air flow at 300 deg by the reaction mixture at the activation stage or by gas-reducer flow treatment at 280 deg. Thermal treatment in the reducing medium of the oxidized catalyst does not lead to complete regeneration of its properties

Supported Co-Mn-Al Mixed Oxides as Catalysts for N2O Decomposition.

Czech Academy of Sciences Publication Activity Database

Pacultová, K.; Karásková, C.; Strakošová, J.; Jirátová, Květa; Obalová, L.

2015-01-01

Roč. 18, č. 20 (2015), s. 1114-1122 ISSN 1631-0748. [AWPAC2014 - International Symposium on Air & Water Pollution Abatement Catalysis. Krakow, 01.09.2014-05.09.2014] R&D Projects: GA ČR GA14-13750S Institutional support: RVO:67985858 Keywords : supported catalysts * heterogeneous catalysis * spinel phase * nitrogen oxides Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 1.798, year: 2015

Magnetic minerals from volcanic Ultisols as heterogeneous Fenton catalysts

International Nuclear Information System (INIS)

Aravena, S.; Pizarro, C.; Rubio, M. A.; Cavalcante, L. C. D.; Garg, V. K.; Pereira, M. C.; Fabris, J. D.

2010-01-01

This study was devoted to the evaluation of the effectiveness of Fenton catalysts, based on magnetically-concentrated portions of iron oxide-rich sand fractions from two magnetic Ultisols, derived from volcanic materials of southern Chile. The samples were labeled according to the municipality where the sample sites are geographically located, namely Metrenco and Collipulli, and were characterized with Moessbauer spectroscopy at 298 K and saturation magnetization (σ) measurements. Moessbauer data revealed a complex magnetic hyperfine structure for these magnetic portions from both soil-sand materials, suggesting relatively complex mineral assemblages. The monitored rate of H 2 O 2 decomposition via heterogeneous Fenton reaction revealed that materials from the Collipulli soil are more efficient Fenton catalyst than are those from the Metrenco soil. The reasons for these differences are from now on being explored on basis of a more detailed chemical investigation of these samples.

Pyrolysis of polyethylene terephthalate containing real waste plastics using Ni loaded zeolite catalysts

Science.gov (United States)

Al-asadi, M.; Miskolczi, N.

2018-05-01

In this work the pyrolysis of polyethylene terephthalate (PET) containing real waste plastic was investigated using different Ni loaded catalysts: Ni/ZSM-5, Ni/y-zeolite, Ni/β-zeolite and Ni/natural zeolite (clinoptilolite). Raw materials were pyrolyzed in a horizontal tubular reactor between 600 and 900°C using 10% of catalysts. It was found, that both temperature increasing and catalysts presence can increase the gas yields, however owing to gasification reactions, the pyrolysis oil yield decreased with increasing temperature. Ni/y-zeolite catalyst had the most benefit in gas yield increasing at low temperature; however Ni/ZSM-5 showed advanced property in gas yield increasing at high temperature. Gases contained hydrogen, carbon oxides and hydrocarbons, which composition was significantly affected by catalysts. Ni loaded zeolites favoured to the formation of hydrogen and branched hydrocarbons; furthermore the concentrations of both CO and CO2 were also increased as function of elevated temperature. That phenomenon was attributed to the further decomposition of PET, especially to the side chain scission reactions. Owing to the Boudouard reaction, the ratio of CO2/CO can increased with temperature. Pyrolysis oils were the mixtures of n-saturated, n-unsaturated, branched, oxygen free aromatics and oxygenated hydrocarbons. Temperature increasing has a significant effect to the aromatization and isomerization reactions, while the catalysts can efficiently decreased the concentration of oxygen containing compounds.

Photocatalytic ozonation of terephthalic acid: a by-product-oriented decomposition study.

Science.gov (United States)

Fuentes, Iliana; Rodríguez, Julia L; Poznyak, Tatyana; Chairez, Isaac

2014-11-01

Terephthalic acid (TA) is considered as a refractory model compound. For this reason, the TA degradation usually requires a prolonged reaction time to achieve mineralization. In this study, vanadium oxide (VxOy) supported on titanium oxide (TiO2) served as a photocatalyst in the ozonation of the TA with light-emitting diodes (LEDs), having a bandwidth centered at 452 nm. The modified catalyst (VxOy/TiO2) in combination with ozone and LEDs improved the TA degradation and its by-products. The results obtained by this system were compared with photolysis, single ozonation, catalytic ozonation, and photocatalytic ozonation of VxOy/TiO2 with UV lamp. The LED-based photocatalytic ozonation showed almost the same decomposition efficiency of the TA, but it was better in comparison with the use of UV lamp. The oxalic acid accumulation, as the final product of the TA decomposition, was directly influenced by either the presence of VxOy or/and the LED irradiation. Several by-products formed during the TA degradation, such as muconic, fumaric, and oxalic acids, were identified. Besides, two unidentified by-products were completely removed during the observed time (60 min). It was proposed that the TA elimination in the presence of VxOy/TiO2 as catalyst was carried out by the combination of different mechanisms: molecular ozone reaction, indirect mechanism conducted by ·OH, and the surface complex formation.

Green synthesis of halloysite nanotubes supported Ag nanoparticles for photocatalytic decomposition of methylene blue

International Nuclear Information System (INIS)

Zou Meiling; Zhu Han; Xu Congsheng; Du Mingliang; Fu Yaqin

2012-01-01

Using tea polyphenols (TPs) as a reductant, Ag nanoparticles (AgNPs) supported on halloysite nanotubes (HNTs) were simply and greenly synthesized for the photocatalytic decomposition of methylene blue (MB). HNTs were initially functionalized by N-β-aminoethyl-γ-aminopropyl trimethoxysilane (AEAPTMS) to introduce amino groups to form N-HNTs to fasten the AgNPs; then AgNPs were synthesized and ‘anchored’ on the surface of the HNTs. Fourier transform infrared spectroscopy was employed to testify the amino groups on the surface of the HNTs. Transmission electron microscopy, field-emission scanning electron microscopy and x-ray diffraction were utilized to characterize the structure and morphology of the synthesized HNTs supported by the AgNPs (AgNPs-N-HNTs). The results showed that the AgNPs had been synthesized and ‘anchored’ onto the surface of the HNTs with a diameter of about 20-30 nm. X-ray photoelectron spectroscopy analysis revealed the chelating interaction between the AgNPs and N atoms together with the TP molecular. The photocatalytic activity of the as-prepared AgNPs-N-HNTs catalyst was evaluated by decomposition of MB; the results showed that the prepared catalyst exhibited excellent catalytic activity and high adsorption capability to MB. (paper)

Understanding Catalytic Activity Trends for NO Decomposition and CO Oxidation using Density Functional Theory and Microkinetic Modeling

DEFF Research Database (Denmark)

Falsig, Hanne

-metal surfaces by combining a database of adsorption energies on stepped metal surfaces with known Brønsted–Evans–Polanyi (BEP) relations for the activation barriers of dissociation of diatomic molecules over stepped transition- and noble-metal surfaces. The potential energy diagram directly points to why Pd......The main aim of this thesis is to understand the catalytic activity of transition metals and noble metals for the direct decomposition of NO and the oxidation of CO. The formation of NOx from combustion of fossil and renewable fuels continues to be a dominant environmental issue. We take one step...... towards rationalizing trends in catalytic activity of transition metal catalysts for NO decomposition by combining microkinetic modelling with density functional theory calculations. We establish the full potential energy diagram for the direct NO decomposition reaction over stepped transition...

Destruction of Toluene by the Combination of High Frequency Discharge Electrodeless Lamp and Manganese Oxide-Impregnated Granular Activated Carbon Catalyst

Directory of Open Access Journals (Sweden)

Jianhui Xu

2014-01-01

Full Text Available The destruction of low concentration of toluene (0–30 ppm has been studied under the UV/photogenerated O3/MnO2-impregnated granular activated carbon (MnO2-impregnated GAC process by the combination of self-made high frequency discharge electrodeless lamp (HFDEL with MnO2-impregnated GAC catalyst. Experimental results showed that the initial toluene concentration can strongly affect the concentration of photogenerated O3 from HFDEL and the efficiency and mass rate of destruction of toluene via HFDEL/MnO2-impregnated GAC system. Active oxygen and hydroxyl radicals generated from HFDEL/MnO2-impregnated GAC system played a key role in the decomposition of toluene process and the intermediates formed by photolysis are more prone to be mineralized by the subsequent MnO2-impregnated GAC catalyst compared to the original toluene, resulting in synergistic mineralization of toluene by HFDEL/MnO2-impregnated GAC system. The role of MnO2-impregnated GAC catalyst is not only to eliminate the residual O3 completely but also to enhance the decomposition and mineralization of toluene.

Hydrogen peroxide decomposition kinetics in aquaculture water

DEFF Research Database (Denmark)

Arvin, Erik; Pedersen, Lars-Flemming

2015-01-01

during the HP decomposition. The model assumes that the enzyme decay is controlled by an inactivation stoichiometry related to the HP decomposition. In order to make the model easily applicable, it is furthermore assumed that the COD is a proxy of the active biomass concentration of the water and thereby......Hydrogen peroxide (HP) is used in aquaculture systems where preventive or curative water treatments occasionally are required. Use of chemical agents can be challenging in recirculating aquaculture systems (RAS) due to extended water retention time and because the agents must not damage the fish...... reared or the nitrifying bacteria in the biofilters at concentrations required to eliminating pathogens. This calls for quantitative insight into the fate of the disinfectant residuals during water treatment. This paper presents a kinetic model that describes the HP decomposition in aquaculture water...

Preparation of polymer composites using nanostructured carbon produced at large scale by catalytic decomposition of methane

International Nuclear Information System (INIS)

Suelves, I.; Utrilla, R.; Torres, D.; Llobet, S. de; Pinilla, J.L.; Lázaro, M.J.; Moliner, R.

2013-01-01

Polymer-based composites were prepared using different concentrations of nanostructured carbons (NCs), produced by catalytic decomposition of methane (CDM). Four carbonaceous nanostructures were produced using different catalysts (with Ni and Fe as active phases) in a rotary bed reactor capable of producing up to 20 g of carbon per hour. The effect of nanostructured carbon on the thermal and electrical behaviour of epoxy-based composites is studied. An increase in the thermal stability and the decrease of electrical resistivity were observed for the composites at carbon contents as low as 1 wt%. The highest reduction of the electrical resistivity was obtained using multi-walled carbon nanotubes obtained with the Fe based catalysts. This effect could be related to the high degree of structural order of these materials. The results were compared with those obtained using a commercial carbon nanofibre, showing that the use of carbon nanostructures from CDM can be a valid alternative to the commercial nanofibres. -- Highlights: ► Preparation of polymer nanocomposites with enhanced thermal and electrical properties. ► Formation of nanostructured carbon materials with different textural and structural properties at large scale. ► Catalytic decomposition of methane to simultaneously produce hydrogen and carbon materials.

Feasibility study of various sulphonation methods for transforming carbon nanotubes into catalysts for the esterification of palm fatty acid distillate

International Nuclear Information System (INIS)

Shuit, Siew Hoong; Tan, Soon Huat

2014-01-01

Highlights: • First report on the production of biodiesel from low-value industrial by-product using sulphonated MWCNTs as catalyst. • Various sulphonation methods were used to transform MWCNTs into catalysts. • SO 3 H were successfully grafted on the surface of MWCNTs, which resulted in a high biodiesel yield and reuse capacity. • The maximum FAME yield by sulphonated MWCNTs was higher than for other popular solid acid catalysts. - Abstract: Sulphonated multi-walled carbon nanotubes were synthesised and utilised as catalysts to transform palm fatty acid distillate, the low-value by-product of palm oil refineries, into the more valuable product of biodiesel. The most common method to prepare carbon-based solid acid catalysts is thermal treatment with concentrated sulphuric acid, which is a time-consuming and energy-intensive process. Therefore, the feasibility of other sulphonation methods, such as the in situ polymerisation of acetic anhydride and sulphuric acid, the thermal decomposition of ammonium sulphate and the in situ polymerisation of poly(sodium4-styrenesulphonate), were examined in this study. The esterification reaction was performed at 170 °C for 3 h at a methanol to palm fatty acid distillate ratio of 20 and catalyst loading of 2 wt% in a pressurised reactor. The fatty acid methyl esters yields achieved by the sulphonated multi-walled carbon nanotubes prepared via thermal treatment with concentrated sulphuric acid, the in situ polymerisation of acetic anhydride and sulphuric acid, the thermal decomposition of ammonium sulphate and the in situ polymerisation of poly(sodium4-styrenesulphonate) were 78.1%, 85.8%, 88.0% and 93.4%, respectively. All catalysts could maintain a high catalytic activity even during the fifth cycle. Among the sulphonation methods, the in situ polymerisation of poly(sodium4-styrenesulphonate) produced the catalyst with the highest acid group density. In addition, the resonance structures of the benzenesulphonic acid

Removal of VOCs by hybrid electron beam reactor with catalyst bed

International Nuclear Information System (INIS)

Kim, Jinkyu; Han, Bumsoo; Kim, Yuri; Lee, J.H.; Park, C.R.; Kim, J.C.; Kim, J.C.; Kim, K.J.

2004-01-01

Electron beam decomposition of volatile organic compounds (VOCs) was studied in order to obtain information for developing effective treatment method of off-gases from industries. We have examined the combination of electron beam and catalyst honeycomb which is either 1% platinum based or ceramic honeycomb- based aluminum oxide, using a hybrid reactor in order to improve removal efficiency and CO 2 formation; and to suppress undesirable by-product formation e.g. O 3 , aerosol, H x C y. , and tar. The experiments were conducted using a pilot-scale treatment system (maximum capacity; 1800 N m 3 /h) that fitted the field size to scale up from the traditional laboratory scale system for VOC removal with electron beam irradiation. Toluene was selected as a typical VOC that was irradiated to investigate product formation, effect of ceramic and catalyst, and factors effecting overall efficiency of degradation. Styrene was selected as the most odorous compound among the VOCs of interest. It was found that VOCs could be destroyed more effectively using a hybrid system with catalyst bed than with electron beam irradiation only

Design of sintering-stable heterogeneous catalysts

DEFF Research Database (Denmark)

Gallas-Hulin, Agata

One of the major issues in the use of metal nanoparticles in heterogeneous catalysis is sintering. Sintering occurs at elevated temperatures because of increased mobility of nanoparticles, leading to their agglomeration and, as a consequence, to the deactivation of the catalyst. It is an emerging...... problem especially for the noble metals-based catalysis. These metals being expensive and scarce, it is worth developing catalyst systems which preserve their activity over time. Encapsulation of nanoparticles inside zeolites is one of the ways to prevent sintering. Entrapment of nanoparticles inside...

Effect of catalyst preparation on the yield of carbon nanotube growth

International Nuclear Information System (INIS)

Escobar, Mariano; Rubiolo, Gerardo; Candal, Roberto; Goyanes, Silvia

2009-01-01

Multi-wall carbon nanotubes (MWCNTs) were synthesized by catalytic chemical vapor deposition (CVD) on catalytic iron nanoparticles dispersed in a silica matrix, prepared by sol gel method. In this contribution, variation of gelation condition on catalyst structure and its influence on the yield of carbon nanotubes growth was studied. The precursor utilized were tetraethyl-orthosilicate and iron nitrate. The sols were dried at two different temperatures in air (25 or 80 deg. C) and then treated at 450 deg. C for 10 h. The xerogels were introduced into the chamber and reduced in a hydrogen/nitrogen (10%v/v) atmosphere at 600 deg. C. MWCNTs were formed by deposition of carbon atoms from decomposition of acetylene at 700 deg. C. The system gelled at RT shows a yield of 100% respect to initial catalyst mass whereas the yield of that gelled at 80 deg. C was lower than 10%. Different crystalline phases are observed for both catalysts in each step of the process. Moreover, TPR analysis shows that iron oxide can be efficiently reduced to metallic iron only in the system gelled at room temperature. Carbon nanotubes display a diameter of about 25-40 nm and several micron lengths. The growth mechanism of MWCNTs is base growth mode for both catalysts.

Effect of catalyst preparation on the yield of carbon nanotube growth

Energy Technology Data Exchange (ETDEWEB)

Escobar, Mariano, E-mail: mescobar@df.uba.a [Dep. Quimica Inorganica, Analitica y Quimica Fisica, FCEyN, UBA, Ciudad Universitaria (1428), Bs As (Argentina); LP and MC, Dep. Fisica, FCEyN, UBA (Argentina); Rubiolo, Gerardo [Unidad de Actividad Materiales, CNEA, Av Gral Paz 1499, San Martin (1650), Bs As (Argentina); Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina); Candal, Roberto [Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina); Instituto de Fisico-quimica de Materiales, Ambiente y Energia (INQUIMAE), CONICET - UBA (Argentina); Goyanes, Silvia [LP and MC, Dep. Fisica, FCEyN, UBA (Argentina); Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) (Argentina)

2009-10-01

Multi-wall carbon nanotubes (MWCNTs) were synthesized by catalytic chemical vapor deposition (CVD) on catalytic iron nanoparticles dispersed in a silica matrix, prepared by sol gel method. In this contribution, variation of gelation condition on catalyst structure and its influence on the yield of carbon nanotubes growth was studied. The precursor utilized were tetraethyl-orthosilicate and iron nitrate. The sols were dried at two different temperatures in air (25 or 80 deg. C) and then treated at 450 deg. C for 10 h. The xerogels were introduced into the chamber and reduced in a hydrogen/nitrogen (10%v/v) atmosphere at 600 deg. C. MWCNTs were formed by deposition of carbon atoms from decomposition of acetylene at 700 deg. C. The system gelled at RT shows a yield of 100% respect to initial catalyst mass whereas the yield of that gelled at 80 deg. C was lower than 10%. Different crystalline phases are observed for both catalysts in each step of the process. Moreover, TPR analysis shows that iron oxide can be efficiently reduced to metallic iron only in the system gelled at room temperature. Carbon nanotubes display a diameter of about 25-40 nm and several micron lengths. The growth mechanism of MWCNTs is base growth mode for both catalysts.

Dispersed catalysts for transforming extra heavy crude oil into transportable upgraded crude: phase identification

Energy Technology Data Exchange (ETDEWEB)

Martinez, S.; Canizales, E.; Machin, I. [Gerencia Depttal de Investigacion Estrategica en Refinacion PDVSA Intevep (Venezuela); Segovia, X.; Rivas, A.; Lopez, E.; Pena, J.P.; Rojas, J.D.; Sardella, R. [Gerencia Depttal de Infraestructura y Mejoramiento en Faja Petrolifera PDVSA Intevep (Venezuela)

2011-07-01

A new technology to convert extra heavy crude oil into transportable upgraded crude has been developed. A water/oil emulsion composed of steam and catalyst precursors is introduced in the feed which then generates unsupported dispersed catalyst in situ under thermal decomposition. The aim of this paper is to characterize the particles. The study was conducted in a laboratory and on a pilot scale on three different vacuum residues using high resolution transmission electron microscopy and a transmission electron microscope. Results showed that the particles were formed by oxides and inorganic sulphur based in transition metals and their sizes ranged between 5 and 120 nm; in addition, good dispersion was observed. This study demonstrated that the process involved in the generation of dispersed catalyst is extremely complex and showed that further work with heavy crude oils and its residua is required to understand the mechanisms involved.

Development of Low Temperature Catalysts for an Integrated Ammonia PEM Fuel Cell

OpenAIRE

Hill, Alfred

2014-01-01

It is proposed that an integrated ammonia-PEM fuel cell could unlock the potential of ammonia to act as a high capacity chemical hydrogen storage vector and enable renewable energy to be delivered eectively to road transport applications. Catalysts are developed for low temperature ammonia decomposition with activity from 450 K (ruthenium and cesium on graphitised carbon nanotubes). Results strongly suggest that the cesium is present on the surface and close proximity to ruthenium nanoparticl...

Study of polyoxide catalysts of methane combustion on Mn, Cu, Ni, rare earth elements, alkaline earth elements base by the X-ray fluorescence analysis method

International Nuclear Information System (INIS)

Grigor'eva, V.P.; Popova, N.M.; Zheksenbaeva, Z.T.; Sass, A.S.; Salakhova, R.Kh.; Dosumov, K.D.

2002-01-01

The results of X-ray fluorescence analysis of polyoxide catalysts on of Mn, Cu, Ni, rare earth elements, alkaline earth elements base supported on 2 % Ce/θ-Al 2 O 3 are presented. This polyoxide catalysts are using for deep methane oxidation. DRON-4-7 X-ray diffractometers was applied for the analysis. It was found, that oxides in Ni-Cu-Cr catalysts after long time heating up to 1200 deg. C have been interacted with catalyst supports with Ni(Cu)Al 2 O 3 aluminates formation and due to its decomposition transformation degree of CH 4 to CO 2 are reduced. Activity of MnBaSrCeLa catalysts after heating up to 1200 deg. C does not changed

Photocatalytic Removal of Phenol under Natural Sunlight over N-TiO2-SiO2 Catalyst: The Effect of Nitrogen Composition in TiO2-SiO2

Directory of Open Access Journals (Sweden)

Viet-Cuong Nguyen

2009-01-01

Full Text Available In this present work, high specific surface area and strong visible light absorption nitrogen doped TiO2-SiO2 photocatalyst was synthesized by using sol-gel coupled with hydrothermal treatment method. Nitrogen was found to improve the specific surface area while it also distorted the crystal phase of the resulting N-TiO2-SiO2 catalyst. As the N/ (TiO2-SiO2 molar ratio was more than 10%, the derived catalyst presented the superior specific surface area up to 260 m2/g. Nevertheless, its photoactivity towards phenol removal was observed to significantly decrease, which could results from the too low crystallinity. The nitrogen content in N-TiO2-SiO2 catalyst was therefore necessary to be optimized in terms of phenol removal efficiency and found at ca. 5%. Under UVA light and natural sunlight irradiation of 80 min, N(5%-TiO2-SiO2 catalyst presented the phenol decomposition efficiencies of 68 and 100%, respectively. It was also interestingly found in this study that the reaction rate was successfully expressed using a Langmuir-Hinshelwood (L-H model, indicating the L-H nature of photocatalytic phenol decomposition reaction on the N-TiO2-SiO2 catalyst.

Structural characteristics of mixed oxides MOx/SiO2 affecting photocatalytic decomposition of methylene blue

International Nuclear Information System (INIS)

Gun’ko, V.M.; Blitz, J.P.; Bandaranayake, B.; Pakhlov, E.M.; Zarko, V.I.; Sulym, I.Ya.; Kulyk, K.S.; Galaburda, M.V.; Bogatyrev, V.M.; Oranska, O.I.; Borysenko, M.V.; Leboda, R.; Skubiszewska-Zięba, J.; Janush, W.

2012-01-01

A series of photocatalysts based on silica (nanoparticulate) supported titania, ceria, and ceria/zirconia were synthesized and characterized by a variety of techniques including surface area measurements, X-ray diffraction, Fourier transform infrared spectroscopy, zeta potential, surface charge density, and photocatalytic behavior toward methylene blue decomposition. Thermal treatment at 600 °C increases the anatase content of the titania based catalysts detected by XRD. Changes in the infrared spectra before and after thermal treatment indicate that at low temperature there are more ≡Si-O-Ti≡ bonds than at high temperature. As these bonds break upon heating the SiO 2 and TiO 2 separate, allowing the TiO 2 anatase phase to form. This results in an increased catalytic activity for the thermally treated samples. Nearly all titania based samples exhibit a negative surface charge density at pH 7 (initial pH of photocatalytic studies) which aids adsorption of methylene blue. The crystallinity of ceria and ceria/zirconia based catalysts are in some cases limited, and in others non-existent. Even though the energy band gap (E g ) can be lower for these catalysts than for the titania based catalysts, their photocatalytic properties are inferior.

A novel process for heavy residue hydroconversion using a recoverable pseudo-homogenous catalyst PHC system

Energy Technology Data Exchange (ETDEWEB)

Romocki, S.M.; Rhodey, W.G. [Mobis Energy Inc., Calgary, AB (Canada)

2008-10-15

This paper described a pseudo-homogenous catalyst (PHC) designed to refine heavy hydrocarbon residues containing sulfur, nitrogen, metals, and asphaltene impurities known to clog pores and deactivate traditional hydrocrackers. The heavy residue hydroconversion (HRH) process incorporated a single particle, chemically generated PHC uniformly distributed in the feed. Thermal decomposition within the reaction system of a water-in-oil emulsion containing ammonium paramolybdate was used to form molybdenum oxide, which was then sulfided within the feed in order to create an ultra-dispersed suspension of catalytically active molybdenum disulfide particles measuring between 2 and 9 nm. A proprietary online catalyst recovery and regeneration step was used to maintain high catalyst activity. The molybdenum was then recovered from a purge stream and then reintroduced to the catalyst preparation area as a catalyst precursor. After being conditioned, the feed was combined with hydrogen and a water-oil catalyst emulsion and introduced into a furnace. Heavy components were cracked, hydrogenated and converted to lighter products. The high performance catalyst system was able to convert 95 per cent of residues at pressures below 7.3 Mpa and at reaction temperatures ranging between 400 and 460 degrees C. The catalyst was tested at a pilot plant using Athabasca vacuum bottoms. It was concluded that the HRH process is now being successfully used to produce 200 barrels of heavy oil per day. Designs for commercial installations are now being prepared. 4 refs., 2 tabs., 2 figs.

Reactions of synthesis gas on silica supported transition metal catalysts

Energy Technology Data Exchange (ETDEWEB)

Niemelae, M. [VTT Chemical Technology, Espoo (Finland). Lab. of Industrial Chemistry

1997-12-31

The effect of catalyst precursor and composition on the activation of CO was investigated using CO hydrogenation as a test reaction. The interrelations of preparation, pretreatment, characteristics and activity were clarified. For Co/SiO{sub 2} catalyst, MgO promotion increased the CO adsorption capacity and the hydrogen uptake, although the extent of reduction for cobalt remained the same or decreased. The conversion per active metallic cobalt site consequently increased in conjunction with MgO promotion, while the effect on overall performance per 1 g of catalyst remained moderate. The precursor affected the performance of Co/SiO{sub 2} considerably. CO was more strongly adsorbed on catalysts of carbonyl origin than on those derived from cobalt nitrate, the activity thus being higher. Although the nitrate derived Co/SiO{sub 2} appeared both to retain its activity and to regain its adsorption capacity better than the catalysts of carbonyl origin, the performance of the latter was superior with time on stream. For tetranuclear cluster based Co-Ru and Co-Rh catalysts, rhodium or ruthenium was in contact with the support and cobalt was enriched on top. On Co-Ru/SiO{sub 2} ruthenium enhanced deactivation, and no benefits in activity or oxygenate selectivity were achieved relative to the monometallic catalysts of cluster origin. The Co-Rh/SiO{sub 2} catalysts were also less active than those derived from monometallic clusters, but they exhibited higher selectivities to oxygenated compounds due to the presence of active sites on the perimeter of the cobalt particles located on rhodium. The highest selectivity to oxygenates was achieved by changing the decomposition atmosphere of Rh{sub 4}(CO){sub 12}/SiO{sub 2} from hydrogen to carbon monoxide. The results also showed two types of active sites to be operative in the formation of oxygenates - one for ethanol and another for aldehydes. (orig.) 69 refs.

Efficient decomposition of formaldehyde at room temperature over Pt/honeycomb ceramics with ultra-low Pt content.

Science.gov (United States)

Nie, Longhui; Zheng, Yingqiu; Yu, Jiaguo

2014-09-14

Pt/honeycomb ceramic (Pt/HC) catalysts with ultra-low Pt content (0.005-0.055 wt%) were for the first time prepared by an impregnation of honeycomb ceramics with Pt precursor and NaBH4-reduction combined method. The microstructures, morphologies and textural properties of the resulting samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), and transmission electron microscopy (TEM). The obtained Pt/HC catalysts were used for catalytic oxidative decomposition of formaldehyde (HCHO) at room temperature. It was found that the as-prepared Pt/HC catalysts can efficiently decompose HCHO in air into CO2 and H2O at room temperature. The catalytic activity of the Pt/HC catalysts increases with increasing the Pt loading in the range of 0.005-0.013 wt%, and the further increase of the Pt loading does not obviously improve catalytic activity. From the viewpoint of cost and catalytic performance, 0.013 wt% Pt loading is the optimal Pt loading amount, and the Pt/HC catalyst with 0.013 wt% Pt loading also exhibited good catalytic stability. Considering practical applications, this work will provide new insights into the low-cost and large-scale fabrication of advanced catalytic materials for indoor air purification.

High temperature performance and stability of Fe-FER catalyst for N2O decomposition

Czech Academy of Sciences Publication Activity Database

Sádovská, Galina; Tabor, Edyta; Sazama, Petr; Lhotka, M.; Bernauer, M.; Sobalík, Zdeněk

2017-01-01

Roč. 89, JAN 2017 (2017), s. 133-137 ISSN 1566-7367 R&D Projects: GA ČR(CZ) GA14-10251S; GA MŠk(CZ) LM2015073 Institutional support: RVO:61388955 Keywords : High temperature N2O decomposition * FER * Iron Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 3.330, year: 2016

Plasma-catalytic decomposition of TCE

Energy Technology Data Exchange (ETDEWEB)

Vandenbroucke, A.; Morent, R.; De Geyter, N.; Leys, C. [Ghent Univ., Ghent (Belgium). Dept. of Applied Physics; Tuan, N.D.M.; Giraudon, J.M.; Lamonier, J.F. [Univ. des Sciences et Technologies de Lille, Villeneuve (France). Dept. de Catalyse et Chimie du Solide

2010-07-01

Volatile organic compounds (VOCs) are gaseous pollutants that pose an environmental hazard due to their high volatility and their possible toxicity. Conventional technologies to reduce the emission of VOCs have their advantages, but they become cost-inefficient when low concentrations have to be treated. In the past 2 decades, non-thermal plasma technology has received growing attention as an alternative and promising remediation method. Non-thermal plasmas are effective because they produce a series of strong oxidizers such as ozone, oxygen radicals and hydroxyl radicals that provide a reactive chemical environment in which VOCs are completely oxidized. This study investigated whether the combination of NTP and catalysis could improve the energy efficiency and the selectivity towards carbon dioxide (CO{sub 2}). Trichloroethylene (TCE) was decomposed by non-thermal plasma generated in a DC-excited atmospheric pressure glow discharge. The production of by-products was qualitatively investigated through FT-IR spectrometry. The results were compared with those from a catalytic reactor. The removal rate of TCE reached a maximum of 78 percent at the highest input energy. The by-products of TCE decomposition were CO{sub 2}, carbon monoxide (CO) hydrochloric acid (HCl) and dichloroacetylchloride. Combining the plasma system with a catalyst located in an oven downstream resulted in a maximum removal of 80 percent, at an energy density of 300 J/L, a catalyst temperature of 373 K and a total air flow rate of 2 slm. 14 refs., 6 figs.

A facile self-assembly approach to prepare palladium/carbon nanotubes catalyst for the electro-oxidation of ethanol

Science.gov (United States)

Wen, Cuilian; Zhang, Xinyuan; Wei, Ying; Zhang, Teng; Chen, Changxin

2018-02-01

A facile self-assembly approach is reported to prepare palladium/carbon nanotubes (Pd/CNTs) catalyst for the electro-oxidation of ethanol. In this method, the Pd-oleate/CNTs was decomposed into the Pd/CNTs at an optimal temperature of 195 °C in air, in which no inert gas is needed for the thermal decomposition process due to the low temperature used and the decomposed products are also environmental friendly. The prepared Pd/CNTs catalyst has a high metallic Pd0 content and the Pd particles in the catalyst are disperse, uniform-sized with an average size of ˜2.1 nm, and evenly distributed on the CNTs. By employing our strategy, the problems including the exfoliation of the metal particles from the CNTs and the aggregation of the metal particles can be solved. Comparing with the commercial Pd/C one, the prepared Pd/CNTs catalyst exhibits a much higher electrochemical activity and stability for the electro-oxidation of ethanol in the direct ethanol fuel cells.

Temperature-programmed reduction and cyclic voltammetry of Pt/carbon-fibre paper catalysts for methanol electrooxidation

International Nuclear Information System (INIS)

Attwood, P.A.; McNicol, B.D.; Short, R.T.

1981-01-01

Temperature-programmed reduction (TPR) and cyclic voltammetry (CV) studies of platinum catalysts supported on pyrographite-coated carbon-fibre paper, and prepared by either ion exchange or impregnation, clearly demonstrate the nature of the interactions between the platinum species and the support. After drying the above catalysts at 120 0 C, the ion-exchanged preparation exhibits the stronger interaction with the carbon support, as might be expected since a chemical interaction with carbon surface groups is known to occur in such catalysts. The presence of a fraction of bulk Pt(NH 3 ) 4 (OH) 2 impregnating salt in the impregnated catalyst has been detected using TPR. After air activation at 300 0 C, subambient reduction peaks were observed and the strength of binding of Pt in the ion-exchanged catalyst was reflected by its increased difficulty of reduction in comparison with that of the impregnated catalyst. The stoichiometry of reduction in ion-exchanged catalysts corresponds to Pt 2+ → Pt 0 in both dried and activated catalysts, with a small amount of Pt 4+ present in the latter. Upon activation the impregnated catalyst showed the presence of some Pt metal, which was thought to arise from the decomposition of the fraction of bulk Pt(NH 3 ) 4 (OH) 2 in the dried catalyst. Activation of ion-exchanged catalysts at temperatures higher than 300 0 C led to a progressive weakening of the Pt-support interaction and consequent smaller Pt surface areas. Activation at 500 0 C in air produced Pt metal exclusively and very low Pt surface areas. The strong interaction between Pt and the carbon support upon activation of the ion-exchanged catalyst at 300 0 C is thought to be the origin of the large metal surface area and the high catalytic activity for methanol electrooxidation found upon reduction

Synthesis, characterization and photocatalytic activity of porous manganese oxide doped titania for toluene decomposition

International Nuclear Information System (INIS)

Jothiramalingam, R.; Wang, M.K.

2007-01-01

The present study describes the photocatalytic degradation of toluene in gas phase on different porous manganese oxide doped titanium dioxide. As synthesized birnessite and cryptomelane type porous manganese oxide were doped with titania and tested for photocatalytic decomposition of toluene in gas phase. The effects of the inlet concentration of toluene, flow rate (retention time) were examined and the relative humidity was maintained constantly. Thermal and textural characterization of manganese oxide doped titania materials were characterized by X-ray diffraction (XRD), thermogravemetry (TG), BET and TEM-EDAX studies. The aim of the present study is to synthesize the porous manganese oxide doped titania and to study its photocatalytic activity for toluene degradation in gas phase. Cryptomelane doped titania catalyst prepared in water medium [K-OMS-2 (W)] is shown the good toluene degradation with lower catalysts loading compared to commercial bulk titania in annular type photo reactor. The higher photocatalytic activity due to various factors such as catalyst preparation method, experimental conditions, catalyst loading, surface area, etc. In the present study manganese oxide OMS doped titania materials prepared by both aqueous and non-aqueous medium, aqueous medium prepared catalyst shows the good efficiency due to the presence of OH bonded groups on the surface of catalyst. The linear forms of different kinetic equations were applied to the adsorption data and their goodness of fit was evaluated based on the R 2 and standard error. The goodness to the linear fit was observed for Elovich model with high R 2 (≥0.9477) value

THE THEORY OF DEVELOPMENT OF SUPPORTED METAL-COMPLEX CATALYSTS

Directory of Open Access Journals (Sweden)

T. L. Rakitskaya

2015-06-01

Full Text Available Some results of the investigations for the purpose of development of supported metal-complex catalysts for phosphine and carbon monoxide oxidation as well as for ozone decomposition are summarized. The activity of such catalysts has been found to depend not only on a nature of a central atom and ligands but also on a nature of supports. The theoretical model explaining mechanisms of surface complex formation taking into account the influence of physicochemical and structural-adsorption properties of the supports (SiO2, Al2O3, carbon materials, zeolites, dispersed silicas, lamellar aluminosilicates, etc. has been proposed. For quantitative description of the support effect, such a thermodynamic parameter as the adsorbed water activity assignable with the help of water vapor adsorption isotherms has been introduced. Successive stability constants of the surface metal complexes have been calculated by the kinetic method and, hence, compositions and partial catalytic activity of the latter have been determined. Taking into account the competitive adsorption of metal ions on the supports, some schemes of formation of surface bimetallic complexes have been suggested. The compositions of the supported metal-complex catalysts have been optimized to meet requirements of their use in respirators and plants for air purification from foregoing gaseous toxicants.

Catalyst preactivation using EURECAT TOTSUCAT CFP technology

Energy Technology Data Exchange (ETDEWEB)

Brahma, N.; Alexander, R.; Robinson, J. [Eurecat US Inc., Houston, TX (United States)

2009-07-01

This presentation described EURECAT's newly developed and patented technology that allows the start up of a hydrotreating process without the introduction of sulphur containing chemicals. This ex-situ process known as TOTSUCAT ensures complete activation and sulphiding of the catalyst prior to loading in the reactor. The benefits of TOTSUCAT include the elimination of sour water formation; the prevention of potential exotherms; minimal hydrogen sulphide (H{sub 2}) pressure; and no need for additional hydrogen. TOTSUCAT can be used in cases where the unit has temperature limitations that prevent a complete activation of the catalyst. The TOTSUCAT cracked feed protection (CFP) is an enhanced treatment that combines the advantages of preactivation with the ability to start up a unit with cracked stocks. It eliminates the need to delay the introduction of cracked feeds for 3 to 5 days after start-up, as is typical in commercial hydroprocessing units. The acidity of the catalyst is reduced in the CFP treatment, making it suitable for early introduction of cracked stocks. As such, the technology has potential use in the field of residual hydrocracking. The technology has been successfully applied in several commercial refineries in North America. tabs., figs.

A molecular molybdenum–schiff base electro-catalyst for generating hydrogen from acetic acid or water

International Nuclear Information System (INIS)

Cao, Jie-Ping; Fang, Ting; Zhou, Ling-Ling; Fu, Ling-Zhi; Zhan, Shuzhong

2014-01-01

Highlights: • The reaction of ligand, H 2 L and MoCl 5 gives a Mo(VI) complex [MoL(O) 2 ] 1. • Complex 1 is capable of catalyzing hydrogen evolution from acetic acid and water. • TOF reaches a maximum of 68 (DMF) and 356 (buffer, pH 6) moles/h, respectively. • Sustained proton reduction catalysis occurs over a 69 h period and no decomposition of 1. - ABSTRACT: The reaction of 2-pyridylamino-N,N-bis(2-methylene-4-ethyl-6-tert-butylphenol) (H 2 L) and MoCl 5 gives a molybdenum(VI) complex [MoL(O) 2 ] 1, a new molecular electrocatalyst, which has been determined by X-ray crystallography. Electrochemical studies show that complex 1 can catalyze hydrogen evolution from acetic acid or aqueous buffer. Turnover frequency (TOF) reaches a maximum of 68 (in N,N-Dimethylformamide (DMF)) and 356 (in buffer, pH 6.0) moles of hydrogen per mole of catalyst per hour, respectively. Sustained proton reduction catalysis occurs at glassy carbon (GC) electrode to give H 2 over a 69 h electrolysis period and no observable decomposition of the catalyst

Oxidation catalyst

Science.gov (United States)

Ceyer, Sylvia T.; Lahr, David L.

2010-11-09

The present invention generally relates to catalyst systems and methods for oxidation of carbon monoxide. The invention involves catalyst compositions which may be advantageously altered by, for example, modification of the catalyst surface to enhance catalyst performance. Catalyst systems of the present invention may be capable of performing the oxidation of carbon monoxide at relatively lower temperatures (e.g., 200 K and below) and at relatively higher reaction rates than known catalysts. Additionally, catalyst systems disclosed herein may be substantially lower in cost than current commercial catalysts. Such catalyst systems may be useful in, for example, catalytic converters, fuel cells, sensors, and the like.

Photo catalyst; Ko shokubai

Energy Technology Data Exchange (ETDEWEB)

NONE

1999-07-01

While titanium oxide is excited by the light, electrons of titanium oxide are taken away by the light energy to form positive holes. Water will be decomposed into hydrogen ion and hydroxy radical (OH) by these positive holes. This hydroxy radical is a strong reactive substance called active oxygen, it decomposes organisms. Besides this photo- catalyst function, the titanium oxide can also make surface of a substance superhydrophilic. The super hydrophilicity results in not forming water drops on the glass surface but spreading all over the surface to prevent a covering of fog on the glass surface. The published patents concerning the photo catalysts were 593 from Jan. 1998 to Jan. 1999. The applicant order is the first TOTO 143, the second Daikin Industry 19, the third Toshiba Raitech, Nitto Denko, Hitachi 17 respectively. (NEDO)

Novel Nano-Composite Catalysts for Renewable Energy Storage Applications

Science.gov (United States)

Devaguptapu, Surya Vamsi

and stability of oxides by engineering their morphology and nanostructures. The high performance bifunctional oxide catalyst is carbon free and can eventually overcome the stability issue for reversible fuel cell and metal-air battery applications. In addition, we have synthesized highly active transition metal doped Carbon Nano Tubes of very small thickness called Graphene Tubes which when integrated with metal oxides can lead to enhanced activity and durability for ORR and OER with current density as high as 25mAcm-2 at 1.6V vs RHE for OER and an onset potential of 1.0V vs RHE during ORR. Finally, we conclude by giving a brief description of the Hydrogen Economy and the role that ammonia decomposition can play in achieving the potential of hydrogen economy. We detail the synthesis procedures of some highly active transition metal nitride- alkali metal imide composites and study their activity for ammonia decomposition. The catalysts show conversion efficiencies as high as 95%.

Effects of various catalysts on hydrogen release and uptake characteristics of LiAlH{sub 4}

Energy Technology Data Exchange (ETDEWEB)

Resan, Mirna; Hampton, Michael D.; Lomness, Janice K. [Department of Chemistry, University of Central Florida, 4000 Central Florida Boulevard, Orlando, FL 32816-2366 (United States); Slattery, Darlene K. [Florida Solar Energy Center, 1679 Clearlake Rd., Cocoa, FL 32922 (United States)

2005-11-01

The effects of various catalysts on the hydrogen release characteristics of LiAlH{sub 4} were studied. The catalysts were incorporated into the alanate by ball milling. The catalysts studied included elemental titanium, TiH{sub 2}, TiCl{sub 4}, TiCl{sub 3}, AlCl{sub 3}, FeCl{sub 3}, elemental iron, elemental nickel, elemental vanadium, and carbon black. Dehydriding/rehydriding properties were characterized by using differential scanning calorimetry coupled with pressure measurement and X-ray diffraction. The addition of TiCl{sub 3} and TiCl{sub 4} to LiAlH{sub 4} eliminated the first step of hydrogen evolution and significantly lowered decomposition temperature of the second step. Doping with elemental iron caused only a slight decrease in the amount of hydrogen released and did not eliminate the first step of hydrogen evolution. Ball milling in the absence of the catalyst was found to decrease the release temperature of hydrogen, while doping with elemental iron did not have any additional effect on the temperature of hydrogen release of LiAlH{sub 4}. (author)

Application of carbon-coated TiO2 for decomposition of methylene blue in a photocatalytic membrane reactor

International Nuclear Information System (INIS)

Mozia, Sylwia; Toyoda, Masahiro; Inagaki, Michio; Tryba, Beata; Morawski, Antoni W.

2007-01-01

An application of carbon-coated TiO 2 for decomposition of methylene blue (MB) in a photocatalytic membrane reactor (PMR), coupling photocatalysis and direct contact membrane distillation (DCMD) was investigated. Moreover, photodegradation of a model pollutant in a batch reactor without membrane distillation (MD) was also examined. Carbon-modified TiO 2 catalysts containing different amount of carbon and commercially available TiO 2 (ST-01) were used in this study. The carbon-coated catalyst prepared from a mixture of ST-01 and polyvinyl alcohol in the mass ratio of 70/30 was the most effective in degradation of MB from all of the photocatalysts applied. Photodecomposition of MB on the recovered photocatalysts was lower than on the fresh ones. The photodegradation of MB in the PMR was slower than in the batch reactor, what probably resulted from shorter time of exposure of the catalyst particles to UV irradiation. The MD process could be successfully applied for separation of photocatalyst and by-products from the feed solution

Decomposition of formic acid over silica encapsulated and amine functionalised gold nanoparticles

DEFF Research Database (Denmark)

Mielby, Jerrik Jørgen; Kunov-Kruse, Andreas Jonas; Kegnæs, Søren

2017-01-01

Formic acid has recently attracted considerable attention as a safe and convenient source of hydrogen for sustainable chemical synthesis and renewable energy storage. Here, we show that silica encapsulated and amine functionalised gold nanoparticles are highly active catalysts for the production...... of hydrogen by vapour phase decomposition of formic acid. The core-shell catalysts are prepared in a reverse micelle system that makes it possible to control the size of the Au nanoparticles and the thickness of the SiO2 shells, which has a large impact on the catalytic activity. The smallest gold...... nanoparticles are 2.2 ± 0.3 nm in diameter and have a turnover frequency (TOF) of up to 958 h−1 at a temperature of 130 °C. Based on detailed in situ ATR-FTIR studies and results from kinetic isotope labelling experiments we propose that the active site is a low-coordinated and amine functionalised Au atom...

Effect of Promoters in Co-Mn-Al Mixed Oxide Catalyst on N2O Decomposition

Czech Academy of Sciences Publication Activity Database

Karásková, K.; Obalová, L.; Jirátová, Květa; Kovanda, F.

2010-01-01

Roč. 160, č. 2 (2010), s. 480-487 ISSN 1385-8947 R&D Projects: GA ČR GA106/09/1664 Institutional research plan: CEZ:AV0Z40720504 Keywords : nitrous oxide * catalytic decomposition * promoter effect Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 3.074, year: 2010

The synthesis of carbon nanocomposites as fuel cell catalyst support and the characterization of fuel cell catalysts by spatially resolved scanning mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Li, Nan

2007-07-01

Ammonia decomposition over Ni/SiO{sub 2} and Ni/MgO was investigated by temperature-programmed desorption (TPD) and temperature-programmed surface reaction (TPSR) in order to produce CO{sub x} free hydrogen fuel for fuel cell application. A highly efficient route for the synthesis of carbon nanocomposites based on electrochemical deposition and iron catalyzed chemical vapor deposition (CVD) was developed in order to obtain a promising substrate for fuel cell catalysts. The duration of electrochemical deposition, temperature and time for the carbon nanotubes (CNTs) growth had been optimized to achieve higher surface area after the growth. Hierarchically structured CNTs composites had been synthesized and electrochemical studies provided evidence for the strong interaction among the substrate and grown CNTs, which are essential for the application in fuel cells. A straightforward strategy was developed to synthesize well dispersed gold nanoparticles with a diameter of 4 to 6 nm on the sidewall of multi-walled carbon nanotubes (MWNTs). A gas flow set-up was developed for the evaluation of fuel cell catalysts by performing scanning mass spectrometry with integrated constant-distance positioning. Methanol oxidation was identified as a suitable test reaction. The diameter of scanning probe was reduced in order to achieve higher spatial resolution. Spatially resolved scanning mass spectrometry was successfully applied to visualize the catalytic activity over Pt-based catalysts and monitor the local activity of a catalysts coated membrane (CCM). The gas-solid phase reaction results were proved to be accurate, reliable and independent of the sample topography. This analytical method opens the way for fast quality control of the catalyst coating with respect to even coating and absence of damages, and for a better understanding of the CCM degradation in polymer membrane electrolyte fuel cells (PEMFCs). (orig.)

[Pd(NH{sub 3}){sub 4}]MoO{sub 4} as a precursor for Pd–Mo-containing catalysts: Thermal behavior, X-ray analysis of the thermolysis products and related catalytic studies

Energy Technology Data Exchange (ETDEWEB)

Gubanov, Alexander I., E-mail: gubanov@niic.nsc.su [Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, Akad. Lavrentiev Prospekt 3, 630090 Novosibirsk (Russian Federation); Novosibirsk State University, Pirogova str. 2, 630090 Novosibirsk (Russian Federation); Filatov, Eugeny Yu.; Semitut, Eugeny Yu.; Smolentsev, Anton I. [Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, Akad. Lavrentiev Prospekt 3, 630090 Novosibirsk (Russian Federation); Novosibirsk State University, Pirogova str. 2, 630090 Novosibirsk (Russian Federation); Snytnikov, Pavel V.; Potemkin, Dmitry I. [Novosibirsk State University, Pirogova str. 2, 630090 Novosibirsk (Russian Federation); Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Akad. Lavrentiev Prospekt 5, 630090 Novosibirsk (Russian Federation); Korenev, Sergey V. [Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, Akad. Lavrentiev Prospekt 3, 630090 Novosibirsk (Russian Federation); Novosibirsk State University, Pirogova str. 2, 630090 Novosibirsk (Russian Federation)

2013-08-20

Highlights: • [Pd(NH{sub 3}){sub 4}]MoO{sub 4} as a precursor for Pd–Mo-containing catalysts. • Different products are formed depending on atmosphere of thermal decomposition. • Thermolysis in He atmosphere affords finely mixed two-phase nanosized system Pd–MoO{sub 2}. • Pd–MoO{sub 2} system can be a promising catalyst both in pure and supported form. - Abstract: Compound [Pd(NH{sub 3}){sub 4}]MoO{sub 4} (1) has been synthesized and characterized by IR spectroscopy, analytical data, powder and single-crystal X-ray crystallography. Thermal properties of 1 have been examined by thermogravimetry. Powder X-ray diffraction has been applied to investigate the nanosized products of thermal decomposition of the precursor in hydrogen (Pd–Mo) and helium (Pd–MoO{sub 2}) atmospheres. Pd–Mo catalysts supported with γ-Al{sub 2}O{sub 3} have been tested in oxidation of CO and H{sub 2} mixtures.

Dual redox catalysts for oxygen reduction and evolution reactions: towards a redox flow Li-O2 battery.

Science.gov (United States)

Zhu, Yun Guang; Jia, Chuankun; Yang, Jing; Pan, Feng; Huang, Qizhao; Wang, Qing

2015-06-11

A redox flow lithium-oxygen battery (RFLOB) by using soluble redox catalysts with good performance was demonstrated for large-scale energy storage. The new device enables the reversible formation and decomposition of Li2O2 via redox targeting reactions in a gas diffusion tank, spatially separated from the electrode, which obviates the passivation and pore clogging of the cathode.

Synthesis and characterization of catalysts for the selective transformation of biomass-derived materials

Science.gov (United States)

Ghampson, Isaac Tyrone

The experimental work in this thesis focuses on generating catalysts for two intermediate processes related to the thermal conversion of lignocellulosic biomass: the synthesis and characterization of mesoporous silica supported cobalt catalysts for the Fischer-Tropsch reaction, and an exploration of the reactivity of bulk and supported molybdenum-based nitride catalysts for the hydrodeoxygenation (HDO) of guaiacol, a lignin model compound. The first section of the work details the synthesis of a series of silica-supported cobalt Fischer-Tropsch catalysts with pore diameters ranging from 2-23 nm. Detailed X-ray diffraction measurements were used to determine the composition and particle diameters of the metal fraction, analyzed as a three-phase system containing Cofcc, Cohcp and CoO particles. Catalyst properties were determined at three stages in catalyst history: (1) after the initial calcination step to thermally decompose the catalyst precursor into Co3O4, (2) after the hydrogen reduction step to activate the catalyst to Co and (3) after the FT reaction. From the study, it was observed that larger pore diameters supported higher turnover frequency; smaller pore diameters yielded larger mole fraction of CoO; XRD on post-reduction and post-FTS catalyst samples indicated significant changes in dispersivity after reduction. In the next section, the catalytic behaviors of unsupported, activated carbon-, alumina-, and SBA-15 mesoporous silica-supported molybdenum nitride catalysts were evaluated for the hydrodeoxygenation of guaiacol (2-methoxy phenol) at 300°C and 5 MPa. The nitride catalysts were prepared by thermal decomposition of bulk and supported ammonium heptamolybdate to form MoO 3 followed by nitridation in either flowing ammonia or a nitrogen/hydrogen mixture. The catalytic properties were strongly affected by the nitriding and purging treatment as well as the physical and chemical properties of support. The overall reaction was influenced by the

Mechanistic Investigation of the Reduction of NOx over Pt- and Rh-Based LNT Catalysts

Directory of Open Access Journals (Sweden)

Lukasz Kubiak

2016-03-01

Full Text Available The influence of the noble metals (Pt vs. Rh on the NOx storage reduction performances of lean NOx trap catalysts is here investigated by transient micro-reactor flow experiments. The study indicates a different behavior during the storage in that the Rh-based catalyst showed higher storage capacity at high temperature as compared to the Pt-containing sample, while the opposite is seen at low temperatures. It is suggested that the higher storage capacity of the Rh-containing sample at high temperature is related to the higher dispersion of Rh as compared to Pt, while the lower storage capacity of Rh-Ba/Al2O3 at low temperature is related to its poor oxidizing properties. The noble metals also affect the catalyst behavior upon reduction of the stored NOx, by decreasing the threshold temperature for the reduction of the stored NOx. The Pt-based catalyst promotes the reduction of the adsorbed NOx at lower temperatures if compared to the Rh-containing sample, due to its superior reducibility. However, Rh-based material shows higher reactivity in the NH3 decomposition significantly enhancing N2 selectivity. Moreover, formation of small amounts of N2O is observed on both Pt- and Rh-based catalyst samples only during the reduction of highly reactive NOx stored at 150 °C, where NOx is likely in the form of nitrites.

Oxygen isotope exchange on palladium catalysts

International Nuclear Information System (INIS)

Kravchuk, L.S.; Beschetvertnaya, T.I.; Novorodskij, V.G.; Novikova, M.G.; Zaretskij, M.V.; Valieva, S.V.

1983-01-01

Oxygen heteromolecular isotope exchange on unreduced palladium catalysts, distingushing by metal content is studied. Content of 18 O in gaseous phase is eoual to 46%. Calculations of heteroexchange rates are conducted with decrease of the 18 O in the gaseous phase over solid sample. Method of oxygen thermodesorption has been used to establish that palladium, deposited on γ-Al 2 O 3 during exchange process is in oxidized state; in this case strength of Pd-O bond is determined by content dispersity) of the metal. It is shown that significant increase of exchange rate on the samples with Pd >> 0.5 mass.% content can be induced as by side decomposition reaction of its oxide and corresponding dilution of gaseous mixture by ''light'' oxygen so by possibility of exchange with oxygen of PdO phase

Chloro-benquinone Modified on Graphene Oxide as Metal-free Catalyst: Strong Promotion of Hydroxyl Radical and Generation of Ultra-Small Graphene Oxide

Science.gov (United States)

Zhao, He; Wang, Juehua; Zhang, Di; Dai, Qin; Han, Qingzhen; Du, Penghui; Liu, Chenming; Xie, Yongbing; Zhang, Yi; Cao, Hongbin; Fan, Zhuangjun

2017-03-01

Carbon-based metal-free catalyst has attracted more and more attention. It is a big challenge to improve catalytic activity of metal-free catalyst for decomposition of H2O2 to produce hydroxyl radical (HO•). Here, we report chloro-benquinone (TCBQ) modified on graphene oxide (GO) as metal-free catalyst for strong promotion of HO•. By the incorporation of GO, the HO• production by H2O2 and TCBQ is significantly promoted. Based on density functional theory, TCBQ modified GO (GO-TCBQ) is more prone to be nucleophilic attacked by H2O2 to yield HO• via electron transfer acceleration. Furthermore, the generated HO• can cut GO nanosheets into uniform ultra-small graphene oxide (USGO) through the cleavage of epoxy and C-C bonds. Interestingly, the damaged GO and in situ formed GO fragments can further enhance decomposition of H2O2 to produce HO•. Different from other catalytic processes, the GO-TCBQ metal-free catalysis process can be enhanced by GO itself, producing more HO•, and uniform USGO also can be generated. Thus, the metal free catalysis will be considered a fabrication method for uniform USGO, and may be extended to other fields including detoxifying organic pollutants and the application as disinfectants.

Controllable synthesis of SnO2 nanowires and nanobelts by Ga catalysts

International Nuclear Information System (INIS)

Xie Xing; Shao Zhibin; Yang Qianhui; Shen Xiaoshuang; Zhu Wei; Hong Xun; Wang Guanzhong

2012-01-01

We report the morphology control of one-dimensional (1D) SnO 2 nanostructures by Ga catalysts using thermal evaporation method. Gallium (Ga), either from decomposition of GaN powder or from Ga metal, is adopted as a catalyst for the growth of long SnO 2 nanowires and nanobelts. At similar experimental conditions, quantities of nanobelts are formed instead of nanowires when the temperature and reaction time are increased. Such approach enables us to synthesize various morphologies of SnO 2 nanobelts with different side facets. Novel nanobelts with [0 0 1] growth direction with high energy side facets are obtained for the first time, which is attributed to the large amount of oxygen vacancies introduced in the nanobelts by the Ga catalysts. - Graphical abstract: Morphology control of one-dimensional SnO 2 nanostructures are realized via a thermal evaporation method. Novel nanobelts along [0 0 1] direction having high energy side facets were fabricated for the first time. Highlights: ► Morphology control of one-dimensional SnO 2 nanostructures are realized by Ga catalysts using thermal evaporation method. ► Oxygen vacancies influenced the growth directions in order to neutralize thermodynamic instability. ► Novel nanobelts with [0 0 1] growth direction with high energy side facets are obtained for the first time.

The Sabatier Principle Illustrated by Catalytic H2O2 Decomposition on Metal Surfaces

DEFF Research Database (Denmark)

Laursen, Anders Bo; Man, Isabela Costinela; Trinhammer, Ole

2011-01-01

Heterogeneous catalysis is important in today’s industry. Hence, it is imperative to introduce students to this field and its tools. A new way of introducing one of these tools, the Sabatier principle, via a laboratory exercise is presented. A volcano plot is constructed for the well-known hetero......Heterogeneous catalysis is important in today’s industry. Hence, it is imperative to introduce students to this field and its tools. A new way of introducing one of these tools, the Sabatier principle, via a laboratory exercise is presented. A volcano plot is constructed for the well......-known heterogeneous H2O2 catalytic decomposition reaction on various metal foils. The activity per catalyst surface area versus the computationally calculated binding energy of OH groups on the catalysts is plotted. The OH group is identified as the only surface intermediate in an intuitive reaction mechanism...

Studies on the decomposition of oxalic acid by nitric acid in presence of catalysts

International Nuclear Information System (INIS)

Noronha, D.M.; Pius, I.C.; Chaudhury, S.

2015-01-01

Impure Plutonium oxalate generated from the recovery of plutonium from waste solutions may require further purification via anion exchange. Conventionally, plutonium oxalate is converted to oxide in a furnace and the oxide is dissolved in Conc. HNO 3 containing HF and purified by anion exchange route. Studies initiated on the decomposition of oxalic acid with Conc. HNO 3 to facilitate direct dissolution of plutonium oxalate and quantitative destruction of oxalate are discussed in this paper. (author)

Photocatalytic carbon dioxide reduction with rhodium-based catalysts in solution and heterogenized within metal-organic frameworks.

Science.gov (United States)

Chambers, Matthew B; Wang, Xia; Elgrishi, Noémie; Hendon, Christopher H; Walsh, Aron; Bonnefoy, Jonathan; Canivet, Jérôme; Quadrelli, Elsje Alessandra; Farrusseng, David; Mellot-Draznieks, Caroline; Fontecave, Marc

2015-02-01

The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2 -storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal-organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2 . There is no precedent for a MOF catalyzing the latter reaction so far. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A comparative study of alumina-supported Ni catalysts prepared by photodeposition and impregnation methods on the catalytic ozonation of 2,4-dichlorophenoxyacetic acid

International Nuclear Information System (INIS)

Rodríguez, Julia L.; Valenzuela, Miguel A.; Tiznado, Hugo; Poznyak, Tatiana; Chairez, Isaac; Magallanes, Diana

2017-01-01

The heterogeneous catalytic ozonation on unsupported and supported oxides has been successfully tested for the removal of several refractory compounds in aqueous solution. In this work, alumina-supported nickel catalysts prepared by photodeposition and impregnation methods were compared in the catalytic ozonation of 2,4-dichlorophenoxyacetic acid (2,4-D). The catalysts were characterized by high-resolution electron microscopy and X-ray photoelectron spectroscopy. The photochemical decomposition of Ni acetylacetonate to produce Ni(OH) 2 , NiO, and traces of Ni° deposited on alumina was achieved in the presence of benzophenone as a sensitizer. A similar surface composition was found with the impregnated catalyst after its reduction with hydrogen at 500 °C and exposed to ambient air. Results indicated a higher initial activity and maleic acid (byproduct) concentration with the photodeposited catalyst (1 wt% Ni) compared to the impregnated catalyst (3 wt% Ni). These findings suggest the use of the photodeposition method as a simple and reliable procedure for the preparation of supported metal oxide/metal catalysts under mild operating conditions.

A comparative study of alumina-supported Ni catalysts prepared by photodeposition and impregnation methods on the catalytic ozonation of 2,4-dichlorophenoxyacetic acid

Energy Technology Data Exchange (ETDEWEB)

Rodríguez, Julia L., E-mail: ozliliana@yahoo.com.mx [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico); Valenzuela, Miguel A. [Lab.Catálisis y Materiales. ESIQIE–Instituto Politécnico Nacional. Zacatenco (Mexico); Tiznado, Hugo [Centro de Nanociencias y Nanotecnología. CNyN Universidad Nacional Autónoma de México (Mexico); Poznyak, Tatiana [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico); Chairez, Isaac [Departamento de Bioprocesos, UPIBI- Instituto Politécnico Nacional (Mexico); Magallanes, Diana [Lab. Ing. Química Ambiental. ESIQIE–Instituto Politécnico Nacional (Mexico)

2017-02-15

The heterogeneous catalytic ozonation on unsupported and supported oxides has been successfully tested for the removal of several refractory compounds in aqueous solution. In this work, alumina-supported nickel catalysts prepared by photodeposition and impregnation methods were compared in the catalytic ozonation of 2,4-dichlorophenoxyacetic acid (2,4-D). The catalysts were characterized by high-resolution electron microscopy and X-ray photoelectron spectroscopy. The photochemical decomposition of Ni acetylacetonate to produce Ni(OH){sub 2}, NiO, and traces of Ni° deposited on alumina was achieved in the presence of benzophenone as a sensitizer. A similar surface composition was found with the impregnated catalyst after its reduction with hydrogen at 500 °C and exposed to ambient air. Results indicated a higher initial activity and maleic acid (byproduct) concentration with the photodeposited catalyst (1 wt% Ni) compared to the impregnated catalyst (3 wt% Ni). These findings suggest the use of the photodeposition method as a simple and reliable procedure for the preparation of supported metal oxide/metal catalysts under mild operating conditions.

Production of phenolic-rich bio-oil from catalytic fast pyrolysis of biomass using magnetic solid base catalyst

International Nuclear Information System (INIS)

Zhang, Zhi-bo; Lu, Qiang; Ye, Xiao-ning; Li, Wen-tao; Hu, Bin; Dong, Chang-qing

2015-01-01

Highlights: • Phenolic-rich bio-oil was selectively produced from catalytic fast pyrolysis of biomass using magnetic solid base catalyst. • The actual yield of twelve major phenolic compounds reached 43.9 mg/g. • The peak area% of all phenolics reached 68.5% at the catalyst-to-biomass ratio of 7. • The potassium phosphate/ferroferric oxide catalyst possessed promising recycling properties. - Abstract: A magnetic solid base catalyst (potassium phosphate/ferroferric oxide) was prepared and used for catalytic fast pyrolysis of poplar wood to selectively produce phenolic-rich bio-oil. Pyrolysis–gas chromatography/mass spectrometry experiments were conducted to investigate the effects of pyrolysis temperature and catalyst-to-biomass ratio on the product distribution. The actual yields of important pyrolytic products were quantitatively determined by the external standard method. Moreover, recycling experiments were performed to determine the re-utilization abilities of the catalyst. The results showed that the catalyst exhibited promising activity to selectively produce phenolic-rich bio-oil, due to its capability of promoting the decomposition of lignin to generate phenolic compounds and meanwhile inhibiting the devolatilization of holocellulose. The maximal phenolic yield was obtained at the pyrolysis temperature of 400 °C and catalyst-to-biomass ratio of 2. The concentration of the phenolic compounds increased monotonically along with the increasing of the catalyst-to-biomass ratio, with the peak area% value increasing from 28.1% in the non-catalytic process to as high as 68.5% at the catalyst-to-biomass ratio of 7. The maximal total actual yield of twelve quantified major phenolic compounds was 43.9 mg/g, compared with the value of 29.0 mg/g in the non-catalytic process. In addition, the catalyst could be easily recovered and possessed promising recycling properties.

Catalyst for the use in the hydrotreatment of a heavy hydrocarbon oil, process to its preparation and process to its use

Energy Technology Data Exchange (ETDEWEB)

Shiroto, Y; Higashi, T; Ono, T

1981-10-01

A catalyst with an improved surface activity and a maintained selectivity is used in the decomposition of asphaltenes and the removal of heavy metals from a heavy hydrocarbon oil by hydrotreatment. The catalyst carrier consists of a calcined combination of a mixture from a clay mineral with double chain structure and at least one oxide-forming substance with a metal from the groups II A, III A, IV A or IV B of the periodic system. The catalytic metal component is selected from the groups V B, VI B, VIII or I B of the periodic system.

Catalytic decomposition of gaseous 1,2-dichlorobenzene over CuOx/TiO₂ and CuOx/TiO₂-CNTs catalysts: Mechanism and PCDD/Fs formation.

Science.gov (United States)

Wang, Qiu-lin; Huang, Qun-xing; Wu, Hui-fan; Lu, Sheng-yong; Wu, Hai-long; Li, Xiao-dong; Yan, Jian-hua

2016-02-01

Gaseous 1,2-dichlorobenzene (1,2-DCBz) was catalytically decomposed in a fixed-bed catalytic reactor using composite copper-based titanium oxide (CuOx/TiO2) catalysts with different copper ratios. Carbon nanotubes (CNTs) were introduced to produce novel CuOx/TiO2-CNTs catalysts by the sol-gel method. The catalytic performances of CuOx/TiO2 and CuOx/TiO2-CNTs on 1,2-DCBz oxidative destruction under different temperatures (150-350 °C) were experimentally examined and the correlation between catalyst structure and catalytic activity was characterized and the role of oxygen in catalytic reaction was discussed. Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) generation during 1,2-DCBz catalytic oxidation by CuOx/TiO2-CNTs composite catalyst was also examined. Results indicate that the 1,2-DCBz destruction/removal efficiencies of CuOx (4 wt%)/TiO2 catalyst at 150 °C and 350 °C with a GHSV of 3400 h(-1) are 59% and 94% respectively and low-temperature (150 °C) catalytic activity of CuOx/TiO2 on 1,2-DCBz oxidation can be improved from 59 to 77% when CNTs are introduced. Furthermore, oxygen either in catalyst or from reaction atmosphere is indispensible in reaction. The former is offered to activate and oxidize the 1,2-DCBz adsorbed on catalyst, thus can be generally consumed during reaction and the oxygen content in catalyst is observed lost from 39.9 to 35.0 wt% after reacting under inert atmosphere; the latter may replenish the vacancy in catalyst created by the consumed oxygen thus extends the catalyst life and raises the destruction/removal efficiency. The introduction of CNTs also increases the Cu(2+)/Cu(+) ratio, chemisorbed oxygen concentration and surface lattice oxygen binding energy which are closely related with catalytic activity. PCDD/Fs is confirmed to be formed when 1,2-DCBz catalytically oxidized by CuOx/TiO2-CNTs composite catalyst with sufficient oxygen (21%), proper temperature (350 °C) and high concentration of 1,2-DCBz feed (120 ppm

Catalysts for liquid phase oxidation of olefins and sulfur compounds; Catalyseurs pour l'oxydation en phase liquide d'olefines et de composes soufres

Energy Technology Data Exchange (ETDEWEB)

Palomeque Santiago, J.F.

2002-07-01

Several basic, acid and acid-base catalysts were studied for the epoxidation of olefins activated or not and dibenzo-thiophene.Hydrotalcite activation by thermic treatment and in situ re-hydration improves catalytic activity for 2-cyclohexene-1-one and isophorone. Bronsted basic sites were found to be more active than Lewis sites. Total conversion of 2-cyclohexene-1-one is reached in 1.5 h in polar solvents. W{sub 7}O{sub 24}{sup 6-} Iso-poly-anion was exchanged onto a meixnerite by a new preparation method, A meso-porous solid was obtained with good catalytic properties for cyclohexene epoxidation 100% selective to epoxide. W{sub 7}O{sub 24}{sup 6-} and WO{sub 5}{sup 2-} anions and phenyl and dodecyl-phospho-tungstates were grafted on hydrotalcites. Due to the acid-base characteristics of these solid catalysts, cyclohexene yields products of allylic reactions. Mg-La, and Mg-Al-La mixed oxides were synthesized and mixed phases were gotten. Their basic characteristics account for hydrogen peroxide decomposition which prevents DBT oxidation reaction to sulfone. On the contrary, Mg-Al re-hydrated hydrotalcites are very active for this reaction and remove 100% of sulfur compounds in 1 hour. New catalyst W-ZrO{sub 2} were synthesized with high acid properties. stable structure with temperature and high DBT conversion in less than 5 minutes of reaction. These catalytic systems can be applied for hydrocarbon desulfurization of fuels like naphtha, gas oil and kerosene. (author)

N, S co-doped carbon spheres with highly dispersed CoO as non-precious metal catalyst for oxygen reduction reaction

Science.gov (United States)

Chen, Linlin; Guo, Xingpeng; Zhang, Guoan

2017-08-01

It is still a great challenge in preparing non-precious metal catalysts with high activity and long-term stability to substitute for precious metal catalysts for oxygen reduction reaction (ORR) in fuel cells. Herein, we report a novel and facile catalyst-N, S co-doped carbon spheres with highly dispersed CoO (CoO@NS-CSs), where biomass glucose spheres act as carbon precursor and H2S, NH3 derived from the decomposition of thiourea not only provide N, S sources but also can etch carbon spheres to produce nanoporous structure. CoO@NS-CSs catalyst exhibits excellent ORR activity with a high onset potential of 0.946 V vs. RHE (reversible hydrogen electrode) and a half-wave potential of 0.821 V vs. RHE through a four-electron pathway in alkaline solution, which is comparable to commercial Pt/C catalyst (onset potential: 0.926 V vs. RHE, half-wave potential: 0.827 V vs. RHE). Furthermore, both the long-term stability and methanol-tolerance of CoO@NS-CSs catalyst are superior to those of commercial Pt/C catalyst. The excellent ORR performance of CoO@NS-CSs catalyst can be attributed to its micro-mesopore structure, high specific surface area (667 m2 g-1), and highly dispersed CoO. This work manifests that the obtained CoO@NS-CSs catalyst is promising to be applied to fuel cells.

Influence of Pd-precursor on the acetoxylation activity of Pd-Sb/TiO{sub 2} catalysts

Energy Technology Data Exchange (ETDEWEB)

Ben-homeid, A. [Benghazi Univ. (Libyan Arab Jamahiriya). Chemistry Dept.; Kalevaru, V.N.; Radnik, J.; Luecke, B.; Martin, A. [Leibniz-Institut fuer Katalyse e.V. an der Universitaet Rostock (Germany)

2013-11-01

The impact of palladium precursors (e.g. chloride-PdCl{sub 2}; acetate-Pd(OAc){sub 2}; nitrate-Pd(NO{sub 3}){sub 2}) on the catalytic properties of Pd-Sb/TiO{sub 2} catalysts used for acetoxylation of toluene has been investigated. The catalysts were characterized by different techniques such as N{sub 2}-adsorption (BET-surface area and pore volume), XRD, TEM, CO-Chemisorption and XPS for better understanding of the catalytic properties of the catalysts. The acetate and nitrate-type precursors exhibited higher surface areas, pore volumes and higher dispersion of Pd, but displayed poor performance compared to chloride precursor. TEM analysis indicated that the size of Pd particles depended upon the nature of Pd-precursor. Among the three, chloride precursor exhibited bigger Pd particles. XPS results revealed that all the fresh catalysts irrespective of Pd-precursor contained Pd in oxidized state (i.e. Pd{sup +2}), while in the spent catalysts such oxidized Pd species were reduced. The catalytic performance was found to depend strongly on the nature of precursor used. Among the three, the catalysts prepared from chloride-type precursor showed much higher overall catalytic activity (68%) than those of nitrate and/or acetate type precursors. Moreover, these two precursors (acetate and nitrate) gave higher total oxidation products due to oxidative decomposition of mainly acetic acid. Furthermore, the catalyst prepared from Cl-precursor revealed easy deactivation due to coke deposition and also due to loss of Pd in the near-surface-region. (orig.)

FY 1980 Report on results of Sunshine Project. Research and development of coal liquefaction techniques (Development of direct hydrogenation type liquefaction plant and researches on liquefaction reactions in the presence of iron-based catalyst); 1980 nendo sekitan ekika gijutsu no kenkyu kaihatsu, chokusetsu suiten ekika plant no kaihatsu seika hokokusho. Tetsukei shokubai ni yoru ekika hanno no kenkyu

Energy Technology Data Exchange (ETDEWEB)

NONE

1981-03-01

This program is aimed at development of iron-based catalyst suited for direct hydrogenation type coal liquefaction by elucidating the effects of the catalyst on the liquefaction reactions. The iron-based catalyst seems to act as the radical stabilizer rather than the reaction promoter, because the increased quantity of the catalyst and increased H{sub 2} pressure share the common pattern rather than the catalyst enhances the activity, which is associated with increased reaction temperature or residence time. This is more notably observed when the coal species is changed to brown coal. In other words, recombination of the decomposition products by polycondensation is accelerated in the presence of the catalyst in decomposition of brown coal from bituminous coal, with the result that the catalyst effects are more notably observed. Whether this results from difference in age between brown coal and bituminous coal or content of specific types of ashes should be elucidated, because this point is considered to deeply relate to eventual development of the liquefaction reaction system. The FY 1980 program includes the primary screening of different types of iron compounds and tests of some iron-metal-based catalysts. (NEDO)

Influence of Temperature and Catalyst on the Decomposition of Potassium Chlorate in a Simple DTA-Apparatus.

Science.gov (United States)

Wiederholt, Erwin

1983-01-01

DTA is a technique in which the temperature difference between sample/reference is measured as a function of temperature, while both are subject to a controlled temperature program. Use of a simple DTA-apparatus in demonstrating catalytic effects of manganese dioxide and aluminum oxide on decomposition temperature of potassium chlorate is…

Commercial- and whitewashing-grade limestone as a heterogeneous catalyst for synthesis of fatty acid methyl esters from used frying oil (UFO)

Energy Technology Data Exchange (ETDEWEB)

Agrawal, Shweta; Singh, Bhaskar; Sharma, Yogesh C. [Banaras Hindu University, Department of Applied Chemistry, Institute of Technology, Varanasi (India); Frometa, Amado Enrique N. [Universidad Tecnologica de Izucar de Matamoros, Puebla (Mexico)

2012-12-15

Commercial-grade limestone used in whitewashing which is a low-cost material has been used as a catalyst for the synthesis of fatty acid methyl esters. The catalyst was characterized by differential thermal analysis/thermogravimetric analysis, X-ray diffraction, and Fourier transform infrared spectroscopy for the study of its physicochemical nature. The catalyst was calcined at 900 C for 2.5 h for the decomposition of calcium carbonate to calcium oxide. The catalyst was further activated by dissolving 1.5 wt% of catalyst in 30 ml methanol (7.5:1, methanol to used frying oil molar ratio) and stirred at 25 C for 1 h on a magnetic stirrer. The transesterification reaction was performed using calcium oxide as a catalyst and then with the ''activated calcium oxide.'' The conversion obtained was 94.4 % with calcium oxide and was found to be lower for the ''activated calcium oxide'' (i.e., 87.36 %). The conversion increased to 96.8 % on increasing the catalyst amount to 2.0 wt% in 5 h. A high yield (>95 %) of fatty acid methyl esters was observed when either calcium oxide or ''activated calcium oxide'' was taken as catalyst. The catalytic activity of calcium oxide obtained from low-grade limestone has been found to be comparable with the laboratory-grade CaO. (orig.)

Constrained Geometry Organotitanium Catalysts Supported on Nanosized Silica for Ethylene (co)Polymerization.

Science.gov (United States)

Li, Kuo-Tseng; Wu, Ling-Huey

2017-05-05

Supported olefin polymerization catalysts can prevent reactor-fouling problems and produce uniform polymer particles. Constrained geometry complexes (CGCs) have less sterically hindered active sites than bis-cyclopentadienyl metallocene catalysts. In the literature, micrometer-sized silica particles were used for supporting CGC catalysts, which might have strong mass transfer limitations. This study aims to improve the activity of supported CGC catalysts by using nanometer-sized silica. Ti[(C₅Me₄)SiMe₂(N t Bu)]Cl₂, a "constrained-geometry" titanium catalyst, was supported on MAO-treated silicas (nano-sized and micro-sized) by an impregnation method. Ethylene homo-polymerization and co-polymerization with 1-octene were carried out in a temperature range of 80-120 °C using toluene as the solvent. Catalysts prepared and polymers produced were characterized. For both catalysts and for both reactions, the maximum activities occurred at 100 °C, which is significantly higher than that (60 °C) reported before for supported bis-cyclopentadienyl metallocene catalysts containing zirconium, and is lower than that (≥140 °C) used for unsupported Ti[(C₅Me₄)SiMe₂(N t Bu)]Me₂ catalyst. Activities of nano-sized catalyst were 2.6 and 1.6 times those of micro-sized catalyst for homopolymerization and copolymerization, respectively. The former produced polymers with higher crystallinity and melting point than the latter. In addition, copolymer produced with nanosized catalyst contained more 1-octene than that produced with microsized catalyst.

Hydrogen production by electrochemical decomposition of formic acid via solid polymer electrolyte

Energy Technology Data Exchange (ETDEWEB)

Kilic, Ebru Oender [KOSGEB Bursa Business Development Center, Besevler Kucuk Sanayi Sitesi 16149 Nilufer/Bursa (Turkey); Koparal, Ali Savas; Oeguetveren, Uelker Bakir [Anadolu University, Iki Eylul Campus, Applied Research Center for Environmental Problems 26555 Eskisehir (Turkey); Anadolu University, Iki Eylul Campus, Department of Environmental Engineering, 26555 Eskisehir (Turkey)

2009-01-15

The aim of this work is to investigate the feasibility of simultaneous hydrogen production by electrochemical decomposition of formic acid via solid polymer electrolyte (SPE) in an electrochemical reactor. Titanium oxide coated with iridium oxide as anode and carbon fibre with Pt catalyst as cathode were used in the experiments. Effects of applied current density, flow rates and temperature of formic acid solution, concentration of supporting electrolyte and pH of the solution on performance of the process have been investigated. The effect of membrane thickness has also been examined. The results suggest that electrolysis using SPE is a promising method for the treatment of organic pollutants. Hydrogen with purity of 99.999% at ambient temperature by using carbon fibre cathode with Pt catalyst can be produced simultaneously and COD removal efficiency of 95% has been achieved not requiring any chemical addition and temperature increase. Also complete electrochemical oxidation of formic acid at the original pH to CO{sub 2} and H{sub 2}O without production of intermediate has been proved by HPLC analysis. (author)

Decomposition techniques

Science.gov (United States)

Chao, T.T.; Sanzolone, R.F.

1992-01-01

Sample decomposition is a fundamental and integral step in the procedure of geochemical analysis. It is often the limiting factor to sample throughput, especially with the recent application of the fast and modern multi-element measurement instrumentation. The complexity of geological materials makes it necessary to choose the sample decomposition technique that is compatible with the specific objective of the analysis. When selecting a decomposition technique, consideration should be given to the chemical and mineralogical characteristics of the sample, elements to be determined, precision and accuracy requirements, sample throughput, technical capability of personnel, and time constraints. This paper addresses these concerns and discusses the attributes and limitations of many techniques of sample decomposition along with examples of their application to geochemical analysis. The chemical properties of reagents as to their function as decomposition agents are also reviewed. The section on acid dissolution techniques addresses the various inorganic acids that are used individually or in combination in both open and closed systems. Fluxes used in sample fusion are discussed. The promising microwave-oven technology and the emerging field of automation are also examined. A section on applications highlights the use of decomposition techniques for the determination of Au, platinum group elements (PGEs), Hg, U, hydride-forming elements, rare earth elements (REEs), and multi-elements in geological materials. Partial dissolution techniques used for geochemical exploration which have been treated in detail elsewhere are not discussed here; nor are fire-assaying for noble metals and decomposition techniques for X-ray fluorescence or nuclear methods be discussed. ?? 1992.

Catalyst. Volume 10, Number 3, Spring 2009

Science.gov (United States)

Ryan, Barbara E., Ed.

2009-01-01

"Catalyst" is a publication of the U.S. Department of Education's Higher Education Center for Alcohol and Other Drug Abuse and Violence Prevention. This issue contains the following articles: (1) The National Study of Student Hazing Initial Findings; (2) The Social Norms Marketing Research Project--An Update; (3) Message From William…

Studies on recycling and utilization of spent catalysts. Preparation of active hydrodemetallization catalyst compositions from spent residue hydroprocessing catalysts

Energy Technology Data Exchange (ETDEWEB)

Marafi, Meena; Stanislaus, Antony [Petroleum Refining Department, Petroleum Research and Studies Center, Kuwait Institute for Scientific Research, P.O. Box 24885, Safat (Kuwait)

2007-02-15

Spent catalysts form a major source of solid wastes in the petroleum refining industries. Due to environmental concerns, increasing emphasis has been placed on the development of recycling processes for the waste catalyst materials as much as possible. In the present study the potential reuse of spent catalysts in the preparation of active new catalysts for residual oil hydrotreating was examined. A series of catalysts were prepared by mixing and extruding spent residue hydroprocessing catalysts that contained C, V, Mo, Ni and Al{sub 2}O{sub 3} with boehmite in different proportions. All prepared catalysts were characterized by chemical analysis and by surface area, pore volume, pore size and crushing strength measurements. The hydrodesulfurization (HDS) and hydrodemetallization (HDM) activities of the catalysts were evaluated by testing in a high pressure fixed-bed microreactor unit using Kuwait atmospheric residue as feed. A commercial HDM catalyst was also tested under similar operating conditions and their HDS and HDM activities were compared with that of the prepared catalysts. The results revealed that catalyst prepared with addition of up to 40 wt% spent catalyst to boehmite had fairly high surface area and pore volume together with large pores. The catalyst prepared by mixing and extruding about 40 wt% spent catalyst with boehmite was relatively more active for promoting HDM and HDS reactions than a reference commercial HDM catalyst. The formation of some kind of new active sites from the metals (V, Mo and Ni) present in the spent catalyst is suggested to be responsible for the high HDM activity of the prepared catalyst. (author)

Graphene supported heterogeneous catalysts for Li–O{sub 2} batteries

Energy Technology Data Exchange (ETDEWEB)

Alaf, M., E-mail: mirac.alaf@bilecik.edu.tr [Bilecik Seyh Edebali University, Engineering Faculty, Department of Metallurgy and Materials Engineering, Gulumbe Campus, Bilecik 11210 (Turkey); Tocoglu, U.; Kartal, M.; Akbulut, H. [Sakarya University, Engineering Faculty, Department of Metallurgy and Materials Engineering, Esentepe Campus, Sakarya 54187 (Turkey)

2016-09-01

Graphical abstract: - Highlights: • Free-standing and flexible electrodes were prepared for Li–air batteries. • α-MnO{sub 2} nanorods, Pt nanoparticles and graphene were used. • α-MnO{sub 2} and Pt catalyst improved OER/ORR kinetics. - Abstract: In this study production and characterization of free-standing and flexible (i) graphene, (ii) α-MnO{sub 2}/graphene, (iii) Pt/graphene (iv) α-MnO{sub 2}/Pt/graphene composite cathodes for Li–air batteries were reported. Graphene supported heterogeneous catalysts were produced by a facile method. In order to prevent aggregation of graphene sheets and increase not only interlayer distance but also surface area, a trace amount multi-wall carbon nano tube (MWCNT) was introduced to the composite structure. The obtained composite catalysts were characterized by SEM, X-ray diffraction, N{sub 2} adsorption–desorption analyze and Raman spectroscopy. The electrochemical characterization tests including galvanostatic charge/discharge and electrochemical impedance spectroscopy (EIS) measurement of catalyst were carried out by using an ECC-Air test cell. These highly active graphene supported heterogeneous composite catalysts provide competitive properties relative to other catalyst materials for Li–air batteries.

Fischer-Tropsch Cobalt Catalyst Activation and Handling Through Wax Enclosure Methods

Science.gov (United States)

Klettlinger, Jennifer L. S.; Yen, Chia H.; Nakley, Leah M.; Surgenor, Angela D.

2016-01-01

Fischer-Tropsch (F-T) synthesis is considered a gas to liquid process which converts syn-gas, a gaseous mixture of hydrogen and carbon monoxide, into liquids of various hydrocarbon chain length and product distributions. Cobalt based catalysts are used in F-T synthesis and are the focus of this paper. One key concern with handling cobalt based catalysts is that the active form of catalyst is in a reduced state, metallic cobalt, which oxidizes readily in air. In laboratory experiments, the precursor cobalt oxide catalyst is activated in a fixed bed at 350 ?C then transferred into a continuous stirred tank reactor (CSTR) with inert gas. NASA has developed a process which involves the enclosure of active cobalt catalyst in a wax mold to prevent oxidation during storage and handling. This improved method allows for precise catalyst loading and delivery into a CSTR. Preliminary results indicate similar activity levels in the F-T reaction in comparison to the direct injection method. The work in this paper was supported by the NASA Fundamental Aeronautics Subsonics Fixed Wing Project.

Study of Supported Nickel Catalysts Prepared by Aqueous Hydrazine Method. Hydrogenating Properties and Hydrogen Storage: Support Effect. Silver Additive Effect

International Nuclear Information System (INIS)

Wojcieszak, R.

2006-06-01

We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports (γ-Al 2 O 3 , amorphous or crystallized SiO 2 , Nb 2 O 5 , CeO 2 and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N 2 , FTIR and FTIR-Pyridine, TEM, STEM, EDS, H 2 -TPR, H 2 -adsorption, H 2 -TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO 2 or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

Catalysts, methods of making catalysts, and methods of use

KAUST Repository

Renard, Laetitia; El Eter, Mohamad; Caps, Valerie; Basset, Jean-Marie

2014-01-01

Embodiments of the present disclosure provide for catalysts, methods of making catalysts, methods of using catalysts, and the like. In an embodiment, the method of making the catalysts can be performed in a single step with a metal nanoparticle precursor and a metal oxide precursor, where a separate stabilizing agent is not needed.

Catalysts, methods of making catalysts, and methods of use

KAUST Repository

Renard, Laetitia

2014-03-06

Embodiments of the present disclosure provide for catalysts, methods of making catalysts, methods of using catalysts, and the like. In an embodiment, the method of making the catalysts can be performed in a single step with a metal nanoparticle precursor and a metal oxide precursor, where a separate stabilizing agent is not needed.

Nature of nitrogen specie in coke and their role in NOx formation during FCC catalyst regeneration

International Nuclear Information System (INIS)

Babich, I.V.; Seshan, K.; Lefferts, L.

2005-01-01

NO x emission during the regeneration of coked fluid catalytic cracking (FCC) catalysts is an environmental problem. In order to follow the route to NO x formation and try to find ways to suppress it, a coked industrial FCC catalyst has been prepared using model N-containing compounds, e.g., pyridine, pyrrole, aniline and hexadecane-pyridine mixture. Nitrogen present in the FCC feed is incorporated as polyaromatic compounds in the coke deposited on the catalyst during cracking. Its functionality has been characterized using XPS. Nitrogen specie of different types, namely, pyridine, pyrrolic or quaternary-nitrogen (Q-N) have been discriminated. Decomposition of the coke during the catalyst regeneration (temperature programmed oxidation (TPO) and isothermal oxidation) has been monitored by GC and MS measurements of the gaseous products formed. The pyrrolic- and pyridinic-type N specie, present more in the outer coke layers, are oxidized under conditions when still large amount of C or CO is available from coke to reduced NO x formed to N 2 . ''Q-N'' type species are present in the inner layer, strongly adsorbed on the acid sites on the catalyst. They are combusted last during regeneration. As most of the coke is already combusted at this point, lack of reductants (C, CO, etc.) results in the presence of NO x in the tail gas

Catalytic N₂O decomposition and reduction by NH₃ over Fe/Beta and Fe/SSZ-13 catalysts

Energy Technology Data Exchange (ETDEWEB)

Wang, Aiyong; Wang, Yilin; Walter, Eric D.; Kukkadapu, Ravi K.; Guo, Yanglong; Lu, Guanzhong; Weber, Robert S.; Wang, Yong; Peden, Charles H. F.; Gao, Feng

2018-02-01

Fe/zeolites are important N₂O abatement catalysts, efficient in direct N₂O decomposition and (selective) catalytic N₂O reduction. In this study, Fe/Beta and Fe/SSZ-13 were synthesized via solution ion-exchange and used to catalyze these two reactions. Nature of the Fe species was probed with UV-vis, Mössbauer and EPR spectroscopies and H2-TPR. The characterizations collectively indicate that isolated and dinuclear Fe sites dominate in Fe/SSZ-13, whereas Fe/Beta contains higher concentrations of oligomeric Fe_xO_y species. H₂-TPR results suggest that Fe-O interactions are weaker in Fe/SSZ-13, as evidenced by the lower reduction temperatures and higher extents of autoreduction during high-temperature pretreatments in inert gas. Kinetic measurements show that Fe/SSZ-13 has higher activity in catalytic N₂O decomposition, thus demonstrating a positive correlation between activity and Fe-O binding, consistent with O₂ desorption being rate-limiting for this reaction. However, Fe/Beta was found to be more active in catalyzing N₂O reduction by NH₃. This indicates that larger active ensembles (i.e., oligomers) are more active for this reaction, consistent with the fact that both N₂O and NH₃ need to be activated in this case. The authors from PNNL gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle. Aiyong Wang gratefully acknowledges the China Scholarship Council for the Joint-Training Scholarship Program with the Pacific

PHOTOCATALYTIC DECOMPOSITION OF GASEOUS TOLUENE BY TIO2 NANOPARTICLES COATED ON ACTIVATED CARBON

Directory of Open Access Journals (Sweden)

A. Rezaee ، Gh. H. Pourtaghi ، A. Khavanin ، R. Sarraf Mamoory ، M. T. Ghaneian ، H. Godini

2008-10-01

Full Text Available Volatile organic compounds are considered as a group of major environmental pollutants and toluene is recognized as one of the representatives. In this research, the photocatalytic activity for toluene removal was studied over TiO2 nanoparticles embeded on activated carbon. Laboratory-scale experiments were conducted in a fixed-bed reactor equipped with 4 w and 8 w UV lamps (peak wavelength at 365 nm to determine the oxidation rates of toluene. The photocatalyst was extensively characterized by means of X- ray diffraction and scan electronmicroscopy. Experiments were conducted under general laboratory temperature (25ºC±2 while the irradiation was provided by the UV lamps. The dependence of the reaction rate on light intensity as well as the deactivation of the catalyst were determined. The results indicated that the rate of the photocatalytic process increased with increasing the intensity of UV irradiation. Using the UV-A lamps, the decomposition rate of toluene was 98%. The stabilized photocatalyst presented remarkable stability (no deactivation and excellent repeatability. The catalyst could be regenerated by UV irradiation in the absence of gas phase. The control experiments confirmed that the photocatalytic effects of toluene onto the TiO2/activated carbon catalysts in the dark conditions were negligible. Reproducibility tests proved that the photocatalytic activity of the photocatalyst remains intact even after several experiments of new added toluene quantities. The study demonstrated that the TiO2/activated carbon catalyst may be a practical and promising way to degrade the toluene under ultraviolet irradiation.

Titania and zirconia binary oxides as catalysts for total oxidation of ethyl acetate and methanol decomposition

Czech Academy of Sciences Publication Activity Database

Tsoncheva, T.; Mileva, A.; Issa, G.; Dimitrov, M.; Kovacheva, D.; Henych, Jiří; Kormunda, M.; Scotti, N.; Slušná, Michaela; Tolasz, Jakub; Štengl, Václav

2018-01-01

Roč. 6, č. 2 (2018), s. 2540-2550 ISSN 2213-3437 Grant - others:AV ČR(CZ) BAS-17-13 Program:Bilaterální spolupráce Institutional support: RVO:61388980 Keywords : Effect of preparation procedure * Ethyl acetate oxidation * Methanol decomposition * Titania-zirconia binary oxides Subject RIV: CA - Inorganic Chemistry OBOR OECD: Inorganic and nuclear chemistry

Deactivation-resistant catalyst for selective catalyst reduction of NOx

DEFF Research Database (Denmark)

2011-01-01

The present invention relates to a catalyst for selective catalytic reduction of NOx in alkali metal containing flue gas using ammonia as reductant, the catalyst comprising a surface with catalytically active sites, wherein the surface is at least partly coated with a coating comprising at least...... one metal oxide. In another aspect the present invention relates to the use of said catalyst and to a method of producing said catalyst. In addition, the present invention relates to a method of treating an catalyst for conferring thereon an improved resistance to alkali poisoning....

Fe-N-C catalyst modified graphene sponge as a cathode material for lithium-oxygen battery

International Nuclear Information System (INIS)

Yu, Ling; Shen, Yue; Huang, Yunhui

2014-01-01

Highlights: • Hydrothermally-synthesized graphene sponge is excellent skeleton of Li-O 2 cathode. • Fe-N-C catalyst loaded on GS was attained via pyrolysis of FePc and GS composites. • High capacity and good cyclability were achieved with Fe-N-GS air electrode. • The synergy of porous structure and catalytic activity leads to the high performance. - Abstract: The cathode of a lithium-oxygen battery needs the synergism of a porous conducting material and a catalyst to facilitate the formation and decomposition of lithium peroxide. Here we introduce a graphene sponge (GS) modified with Fe-N-C catalyst for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). The porous, 3-dimensional conductive and free standing nature of the graphene sponge makes it become excellent skeleton of cathode for lithium-oxygen battery. The Fe-N-C catalyst nanoparticles dispersed uniformly on the graphene sheets show excellent catalytic reactivity in both discharge and charge processes. This kind of composite material greatly improves the capacity and cyclability of the lithium-oxygen battery. With dimethyl sulphoxide as electrolyte, the capacity reaches 6762 mAh g −1 which is twice of the pure graphene sponge. In addition, the cell containing Fe-N-GS air electrode exhibits stable cyclic performance and effective reduction of charge potential plateau, indicating that Fe-N-GS is promising as an OER catalyst in rechargeable lithium-air batteries

Degradation reaction of Diazo reactive black 5 dye with copper (II) sulfate catalyst in thermolysis treatment.

Science.gov (United States)

Lau, Yen-Yie; Wong, Yee-Shian; Ang, Tze-Zhang; Ong, Soon-An; Lutpi, Nabilah Aminah; Ho, Li-Ngee

2018-03-01

The theme of present research demonstrates performance of copper (II) sulfate (CuSO 4 ) as catalyst in thermolysis process to treat reactive black 5 (RB 5) dye. During thermolysis without presence of catalyst, heat was converted to thermal energy to break the enthalpy of chemical structure bonding and only 31.62% of color removal. With CuSO 4 support as auxiliary agent, the thermally cleaved molecular structure was further destabilized and reacted with CuSO 4 . Copper ions functioned to delocalize the coordination of π of the lone paired electron in azo bond, C=C bond of the sp 2 carbon to form C-C of the sp 3 amorphous carbon in benzene and naphthalene. Further, the radicals of unpaired electrons were stabilized and RB 5 was thermally decomposed to methyl group. Zeta potential measurement was carried out to analyze the mechanism of RB 5 degradation and measurement at 0 mV verified the critical chemical concentration (CCC) (0.7 g/L copper (II) sulfate), as the maximum 92.30% color removal. The presence of copper (II) sulfate catalyst has remarkably increase the RB 5 dye degradation as the degradation rate constant without catalyst, k 1 is 6.5224 whereas the degradation rate constant with catalyst, k 2 is 25.6810. This revealed the correlation of conversion of thermal energy from heat to break the chemical bond strength, subsequent fragmentation of RB 5 dye molecular mediated by copper (II) sulfate catalyst. The novel framework on thermolysis degradation of molecular structure of RB 5 with respect to the bond enthalpy and interfacial intermediates decomposition with catalyst reaction were determined.

Development of structural characterisation tools for catalysts; Developpement d'outils de caracterisation structurale de catalyseurs

Energy Technology Data Exchange (ETDEWEB)

Lynch, J.

1999-10-01

Because of the diversity of their compositions and structures, and the treatments needed to render them active, heterogeneous catalysts present a major challenge in structural characterisation. Electron microscopy provides textural and structural information at the scale of the individual particle. We have been able to analyse epitaxial relationships between nanometer size particles and their support and to determine which crystal faces are most exposed. Chemical analysis can be carried out on individual particles in a bimetallic catalyst. Limitations of this technique are shown for characterisation of catalysts at the atomic scale or in reactive conditions. Here, global analysis methods based on X-ray absorption and diffraction provide more information. W-ray absorption fine structure analysis has been applied to sub-nanometer size particles in platinum based catalysts to explore interactions between the metal and reactive gases such as hydrocarbons and H{sub 2}S. Differences observed between mono-metallic and bimetallic solids lead to structural models to explain differences in catalyst reactivity. X-ray diffraction, combined with electron microscopy, shows the presence of different forms of extra-framework aluminium is steamed zeolites. Quantification of some these forms has been possible and a study of their reactivity towards different de-aluminating agents has been achieved. Work in progress shows the advantages of a combination of X-ray diffraction and absorption to study decomposition of hydrotalcites to form mixed oxides as well as possibilities in infra-red spectroscopy of adsorbed CO to determine surface sites in Fischer Tropsch catalysts. Use of in-situ analysis cells enables a detailed description of catalyst structure in reactive atmospheres and opens the possibility of correlating structure with catalytic activity. (author)

Carbon-free H2 production from ammonia triggered at room temperature with an acidic RuO2/γ-Al2O3 catalyst.

Science.gov (United States)

Nagaoka, Katsutoshi; Eboshi, Takaaki; Takeishi, Yuma; Tasaki, Ryo; Honda, Kyoko; Imamura, Kazuya; Sato, Katsutoshi

2017-04-01

Ammonia has been suggested as a carbon-free hydrogen source, but a convenient method for producing hydrogen from ammonia with rapid initiation has not been developed. Ideally, this method would require no external energy input. We demonstrate hydrogen production by exposing ammonia and O 2 at room temperature to an acidic RuO 2 /γ-Al 2 O 3 catalyst. Because adsorption of ammonia onto the catalyst is exothermic, the catalyst bed is rapidly heated to the catalytic ammonia autoignition temperature, and subsequent oxidative decomposition of ammonia produces hydrogen. A differential calorimeter combined with a volumetric gas adsorption analyzer revealed a large quantity of heat evolved both with chemisorption of ammonia onto RuO 2 and acidic sites on the γ-Al 2 O 3 and with physisorption of multiple ammonia molecules.

An operando optical fiber UV–vis spectroscopic study of the catalytic decomposition of NO and N2O over Cu-ZSM-5

NARCIS (Netherlands)

Weckhuysen, B.M.; Groothaert, M.H.; Lievens, K.; Leeman, H.; Schoonheydt, R.A.

2003-01-01

The role of the bis(μ-oxo)dicopper core, i.e., [Cu2(μ-O)2]2+, in the decomposition of NO and N2O by the Cu-ZSM-5 zeolite has been studied with combined operando UV–vis monitoring of the catalyst and on-line GC analysis. An optical fiber was mounted on the outer surface of the quartz wall of the

More active and sulfur resistant bimetallic Pd-Ni catalysts

Energy Technology Data Exchange (ETDEWEB)

Betti, Carolina; Carrara, Nicolás; Badano, Juan; Lederhos, Cecilia; Vera, Carlos; Quiroga, Mónica, E-mail: mquiroga@fiq.unl.edu.ar [Instituto de Investigaciones en Catálisis y Petroquímica, INCAPE (FIQ-UNL, CONICET), Santa Fe (Argentina)

2018-02-15

The influence of the kind of metal precursor and the sequence of impregnation on the properties of Pd-Ni catalysts was evaluated during the test reaction of selective hydrogenation of styrene to ethylbenzene by means of physicochemical characterization. The focus was put on the final hydrogenating activity and the resistance to deactivation by sulfide compounds (thiophene). The used techniques of characterization were ICP, XPS, XDR, TPR, CO chemisorption and TEM. XPS results indicated the presence of different Pd species: Pd{sup δ-}, Pd{sup 0} and Pd{sup δ+}. In the case of the Ni containing catalysts, Ni{sup 0} and NiO species were also detected. These palladium and nickel species would be responsible of the variation of activity and sulfur resistance of the catalysts. NiClPd catalysts had a higher resistance to deactivation by sulfur poisoning. This was associated to a higher concentration of Pd{sup η+}Cl{sub x}O{sub y} species that would prevent the adsorption of thiophene by both steric and electronic effects. It could also be due to the lower concentration of Pd{sup 0} and Ni{sup 0} on these catalysts, as compared to those shown by the PdNiCl catalysts. Both the Pd{sup 0} and Ni{sup 0} species are more prone to poisoning because of their higher electronic availability. (author)

Chromium-based metal-organic framework MIL-101 as a highly effective catalyst in plasma for toluene removal

Science.gov (United States)

Wu, Junliang; Xia, Qibin; Xiao, Jing; Li, Zhong

2017-11-01

Catalytic performance of MIL-101—a type of chromium-based metal-organic frameworks (MOFs)—in a plasma catalysis system for toluene removal was experimentally studied. The MIL-101 was synthesized using a hydrothermal method, and its catalytic performance was compared to two other catalysts, Cr2O3/γ-Al2O3 and γ-Al2O3, in a dielectric barrier discharge (DBD) reactor. Results showed that the presence of a catalyst in plasma changed the voltage and current characteristic substantially, and promoted the performance of the plasma reactor. Among the catalysts, the MIL-101 exhibited a significantly high toluene conversion, which was 20% and 35% higher than Cr2O3/γ-Al2O3 and γ-Al2O3, respectively, under the same testing conditions, as well as higher carbon balance and CO2 selectivity. The analysis of by-products on the surfaces of the catalysts before and after reaction demonstrated that MIL-101 had better resistance towards by-products accumulation compared to Cr2O3/γ-Al2O3 and γ-Al2O3. The loading of MnO x on MIL-101 further promoted its catalytic performance. MIL-101 exhibits attractive catalytic properties as a catalyst in a plasma catalysis system for the decomposition of volatile organic compounds.

Chromium-based metal-organic framework MIL-101 as a highly effective catalyst in plasma for toluene removal

International Nuclear Information System (INIS)

Wu, Junliang; Xia, Qibin; Xiao, Jing; Li, Zhong

2017-01-01

Catalytic performance of MIL-101—a type of chromium-based metal-organic frameworks (MOFs)—in a plasma catalysis system for toluene removal was experimentally studied. The MIL-101 was synthesized using a hydrothermal method, and its catalytic performance was compared to two other catalysts, Cr 2 O 3 / γ -Al 2 O 3 and γ -Al 2 O 3 , in a dielectric barrier discharge (DBD) reactor. Results showed that the presence of a catalyst in plasma changed the voltage and current characteristic substantially, and promoted the performance of the plasma reactor. Among the catalysts, the MIL-101 exhibited a significantly high toluene conversion, which was 20% and 35% higher than Cr 2 O 3 / γ -Al 2 O 3 and γ -Al 2 O 3 , respectively, under the same testing conditions, as well as higher carbon balance and CO 2 selectivity. The analysis of by-products on the surfaces of the catalysts before and after reaction demonstrated that MIL-101 had better resistance towards by-products accumulation compared to Cr 2 O 3 / γ -Al 2 O 3 and γ -Al 2 O 3 . The loading of MnO x on MIL-101 further promoted its catalytic performance. MIL-101 exhibits attractive catalytic properties as a catalyst in a plasma catalysis system for the decomposition of volatile organic compounds. (paper)

Selective Production of Aromatics from 2-Octanol on Zinc Ion-Exchanged MFI Zeolite Catalysts

Directory of Open Access Journals (Sweden)

Masakazu Iwamoto

2015-12-01

Full Text Available The aromatization of 2-octanol derived from castor oil as a byproduct in the formation of sebacic acid was investigated on various zeolite catalysts. Zn ion-exchanged MFI (ZSM-5 zeolites with small silica/alumina ratios and zinc contents of 0.5 to 2.0 wt. % were determined to exhibit good and stable activity for the reaction at 623 to 823 K. The yield of aromatics was 62% at 773 K and the space velocity 350 to 1400 h−1. The temperature and contact time dependences of the product distributions indicated the reaction pathways of 2-octanol→dehydration to 2-octene→decomposition to C5 and C3 compounds→further decomposition to small alkanes and alkenes→aromatization with dehydrogenation. Alcohols with carbon numbers of 5 to 8 exhibited similar distributions of products compared to 2-octanol, while corresponding carbonyl compounds demonstrated different reactivity.

Production of hydrogen with methane decomposition using Ni-Mn/Ce-ZrO{sub 2} catalysts; Produccion de hidrogeno via descomposicion de metano mediante catalizadores de Ni-Mn/Ce-ZrO{sub 2}

Energy Technology Data Exchange (ETDEWEB)

Diaz, C; Hernandez-Pichardo, M L; Valenzuela, M A [Instituto Politecnico Nacional-ESIQIE, Mexico, D.F. (Mexico); Del Angel, P; Montoya de la Fuente, J.A. [Instituto Mexicano del Petroleo, Mexico, D.F. (Mexico)

2009-09-15

The catalytic decomposition of methane makes it possible to obtain CO and CO{sub 2} free hydrogen, which is a desirable characteristic for fuel cell applications. In addition, this method simultaneously obtains diverse carbon nanostructures with a large variety of applications. This work prepared catalysts with different Ni contents supported by Ce-Zr mixed oxides and doped with manganese to promote activity. The supports were synthesized with surfactant-assisted coprecipitation. The Ni and Mn deposits were performed using conventional impregnation for evaluation in the methane decomposition catalyst at 500 degrees Celsius. It was observed that with the incorporation of 1% of Mn into the Ni0 active phase, the conversion of methane into hydrogen and carbon nanostructures increased. The results of reduction at the programmed temperature indicate that the addition of Mn enables the formation of different NiO{sub x} species, increasing dispersion and the degree of reduction to Ni0. Analyses with electron and transmission microscopy show the formation of distinct species of carbon, including nanotubes, nanofibers and concentric onion-like structures, as well as a significant formation of encapsulated Ni0 particles. [Spanish] La descomposicion catalitica de metano permite la obtencion de hidrogeno libre de CO y CO{sub 2}, lo cual es una caracteristica deseable para su aplicacion en celdas de combustible. Ademas, por esta ruta, simultaneamente se obtienen diversas nanoestructuras de carbono con una gran variedad de aplicaciones. En este trabajo se prepararon catalizadores con diferentes contenidos de Ni soportados en oxidos mixtos Ce-Zr y se doparon con manganeso como promotor de actividad. Los soportes se sintetizaron por coprecipitacion asistida por surfactante y el deposito del Ni y del Mn se efectuo por impregnacion convencional para su evaluacion en la descomposicion catalitica de metano a 500 grados centigrados. Se observo que mediante la incorporacion de 1% de Mn a

Coupling molecular catalysts with nanostructured surfaces for efficient solar fuel production

Science.gov (United States)

Jin, Tong

photosensitizers. In Chapter 3, effective coupling of the macrocyclic Co(III) complex with titanium dioxide (TiO¬2) nanoparticles was achieved by two deposition methods. The synthesized hybrid photocatalysts were thoroughly characterized with a variety of techniques. Upon UV light irradiation, photoexcited electrons in TiO2 nanoparticles were transferred to the surface Co(III) catalyst for CO2 reduction. Production of carbon monoxide (CO) from CO2 was confirmed by isotope labeling combined with infrared spectroscopy. Deposition of the Co(III) catalyst through Ti-O-Co linkages was essential for the photo-induced electron transfer and CO2-reduction activity using the hybrid photocatalysts. In Chapter 4, molecular Re(I) and Co(II) catalysts were coupled with silicon-based photoelectrodes, including a silicon nanowire (SiNW) photoelectrode, to achieve photoelectrochemical CO2 reduction. Photovoltages between 300-600 mV were obtained using the molecular catalysts on the silicon photoelectrodes. SiNWs exhibited enhanced properties, including significantly higher photovoltages than a planar silicon photoelectrode, the ability to protect one of the molecular catalysts from photo-induced decomposition, and excellent selectivity towards CO production in CO2 reduction. Recent theoretical and experimental work have demonstrated low-energy, binuclear pathways for CO2-to-CO conversion using several molecular catalysts. In such binuclear pathways, two metal centers work cooperatively to achieve two-electron CO2 reduction. Chapter 5 describes our effort to promote the binuclear pathway by grafting the molecular Co(III) catalyst onto silica surfaces. Different linking strategies were attempted to achieve this goal by planting the surface Co(III) sites in close proximity.

Surface chemistry and catalytic properties of VOX/Ti-MCM-41 catalysts for dibenzothiophene oxidation in a biphasic system

Science.gov (United States)

González, J.; Chen, L. F.; Wang, J. A.; Manríquez, Ma.; Limas, R.; Schachat, P.; Navarrete, J.; Contreras, J. L.

2016-08-01

A series of vanadium oxide supported on Ti-MCM-41 catalysts was synthesized via the incipient impregnation method by varying the vanadia loading from 5 wt% to 10, 15, 20 and 25 wt%. These catalysts were characterized by a variety of advanced techniques for investigating their crystalline structure, textural properties, and surface chemistry information including surface acidity, reducibility, vanadium oxidation states, and morphological features. The catalytic activities of the catalysts were evaluated in a biphasic reaction system for oxidative desulfurization (ODS) of a model diesel containing 300 ppm of dibenzothiophene (DBT) where acetonitrile was used as extraction solvent and H2O2 as oxidant. ODS activity was found to be proportional to the V5+/(V4+ + V5+) values of the catalysts, indicating that the surface vanadium pentoxide (V2O5) was the active phase. Reaction temperature would influence significantly the ODS efficiency; high temperature, i.e., 80 °C, would lead to low ODS reaction due to the partial decomposition of oxidant. All the catalysts contained both Lewis and Brønsted acid sites but the former was predominant. The catalysts with low vanadia loading (5 or 10 wt%V2O5) had many Lewis acid sites and could strongly adsorb DBT molecule via the electron donation/acceptance action which resulted in an inhibition for the reaction of DBT with the surface peroxometallic species. The catalyst with high vanadia loading (25wt%V2O5/Ti-MCM-41) showed the highest catalytic activity and could remove 99.9% of DBT at 60 °C within 60 min.

Structure-Activity Relationship in the N2O Decomposition over Ni-(Mg)-Al and Ni-(Mg)-Mn Mixed Oxides Prepared from Hydrotalcite-like Precursors

Czech Academy of Sciences Publication Activity Database

Obalová, L.; Jirátová, Květa; Kovanda, F.; Valášková, M.; Balabánová, Jana; Pacultová, K.

2006-01-01

Roč. 248, 1-2 (2006), s. 210-219 ISSN 1381-1169 R&D Projects: GA ČR(CZ) GA106/05/0366; GA ČR(CZ) GA104/04/2116 Institutional research plan: CEZ:AV0Z40720504 Keywords : N2O decomposition * mixed oxide catalyst * layered double hydroxides Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 2.511, year: 2006

Hydrogen production using thermocatalytic decomposition of methane on Ni30/activated carbon and Ni30/carbon black.

Science.gov (United States)

Srilatha, K; Viditha, V; Srinivasulu, D; Ramakrishna, S U B; Himabindu, V

2016-05-01

Hydrogen is an energy carrier of the future need. It could be produced from different sources and used for power generation or as a transport fuel which mainly in association with fuel cells. The primary challenge for hydrogen production is reducing the cost of production technologies to make the resulting hydrogen cost competitive with conventional fuels. Thermocatalytic decomposition (TCD) of methane is one of the most advantageous processes, which will meet the future demand, hence an attractive route for COx free environment. The present study deals with the production of hydrogen with 30 wt% of Ni impregnated in commercially available activated carbon and carbon black catalysts (samples coded as Ni30/AC and Ni30/CB, respectively). These combined catalysts were not attempted by previous studies. Pure form of hydrogen is produced at 850 °C and volume hourly space velocity (VHSV) of 1.62 L/h g on the activity of both the catalysts. The analysis (X-ray diffraction (XRD)) of the catalysts reveals moderately crystalline peaks of Ni, which might be responsible for the increase in catalytic life along with formation of carbon fibers. The activity of carbon black is sustainable for a longer time compared to that of activated carbon which has been confirmed by life time studies (850 °C and 54 sccm of methane).

Hydrogen Temperature-Programmed Desorption in Platinum Catalysts: Decomposition and Isotopic Exchange by Spillover Hydrogen of Chemisorbed Ammonia.

NARCIS (Netherlands)

Koningsberger, D.C.; Miller, J.T.; Meyers, B.L.; Barr, M.K.; Modica, F.S.

1996-01-01

H{2}-TPD of Pt/alumina catalysts display multiple hydrogendesorptions. In addition to chemisorbed hydrogen (Peak I) atapproximately 175}o{C, there is a small hydrogen desorption (PeakII) at about 250}o{C and a large, irreversible hydrogen desorption(Peak III) at 450}o{C. The quantity of hydrogen

A DRIFTS study of the partial oxidation of ethanol on Rh catalysts; Estudo da oxidacao parcial do etanol em catalisadores de Rh por DRIFTS

Energy Technology Data Exchange (ETDEWEB)

Oliveira, Raquel Lima; Passos, Fabio Barboza, E-mail: fbpassos@vm.uff.br [Universidade Federal Fluminense (UFF), Niteroi, RJ (Brazil). Departamento de Engenharia Quimica e de Petroleo

2013-09-01

The partial oxidation of ethanol on {gamma}-Al{sub 2}O{sub 3}, CeO{sub 2}, ZrO{sub 2} and Ce{sub x}Zr{sub 1-x}O{sub 2} supported rhodium catalysts was investigated by Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The catalysts were characterized by temperature-programmed reduction (TPR) and cyclohexane dehydrogenation. DRIFTS studies on the partial oxidation of ethanol showed that ethanol is adsorbed dissociatively, through O-H bond breaking, with the formation of ethoxy species, followed by successive dehydrogenation to acetaldehyde and acetyl species. Further oxidation to acetate and carbonate species lead to the formation of CO, CH{sub 4} and H{sub 2} by decomposition. The presence of CeO{sub 2} in the catalysts favored the oxidation steps due to its oxygen storage capacity. (author)

Uranium oxide nanocrystals by microwave-assisted thermal decomposition. Electronic and structural properties

Energy Technology Data Exchange (ETDEWEB)

Leduc, Jennifer; Mathur, Sanjay [Institute of Inorganic Chemistry, University of Cologne (Germany); Pacold, Joseph I.; Shuh, David K. [Chemical Sciences Division, The Glenn T. Seaborg Center, Lawrence Berkeley National Laboratory, Berkeley, CA (United States); Dong, Chung-Li [Department of Physics, Tamkang University, Tamsui, Taiwan (China)

2018-01-17

Uranium oxides have attracted much attention not only in the context of nuclear energy generation but also for their application as pristine catalysts or as supports for other (transition metal) oxides and (precious) metals. Their propensity to adopt high coordination numbers and manifest multiple oxidation states (from +II to +VI) makes them attractive candidates for catalyzed transformation reactions. Herein, we report a new synthesis route to phase-pure, crystalline UO{sub 2} nanoparticles via microwave-assisted decomposition of a molecular uranium(IV) precursor. The electronic structure and optical absorption properties of these nanocrystals were investigated using spectroscopic methods to evaluate their suitability for photo(electro)catalytic applications. (copyright 2018 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Uranium oxide nanocrystals by microwave-assisted thermal decomposition. Electronic and structural properties

International Nuclear Information System (INIS)

Leduc, Jennifer; Mathur, Sanjay; Pacold, Joseph I.; Shuh, David K.; Dong, Chung-Li

2018-01-01

Uranium oxides have attracted much attention not only in the context of nuclear energy generation but also for their application as pristine catalysts or as supports for other (transition metal) oxides and (precious) metals. Their propensity to adopt high coordination numbers and manifest multiple oxidation states (from +II to +VI) makes them attractive candidates for catalyzed transformation reactions. Herein, we report a new synthesis route to phase-pure, crystalline UO 2 nanoparticles via microwave-assisted decomposition of a molecular uranium(IV) precursor. The electronic structure and optical absorption properties of these nanocrystals were investigated using spectroscopic methods to evaluate their suitability for photo(electro)catalytic applications. (copyright 2018 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

An introduction to catalyst

International Nuclear Information System (INIS)

Jeon, Hak Je

1988-11-01

This book explains basic conception of catalyst such as definition, velocity of chemical reaction and velocity of catalyst reaction, absorption with absorption energy and chemical absorption, pore structure with the role of pore and measurement of pore structure, catalyst activity on solid structure, electrical property on catalyst activity, choice and design of catalyst, catalytic reaction with reaction velocity and chemical equilibrium and reaction velocity model, measurement of reaction velocity and material analysis, catalyst for mixed compound, catalyst for solid acid and catalyst for supported metal.

Oxidative degradation of the organometallic iron(II) complex [Fe{bis[3-(pyridin-2-yl)-1H-imidazol-1-yl]methane}(MeCN)(PMe3)](PF6)2: structure of the ligand decomposition product trapped via coordination to iron(II).

Science.gov (United States)

Haslinger, Stefan; Pöthig, Alexander; Cokoja, Mirza; Kühn, Fritz E

2015-12-01

Iron is of interest as a catalyst because of its established use in the Haber-Bosch process and because of its high abundance and low toxicity. Nitrogen-heterocyclic carbenes (NHC) are important ligands in homogeneous catalysis and iron-NHC complexes have attracted increasing attention in recent years but still face problems in terms of stability under oxidative conditions. The structure of the iron(II) complex [1,1'-bis(pyridin-2-yl)-2,2-bi(1H-imidazole)-κN(3)][3,3'-bis(pyridin-2-yl-κN)-1,1'-methanediylbi(1H-imidazol-2-yl-κC(2))](trimethylphosphane-κP)iron(II) bis(hexafluoridophosphate), [Fe(C17H14N6)(C16H12N6)(C3H9P)](PF6)2, features coordination by an organic decomposition product of a tetradentate NHC ligand in an axial position. The decomposition product, a C-C-coupled biimidazole, is trapped by coordination to still-intact iron(II) complexes. Insights into the structural features of the organic decomposition products might help to improve the stability of oxidation catalysts under harsh conditions.

The Reduction Reaction of Dissolved Oxygen in Water by Hydrazine over Platinum Catalyst Supported on Activated Carbon Fiber

Energy Technology Data Exchange (ETDEWEB)

Park, K.K.; Moon, J.S. [Korea Electric Power Research Institute, Taejon (Korea)

1999-07-01

The reduction reaction of dissolved oxygen (DO) by hydrazine was investigated on activated carbon fiber (ACF) and Pt/ACF catalysts using a batch reactor with an external circulating loop. The ACF itself showed catalytic activity and this was further improved by supporting platinum on ACF. The catalytic role platinum is ascribed to its acceleration of hydrazine decomposition, based on electric potential and current measurements as well as the kinetic study. (author). 15 refs., 13 figs.

Catalytic Decomposition of Nitrous Oxide over Catalysts Prepared from Co/Mg-Mn/Al Hydrotalcite-like Compounds

Czech Academy of Sciences Publication Activity Database

Obalová, L.; Jirátová, Květa; Kovanda, F.; Pacultová, K.; Lacný, Z.; Mikulová, Zuzana

2005-01-01

Roč. 60, 3-4 (2005), s. 289-297 ISSN 0926-3373 R&D Projects: GA ČR(CZ) GA106/05/0366; GA ČR(CZ) GA104/04/2116; GA ČR(CZ) GA106/02/0523 Institutional research plan: CEZ:AV0Z40720504 Keywords : decomposition of nitrous oxide * hydrotalcite-like compounds Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 3.809, year: 2005

Implementation of domain decomposition and data decomposition algorithms in RMC code

International Nuclear Information System (INIS)

Liang, J.G.; Cai, Y.; Wang, K.; She, D.

2013-01-01

The applications of Monte Carlo method in reactor physics analysis is somewhat restricted due to the excessive memory demand in solving large-scale problems. Memory demand in MC simulation is analyzed firstly, it concerns geometry data, data of nuclear cross-sections, data of particles, and data of tallies. It appears that tally data is dominant in memory cost and should be focused on in solving the memory problem. Domain decomposition and tally data decomposition algorithms are separately designed and implemented in the reactor Monte Carlo code RMC. Basically, the domain decomposition algorithm is a strategy of 'divide and rule', which means problems are divided into different sub-domains to be dealt with separately and some rules are established to make sure the whole results are correct. Tally data decomposition consists in 2 parts: data partition and data communication. Two algorithms with differential communication synchronization mechanisms are proposed. Numerical tests have been executed to evaluate performance of the new algorithms. Domain decomposition algorithm shows potentials to speed up MC simulation as a space parallel method. As for tally data decomposition algorithms, memory size is greatly reduced

The Enthalpy of Decomposition of Hydrogen Peroxide: A General Chemistry Calorimetry Experiment

Science.gov (United States)

Marzzacco, Charles J.

1999-11-01

A calorimetry experiment involving the catalytic decomposition of aqueous hydrogen peroxide is presented. The experiment is simple, inexpensive, and colorful. In its simplest form, it can be performed in less than one hour; therefore, it is quite suitable for high school labs, which often have time restrictions. The chemicals required are household or commercial 3% H2O2(aq) and 0.50 M Fe(NO3)3(aq). Styrofoam cup calorimeters and thermometers with a range from 20 to 50 oC are also required. Ideally, the thermometers should be precise to 0.01 oC. The temperature of the H2O2 solution is monitored before and after the Fe(NO3)3 catalyst is added. The addition of the catalyst results in a color change and the evolution of heat and bubbles of oxygen. At the conclusion of the reaction, the color of the reaction mixture returns to that of the original Fe(NO3)3 solution. The heat change for the reaction is determined from the temperature change, the specific heat of the solution, and the calorimeter constant. The experimental enthalpy change for the reaction is in excellent agreement with the literature value.

Tin and tin-titanium as catalyst components for reversible hydrogen storage of sodium aluminium hydride

Energy Technology Data Exchange (ETDEWEB)

Qi Jia Fu; Shik Chi Tsang [University of Reading, Reading (United Kingdom). Surface and Catalysis Research Centre, School of Chemistry

2006-10-15

This paper is concerned with the effects of adding tin and/or titanium dopant to sodium aluminium hydride for both dehydrogenation and re-hydrogenation reactions during their reversible storage of molecular hydrogen. Temperature programmed decomposition (TPD) measurements show that the dehydrogenation kinetics of NaAlH{sub 4} are significantly enhanced upon doping the material with 2 mol% of tributyltin hydride, Sn(Bu)3H but the tin catalyst dopant is shown to be inferior than titanium. On the other hand, in this preliminary work, a significant synergetic catalytic effect is clearly revealed in material co-doped with both titanium and tin catalysts which shows the highest reversible rates of dehydrogenation and re-hydrogenation (after their hydrogen depletion). The re-hydrogenation rates of depleted Sn/Ti/NaAlH{sub 4} evaluated at both 9.5 and 140 bars hydrogen are also found to be favourable compared to the Ti/NaAlH{sub 4}, which clearly suggest the importance of the catalyst choice. Basing on these results some mechanistic insights for the catalytic reversible dehydrogenation and re-hydrogenation processes of Sn/Ti/NaAlH{sub 4} are therefore made. 31 refs., 8 figs., 2 tabs.

On factors controlling activity of submonolayer bimetallic catalysts: Nitrogen desorption

Energy Technology Data Exchange (ETDEWEB)

Guo, Wei; Vlachos, Dionisios G., E-mail: vlachos@udel.edu [Center for Catalytic Science and Technology, Catalysis Center for Energy Innovation, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, Delaware 19716 (United States)

2014-01-07

We model N{sub 2} desorption on submonolayer bimetallic surfaces consisting of Co clusters on Pt(111) via first-principles density functional theory-based kinetic Monte Carlo simulations. We find that submonolayer structures are essential to rationalize the high activity of these bimetallics in ammonia decomposition. We show that the N{sub 2} desorption temperature on Co/Pt(111) is about 100 K higher than that on Ni/Pt(111), despite Co/Pt(111) binding N weaker at low N coverages. Co/Pt(111) has substantially different lateral interactions than single metals and Ni/Pt. The lateral interactions are rationalized with the d-band center theory. The activity of bimetallic catalysts is the result of heterogeneity of binding energies and reaction barriers among sites, and the most active site can differ on various bimetallics. Our results are in excellent agreement with experimental data and demonstrate for the first time that the zero-coverage descriptor, used until now, for catalyst activity is inadequate due not only to lacking lateral interactions but importantly to presence of multiple sites and a complex interplay of thermodynamics (binding energies, occupation) and kinetics (association barriers) on those sites.

First-principles study on the initial decomposition process of CH3NH3PbI3

Science.gov (United States)

Xue, Yuanbin; Shan, Yueyue; Xu, Hu

2017-09-01

Hybrid perovskites are promising materials for high-performance photovoltaics. Unfortunately, hybrid perovskites readily decompose in particular under humid conditions, and the mechanisms of this phenomenon have not yet been fully understood. In this work, we systematically studied the possible mechanisms and the structural properties during the initial decomposition process of MAPbI3 (MA = CH3NH3+) using first-principles calculations. The theoretical results show that it is energetically favorable for PbI2 to nucleate and crystalize from the MAPbI3 matrix ahead of other decomposition products. Additionally, the structural instability is an intrinsic property of MAPbI3, regardless of whether the system is exposed to humidity. We find that H2O could facilitate the desorption of gaseous components, acting as a catalyst to transfer the H+ ion. These results provide insight into the cause of the instability of MAPbI3 and may improve our understanding of the properties of hybrid perovskites.

Thermal decomposition of biphenyl (1963); Decomposition thermique du biphenyle (1963)

Energy Technology Data Exchange (ETDEWEB)

Clerc, M [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1962-06-15

The rates of formation of the decomposition products of biphenyl; hydrogen, methane, ethane, ethylene, as well as triphenyl have been measured in the vapour and liquid phases at 460 deg. C. The study of the decomposition products of biphenyl at different temperatures between 400 and 460 deg. C has provided values of the activation energies of the reactions yielding the main products of pyrolysis in the vapour phase. Product and Activation energy: Hydrogen 73 {+-} 2 kCal/Mole; Benzene 76 {+-} 2 kCal/Mole; Meta-triphenyl 53 {+-} 2 kCal/Mole; Biphenyl decomposition 64 {+-} 2 kCal/Mole; The rate of disappearance of biphenyl is only very approximately first order. These results show the major role played at the start of the decomposition by organic impurities which are not detectable by conventional physico-chemical analysis methods and the presence of which accelerates noticeably the decomposition rate. It was possible to eliminate these impurities by zone-melting carried out until the initial gradient of the formation curves for the products became constant. The composition of the high-molecular weight products (over 250) was deduced from the mean molecular weight and the dosage of the aromatic C - H bonds by infrared spectrophotometry. As a result the existence in tars of hydrogenated tetra, penta and hexaphenyl has been demonstrated. (author) [French] Les vitesses de formation des produits de decomposition du biphenyle: hydrogene, methane, ethane, ethylene, ainsi que des triphenyles, ont ete mesurees en phase vapeur et en phase liquide a 460 deg. C. L'etude des produits de decomposition du biphenyle a differentes temperatures comprises entre 400 et 460 deg. C, a fourni les valeurs des energies d'activation des reactions conduisant aux principaux produits de la pyrolyse en phase vapeur. Produit et Energie d'activation: Hydrogene 73 {+-} 2 kcal/Mole; Benzene 76 {+-} 2 kcal/Mole; Metatriphenyle, 53 {+-} 2 kcal/Mole; Decomposition du biphenyle 64 {+-} 2 kcal/Mole; La

Thermal Decomposition of Calcium Perchlorate/Iron-Mineral Mixtures: Implications of the Evolved Oxygen from the Rocknest Eolian Deposit in Gale Crater, Mars

Science.gov (United States)

Bruck, A. M.; Sutter, B.; Ming, D. W.; Mahaffy, P.

2014-01-01

A major oxygen release between 300 and 500 C was detected by the Mars Curiosity Rover Sample Analysis at Mars (SAM) instrument at the Rocknest eolian deposit. Thermal decomposition of perchlorate (ClO4-) salts in the Rocknest samples are a possible explanation for this evolved oxygen release. Releative to Na-, K-, Mg-, and Fe-perchlorate, the thermal decomposition of Ca-perchlorate in laboratory experiments released O2 in the temperature range (400-500degC) closest to the O2 release temperatures observed for the Rocknest material. Furthermore, calcium perchlorate could have been the source of Cl in the chlorinated-hydrocarbons species that were detected by SAM. Different components in the Martian soil could affect the decomposition temperature of calcium per-chlorate or another oxychlorine species. This interaction of the two components in the soil could result in O2 release temperatures consistent with those detected by SAM in the Rocknest materials. The decomposition temperatures of various alkali metal perchlorates are known to decrease in the presence of a catalyst. The objective of this work is to investigate catalytic interactions on calcium perchlorate from various iron-bearing minerals known to be present in the Rocknest material

Plasmonic Ag-pillared rectorite as catalyst for degradation of 2,4-DCP in the H{sub 2}O{sub 2}-containing system under visible light irradiation

Energy Technology Data Exchange (ETDEWEB)

Chen, Yunfang [School of Chemistry and Environment, South China Normal University, Guangzhou 510006, Guangdong (China); Fang, Jianzhang, E-mail: fangjzh@scnu.edu.cn [School of Chemistry and Environment, South China Normal University, Guangzhou 510006, Guangdong (China); Guangdong Technology Research Center for Ecological Management and Remediation of Urban Water System, Guangzhou 510006 (China); Lu, Shaoyou [Shenzhen Center for Disease Control and Prevention, Shenzhen 518055 (China); Wu, Yan; Chen, Dazhi; Huang, Liyan [Institute of Engineering Technology of Guangdong Province, Key Laboratory of Water Environmental Pollution Control of Guangdong Province, Guangzhou 510440 (China); Cheng, Cong; Ren, Lu; Zhu, Ximiao [School of Chemistry and Environment, South China Normal University, Guangzhou 510006, Guangdong (China); Fang, Zhanqiang [School of Chemistry and Environment, South China Normal University, Guangzhou 510006, Guangdong (China); Guangdong Technology Research Center for Ecological Management and Remediation of Urban Water System, Guangzhou 510006 (China)

2015-10-30

Highlights: • The Ag-R catalyst was synthesized via a novel thermal decomposition method. • Ag-R catalyst possessed the synergistic effects of SPR and adsorption capacity. • The degradation of 2,4-DCP was evaluated in Ag-R/H{sub 2}O{sub 2}/visible light system. - Abstract: This study aims at photocatalytic degradation of 2,4-DCP with the assistance of H{sub 2}O{sub 2} in aqueous solution by a composite catalyst of Ag-rectorite. The catalysts were prepared via a novel thermal decomposition method followed after the cation-exchange process. The synthesized nano-materials were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET) surface analyzer, Ultraviolet–visible light (UV–vis) absorption spectra, field-emission scanning electron microscope (FE-SEM) and transmission electron microscope (TEM). The different mechanisms of degradation process with or without visible light irradiation were discussed, respectively. Moreover, the degradation efficiency of 2,4-DCP wastewater under Ag-rectorite/H{sub 2}O{sub 2}/visible light system was investigated by series of experiments, concerning on effects of major operation factors, such as H{sub 2}O{sub 2} dosage and the initial pH value. The highest degradation rate was observed when adding 0.18 mL H{sub 2}O{sub 2} into 50 mL 2,4-DCP solution, and the optimal pH value was 4 for the reaction. Afterwards, total organic carbon (TOC) experiments were carried out to evaluate the mineralization ratio of 2,4-DCP.

Conversion of KCl into KBH4 by Mechano-Chemical Reaction and its Catalytic Decomposition

Science.gov (United States)

Bilen, Murat; Gürü, Metin; Çakanyildirim, Çetin

2017-07-01

Production of KBH4, in the presence of KCl, B2O3 and MgH2 by means of a mechanical reaction and a dehydrogenation kinetic, constitute the main parts of this study. Operating time and reactant ratio are considered as two parameters for the mechanical reaction to obtain the maximum yield. The production process was carried out in a ball milling reactor, and the product residue was purified with ethylene diamine (EDA) and subsequently characterized by Fourier Transform Infrared Spectroscopy (FT-IR) and x-ray Diffraction (XRD) analyses. Optimum time for mechano-chemical treatment and reactant ratio (MgH2/KCl) were obtained as 1000 min and 1.0, respectively. Synthesized and commercial KBH4 were compared by hydrolysis tests in the presence of Co1-xNix/Al2O3 heterogeneous catalyst. Hydrogen generation rates, activation energy and order of the KBH4 decomposition reaction were obtained as 1578 {mL}_{{{{H}}2 }} \\min^{ - 1} {g}_{{catalyst}}^{ - 1}, 39.2 kJ mol-1 and zero order, respectively.

Determination of Trace Anions in Concentrated Hydrogen Peroxide by Direct Injection Ion Chromatography with Conductivity Detection after Pt-Catalyzed On-Line Decomposition

International Nuclear Information System (INIS)

Kim, Do Hee; Lee, Bo Kyung; Lee, Dong Soo

1999-01-01

A method has been developed for the determination of trace anion impurities in concentrated hydrogen peroxide. The method involves on-line decomposition of hydrogen peroxide, ion chromatographic separation and subsequent suppressed-type conductivity detection. H 2 O 2 is decomposed in Pt-catalyst filled Gore-Tex membrane tubing and the resulting aqueous solution containing analytes is introduced to the injection valve of an ion chromatograph for periodic determinations. The oxygen gas evolving within the membrane tubing escapes freely through the membrane wall causing no problem in ion chromatographic analysis. Decomposition efficiency is above 99.99% at a flow rate of 0.4mL/min for a 30% hydrogen peroxide concentration. Analytes are quantitatively retained. The analysis results for several brands of commercial hydrogen peroxides are reported

Synergistic effect of carbon nanofiber/nanotube composite catalyst on carbon felt electrode for high-performance all-vanadium redox flow battery.

Science.gov (United States)

Park, Minjoon; Jung, Yang-jae; Kim, Jungyun; Lee, Ho il; Cho, Jeaphil

2013-10-09

Carbon nanofiber/nanotube (CNF/CNT) composite catalysts grown on carbon felt (CF), prepared from a simple way involving the thermal decomposition of acetylene gas over Ni catalysts, are studied as electrode materials in a vanadium redox flow battery. The electrode with the composite catalyst prepared at 700 °C (denoted as CNF/CNT-700) demonstrates the best electrocatalytic properties toward the V(2+)/V(3+) and VO(2+)/VO2(+) redox couples among the samples prepared at 500, 600, 700, and 800 °C. Moreover, this composite electrode in the full cell exhibits substantially improved discharge capacity and energy efficiency by ~64% and by ~25% at 40 mA·cm(-2) and 100 mA·cm(-2), respectively, compared to untreated CF electrode. This outstanding performance is due to the enhanced surface defect sites of exposed edge plane in CNF and a fast electron transfer rate of in-plane side wall of the CNT.

A novel hydrolysis method to synthesize chromium hydroxide nanoparticles and its catalytic effect in the thermal decomposition of ammonium perchlorate

International Nuclear Information System (INIS)

Li, Ping; Zhou, Zhen; Xu, Hongbin; Zhang, Yi

2012-01-01

Highlights: ► Synthesis of Cr(OH) 3 nanoparticles in Cr 3+ –F − aqueous solution. ► The F − ion tailors coagulated materials, Cr(OH) 3 nanoparticles are obtained. ► Adding nanosized Cr(OH) 3 , AP thermal decomposition temperature decreases to 200 °C. ► The nanosized Cr(OH) 3 catalyzes NH 3 oxidation, accelerating AP thermal decomposition. - Abstract: A procedure for the preparation of spherical Cr(OH) 3 nanoparticles was developed based on the aging of chromium nitrate aqueous solutions in the presence of sodium fluoride, urea, and polyvinylpyrrolidone. Using scanning electron microscopy, transmission electron microscopy, and energy dispersive spectroscopy, the morphological characteristics of Cr(OH) 3 were controlled by altering the molar ratio of fluoride ion to chromium ion, as well as the initial pH and chromium ion concentration. The prepared nanosized Cr(OH) 3 decreased the temperature required to decompose ammonium perchlorate from 450 °C to about 250 °C as the catalyst. The possible catalytic mechanism of the thermal decomposition of ammonium perchlorate was also discussed.

Ruthenium cluster-like chalcogenide as a methanol tolerant cathode catalyst in air-breathing laminar flow fuel cells

International Nuclear Information System (INIS)

Whipple, Devin T.; Jayashree, Ranga S.; Egas, Daniela; Alonso-Vante, Nicolas; Kenis, Paul J.A.

2009-01-01

This paper reports the incorporation of a cluster-like Ru x Se y as a methanol tolerant cathode catalyst in a laminar flow fuel cell. The effect on cell performance of several concentrations of methanol in the cathode stream was investigated for the Ru x Se y catalyst and compared to a conventional platinum catalyst. While the Pt catalyst exhibited up to ∼80% drop in power density, the Ru x Se y catalyst showed no decrease in performance when the cathode was exposed to methanol. At several methanol concentrations the Ru x Se y catalyst performed better than the Pt catalyst. This demonstration of a methanol tolerant catalyst in a laminar flow fuel cell opens up the way for further miniaturization of the cell design and simplification of its operation as the need for an electrolyte stream to prevent fuel crossover has been eliminated.

Impeded solid state reactions and transformations in ceramic catalysts supports and catalysts

Directory of Open Access Journals (Sweden)

Ernő E. Kiss

2012-12-01

Full Text Available Impeded chemical reactions and impeded polymorphous transformation in materials are discussed, as desired effects, for stabilization of ceramic catalyst supports and ceramic based catalysts. This paper gives a short overview about the possibilities of slowing down the aging processes in ceramic catalyst supports and catalysts. Special attention is given to alumina and titania based catalysts.

Report on the achievements in the Sunshine Project in fiscal 1990 on research and development of coal energy. Studies on coal liquefying catalysts and a method for analyzing liquefied oil; 1990 nendo sekitan ekikayo shokubai oyobi ekikayu bunsekiho no kenkyu seika hokokusho

Energy Technology Data Exchange (ETDEWEB)

NONE

1991-03-01

This paper describes the achievements in the Sunshine Project in fiscal 1990 on research of coal liquefying catalysts and a method for analyzing liquefied oil. Regenerating deteriorated hydrogenating catalysts for coal liquefied oil makes the restoration non-reversible because of residual sulfate. Discussions were given on the regenerating mechanisms. It was found that adding Ru enhances activity of an Ni-Mo catalyst for hydrogenating denitrification and hydrogenation. In studying coal liquefying reaction, a basic study was performed to analyze a catalytic mechanism in the hydrogenating decomposition. Sequential lightening reaction process is being analyzed at molecular levels on coal, preasphaltene, asphaltene and oil. Investigations were carried out on hydrogenating denitrification, deoxygenation, ring opening, decomposition mechanism and catalytic action. A study on precision structural analysis has begun on PSU circulating solvent as a NEDO bituminous coal liquefaction supporting technology. In fiscal 1990, a preliminary study was performed to identify the overall image of the composition of the Wandoan coal liquefied oil. Detailed analysis was executed on naphthalenes and their hydrides. This paper also describes composition analysis and reaction analysis by using the GC/MS ion chromatogram method. It also dwells on the study on catalyst utilizing systems. (NEDO)

High-BTU gas production from tar-bearing hot coke oven gas over iron catalyst

Energy Technology Data Exchange (ETDEWEB)

L.Y. Li; K. Morishita; T. Takarada [Gunma University, Gunma (Japan). Department of Biological and Chemical Engineering

2005-07-01

To utilize the tar-bearing hot coke oven gas (the by-product of coke making process) more effectively, a process was developed by converting the hot coke oven gas into a methane rich high-BTU gas over iron-bearing catalysts. The catalytic behaviour of Indonesian limonite ore was mainly discussed. For a reference, a conventional nickel catalyst (Ni/Al{sub 2}O{sub 3}) was employed. Laboratory scale tests were carried out in a two-stage fixed-bed reactor at ambient pressure. A bituminous coal sample was heated at first stage, the volatiles was carried by feed gas and decomposed at second stage. The limonite promoted hydropyrolysis of coal volatiles similar to Ni/Al{sub 2}O{sub 3} catalyst. High yields of total product gas and methane were obtained at 50 vol.% hydrogen atmosphere with a feed gas of 60 ml min{sup -1} hydrogen and 60 ml min{sup -1} nitrogen. After experiments, hydrocarbons heavier than ethane were not observed. Also that, carbon balance was more than 99.8% in coal char, product gases and carbon deposits. It was considered that coal volatiles converted into light gases and carbon almost completely in catalyst bed. Yields of product gas and methane depended upon catalytic temperature. At 923 K, the maximum yield of product gas was achieved at 74.3% for limonite catalyst on carbon balance with methane 83.2 vol.% of the carbonaceous gas products. Comparing with limonite, Fe/Al{sub 2}O{sub 3} and BOF dust samples showed low activities on coal volatiles catalytic decomposition. 21 refs., 5 figs., 3 tabs.

Preparation and characterization of Pt catalysts supported on TiO2 and ZrO2 stabilized with La2O3 for the elimination of nitric oxide

International Nuclear Information System (INIS)

Aguilar V, A.

2001-01-01

The objective of this work is the preparation and characterization of catalytic materials with a platinum base, supported in simple and mixed oxides of titanium (TiO 2 ) and zirconia (ZrO 2 ) which were stabilized with 10 % in mole of lanthanum (La 2 O 3 ), the preparation technique of the supports is the one of precipitation, additioning a nominal charge of 1% in weight of active phase (Pt) by means of the impregnation method by conventional wetting. All the solids were calcinated at 500 Centigrade and subsequently reduced to the same temperature in air and hydrogen flow respectively. Their characterization was applying the techniques such as: Thermal gravimetric analysis (TGA), Differential scanning calorimetry (DSC), Surface area (BET), X-ray diffraction (XRD), Scanning electron microscopy (SEM), Decomposition of 2-propanol, Catalytic activity and selectivity. The application of these techniques allow to define and to explain the influence of the preparation method and of the thermal treatments to which were submitted the catalysts, in special the Surface area, X-ray diffraction and Scanning electron microscopy which demonstrated in evidence the morphologic structure and of crystalline phases present in the catalysts under study. The decomposition of 2-propanol, catalytic activity and selectivity show the supports and catalysts skill for the determination of acid or base sites, moreover of the selective reduction of nitric oxide respectively, the results seem to indicate that the preparation technique, precursors and the thermal treatments to what these materials were submitted have an influence on the catalyst and by consequence in the reduction reaction of nitric oxide. (Author)

Catalyst support structure, catalyst including the structure, reactor including a catalyst, and methods of forming same

Science.gov (United States)

Van Norman, Staci A.; Aston, Victoria J.; Weimer, Alan W.

2017-05-09

Structures, catalysts, and reactors suitable for use for a variety of applications, including gas-to-liquid and coal-to-liquid processes and methods of forming the structures, catalysts, and reactors are disclosed. The catalyst material can be deposited onto an inner wall of a microtubular reactor and/or onto porous tungsten support structures using atomic layer deposition techniques.

The use of ultrasmall iron(0) nanoparticles as catalysts for the selective hydrogenation of unsaturated C-C bonds.

Science.gov (United States)

Kelsen, Vinciane; Wendt, Bianca; Werkmeister, Svenja; Junge, Kathrin; Beller, Matthias; Chaudret, Bruno

2013-04-28

The performance of well-defined ultrasmall iron(0) nanoparticles (NPs) as catalysts for the selective hydrogenation of unsaturated C-C and C=X bonds is reported. Monodisperse iron nanoparticles of about 2 nm size are synthesized by the decomposition of {Fe(N[Si(CH3)3]2)2}2 under dihydrogen. They are found to be active for the hydrogenation of various alkenes and alkynes under mild conditions and weakly active for C=O bond hydrogenation.

Radiation decomposition of technetium-99m radiopharmaceuticals

International Nuclear Information System (INIS)

Billinghurst, M.W.; Rempel, S.; Westendorf, B.A.

1979-01-01

Technetium-99m radiopharmaceuticals are shown to be subject to autoradiation-induced decomposition, which results in increasing abundance of pertechnetate in the preparation. This autodecomposition is catalyzed by the presence of oxygen, although the removal of oxygen does not prevent its occurrence. The initial appearance of pertechnetate in the radiopharmaceutical is shown to be a function of the amount of radioactivity, the quantity of stannous ion used, and the ratio of /sup 99m/Tc to total technetium in the preparation

Process Intensification of Alkynol Semihydrogenation in a Tube Reactor Coated with a Pd/ZnO Catalyst

Directory of Open Access Journals (Sweden)

Nikolay Cherkasov

2017-11-01

Full Text Available Semihydrogenation of 2-methyl-3-butyn-2-ol (MBY was studied in a 5 m tube reactor wall-coated with a 5 wt% Pd/ZnO catalyst. The system allowed for the excellent selectivity towards the intermediate alkene of 97.8 ± 0.2% at an ambient H2 pressure and a MBY conversion below 90%. The maximum alkene yield reached 94.6% under solvent-free conditions and 96.0% in a 30 vol % MBY aqueous solution. The reactor stability was studied for 80 h on stream with a deactivation rate of only 0.07% per hour. Such a low deactivation rate provides a continuous operation of one month with only a two-fold decrease in catalyst activity and a metal leaching below 1 parts per billion (ppb. The excellent turn-over numbers (TON of above 105 illustrates a very efficient utilisation of the noble metal inside catalyst-coated tube reactors. When compared to batch operation at 70 °C, the reaction rate in flow reactor can be increased by eight times at a higher reaction temperature, keeping the same product decomposition of about 1% in both cases.

Nanosheet Supported Single-Metal Atom Bifunctional Catalyst for Overall Water Splitting.

Science.gov (United States)

Ling, Chongyi; Shi, Li; Ouyang, Yixin; Zeng, Xiao Cheng; Wang, Jinlan

2017-08-09

Nanosheet supported single-atom catalysts (SACs) can make full use of metal atoms and yet entail high selectivity and activity, and bifunctional catalysts can enable higher performance while lowering the cost than two separate unifunctional catalysts. Supported single-atom bifunctional catalysts are therefore of great economic interest and scientific importance. Here, on the basis of first-principles computations, we report a design of the first single-atom bifunctional eletrocatalyst, namely, isolated nickel atom supported on β 12 boron monolayer (Ni 1 /β 12 -BM), to achieve overall water splitting. This nanosheet supported SAC exhibits remarkable electrocatalytic performance with the computed overpotential for oxygen/hydrogen evolution reaction being just 0.40/0.06 V. The ab initio molecular dynamics simulation shows that the SAC can survive up to 800 K elevated temperature, while enacting a high energy barrier of 1.68 eV to prevent isolated Ni atoms from clustering. A viable experimental route for the synthesis of Ni 1 /β 12 -BM SAC is demonstrated from computer simulation. The desired nanosheet supported single-atom bifunctional catalysts not only show great potential for achieving overall water splitting but also offer cost-effective opportunities for advancing clean energy technology.

Kinetic Model of Resin-Catalyzed Decomposition of Acetone Cyanohydrin in Organic Solvent%有机溶剂中树脂催化丙酮氰醇分解反应的动力学模型

Institute of Scientific and Technical Information of China (English)

章亭洲; 杨立荣; 朱自强; 吴坚平

2003-01-01

Decomposition of acetone cyanohydrin is the first-step reaction for preparing (S)-α-cyano-3-phenoxybenzyl alcohol (CPBA) by the one-pot method in organic media. Considering the compatibility of bio-catalysts with chemical catalysts and the successive operation in the bioreactor, anion exchange resin (D301) wasused as catalyst for this reaction. External diffusion limitation was excluded by raising rotational speed to higherthan 190r@min-1 in both solvents. Internal diffusion limitation was verified to be insignificant in this reactionsystem. The effect of acetone cyanohydrin concentration on the reaction was also investigated. An intrinsic kineticmodel was proposed when the mass transfer limitation was excluded, and the average deviation of the model is10.5%.

Design of heterogeneous catalysts

DEFF Research Database (Denmark)

Frey, Anne Mette

was inspired by a computational screening, suggesting that alloys such as Ni-Fe, Co-Ni, and Co-Fe should show superior activity to the industrially used nickel catalyst. Especially the Ni-Fe system was considered to be interesting, since such alloy catalysts should be both more active and cheaper than the Ni...... catalyst. The results from the screening were experimentally verified for CO hydrogenation, CO2 hydrogenation, and simultaneous CO and CO2 hydrogenation by bimetallic Ni-Fe catalysts. These catalysts were found to be highly active and selective. The Co-Ni and Co-Fe systems were investigated for CO...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

Recent Scientific Progress on Developing Supported Ni Catalysts for Dry (CO2 Reforming of Methane

Directory of Open Access Journals (Sweden)

Hyun Ook Seo

2018-03-01

Full Text Available Two major green house gases (CO2 and CH4 can be converted into useful synthetic gas (H2 and CO during dry reforming of methane (DRM reaction, and a lot of scientific efforts has been made to develop efficient catalysts for dry reforming of methane (DRM. Noble metal-based catalysts can effectively assist DRM reaction, however they are not economically viable. Alternatively, non-noble based catalysts have been studied so far, and supported Ni catalysts have been considered as a promising candidate for DRM catalyst. Main drawback of Ni catalysts is its catalytic instability under operating conditions of DRM (>700 °C. Recently, it has been demonstrated that the appropriate choice of metal-oxide supports can address this issue since the chemical and physical of metal-oxide supports can prevent coke formation and stabilize the small Ni nanoparticles under harsh conditions of DRM operation. This mini-review covers the recent scientific findings on the development of supported Ni catalysts for DRM reaction, including the synthetic methods of supported Ni nanoparticles with high sintering resistance.

Optimization of Cs Content in Co-Mn-Al Mixed Oxide as Catalyst for N2O Decomposition.

Czech Academy of Sciences Publication Activity Database

Chromčáková, Ž.; Obalová, L.; Kustrowski, P.; Drozdek, M.; Karásková, K.; Jirátová, Květa; Kovanda, F.

2015-01-01

Roč. 41, č. 12 (2015), s. 9319-9332 ISSN 0922-6168. [Pannonian Symposium on Catalysis /12./. Třešť, 16.09.2014-20.09.2014] R&D Projects: GA ČR GA14-13750S Institutional support: RVO:67985858 Keywords : nitrous oxide * mixed oxide catalysts * cesium promoter * layered double hydroxides Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 1.833, year: 2015

Calcined hydrotalcites for the catalytic decomposition of N{sub 2}O in simulated process streams

Energy Technology Data Exchange (ETDEWEB)

Armor, J.N.; Braymer, T.A.; Farris, T.S.; Li, Y.; Petrocelli, F.P.; Weist, E.L. [Air Products and Chemicals, Inc., Allentown, PA (United States); Kannan, S.; Swamy, C.S. [Department of Chemistry, Indian Institute of Technology, Madras (India)

1996-01-18

Various hydrotalcite based catalysts were prepared for testing for the catalytic decomposition of N{sub 2}O. Co-Al, Ni-Al, Co/Pd-Al, Co/Rh-Al, and Co/Mg-Al substituted hydrotalcites and Co-La-Al hydroxides offer very good activity at modest temperatures. Precalcination of these materials at ca. 450-500C, which destroys the hydrotalcite phase, is necessary for optimum activity and life. For Co substituted hydrotalcites, the optimal ratio of Co/Al is 3.0. The temperature for 50% conversion of N{sub 2}O of these calcined cobalt hydrotalcites is ca. 75C lower than for the previous highly active Co-ZSM-5. These calcined cobalt hydrotalcite materials display sustained life at temperatures in excess of 670C in an O{sub 2} rich, wet stream with high levels of N{sub 2}O (10%). Excess O{sub 2} does not seriously impact N{sub 2}O decomposition, but the combination of both water vapor and O{sub 2} does reduce activity by ca. 50%

Hydrogen production by ethanol partial oxidation over nano-iron oxide catalysts produced by chemical vapour synthesis

Energy Technology Data Exchange (ETDEWEB)

Ahmed, Wael Ahmed Abou Taleb Sayed

2011-01-13

This work presents the experimental results of the synthesis of unsupported and supported SiC iron oxide nanoparticles and their catalytic activity towards ethanol partial oxidation. For comparison, further unsupported iron oxide phases were investigated towards the ethanol partial oxidation. These {gamma}-Fe{sub 2}O{sub 3} and {alpha}/{gamma}-Fe{sub 2}O{sub 3} phase catalysts were prepared by the CVS method using Fe(CO){sub 5} as precursor, supplied by another author. The {alpha}-Fe{sub 2}O{sub 3} and SiC nanoparticles were prepared by the CVS method using a home made hot wall reactor technique at atmospheric pressure. Ferrocene and tetramethylsilane were used as precursor for the production process. Process parameters of precursor evaporation temperature, precursor concentration, gas mixture velocity and gas mixture dilution were investigated and optimised to produce particle sizes in a range of 10 nm. For Fe{sub 2}O{sub 3}/SiC catalyst series production, a new hot wall reactor setup was used. The particles were produced by simultaneous thermal decomposition of ferrocene and tetramethylsilane in one reactor from both sides. The production parameters of inlet tube distance inside the reactor, precursor evaporation temperature and carrier gas flow were investigated to produce a series of samples with different iron oxide content. The prepared catalysts composition, physical and chemical properties were characterized by XRD, EDX, SEM, BET surface area, FTIR, XPS and dynamic light scattering (DLS) techniques. The catalytic activity for the ethanol gas-phase oxidation was investigated in a temperature range from 260 C to 290 C. The product distributions obtained over all catalysts were analysed with mass spectrometry analysis tool. The activity of bulk Fe{sub 2}O{sub 3} and SiC nanoparticles was compared with prepared nano-iron oxide phase catalysts. The reaction parameters, such as reaction temperature and O{sub 2}/ethanol ratio were investigated. The catalysts

Decompositions of manifolds

CERN Document Server

Daverman, Robert J

2007-01-01

Decomposition theory studies decompositions, or partitions, of manifolds into simple pieces, usually cell-like sets. Since its inception in 1929, the subject has become an important tool in geometric topology. The main goal of the book is to help students interested in geometric topology to bridge the gap between entry-level graduate courses and research at the frontier as well as to demonstrate interrelations of decomposition theory with other parts of geometric topology. With numerous exercises and problems, many of them quite challenging, the book continues to be strongly recommended to eve

Highly dispersed metal catalyst

Science.gov (United States)

Xiao, Xin; West, William L.; Rhodes, William D.

2016-11-08

A supported catalyst having an atomic level single atom structure is provided such that substantially all the catalyst is available for catalytic function. A process of forming a single atom catalyst unto a porous catalyst support is also provided.

Preparation and characterization of stable copper/zinc oxide/alumina catalysts for methanol synthesis

Energy Technology Data Exchange (ETDEWEB)

Hoeppener, R H; Doesburg, E B; Scholten, J J

1986-08-15

A series of Cu/ZnO/Al/sub 2/O/sub 3/ catalysts for the low pressure methanol synthesis has been prepared by coprecipitation with a sodium carbonate solution from solutions of a mixture of the corresponding metal nitrates, followed by drying, calcination and reduction. The catalysts and their precursors were analyzed by techniques like X-ray diffraction, X-ray line broadening, differential thermal analysis, chemical analysis, adsorptive decomposition of N/sub 2/O and B.E.T.-measurements. The catalytic activity for the methanol synthesis was determined in a flow reactor under industrial conditions. Depending on the metal ion ratio in the initial metal nitrate solutions different compounds were formed during coprecipitation, like rosasite, malachite, Cu, Zn-hydrotalcite and a ternary compound which was called roderite. Its structure is unknown and it contains, besides Zn/sup 2+/, up to 28 at% Cu/sup 2+/ and up to 17 at% Al/sup 3+/. Addition of 7 at% Mg/sup 2+/ stabilizes the Cu, Zn-hydrotalcite structure but leads to a drastic decrease in catalytic activity. The rate of methanol production depends on the phase composition of the precursors. Rosasite containing precursors give the highest activity; hydrotalcite proves to be an excellent catalyst stabilizer which evokes the formation of small Cu and ZnO particles. Mg/sup 2+/ inhibits methanol production. 6 figs., 1 tab., 18 refs.

Thermal decomposition of pyrite

International Nuclear Information System (INIS)

Music, S.; Ristic, M.; Popovic, S.

1992-01-01

Thermal decomposition of natural pyrite (cubic, FeS 2 ) has been investigated using X-ray diffraction and 57 Fe Moessbauer spectroscopy. X-ray diffraction analysis of pyrite ore from different sources showed the presence of associated minerals, such as quartz, szomolnokite, stilbite or stellerite, micas and hematite. Hematite, maghemite and pyrrhotite were detected as thermal decomposition products of natural pyrite. The phase composition of the thermal decomposition products depends on the terature, time of heating and starting size of pyrite chrystals. Hematite is the end product of the thermal decomposition of natural pyrite. (author) 24 refs.; 6 figs.; 2 tabs

Danburite decomposition by sulfuric acid

International Nuclear Information System (INIS)

Mirsaidov, U.; Mamatov, E.D.; Ashurov, N.A.

2011-01-01

Present article is devoted to decomposition of danburite of Ak-Arkhar Deposit of Tajikistan by sulfuric acid. The process of decomposition of danburite concentrate by sulfuric acid was studied. The chemical nature of decomposition process of boron containing ore was determined. The influence of temperature on the rate of extraction of boron and iron oxides was defined. The dependence of decomposition of boron and iron oxides on process duration, dosage of H 2 SO 4 , acid concentration and size of danburite particles was determined. The kinetics of danburite decomposition by sulfuric acid was studied as well. The apparent activation energy of the process of danburite decomposition by sulfuric acid was calculated. The flowsheet of danburite processing by sulfuric acid was elaborated.

Iron phthalocyanine supported on amidoximated PAN fiber as effective catalyst for controllable hydrogen peroxide activation in oxidizing organic dyes

International Nuclear Information System (INIS)

Han, Zhenbang; Han, Xu; Zhao, Xiaoming; Yu, Jiantao; Xu, Hang

2016-01-01

Iron(II) phthalocyanine was immobilized onto amidoximated polyacrylonitrile fiber to construct a bioinspired catalytic system for oxidizing organic dyes by H 2 O 2 activation. The amidoxime groups greatly helped to anchor Iron(II) phthalocyanine molecules onto the fiber through coordination interaction, which has been confirmed by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and UV diffuse reflectance spectroscopy analyses. Electron spin resonance studies indicate that the catalytic process of physically anchored Iron(II) phthalocyanine performed via a hydroxyl radical pathway, while the catalyst bonded Iron(II) phthalocyanine through coordination effect could selectively catalyze the H 2 O 2 decomposition to generate high-valent iron-oxo species. This may result from the amidoxime groups functioning as the axial fifth ligands to favor the heterolytic cleavage of the peroxide O−O bond. This feature also enables the catalyst to only degrade the dyes adjacent to the catalytic active centers and enhances the efficient utilization of H 2 O 2 . In addition, this catalyst could effectively catalyze the mineralization of organic dyes and can be easily recycled without any loss of activity.

Hydrodeoxygenation of O-containing polycyclic model compounds using a novel organometallic catalyst-precursor

Energy Technology Data Exchange (ETDEWEB)

Kirby, S.R.; Song, C.S.; Schobert, H.H. [Pennsylvania State University, University Park, PA (United States). Dept. of Materials Science and Engineering

1996-09-05

Compounds containing oxygen functional groups, especially phenols, are undesirable components of coal-derived liquids. Removal of these compounds from the products of coal liquefaction is required. A beneficial alternative would be the removal of these compounds, or the prevention of their formation, during the liquefaction reaction itself, rather than as a separate processing step. A novel organometallic catalyst precursor containing Co and Mo has been studied as a potential hydrogenation catalyst for coal liquefaction. To ascertain the hydrodeoxygenation activity of this catalyst under liquefaction conditions, model compounds were investigated. Anthrone, 2,6-di-r-btuyl-4-methyl-phenol, dinaphthyl ether and xanthene were reacted in the presence of the Co-Mo catalyst precursor and a precursor containing only Mo over a range of temperatures, providing a comparison of conversions to deoxygenated products. These conversions give an indication of the hydrodeoxygenating abilities of organometallic catalyst precursors within a coal liquefaction system. For example, at 400{degree}C dinaphthyl ether was converted 100% (4.5% O-containing products) in the presence of the Co-Mo organometallic precursor, compared to 76.5% conversion (7.4% O-products) in the presence of the Mo catalyst.

Effect of coke and catalyst structure on oxidative regeneration of hydroprocessing catalysts

Energy Technology Data Exchange (ETDEWEB)

Furimsky, E. (CANMET, Ottawa, ON (Canada). Energy Research Laboratories)

1991-04-01

Two industrial hydroprocessing catalysts used for upgrading an atmospheric residue and a gas oil, respectively were regenerated in a fixed bed using air and 2 vol.% O{sub 2}+N{sub 2} balance mixture. The regeneration in air resulted in a significant sintering of the catalyst's material. The surface area of catalysts regenerated in 2 vol.% O{sub 2} mixture was similar to that of fresh catalysts, whereas a significant loss of surface area was observed after regeneration in air. The X-ray diffraction pattern of catalysts regenerated in 2 vol.% O{sub 2}+N{sub 2} balance mixture was also similar to that of fresh catalysts. 22 refs., 9 figs., 7 tabs.

Hydroprocessing catalyst development

Energy Technology Data Exchange (ETDEWEB)

Boorman, P.M.; Kydd, R.A.; Sorensen, T.S.; Chong, K.; Lewis, J.

1992-08-01

Co-Mo and Ni-Mo hydroprocessing catalysts were examined for their activity in removal of sulfur from thiophene in model compounds, and in the cracking and hydrocracking of cumene. Three types of support materials were examined: carbon, modified carbon, and carbon covered alumina. The objective of the study was to examine the correlation between catalyst activity in the hydrodenitrogenation of model compounds, and the resistance of the catalyst to nitrogen poisoning during use in the hydroprocessing of gas oils. The use of model compound testing provided information on the individual catalytic reactions promoted by those materials. Infrared spectroscopy was used to study surface species on the catalysts and to explain many of the trends in activity observed, revealing the role of fluoride and phosphorus as a secondary promoter. Testing of the catalysts in hydrotreating of gas oils allowed comparison of model compound results with those from a real feedstock. The gas oil was also spiked with a model nitrogen compound and the results from catalytic hydrotreating of this material were compared with those from unspiked material. A key finding was that the carbon supported catalysts were the most effective in treating high-nitrogen feeds. The very favorable deactivation properties of carbon and carbon-covered alumina supported catalysts make these promising from an industrial point of view where catalyst deactivation is a limiting factor. 171 refs., 25 figs., 43 tabs.

Fabrication of porous MgCo2O4 with rod-like morphology and its superb catalytic activity towards ammonium perchlorate thermal decomposition

Science.gov (United States)

Li, Gang; Liu, Xiaoli; Bai, Weiyang

2018-03-01

In this paper, porous MgCo2O4 with rod-like morphology was successfully synthesized through the thermal treatment of metal oxalates precursor originated by the reaction of metal sulfates and oxalic acid, without the addition of other additives. The porous rod-like MgCo2O4, with a diameter of several hundred nanometers and a length of several micrometers, was formed through the agglomeration of numerous crystalline grains sized in 10–25 nm. Its catalytic effect on ammonium perchlorate (AP) thermal decomposition was evaluated using differential scanning calorimetry (DSC) techniques. It was found that the pyrolysis temperature of AP reduced by 129 °C and the heat release increased more than 3.19-fold with a 2 wt% addition of MgCo2O4. Meanwhile, the addition of MgCo2O4 resulted in an AP decomposition activation energy reduction from 216 kJ mol‑1 to 155 kJ mol‑1, calculated using the Kissinger correlation. This study provides new insights into the design and development of high performance catalysts for AP thermal decomposition.

Suppressing propylene carbonate decomposition by coating graphite electrode foil with silver

International Nuclear Information System (INIS)

Gao, J.; Zhang, H.P.; Fu, L.J.; Zhang, T.; Wu, Y.P.; Takamura, T.; Wu, H.Q.; Holze, R.

2007-01-01

A method has been developed to suppress the decomposition of propylene carbonate (PC) by coating graphite electrode foil with a layer of silver. Results from electrochemical impedance measurements show that the Ag-coated graphite electrode presents lower charge transfer resistance and faster diffusion of lithium ions in comparison with the virginal one. Cyclic voltammograms and discharge-charge measurements suggest that the decomposition of propylene carbonate and co-intercalation of solvated lithium ions are prevented, and lithium ions can reversibly intercalate into and deintercalate from the Ag-coated graphite electrode. These results indicate that Ag-coating is a good way to improve the electrochemical performance of graphitic carbon in PC-based electrolyte solutions

Hydrogen Production via Steam Reforming of Ethyl Alcohol over Palladium/Indium Oxide Catalyst

Directory of Open Access Journals (Sweden)

Tetsuo Umegaki

2009-01-01

Full Text Available We report the synergetic effect between palladium and indium oxide on hydrogen production in the steam reforming reaction of ethyl alcohol. The palladium/indium oxide catalyst shows higher hydrogen production rate than indium oxide and palladium. Palladium/indium oxide affords ketonization of ethyl alcohol with negligible by-product carbon monoxide, while indium oxide mainly affords dehydration of ethyl alcohol, and palladium affords decomposition of ethyl alcohol with large amount of by-product carbon monoxide. The catalytic feature of palladium/indium oxide can be ascribed to the formation of palladium-indium intermetallic component during the reaction as confirmed by X-ray diffraction and X-ray photoelectron spectroscopic measurements.

Characterization and Utilization of Calcium Oxide (CaO Thermally Decomposed from Fish Bones as a Catalyst in the Production of Biodiesel from Waste Cooking Oil

Directory of Open Access Journals (Sweden)

Aldes Lesbani

2016-12-01

Full Text Available Thermal decomposition of fish bones to obtain calcium oxide (CaO was conducted at various temperatures of 400, 500, 800, 900, 1000, and 1100 °C. The calcium oxide was then characterized using X-ray diffractometer, FTIR spectrophotometer, and SEM analysis. The calcium oxide obtained from the decomposition at 1000 °C was then used as a catalyst in the production of biodiesel from waste cooking oil. Diffraction pattern of the calcium oxide produced from decomposition at 1000 °C showed a pattern similar to that of the calcium oxide produced by the Joint Committee on Powder Diffraction Standard (JCDPS. The diffractions of 2θvalues at 1000 °C were 32.2, 37.3, 53.8, 64.1, and67.3 deg. The FTIR spectrum of calcium oxide decomposed at 1000 °C has a specific vibration at wave-length 362 cm-1, which is similar to the specific vibration of Ca-O. SEM analysis of the calcium oxide indicated that the calcium oxide’s morphology shows a smaller size and a more homogeneous structure, compared to those of fish bones. Theuse of calcium oxide as a catalyst in the production of biodiesel from waste cooking oil resulted in iod number of 15.23 g/100 g KOH, density of 0.88 g/cm3, viscosity of 6.00 cSt, and fatty acid value of 0.56 mg/KOH. These characteristic values meet the National Standard of Indonesia (SNI for biodiesel.

Effect of high-temperature treatment on Fe/ZSM-5 prepared by chemical vapor deposition of FeCl3. II. Nitrous oxide decomposition, selective oxidation of benzene to phenol, and selective reduction of nitric oxide by isobutane

NARCIS (Netherlands)

Zhu, Q.; Teeffelen, van R.M.; Santen, van R.A.; Hensen, E.J.M.

2004-01-01

The catalytic performance (nitrous oxide decomposition, hydroxylation of benzene to phenol with nitrous oxide, and selective reduction of nitric oxide by i-butane) was evaluated for a set of HZSM-5 and sublimed Fe/ZSM-5 catalysts, which have been extensively characterized in an earlier contribution

Supported catalyst systems and method of making biodiesel products using such catalysts

Science.gov (United States)

Kim, Manhoe; Yan, Shuli; Salley, Steven O.; Ng, K. Y. Simon

2015-10-20

A heterogeneous catalyst system, a method of preparing the catalyst system and a method of forming a biodiesel product via transesterification reactions using the catalyst system is disclosed. The catalyst system according to one aspect of the present disclosure represents a class of supported mixed metal oxides that include at least calcium oxide and another metal oxide deposited on a lanthanum oxide or cerium oxide support. Preferably, the catalysts include CaO--CeO.sub.2ZLa.sub.2O.sub.3 or CaO--La.sub.2O.sub.3/CeO.sub.2. Optionally, the catalyst may further include additional metal oxides, such as CaO--La.sub.2O.sub.3--GdOxZLa.sub.2O.sub.3.

Azimuthal decomposition of optical modes

CSIR Research Space (South Africa)

Dudley, Angela L

2012-07-01

Full Text Available This presentation analyses the azimuthal decomposition of optical modes. Decomposition of azimuthal modes need two steps, namely generation and decomposition. An azimuthally-varying phase (bounded by a ring-slit) placed in the spatial frequency...

Hierarchical hybrid peroxidase catalysts for remediation of phenol wastewater

KAUST Repository

Duan, Xiaonan

2014-02-20

We report a new family of hierarchical hybrid catalysts comprised of horseradish peroxidase (HRP)-magnetic nanoparticles for advanced oxidation processes and demonstrate their utility in the removal of phenol from water. The immobilized HRP catalyzes the oxidation of phenols in the presence of H2O2, producing free radicals. The phenoxy radicals react with each other in a non-enzymatic process to form polymers, which can be removed by precipitation with salts or condensation. The hybrid peroxidase catalysts exhibit three times higher activity than free HRP and are able to remove three times more phenol from water compared to free HRP under similar conditions. In addition, the hybrid catalysts reduce substrate inhibition and limit inactivation from reaction products, which are common problems with free or conventionally immobilized enzymes. Reusability is improved when the HRP-magnetic nanoparticle hybrids are supported on micron-scale magnetic particles, and can be retained with a specially designed magnetically driven reactor. The performance of the hybrid catalysts makes them attractive for several industrial and environmental applications and their development might pave the way for practical applications by eliminating most of the limitations that have prevented the use of free or conventionally immobilized enzymes. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hierarchical hybrid peroxidase catalysts for remediation of phenol wastewater

KAUST Repository

Duan, Xiaonan; Corgié , Sté phane C.; Aneshansley, Daniel J.; Wang, Peng; Walker, Larry P.; Giannelis, Emmanuel P.

2014-01-01

We report a new family of hierarchical hybrid catalysts comprised of horseradish peroxidase (HRP)-magnetic nanoparticles for advanced oxidation processes and demonstrate their utility in the removal of phenol from water. The immobilized HRP catalyzes the oxidation of phenols in the presence of H2O2, producing free radicals. The phenoxy radicals react with each other in a non-enzymatic process to form polymers, which can be removed by precipitation with salts or condensation. The hybrid peroxidase catalysts exhibit three times higher activity than free HRP and are able to remove three times more phenol from water compared to free HRP under similar conditions. In addition, the hybrid catalysts reduce substrate inhibition and limit inactivation from reaction products, which are common problems with free or conventionally immobilized enzymes. Reusability is improved when the HRP-magnetic nanoparticle hybrids are supported on micron-scale magnetic particles, and can be retained with a specially designed magnetically driven reactor. The performance of the hybrid catalysts makes them attractive for several industrial and environmental applications and their development might pave the way for practical applications by eliminating most of the limitations that have prevented the use of free or conventionally immobilized enzymes. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Thermal decomposition of lutetium propionate

DEFF Research Database (Denmark)

Grivel, Jean-Claude

2010-01-01

The thermal decomposition of lutetium(III) propionate monohydrate (Lu(C2H5CO2)3·H2O) in argon was studied by means of thermogravimetry, differential thermal analysis, IR-spectroscopy and X-ray diffraction. Dehydration takes place around 90 °C. It is followed by the decomposition of the anhydrous...... °C. Full conversion to Lu2O3 is achieved at about 1000 °C. Whereas the temperatures and solid reaction products of the first two decomposition steps are similar to those previously reported for the thermal decomposition of lanthanum(III) propionate monohydrate, the final decomposition...... of the oxycarbonate to the rare-earth oxide proceeds in a different way, which is here reminiscent of the thermal decomposition path of Lu(C3H5O2)·2CO(NH2)2·2H2O...

A Comparative Study of TiO2-supported and Bulk Co-Mn-Al Catalysts for N2O Decomposition

Czech Academy of Sciences Publication Activity Database

Karásková, K.; Chromčáková, Ž.; Študentová, S.; Matějka, V.; Jirátová, Květa; Obalová, L.

2012-01-01

Roč. 191, č. 1 (2012), s. 112-115 ISSN 0920-5861 R&D Projects: GA ČR GA106/09/1664 Institutional support: RVO:67985858 Keywords : nitrous oxide * catalytic decomposition * layered double hydroxides Subject RIV: CI - Industrial Chemistry, Chemical Engineering Impact factor: 2.980, year: 2012

Graphitized Carbon: A Promising Stable Cathode Catalyst Support Material for Long Term PEMFC Applications.

Science.gov (United States)

Mohanta, Paritosh Kumar; Regnet, Fabian; Jörissen, Ludwig

2018-05-28

Stability of cathode catalyst support material is one of the big challenges of polymer electrolyte membrane fuel cells (PEMFC) for long term applications. Traditional carbon black (CB) supports are not stable enough to prevent oxidation to CO₂ under fuel cell operating conditions. The feasibility of a graphitized carbon (GC) as a cathode catalyst support for low temperature PEMFC is investigated herein. GC and CB supported Pt electrocatalysts were prepared via an already developed polyol process. The physical characterization of the prepared catalysts was performed using transmission electron microscope (TEM), X-ray Powder Diffraction (XRD) and inductively coupled plasma optical emission spectrometry (ICP-OES) analysis, and their electrochemical characterizations were conducted via cyclic voltammetry(CV), rotating disk electrode (RDE) and potential cycling, and eventually, the catalysts were processed using membrane electrode assemblies (MEA) for single cell performance tests. Electrochemical impedance spectroscopy (EIS) and scanning electrochemical microscopy (SEM) have been used as MEA diagonostic tools. GC showed superior stability over CB in acid electrolyte under potential conditions. Single cell MEA performance of the GC-supported catalyst is comparable with the CB-supported catalyst. A correlation of MEA performance of the supported catalysts of different Brunauer⁻Emmett⁻Teller (BET) surface areas with the ionomer content was also established. GC was identified as a promising candidate for catalyst support in terms of both of the stability and the performance of fuel cell.

Three-pattern decomposition of global atmospheric circulation: part I—decomposition model and theorems

Science.gov (United States)

Hu, Shujuan; Chou, Jifan; Cheng, Jianbo

2018-04-01

In order to study the interactions between the atmospheric circulations at the middle-high and low latitudes from the global perspective, the authors proposed the mathematical definition of three-pattern circulations, i.e., horizontal, meridional and zonal circulations with which the actual atmospheric circulation is expanded. This novel decomposition method is proved to accurately describe the actual atmospheric circulation dynamics. The authors used the NCEP/NCAR reanalysis data to calculate the climate characteristics of those three-pattern circulations, and found that the decomposition model agreed with the observed results. Further dynamical analysis indicates that the decomposition model is more accurate to capture the major features of global three dimensional atmospheric motions, compared to the traditional definitions of Rossby wave, Hadley circulation and Walker circulation. The decomposition model for the first time realized the decomposition of global atmospheric circulation using three orthogonal circulations within the horizontal, meridional and zonal planes, offering new opportunities to study the large-scale interactions between the middle-high latitudes and low latitudes circulations.

High-Activity Dealloyed Catalysts

Energy Technology Data Exchange (ETDEWEB)

Kongkanand, Anusorn [General Motors LLC, Pontiac, MI (United States)

2014-09-30

Reduction of costly Pt usage in proton exchange membrane fuel cell electrodes is one of the major challenges towards development and commercialization of fuel cell vehicles. Although few have met the initial-kinetic activity requirements in a realistic fuel cell device, no catalyst material has ever met the demanding fuel cell durability targets set by DOE. In this project, a team of 4 universities and 2 companies came together to investigate a concept that appeared promising in preliminary non-fuel cell tests then to further develop the catalyst to a mature level ready for vehicle implementation. The team consists of academia with technical leadership in their respective areas, a catalyst supplier, and a fuel cell system integrator.The tightly collaborative project enabled development of a highly active and durable catalyst with performance that significantly exceeds that of previous catalysts and meets the DOE targets for the first time (Figure 1A). The catalyst was then further evaluated in full-active-area stack in a realistic vehicle operating condition (Figure 1B). This is the first public demonstration that one can realize the performance benefit and Pt cost reduction over a conventional pure Pt catalyst in a long-term realistic PEMFC system. Furthermore, systematic analyses of a range of catalysts with different performance after fuel cell testing allowed for correlation between catalyst microstructure and its electrocatalytic activity and durability. This will in turn aid future catalyst development.

Surface chemistry and catalytic properties of VOX/Ti-MCM-41 catalysts for dibenzothiophene oxidation in a biphasic system

International Nuclear Information System (INIS)

González, J.; Chen, L.F.; Wang, J.A.; Manríquez, Ma.; Limas, R.; Schachat, P.; Navarrete, J.; Contreras, J.L.

2016-01-01

Highlights: • Oxidative desulfurization of model diesel was tested in a biphasic system. • ODS activity was proportional to the V 5+ /(V 4+ + V 5+ ) values of the catalysts. • Lewis acidity was related to vanadium content and catalytic activity. • 99.9% DBT was oxidized using 25%V 2 O 5 /Ti-MCM-41 at 60 °C within 60 min. - Abstract: A series of vanadium oxide supported on Ti-MCM-41 catalysts was synthesized via the incipient impregnation method by varying the vanadia loading from 5 wt% to 10, 15, 20 and 25 wt%. These catalysts were characterized by a variety of advanced techniques for investigating their crystalline structure, textural properties, and surface chemistry information including surface acidity, reducibility, vanadium oxidation states, and morphological features. The catalytic activities of the catalysts were evaluated in a biphasic reaction system for oxidative desulfurization (ODS) of a model diesel containing 300 ppm of dibenzothiophene (DBT) where acetonitrile was used as extraction solvent and H 2 O 2 as oxidant. ODS activity was found to be proportional to the V 5+ /(V 4+ + V 5+ ) values of the catalysts, indicating that the surface vanadium pentoxide (V 2 O 5 ) was the active phase. Reaction temperature would influence significantly the ODS efficiency; high temperature, i.e., 80 °C, would lead to low ODS reaction due to the partial decomposition of oxidant. All the catalysts contained both Lewis and Brønsted acid sites but the former was predominant. The catalysts with low vanadia loading (5 or 10 wt%V 2 O 5 ) had many Lewis acid sites and could strongly adsorb DBT molecule via the electron donation/acceptance action which resulted in an inhibition for the reaction of DBT with the surface peroxometallic species. The catalyst with high vanadia loading (25wt%V 2 O 5 /Ti-MCM-41) showed the highest catalytic activity and could remove 99.9% of DBT at 60 °C within 60 min.

Preventing maritime transport of pathogens: the remarkable antimicrobial properties of silver-supported catalysts for ship ballast water disinfection.

Science.gov (United States)

Theologides, C P; Theofilou, S P; Anayiotos, A; Costa, C N

2017-07-01

Ship ballast water (SBW) antimicrobial treatment is considered as a priority issue for the shipping industry. The present work investigates the possibility of utilizing antimicrobial catalysis as an effective method for the treatment of SBW. Taking into account the well-known antimicrobial properties of ionic silver (Ag + ), five silver-supported catalysts (Ag/γ-Al 2 O 3 ) with various loadings (0.05, 0.1, 0.2, 0.5, and 1 wt%) were prepared and examined for the antimicrobial treatment of SBW. The bactericidal activity of the aforementioned catalysts was investigated towards the inhibition of Escherichia coli (Gram-negative) and Escherichia faecalis (Gram-positive) bacteria. Catalytic experiments were conducted in a three-phase continuous flow stirred tank reactor, used in a semi-batch mode. It was found that using the catalyst with the lowest metal loading, the inhibition of E. coli reached 95.8% after 30 minutes of treatment of an E. coli bacterial solution, while the inhibition obtained for E. faecalis was 76.2% after 60 minutes of treatment of an E. faecalis bacterial solution. Even better results (100% inhibition after 5 min of reaction) were obtained using the catalysts with higher Ag loadings. The results of the present work indicate that the prepared monometallic catalysts exert their antimicrobial activity within a short period of time, revealing, for the first time ever, that the field of antimicrobial heterogeneous catalysis using deposited ionic silver on a solid support may prove decisive for the disinfection of SBW.

Development of Molecular Catalysts to Bridge the Gap between Heterogeneous and Homogeneous Catalysts

Science.gov (United States)

Ye, Rong

Catalysts, heterogeneous, homogeneous, and enzymatic, are comprised of nanometer-sized inorganic and/or organic components. They share molecular factors including charge, coordination, interatomic distance, bonding, and orientation of catalytically active atoms. By controlling the governing catalytic components and molecular factors, catalytic processes of a multichannel and multiproduct nature could be run in all three catalytic platforms to create unique end-products. Unifying the fields of catalysis is the key to achieving the goal of 100% selectivity in catalysis. Recyclable catalysts, especially those that display selective reactivity, are vital for the development of sustainable chemical processes. Among available catalyst platforms, heterogeneous catalysts are particularly well-disposed toward separation from the reaction mixture via filtration methods, which renders them readily recyclable. Furthermore, heterogeneous catalysts offer numerous handles - some without homogeneous analogues - for performance and selectivity optimization. These handles include nanoparticle size, pore profile of porous supports, surface ligands and interface with oxide supports, and flow rate through a solid catalyst bed. Despite these available handles, however, conventional heterogeneous catalysts are themselves often structurally heterogeneous compared to homogeneous catalysts, which complicates efforts to optimize and expand the scope of their reactivity and selectivity. Ongoing efforts are aimed to address the above challenge by heterogenizing homogeneous catalysts, which can be defined as the modification of homogeneous catalysts to render them in a separable (solid) phase from the starting materials and products. Specifically, we grow the small nanoclusters in dendrimers, a class of uniform polymers with the connectivity of fractal trees and generally radial symmetry. Thanks to their dense multivalency, shape persistence and structural uniformity, dendrimers have proven to

Communicating catalysts

Science.gov (United States)

Weckhuysen, Bert M.

2018-06-01

The beauty and activity of enzymes inspire chemists to tailor new and better non-biological catalysts. Now, a study reveals that the active sites within heterogeneous catalysts actively cooperate in a fashion phenomenologically similar to, but mechanistically distinct, from enzymes.

Preparation of iron molybdate catalysts for methanol to formaldehyde oxidation based on ammonium molybdoferrate(II precursor

Directory of Open Access Journals (Sweden)

N.V. Nikolenko

2018-03-01

Full Text Available It was demonstrated that iron molybdate catalysts for methanol oxidation can be prepared using Fe(II as a precursor instead of Fe(III. This would allow for reduction of acidity of preparation solutions as well as elimination of Fe(III oxide impurities which are detrimental for the process selectivity. The system containing Fe(II and Mo(VI species in aqueous solution was investigated using UV–Vis spectroscopy. It was demonstrated that three types of chemical reactions occur in the Fe(II–Mo(VI system: (i formation of complexes between Fe(II and molybdate(VI ions, (ii inner sphere oxidation of coordinated Fe(II by Mo(VI and (iii decomposition of the Fe–Mo complexes to form scarcely soluble Fe(III molybdate, Mo(VI hydrous trioxide and molybdenum blue. Solid molybdoferrate(II prepared by interaction of Fe(II and Mo(VI in solution was characterized by EDXA, TGA, DTA and XRD and a scheme of its thermal evolution proposed. The iron molybdate catalyst prepared from Fe(II precursor was tested in methanol-to-formaldehyde oxidation in a continuous flow fixed-bed reactor to show similar activity and selectivity to the conventional catalyst prepared with the use of Fe(III.

Analysis of the critical step in catalytic carbodiimide transformation: proton transfer from amines, phosphines, and alkynes to guanidinates, phosphaguanidinates, and propiolamidinates with Li and Al catalysts.

Science.gov (United States)

Rowley, Christopher N; Ong, Tiow-Gan; Priem, Jessica; Richeson, Darrin S; Woo, Tom K

2008-12-15

While lithium amides supported by tetramethylethylenediamine (TMEDA) are efficient catalysts in the synthesis of substituted guanidines via the guanylation of an amine with carbodiimide, as well as the guanylation of phosphines and conversion of alkynes into propiolamidines, aluminum amides are only efficient catalysts for the guanylation of amides. Density functional theory (DFT) calculations were used to explain this difference in activity. The origin of this behavior is apparent in the critical step where a proton is transferred from the substrate to a metal guanidinate. The activation energies of these steps are modest for amines, phosphines, and alkynes when a lithium catalyst was used, but are prohibitively high for the analogous reactions with phosphines and alkynes for aluminum amide catalysts. Energy decomposition analysis (EDA) indicates that these high activations energies are due to the high energetic cost of the detachment of a chelating guanidinate nitrogen from the aluminum in the proton transfer transition state. Amines are able to adopt an ideal geometry for facile proton transfer to the aluminum guanidinate and concomitant Al-N bond formation, while phosphines and alkynes are not.

Alkali/TX[sub 2] catalysts for CO/H[sub 2] conversion to C[sub 1]-C[sub 4] alcohols

Energy Technology Data Exchange (ETDEWEB)

Klier, K.; Herman, R.G.; Bastian, R.D.; Flanagan, K.L.

1989-01-01

Ruthenium disulfide catalysts have been synthesized, tested, and characterized during this period of research. It was observed that both the undoped and Cs-doped RuS[sub 2] catalysts produced alcohols and lower amounts of hydrocarbons from H[sub 2]/CO = 1.0 synthesis gas at temperatures above 300[degree]C. Calcination and catalytic testing resulted in partial reduction of the RuS[sub 2] to Ru[sup o]. Calcination under H[sub 2]S prevented the partial reduction of the RuS[sub 2] catalyst, but subsequent catalytic testing again resulted in the formation of a quantity of Ru[sup o]. A Cs-doped RuS[sub 2] catalyst was prepared, but it might have had too high of a loading of Cs. Upon testing, a lower activity was observed for the doped catalyst compared with the undoped catalyst, but the alcohol selectivity was the same for the two catalysts.

Methods of making textured catalysts

Science.gov (United States)

Werpy, Todd [West Richland, WA; Frye, Jr., John G.; Wang, Yong [Richland, WA; Zacher, Alan H [Kennewick, WA

2010-08-17

A textured catalyst having a hydrothermally-stable support, a metal oxide and a catalyst component is described. Methods of conducting aqueous phase reactions that are catalyzed by a textured catalyst are also described. The invention also provides methods of making textured catalysts and methods of making chemical products using a textured catalyst.

A comprehensive small and pilot-scale fixed-bed reactor approach for testing Fischer–Tropsch catalyst activity and performance on a BTL route

Directory of Open Access Journals (Sweden)

Piyapong Hunpinyo

2017-05-01

Full Text Available Ruthenium (Ru-based catalysts were prepared by the sol–gel technique for biomass-to-liquid (BTL operation and had their performance tested under different conditions. The catalytic study was carried out in two steps using a simple and reliable method. In the first step, the effects of reaction temperatures and inlet H2/CO molar feed ratios obtained from biomass gasification were investigated on the catalyst performance. A set of experimental results obtained in a laboratory fixed bed reactor was described and summarized. Moreover, a simplified Langmuir–Hinshelwood–Hougen–Watson (LHHW kinetic model was proposed with two promising models, where the surface decomposition of carbon monoxide was assumed as the rate determining step (RDS. In the second step, a FT pilot plant was conducted to validate the catalyst performance, especially the conversion efficiency, heat and mass transfer effects, and system controllability. The results indicated that our catalyst performances under mild conditions were not significantly different in many regards from those previously reported for a severe condition, as especially Ru-based catalyst can be performed to vary over a wide range of conditions to yield specific liquid productivity. The results in terms of the hydrocarbon product distribution obtained from the pilot scale operations were similar with that obtained from the related lab scale experiments.

DFT + U investigation on the adsorption and initial decomposition of methylamine by a Pt single-atom catalyst supported on rutile (110) TiO{sub 2}

Energy Technology Data Exchange (ETDEWEB)

Lv, Cun-Qin [College of Chemistry and Environmental Engineering, Shanxi Datong University, Datong 037009, Shanxi Province (China); Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071 (China); Liu, Jian-Hong, E-mail: ljh173@126.com [College of Chemistry and Environmental Engineering, Shanxi Datong University, Datong 037009, Shanxi Province (China); Guo, Yong; Li, Xue-Mei [College of Chemistry and Environmental Engineering, Shanxi Datong University, Datong 037009, Shanxi Province (China); Wang, Gui-Chang, E-mail: wangguichang@nankai.edu.cn [Department of Chemistry, Tianjin Key Lab. of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin 300071 (China)

2016-12-15

Highlights: • DFT + U is used to investigate the initial decomposition of methylamine. • The adsorption characteristics of possible intermediates involved in methylamine initial decomposition are discussed. • The energy barriers of the possible elementary reactions involved are obtained. • C−H bond scission is the most favored among the C−H, N−H and C−N bond breakings in methylamine. - Abstract: The adsorption and initial decomposition for methylamine catalyzed by a single Pt atom supported on rutile (110) titania (namely, Pt{sub 1}/TiO{sub 2}–R(110)) surface have been investigated by the density functional theory slab calculations with Hubbard corrections (DFT + U). The main purpose of the work is to better understand the role of dispersed platinum metal on the surface of rutile (110) titania in the initial decomposition of methylamine. Our calculated results show that the barriers increased with the order of C−H < N−H < C−N, which indicates that the C−H bond is the easiest to decompose and the C−N bond is the most difficult to break.

N2O Catalytic Decomposition - Effect of Pelleting Pressure on Activity of Co-Mn-Al Mixed Oxide Catalyst

Czech Academy of Sciences Publication Activity Database

Galejová, K.; Obalová, L.; Jirátová, Květa; Pacultová, K.; Kovanda, F.

2009-01-01

Roč. 63, č. 2 (2009), s. 172-179 ISSN 0366-6352. [International Conference of the Slovak-Society-of-Chemical-Engineering /35./. Tatranske Matliare, 26.05.2008-30.05.2008] R&D Projects: GA ČR GA104/07/1400 Institutional research plan: CEZ:AV0Z40720504 Keywords : pelleting pressure * nitrous oxide * catalytic decomposition Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 0.791, year: 2009

In-situ hydrodeoxygenation of phenol by supported Ni catalyst-explanation for catalyst performance

DEFF Research Database (Denmark)

Wang, Ze; Zeng, Ying; Lin, Weigang

2017-01-01

In-situ hydrodeoxygenation of phenol with aqueous hydrogen donor over supported Ni catalyst was investigated. The supported Ni catalysts exerted very poor performance, if formic acid was used as the hydrogen donor. Catalyst modification by loading K, Na, Mg or La salt could not make the catalyst...... performance improved. If gaseous hydrogen was used as the hydrogen source the activity of Ni/Al2O3 was pretty high. CO2 was found poisonous to the catalysis, due to the competitive adoption of phenol with CO2. If formic acid was replaced by methanol, the catalyst performance improved remarkably, with major...... products of cyclohexanone and cyclohexanol. The better effect of methanol enlightened the application of the supported Ni catalyst in in-situ hydrodeoxygenation of phenol....

Non-PGM cell catalysts

Energy Technology Data Exchange (ETDEWEB)

Colon-Mercado, H. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Elvington, M. [Savannah River Consulting, Aiken, SC (United States); Ganesan, P. [Savannah River Consulting, Aiken, SC (United States)

2017-09-27

A unique approach has been developed to probe the non-PGM catalyst active site for the Oxygen Reduction Reaction (ORR) for PEMFCs. Iron based functionalities have been engineered into a variety of catalysts to evaluate their impact on activity for the ORR. A series of high surface area catalysts were synthesized and the impact of the chemical structure on the electrochemical and electrocatalytic properties was investigated. Elemental and surface analyses of the prepared catalysts reveal the incorporation of iron in a targeted and controlled manner. A high surface area framework catalyst was prepared that shows exceptional activity, comparable to state-of-the-art materials. The results of this research project provided critical seed data for the newly awarded ElectroCat project, which focuses on rationally designed framework catalysts for the oxygen reduction reaction.

Molecular modelling of the decomposition of NH{sub 3} over CoO(100)

Energy Technology Data Exchange (ETDEWEB)

Shojaee, Kambiz; Haynes, Brian S.; Montoya, Alejandro, E-mail: alejandro.montoya@sydney.edu.au

2015-04-15

Spin-polarised density functional theory using the PBE + U approach are used to determine reaction pathways of successive NH{sub 3} dehydrogenation on the CoO(100) surface. NH{sub 3} dehydrogenation promotes noticeable displacements of the surface CoO sites, in particular due to the binding of NH{sub 2} and H species. Surface lattice O has low activity towards dehydrogenation, reflected in energy barriers that are in the range of 292 kJ mol{sup −1} to 328 kJ mol{sup −1}. There is a preference of surface NH{sub 3} dehydrogenation to N{sub 2} rather than towards NO, due to a high-energy penalty of surface O vacancy formation. The presence of CoO in cobalt oxide catalysts not only may decline the ammonia conversion but also alter the selectivity towards N{sub 2} rather than NO. - Highlights: • Minimum reactions pathways of ammonia decomposition were studied using density functional theory. • The bonding characteristics of NH{sub x} and H on the CoO(100) surface were analysed using Layer-projected density of states. • Dehydrogenations of NH{sub 3}, NH{sub 2} and NH are highly activated. • The presence of strongly bound lattice oxygen favours the ammonia decomposition towards N{sub 2}.

Selective Hydrogenation of Acrolein Over Pd Model Catalysts: Temperature and Particle-Size Effects.

Science.gov (United States)

O'Brien, Casey P; Dostert, Karl-Heinz; Schauermann, Swetlana; Freund, Hans-Joachim

2016-10-24

The selectivity in the hydrogenation of acrolein over Fe 3 O 4 -supported Pd nanoparticles has been investigated as a function of nanoparticle size in the 220-270 K temperature range. While Pd(111) shows nearly 100 % selectivity towards the desired hydrogenation of the C=O bond to produce propenol, Pd nanoparticles were found to be much less selective towards this product. In situ detection of surface species by using IR-reflection absorption spectroscopy shows that the selectivity towards propenol critically depends on the formation of an oxopropyl spectator species. While an overlayer of oxopropyl species is effectively formed on Pd(111) turning the surface highly selective for propenol formation, this process is strongly hindered on Pd nanoparticles by acrolein decomposition resulting in CO formation. We show that the extent of acrolein decomposition can be tuned by varying the particle size and the reaction temperature. As a result, significant production of propenol is observed over 12 nm Pd nanoparticles at 250 K, while smaller (4 and 7 nm) nanoparticles did not produce propenol at any of the temperatures investigated. The possible origin of particle-size dependence of propenol formation is discussed. This work demonstrates that the selectivity in the hydrogenation of acrolein is controlled by the relative rates of acrolein partial hydrogenation to oxopropyl surface species and of acrolein decomposition, which has significant implications for rational catalyst design. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Aerosol processing: a wind of innovation in the field of advanced heterogeneous catalysts.

Science.gov (United States)

Debecker, Damien P; Le Bras, Solène; Boissière, Cédric; Chaumonnot, Alexandra; Sanchez, Clément

2018-04-16

Aerosol processing is long known and implemented industrially to obtain various types of divided materials and nanomaterials. The atomisation of a liquid solution or suspension produces a mist of aerosol droplets which can then be transformed via a diversity of processes including spray-drying, spray pyrolysis, flame spray pyrolysis, thermal decomposition, micronisation, gas atomisation, etc. The attractive technical features of these aerosol processes make them highly interesting for the continuous, large scale, and tailored production of heterogeneous catalysts. Indeed, during aerosol processing, each liquid droplet undergoes well-controlled physical and chemical transformations, allowing for example to dry and aggregate pre-existing solid particles or to synthesise new micro- or nanoparticles from mixtures of molecular or colloidal precursors. In the last two decades, more advanced reactive aerosol processes have emerged as innovative means to synthesise tailored-made nanomaterials with tunable surface properties, textures, compositions, etc. In particular, the "aerosol-assisted sol-gel" process (AASG) has demonstrated tremendous potential for the preparation of high-performance heterogeneous catalysts. The method is mainly based on the low-cost, scalable, and environmentally benign sol-gel chemistry process, often coupled with the evaporation-induced self-assembly (EISA) concept. It allows producing micronic or submicronic, inorganic or hybrid organic-inorganic particles bearing tuneable and calibrated porous structures at different scales. In addition, pre-formed nanoparticles can be easily incorporated or formed in a "one-pot" bottom-up approach within the porous inorganic or hybrid spheres produced by such spray drying method. Thus, multifunctional catalysts with tailored catalytic activities can be prepared in a relatively simple way. This account is an overview of aerosol processed heterogeneous catalysts which demonstrated interesting performance in

Activity of nanosized titania synthesized from thermal decomposition of titanium (IV n-butoxide for the photocatalytic degradation of diuron

Directory of Open Access Journals (Sweden)

Jitlada Klongdee, Wansiri Petchkroh, Kosin Phuempoonsathaporn, Piyasan Praserthdam, Alisa S. Vangnai and Varong Pavarajarn

2005-01-01

Full Text Available Nanoparticles of anatase titania were synthesized by the thermal decomposition of titanium (IV n-butoxide in 1,4-butanediol. The powder obtained was characterized by various characterization techniques, such as XRD, BET, SEM and TEM, to confirm that it was a collection of single crystal anatase with particle size smaller than 15 nm. The synthesized titania was employed as catalyst for the photodegradation of diuron, a herbicide belonging to the phenylurea family, which has been considered as a biologically active pollutant in soil and water. Although diuron is chemically stable, degradation of diuron by photocatalyzed oxidation was found possible. The conversions achieved by titania prepared were in the range of 70–80% within 6 h of reaction, using standard UV lamps, while over 99% conversion was achieved under solar irradiation. The photocatalytic activity was compared with that of the Japanese Reference Catalyst (JRC-TIO-1 titania from the Catalysis Society of Japan. The synthesized titania exhibited higher rate and efficiency in diuron degradation than reference catalyst. The results from the investigations by controlling various reaction parameters, such as oxygen dissolved in the solution, diuron concentration, as well as light source, suggested that the enhanced photocatalytic activity was the result from higher crystallinity of the synthesized titania.

Global decomposition experiment shows soil animal impacts on decomposition are climate-dependent

Czech Academy of Sciences Publication Activity Database

Wall, D.H.; Bradford, M.A.; John, M.G.St.; Trofymow, J.A.; Behan-Pelletier, V.; Bignell, D.E.; Dangerfield, J.M.; Parton, W.J.; Rusek, Josef; Voigt, W.; Wolters, V.; Gardel, H.Z.; Ayuke, F. O.; Bashford, R.; Beljakova, O.I.; Bohlen, P.J.; Brauman, A.; Flemming, S.; Henschel, J.R.; Johnson, D.L.; Jones, T.H.; Kovářová, Marcela; Kranabetter, J.M.; Kutny, L.; Lin, K.-Ch.; Maryati, M.; Masse, D.; Pokarzhevskii, A.; Rahman, H.; Sabará, M.G.; Salamon, J.-A.; Swift, M.J.; Varela, A.; Vasconcelos, H.L.; White, D.; Zou, X.

2008-01-01

Roč. 14, č. 11 (2008), s. 2661-2677 ISSN 1354-1013 Institutional research plan: CEZ:AV0Z60660521; CEZ:AV0Z60050516 Keywords : climate decomposition index * decomposition * litter Subject RIV: EH - Ecology, Behaviour Impact factor: 5.876, year: 2008

Alloy catalyst material

DEFF Research Database (Denmark)

2014-01-01

The present invention relates to a novel alloy catalyst material for use in the synthesis of hydrogen peroxide from oxygen and hydrogen, or from oxygen and water. The present invention also relates to a cathode and an electrochemical cell comprising the novel catalyst material, and the process use...... of the novel catalyst material for synthesising hydrogen peroxide from oxygen and hydrogen, or from oxygen and water....

Decomposition methods for unsupervised learning

DEFF Research Database (Denmark)

Mørup, Morten

2008-01-01

This thesis presents the application and development of decomposition methods for Unsupervised Learning. It covers topics from classical factor analysis based decomposition and its variants such as Independent Component Analysis, Non-negative Matrix Factorization and Sparse Coding...... methods and clustering problems is derived both in terms of classical point clustering but also in terms of community detection in complex networks. A guiding principle throughout this thesis is the principle of parsimony. Hence, the goal of Unsupervised Learning is here posed as striving for simplicity...... in the decompositions. Thus, it is demonstrated how a wide range of decomposition methods explicitly or implicitly strive to attain this goal. Applications of the derived decompositions are given ranging from multi-media analysis of image and sound data, analysis of biomedical data such as electroencephalography...

Dictionary-Based Tensor Canonical Polyadic Decomposition

Science.gov (United States)

Cohen, Jeremy Emile; Gillis, Nicolas

2018-04-01

To ensure interpretability of extracted sources in tensor decomposition, we introduce in this paper a dictionary-based tensor canonical polyadic decomposition which enforces one factor to belong exactly to a known dictionary. A new formulation of sparse coding is proposed which enables high dimensional tensors dictionary-based canonical polyadic decomposition. The benefits of using a dictionary in tensor decomposition models are explored both in terms of parameter identifiability and estimation accuracy. Performances of the proposed algorithms are evaluated on the decomposition of simulated data and the unmixing of hyperspectral images.

Minimizing Isolate Catalyst Motion in Metal-Assisted Chemical Etching for Deep Trenching of Silicon Nanohole Array.

Science.gov (United States)

Kong, Lingyu; Zhao, Yunshan; Dasgupta, Binayak; Ren, Yi; Hippalgaonkar, Kedar; Li, Xiuling; Chim, Wai Kin; Chiam, Sing Yang

2017-06-21

The instability of isolate catalysts during metal-assisted chemical etching is a major hindrance to achieve high aspect ratio structures in the vertical and directional etching of silicon (Si). In this work, we discussed and showed how isolate catalyst motion can be influenced and controlled by the semiconductor doping type and the oxidant concentration ratio. We propose that the triggering event in deviating isolate catalyst motion is brought about by unequal etch rates across the isolate catalyst. This triggering event is indirectly affected by the oxidant concentration ratio through the etching rates. While the triggering events are stochastic, the doping concentration of silicon offers a good control in minimizing isolate catalyst motion. The doping concentration affects the porosity at the etching front, and this directly affects the van der Waals (vdWs) forces between the metal catalyst and Si during etching. A reduction in the vdWs forces resulted in a lower bending torque that can prevent the straying of the isolate catalyst from its directional etching, in the event of unequal etch rates. The key understandings in isolate catalyst motion derived from this work allowed us to demonstrate the fabrication of large area and uniformly ordered sub-500 nm nanoholes array with an unprecedented high aspect ratio of ∼12.

Synthesis and nature of heterogeneous catalysts of low-valent tungsten supported on alumina

Energy Technology Data Exchange (ETDEWEB)

Brenner, A.; Hucul, D.A.

1980-01-01

Temperature-programed decomposition of catalysts prepared from zero-valent W(CO)/sub 6/ and alumina under rigorously air-free conditions showed a low-temperature carbon monoxide desorption peak at 110/sup 0/-172/sup 0/C, depending on alumina pretreatment, in which a relatively stable surface W(CO)/sub 3/ complex was formed; and a high-temperature carbon monoxide desorption peak at 257/sup 0/ to > 400/sup 0/C, which gave zero-valent tungsten if the ratio of hydroxyl groups of alumina to tungsten surface complexes was low, and hexavalent tungsten if the ratio was high. Up to about half the W(CO)/sub 6/ sublimated from the alumina during activation.

Catalyst for microelectromechanical systems microreactors

Science.gov (United States)

Morse, Jeffrey D [Martinez, CA; Sopchak, David A [Livermore, CA; Upadhye, Ravindra S [Pleasanton, CA; Reynolds, John G [San Ramon, CA; Satcher, Joseph H [Patterson, CA; Gash, Alex E [Brentwood, CA

2010-06-29

A microreactor comprising a silicon wafer, a multiplicity of microchannels in the silicon wafer, and a catalyst coating the microchannels. In one embodiment the catalyst coating the microchannels comprises a nanostructured material. In another embodiment the catalyst coating the microchannels comprises an aerogel. In another embodiment the catalyst coating the microchannels comprises a solgel. In another embodiment the catalyst coating the microchannels comprises carbon nanotubes.

Cellular decomposition in vikalloys

International Nuclear Information System (INIS)

Belyatskaya, I.S.; Vintajkin, E.Z.; Georgieva, I.Ya.; Golikov, V.A.; Udovenko, V.A.

1981-01-01

Austenite decomposition in Fe-Co-V and Fe-Co-V-Ni alloys at 475-600 deg C is investigated. The cellular decomposition in ternary alloys results in the formation of bcc (ordered) and fcc structures, and in quaternary alloys - bcc (ordered) and 12R structures. The cellular 12R structure results from the emergence of stacking faults in the fcc lattice with irregular spacing in four layers. The cellular decomposition results in a high-dispersion structure and magnetic properties approaching the level of well-known vikalloys [ru

Iron phthalocyanine supported on amidoximated PAN fiber as effective catalyst for controllable hydrogen peroxide activation in oxidizing organic dyes

Energy Technology Data Exchange (ETDEWEB)

Han, Zhenbang, E-mail: hzbang@aliyun.com [School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Key Laboratory of Advanced Textile Composite Materials, Ministry of Education of China, Tianjin 300387 (China); Han, Xu [School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Zhao, Xiaoming, E-mail: zhaoxiaoming@tjpu.edu.cn [School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China); Key Laboratory of Advanced Textile Composite Materials, Ministry of Education of China, Tianjin 300387 (China); Yu, Jiantao; Xu, Hang [School of Textiles, Tianjin Polytechnic University, Tianjin 300387 (China)

2016-12-15

Iron(II) phthalocyanine was immobilized onto amidoximated polyacrylonitrile fiber to construct a bioinspired catalytic system for oxidizing organic dyes by H{sub 2}O{sub 2} activation. The amidoxime groups greatly helped to anchor Iron(II) phthalocyanine molecules onto the fiber through coordination interaction, which has been confirmed by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and UV diffuse reflectance spectroscopy analyses. Electron spin resonance studies indicate that the catalytic process of physically anchored Iron(II) phthalocyanine performed via a hydroxyl radical pathway, while the catalyst bonded Iron(II) phthalocyanine through coordination effect could selectively catalyze the H{sub 2}O{sub 2} decomposition to generate high-valent iron-oxo species. This may result from the amidoxime groups functioning as the axial fifth ligands to favor the heterolytic cleavage of the peroxide O−O bond. This feature also enables the catalyst to only degrade the dyes adjacent to the catalytic active centers and enhances the efficient utilization of H{sub 2}O{sub 2}. In addition, this catalyst could effectively catalyze the mineralization of organic dyes and can be easily recycled without any loss of activity.

Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

International Nuclear Information System (INIS)

Esrafili, Mehdi D.; Sharifi, Fahimeh; Nematollahi, Parisa

2016-01-01

Highlights: • The reduction of N 2 O by CO molecule is investigated over Al- and Si-decorated graphene oxides (Al-/Si-GO). • The N 2 O decomposition process can take place with a negligible activation energy over both surfaces. • Al-GO and Si-GO can be used as an efficient metal-free catalyst for the reduction of N 2 O molecule at ambient conditions. - Abstract: The structural and catalytic properties of Al- or Si-decorated graphene oxide (Al-/Si-GO) are studied by means of density functional theory calculations. The relatively large adsorption energy together with the small Al−O or Si−O binding distances indicate that the epoxy groups over the GO surface can strongly stabilize the single Al or Si atom. Hence, Al-GO and Si-GO are stable enough to be utilized in catalytic reduction of N 2 O by CO molecule. It is found that the adsorption and decomposition of N 2 O molecule over Si-GO is more favorable than over Al-GO, due to its larger adsorption energy (E ads ) and charge transfer (q CT ) values. On the other hand, the CO molecule is physically adsorbed over both surfaces, with relatively small E ads and q CT values. Therefore, at the presence of N 2 O and CO molecules as the reaction gas, the Al or Si atom of the surface should be dominantly covered by N 2 O molecule. Our results indicate that the N 2 O decomposition process can take place with a negligible activation energy over Al-/Si-GO surface, where the N 2 molecule can be easily released from the surface. Then, the activated oxygen atom (O ads ) which remains over the surface reacts with the CO molecule to form the CO 2 molecule via the reaction O ads + CO → CO 2 . Based on the calculated activation energies, it is suggested that both Al-GO and Si-GO can be used as an efficient metal-free catalyst for the reduction of N 2 O molecule at ambient conditions.

Photochemical decomposition of H2O and HN3 using colloidal semiconductor catalysts as a method of tritium recovery from water

International Nuclear Information System (INIS)

Monserrat, K.J.; D'Souza, L.M.

1985-02-01

Colloidal semiconductor redox catalysts were used to accelerate the photodecomposition of water and ammonia in aqueous solution. Parameters that affect overall catalytic efficiency, e.g. support material, doping and surface modification, were investigated

Nitrogen Chemistry and Coke Transformation of FCC Coked Catalyst during the Regeneration Process

Science.gov (United States)

Shi, Junjun; Guan, Jianyu; Guo, Dawei; Zhang, Jiushun; France, Liam John; Wang, Lefu; Li, Xuehui

2016-06-01

Regeneration of the coked catalyst is an important process of fluid catalytic cracking (FCC) in petroleum refining, however, this process will emit environmentally harmful gases such as nitrogen and carbon oxides. Transformation of N and C containing compounds in industrial FCC coke under thermal decomposition was investigated via TPD and TPO to examine the evolved gaseous species and TGA, NMR and XPS to analyse the residual coke fraction. Two distinct regions of gas evolution are observed during TPD for the first time, and they arise from decomposition of aliphatic carbons and aromatic carbons. Three types of N species, pyrrolic N, pyridinic N and quaternary N are identified in the FCC coke, the former one is unstable and tends to be decomposed into pyridinic and quaternary N. Mechanisms of NO, CO and CO2 evolution during TPD are proposed and lattice oxygen is suggested to be an important oxygen resource. Regeneration process indicates that coke-C tends to preferentially oxidise compared with coke-N. Hence, new technology for promoting nitrogen-containing compounds conversion will benefit the in-situ reduction of NO by CO during FCC regeneration.

The fabrication of a carbon nanotube array using a catalyst-poisoning layer in the inverse nano-sphere lithography method

International Nuclear Information System (INIS)

Tsai, Tsung-Yen; Chen, Tsung-Han; Tai, Nyan-Hwa; Chang, Shih-Chin; Hsu, Hui-Chen; Joseph Palathinkal, Thomas

2009-01-01

A new method for the fabrication of periodic CNT arrays was developed in this study, which involves the use of the inverse nano-sphere lithography (INSL) process. Mo of a honeycomb pattern, acting as a catalyst-poisoning layer, was produced by the nano-sphere lithography (NSL) process; the Mo poisoned the catalyst and prevented CNT growth where deposited, and as a result, a periodic CNT pattern was obtained. Using this method, the uniformity of the CNT array can be improved by preventing the negative effect of arrangement defects in self-assembled monolayers. The size and the period of the CNT array can be adjusted by careful selection of the polystyrene (PS) sphere diameter. X-ray photoelectron spectroscope (XPS) analysis revealed that the Co catalyst was ineffective on the areas of Mo deposition due to the diffusion of Co into the Mo layer.

The fabrication of a carbon nanotube array using a catalyst-poisoning layer in the inverse nano-sphere lithography method

Energy Technology Data Exchange (ETDEWEB)

Tsai, Tsung-Yen; Chen, Tsung-Han; Tai, Nyan-Hwa; Chang, Shih-Chin; Hsu, Hui-Chen; Joseph Palathinkal, Thomas, E-mail: nhtai@mx.nthu.edu.t [Department of Materials Science and Engineering, National Tsing Hua University, 101, Section 2, Kuang-Fu Road, Hsinchu, 30013, Taiwan (China)

2009-07-29

A new method for the fabrication of periodic CNT arrays was developed in this study, which involves the use of the inverse nano-sphere lithography (INSL) process. Mo of a honeycomb pattern, acting as a catalyst-poisoning layer, was produced by the nano-sphere lithography (NSL) process; the Mo poisoned the catalyst and prevented CNT growth where deposited, and as a result, a periodic CNT pattern was obtained. Using this method, the uniformity of the CNT array can be improved by preventing the negative effect of arrangement defects in self-assembled monolayers. The size and the period of the CNT array can be adjusted by careful selection of the polystyrene (PS) sphere diameter. X-ray photoelectron spectroscope (XPS) analysis revealed that the Co catalyst was ineffective on the areas of Mo deposition due to the diffusion of Co into the Mo layer.

Enhancing Catalyzed Decomposition of Na2CO3 with Co2MnO x Nanowire-Decorated Carbon Fibers for Advanced Na-CO2 Batteries.

Science.gov (United States)

Fang, Cong; Luo, Jianmin; Jin, Chengbin; Yuan, Huadong; Sheng, Ouwei; Huang, Hui; Gan, Yongping; Xia, Yang; Liang, Chu; Zhang, Jun; Zhang, Wenkui; Tao, Xinyong

2018-05-23

The metal-CO 2 batteries, especially Na-CO 2 , batteries come into sight owing to their high energy density, ability for CO 2 capture, and the abundance of sodium resource. Besides the sluggish electrochemical reactions at the gas cathodes and the instability of the electrolyte at a high voltage, the final discharge product Na 2 CO 3 is a solid and poor conductor of electricity, which may cause the high overpotential and poor cycle performance for the Na-CO 2 batteries. The promotion of decomposition of Na 2 CO 3 should be an efficient strategy to enhance the electrochemical performance. Here, we design a facile Na 2 CO 3 activation experiment to screen the efficient cathode catalyst for the Na-CO 2 batteries. It is found that the Co 2 MnO x nanowire-decorated carbon fibers (CMO@CF) can promote the Na 2 CO 3 decomposition at the lowest voltage among all these metal oxide-decorated carbon fiber structures. After assembling the Na-CO 2 batteries, the electrodes based on CMO@CF show lower overpotential and better cycling performance compared with the electrodes based on pristine carbon fibers and other metal oxide-modified carbon fibers. We believe this catalyst screening method and the freestanding structure of the CMO@CF electrode may provide an important reference for the development of advanced Na-CO 2 batteries.

Effect of calcination temperature on the H{sub 2}O{sub 2} decomposition activity of nano-crystalline Co{sub 3}O{sub 4} prepared by combustion method

Energy Technology Data Exchange (ETDEWEB)

Makhlouf, M.Th. [Chemistry Department, Faculty of Science, Assiut University, 71516 Assiut (Egypt); Abu-Zied, B.M., E-mail: babuzied@aun.edu.eg [Chemistry Department, Faculty of Science, Assiut University, 71516 Assiut (Egypt); Mansoure, T.H. [Chemistry Department, Faculty of Science, Assiut University, 71516 Assiut (Egypt)

2013-06-01

Cobalt oxide nano-particles were prepared by combustion method using urea as a combustion fuel. The effects of calcination temperature, 350–1000 °C, on the physicochemical, surface and catalytic properties of the prepared Co{sub 3}O{sub 4} nano-particles were studied. The products were characterized by thermal analyses (TGA and DTA), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. Textural features of the obtained catalysts were investigated using nitrogen adsorption at −196 °C. X-ray diffraction confirmed that the resulting oxide was pure single-crystalline Co{sub 3}O{sub 4} nano-particles. Transmission electron microscopy indicating that, the crystallite size of Co{sub 3}O{sub 4} nano-crystals was in the range of 8–34 nm. The catalytic activities of prepared nano-crystalline Co{sub 3}O{sub 4} catalysts were tested for H{sub 2}O{sub 2} decomposition at 35–50 °C temperature range. Experimental results revealed that, the catalytic decomposition of H{sub 2}O{sub 2} decreases with increasing the calcination temperature. This was correlated with the observed particle size increase accompanying the calcination temperature rise.

Regeneration of Hydrotreating and FCC Catalysts

Energy Technology Data Exchange (ETDEWEB)

CM Wai; JG Frye; JL Fulton; LE Bowman; LJ Silva; MA Gerber

1999-09-30

Hydrotreating, hydrocracking, and fluid catalytic cracking (FCC) catalysts are important components of petroleum refining processes. Hydrotreating and hydrocracking catalysts are used to improve the yield of high-quality light oil fractions from heavier crude oil and petroleum feedstocks containing high levels of impurities. FCC catalysts improve the yield of higher octane gasoline from crude oil. Residuum hydrotreating and cracking catalysts are susceptible to irreversible deactivation caused by adsorption of sulfur and by metals impurities, such as vanadium and nickel. The gradual buildup of these impurities in a hydrotreating catalyst eventually plugs the pores and deactivates it. Nickel and vanadium adversely affect the behavior of cracking catalysts, reducing product yield and quality. Replacing deactivated catalysts represents a significant cost in petroleum refining. Equally important are the costs and potential liabilities associated with treating and disposing spent catalysts. For example, recent US Environmental Protection Agency rulings have listed spent hydrotreating and hydrorefining catalysts as hazardous wastes. FCC catalysts, though more easily disposed of as road-base or as filler in asphalt and cement, are still an economic concern mainly because of the large volumes of spent catalysts generated. New processes are being considered to increase the useful life of catalysts or for meeting more stringent disposal requirements for spent catalysts containing metals. This report discusses a collaborative effort between Pacific Northwest National Laboratory (PNNL) and Phillips Petroleum, Inc., to identify promising chemical processes for removing metals adhered to spent hydrodesulfurization (HDS, a type of hydrotreating catalyst) and FCC catalysts. This study, conducted by PNNL, was funded by the US Department of Energy's Bartlesville Project Office. Fresh and spent catalysts were provided by Phillips Petroleum. The FCC catalyst was a rare

Study on the Hydrolysis Kinetics of Xylan on Different Acid Catalysts

Energy Technology Data Exchange (ETDEWEB)

Na, Byeong-Il; Lee, Jae-Won [Chonnam National University, Gwangju (Korea, Republic of)

2014-04-15

In this study, we investigated kinetic model for the acid-catalyzed xylan hydrolysis at temperature 120-150 .deg. C. Also, we analyzed the kinetic parameters for xylose production and furfural decomposition. The hydrolysis of xylan and the degradation of xylose were promoted by high reaction temperature and acid concentration. The optimal hydrolysis condition for the highest reaction rate constants (k{sub 1}) was different depending on the acid catalysts. Among sulfuric, oxalic and maleic acid, the xylan reaction rate constants (k{sub 1}) to xylose had the highest value of 0.0241 min{sup -1} when 100 mM sulfuric acid was used at 120 .deg. C. However, sulfuric acid induced more xylose degradation compared to oxalic and maleic acid hydrolysis. The activation energy for xylan degradation was the highest when sulfuric acid was used.

Catalysts for synthetic liquid fuels

Energy Technology Data Exchange (ETDEWEB)

Bruce, L.A.; Turney, T.W.

1987-12-01

Fischer-Tropsch catalysts have been designed, characterized and tested for the selective production of hydrocarbons suitable as synthetic liquid transport fuels from synthesis gas (i.e., by the reduction of carbon monoxide with hydrogen). It was found that hydrocarbons in the middle distillate range, or suitable for conversion to that range, could be produced over several of the new catalyst systems. The various catalysts examined included: (1) synthetic cobalt clays, mainly cobalt chlorites; (2) cobalt hydrotalcites; (3) ruthenium metal supported on rare earth oxides of high surface area; and (4) a novel promoted cobalt catalyst. Active and selective catalysts have been obtained, in each category. With the exception of the clays, reproducibility of catalyst performance has been good. Catalysts in groups 2 and 4 have exhibited very high activity, with long lifetimes and easy regeneration.

Influence of vanadium oxidation states on the performance of V-Mg-Al mixed-oxide catalysts for the oxidative dehydrogenation of propane

International Nuclear Information System (INIS)

Schacht, L.; Navarrete, J.; Schacht, P.; Ramirez, M. A.

2010-01-01

V-Mg-Al mixed-oxide catalysts for oxidative dehydrogenation of propane were prepared by thermal decomposition of Mg-Al-layered double hydroxides with vanadium interlayer doping. The obtained catalysts were tested for the oxidative dehydrogenation of propane, obtaining good results in catalytic activity (conversion 16.55 % and selectivity 99.97 %) Results indicated that catalytic performance of these materials depends on how vanadium is integrated in the layered structure, which is determined by the Mg/Al ratio. Vanadium interlayer doping modifies the oxidation state of vanadium and consequently catalytic properties. Surface properties were studied by X-ray photoelectron spectroscopic and diffuse reflectance, UV-visible spectroscopy, and temperature programmed reduction. The analyses provided information about the oxidation state, before and after the reaction. From these results, it is suggested that selectivity to propylene and catalytic activity depend mainly of vanadium oxidation state. (Author)

Influence of vanadium oxidation states on the performance of V-Mg-Al mixed-oxide catalysts for the oxidative dehydrogenation of propane

Energy Technology Data Exchange (ETDEWEB)

Schacht, L. [IPN, Escuela Superior de Fisica y Matematicas, Departamento de Ciencia de Materiales, Av. IPN s/n, Edificio 9, Col. Lindavista, 07738 Mexico D. F. (Mexico); Navarrete, J.; Schacht, P.; Ramirez, M. A., E-mail: pschacha@imp.m [Instituto Mexicano del Petroleo, Programa de Ingenieria Molecular, Eje Central Lazaro Cardenas No. 152, 07730 Mexico D. F. (Mexico)

2010-07-01

V-Mg-Al mixed-oxide catalysts for oxidative dehydrogenation of propane were prepared by thermal decomposition of Mg-Al-layered double hydroxides with vanadium interlayer doping. The obtained catalysts were tested for the oxidative dehydrogenation of propane, obtaining good results in catalytic activity (conversion 16.55 % and selectivity 99.97 %) Results indicated that catalytic performance of these materials depends on how vanadium is integrated in the layered structure, which is determined by the Mg/Al ratio. Vanadium interlayer doping modifies the oxidation state of vanadium and consequently catalytic properties. Surface properties were studied by X-ray photoelectron spectroscopic and diffuse reflectance, UV-visible spectroscopy, and temperature programmed reduction. The analyses provided information about the oxidation state, before and after the reaction. From these results, it is suggested that selectivity to propylene and catalytic activity depend mainly of vanadium oxidation state. (Author)

Multiresolution signal decomposition schemes

NARCIS (Netherlands)

J. Goutsias (John); H.J.A.M. Heijmans (Henk)

1998-01-01

textabstract[PNA-R9810] Interest in multiresolution techniques for signal processing and analysis is increasing steadily. An important instance of such a technique is the so-called pyramid decomposition scheme. This report proposes a general axiomatic pyramid decomposition scheme for signal analysis

Symmetric Tensor Decomposition

DEFF Research Database (Denmark)

Brachat, Jerome; Comon, Pierre; Mourrain, Bernard

2010-01-01

We present an algorithm for decomposing a symmetric tensor, of dimension n and order d, as a sum of rank-1 symmetric tensors, extending the algorithm of Sylvester devised in 1886 for binary forms. We recall the correspondence between the decomposition of a homogeneous polynomial in n variables...... of polynomial equations of small degree in non-generic cases. We propose a new algorithm for symmetric tensor decomposition, based on this characterization and on linear algebra computations with Hankel matrices. The impact of this contribution is two-fold. First it permits an efficient computation...... of the decomposition of any tensor of sub-generic rank, as opposed to widely used iterative algorithms with unproved global convergence (e.g. Alternate Least Squares or gradient descents). Second, it gives tools for understanding uniqueness conditions and for detecting the rank....

Synthesis H-Zeolite catalyst by impregnation KI/KIO3 and performance test catalyst for biodiesel production

Science.gov (United States)

Widayat, W.; Rizky Wicaksono, Adit; Hakim Firdaus, Lukman; Okvitarini, Ndaru

2016-02-01

The objective of this research is to produce H-catalyst catalyst that was impregnated with KI/KIO3. The catalyst was analyzed about surface area, X-Ray Diffraction (XRD) and performance test of catalyst for biodiesel production. An H-Zeolite catalyst was synthesized from natural zeolite with chemical treatment processing, impregnation KI/KIO3 and physical treatment. The results shows that the surface area of the catalyst by 27.236 m2/g at a concentration of 5% KI. XRD analysis shows peak 2-θ at 23.627o indicating that KI was impregnated on H-zeolite catalyst. The catalyst was tested in production of biodiesel using palm oil with conventional methods for 3 hour at temperature of 70-80 oC. The result for conversion Fatty Acid Methyl Ester (FAME) reached maximum value on 87.91% under production process using catalyst 5% KIO3-H zeolite.

Regeneration of LOHC dehydrogenation catalysts: In-situ IR spectroscopy on single crystals, model catalysts, and real catalysts from UHV to near ambient pressure

International Nuclear Information System (INIS)

Amende, Max; Kaftan, Andre; Bachmann, Philipp; Brehmer, Richard; Preuster, Patrick; Koch, Marcus

2016-01-01

Graphical abstract: - Highlights: • We examine the regeneration of Pt-based catalysts poisoned by LOHC degradation. • A microscopic mechanism of the removal of degradation products from Pt is proposed. • Results of our UHV studies on model catalysts are transferred to real catalysis. • Oxidative regeneration of Pt/alumina is possible under mild conditions (600 K). • The degree and temperature regime of regeneration depends on the catalyst morphology. - Abstract: The Liquid Organic Hydrogen Carrier (LOHC) concept offers an efficient route to store hydrogen using organic compounds that are reversibly hydrogenated and dehydrogenated. One important challenge towards application of the LOHC technology at a larger scale is to minimize degradation of Pt-based dehydrogenation catalysts during long-term operation. Herein, we investigate the regeneration of Pt/alumina catalysts poisoned by LOHC degradation. We combine ultrahigh vacuum (UHV) studies on Pt(111), investigations on well-defined Pt/Al_2O_3 model catalysts, and near-ambient pressure (NAP) measurements on real core–shell Pt/Al_2O_3 catalyst pellets. The catalysts were purposely poisoned by reaction with the LOHC perhydro-dibenzyltoluene (H18-MSH) and with dicyclohexylmethane (DCHM) as a simpler model compound. We focus on oxidative regeneration under conditions that may be applied in real dehydrogenation reactors. The degree of poisoning and regeneration under oxidative reaction conditions was quantified using CO as a probe molecule and measured by infrared reflection-absorption spectroscopy (IRAS) and diffuse reflectance Fourier transform IR spectroscopy (DRIFTS) for planar model systems and real catalysts, respectively. We find that regeneration strongly depends on the composition of the catalyst surface. While the clean surface of a poisoned Pt(111) single crystal is fully restored upon thermal treatment in oxygen up to 700 K, contaminated Pt/Al_2O_3 model catalyst and core–shell pellet were only

Regeneration of LOHC dehydrogenation catalysts: In-situ IR spectroscopy on single crystals, model catalysts, and real catalysts from UHV to near ambient pressure

Energy Technology Data Exchange (ETDEWEB)

Amende, Max, E-mail: max.amende@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Kaftan, Andre, E-mail: andre.kaftan@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Bachmann, Philipp, E-mail: philipp.bachmann@fau.de [Lehrstuhl für Physikalische Chemie II, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Brehmer, Richard, E-mail: richard.brehmer@fau.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Preuster, Patrick, E-mail: patrick.preuster@fau.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); Koch, Marcus, E-mail: marcus.koch@crt.cbi.uni-erlangen.de [Lehrstuhl für Chemische Reaktionstechnik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen (Germany); and others

2016-01-01

Graphical abstract: - Highlights: • We examine the regeneration of Pt-based catalysts poisoned by LOHC degradation. • A microscopic mechanism of the removal of degradation products from Pt is proposed. • Results of our UHV studies on model catalysts are transferred to real catalysis. • Oxidative regeneration of Pt/alumina is possible under mild conditions (600 K). • The degree and temperature regime of regeneration depends on the catalyst morphology. - Abstract: The Liquid Organic Hydrogen Carrier (LOHC) concept offers an efficient route to store hydrogen using organic compounds that are reversibly hydrogenated and dehydrogenated. One important challenge towards application of the LOHC technology at a larger scale is to minimize degradation of Pt-based dehydrogenation catalysts during long-term operation. Herein, we investigate the regeneration of Pt/alumina catalysts poisoned by LOHC degradation. We combine ultrahigh vacuum (UHV) studies on Pt(111), investigations on well-defined Pt/Al{sub 2}O{sub 3} model catalysts, and near-ambient pressure (NAP) measurements on real core–shell Pt/Al{sub 2}O{sub 3} catalyst pellets. The catalysts were purposely poisoned by reaction with the LOHC perhydro-dibenzyltoluene (H18-MSH) and with dicyclohexylmethane (DCHM) as a simpler model compound. We focus on oxidative regeneration under conditions that may be applied in real dehydrogenation reactors. The degree of poisoning and regeneration under oxidative reaction conditions was quantified using CO as a probe molecule and measured by infrared reflection-absorption spectroscopy (IRAS) and diffuse reflectance Fourier transform IR spectroscopy (DRIFTS) for planar model systems and real catalysts, respectively. We find that regeneration strongly depends on the composition of the catalyst surface. While the clean surface of a poisoned Pt(111) single crystal is fully restored upon thermal treatment in oxygen up to 700 K, contaminated Pt/Al{sub 2}O{sub 3} model catalyst and

Thermal decomposition of beryllium perchlorate tetrahydrate

International Nuclear Information System (INIS)

Berezkina, L.G.; Borisova, S.I.; Tamm, N.S.; Novoselova, A.V.

1975-01-01

Thermal decomposition of Be(ClO 4 ) 2 x4H 2 O was studied by the differential flow technique in the helium stream. The kinetics was followed by an exchange reaction of the perchloric acid appearing by the decomposition with potassium carbonate. The rate of CO 2 liberation in this process was recorded by a heat conductivity detector. The exchange reaction yielding CO 2 is quantitative, it is not the limiting one and it does not distort the kinetics of the process of perchlorate decomposition. The solid products of decomposition were studied by infrared and NMR spectroscopy, roentgenography, thermography and chemical analysis. A mechanism suggested for the decomposition involves intermediate formation of hydroxyperchlorate: Be(ClO 4 ) 2 x4H 2 O → Be(OH)ClO 4 +HClO 4 +3H 2 O; Be(OH)ClO 4 → BeO+HClO 4 . Decomposition is accompained by melting of the sample. The mechanism of decomposition is hydrolytic. At room temperature the hydroxyperchlorate is a thick syrup-like compound crystallizing after long storing

Effect of process temperature on morphology of CNTs grown in a vertically fluidized bed reactor with Fe{sub 2}O{sub 3}/Al{sub 2}O{sub 3} catalyst

Energy Technology Data Exchange (ETDEWEB)

Shukrullah, Shazia, E-mail: zshukrullah@gmail.com; Mohamed, Norani Muti, E-mail: noranimuti-mohamed@petronas.com.my; Shaharun, Maizatul Shima, E-mail: maizats@petronas.com.my [Department of Fundamental and Applied Sciences, Universiti Teknologi PETRONAS, 31750 Tronoh, Perak (Malaysia)

2015-07-22

Carbon nanotubes (CNTs) are one of the most researched materials due to their exceptional mechanical and electrical properties. Among the various techniques, catalytic chemical vapor deposition in a fluidized bed reactor is the most promising technique for bulk production of CNTs. To meet the demand of good quality along with the bulk production of CNTs, the effect of reaction temperature on the micro structures, morphology, diameter, quality and quantity of CNTs was investigated in these studies. CNTs were synthesized at process temperature ranging from 700-850°C by catalytic decomposition of C{sub 2}H{sub 4} on Fe{sub 2}O{sub 3}/Al{sub 2}O{sub 3} catalyst a vertical fluidized bed reactor. The microstructures of the grown CNTs at different reaction temperatures were investigated by using scanning electron microscope. The results of this study depicted a positive correlation between the average diameter of CNTs and reaction temperature. Narrow diameters (35∼40 nm) of CNTs with fewer defects were found at the low and mild temperatures, in particular 800°C. At this temperature, a dynamic equilibrium between the rate of C{sub 2}H{sub 4} decomposition and CNTs quantity was found due to maximum carbon diffusion over catalyst. The CNTs produced with Fe{sub 2}O{sub 3}/Al{sub 2}O{sub 3} catalyst wer e also exhibiting high quality with relatively small mean outer diameter and fewer surface defects.

Development of high performance catalyst for off-gas treatment system in BWR

International Nuclear Information System (INIS)

Kawasaki, Toru; Kawabe, Kenichi; Maeda, Kiyomitsu; Matsubara, Hirofumi; Aizawa, Motohiro; Iizuka, Hidehiro; Kumagai, Naoki

2011-01-01

A high performance catalyst for off-gas treatment system in boiling water reactor (BWR) has been developed. The hydrogen concentration in the outlets of off-gas recombiners increased at several BWR plants in Japan. These phenomena were caused by deactivation of catalysts for the recombiners, and we assumed two types of deactivation mechanisms. The first cause was an increase of the amount of boehmite in the catalyst support due to alternation of the manufacturing process. The other cause was catalysts being poisoned by cyclic siloxanes that were introduced from the silicone sealant used in the upstream of the off-gas recombiners. The catalysts were manufactured by Pt adhering on alumina support. The conventional catalyst (CAT-A) used the aqueous solution of the chloroplatinic acid for adhesion of Pt. A dechlorination process by autoclave was applied to prevent the equipment at the downstream of the recombiners from stress corrosion cracking, but this process caused the support material to transform into boehmite. The boehmite-rich catalysts were deactivated more easily by organic silicon than gamma alumina-rich catalysts. Therefore, the CAT-A was replaced at many Japanese BWR plants by the improved catalyst (CAT-B), and their support was transformed into more stable gamma alumina by heating at 500degC. However, the siloxanes keep being detected in the off-gas though the source of siloxane had been removed and there still remain possibilities to deactivate the catalysts. Therefore, we have been developing high performance catalyst (CAT-C) that has higher activity and durability against poisoning. We investigated the properties of CAT-C by performance tests and instrumental analyses. The dependency of thermal output of nuclear reactor, and durability against siloxane poisoning were investigated. We found that CAT-C showed higher performance and better properties than CAT-B did. Moreover, we have been developing a modeling method to evaluate the hydrogen recombination

Surface chemistry and catalytic properties of VO{sub X}/Ti-MCM-41 catalysts for dibenzothiophene oxidation in a biphasic system

Energy Technology Data Exchange (ETDEWEB)

González, J. [ESIQIE, Instituto Politécnico Nacional, Av. Instituto Politécnico Nacional s/n, 07738 Col. Zacatenco, Mexico City (Mexico); Chen, L.F., E-mail: lchen@ipn.mx [ESIQIE, Instituto Politécnico Nacional, Av. Instituto Politécnico Nacional s/n, 07738 Col. Zacatenco, Mexico City (Mexico); Wang, J.A.; Manríquez, Ma.; Limas, R. [ESIQIE, Instituto Politécnico Nacional, Av. Instituto Politécnico Nacional s/n, 07738 Col. Zacatenco, Mexico City (Mexico); Schachat, P.; Navarrete, J. [Dirección de Investigación, Instituto Mexicano del Petróleo, Eje Lázaro Cárdenas 152, 07730 México D.F. (Mexico); Contreras, J.L. [Laboratorio de Catálisis y Polímeros, División de Ciencias Básicas e Ingeniería, Universidad Autónoma Metropolitana-A, Av. San Pablo No. 180, 02200 México D.F. (Mexico)

2016-08-30

Highlights: • Oxidative desulfurization of model diesel was tested in a biphasic system. • ODS activity was proportional to the V{sup 5+}/(V{sup 4+} + V{sup 5+}) values of the catalysts. • Lewis acidity was related to vanadium content and catalytic activity. • 99.9% DBT was oxidized using 25%V{sub 2}O{sub 5}/Ti-MCM-41 at 60 °C within 60 min. - Abstract: A series of vanadium oxide supported on Ti-MCM-41 catalysts was synthesized via the incipient impregnation method by varying the vanadia loading from 5 wt% to 10, 15, 20 and 25 wt%. These catalysts were characterized by a variety of advanced techniques for investigating their crystalline structure, textural properties, and surface chemistry information including surface acidity, reducibility, vanadium oxidation states, and morphological features. The catalytic activities of the catalysts were evaluated in a biphasic reaction system for oxidative desulfurization (ODS) of a model diesel containing 300 ppm of dibenzothiophene (DBT) where acetonitrile was used as extraction solvent and H{sub 2}O{sub 2} as oxidant. ODS activity was found to be proportional to the V{sup 5+}/(V{sup 4+} + V{sup 5+}) values of the catalysts, indicating that the surface vanadium pentoxide (V{sub 2}O{sub 5}) was the active phase. Reaction temperature would influence significantly the ODS efficiency; high temperature, i.e., 80 °C, would lead to low ODS reaction due to the partial decomposition of oxidant. All the catalysts contained both Lewis and Brønsted acid sites but the former was predominant. The catalysts with low vanadia loading (5 or 10 wt%V{sub 2}O{sub 5}) had many Lewis acid sites and could strongly adsorb DBT molecule via the electron donation/acceptance action which resulted in an inhibition for the reaction of DBT with the surface peroxometallic species. The catalyst with high vanadia loading (25wt%V{sub 2}O{sub 5}/Ti-MCM-41) showed the highest catalytic activity and could remove 99.9% of DBT at 60 °C within 60 min.

Enhanced decomposition of dimethyl phthalate via molecular oxygen activated by Fe-Fe{sub 2}O{sub 3}/AC under microwave irradiation

Energy Technology Data Exchange (ETDEWEB)

Chen, Yiling [Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079 (China); Ai, Zhihui, E-mail: jennifer.ai@mail.ccnu.edu.cn [Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079 (China); Zhang, Lizhi [Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079 (China)

2012-10-15

Highlights: Black-Right-Pointing-Pointer Microwave irradiation induces the electrons transferring from AC to Fe-Fe{sub 2}O{sub 3} and reacts with molecular oxygen. Black-Right-Pointing-Pointer Microwave heating accelerates the electron transferring from AC to Fe-Fe{sub 2}O{sub 3} to generate reactive oxygen species. Black-Right-Pointing-Pointer This environmental remediation method is feasible for aqueous organic pollutants treatment. - Abstract: In this study, we demonstrate that the decomposition of dimethyl phthalate under microwave irradiation could be greatly enhanced over Fe-Fe{sub 2}O{sub 3} nanowires supported on activated carbon (Fe-Fe{sub 2}O{sub 3}/AC). The great enhanced decomposition of dimethyl phthalate could be attributed to a unique microwave induced molecular oxygen activation process. Upon microwave irradiation, electrons could be transferred from activated carbon to zero-valent iron, and then react with molecular oxygen to form O{sub 2}{center_dot}{sup -} and {center_dot}OH radicals for the decomposition of dimethyl phthalate. The deactivation and the regeneration of Fe-Fe{sub 2}O{sub 3}/AC catalyst were systematically studied. We also found that microwave heating could accelerate the electron transferring from AC to Fe-Fe{sub 2}O{sub 3} to generate more reactive oxygen species for the decomposition of DMP than conventional oil bath heating. This novel molecular oxygen activation approach may find applications for wastewater treatment and drinking water purification.

Nanoscale intimacy in bifunctional catalysts for selective conversion of hydrocarbons

Science.gov (United States)

Zecevic, Jovana; Vanbutsele, Gina; de Jong, Krijn P.; Martens, Johan A.

2015-12-01

The ability to control nanoscale features precisely is increasingly being exploited to develop and improve monofunctional catalysts. Striking effects might also be expected in the case of bifunctional catalysts, which are important in the hydrocracking of fossil and renewable hydrocarbon sources to provide high-quality diesel fuel. Such bifunctional hydrocracking catalysts contain metal sites and acid sites, and for more than 50 years the so-called intimacy criterion has dictated the maximum distance between the two types of site, beyond which catalytic activity decreases. A lack of synthesis and material-characterization methods with nanometre precision has long prevented in-depth exploration of the intimacy criterion, which has often been interpreted simply as ‘the closer the better’ for positioning metal and acid sites. Here we show for a bifunctional catalyst—comprising an intimate mixture of zeolite Y and alumina binder, and with platinum metal controllably deposited on either the zeolite or the binder—that closest proximity between metal and zeolite acid sites can be detrimental. Specifically, the selectivity when cracking large hydrocarbon feedstock molecules for high-quality diesel production is optimized with the catalyst that contains platinum on the binder, that is, with a nanoscale rather than closest intimacy of the metal and acid sites. Thus, cracking of the large and complex hydrocarbon molecules that are typically derived from alternative sources, such as gas-to-liquid technology, vegetable oil or algal oil, should benefit especially from bifunctional catalysts that avoid locating platinum on the zeolite (the traditionally assumed optimal location). More generally, we anticipate that the ability demonstrated here to spatially organize different active sites at the nanoscale will benefit the further development and optimization of the emerging generation of multifunctional catalysts.

Effect of Different Catalyst Deposition Technique on Aligned Multiwalled Carbon Nanotubes Grown by Thermal Chemical Vapor Deposition

Directory of Open Access Journals (Sweden)

Mohamed Shuaib Mohamed Saheed

2014-01-01

Full Text Available The paper reported the investigation of the substrate preparation technique involving deposition of iron catalyst by electron beam evaporation and ferrocene vaporization in order to produce vertically aligned multiwalled carbon nanotubes array needed for fabrication of tailored devices. Prior to the growth at 700°C in ethylene, silicon dioxide coated silicon substrate was prepared by depositing alumina followed by iron using two different methods as described earlier. Characterization analysis revealed that aligned multiwalled carbon nanotubes array of 107.9 µm thickness grown by thermal chemical vapor deposition technique can only be achieved for the sample with iron deposited using ferrocene vaporization. The thick layer of partially oxidized iron film can prevent the deactivation of catalyst and thus is able to sustain the growth. It also increases the rate of permeation of the hydrocarbon gas into the catalyst particles and prevents agglomeration at the growth temperature. Combination of alumina-iron layer provides an efficient growth of high density multiwalled carbon nanotubes array with the steady growth rate of 3.6 µm per minute for the first 12 minutes and dropped by half after 40 minutes. Thicker and uniform iron catalyst film obtained from ferrocene vaporization is attributed to the multidirectional deposition of particles in the gaseous form.

Some nonlinear space decomposition algorithms

Energy Technology Data Exchange (ETDEWEB)

Tai, Xue-Cheng; Espedal, M. [Univ. of Bergen (Norway)

1996-12-31

Convergence of a space decomposition method is proved for a general convex programming problem. The space decomposition refers to methods that decompose a space into sums of subspaces, which could be a domain decomposition or a multigrid method for partial differential equations. Two algorithms are proposed. Both can be used for linear as well as nonlinear elliptic problems and they reduce to the standard additive and multiplicative Schwarz methods for linear elliptic problems. Two {open_quotes}hybrid{close_quotes} algorithms are also presented. They converge faster than the additive one and have better parallelism than the multiplicative method. Numerical tests with a two level domain decomposition for linear, nonlinear and interface elliptic problems are presented for the proposed algorithms.

Spent catalyst waste management. A review. Part 1. Developments in hydroprocessing catalyst waste reduction and use

Energy Technology Data Exchange (ETDEWEB)

Marafi, M.; Stanislaus, A. [Petroleum Refining Department, Petroleum Research and Studies Center, Kuwait Institute for Scientific Research, P.O. Box 24885, 13109-Safat (Kuwait)

2008-04-15

Solid catalysts containing metals, metal oxides or sulfides, which play a key role in the refining of petroleum to clean fuels and many other valuable products, become solid wastes after use. In many refineries, the spent catalysts discarded from hydroprocessing units form a major part of these solid wastes. Disposal of spent hydroprocessing catalysts requires compliance with stringent environmental regulations because of their hazardous nature and toxic chemicals content. Various options such as minimizing spent catalyst waste generation by regeneration and reuse, metals recovery, utilization to produce useful materials and treatment for safe disposal, could be considered to deal with the spent catalyst environmental problem. In this paper, information available in the literature on spent hydroprocessing catalyst waste reduction at source by using improved more active and more stable catalysts, regeneration, rejuvenation and reuse of deactivated catalysts in many cycles, and reusing in other processes are reviewed in detail with focus on recent developments. Available methods for recycling of spent hydroprocessing catalysts by using them as raw materials for the preparation of active new catalysts and many other valuable products are also reviewed. (author)

Automotive Catalyst State Diagnosis Using Microwaves

Directory of Open Access Journals (Sweden)

Moos Ralf

2015-01-01

Full Text Available The state of catalysts plays a key role in automotive exhaust gas aftertreatment. The soot or ash loading of Diesel particulate filters, the oxygen loading degree in three-way catalysts, the amount of stored ammonia in SCR catalysts, or the NOx loading degree in NOx storage catalysts are important parameters that are today determined indirectly and in a model-based manner with gas sensors installed upstream and/or downstream of the catalysts. This contribution gives an overview on a novel approach to determine the catalyst state directly by a microwave-based technique. The method exploits the fact that the catalyst housing acts as a microwave cavity resonator. As “sensing” elements, one or two simple antennas are mounted inside the catalyst canning. The electrical properties of the catalyst device (ceramic honeycomb plus coating and storage material can be measured. Preferably, the resonance characteristics, e.g., the resonance frequencies, of selected cavity modes are observed. The information on the catalyst interior obtained in such a contactless manner is very well correlated with the catalyst state as will be demonstrated for different exhaust gas aftertreatment systems.

Catalyst in Basic Oleochemicals

Directory of Open Access Journals (Sweden)

Eva Suyenty

2007-10-01

Full Text Available Currently Indonesia is the world largest palm oil producer with production volume reaching 16 million tones per annum. The high crude oil and ethylene prices in the last 3 – 4 years contribute to the healthy demand growth for basic oleochemicals: fatty acids and fatty alcohols. Oleochemicals are starting to replace crude oil derived products in various applications. As widely practiced in petrochemical industry, catalyst plays a very important role in the production of basic oleochemicals. Catalytic reactions are abound in the production of oleochemicals: Nickel based catalysts are used in the hydrogenation of unsaturated fatty acids; sodium methylate catalyst in the transesterification of triglycerides; sulfonic based polystyrene resin catalyst in esterification of fatty acids; and copper chromite/copper zinc catalyst in the high pressure hydrogenation of methyl esters or fatty acids to produce fatty alcohols. To maintain long catalyst life, it is crucial to ensure the absence of catalyst poisons and inhibitors in the feed. The preparation methods of nickel and copper chromite catalysts are as follows: precipitation, filtration, drying, and calcinations. Sodium methylate is derived from direct reaction of sodium metal and methanol under inert gas. The sulfonic based polystyrene resin is derived from sulfonation of polystyrene crosslinked with di-vinyl-benzene. © 2007 BCREC UNDIP. All rights reserved.[Presented at Symposium and Congress of MKICS 2007, 18-19 April 2007, Semarang, Indonesia][How to Cite: E. Suyenty, H. Sentosa, M. Agustine, S. Anwar, A. Lie, E. Sutanto. (2007. Catalyst in Basic Oleochemicals. Bulletin of Chemical Reaction Engineering and Catalysis, 2 (2-3: 22-31.  doi:10.9767/bcrec.2.2-3.6.22-31][How to Link/DOI: http://dx.doi.org/10.9767/bcrec.2.2-3.6.22-31 || or local: http://ejournal.undip.ac.id/index.php/bcrec/article/view/6

Synthesis of subnanometer-diameter vertically aligned single-walled carbon nanotubes with copper-anchored cobalt catalysts

Science.gov (United States)

Cui, Kehang; Kumamoto, Akihito; Xiang, Rong; An, Hua; Wang, Benjamin; Inoue, Taiki; Chiashi, Shohei; Ikuhara, Yuichi; Maruyama, Shigeo

2016-01-01

We synthesize vertically aligned single-walled carbon nanotubes (VA-SWNTs) with subnanometer diameters on quartz (and SiO2/Si) substrates by alcohol CVD using Cu-anchored Co catalysts. The uniform VA-SWNTs with a nanotube diameter of 1 nm are synthesized at a CVD temperature of 800 °C and have a thickness of several tens of μm. The diameter of SWNTs was reduced to 0.75 nm at 650 °C with the G/D ratio maintained above 24. Scanning transmission electron microscopy energy-dispersive X-ray spectroscopy (EDS-STEM) and high angle annular dark field (HAADF-STEM) imaging of the Co/Cu bimetallic catalyst system showed that Co catalysts were captured and anchored by adjacent Cu nanoparticles, and thus were prevented from coalescing into a larger size, which contributed to the small diameter of SWNTs. The correlation between the catalyst size and the SWNT diameter was experimentally clarified. The subnanometer-diameter and high-quality SWNTs are expected to pave the way to replace silicon for next-generation optoelectronic and photovoltaic devices.We synthesize vertically aligned single-walled carbon nanotubes (VA-SWNTs) with subnanometer diameters on quartz (and SiO2/Si) substrates by alcohol CVD using Cu-anchored Co catalysts. The uniform VA-SWNTs with a nanotube diameter of 1 nm are synthesized at a CVD temperature of 800 °C and have a thickness of several tens of μm. The diameter of SWNTs was reduced to 0.75 nm at 650 °C with the G/D ratio maintained above 24. Scanning transmission electron microscopy energy-dispersive X-ray spectroscopy (EDS-STEM) and high angle annular dark field (HAADF-STEM) imaging of the Co/Cu bimetallic catalyst system showed that Co catalysts were captured and anchored by adjacent Cu nanoparticles, and thus were prevented from coalescing into a larger size, which contributed to the small diameter of SWNTs. The correlation between the catalyst size and the SWNT diameter was experimentally clarified. The subnanometer-diameter and high

Nanostructured CoP: An efficient catalyst for degradation of organic pollutants by activating peroxymonosulfate

Energy Technology Data Exchange (ETDEWEB)

Luo, Rui; Liu, Chao; Li, Jiansheng, E-mail: lijsh@mail.njust.edu.cn; Wang, Jing; Hu, Xingru; Sun, Xiuyun; Shen, Jinyou; Han, Weiqing; Wang, Lianjun

2017-05-05

Highlights: • The CoP/PMS system was first presented for decomposition of pollutants. • CoP exhibited dramatic catalytic activity. • Broadened pH range and favorable anti-interference of anions were achieved. • A possible mechanism for activation of PMS by CoP was proposed. - Abstract: A new catalyst system of CoP/peroxymonosulfate (PMS) is presented, which achieved significant improvement in catalytic activity. Nanostructured CoP, obtained by a simple solid-state reaction, exhibited dramatic catalytic activity with 97.2% degradation of orange II of 100 ppm within 4 min. Moreover, the high efficiency could be reached for other phenolic pollutants, i.e., phenol and 4-chlorophenol. The reaction rate is much higher than the most reported catalysts. Effect of parameters on catalytic activity of the catalyst was studied in detail. Notably, initial pH of the solution had a slight negative effect on the catalytic performance over the pH range 4.07–10.92, suggesting that CoP has the great adaptability of pH. CoP/PMS demonstrated excellent anti-interference performance toward anions (Cl{sup −}, NO{sub 3}{sup −}, and HCO{sub 3}{sup −}). In addition, the pathway of degradation of orange II is proposed by analyzing its intermediates. Based on the XPS spectra of CoP, the identification of the reactive species (·OH and SO{sub 4}·{sup −}) by electron paramagnetic resonance (EPR) analysis and quenching tests, a possible mechanism for activation of PMS by CoP was proposed. Considering the dramatic catalytic activity, a wide range of pH catalyst suited, CoP is believed to provide robust support for the promising industrial application of AOPs.

Decomposition of Multi-player Games

Science.gov (United States)

Zhao, Dengji; Schiffel, Stephan; Thielscher, Michael

Research in General Game Playing aims at building systems that learn to play unknown games without human intervention. We contribute to this endeavour by generalising the established technique of decomposition from AI Planning to multi-player games. To this end, we present a method for the automatic decomposition of previously unknown games into independent subgames, and we show how a general game player can exploit a successful decomposition for game tree search.

Detailed profiling of CNTs arrays along the growth window in a floating catalyst reactor

International Nuclear Information System (INIS)

Maghrebi, Morteza; Khodadadi, Abbas Ali; Mortazavi, Yadollah; Mhaisalkar, Subodh

2009-01-01

We report a detailed longitudinal and depth profiles of multi-wall carbon nanotubes (CNTs) arrays synthesized using xylene and ferrocene in a floating catalyst reactor. Point to point analyses of the CNTs grown in a 'growth window' with CNTs arrays longer than 0.5 mm were performed using optical microscopy, Raman spectroscopy, FESEM, high-resolution TGA/DTA, and TEM techniques. The heights of the CNTs arrays show a maximum at a mid point of the growth window, while a reverse trend of minimum is observed for iron-to-CNTs atomic ratios. The ratio of amorphous carbon to CNTs sharply increases along the growth window and from the bottom to top of CNTs arrays. The CNTs diameter also increases along the growth window, due to deposition of the amorphous carbon, which can be almost removed by temperature programmed oxidation up to around 500 deg. C. A base growth mechanism, the variations of catalyst content, residence time and temperature profile along the growth window, the adsorption and decomposition of polycyclic aromatic hydrocarbons to amorphous carbon, and a limited diffusion of hydrocarbon species through the arrays covered by excessive amorphous carbon may explain the results.

Hydroprocessing catalysts utilization and regeneration schemes

Energy Technology Data Exchange (ETDEWEB)

Furimsky, E.

The catalyst reactor inventory represents an important part of the cost of hydroprocessing operation. The selection of a suitable catalyst and reactor is influenced by feedstock properties. Processes ensuring an uninterrupted operation during catalyst addition and withdrawal are preferred for processing high asphaltene and metal content feedstocks. The spent catalyst can be regenerated and returned to the operation if the extent of its deactivation is not high. The regeneration may be performed either in-situ or off-site. The former is suitable for fixed bed reactors whereas the catalyst from ebullated bed reactors must be regenerated off-site. The regeneration of spent catalysts heavily loaded with metals such as V, Ni and Fe may not be economic. Such catalysts may be suitable for metal reclamation. An environmentally safe method for catalyst disposal must be found if neither regeneration nor metal reclamation from spent catalysts can be performed.

Systematic Identification of Promoters for Methane Oxidation Catalysts Using Size- and Composition-Controlled Pd-Based Bimetallic Nanocrystals.

Science.gov (United States)

Willis, Joshua J; Goodman, Emmett D; Wu, Liheng; Riscoe, Andrew R; Martins, Pedro; Tassone, Christopher J; Cargnello, Matteo

2017-08-30

Promoters enhance the performance of catalytic active phases by increasing rates, stability, and/or selectivity. The process of identifying promoters is in most cases empirical and relies on testing a broad range of catalysts prepared with the random deposition of active and promoter phases, typically with no fine control over their localization. This issue is particularly relevant in supported bimetallic systems, where two metals are codeposited onto high-surface area materials. We here report the use of colloidal bimetallic nanocrystals to produce catalysts where the active and promoter phases are colocalized to a fine extent. This strategy enables a systematic approach to study the promotional effects of several transition metals on palladium catalysts for methane oxidation. In order to achieve these goals, we demonstrate a single synthetic protocol to obtain uniform palladium-based bimetallic nanocrystals (PdM, M = V, Mn, Fe, Co, Ni, Zn, Sn, and potentially extendable to other metal combinations) with a wide variety of compositions and sizes based on high-temperature thermal decomposition of readily available precursors. Once the nanocrystals are supported onto oxide materials, thermal treatments in air cause segregation of the base metal oxide phase in close proximity to the Pd phase. We demonstrate that some metals (Fe, Co, and Sn) inhibit the sintering of the active Pd metal phase, while others (Ni and Zn) increase its intrinsic activity compared to a monometallic Pd catalyst. This procedure can be generalized to systematically investigate the promotional effects of metal and metal oxide phases for a variety of active metal-promoter combinations and catalytic reactions.

Alternative alkali resistant deNOx catalysts

DEFF Research Database (Denmark)

Putluru, Siva Sankar Reddy; Kristensen, Steffen Buus; Due-Hansen, Johannes

2012-01-01

by onepot sol–gel method. All catalysts were characterized by BET, XRPD and NH3-TPD. Initial SCR activities of 8 out of 9 catalysts showed higher NO conversion at least at one temperature in the temperature range 300–500 ◦C compared to the conventional V2O5-WO3/TiO2 catalyst. After potassium poisoning (100......Alternative alkali resistant deNOx catalysts were prepared using three different supports ZrO2, TiO2 and Mordenite zeolite. The majority of the catalysts were prepared by incipient wetness impregnation of a commercial support, with vanadium, copper or iron precursor, one catalyst was prepared......–130 µmol of K/g of catalyst) the relative drop in SCR activity and acidity was lower for all the alternative catalysts compared to the industrial V2O5-WO3/TiO2 catalyst. Furthermore, Cu/MOR and Nano-V2O5/Sul-TiO2 catalysts showed 8–16 times higher SCR activities than the conventional even after high...

Nano-Engineered Catalysts for Direct Methanol Fuel Cells

Science.gov (United States)

Myung, Nosang; Narayanan, Sekharipuram; Wiberg, Dean

2008-01-01

, determine the sizes and surface areas of the catalytic particles. Hence, the small features and large surface areas of the porosity translate to the desired small particle size and large surface area of the catalyst (see figure). When polytetrafluoroethylene is included, it is for the purpose of imparting hydrophobicity in order to prevent water from impeding the desired diffusion of gases through the catalyst layer. To incorporate polytetrafluoroethylene into a catalytic-metal/polytetrafluoroethylene nanocomposite, one suspends polytetrafluoroethylene nanoparticles in the electrodeposition solution. The polytetrafluoroethylene content can be varied to obtain the desired degree of hydrophobicity and permeability by gas.

Production of ammonia from plasma-catalytic decomposition of urea: Effects of carrier gas composition.

Science.gov (United States)

Fan, Xing; Li, Jian; Qiu, Danqi; Zhu, Tianle

2018-04-01

Effects of carrier gas composition (N 2 /air) on NH 3 production, energy efficiency regarding NH 3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al 2 O 3 -packed dielectric barrier discharge (DBD) reactor at room temperature. Results show that the presence of O 2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH 3 . The final yield of NH 3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23kV, respectively when air was used as the carrier gas instead of N 2 . From the viewpoint of energy savings, however, air carrier gas is better than N 2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al 2 O 3 catalyst to give NH 3 and CO 2 as the main products. Compared to a small amount of N 2 O formed with N 2 as the carrier gas, however, more byproducts including N 2 O and NO 2 in the gas phase and NH 4 NO 3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH 3 , the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma. Copyright © 2017. Published by Elsevier B.V.

In-situ characterization of heterogeneous catalysts

CERN Document Server

Rodriguez, Jose A; Chupas, Peter J

2013-01-01

Helps researchers develop new catalysts for sustainable fuel and chemical production Reviewing the latest developments in the field, this book explores the in-situ characterization of heterogeneous catalysts, enabling readers to take full advantage of the sophisticated techniques used to study heterogeneous catalysts and reaction mechanisms. In using these techniques, readers can learn to improve the selectivity and the performance of catalysts and how to prepare catalysts as efficiently as possible, with minimum waste. In-situ Characterization of Heterogeneous Catalysts feat

Reuse of Hydrotreating Spent Catalyst

International Nuclear Information System (INIS)

Habib, A.M.; Menoufy, M.F.; Amhed, S.H.

2004-01-01

All hydro treating catalysts used in petroleum refining processes gradually lose activity through coking, poisoning by metal, sulfur or halides or lose surface area from sintering at high process temperatures. Waste hydrotreating catalyst, which have been used in re-refining of waste lube oil at Alexandria Petroleum Company (after 5 years lifetime) compared with the same fresh catalyst were used in the present work. Studies are conducted on partial extraction of the active metals of spent catalyst (Mo and Ni) using three leaching solvents,4% oxidized oxalic acid, 10% aqueous sodium hydroxide and 10% citric acid. The leaching experiments are conducting on the de coked extrude [un crushed] spent catalyst samples. These steps are carried out in order to rejuvenate the spent catalyst to be reused in other reactions. The results indicated that 4% oxidized oxalic acid leaching solution gave total metal removal 45.6 for de coked catalyst samples while NaOH gave 35% and citric acid gave 31.9 % The oxidized leaching agent was the most efficient leaching solvent to facilitate the metal removal, and the rejuvenated catalyst was characterized by the unchanged crystalline phase The rejuvenated catalyst was applied for hydrodesulfurization (HDS) of vacuum gas oil as a feedstock, under different hydrogen pressure 20-80 bar in order to compare its HDS activity

ALKALI RESISTANT CATALYST

DEFF Research Database (Denmark)

2008-01-01

The present invention concerns the selective removal of nitrogen oxides (NOx) from gasses. In particular, the invention concerns a process, a catalyst and the use of a catalyst for the selective removal of nitrogen oxides in the presence of ammonia from gases containing a significant amount...... of alkali metal and/or alkali-earth compounds which process comprises using a catalyst combined of (i) a formed porous superacidic support, said superacidic support having an Hammett acidity stronger than Ho=-12, and (ii) a metal oxide catalytic component deposited on said superacidic support selected from...

Syngas production from ethanol dry reforming over Rh/CeO2 catalyst

Directory of Open Access Journals (Sweden)

Shulin Zhao

2018-01-01

Full Text Available Carbon dioxide reforming of ethanol over Rh/CeO2 catalyst was deeply investigated at different reaction temperatures of 450–700 °C and reactant ratios (CO2/ethanol from 1 to 3 under atmospheric pressure. The obtained results indicated that Rh/CeO2 catalyst presented a promising activity and stability for syngas production from renewable bio-ethanol instead of conventional methane. Typically, CO2-rich conditions (CO2/ethanol = 3 were favorable for reaction process and dynamic coke cleaning, which led to remarkably stable performance over 65 h on stream. The strong redox capacity of CeO2 support might also accelerate CO2 activation and prevent the carbon accumulation over the catalyst surface. Additionally, tunable H2/CO ratios were available by changing the CO2/ethanol ratios. The results from characterization of samples before and after catalytic tests allowed to establish the relationship between textural properties and catalytic performance.

The influence of desilication on high-silica MFI and its catalytic performance for N2O decomposition

Science.gov (United States)

Shen, Qun; Wu, Minfang; Wang, Hui; Sun, Nannan; He, Chi; Wei, Wei

2018-05-01

A series of MFI zeolites with different Si/Al ratios were pretreated by a basic solution and their catalytic activity was evaluated in N2O decomposition after iron exchange. The performance of Fe-ZSM-5 catalysts could be improved by alkaline pretreatment. Among these samples, the activity curve of Fe-Z5-250-S sample could move to low temperature by >100 °C with a good preservation of hydrothermal stability. It is found that with the meso-microporous hybrid structure, the content of iron as active metal is significantly increased. Additionally, well preservation of the chemical environment around the tetrahedral aluminum and the site accessibility probably may be the other important factors to influence the catalytic activity.

Decomposition of diesel oil by various microorganisms

Energy Technology Data Exchange (ETDEWEB)

Suess, A; Netzsch-Lehner, A

1969-01-01

Previous experiments demonstrated the decomposition of diesel oil in different soils. In this experiment the decomposition of /sup 14/C-n-Hexadecane labelled diesel oil by special microorganisms was studied. The results were as follows: (1) In the experimental soils the microorganisms Mycoccus ruber, Mycobacterium luteum and Trichoderma hamatum are responsible for the diesel oil decomposition. (2) By adding microorganisms to the soil an increase of the decomposition rate was found only in the beginning of the experiments. (3) Maximum decomposition of diesel oil was reached 2-3 weeks after incubation.

Thermal and catalytic decomposition behavior of PVC mixed plastic waste with petroleum residue

Energy Technology Data Exchange (ETDEWEB)

Ali, Mohammad Farhat; Siddiqui, Mohammad Nahid [Department of Chemistry, King Fahd University of Petroleum and Minerals, Dhahran 31261 (Saudi Arabia)

2005-08-15

The pyrolysis and hydropyrolysis of PVC mixed plastic waste alone and with petroleum residue was carried out at 150 and 350{sup o}C under N{sub 2} gas and at 430{sup o}C under 6.5MPa H{sub 2} gas pressure. The behavior of plastic waste during thermal and catalytic decomposition has also been studied in single- and two-stage reaction processes. In the individual pyrolysis process, both the petroleum residue and polystyrene (PS) undergo more than 90% conversion to liquid and gaseous products, whereas low-density polyethylene (LDPE) and high-density polyethylene (HDPE) yielded lower conversions products, and polypropylene (PP) and polyvinyl chloride (PVC) afforded somewhere a moderate to high conversion products. In a single-stage pyrolysis reaction, PVC was processed with petroleum residue at 150 and 430{sup o}C, under N{sub 2} gas for 1h at each temperature in a glass reactor. The model PVC and waste PVC showed slight variations in the products distribution obtained from the glass reactor. In two-stage process, model PVC, vacuum gas oil (VGO) and a number of different catalysts were used in a stainless steel autoclave micro tubular reactor at 350{sup o}C under the stream of N{sub 2} gas for 1h and at 430{sup o}C under 950psi (6.5MPa) H{sub 2} pressure for the duration of 2h. Significantly, different products distributions were obtained. Among the catalysts used, fluid catalytic cracking (FCC) and hydrocracking catalysts (HC-1) were most effective in producing liquid fuel (hexane soluble) materials. The study shows that the catalytic coprocessing of PVC with VGO is a feasible process by which PVC and VGO materials can be converted into transportation fuels.

Cuboid Ni2 P as a Bifunctional Catalyst for Efficient Hydrogen Generation from Hydrolysis of Ammonia Borane and Electrocatalytic Hydrogen Evolution.

Science.gov (United States)

Du, Yeshuang; Liu, Chao; Cheng, Gongzhen; Luo, Wei

2017-11-16

The design of high-performance catalysts for hydrogen generation is highly desirable for the upcoming hydrogen economy. Herein, we report the colloidal synthesis of nanocuboid Ni 2 P by the thermal decomposition of nickel chloride hexahydrate (NiCl 2 ⋅6 H 2 O) and trioctylphosphine. The obtained nanocuboid Ni 2 P was characterized by using powder X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and inductively coupled plasma atomic emission spectroscopy. For the first time, the as-synthesized nanocuboid Ni 2 P is used as a bifunctional catalyst for hydrogen generation from the hydrolysis of ammonia borane and electrocatalytic hydrogen evolution. Owing to the strong synergistic electronic effect between Ni and P, the as-synthesized Ni 2 P exhibits catalytic performance that is superior to its counterpart without P doping. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Multilinear operators for higher-order decompositions.

Energy Technology Data Exchange (ETDEWEB)

Kolda, Tamara Gibson

2006-04-01

We propose two new multilinear operators for expressing the matrix compositions that are needed in the Tucker and PARAFAC (CANDECOMP) decompositions. The first operator, which we call the Tucker operator, is shorthand for performing an n-mode matrix multiplication for every mode of a given tensor and can be employed to concisely express the Tucker decomposition. The second operator, which we call the Kruskal operator, is shorthand for the sum of the outer-products of the columns of N matrices and allows a divorce from a matricized representation and a very concise expression of the PARAFAC decomposition. We explore the properties of the Tucker and Kruskal operators independently of the related decompositions. Additionally, we provide a review of the matrix and tensor operations that are frequently used in the context of tensor decompositions.

Paraffin Alkylation Using Zeolite Catalysts in a slurry reactor: Chemical Engineering Principles to Extend Catalyst Lifetime

NARCIS (Netherlands)

Jong, K.P. de; Mesters, C.M.A.M.; Peferoen, D.G.R.; Brugge, P.T.M. van; Groot, C. de

1996-01-01

The alkylation of isobutane with 2-butene is carried out using a zeolitic catalyst in a well stirred slurry reactor. Whereas application of fixed bed technology using a solid acid alkylation catalyst has in the led to catalysts lifetimes in the range of minutes, in this work we report catalyst

Hydroxide catalysts for lignin depolymerization

Science.gov (United States)

Beckham, Gregg T; Biddy, Mary J.; Kruger, Jacob S.; Chmely, Stephen C.; Sturgeon, Matthew

2017-10-17

Solid base catalysts and their use for the base-catalyzed depolymerization (BCD) of lignin to compounds such as aromatics are presented herein. Exemplary catalysts include layered double hydroxides (LDHs) as recyclable, heterogeneous catalysts for BCD of lignin.

Hydroxide catalysts for lignin depolymerization

Energy Technology Data Exchange (ETDEWEB)

Beckham, Gregg T.; Biddy, Mary J.; Chmely, Stephen C.; Sturgeon, Matthew

2017-04-25

Solid base catalysts and their use for the base-catalyzed depolymerization (BCD) of lignin to compounds such as aromatics are presented herein. Exemplary catalysts include layered double hydroxides (LDHs) as recyclable, heterogeneous catalysts for BCD of lignin.

Fe1-xZnxS ternary solid solution as an efficient Fenton-like catalyst for ultrafast degradation of phenol.

Science.gov (United States)

Gao, Jing; Liu, Yutang; Xia, Xinnian; Wang, Longlu; Dong, Wanyue

2018-07-05

Heterogeneous Fenton-like system has been proved to be an promising alternative to Fenton system due to its easy separation. However, it's a challenge to design heterogeneous Fenton-like catalysts with high activity and great durability. Here, ternary solid solution Fe 1-x Zn x S were prepared via hydrothermal synthesis as heterogeneous Fenton-like catalysts. The Fe 0.7 Zn 0.3 S sample exhibited state of the art activity for yielding OH by H 2 O 2 decomposition, and the ultrafast degradation of phenol was achieved in 4 min at initial acidic condition under room temperature. The phenol degradation rate constant of Fe 0.7 Zn 0.3 S was 99 and 70 times of ZnS and FeS, respectively. Further, we show that the unique structural configuration of iron atoms, the formation of FeS 2 -pyrite with (200) plane, are responsible for the excellent activity. The intermediate products were identified by LC-MS and a possible pathway was accordingly proposed to elucidate the mechanism of phenol degradation by OH. Overall, this work provides an idea for the rational design of the relevant heterogeneous Fenton-like catalysts. Copyright © 2018 Elsevier B.V. All rights reserved.

To prevent the occurrence of black water agglomerate through delaying decomposition of cyanobacterial bloom biomass by sediment microbial fuel cell.

Science.gov (United States)

Zhou, Yan-Li; Jiang, He-Long; Cai, Hai-Yuan

2015-04-28

Settlement of cyanobacterial bloom biomass (CBB) into sediments in eutrophic lakes often induced the occurrence of black water agglomerate and then water quality deterioration. This study investigated the effect of sediment microbial fuel cell (SMFC) on CBB removal in sediments and related water pollution. Sediment bulking and subsequent black water from decomposition of settled CBB happened without SMFC, but were not observed over 100-day experiments with SMFC employment. While CBB in sediments improved power production from SMFC, the removal efficiency of organic matters in CBB-amended sediments with SMFC was significantly lower than that without SMFC. Pyrosequencing analysis showed higher abundances of the fermentative Clostridium and acetoclastic methanogen in CBB-amended bulk sediments without SMFC than with SMFC at the end of experiments. Obviously, SMFC operation changed the microbial community in CBB-amended sediments, and delayed the CBB degradation against sediment bulking. Thus, SMFC could be potentially applied as pollution prevention in CBB-settled and sensitive zones in shallow lakes. Copyright © 2015 Elsevier B.V. All rights reserved.

Decomposition of tetrachloroethylene by ionizing radiation

International Nuclear Information System (INIS)

Hakoda, T.; Hirota, K.; Hashimoto, S.

1998-01-01

Decomposition of tetrachloroethylene and other chloroethenes by ionizing radiation were examined to get information on treatment of industrial off-gas. Model gases, airs containing chloroethenes, were confined in batch reactors and irradiated with electron beam and gamma ray. The G-values of decomposition were larger in the order of tetrachloro- > trichloro- > trans-dichloro- > cis-dichloro- > monochloroethylene in electron beam irradiation and tetrachloro-, trichloro-, trans-dichloro- > cis-dichloro- > monochloroethylene in gamma ray irradiation. For tetrachloro-, trichloro- and trans-dichloroethylene, G-values of decomposition in EB irradiation increased with increase of chlorine atom in a molecule, while those in gamma ray irradiation were almost kept constant. The G-value of decomposition for tetrachloroethylene in EB irradiation was the largest of those for all chloroethenes. In order to examine the effect of the initial concentration on G-value of decomposition, airs containing 300 to 1,800 ppm of tetrachloroethylene were irradiated with electron beam and gamma ray. The G-values of decomposition in both irradiation increased with the initial concentration. Those in electron beam irradiation were two times larger than those in gamma ray irradiation

Hydrous titanium oxide-supported catalysts

International Nuclear Information System (INIS)

Dosch, R.G.; Stohl, F.V.; Richardson, J.T.

1990-01-01

Catalysts were prepared on hydrous titanium oxide (HTO) supports by ion exchange of an active metal for Na + ions incorporated in the HTO support during preparation by reaction with the parent Ti alkoxide. Strong active metal-HTO interactions as a result of the ion exchange reaction can require significantly different conditions for activation as compared to catalysts prepared by more widely used incipient wetness methods. The latter catalysts typically involve conversion or while the HTO catalysts require the alteration of electrostatic bonds between the metal and support with subsequent alteration of the support itself. In this paper, the authors discuss the activation, via sulfidation or reduction, of catalysts consisting of Co, Mo, or Ni-Mo dispersed on HTO supports by ion exchange. Correlations between the activation process and the hydrogenation, hydrodeoxygenation, and hydrodesulfurization activities of the catalysts are presented

Decomposition of Sodium Tetraphenylborate

International Nuclear Information System (INIS)

Barnes, M.J.

1998-01-01

The chemical decomposition of aqueous alkaline solutions of sodium tetraphenylborate (NaTPB) has been investigated. The focus of the investigation is on the determination of additives and/or variables which influence NaTBP decomposition. This document describes work aimed at providing better understanding into the relationship of copper (II), solution temperature, and solution pH to NaTPB stability

Fabrication of nanostructured clay-carbon nanotube hybrid nanofiller by chemical vapour deposition

International Nuclear Information System (INIS)

Manikandan, Dhanagopal; Mangalaraja, Ramalinga Viswanathan; Siddheswaran, Rajendran; Avila, Ricardo E.; Ananthakumar, Solaiappan

2012-01-01

Growth of multiwalled carbon nanotube (CNT) assemblies by chemical vapour decomposition (CVD) technique was achieved through decomposition of acetylene using iron impregnated montmorillonite (MM) catalysts. Various amounts of iron loaded montmorillonite catalysts were prepared by wet impregnation method and calcined at 450 °C. The catalysts were subjected to X-ray diffraction (XRD) and surface area analyses. Acetylene decomposition at a feed ratio of N 2 :H 2 :C 2 H 2 = 1:1:0.18 was conducted in the presence of iron impregnated montmorillonite catalysts in the CVD reactor for the growth of CNT structures. The role of Fe-activated clay catalyst on the formation of CNT structures has been systematically examined at various temperatures and correlated with the morphological features of CNTs. Catalyst assisted acetylene decomposition results the formation of different carbon nanostructures such as nanotubes, nanofibres and nanoflakes. These clay-CNT products were characterised for their morphological, thermal, qualitative and quantitative analyses. The morphological variations of CNT assemblies reveal Fe-montmorillonite catalysts have high selectivity at given reaction conditions. Thermogravimetric and Raman spectral analyses prove that the CNTs contain a good crystallanity and less structural defects.

Fabrication of nanostructured clay-carbon nanotube hybrid nanofiller by chemical vapour deposition

Energy Technology Data Exchange (ETDEWEB)

Manikandan, Dhanagopal, E-mail: dmani_cat@yahoo.co.in [Department of Materials Engineering, Faculty of Engineering, University of Concepcion, Concepcion (Chile); Mangalaraja, Ramalinga Viswanathan, E-mail: mangal@udec.cl [Department of Materials Engineering, Faculty of Engineering, University of Concepcion, Concepcion (Chile); Siddheswaran, Rajendran [Department of Materials Engineering, Faculty of Engineering, University of Concepcion, Concepcion (Chile); Avila, Ricardo E. [Personal Dosimetry Section, Chilean Nuclear Energy Commission, Santiago (Chile); Ananthakumar, Solaiappan [Materials and Minerals Division, National Institute for Interdisciplinary Science and Technology (NIIST), Trivandrum, Kerala (India)

2012-03-01

Growth of multiwalled carbon nanotube (CNT) assemblies by chemical vapour decomposition (CVD) technique was achieved through decomposition of acetylene using iron impregnated montmorillonite (MM) catalysts. Various amounts of iron loaded montmorillonite catalysts were prepared by wet impregnation method and calcined at 450 Degree-Sign C. The catalysts were subjected to X-ray diffraction (XRD) and surface area analyses. Acetylene decomposition at a feed ratio of N{sub 2}:H{sub 2}:C{sub 2}H{sub 2} = 1:1:0.18 was conducted in the presence of iron impregnated montmorillonite catalysts in the CVD reactor for the growth of CNT structures. The role of Fe-activated clay catalyst on the formation of CNT structures has been systematically examined at various temperatures and correlated with the morphological features of CNTs. Catalyst assisted acetylene decomposition results the formation of different carbon nanostructures such as nanotubes, nanofibres and nanoflakes. These clay-CNT products were characterised for their morphological, thermal, qualitative and quantitative analyses. The morphological variations of CNT assemblies reveal Fe-montmorillonite catalysts have high selectivity at given reaction conditions. Thermogravimetric and Raman spectral analyses prove that the CNTs contain a good crystallanity and less structural defects.

Methanol conversion to hydrocarbons using modified clinoptilolite catalysts. Investigation of catalyst lifetime and reactivation

Energy Technology Data Exchange (ETDEWEB)

Hutchings, G J; Themistocleous, T; Copperthwaite, R G

1988-10-17

A study of the deactivation and reactivation of modified clinoptilolite catalysts for methanol conversion to hydrocarbons is reported. Clinoptilolite catalysts, modified by either ammonium ion exchange or hydrochloric acid treatment, exhibit a short useful catalyst lifetime for this reaction (ca. 2-3 h) due to a high rate of coke deposition (3-5.10/sup -3/ g carbon/g catalyst/h). A comparative study of reactivation using oxygen, nitrous oxide and ozone/oxygen as oxidants indicated that nitrous oxide reactivation gives improved catalytic performance when compared to the activity and lifetime of the fresh catalyst. Both oxygen and ozone/oxygen were found to be ineffective for the reactivation of clinoptilolite. Initial studies of in situ on-line reactivation are also described. 3 figs., 15 refs., 4 tabs.

Identifying Different Types of Catalysts for CO2 Reduction by Ethane through Dry Reforming and Oxidative Dehydrogenation.

Science.gov (United States)

Porosoff, Marc D; Myint, Myat Noe Zin; Kattel, Shyam; Xie, Zhenhua; Gomez, Elaine; Liu, Ping; Chen, Jingguang G

2015-12-14