Nonalloyed carbon-supported PtRu catalysts for PEMFC applications

NARCIS (Netherlands)

Papageorgopoulos, D.C.; Heer, de M.P.; Keijzer, M.; Pieterse, J.A.Z.; Bruijn, de F.A.

2004-01-01

PtRu(1:1)/C catalysts were prepared by a process that was claimed previously to lead to nonalloyed Pt and Ru particles, using twodifferent precursors, Ru nitrosyl nitrate and Ru chloride hydrate. Both X-ray diffraction and characterization by cyclic voltammetrypoint toward Pt and Ru being present as

Nonalloyed carbon-supported PtRu catalysts for PEMFC applications

NARCIS (Netherlands)

Papageorgopoulos, D.C.; De Heer, M.P.; Keijzer, M.; Pieterse, J.A.Z.; de Bruijn, F. A.

2004-01-01

PtRu(1:1)/C catalysts were prepared by a process that was claimed previously to lead to non-alloyed Pt and Ru particles, using two different precursors, Ru nitrosyl nitrate and Ru chloride hydrate. Both X-ray diffraction and characterization by cyclic voltammetry point toward Pt and Ru being present

103Ru/103mRh generator

International Nuclear Information System (INIS)

Bartos, B.; Kowalska, E.; Bilewicz, A.; Skarnemark, G.

2009-01-01

103m Rh is a very promising radionuclide for Auger electron therapy due to its very low photon/electron ratio. The goal of the present work was the elaboration a method for production of large quantities of 103m Rh for generator system. It was found that the combination of solvent extraction with evaporation of 103 RuO 4 followed by decomposition of H 5 IO 6 makes it possible to produce 103m Rh of high radionuclidic and chemical purity. (author)

Hybridization and magnetism in U(Ru, Rh)X, X=Al, Ga

NARCIS (Netherlands)

Sechovsky, V.; Havela, L.; Boer, de F.R.; Veenhuizen, P.A.; Sugiyama, K.; Kuroda, T.; Sugiura, T.; Ono, M.; Date, M.; Yamagishi, A.

1992-01-01

Results of magnetic studies of pseudoternary U(Ru, Rh)Al and U(Ru, Rh)Ga systems are presented. Reduction of the 5f-4d hybridization with increasing Rh content is reflected in a gradual transition from paramagnetic (spin fluctuation) behaviour of URuX to ferromagnetism in URhX. The huge uniaxial

PtRu/C and PtRuBi/C electrocatalysts prepared by two different methodologies of borohydride reduction process for ethanol electro-oxidation

Energy Technology Data Exchange (ETDEWEB)

Brandalise, Michele; Tusi, Marcelo Marques; Piasentin, Ricardo Marcelo; Correa, Olandir Vercino; Linardi, Marcelo; Spinace, Estevam Vitorio; Oliveira Neto, Almir, E-mail: brandalise@usp.br, E-mail: mmtusi@usp.br, E-mail: rmpiasen@ipen.br, E-mail: ovcorrea@ipen.br, E-mail: mlinardi@ipen.br, E-mail: espinace@ipen.br, E-mail: aolivei@ipen.br [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

2009-07-01

PtRu/C (50:50) and PtRuBi/C (50:40:10) electrocatalysts were prepared by borohydride reduction using H{sub 2}PtCl{sub 6.6}H{sub 2}O, RuCl{sub 3.x}H{sub 2}O and Bi(NO{sub 3}){sub 3.5}H{sub 2}O as metals sources and Vulcan XC72 as support. The borohydride solution was added in two different ways: drop by drop and rapid addition of all the solution. The obtained electrocatalysts were characterized by EDX, XRD and cyclic voltammetry. The electro-oxidation of ethanol was studied by cyclic voltammetry and chronoamperometry at room temperature and on a single cell of a direct ethanol fuel cell (DEFC) at 100 deg C. PtRuBi/C electrocatalysts showed superior performance for ethanol electro-oxidation than PtRu/C electrocatalysts prepared in a similar way. However, PtRuBi/C electrocatalyst prepared by rapid addition of the borohydride solution showed superior performance for ethanol electro oxidation at room temperature, while PtRuBi/C electrocatalyst prepared by addition drop by drop of borohydride solution showed superior performance on DEFC at 100 deg C. (author)

PtRu/C and PtRuBi/C electrocatalysts prepared by two different methodologies of borohydride reduction process for ethanol electro-oxidation

International Nuclear Information System (INIS)

Brandalise, Michele; Tusi, Marcelo Marques; Piasentin, Ricardo Marcelo; Correa, Olandir Vercino; Linardi, Marcelo; Spinace, Estevam Vitorio; Oliveira Neto, Almir

2009-01-01

PtRu/C (50:50) and PtRuBi/C (50:40:10) electrocatalysts were prepared by borohydride reduction using H 2 PtCl 6.6 H 2 O, RuCl 3.x H 2 O and Bi(NO 3 ) 3.5 H 2 O as metals sources and Vulcan XC72 as support. The borohydride solution was added in two different ways: drop by drop and rapid addition of all the solution. The obtained electrocatalysts were characterized by EDX, XRD and cyclic voltammetry. The electro-oxidation of ethanol was studied by cyclic voltammetry and chronoamperometry at room temperature and on a single cell of a direct ethanol fuel cell (DEFC) at 100 deg C. PtRuBi/C electrocatalysts showed superior performance for ethanol electro-oxidation than PtRu/C electrocatalysts prepared in a similar way. However, PtRuBi/C electrocatalyst prepared by rapid addition of the borohydride solution showed superior performance for ethanol electro oxidation at room temperature, while PtRuBi/C electrocatalyst prepared by addition drop by drop of borohydride solution showed superior performance on DEFC at 100 deg C. (author)

Preparation and characterization of Pt/C and Pt-Ru/C electrocatalysts for direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Liu, Zhaolin; Ling, Xing Yi; Su, Xiaodi; Lee, Jim Yang; Gan, Leong Ming [Institute of Materials Research and Engineering, 3 Research Link, Singapore 117602 (Singapore)

2005-09-26

Nano-sized Pt and Pt-Ru colloids are prepared by a microwave-assisted polyol process, and transferred to a toluene solution of decanthiol. Vulcan XC-72 is then added to the toluene solution to adsorb the thiolated Pt and Pt-Ru colloids. Transmission electron microscopy examinations show nearly spherical particles and narrow size distributions for both supported and unsupported metals. The carbon-supported Pt and Pt-Ru nanoparticles are activated by thermal treatment to remove the thiol stabilizing shell. All Pt and Pt-Ru catalysts (except Pt{sub 23}-Ru{sub 77}) give the X-ray diffraction pattern of a face-centered cubic (fcc) crystal structure, whereas the Pt{sub 23}-Ru{sub 77} alloy is more typical of the hexagonal close packed (hcp) structure. The electro-oxidation of liquid ethanol on these catalysts is investigated at room temperature by cyclic voltammetry. The results demonstrate that the alloy catalyst is catalytically more active than pure platinum. Preliminary tests on a single cell of a direct ethanol fuel cell (DEFC) indicate that a Pt{sub 52}-Ru{sub 48}/C anode catalyst gives the best electrocatalytic performance among all the carbon-supported Pt and Pt-Ru catalysts. (author)

Co-catalytic effect of Rh and Ru for the ethanol electro-oxidation in amorphous microparticulated alloys

Energy Technology Data Exchange (ETDEWEB)

Blanco, Tamara C.; Pierna, Angel R.; Barroso, Javier [Dpto. de Ingenieria Quimica y del Medio Ambiente, Universidad del Pais Vasco, San Sebastian (Spain)

2011-11-15

The ethanol electro-oxidation on platinum catalyst in acid media leads to the formation of acetaldehyde and acetic acid as main products. Another problem is the poisoning of the electro-catalyst surface with CO formed during the fuel oxidation reaction. To increase the performance of Direct Ethanol Fuel Cells (DEFCs) it is necessary to develop new electrode materials or modification of the existing Pt catalysts. This work presents the electrochemical response to ethanol and CO oxidation of different compositional amorphous alloys obtained by ball milling technique, used as electrodes. Alloys with Ni{sub 59}Nb{sub 40}Pt{sub 0.6}Rh{sub 0.4} and Ni{sub 59}Nb{sub 40}Pt{sub 0.6}Rh{sub 0.2}Ru{sub 0.2} composi-tions were studied. The current density towards ethanol oxidation decreases with the presence of ruthenium; however, this electrode shows the best tolerance to CO, with lower surface coverage (copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

Co-catalytic effect of Rh and Ru for the ethanol electro-oxidation in amorphous microparticulated alloys

International Nuclear Information System (INIS)

Blanco, Tamara C.; Pierna, Angel R.; Barroso, Javier

2011-01-01

The ethanol electro-oxidation on platinum catalyst in acid media leads to the formation of acetaldehyde and acetic acid as main products. Another problem is the poisoning of the electro-catalyst surface with CO formed during the fuel oxidation reaction. To increase the performance of Direct Ethanol Fuel Cells (DEFCs) it is necessary to develop new electrode materials or modification of the existing Pt catalysts. This work presents the electrochemical response to ethanol and CO oxidation of different compositional amorphous alloys obtained by ball milling technique, used as electrodes. Alloys with Ni 59 Nb 40 Pt 0.6 Rh 0.4 and Ni 59 Nb 40 Pt 0.6 Rh 0.2 Ru 0.2 composi-tions were studied. The current density towards ethanol oxidation decreases with the presence of ruthenium; however, this electrode shows the best tolerance to CO, with lower surface coverage (copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

Pt and Ru X-ray absorption spectroscopy of PtRu anode catalysts in operating direct methanol fuel cells.

Science.gov (United States)

Stoupin, Stanislav; Chung, Eun-Hyuk; Chattopadhyay, Soma; Segre, Carlo U; Smotkin, Eugene S

2006-05-25

In situ X-ray absorption spectroscopy, ex situ X-ray fluorescence, and X-ray powder diffraction enabled detailed core analysis of phase segregated nanostructured PtRu anode catalysts in an operating direct methanol fuel cell (DMFC). No change in the core structures of the phase segregated catalyst was observed as the potential traversed the current onset potential of the DMFC. The methodology was exemplified using a Johnson Matthey unsupported PtRu (1:1) anode catalyst incorporated into a DMFC membrane electrode assembly. During DMFC operation the catalyst is essentially metallic with half of the Ru incorporated into a face-centered cubic (FCC) Pt alloy lattice and the remaining half in an amorphous phase. The extended X-ray absorption fine structure (EXAFS) analysis suggests that the FCC lattice is not fully disordered. The EXAFS indicates that the Ru-O bond lengths were significantly shorter than those reported for Ru-O of ruthenium oxides, suggesting that the phases in which the Ru resides in the catalysts are not similar to oxides.

Preparation and characterization of Pt/C and Pt sbnd Ru/C electrocatalysts for direct ethanol fuel cells

Science.gov (United States)

Liu, Zhaolin; Ling, Xing Yi; Su, Xiaodi; Lee, Jim Yang; Gan, Leong Ming

Nano-sized Pt and Pt sbnd Ru colloids are prepared by a microwave-assisted polyol process, and transferred to a toluene solution of decanthiol. Vulcan XC-72 is then added to the toluene solution to adsorb the thiolated Pt and Pt sbnd Ru colloids. Transmission electron microscopy examinations show nearly spherical particles and narrow size distributions for both supported and unsupported metals. The carbon-supported Pt and Pt sbnd Ru nanoparticles are activated by thermal treatment to remove the thiol stabilizing shell. All Pt and Pt sbnd Ru catalysts (except Pt 23sbnd Ru 77) give the X-ray diffraction pattern of a face-centered cubic (fcc) crystal structure, whereas the Pt 23sbnd Ru 77 alloy is more typical of the hexagonal close packed (hcp) structure. The electro-oxidation of liquid ethanol on these catalysts is investigated at room temperature by cyclic voltammetry. The results demonstrate that the alloy catalyst is catalytically more active than pure platinum. Preliminary tests on a single cell of a direct ethanol fuel cell (DEFC) indicate that a Pt 52sbnd Ru 48/C anode catalyst gives the best electrocatalytic performance among all the carbon-supported Pt and Pt sbnd Ru catalysts.

Structural and physical properties of new uranium and transition element ternary stannides (Fe, Co, Ni, Ru, Rh, Pd, Ir, Pt); Proprietes structurales et physiques de nouveaux stannures ternaires a base d'uranium et d'element de transition (Fe, Co, Ni, Rh, Pd, Ir, Pt)

Energy Technology Data Exchange (ETDEWEB)

Mirambet, F

1993-12-15

This work is dedicated to the study of ternary stannides based on uranium. The author reviews the structural, magnetic and electric properties of different families of stannides. The study of the U{sub 2}M{sub 2}Sn family where M stands for Fe, Co, Ni, Ru, Rh, Pd, Ir and Pt shows that the magnetic behaviour of uranium in these compounds is strongly influenced by the transition element M, which is explained by the hybridization force 5f(U) - nd(M) that depends on the number of electrons on the d shell of the M element. For instance, for the elements whose d shell is low filled (Fe, Ru), the U{sub 2}M{sub 2}Sn stannides show no magnetic order. On the other hand, when the number of d-electrons increases, a magnetic order appears progressively.

Magnetic behavior in heterometallic one-dimensional chains or octanuclear complex regularly aligned with metal-metal bonds as -Rh-Rh-Pt-Cu-Pt

Science.gov (United States)

Uemura, Kazuhiro

2018-06-01

Heterometallic one-dimensional chains, [{Rh2(O2CCH3)4}{Pt2Cu(piam)4(NH3)4}]n(PF6)2n (1 and 2, piam = pivalamidate) and [{Rh2(O2CCH3)4}{Pt2Cu(piam)4(NH3)4}2](CF3CO2)2(ClO4)2·2H2O (3), are paramagnetic one-dimensional chains or octanuclear complexes that are either aligned as -Rh-Rh-Pt-Cu-Pt- (1 and 2) or as Pt-Cu-Pt-Rh-Rh-Pt-Cu-Pt (3) with metal-metal bonds. Compounds 1-3 have rare structures, from the standpoint of that the paramagnetic species of Cu atoms are linked by direct metal-metal bonds. Magnetic susceptibility measurements for 1-3 performed at temperatures of 2 K-300 K indicated that the unpaired electrons localize in the Cu 3dx2-y2 orbitals, where S = 1/2 Cu(II) atoms are weakly antiferromagnetically coupled with J = -0.35 cm-1 (1), -0.47 cm-1 (2), and -0.45 cm-1 (3).

Methanol oxidation catalysis and substructure of PtRu bimetallic nanoparticles

Energy Technology Data Exchange (ETDEWEB)

Nitani, Hiroaki; Nakagawa, Takashi; Ono, Takahiro; Honda, Yusuke; Koizumi, Akiko; Seino, Satoshi; Yamamoto, Takao A. [Graduate School of Engineering, Osaka University, 2-1 Yamada-oka, Suita, Osaka 565-0871 (Japan); Daimon, Hideo; Kurobe, Yukiko [Development and Technology Division, Hitachi Maxell Ltd., 6-20-1 Kinunodai, Tsukubamirai, Ibaraki 300-2496 (Japan)

2007-07-15

Catalytic material of PtRu nanoparticles supported on carbon (PtRu/C) for direct methanol fuel cells was synthesized by a polyol reduction method. Addition of phosphorus was effective for downsizing PtRu particles and improving their catalytic activity. The activity obtained was six times of that of a commercial catalysis. The samples were analyzed by techniques of X-ray absorption fine structure (XAFS) at Pt L{sub III}-edge and Ru K-edge, transmission electron microscope (TEM), X-ray diffraction (XRD) and X-ray fluorescence (XRF). These results indicated a core-shell structure consisting of a Pt-rich core and Ru-rich shell. By examining coordination numbers determined by XAFS analysis, we found a clear correlation between the catalytic activity and the Pt-Ru atomic pair frequency occurring on the particle surface, which supports the 'bi-functional mechanism'. (author)

Methanol Electro-Oxidation on Pt-Ru Alloy Nanoparticles Supported on Carbon Nanotubes

Directory of Open Access Journals (Sweden)

Yangchuan Xing

2009-09-01

Full Text Available Carbon nanotubes (CNTs have been investigated in recent years as a catalyst support for proton exchange membrane fuel cells. Improved catalyst activities were observed and attributed to metal-support interactions. We report a study on the kinetics of methanol electro-oxidation on CNT supported Pt-Ru alloy nanoparticles. Alloy catalysts with different compositions, Pt53Ru47/CNT, Pt69Ru31/CNT and Pt77Ru23/CNT, were prepared and investigated in detail. Experiments were conducted at various temperatures, electrode potentials, and methanol concentrations. It was found that the reaction order of methanol electro-oxidation on the PtRu/CNT catalysts was consistent with what has been reported for PtRu alloys with a value of 0.5 in methanol concentrations. However, the electro-oxidation reaction on the PtRu/CNT catalysts displayed much lower activation energies than that on the Pt-Ru alloy catalysts unsupported or supported on carbon black (PtRu/CB. This study provides an overall kinetic evaluation of the PtRu/CNT catalysts and further demonstrates the beneficial role of CNTs.

Activity of carbon supported Pt3Ru2 nanocatalyst in CO oxidation

Directory of Open Access Journals (Sweden)

KSENIJA DJ. POPOVIĆ

2009-08-01

Full Text Available The electrocatalytic activity of Pt3Ru2/C nanocatalyst toward the electro-oxidation of bulk CO was examined in acid and alkaline solution at ambient temperature using the thin-film, rotating disk electrode (RDE method. The catalyst was characterized by XRD analysis. The XRD pattern revealed that the Pt3Ru2/C catalyst consisted of two structures, i.e., Pt–Ru-fcc and Ru-hcp (a solid solution of Ru in Pt and a small amount of Ru or a solid solution of Pt in Ru. Electrocatalytic activities were measured by applying potentiodynamic and steady state techniques. The oxidation of CO on the Pt3Ru2/C catalyst was influenced by pH and anions from the supporting electrolytes. The Pt3Ru2/C was more active in alkaline than in acid solution, as well as in perchloric than in sulfuric acid. Comparison of CO oxidation on Pt3Ru2/C and Pt/C revealed that the Pt3Ru2/C was more active than Pt/C in acid solution, while both catalysts had a similar activity in alkaline solution.

Significance of β-dehydrogenation in ethanol electro-oxidation on platinum doped with Ru, Rh, Pd, Os and Ir.

Science.gov (United States)

Sheng, Tian; Lin, Wen-Feng; Hardacre, Christopher; Hu, P

2014-07-14

In the exploration of highly efficient direct ethanol fuel cells (DEFCs), how to promote the CO2 selectivity is a key issue which remains to be solved. Some advances have been made, for example, using bimetallic electrocatalysts, Rh has been found to be an efficient additive to platinum to obtain high CO2 selectivity experimentally. In this work, the mechanism of ethanol electrooxidation is investigated using the first principles method. It is found that CH3CHOH* is the key intermediate during ethanol electrooxidation and the activity of β-dehydrogenation is the rate determining factor that affects the completeness of ethanol oxidation. In addition, a series of transition metals (Ru, Rh, Pd, Os and Ir) are alloyed on the top layer of Pt(111) in order to analyze their effects. The elementary steps, α-, β-C-H bond and C-C bond dissociations, are calculated on these bimetallic M/Pt(111) surfaces and the formation potential of OH* from water dissociation is also calculated. We find that the active metals increase the activity of β-dehydrogenation but lower the OH* formation potential resulting in the active site being blocked. By considering both β-dehydrogenation and OH* formation, Ru, Os and Ir are identified to be unsuitable for the promotion of CO2 selectivity and only Rh is able to increase the selectivity of CO2 in DEFCs.

Ternary Pt9RhFex Nanoscale Alloys as Highly Efficient Catalysts with Enhanced Activity and Excellent CO-Poisoning Tolerance for Ethanol Oxidation.

Science.gov (United States)

Wang, Peng; Yin, Shibin; Wen, Ying; Tian, Zhiqun; Wang, Ningzhang; Key, Julian; Wang, Shuangbao; Shen, Pei Kang

2017-03-22

To address the problems of high cost and poor stability of anode catalysts in direct ethanol fuel cells (DEFCs), ternary nanoparticles Pt 9 RhFe x (x = 1, 3, 5, 7, and 9) supported on carbon powders (XC-72R) have been synthesized via a facile method involving reduction by sodium borohydride followed by thermal annealing in N 2 at ambient pressure. The catalysts are physically characterized by X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy, and their catalytic performance for the ethanol oxidation reaction (EOR) is evaluated by cyclic and linear scan voltammetry, CO-stripping voltammograms, and chronopotentiometry. All the Pt 9 RhFe x /C catalysts of different atomic ratios produce high EOR catalytic activity. The catalyst of atomic ratio composition 9:1:3 (Pt/Rh/Fe) has the highest activity and excellent CO-poisoning tolerance. Moreover, the enhanced EOR catalytic activity on Pt 9 RhFe 3 /C when compared to Pt 9 Rh/C, Pt 3 Fe/C, and Pt/C clearly demonstrates the presence of Fe improves catalytic performance. Notably, the onset potential for CO oxidation on Pt 9 RhFe 3 /C (0.271 V) is ∼55, 75, and 191 mV more negative than on Pt 9 Rh/C (0.326 V), Pt 3 Fe/C (0.346 V), and Pt/C (0.462 V), respectively, which implies the presence of Fe atoms dramatically improves CO-poisoning tolerance. Meanwhile, compared to the commercial PtRu/C catalyst, the peak potential on Pt 9 RhFe 3 /C for CO oxidation was just slightly changed after several thousand cycles, which shows high stability against the potential cycling. The possible mechanism by which Fe and Rh atoms facilitate the observed enhanced performance is also considered herein, and we conclude Pt 9 RhFe 3 /C offers a promising anode catalyst for direct ethanol fuel cells.

Preparation of supported PtRu/C electrocatalyst for direct methanol fuel cells

International Nuclear Information System (INIS)

Jiang Luhua; Sun Gongquan; Zhao Xinsheng; Zhou Zhenhua; Yan Shiyou; Tang Shuihua; Wang Guoxiong; Zhou Bing; Xin Qin

2005-01-01

In this work, high-surface supported PtRu/C were prepared with Ru(NO)(NO 3 ) 3 and [Pt(H 2 NCH 2 CH 2 NH 2 ) 2 ]Cl 2 as the precursors and hydrogen as a reducing agent. XRD and TEM analyses showed that the PtRu/C catalysts with different loadings possessed small and homogeneous metal particles. Even at high metal loading (40 wt.% Pt, 20 wt.% Ru) the mean metal particle size is less than 4 nm. Meanwhile, the calculated Pt crystalline lattice parameter and Pt (2 2 0) peak position indicated that the geometric structure of Pt was modified by Ru atoms. Among the prepared catalysts, the lattice parameter of 40-20 wt.% PtRu/C contract most. Cyclic voltammetry (CV), chronoamperometry (CA), CO stripping and single direct methanol fuel cell tests jointly suggested that the 40-20 wt.% PtRu/C catalyst has the highest electrochemical activity for methanol oxidation

MnO2/CNT supported Pt and PtRu nanocatalysts for direct methanol fuel cells.

Science.gov (United States)

Zhou, Chunmei; Wang, Hongjuan; Peng, Feng; Liang, Jiahua; Yu, Hao; Yang, Jian

2009-07-07

Pt/MnO2/carbon nanotube (CNT) and PtRu/MnO2/CNT nanocomposites were synthesized by successively loading hydrous MnO2 and Pt (or PtRu alloy) nanoparticles on CNTs and were used as anodic catalysts for direct methanol fuel cells (DMFCs). The existence of MnO2 on the surface of CNTs effectively increases the proton conductivity of the catalyst, which then could remarkably improve the performance of the catalyst in methanol electro-oxidation. As a result, Pt/MnO2/CNTs show higher electrochemical active surface area and better methanol electro-oxidation activity, compared with Pt/CNTs. As PtRu alloy nanoparticles were deposited on the surface of MnO2/CNTs instead of Pt, the PtRu/MnO2/CNT catalyst shows not only excellent electro-oxidation activity to methanol with forward anodic peak current density of 901 A/gPt but also good CO oxidation ability with lower preadsorbed CO oxidation onset potential (0.33 V vs Ag/AgCl) and peak potential (0.49 V vs Ag/AgCl) at room temperature.

Pt and PtRu catalyst bilayers increase efficiencies for ethanol oxidation in proton exchange membrane electrolysis and fuel cells

Science.gov (United States)

Altarawneh, Rakan M.; Pickup, Peter G.

2017-10-01

Polarization curves, product distributions, and reaction stoichiometries have been measured for the oxidation of ethanol at anodes consisting of Pt and PtRu bilayers and a homogeneous mixture of the two catalysts. These anode structures all show synergies between the two catalysts that can be attributed to the oxidation of acetaldehyde produced at the PtRu catalyst by the Pt catalyst. The use of a PtRu layer over a Pt layer produces the strongest effect, with higher currents than a Pt on PtRu bilayer, mixed layer, or either catalyst alone, except for Pt at high potentials. Reaction stoichiometries (average number of electrons transferred per ethanol molecule) were closer to the values for Pt alone for both of the bilayer configurations but much lower for PtRu and mixed anodes. Although Pt alone would provide the highest overall fuel cell efficiency at low power densities, the PtRu on Pt bilayer would provide higher power densities without a significant loss of efficiency. The origin of the synergy between the Pt and PtRu catalysts was elucidated by separation of the total current into the individual components for generation of carbon dioxide and the acetaldehyde and acetic acid byproducts.

The electrocatalytic properties of carbon supported PtRu/C nanoalloys in oxidation of small organic molecules: Comparison with Pt/C catalyst

Directory of Open Access Journals (Sweden)

Lović Jelena D.

2012-01-01

Full Text Available The electrocatalytic activity of carbon supported PtRu/C catalysts, with different composition, toward the electrooxidation of methanol, CO and formic acid were examined in acid and alkaline solution at ambient temperature using thin-film rotating disk electrode (RDE method and compared with activity of Pt/C. The catalysts were characterized by XRD, AFM and STM techniques. XRD pattern revealed that PtRu-1/C catalyst is consisted of two structures e.g. Pt-Ru-fcc and Ru-hcp (the solid solution of Ru in Pt and the small amount of Ru or solid solution of Pt in Ru, as opposed to PtRu-2/C catalyst which is consisted of one structure mostly, Pt-Ru-fcc. According to STM images, PtRu as well as Pt, particles size were between 2 and 6 nm, which is in a good agreement with the mean particles size determined by XRD. To establish the activity and stability of the catalysts potentiodynamic and quasi steady-state measurements were performed. It was found that the activity of Pt and PtRu for CO and methanol oxidation is a strong function of pH of solution. The kinetics are much higher in alkaline than in acid solution and the difference between Pt/C and PtRu/C is much less pronounced in alkaline media. Results presented in this work indicate that activity of PtRu catalysts depends on catalyst composition, e.g. on Pt/Ru atomic ratio, as well as on alloying degree of catalysts. Comparison of CO, methanol and formic acid oxidation on PtRu-2/C, PtRu-1/C and Pt/C catalysts revealed that PtRu-2/C is the most active one. It was shown that the PtRu-2/C catalyst, due to fact that it is consisted of only one phase, with high alloying degree, through the bifunctional mechanism improved by electronic effect, achieve the activity two times higher related to PtRu-1/C in the oxidation of all organic molecules investigated, and about three times higher compared to Pt/C in the oxidation of methanol and CO, and five times higher in formic acid oxidation.

A Synthetic Pseudo-Rh: NOx Reduction Activity and Electronic Structure of Pd-Ru Solid-solution Alloy Nanoparticles

Science.gov (United States)

Sato, Katsutoshi; Tomonaga, Hiroyuki; Yamamoto, Tomokazu; Matsumura, Syo; Zulkifli, Nor Diana Binti; Ishimoto, Takayoshi; Koyama, Michihisa; Kusada, Kohei; Kobayashi, Hirokazu; Kitagawa, Hiroshi; Nagaoka, Katsutoshi

2016-06-01

Rh is one of the most important noble metals for industrial applications. A major fraction of Rh is used as a catalyst for emission control in automotive catalytic converters because of its unparalleled activity toward NOx reduction. However, Rh is a rare and extremely expensive element; thus, the development of Rh alternative composed of abundant elements is desirable. Pd and Ru are located at the right and left of Rh in the periodic table, respectively, nevertheless this combination of elements is immiscible in the bulk state. Here, we report a Pd-Ru solid-solution-alloy nanoparticle (PdxRu1-x NP) catalyst exhibiting better NOx reduction activity than Rh. Theoretical calculations show that the electronic structure of Pd0.5Ru0.5 is similar to that of Rh, indicating that Pd0.5Ru0.5 can be regarded as a pseudo-Rh. Pd0.5Ru0.5 exhibits better activity than natural Rh, which implies promising applications not only for exhaust-gas cleaning but also for various chemical reactions.

A DFT study of Ru, Rh, Pd, Os, Ir, and Pt clusters as catalysts for methane dissociation in a direct methane fuel cell (DMHFC)

Energy Technology Data Exchange (ETDEWEB)

Psofogiannakisa, G. [Ottawa Univ., Ottawa, ON (Canada). Dept. of Chemical Engineering; Ottawa, Univ., Ottawa, ON (Canada). Centre for Catalysis Research and Innovation; St-Amant, A. [Ottawa Univ., Ottawa, ON (Canada). Dept. of Chemistry; Ternan, M. [Ottawa Univ., Ottawa, ON (Canada). Centre for Catalysis Research and Innovation; EnPross Inc., Ottawa, ON (Canada)

2008-07-01

The rate limiting step in a direct methane hydrocarbon fuel cell (DMHFC) is the dissociative chemisorption of methane. Quantum mechanical computations were used to examine the terrace, kink, and step sites on 6 different clusters of group 8 transition metals, notably Ru, Rh, Pd, Os, Ir, and Pt. The computations involved the anodic reaction of a DMHFC with a polymer electrolyte that operates at atmospheric pressure and temperatures higher than 120 degrees C. The interaction between molecular fragments and a surface (Pt) were described and density functional theory (DFT) calculations were performed using Guassian software. The geometries of 5 different platinum clusters were examined along with their electronic energy barriers. The biggest contribution to the stabilization energy came from the overlap between the sigma bond in methane and unoccupied sd hybrid orbitals in the Pt bonding atom. The study showed that when relaxation was allowed, the displacement of the bonding metal atom was 0.36 to 0.52 A. The electronic energy barrier often increased as d-orbital occupancy increased. For the kink surface sites, the energy barriers were considerably smaller for the 5d transition metals than for the 4d transition metals. 5 refs., 1 tab.

Comparison of different promotion effect of PtRu/C and PtSn/C electrocatalysts for ethanol electro-oxidation

Energy Technology Data Exchange (ETDEWEB)

Li, Huanqiao; Cao, Lei [Direct Alcohol Fuel Cell Laboratory, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Graduate School of the Chinese Academy Sciences, Beijing 100039 (China); Sun, Gongquan; Jiang, Luhua [Direct Alcohol Fuel Cell Laboratory, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Xin, Qin [Direct Alcohol Fuel Cell Laboratory, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China)

2007-08-01

Well dispersed PtSn/C, PtRu/C and Pt/C electrocatalysts were synthesized by a modified polyol process and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM) and inductively coupled plasma-atomic emission spectrometry techniques. XRD patterns show that Ru induces the contraction of Pt lattice parameter while Sn makes the Pt crystal lattice extended. Ethanol oxidation activities on the catalysts were studied via cyclic voltammetry (CV) and chronoamperometry (CA) methods at room temperature. It is found that the electrode potential plays an important role in the electrochemical behavior of ethanol oxidation on PtRu/C and PtSn/C catalysts. In the lower potential region, PtSn/C possesses higher performance for ethanol oxidation, while in the higher potential region PtRu/C is more active. The different promotion effects of PtSn/C and PtRu/C to ethanol oxidation can be explained by the structural effect and modified bi-functional mechanism in different potential region. Single cell test of a direct ethanol fuel cell (DEFC) was also carried out to elucidate the promotion effect of PtRu/C and PtSn/C catalysts on the ethanol oxidation at 90 C. (author)

Comparison of different promotion effect of PtRu/C and PtSn/C electrocatalysts for ethanol electro-oxidation

International Nuclear Information System (INIS)

Li, Huanqiao; Sun, Gongquan; Cao, Lei; Jiang, Luhua; Xin, Qin

2007-01-01

Well dispersed PtSn/C, PtRu/C and Pt/C electrocatalysts were synthesized by a modified polyol process and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM) and inductively coupled plasma-atomic emission spectrometry techniques. XRD patterns show that Ru induces the contraction of Pt lattice parameter while Sn makes the Pt crystal lattice extended. Ethanol oxidation activities on the catalysts were studied via cyclic voltammetry (CV) and chronoamperometry (CA) methods at room temperature. It is found that the electrode potential plays an important role in the electrochemical behavior of ethanol oxidation on PtRu/C and PtSn/C catalysts. In the lower potential region, PtSn/C possesses higher performance for ethanol oxidation, while in the higher potential region PtRu/C is more active. The different promotion effects of PtSn/C and PtRu/C to ethanol oxidation can be explained by the structural effect and modified bi-functional mechanism in different potential region. Single cell test of a direct ethanol fuel cell (DEFC) was also carried out to elucidate the promotion effect of PtRu/C and PtSn/C catalysts on the ethanol oxidation at 90 o C

Microwave sinthesys and characterization of Pt and Pt-Rh-Sn electrocatalysts for ethanol oxidation

Directory of Open Access Journals (Sweden)

Jovanović Vladislava M.

2011-01-01

Full Text Available Carbon supported Pt and Pt-Rh-Sn catalysts were synthesized by microwave-polyol method in ethylene glycol solution and investigated for the ethanol electro-oxidation reaction. The catalysts were characterized in terms of structure, morphology and composition by employing XRD, STM and EDX techniques. STM analysis indicated rather uniform particles and particle size of below 2 nm for both catalysts. XRD analysis of the Pt/C catalyst revealed two phases, one with the main characteristic peaks of face centered cubic crystal structure (fcc of platinum and another related to graphite like structure of carbon support Vulcan XC-72R. However, in XRD pattern of the Pt-Rh-Sn/C catalyst diffraction peaks for Pt, Rh or Sn cannot be resolved, indicating an extremely low crystallinity. The small particle sizes and homogeneous size distributions of both catalysts should be attributed to the advantages of microwave assisted modified polyol process in ethylene glycol solution. Pt-Rh- Sn/C catalyst is highly active for the ethanol oxidation with the onset potential shifted for more than 150 mV to negative values and with currents nearly 5 times higher in comparison to Pt/C catalyst. The stability tests of the catalysts, as studied by the chronoamperometric experiments, reveal that the Pt-Rh-Sn/C catalyst is evidently less poisoned then Pt/C catalyst. The increased activity of Pt-Rh-Sn/C in comparison to Pt/C catalyst is most probably promoted by bifunctional mechanism and the electronic effect of alloyed metals.

Spontaneous deposition of Ru on Pt (100: morphological and electrochemical studies. Preliminary results of ethanol oxidation at Pt(100/Ru

Directory of Open Access Journals (Sweden)

Colle Vinicius D.

2003-01-01

Full Text Available In the present work ruthenium was deposited in submonolayer amounts on Pt(100 by spontaneous deposition at several deposition times. The Pt (100/Ru surfaces were analyzed using ex-situ STM to image the deposits characteristic of ruthenium on Pt (100. It was observed the formation of ruthenium islands with diameters between 1.0 and 4.5 nm with bi-atomic thickness in the center of the islands. A homogeneous distribution of the ruthenium islands on the platinum terraces was found, with no preferential deposition on steps or surface defect sites. The ruthenium coverage degree had been calculated by the decrease of charge of the hydrogen adsorption-desorption peaks in the cyclic voltammograms of the Pt(100/Ru electrodes. The Pt(100/Ru electrodes with a ruthenium coverage degree of ca. 0.3 showed a high activity for the ethanol electrooxidation. The electrochemical experimental results support strongly the bifunctional mechanism for the enhanced ethanol oxidation.

Effect of the structural characteristics of binary Pt-Ru and ternary Pt-Ru-M fuel cell catalysts on the activity of ethanol electrooxidation in acid medium.

Science.gov (United States)

Antolini, Ermete

2013-06-01

In view of their possible use as anode materials in acid direct ethanol fuel cells, the electrocatalytic activity of Pt-Ru and Pt-Ru-M catalysts for ethanol oxidation has been investigated. This minireview examines the effects of the structural characteristics of Pt-Ru, such as the degree of alloying and Ru oxidation state, on the electrocatalytic activity for ethanol oxidation. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Study the Polyol Process of Preparing the ru Doped FePt Nanoparticles

Science.gov (United States)

Lee, Chih-Hao; Hsu, Jen-Ho; Su, Hui-Chia; Huang, Tzu Wen

The structure of Ru doped FePt nanoparticles using polyol process was studied. The particle size grown is around 5 nm, and a shell structure might be formed. By selecting the time and temperature of adding the Ru precursors into solution, three different processes to synthesize the FePtRu particles were studied resulting in different growing mechanics. The possible models during the reaction process are also discussed. The phase transition temperature for the as-grown FCC FePt nanoparticle to transform into L10 FePt nanoparticle is about 823 K which is about the same as the one without doping Ru atoms. From the XAS study of each element, the possible scenario is that: although Ru atoms with the size close to the Pt, they do not totally replace the Pt sites in the FePt alloy. Instead, most of Ru formed a shell outside the FePt nanoparticles and Fe atoms are replaced.

Core-level binding energy shifts in Pt Ru nanoparticles: A puzzle resolved

Science.gov (United States)

Lewera, Adam; Zhou, Wei Ping; Hunger, Ralf; Jaegermann, Wolfram; Wieckowski, Andrzej; Yockel, Scott; Bagus, Paul S.

2007-10-01

Synchrotron measurements of Pt and Ru core-level binding energies, BE's, in Pt-Ru nanoparticles, as a function of Pt content, quantify earlier indications that the Pt 4f BE shift is much larger than the Ru 3d BE shift. A complementary theoretical analysis relates the BE shifts to changes in the metal-metal distances as the composition of the nanoparticle changes. We establish that the large Pt and small Ru BE shifts arise from the different response of these metals to changes in the bond distances, an unexpected result. Our results give evidence that the magnitudes of the BE shifts depend on whether the d band is open, as for Ru, or essentially filled, as for Pt.

The Design, Synthesis and Study of Mixed-Metal Ru,Rh and Os, Rh Complexes with Biologically Relevant Reactivity

OpenAIRE

Wang, Jing

2013-01-01

A series of mixed-metal bimetallic complexes [(TL)2M(dpp)RhCl2(TL)]3 (M = Ru and Os, terminal ligands (TL) = phen, Ph2phen, Me2phen and bpy, terminal ligands (TL) = phen, bpy and Me2bpy ), which couple one Ru or Os polyazine light absorber (LA) to a cis-RhIIICl2 center through a dpp bridging ligand (BL), were synthesized using a building block method. These are related to previously studied trimetallic systems [{(TL)2M(dpp)2RhCl2]5+, but the bimetallics are synthetically more complex to prepa...

Partitioning of rhodium and ruthenium between Pd–Rh–Ru and (Ru,Rh)O{sub 2} solid solutions in high-level radioactive waste glass

Energy Technology Data Exchange (ETDEWEB)

Sugawara, Toru, E-mail: toru@gipc.akita-u.ac.jp [Center for Engineering Science, Akita University, 1-1, Tegatagakuenmachi, Akita City, Akita 010-8502 (Japan); Ohira, Toshiaki [Center for Engineering Science, Akita University, 1-1, Tegatagakuenmachi, Akita City, Akita 010-8502 (Japan); Komamine, Satoshi; Ochi, Eiji [Research and Development Department, Reprocessing Business Division, Japan Nuclear Fuel Limited, 4-108, Okitsuke, Obuchi, Rokkasho-mura, Aomori 039-3212 (Japan)

2015-10-15

The partitioning of rhodium and ruthenium between Pd–Rh–Ru alloy with a face-centered cubic (FCC) structure and (Ru,Rh)O{sub 2} solid solution has been investigated between 1273 and 1573 K at atmospheric oxygen fugacity. The rhodium and ruthenium contents in FCC increase, while the RhO{sub 2} content in (Ru,Rh)O{sub 2} decreases with increasing temperature due to progressive reduction of the system. Based on the experimental results and previously reported thermodynamic data, the thermodynamic mixing properties of FCC phase and (Ru,Rh)O{sub 2} have been calibrated in an internally consistent manner. Phase equilibrium of platinum grope metals in an HLW glass was calculated by using the obtained thermodynamic parameters.

Pt and PtRu nanoparticles supported on N-doped carbons as electrocatalysts for methanol electro oxidation

Energy Technology Data Exchange (ETDEWEB)

Pereira, Viviane Santos; Silva, Julio Cesar Martins; Oliveira Neto, Almir; Spinace, Estevam Vitorio, E-mail: viviane_sp_saopaulo@yahoo.com.br [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

2016-07-01

Full text: Methanol is a liquid transportation fuel that can be produced from fossil or renewable resources. Fuel cells employing methanol directly as fuel (Direct Methanol Fuel Cell - DMFC) are very attractive as power source for portable, mobile and stationary applications [1]. PtRu/C electrocatalyst has been considered the best electrocatalyst for methanol electro-oxidation, however, its performance is strongly dependent on the method of preparation and on the characteristics of the carbon support. N-doped carbons with different N contents (1, 2 and 5 wt%) were prepared by thermal treatment of carbon with urea at 800 deg C. Pt and PtRu nanoparticles were supported on N-doped carbons by coreduction of Pt(IV) and Ru(III) ions using an alcohol-reduction process [2]. The obtained materials were characterized by Energy Dispersive X-ray spectroscopy, X-ray diffraction, Transmission electron microscopy and Cyclic Voltammetry. Pt and PtRu nanoparticles supported on N-doped carbons showed superior performance for methanol electro-oxidation when compared to the materials supported on non-modified carbon and to Pt/C and PtRu/C commercial electrocatalysts. Pt/C and PtRu/C prepared with the carbon modified with 2.5 wt% of N content showed the best activities. (author) [1] Y. Zhou, K. Neyerlin, T.S. Olson, S. Pylypenko, J. Bult, H.N. Dinh, T. Gennett, Z. Shao and R. O'Hayre, Energy Environ. Sci. 3, 1437 (2010); [2] E.V. Spinace, A.Oliveira Neto, T.R.R. Vasconcellos, M. Linardi, J. Power Sources 137, 17 (2004)

Electro-oxidation of ethanol and ethylene glycol on carbon-supported nano-Pt and -PtRu catalyst in acid solution

International Nuclear Information System (INIS)

Chatterjee, Moitrayee; Chatterjee, Abhik; Ghosh, Susanta; Basumallick, I.

2009-01-01

Present paper reports kinetics of electro-oxidation of ethanol (EtOH) and ethylene glycol (EG) onto Pt and PtRu nanocatalysts of different compositions in the temperature range of 298-318 K. These catalysts have been characterized by SEM, EDX, XRD, CV and amperometry. It has been observed that apparent activation energies for oxidation of EtOH and EG pass through a minimum at about 15-20 at.% of Ru in the PtRu alloy catalysts. Anodic peak current vs. composition curve also shows a maximum around this composition. The results have been explained by a geometric model, which proposes requirement of an ensemble of three Pt atoms with an adjacent Ru atom onto PtRu surface for an efficient electro-oxidation of EtOH or EG. This is further supported from statistical data analysis of probability of occurrence of such ensembles onto PtRu alloy surface. Present results also suggest that electro-oxidation of EG onto nano-PtRu catalyst surfaces follows a different path from that of EtOH at alloy composition less than 15 at.% of Ru.

Electro-oxidation of ethanol and ethylene glycol on carbon-supported nano-Pt and -PtRu catalyst in acid solution

Energy Technology Data Exchange (ETDEWEB)

Chatterjee, Moitrayee; Chatterjee, Abhik; Ghosh, Susanta [Electrochemical Laboratory, Department of Chemistry, Visva-Bharati University, Santiniketan 731235 (India); Basumallick, I., E-mail: ibasumallick@yahoo.co.u [Electrochemical Laboratory, Department of Chemistry, Visva-Bharati University, Santiniketan 731235 (India)

2009-12-01

Present paper reports kinetics of electro-oxidation of ethanol (EtOH) and ethylene glycol (EG) onto Pt and PtRu nanocatalysts of different compositions in the temperature range of 298-318 K. These catalysts have been characterized by SEM, EDX, XRD, CV and amperometry. It has been observed that apparent activation energies for oxidation of EtOH and EG pass through a minimum at about 15-20 at.% of Ru in the PtRu alloy catalysts. Anodic peak current vs. composition curve also shows a maximum around this composition. The results have been explained by a geometric model, which proposes requirement of an ensemble of three Pt atoms with an adjacent Ru atom onto PtRu surface for an efficient electro-oxidation of EtOH or EG. This is further supported from statistical data analysis of probability of occurrence of such ensembles onto PtRu alloy surface. Present results also suggest that electro-oxidation of EG onto nano-PtRu catalyst surfaces follows a different path from that of EtOH at alloy composition less than 15 at.% of Ru.

Radiolytic synthesis of carbon-supported PtRu nanoparticles using high-energy electron beam: effect of pH control on the PtRu mixing state and the methanol oxidation activity

International Nuclear Information System (INIS)

Ohkubo, Yuji; Kageyama, Satoru; Seino, Satoshi; Nakagawa, Takashi; Kugai, Junichiro; Nitani, Hiroaki; Ueno, Koji; Yamamoto, Takao A.

2013-01-01

Electrode catalysts composed of carbon-supported PtRu nanoparticles (PtRu/C) for use as a direct methanol fuel cell anode were synthesized by the reduction of precursor ions in an aqueous solution via irradiation with a high-energy electron beam. The effect of pH control in the precursor solution on the PtRu mixing state and the methanol oxidation activity was studied in order to enhance the catalytic activity for methanol oxidation. The PtRu/C structures were characterized by transmission electron microscopy, inductively coupled plasma atomic emission spectrometry, X-ray fluorescence spectrometry, and X-ray diffraction and X-ray absorption fine structure techniques. The methanol oxidation activity was evaluated by linear sweep voltammetry. The initial pH of the precursor solution has little influence on the average grain size for the metal particles (approximately 3.5 nm) on the carbon particle supports, but the dispersibility of the metal particles, PtRu mixing state, and methanol oxidation activity differed. The maintenance of a low pH in the precursor solution gave the best dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles, whereas, a high pH gave the best PtRu mixing state and the highest oxidation current although a low dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles was obtained. The PtRu mixing state strongly correlated with the methanol oxidation current. In addition, a high pH was more effective for PtRu mixing when using an electron beam irradiation reduction method, because the complexation reaction of the chelating agents was improved, which resulted in an enhancement of the catalytic activity for methanol oxidation.

Radiolytic synthesis of carbon-supported PtRu nanoparticles using high-energy electron beam: effect of pH control on the PtRu mixing state and the methanol oxidation activity

Energy Technology Data Exchange (ETDEWEB)

Ohkubo, Yuji, E-mail: okubo@mit.eng.osaka-u.ac.jp; Kageyama, Satoru; Seino, Satoshi; Nakagawa, Takashi; Kugai, Junichiro [Osaka University, Graduate School of Engineering (Japan); Nitani, Hiroaki [High Energy Accelerator Research Organization (KEK), Institute of Materials Structure Science (Japan); Ueno, Koji [Japan Electron Beam Irradiation Service Ltd (Japan); Yamamoto, Takao A. [Osaka University, Graduate School of Engineering (Japan)

2013-05-15

Electrode catalysts composed of carbon-supported PtRu nanoparticles (PtRu/C) for use as a direct methanol fuel cell anode were synthesized by the reduction of precursor ions in an aqueous solution via irradiation with a high-energy electron beam. The effect of pH control in the precursor solution on the PtRu mixing state and the methanol oxidation activity was studied in order to enhance the catalytic activity for methanol oxidation. The PtRu/C structures were characterized by transmission electron microscopy, inductively coupled plasma atomic emission spectrometry, X-ray fluorescence spectrometry, and X-ray diffraction and X-ray absorption fine structure techniques. The methanol oxidation activity was evaluated by linear sweep voltammetry. The initial pH of the precursor solution has little influence on the average grain size for the metal particles (approximately 3.5 nm) on the carbon particle supports, but the dispersibility of the metal particles, PtRu mixing state, and methanol oxidation activity differed. The maintenance of a low pH in the precursor solution gave the best dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles, whereas, a high pH gave the best PtRu mixing state and the highest oxidation current although a low dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles was obtained. The PtRu mixing state strongly correlated with the methanol oxidation current. In addition, a high pH was more effective for PtRu mixing when using an electron beam irradiation reduction method, because the complexation reaction of the chelating agents was improved, which resulted in an enhancement of the catalytic activity for methanol oxidation.

Preparation of PtRu/C and PtSn/C electrocatalysts using electron beam irradiation for direct and ethanol fuel cell

International Nuclear Information System (INIS)

Silva, Dionisio Furtunato da

2009-01-01

PtRu/C and PtSn/C electrocatalysts were prepared using electron beam irradiation. The metal ions were dissolved in water/2-propanol and water/ethylene glycol solutions and the carbon support was added. The resulting mixtures were irradiated under stirring. The effect of water/ethylene glycol and water/2-propanol (v/v) ratio, Pt:Ru and Pt:Sn atomic ratios, the irradiation time and dose rate were studied. The obtained materials were characterized by Energy dispersive analysis of X-rays (EDX), X-ray diffraction (XRD), cyclic voltammetry (CV) and Moessbauer spectroscopy. The electro-oxidation of methanol and ethanol were studied by cyclic voltammetry and chronoamperometry using the thin porous coating technique. The electrocatalysts were also tested on the Direct Methanol and Ethanol Fuel Cells. PtRu/C electrocatalysts prepared in water/ethylene glycol showed Pt:Ru atomic ratios different from the nominal ones. The results suggested that part of the Ru(III) ions were not reduced. The obtained materials showed the face-centered cubic (fcc) structure of Pt and Pt alloys with crystallite sizes of 2-3 nm. PtRu/C electrocatalysts prepared in water/2-propanol showed Pt:Ru atomic ratios similar to the nominal ones. The obtained materials also showed the fcc structure of platinum and platinum alloys with crystallite sizes of 3-4 nm. PtSn/C electrocatalysts prepared in water/ethylene glycol and water/2-propanol showed Pt:Sn atomic ratios similar to the nominal ones. The obtained materials showed the platinum (fcc) phase with crystallite sizes in the range of 2 - 4 nm and a SnO 2 (cassiterite) phase. The obtained PtRu/C and PtSn/C electrocatalysts showed similar or superior performance for methanol and ethanol electro-oxidation compared to commercial PtRu/C (E-TEK) and PtSn/C (BASF) electrocatalysts. (author)

PtRu nanoparticles dispersed on nitrogen-doped carbon nanohorns as an efficient electrocatalyst for methanol oxidation reaction

International Nuclear Information System (INIS)

Zhang, Linwei; Gao, Ang; Liu, Yan; Wang, Yuan; Ma, Jiantai

2014-01-01

Highlights: • A novel anode catalyst is synthesized using N-doped carbon nanohorns as support. • PtRu/NCNHs exhibits an excellent activity for MOR relative to PtRu/C catalysts. • The enhancement is due to the electronic interaction between NCNHs and PtRu NPs. - Abstract: A novel anode catalyst (PtRu/NCNHs) assembled with nitrogen-doped carbon nanohorns (NCNHs) and PtRu nanoparticles (1.9 nm) exhibits an obvious enhancement in the tolerance to carbonaceous intermediates and the electocatalytic activity for methanol oxidation reaction (MOR) in comparison to a commercial PtRu/C-JM catalyst and a home-made PtRu/Vulcan catalyst. The MOR mass activity of PtRu/NCNHs (850 mA mg −1 PtRu ) is 2.5 times as high as that of PtRu/C-JM (341 mA mg −1 PtRu ). The MOR specific activity of PtRu/NCNHs is 1.8 times as high as that of PtRu/Vulcan having similar Pt/Ru atomic ratios, specific electrochemical surface areas and particle sizes of PtRu NPs. The electronic interaction between PtRu NPs and NCNHs is responsible for the enhancement in the MOR activity of PtRu/NCNHs

CO and ethanol electro-oxidation on Pt-Rh/C

OpenAIRE

Calderón-Cárdenas, Alfredo; Ortiz-Restrepo, John E.; Mancilla-Valencia, Nelson D.; Torres-Rodriguez, Gerardo A.; Lima, Fabio H. B.; Bolaños-Rivera, Alberto; Gonzalez, Ernesto R.; Lizcano-Valbuena, William H.

2014-01-01

In this work we studied the effect of the composition and thermal treatment in H2 of Pt-Rh/C materials with atomic ratios close to Pt:Rh 3:1, 1:1 and 1:3 and metal loading of 40 wt. %, for the COads and ethanol oxidation. Catalysts were prepared by chemical reduction with formic acid and physically characterized by energy dispersive X-rays spectroscopy (EDX), electron backscattering (EBS) and transmission electron microscopy (TEM), showing Pt:Rh ratios close to the nominals values, similar av...

Preparation and characterization of multi-walled carbon nanotube (MWCNTs)-supported Pt-Ru catalyst for methanol electrooxidation

Energy Technology Data Exchange (ETDEWEB)

Yang Chunwei [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China)], E-mail: cw.yang@hit.edu.cn; Wang Dianlong; Hu Xinguo; Dai Changsong [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Zhang Liang [School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081 (China)

2008-01-10

Multi-walled carbon nanotubes (MWCNTs) as a support of PtRu catalyst nanocomposites were prepared by colloid method in this work. Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) all indicate that ultrasonic treatment can effectively functionalize MWCNTs, endowing them with groups that can act as nucleation sites which can favor well-dispersed deposition of PtRu clusters on their surface. The PtRu/MWCNTs catalysts have a high and homogeneous dispersion of spherical PtRu metal particles with a narrow particle-size distribution. From XPS tests, in PtRu/MWCNTs catalysts Ru can weaken the out-shell electrons of Pt because a part of Ru form alloy with Pt. The remnant Ru exists in oxidation and provides abundant oxygen to nearby Pt, as accelerated desorption and oxidation of intermediate products of methanol oxidation at surface of Pt. By a series of electrochemistry measurements, the PtRu/MWCNTs catalysts display significantly higher performance than the PtRu/XC-72 catalysts. Finally, schematic procedures for the oxidation of MWCNTs and synthesis of PtRu/MWCNTs catalysts were given.

Preparation and characterization of multi-walled carbon nanotube (MWCNTs)-supported Pt-Ru catalyst for methanol electrooxidation

International Nuclear Information System (INIS)

Yang Chunwei; Wang Dianlong; Hu Xinguo; Dai Changsong; Zhang Liang

2008-01-01

Multi-walled carbon nanotubes (MWCNTs) as a support of PtRu catalyst nanocomposites were prepared by colloid method in this work. Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) all indicate that ultrasonic treatment can effectively functionalize MWCNTs, endowing them with groups that can act as nucleation sites which can favor well-dispersed deposition of PtRu clusters on their surface. The PtRu/MWCNTs catalysts have a high and homogeneous dispersion of spherical PtRu metal particles with a narrow particle-size distribution. From XPS tests, in PtRu/MWCNTs catalysts Ru can weaken the out-shell electrons of Pt because a part of Ru form alloy with Pt. The remnant Ru exists in oxidation and provides abundant oxygen to nearby Pt, as accelerated desorption and oxidation of intermediate products of methanol oxidation at surface of Pt. By a series of electrochemistry measurements, the PtRu/MWCNTs catalysts display significantly higher performance than the PtRu/XC-72 catalysts. Finally, schematic procedures for the oxidation of MWCNTs and synthesis of PtRu/MWCNTs catalysts were given

Effects of composition on structure and activity of PtRu/C catalysts.

Science.gov (United States)

Wiltshire, Richard J K; King, Colin R; Rose, Abigail; Wells, Peter P; Davies, Hazel; Hogarth, Martin P; Thompsett, David; Theobald, Brian; Mosselmans, Fredrick W; Roberts, Mark; Russell, Andrea E

2009-04-07

A series of carbon supported PtRu bimetallic catalysts with varying Pt:Ru ratio were prepared and characterised using ex situ and in situ XRD, in situ EXAFS at 0 V vs. RHE, ex situ XPS and monolayer CO stripping voltammetry. Although the catalysts were found to be well mixed/alloyed, with no evidence of unalloyed Ru (oxides) present, the surfaces of the electrocatalyst nanoparticles were found to be enriched with Pt compared to the nominal bulk composition. The methanol oxidation activities of the catalysts were determined in 1.0 mol dm(-3) H2SO4. In agreement with published studies of polycrystalline bulk PtRu alloys the catalyst with a 0.6 surface fraction of Pt was found to give the best methanol oxidation activity at 30 degrees C. However, at 80 degrees C a greater surface fraction of Ru could be tolerated, with some activity at low current densities found for a Pt surface fraction as low as 0.2. The results support the conclusion that a limited amount of methanol dehydrogenation occurs at Ru sites or Ru dominated surface ensembles at 80 degrees C.

O2-enhanced methanol oxidation reaction at novel Pt-Ru-C co-sputtered electrodes

International Nuclear Information System (INIS)

Umeda, Minoru; Matsumoto, Yosuke; Inoue, Mitsuhiro; Shironita, Sayoko

2013-01-01

Highlights: ► Novel Pt-Ru-C electrodes were prepared by a co-sputtering technique. ► Co-sputtered electrodes with C result in highly efficient O 2 -enhanced methanol oxidation. ► Pt–Ru-alloy-based co-sputtered electrode induces a negative onset potential of methanol oxidation. ► The Pt-Ru-C electrodes allow a negative onset potential of O 2 -enhanced methanol oxidation. ► The optimum atomic ratios of Pt-Ru-C are Pt: 0.24–0.80, Ru: 0.14–0.61, C: 0.06–0.37. -- Abstract: A Pt-Ru-C electrode has been developed using a co-sputtering technique for use as the anode catalyst of a mixed-reactant fuel cell. The physical and electrochemical characteristics of the electrodes demonstrate that co-sputtered Pt and Ru form a Pt–Ru alloy. The crystallite sizes of the catalysts investigated in this study are reduced by the addition of C to the Pt–Ru alloy. Cu stripping voltammograms suggest that the sputtering of C and the formation of the Pt–Ru alloy synergically increase the electrochemical surface area of the electrodes. The methanol oxidation performances of the prepared electrodes were evaluated in N 2 and O 2 atmospheres; the Pt-Ru-C electrodes achieve an O 2 -induced negative shift in the onset potential of the methanol oxidation (E onset ) and enhance the methanol oxidation current density in the O 2 atmosphere. The mechanism of O 2 -enhanced methanol oxidation with a negative E onset at the Pt-Ru-C electrodes is attributed to a change in the electronic structure of Pt due to the formation of Pt–Ru alloy and the generation of O-based adsorption species by the reduction of O 2 . Finally, the composition of the Pt-Ru-C electrode for the O 2 -enhanced methanol oxidation with a negative E onset was found to be optimal at an atomic ratio of Pt: 0.24–0.80, Ru: 0.14–0.61, and C: 0.06–0.37

Particle size dependence of CO tolerance of anode PtRu catalysts for polymer electrolyte fuel cells

Science.gov (United States)

Yamanaka, Toshiro; Takeguchi, Tatsuya; Wang, Guoxiong; Muhamad, Ernee Noryana; Ueda, Wataru

An anode catalyst for a polymer electrolyte fuel cell must be CO-tolerant, that is, it must have the function of hydrogen oxidation in the presence of CO, because hydrogen fuel gas generated by the steam reforming process of natural gas contains a small amount of CO. In the present study, PtRu/C catalysts were prepared with control of the degree of Pt-Ru alloying and the size of PtRu particles. This control has become possible by a new method of heat treatment at the final step in the preparation of catalysts. The CO tolerances of PtRu/C catalysts with the same degree of Pt-Ru alloying and with different average sizes of PtRu particles were thus compared. Polarization curves were obtained with pure H 2 and CO/H 2 (CO concentrations of 500-2040 ppm). It was found that the CO tolerance of highly dispersed PtRu/C (high dispersion (HD)) with small PtRu particles was much higher than that of poorly dispersed PtRu/C (low dispersion (LD)) with large metal particles. The CO tolerance of PtRu/C (HD) was higher than that of any commercial PtRu/C. The high CO tolerance of PtRu/C (HD) is thought to be due to efficient concerted functions of Pt, Ru, and their alloy.

Ternary Pt-Ru-Ni catalytic layers for methanol electrooxidation prepared by electrodeposition and galvanic replacement

Directory of Open Access Journals (Sweden)

Athanasios ePapaderakis

2014-06-01

Full Text Available Ternary Pt-Ru-Ni deposits on glassy carbon substrates, Pt-Ru(Ni/GC, have been formed by initial electrodeposition of Ni layers onto glassy carbon electrodes, followed by their partial exchange for Pt and Ru, upon their immersion into equimolar solutions containing complex ions of the precious metals. The overall morphology and composition of the deposits has been studied by SEM microscopy and EDS spectroscopy. Continuous but nodular films have been confirmed, with a Pt÷Ru÷Ni % bulk atomic composition ratio of 37÷12÷51 (and for binary Pt-Ni control systems of 47÷53. Fine topographical details as well as film thickness have been directly recorded using AFM microscopy. The composition of the outer layers as well as the interactions of the three metals present have been studied by XPS spectroscopy and a Pt÷Ru÷Ni % surface atomic composition ratio of 61÷12÷27 (and for binary Pt-Ni control systems of 85÷15 has been found, indicating the enrichment of the outer layers in Pt; a shift of the Pt binding energy peaks to higher values was only observed in the presence of Ru and points to an electronic effect of Ru on Pt. The surface electrochemistry of the thus prepared Pt-Ru(Ni/GC and Pt(Ni/GC electrodes in deaerated acid solutions (studied by cyclic voltammetry proves the existence of a shell consisting exclusively of Pt-Ru or Pt. The activity of the Pt-Ru(Ni deposits towards methanol oxidation (studied by slow potential sweep voltammetry is higher from that of the Pt(Ni deposit and of pure Pt; this enhancement is attributed both to the well-known Ru synergistic effect due to the presence of its oxides but also (based on the XPS findings to a modification effect of Pt electronic properties.

H2-splitting on Pt/Ru alloys supported on sputtered HOPG

DEFF Research Database (Denmark)

Fiordaliso, Elisabetta Maria; Dahl, Søren; Chorkendorff, Ib

2011-01-01

to strain and ligand effects, caused by the compression of the surface due to the presence of the larger Pt atoms in the neighboring Ru atoms. The apparent energy of desorption at equilibrium, Eapp, for the three Pt-Ru systems is found to decrease with an increasing amount of Ru in the alloys...

PtRu colloid nanoparticles for CO oxidation in microfabricated reactors

DEFF Research Database (Denmark)

Klerke, Asbjørn; Saadi, Souheil; Toftegaard, Maja Bøg

2006-01-01

The catalytic activity of PtRu colloid nanoparticles for CO oxidation is investigated in microfabricated reactors. The measured catalytic performance describes a volcano curve as a function of the Pt/Ru ratio. The apparent activation energies for the different alloy catalysts are between 21 and 1...

Preparation and characterization of PtRu/C, PtBi/C, PtRuBi/C electrocatalysts for direct electro-oxidation of ethanol in PEM fuels cells using the method of reduction by sodium borohydride

International Nuclear Information System (INIS)

Brandalise, Michele

2010-01-01

Pt/C, PtBi/C, PtRu/C and PtRuBi/C electrocatalysts were prepared by a borohydride reduction methodology and tested for ethanol oxidation. This methodology consists in mix a solution with sodium hydroxide and sodium borohydride to a mixture containing water/isopropyl alcohol, metallic precursors and the Vulcan XC 72 carbon support. It was studied the addition method of borohydride (drop by drop addition or rapid addition). The obtained electrocatalysts were characterized by energy dispersive X ray spectroscopy (EDX), thermogravimetric analysis (TGA), X ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry. The ethanol electro-oxidation was studied by cyclic voltammetry and chronoamperometry using the thin porous coating technique. The electrocatalysts were tested in real conditions of operation by unit cell tests. The stability of PtRuBi/C electrocatalysts was evaluated by cyclic voltammetry, chronoamperometry using the ultra-thin porous coating technique and ring-disk electrode. The PtRuBi/C electro catalyst apparently presented a good performance for ethanol electro-oxidation but experimental evidences showed accentuated bismuth dissolution. (author)

PtRu nanoparticles embedded in nitrogen doped carbon with highly stable CO tolerance and durability

Science.gov (United States)

Ling, Ying; Yang, Zehui; Yang, Jun; Zhang, Yunfeng; Zhang, Quan; Yu, Xinxin; Cai, Weiwei

2018-02-01

As is well known, the lower durability and sluggish methanol oxidation reaction (MOR) of PtRu alloy electrocatalyst blocks the commercialization of direct methanol fuel cells (DMFCs). Here, we design a new PtRu electrocatalyst, with highly stable CO tolerance and durability, in which the PtRu nanoparticles are embedded in nitrogen doped carbon layers derived from carbonization of poly(vinyl pyrrolidone). The newly fabricated electrocatalyst exhibits no loss in electrochemical surface area (ECSA) and MOR activity after potential cycling from 0.6-1.0 V versus reversible hydrogen electrode, while commercial CB/PtRu retains only 50% of its initial ECSA. Meanwhile, due to the same protective layers, the Ru dissolution is decelerated, resulting in stable CO tolerance. Methanol oxidation reaction (MOR) testing indicates that the activity of newly fabricated electrocatalyst is two times higher than that of commercial CB/PtRu, and the fuel cell performance of the embedded PtRu electrocatalyst was comparable to that of commercial CB/PtRu. The embedded PtRu electrocatalyst is applicable in real DMFC operation. This study offers important and useful information for the design and fabrication of durable and CO tolerant electrocatalysts.

Effect of TiO_2 Loading on Pt-Ru Catalysts During Alcohol Electrooxidation

International Nuclear Information System (INIS)

Hasa, Bjorn; Kalamaras, Evangelos; Papaioannou, Evangelos I.; Vakros, John; Sygellou, Labrini; Katsaounis, Alexandros

2015-01-01

Highlights: • TiO_2 can be used to modify Pt-Ru based electrodes for alcohol oxidation. • TiO_2 modified electrodes with lower amount of metals had higher active surface area than pure Pt-Ru electrodes. • TiO_2 modified electrodes showed comparable performance with pure Pt-Ru electrode both in a single cell and in a PEM fuel cell under alcohol fuelling. - Abstract: In this study, Pt-Ru based electrodes modified by TiO_2 were prepared by means of thermal decomposition of chloride and isopropoxide precursors on Ti substrates, characterised by X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), X-ray Photoelectron Spectroscopy (XPS), electrochemical techniques and CO stripping and used as anodes for alcohol oxidation. The minimization of the metal loading without electrocatalytic activity losses was also explored. TiO_2 was chosen due to its chemical stability, low cost and excellent properties as substrate for metal dispersion. It was found that TiO_2 loading up to 50% results in a 3-fold increase of the Electrochemically Active Surface (EAS). This conclusion has been confirmed by CO stripping experiments. All samples have been evaluated during the electrochemical oxidation of methanol, ethanol and glycerol. In all cases, the Pt_2_5-Ru_2_5-(TiO_2)_5_0 electrode had better electrocatalytic activity than the pure Pt_5_0-Ru_5_0 anode. The best modified electrode, (Pt_2_5-Ru_2_5-(TiO_2)_5_0), was also evaluated as anode in a PEM fuel cell under methanol fuelling conditions. The observed higher performance of the TiO_2 modified electrodes was attributed to the enhanced Pt-Ru dispersion as well as the formation of smaller Pt and Ru particles.

Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability.

Science.gov (United States)

Jackson, Ariel; Strickler, Alaina; Higgins, Drew; Jaramillo, Thomas Francisco

2018-01-12

Improving the performance of oxygen reduction reaction (ORR) electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs). Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C) prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mg Pt -1 at 0.9 V versus the reversible hydrogen electrode (RHE), which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing) are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mg Pt -1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s -1 ), maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS) analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

Effect of W on activity of Pt-Ru/C catalyst for methanol electrooxidation in acidic medium

International Nuclear Information System (INIS)

Wang Zhenbo; Zuo Pengjian; Yin Geping

2009-01-01

The effect of W on the activity of Pt-Ru/C catalyst was investigated. The Pt-Ru-W/C and Pt-Ru/C-TR catalysts were prepared by thermal reduction method. Comparison was made to a homemade Pt-Ru/C-CR catalyst prepared by chemical reduction. Their performances were tested by using a glassy carbon thin film electrode through cyclic voltammetric and chronoamperometric curves. The particle size, structure, composition, and surface state of homemade catalyst were determined by means of X-ray diffraction (XRD), energy dispersive analysis of X-ray (EDAX), transmission electron microscopy (TEM), and X-ray photoelectron spectrometry (XPS). The result of XRD analysis shows that the homemade ternary catalyst exhibits face-centered cubic structure and has smaller lattice parameter than Pt-alone and homemade Pt-Ru/C catalysts. The particle size of Pt-Ru-W/C catalyst is relatively large of 6.5 nm. Its electrochemically active specific area is 20 m 2 g -1 less than that of Pt-Ru/C-CR, and much twice as big as that of Pt-Ru/C-TR. But, XPS analysis shows that the addition of W changes the surface state of Pt components in the alloy and can clean Pt surface active sites which are adsorbed by hydrogen. The electrocatalytic activity and tolerance performance to CO ads of Pt-Ru-W/C catalyst for methanol electrooxidation is the best due to the promoting function of W in comparison with homemade Pt-Ru/C ones.

Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media

International Nuclear Information System (INIS)

Stojmenović, Marija; Momčilović, Milan; Gavrilov, Nemanja; Pašti, Igor A.; Mentus, Slavko; Jokić, Bojan; Babić, Biljana

2015-01-01

Ordered mesoporous carbon, volume-doped up to 3 w.% with Pt, Ru and Pt-Ru nanoparticles was synthesized by evaporation-induced self-assembly method, under acidic conditions. The content of incorporated metal was determined by EDX analysis. The X-ray diffractometry confirmed the existence of highly dispersed metallic phases in doped samples. Specific surface area was determined by N 2 -physisorption measurements to range between 452 and 545 m 2 g −1 . Raman spectroscopy of investigated materials indicated highly disordered carbon structure with crystallite sizes around 1.4 nm. In a form of thin-layer electrode on glassy carbon support, in 0.1 M KOH solution, the prepared materials displayed high activity toward oxygen reduction reaction (ORR) in alkaline media, with onset potentials more positive than −0.10 V vs. SCE. The kinetics of O 2 reduction was found to be affected by both the specific surface area and the concentration of metal dopants. The ethanol tolerance of (Pt, Ru)-doped OMCs was found to be higher than that of common Pt/C ORR catalysts. Presented study provides a new route for the synthesis of active and selective ORR catalysts in alkaline media, being competitive with, or superior to, the existing ones in terms of performance and price

Pt-Ru nanoparticles supported on functionalized carbon as electrocatalysts for the methanol oxidation

International Nuclear Information System (INIS)

Salgado, J.R.C.; Fernandes, J.C.S.; Botelho do Rego, A.M.; Ferraria, A.M.; Duarte, R.G.; Ferreira, M.G.S.

2011-01-01

Highlights: → The functionalized carbon using acid solutions contains surface oxygenated groups. → Uniform dispersion of PtRu nanoparticles on the carbon surface was achieved. → Physical analysis showed the formation of PtRu alloy catalysts on functionalized carbon. → PtRu alloy catalysts on functionalized carbon enhanced the methanol oxidation rate. - Abstract: Platinum-ruthenium alloy electrocatalysts, for methanol oxidation reaction, were prepared on carbons thermally treated in helium atmosphere or chemically functionalized in H 2 O 2 , or in HNO 3 + H 2 SO 4 or in HNO 3 solutions. The functionalized carbon that is produced using acid solutions contains more surface oxygenated functional groups than carbon treated with H 2 O 2 solution or HeTT. The XRD/HR-TEM analysis have showed the existence of a higher alloying degree for Pt-Ru electrocatalysts supported on functionalized carbon, which present superior electrocatalytic performance, assessed by cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy, as compared to electrocatalysts on unfunctionalized carbon. It also was found that Pt-Ru alloy electrocatalysts on functionalized carbon improve the reaction rate compared to Pt-Ru on carbons treated with H 2 O 2 solution and thermally. A mechanism is discussed, where oxygenated groups generated from acid functionalization of carbon and adsorbed on Pt-Ru electrocatalysts are considered to enhance the electrocatalytic activity of the methanol oxidation reaction.

Electrocatalytic activity of atomic layer deposited Pt-Ru catalysts onto N-doped carbon nanotubes

NARCIS (Netherlands)

Johansson, A.-C.; Larsen, J.V.; Verheijen, M.A.; Haugshøj, K.B.; Clausen, H.; Kessels, W.M.M.; Christensen, L.H.; Thomsen, E.V.

2014-01-01

Pt-Ru catalysts of various compositions, between 0 and 100 at.% of Ru, were deposited onto N-doped multi-walled carbon nanotubes (N-CNTs) by atomic layer deposition (ALD) at 250 C. The Pt and Ru precursors were trimethyl(methylcyclopentadienyl)platinum (MeCpPtMe3) and

Electrochemical, spectroscopic, and photophysical properties of structurally diverse polyazine-bridged Ru(II),Pt(II) and Os(II),Ru(II),Pt(II) supramolecular motifs.

Science.gov (United States)

Knoll, Jessica D; Arachchige, Shamindri M; Wang, Guangbin; Rangan, Krishnan; Miao, Ran; Higgins, Samantha L H; Okyere, Benjamin; Zhao, Meihua; Croasdale, Paul; Magruder, Katherine; Sinclair, Brian; Wall, Candace; Brewer, Karen J

2011-09-19

Five new tetrametallic supramolecules of the motif [{(TL)(2)M(dpp)}(2)Ru(BL)PtCl(2)](6+) and three new trimetallic light absorbers [{(TL)(2)M(dpp)}(2)Ru(BL)](6+) (TL = bpy = 2,2'-bipyridine or phen = 1,10-phenanthroline; M = Ru(II) or Os(II); BL = dpp = 2,3-bis(2-pyridyl)pyrazine, dpq = 2,3-bis(2-pyridyl)quinoxaline, or bpm = 2,2'-bipyrimidine) were synthesized and their redox, spectroscopic, and photophysical properties investigated. The tetrametallic complexes couple a Pt(II)-based reactive metal center to Ru and/or Os light absorbers through two different polyazine BL to provide structural diversity and interesting resultant properties. The redox potential of the M(II/III) couple is modulated by M variation, with the terminal Ru(II/III) occurring at 1.58-1.61 V and terminal Os(II/III) couples at 1.07-1.18 V versus Ag/AgCl. [{(TL)(2)M(dpp)}(2)Ru(BL)](PF(6))(6) display terminal M(dπ)-based highest occupied molecular orbitals (HOMOs) with the dpp(π*)-based lowest unoccupied molecular orbital (LUMO) energy relatively unaffected by the nature of BL. The coupling of Pt to the BL results in orbital inversion with localization of the LUMO on the remote BL in the tetrametallic complexes, providing a lowest energy charge separated (CS) state with an oxidized terminal Ru or Os and spatially separated reduced BL. The complexes [{(TL)(2)M(dpp)}(2)Ru(BL)](6+) and [{(TL)(2)M(dpp)}(2)Ru(BL)PtCl(2)](6+) efficiently absorb light throughout the UV and visible regions with intense metal-to-ligand charge transfer (MLCT) transitions in the visible at about 540 nm (M = Ru) and 560 nm (M = Os) (ε ≈ 33,000-42,000 M(-1) cm(-1)) and direct excitation to the spin-forbidden (3)MLCT excited state in the Os complexes about 720 nm. All the trimetallic and tetrametallic Ru-based supramolecular systems emit from the terminal Ru(dπ)→dpp(π*) (3)MLCT state, λ(max)(em) ≈ 750 nm. The tetrametallic systems display complex excited state dynamics with quenching of the (3)MLCT emission at

Pt-Ru/CeO2/carbon nanotube nanocomposites: an efficient electrocatalyst for direct methanol fuel cells.

Science.gov (United States)

Sun, Zhenyu; Wang, Xiang; Liu, Zhimin; Zhang, Hongye; Yu, Ping; Mao, Lanqun

2010-07-20

Pt-Ru/CeO(2)/multiwalled carbon nanotube (MWNT) electrocatalysts were prepared using a rapid sonication-facilitated deposition method and were characterized by X-ray diffraction (XRD), X-ray photoemission spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersive spectroscopy (EDS), and voltammetry. Morphological characterization by TEM revealed that CeO(2) nanoparticles (NPs) were in intimate contact with Pt-Ru NPs, and both were highly dispersed on the exteriors of nanotubes with a small size and a very narrow size distribution. Compared with the Pt-Ru/MWNT and Pt/MWNT electrocatalysts, the as-prepared Pt-Ru/CeO(2)/MWNT exhibited a significantly improved electrochemically active surface area (ECSA) and a remarkably enhanced activity toward methanol oxidation. The effects of the Pt-Ru loading and the Pt-to-Ru molar ratio on the electrocatalytic activity of Pt-Ru/CeO(2)/MWNT for methanol oxidation were investigated. We found that a maximum activity toward methanol oxidation reached at the 10 wt % of Pt-Ru loading and 1:1 of Pt-to-Ru ratio. Moreover, the role of CeO(2) in the catalysts for the enhancement of methanol oxidation was discussed in terms of both bifunctional mechanism and electronic effects.

Ethylene glycol oxidation on Pt and Pt-Ru nanoparticle decorated polythiophene/multiwalled carbon nanotube composites for fuel cell applications

International Nuclear Information System (INIS)

Selvaraj, Vaithilingam; Alagar, Muthukaruppan

2008-01-01

A novel supporting material containing polythiophene (PTh) and multiwalled carbon nanotubes (MWCNTs) (PTh-CNTs) is prepared by in situ polymerization of thiophene on carbon nanotubes using FeCl 3 as oxidizing agent under sonication. The prepared polythiophene/CNT composites are further decorated with Pt and Pt-Ru nanoparticles by chemical reduction of the corresponding metal salts using HCHO as reducing agent at pH = 11 (Pt/PTh-CNT and Pt-Ru/PTh-CNT). The fabricated composite films decorated with nanoparticles were investigated towards the electrochemical oxidation of ethylene glycol (EG). The presence of carbon nanotubes in conjugation with a conducting polymer produces a good catalytic effect, which might be due to the higher electrochemically accessible surface areas, electronic conductivity and easier charge-transfer at polymer/electrolyte interfaces, which allows higher dispersion of Pt and Pt-Ru nanoparticles. Such nanoparticle modified PTh-CNT electrodes exhibit better catalytic behavior towards ethylene glycol oxidation. Results show that Pt/PTh-CNT and Pt-Ru/PTh-CNT modified electrodes show enhanced electrocatalytic activity and stability towards the electro-oxidation of ethylene glycol than the Pt/PTh electrodes, which shows that the composite film is more promising for applications in fuel cells

CO tolerance of PdPt/C and PdPtRu/C anodes for PEMFC

International Nuclear Information System (INIS)

Garcia, Amanda C.; Paganin, Valdecir A.; Ticianelli, Edson A.

2008-01-01

The performance of H 2 /O 2 proton exchange membrane fuel cells (PEMFCs) fed with CO-contaminated hydrogen was investigated for anodes with PdPt/C and PdPtRu/C electrocatalysts. The physicochemical properties of the catalysts were characterized by energy dispersive X-ray (EDX) analyses, X-ray diffraction (XRD) and 'in situ' X-ray absorption near edge structure (XANES). Experiments were conducted in electrochemical half and single cells by cyclic voltammetry (CV) and I-V polarization measurements, while DEMS was employed to verify the formation of CO 2 at the PEMFC anode outlet. A quite high performance was achieved for the PEMFC fed with H 2 + 100 ppm CO with the PdPt/C and PdPtRu/C anodes containing 0.4 mg metal cm -2 , with the cell presenting potential losses below 200 mV at 1 A cm -2 , with respect to the system fed with pure H 2 . For the PdPt/C catalysts no CO 2 formation was seen at the PEMFC anode outlet, indicating that the CO tolerance is improved due to the existence of more free surface sites for H 2 electrooxidation, probably due to a lower Pd-CO interaction compared to pure Pd or Pt. For PdPtRu/C the CO tolerance may also have a contribution from the bifunctional mechanism, as shown by the presence of CO 2 in the PEMFC anode outlet

Kinetic study of methanol oxidation on carbon-supported PtRu electrocatalyst

International Nuclear Information System (INIS)

Gojkovic, S.Lj.; Vidakovic, T.R.; Durovic, D.R.

2003-01-01

Methanol electrooxidation was investigated on the carbon-supported PtRu electrocatalyst (1:1 atomic ratio) in acid media. X-ray diffraction measurement indicated alloying of Pt and Ru. Cyclic voltammetry of the sample reflects the amount of Ru in the catalyst and its ability to adsorb OH radicals. Tafel plots for the oxidation of 0.02-3 M methanol in the solutions containing 0.05-1 M HClO 4 and in the temperature range 27-40 deg. C showed reasonably well-defined linear region with the slope of about 115 mV dec -1 at the low currents, irrespective of the experimental conditions employed. Reaction order with respect to methanol was found to be 0.5. A correlation between methanol oxidation rate and pseudocapacitive current of OH adsorption on Ru sites was established. It was proposed that bifunctional mechanism is operative with the reaction between methanol residues adsorbed on Pt sites and OH radicals adsorbed on Ru sites as the rate-determining step

Preparation of Pt Ru/C + rare earths by the method of reduction by alcohol for the electro-oxidation of ethanol; Preparacao de eletrocatalisadores PtRu/C + terras raras pelo metodo da reducao por alcool para a eletro-oxidacao do etanol

Energy Technology Data Exchange (ETDEWEB)

Tusi, M M; Rodrigues, R M.S.; Spinace, E V; Oliveira Neto, A., E-mail: aolivei@ipen.b, E-mail: espinace@ipen.b [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

2010-07-01

PtRu/C electrocatalyst was prepared in a single step, while that PtRu/85%C-15%Ce, PtRu/85%C-15%La, PtRu/85%C-15%Nd and PtRu/85%C-15%Er electrocatalyst were prepared in a two step. In the first step a Carbon Vulcan XC72 + rare earth supports were prepared. In the second step PtRu electrocatalyst were prepared by an alcohol-reduction process using ethylene glycol as solvent and reducing agent and supported on Vulcan XC72 + earth rare. The obtained electrocatalysts were characterized by EDAX, XRD and chronoamperometry. The electro-oxidation of ethanol was studied by chronoamperometry at room temperature. PtRu/85%C- 15%Ce electrocatalyst showed a significant increase of performance for ethanol oxidation compared to PtRu/C electrocatalyst. (author)

Engineering Ru@Pt Core-Shell Catalysts for Enhanced Electrochemical Oxygen Reduction Mass Activity and Stability

Directory of Open Access Journals (Sweden)

Ariel Jackson

2018-01-01

Full Text Available Improving the performance of oxygen reduction reaction (ORR electrocatalysts is essential for the commercial efficacy of many renewable energy technologies, including low temperature polymer electrolyte fuel cells (PEFCs. Herein, we report highly active and stable carbon-supported Ru@Pt core-shell nanoparticles (Ru@Pt/C prepared by a wet chemical synthesis technique. Through rotating disc electrode testing, the Ru@Pt/C achieves an ORR Pt mass-based activity of 0.50 A mgPt−1 at 0.9 V versus the reversible hydrogen electrode (RHE, which exceeds the activity of the state-of-the-art commercial Pt/C catalyst as well as the Department of Energy 2020 PEFC electrocatalyst activity targets for transportation applications. The impact of various synthetic parameters, including Pt to Ru ratios and catalyst pretreatments (i.e., annealing are thoroughly explored. Pt-based mass activity of all prepared Ru@Pt/C catalysts was found to exceed 0.4 mgPt−1 across the range of compositions investigated, with the maximum activity catalyst having a Ru:Pt ratio of 1:1. This optimized composition of Ru@Pt/C catalyst demonstrated remarkable stability after 30,000 accelerated durability cycles (0.6 to 1.0 V vs. RHE at 125 mV s−1, maintaining 85% of its initial mass activity. Scanning transmission electron microscopy energy dispersive spectroscopy (STEM-EDS analysis at various stages of electrochemical testing demonstrated that the Pt shell can provide sufficient protection against the dissolution of the otherwise unstable Ru core.

Effect of the structure of Pt-Ru/C particles on COad monolayer vibrational properties and electrooxidation kinetics

International Nuclear Information System (INIS)

Maillard, Frederic; Bonnefont, Antoine; Chatenet, Marian; Guetaz, Laure; Doisneau-Cottignies, Beatrice; Roussel, Herve; Stimming, Ulrich

2007-01-01

In this paper, we combined FTIR spectroscopy and CO ad stripping voltammetry to investigate CO ad adsorption and electrooxidation on Pt-Ru/C nanoparticles. The Pt:Ru elemental composition and the metal loading were determined by ICP-AES. The X-ray diffraction patterns of the Pt-Ru/C indicated formation of a Pt-Ru (fcc) alloy. HREM images revealed an increase in the fraction of agglomerated Pt-Ru/C particles with increasing the metal loading and showed that agglomerated Pt-Ru/C nanoparticles present structural defects such as twins or grain boundaries. In addition, isolated Pt-Ru/C nanoparticles have similar mean particle size (ca. 2.5 nm) and particle size distributions whatever the metal loading. Therefore, we could determine precisely the effect of particle agglomeration on the CO ad vibrational properties and electrooxidation kinetics. FTIR measurements revealed a main CO ad stretching band at ca. ν-bar CO L =2030cm -1 , which we ascribed to a-top CO ad on Pt domains electronically modified by the presence of Ru. As the metal loading increased, the position of this band was blue shifted by ca. 5 cm -1 and a shoulder around 2005 cm -1 developed, which was ascribed to a-top CO ad on Ru domains. The reason for this was suggested to be the increasing size of Ru domains on agglomerated Pt-Ru/C particles, which lifts dipole-dipole coupling and allows two vibrational features to be observed (CO ad /Ru, CO ad /Pt). This is evidence that FTIR spectroscopy can be used to probe small chemical fluctuations of the Pt-Ru/C surface. Finally, we comment on the CO ad electrooxidation kinetics. We observed that CO ad was converted more easily into CO 2 as the metal loading, i.e. the fraction of agglomerated Pt-Ru/C nanoparticles, increased

Kinetic study of methanol oxidation on Pt2Ru3/C catalyst in the alkaline media

Directory of Open Access Journals (Sweden)

A. V. TRIPKOVIC

2007-11-01

Full Text Available The interaction of acridine orange (AO with double-stranded (ds The electrochemical oxidation of methanol in NaOH solution was examined on a thin film Pt2Ru3/C electrode. The XRD pattern revealed that the Pt2Ru3 alloy consisted of a solid solution of Ru in Pt and a small amount of Ru or a solid solution of Pt in Ru. It was shown that in alkaline solution, the difference in activity between Pt/C and Pt2Ru3/C is significantly smaller than in acid solution. It is proposed that the reaction follows a quasi bifunctional mechanism. The kinetic parameters indicated that the chemical reaction between adsorbed COad and OHad species could be the rate limiting step.

Combinatorial investigation of Pt-Ru-Sn alloys as an anode electrocatalysts for direct alcohol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Chu, Young Hwan [Department of New Energy.Resource Engineering, College of Science and Engineering, Sangji University, 124, Sangjidae-gil, Wonju-si, Gangwon-Do 220-702 (Korea); Shul, Yong Gun [Department of Chemical and Biomolecular Engineering, Yonsei University, 134, Shinchon-Dong, Seodaemun-Gu, Seoul 120-749 (Korea)

2010-10-15

Low-temperature direct alcohol fuel cells fed with different kinds of alcohol (methanol, ethanol and 2-propanol) have been investigated by employing ternary electrocatalysts (Pt-Ru-Sn) as anode catalysts. Combinatorial chemistry has been applied to screen the 66-PtRuSn-anode arrays at the same time to reduce cost, time, and effort when we select the optimum composition of electrocatalysts for DAFCs (Direct Alcohol Fuel Cells). PtRuSn (80:20:0) showed the lowest onset potential for methanol electro-oxidation, PtRuSn (50:0:50) for ethanol, and PtRuSn (20:70:10) for 2-propanol in CV results respectively, and single cell performance test indicated that Ru is more suitable for direct methanol fuel cell system, Sn for direct ethanol fuel cell system, and 2-propanol could be applied as fuel with low platinum composition anode electrocatalyst. The single cell performance results and electrochemical results (CV) were well matched with the combinatorial electrochemical results. As a result, we could verify the availability of combinatorial chemistry by comparing the results of each extreme electrocatalysts compositions as follows: PtRuSn (80:20:0) for methanol, PtRuSn (50:0:50) for ethanol and PtRuSn (20:70:10) for 2-propanol. (author)

Challenges in bimetallic multilayer structure formation: Pt growth on Cu monolayers on Ru(0001)

DEFF Research Database (Denmark)

Mancera, Luis A.; Engstfeld, Albert Kilian; Bensch, Andreas

2017-01-01

In a joint experimental and theoretical study, we investigated the formation and morphology of PtCu/Ru(0001) bimetallic surfaces grown at room and higher temperatures under UHV conditions. We obtained the PtCu/Ru(0001) surfaces by deposition of Pt atoms on a previously created Cu/Ru(0001) structure...... which includes only one Cu monolayer. Bimetallic surfaces prepared at different Pt coverages are investigated using STM imaging, revealing the existence of reconstruction lines and Cu islands. Although primarily created Cu islands continue growing in size by increasing Pt coverage, a continuous...

Tropanol esters of metallocene carboxylic acids. Syntheses, labelling with 103Ru and sup(103m)Rh and organ distribution

International Nuclear Information System (INIS)

Wenzel, M.; Wu, Y.

1988-01-01

The tropanol esters of the carboxylic acids of ferrocene, 103 Ru-ruthenocene and sup(103m)Rh-rhodocinium were synthezised. The organ distribution of the 103 Ru or sup(103m)Rh labelled tropanol-esters were investigated. Only the 103 Ru labelled ester showed a high heart/blood ratio. (author)

Sol-Gel Process for Making Pt-Ru Fuel-Cell Catalysts

Science.gov (United States)

Narayanan, Sekharipuram; Valdez, Thomas; Kumta, Prashant; Kim, Y.

2005-01-01

A sol-gel process has been developed as a superior alternative to a prior process for making platinum-ruthenium alloy catalysts for electro-oxidation of methanol in fuel cells. The starting materials in the prior process are chloride salts of platinum and ruthenium. The process involves multiple steps, is time-consuming, and yields a Pt-Ru product that has relatively low specific surface area and contains some chloride residue. Low specific surface area translates to incomplete utilization of the catalytic activity that might otherwise be available, while chloride residue further reduces catalytic activity ("poisons" the catalyst). In contrast, the sol-gel process involves fewer steps and less time, does not leave chloride residue, and yields a product of greater specific area and, hence, greater catalytic activity. In this sol-gel process (see figure), the starting materials are platinum(II) acetylacetonate [Pt(C5H7O2)2, also denoted Pt-acac] and ruthenium(III) acetylacetonate [Ru(C5H7O2)3, also denoted Ru-acac]. First, Pt-acac and Ru-acac are dissolved in acetone at the desired concentrations (typically, 0.00338 moles of each salt per 100 mL of acetone) at a temperature of 50 C. A solution of 25 percent tetramethylammonium hydroxide [(CH3)4NOH, also denoted TMAH] in methanol is added to the Pt-acac/Ruacac/ acetone solution to act as a high-molecular-weight hydrolyzing agent. The addition of the TMAH counteracts the undesired tendency of Pt-acac and Ru-acac to precipitate as separate phases during the subsequent evaporation of the solvent, thereby helping to yield a desired homogeneous amorphous gel. The solution is stirred for 10 minutes, then the solvent is evaporated until the solution becomes viscous, eventually transforming into a gel. The viscous gel is dried in air at a temperature of 170 C for about 10 hours. The dried gel is crushed to make a powder that is the immediate precursor of the final catalytic product. The precursor powder is converted to the

Evaluation of Pt-Ru-Ni and Pt-Sn-Ni catalysts as anodes in direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Ribadeneira, Esteban; Hoyos, Bibian A. [Escuela de Procesos y Energia, Facultad de Minas, Universidad Nacional de Colombia, Medellin (Colombia)

2008-05-15

In this study, the electrooxidation of ethanol on carbon supported Pt-Ru-Ni and Pt-Sn-Ni catalysts is electrochemically studied through cyclic voltammetry at 50 C in direct ethanol fuel cells. All electrocatalysts are prepared using the ethylene glycol-reduction process and are chemically characterized by energy-dispersive X-ray analysis (EDX). For fuel cell evaluation, electrodes are prepared by the transfer-decal method. Nickel addition to the anode improves DEFC performance. When Pt{sub 75}Ru{sub 15}Ni{sub 10}/C is used as an anode catalyst, the current density obtained in the fuel cell is greater than that of all other investigated catalysts. Tri-metallic catalytic mixtures have a higher performance relative to bi-metallic catalysts. These results are in agreement with CV results that display greater activity for PtRuNi at higher potentials. (author)

Soft landing of bare PtRu nanoparticles for electrochemical reduction of oxygen.

Science.gov (United States)

Johnson, Grant E; Colby, Robert; Engelhard, Mark; Moon, Daewon; Laskin, Julia

2015-08-07

Magnetron sputtering of two independent Pt and Ru targets coupled with inert gas aggregation in a modified commercial source has been combined with soft landing of mass-selected ions to prepare bare 4.5 nm diameter PtRu nanoparticles on glassy carbon electrodes with controlled size and morphology for electrochemical reduction of oxygen in solution. Employing atomic force microscopy (AFM) it is shown that the nanoparticles bind randomly to the glassy carbon electrode at a relatively low coverage of 7 × 10(4) ions μm(-2) and that their average height is centered at 4.5 nm. Scanning transmission electron microscopy images obtained in the high-angle annular dark field mode (HAADF-STEM) further confirm that the soft-landed PtRu nanoparticles are uniform in size. Wide-area scans of the electrodes using X-ray photoelectron spectroscopy (XPS) reveal the presence of both Pt and Ru in atomic concentrations of ∼9% and ∼33%, respectively. Deconvolution of the high energy resolution XPS spectra in the Pt 4f and Ru 3d regions indicates the presence of both oxidized Pt and Ru. The substantially higher loading of Ru compared to Pt and enrichment of Pt at the surface of the nanoparticles is confirmed by wide-area analysis of the electrodes using time-of-flight medium energy ion scattering (TOF-MEIS) employing both 80 keV He(+) and O(+) ions. The activity of electrodes containing 7 × 10(4) ions μm(-2) of bare 4.5 nm PtRu nanoparticles toward the electrochemical reduction of oxygen was evaluated employing cyclic voltammetry (CV) in 0.1 M HClO4 and 0.5 M H2SO4 solutions. In both electrolytes a pronounced reduction peak was observed during O2 purging of the solution that was not evident during purging with Ar. Repeated electrochemical cycling of the electrodes revealed little evolution in the shape or position of the voltammograms indicating high stability of the nanoparticles supported on glassy carbon. The reproducibility of the nanoparticle synthesis and deposition was

Electrocatalytic properties of carbon-supported Pt-Ru catalysts with the high alloying degree for formic acid electrooxidation

Energy Technology Data Exchange (ETDEWEB)

Chen, Yu.; Zhou, Yiming; Tang, Yawen; Lu, Tianhong [College of Chemistry and Environmental Science, Nanjing Normal University, Nanjing 210097 (China)

2010-07-01

A series of carbon-supported bimetallic Pt-Ru catalysts with high alloying degree and different Pt/Ru atomic ratio have been prepared by a chemical reduction method in the H{sub 2}O/ethanol/tetrahydrofuran (THF) mixture solvent. The structural and electronic properties of catalysts are characterized using X-ray reflection (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM). The electrooxidation of formic acid on these Pt-Ru nanoparticles are investigated by using cyclic voltammetry, chronoamperometry and CO-stripping measurements. The results of electrochemical measurements illustrate that the alloying degree and Pt/Ru atomic ratio of Pt-Ru catalyst play an important role in the electrocatalytic activity of the Pt-Ru/C catalyst for formic acid electrooxidation due to the bifunctional mechanism and the electronic effect. Since formic acid is an intermediate in the methanol electrooxidation on Pt electrode in acidic electrolyte, the observation provides an additional fundamental understanding of the structure-activity relationship of Pt-Ru catalyst for methanol electrooxidation. (author)

Co-catalytic effect of nickel in Pt-Ru/C and Pt-Sn/C electrocatalysts for ethanol electrooxidation

OpenAIRE

Ribadeneira, R. E.; Hoyos, B. A.

2010-01-01

In the present study, we examined the effect of adding nickel to Pt-Ru and Pt-Sn catalysts for ethanol electrooxidation. The alcohol-reduction process with ethylene glycol was used to prepare ten electrocatalysts. These were microchemically and physically characterized by EDX and XRD analysis. The electrocatalysts were evaluated at mini-electrodes with cyclic voltammetry at 25 and 50 °C in sulfuric acid and ethanol solutions, and as anodes in fuel cell tests. Nickel addition to Pt-Ru mixtures...

Metal-metal bonding and aromaticity in [M2(NHCHNH)3]2 (μ-E)2 (E = O, S; M = Nb, Mo, Tc, Ru, Rh).

Science.gov (United States)

Yan, Xiuli; Meng, Lingpeng; Sun, Zheng; Li, Xiaoyan

2016-02-01

The nature of M-M bonding and aromaticity of [M2(NHCHNH)3]2(μ-E)2 (E = O, S; M = Nb, Mo, Tc, Ru, Rh) was investigated using atoms in molecules (AIM) theory, electron localization function (ELF), natural bond orbital (NBO) and molecular orbital analysis. These analyses led to the following main conclusions: in [M2(NHCHNH)3]2(μ-E)2 (E = O, S; M = Nb, Mo, Tc, Ru, Rh), the Nb-Nb, Ru-Ru, and Rh-Rh bonds belong to "metallic" bonds, whereas Mo-Mo and Tc-Tc drifted toward the "dative" side; all these bonds are partially covalent in character. The Nb-Nb, Mo-Mo, and Tc-Tc bonds are stronger than Ru-Ru and Rh-Rh bonds. The M-M bonds in [M2(NHCHNH)3]2(μ-S)2 are stronger than those in [M2(NHCHNH)3]2(μ-O)2 for M = Nb, Mo, Tc, and Ru. The NICS(1)ZZ values show that all of the studied molecules, except [Ru2(NHCHNH)3]2(μ-O)2, are aromaticity molecules. O-bridged compounds have more aromaticity than S-bridged compounds. Graphical Abstract Left Molecular graph, and right electron localization function (ELF) isosurface of [M2(NHCHNH)3]2(μ-E)2(E = O, S; M = Nb, Mo, Tc, Ru, Rh).

Synthesis and Electrocatalytic Performance of Multi-Component Nanoporous PtRuCuW Alloy for Direct Methanol Fuel Cells

Directory of Open Access Journals (Sweden)

Xiaoting Chen

2015-06-01

Full Text Available We have prepared a multi-component nanoporous PtRuCuW (np-PtRuCuW electrocatalyst via a combined chemical dealloying and mechanical alloying process. The X-ray diffraction (XRD, transmission electron microscopy (TEM and electrochemical measurements have been applied to characterize the microstructure and electrocatalytic activities of the np-PtRuCuW. The np-PtRuCuW catalyst has a unique three-dimensional bi-continuous ligament structure and the length scale is 2.0 ± 0.3 nm. The np-PtRuCuW catalyst shows a relatively high level of activity normalized to mass (467.1 mA mgPt−1 and electrochemically active surface area (1.8 mA cm−2 compared to the state-of-the-art commercial PtC and PtRu catalyst at anode. Although the CO stripping peak of np-PtRuCuW 0.47 V (vs. saturated calomel electrode, SCE is more positive than PtRu, there is a 200 mV negative shift compared to PtC (0.67 V vs. SCE. In addition, the half-wave potential and specific activity towards oxygen reduction of np-PtRuCuW are 0.877 V (vs. reversible hydrogen electrode, RHE and 0.26 mA cm−2, indicating a great enhancement towards oxygen reduction than the commercial PtC.

High-temperature electrochemical characterization of Ru core Pt shell fuel cell catalyst

Energy Technology Data Exchange (ETDEWEB)

Bokach, D.; Fuente, J.L.G. de la; Tsypkin, M.; Ochal, P.; Tunold, R.; Sunde, S.; Seland, F. [Department of Materials Science and Engineering, Norwegian University of Science and Technology (NTNU), Sem Saelands veg 12, N-7491 Trondheim (Norway); Endsjoe, I.C. [Washington Mills AS, NO-7300 Orkanger (Norway)

2011-12-15

The electrooxidation of methanol was studied at elevated temperature and pressure by cyclic voltammetry and constant potential experiments at real fuel cell electrocatalysts. Ruthenium core and platinum shell nanoparticles were synthesized by a sequential polyol route, and characterized electrochemically by CO stripping at room temperature to quickly confirm the structure of the synthesized core-shell structure as compared to pure commercial Pt/C and Pt-Ru/C alloy catalysts. A significant promotional effect of Pt decorated Ru cores in the methanol oxidation was found at elevated temperatures and rather high-electrode potentials. A negative potential shift of the methanol oxidation peak is observed for the Ru rate at Pt/C core-shell catalyst at moderate temperatures, while a significant shift to positive potentials of the methanol oxidation peak occurs for Pt/C catalysts. The onset potential for methanol oxidation is lowered some 200 mV from room temperature and up to 120 C for all electrocatalysts, indicating that it is the thermal activity of water adsorption that dictates the onset potential. Direct methanol fuel cell experiments showed only small performance differences between Ru rate at Pt/C and Pt/C anode electrocatalysts, suggesting the necessity of render possible the formation of surface oxygen species at lower electrode potentials. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Synthesis and characterization of PtRuMo/C nanoparticle electrocatalyst for direct ethanol fuel cell

Energy Technology Data Exchange (ETDEWEB)

Wang, Zhen-Bo; Yin, Ge-Ping [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Lin, Yong-Ge [Department of Chemistry, University of Puerto Rico, Rio Piedras Campus, San Juan, PR 00931 (United States)

2007-07-10

This research aims at enhancement of the performance of anodic catalysts for the direct ethanol fuel cell (DEFC). Two distinct DEFC nanoparticle electrocatalysts, PtRuMo/C and PtRu/C, were prepared and characterized, and one glassy carbon working electrode for each was employed to evaluate the catalytic performance. The cyclic-voltammetric, chronoamperometric, and amperometric current-time measurements were done in the solution 0.5 mol L{sup -1} CH{sub 3}CH{sub 2}OH and 0.5 mol L{sup -1} H{sub 2}SO{sub 4}. The composition, particle sizes, lattice parameters, morphology, and the oxidation states of the metals on nanoparticle catalyst surfaces were determined by energy dispersive analysis of X-ray (EDAX), X-ray diffraction (XRD), transmission electron micrographs (TEM) and X-ray photoelectron spectrometer (XPS), respectively. The results of XRD analysis showed that both PtRuMo/C and PtRu/C had a face-centered cubic (fcc) structure with smaller lattice parameters than that of pure platinum. The typical particle sizes were only about 2.5 nm. Both electrodes showed essentially the same onset potential as shown in the CV for ethanol electrooxidation. Despite their comparable active specific areas, PtRuMo/C was superior to PtRu/C in respect of the catalytic activity, durability and CO-tolerance. The effect of Mo in the PtRuMo/C nanoparticle catalyst was illustrated with a bifunctional mechanism, hydrogen-spillover effect and the modification on the Pt electronic states. (author)

Measurement of the Ru surface content of electrodeposited PtRu electrodes with the electrochemical quartz crystal microbalance: implications for methanol and CO electrooxidation

NARCIS (Netherlands)

Frelink, T.; Visscher, W.; Veen, van J.A.R.

1996-01-01

To obtain the surface content of Ru in rough electrocodeposited PtRu electrodes, the mass change of a Pt electrode during Ru deposition was measured with the electrochemical quartz crystal microbalance (EQCMB). It is shown that there is a correlation between the potential of the surface oxide

Electrocatalytic oxidation of methanol on (Pb) lead modified by Pt, Pt-Ru and Pt-Sn microparticles dispersed into poly(o-phenylenediamine) film

Energy Technology Data Exchange (ETDEWEB)

Golikand, Ahmad Nozad; Maragheh, Mohammad Ghannadi; Irannejad, Leila [Jaber Ibn Hayan Research Lab., Atomic Energy Organization of Iran (AEOI), Tehran (Iran); Golabi, Seyed Mehdi [Electroanalytical Chemistry Lab., Faculty of Chemistry, University of Tabriz, Tabriz (Iran)

2005-08-18

The electrocatalytic oxidation of methanol at a (Pb) lead electrode modified by Pt, Pt-Ru and Pt-Sn microparticles dispersed into poly(o-phenylenediamine) (PoPD) film has been investigated using cyclic voltammetry as analytical technique and 0.5M sulfuric acid as supporting electrolyte. It has been shown that the presence of PoPD film increases considerably the efficiency of deposited Pt and Pt alloys microparticles toward the electrocatalytic oxidation of methanol. The catalytic activity of Pt particles is further enhanced when Ru and especially Sn, is co-deposited in the polymer film. The effects of various parameters such as concentration of methanol, medium temperature as well as the long term stability of modified electrodes have also been investigated. (author)

Diethyl Ether Production during Catalytic Dehydration of Ethanol over Ru- and Pt- modified H-beta Zeolite Catalysts.

Science.gov (United States)

Kamsuwan, Tanutporn; Praserthdam, Piyasan; Jongsomjit, Bunjerd

2017-01-01

In the present study, the catalytic dehydration of ethanol over H-beta zeolite (HBZ) catalyst with ruthenium (Ru-HBZ) and platinum (Pt-HBZ) modification was investigated. Upon the reaction temperature between 200 and 400°C, it revealed that ethanol conversion and ethylene selectivity increased with increasing temperature for both Ru and Pt modification. At lower temperature (200 to 250°C), diethyl ether (DEE) was the major product. It was found that Ru and Pt modification on HBZ catalyst can result in increased DEE yield at low reaction temperature due to increased ethanol conversion without a significant change in DEE selectivity. By comparing the DEE yield of all catalysts in this study, the Ru-HBZ catalyst apparently exhibited the highest DEE yield (ca. 47%) at 250°C. However, at temperature from 350 to 400°C, the effect of Ru and Pt was less pronounced on ethylene yield. With various characterization techniques, the effects of Ru and Pt modification on HBZ catalyst were elucidated. It revealed that Ru and Pt were present in the highly dispersed forms and well distributed in the catalyst granules. It appeared that the weak acid sites measured by NH 3 temperature-programmed desorption technique also decreased with Ru and Pt promotion. Thus, the increased DEE yields with the Ru and Pt modification can be attributed to the presence of optimal weak acid sites leading to increased intrinsic activity of the catalysts. It can be concluded that the modification of Ru and Pt on HBZ catalyst can improve the DEE yields by ca. 10%.

Improvement on electrochemical performance by partial replacement of Ru@Pt core-shell nanocatalyst by temperature modification

International Nuclear Information System (INIS)

Chang, Chih-Juei; Lin, Liang-You; Tseng, Fan-Gang

2014-01-01

In this paper, the homemade open-loop reduction system (OLRS), and redox transmetalation method were utilized to produce the core-shell Ru (ruthenium)/Pt (platinum) catalysts on the carbon cloth (CC) for direct methanol fuel cell (DMFC) application. By adjusting pH value and heating to proper temperature of the ionized reduction environment, Pt 4+ can be first converted into Pt 2+ to allow partial Ru replacement with Pt by redox transmetalation and produce Ru@Pt core-shell nanostructures[1]. And we change the reduction temperature to see how it affects the efficiency of the DMFC. The scanning electron microscopic (SEM) top-view micrographs showing that the apparent Ru@Pt nanoparticles successfully deposited on both the inner and outer surfaces of the hydrophilically-treated CC. At high SEM magnification, the small size and high-density distribution of the Ru@Pt nanoparticles were clearly observed on the hydrophilically-treated CC, and much more Pt@Ru catalyst deposit on the CC surface with the sample of 80 °C. The electrosorption charges of hydrogen ion (Q H ) and the peak current density (I P ) of the samples in the cyclic voltammetry (CV) curves. The magnitude of peak current density is positive correlation to the temperature. However, the CO tolerance, indicated that the better CO tolerance contributed to the less Pt replace on Ru cluster, which allow the Ru oxidizing CO to CO 2 efficiently, is negative correlation-- to the temperature. The sample of 50 °C shows the better combination catalyst efficiency between the CO tolerance and the electrochemical performance

PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells.

Science.gov (United States)

Cui, Zhiming; Li, Chang Ming; Jiang, San Ping

2011-09-28

A simple self-assembly approach has been developed to functionalize carbon nanotubes (CNTs) with chitosan (CS) and heteropolyacids (HPAs) of phosphomolybdic acid (H(3)PMo(12)O(40), HPMo) and phosphotungstic acid (H(3)PW(12)O(40), HPW). The non-covalent functionalization method, which introduces homogenous surface functional groups with no detrimental effect on graphene structures of CNTs, can be carried out at room temperature without the use of corrosive acids. The PtRu nanoparticles supported on HPAs-CS-CNTs have a uniform distribution and much smaller size as compared to those of the PtRu nanoparticles supported on conventional acid treated CNTs (PtRu/AO-CNTs). The onset and peak potentials for CO(ad) oxidation on PtRu/HPAs-CS-CNTs catalysts are more negative than those on PtRu/AO-CNTs, indicating that HPAs facilitate the electro-oxidation of CO. The PtRu/HPMo-CS-CNTs catalyst has a higher electrocatalytic activity for methanol oxidation and higher tolerance toward CO poisoning than PtRu/HPW-CS-CNTs. The better electrocatalytic enhancement of HPMo on the PtRu/HPAs-CS-CNTs catalyst is most likely related to the fact that molybdenum-containing HPAs such as HPMo have more labile terminal oxygen to provide additional active oxygen sites while accelerating the CO and methanol oxidation in a similar way to that of Ru in the PtRu binary alloy system.

Investigation of ethanol electrooxidation on a Pt-Ru-Ni/C catalyst for a direct ethanol fuel cell

Energy Technology Data Exchange (ETDEWEB)

Wang, Zhen-Bo; Yin, Ge-Ping; Zhang, Jian; Sun, Ying-Chao; Shi, Peng-Fei [Department of Applied Chemistry, Harbin Institute of Technology, Harbin (China 150001)

2006-09-29

This research is aimed to improve the utilization and activity of anodic alloy catalysts and thus to lower the contents of noble metals and the catalyst loading on anodes for ethanol electrooxidation. The DEFC anodic catalysts, Pt-Ru-Ni/C and Pt-Ru/C, were prepared by a chemical reduction method. Their performances were tested by using a glassy carbon working electrode and cyclic voltammetric curves, chronoamperometric curves and half cell measurement in a solution of 0.5molL{sup -1} CH{sub 3}CH{sub 2}OH and 0.5molL{sup -1} H{sub 2}SO{sub 4}. The composition of the Pt-Ru-Ni and Pt-Ru surface particles were determined by EDAX analysis. The particle size and lattice parameter of the catalysts were determined by means of X-ray diffraction (XRD). XRD analysis showed that both of the catalysts exhibited face centered cubic structures and had smaller lattice parameters than a Pt-alone catalyst. Their particle sizes were small, about 4.5nm. No significant differences in the ethanol electrooxidation on both electrodes were found using cyclic voltammetry, especially regarding the onset potential for ethanol electrooxidation. The electrochemically active specific areas of the Pt-Ru-Ni/C and Pt-Ru/C catalysts were almost the same. But, the catalytic activity of the Pt-Ru-Ni/C catalyst was higher for ethanol electrooxidation than that of the Pt-Ru/C catalyst. Their tolerance to CO formed as one of the intermediates of ethanol electrooxidation, was better than that of the Pt-Ru/C catalyst. (author)

Synthesis and characterization of PtRu/C catalysts obtained by colloidal and deposition methods for fuel cell applications

Directory of Open Access Journals (Sweden)

Egberto Gomes Franco

2005-06-01

Full Text Available The purpose of this investigation was to compare catalysts produced by the Bönnemann - colloidal method (PtRu (B1 and PtRu (B2, and those produced by the spontaneous deposition method (PtRu (SD. The catalysts produced by both methods had good electrochemical behavior for methanol oxidation for proton exchange membrane fuel cell applications. The structure of the catalyst was examined by transmission electron microscopy (TEM. Energy dispersive spectroscopic analysis (EDS was used to determine the semi-quantitative composition of the catalysts, and the electrochemical behavior was determined by cyclic voltammetry (CV. The diffractograms of the binary catalysts revealed platinum and ruthenium as the only crystalline phases, as per ICDD data base. The PtRu (B1 catalyst, treated in a reducing atmosphere, has the same structure as PtRu (B2, treated in an oxidising/reducing atmosphere, except that the crystallite size was around 1.7 nm for PtRu (B1 instead of 9.9 nm for PtRu (B2. The catalysts PtRu (B2 and PtRu (SD showed similar cyclic voltammetric behavior, which was better than that of PtRu (B1. Both methods are suitable for the production of electrocatalysts for fuel cell applications. The colloidal method is more expensive than the deposition method, but the former permits the production of ternary and quaternary catalyst systems with enhanced CO tolerance.

Preparation of Pt Ru/C + rare earths by the method of reduction by alcohol for the electro-oxidation of ethanol

International Nuclear Information System (INIS)

Tusi, M.M.; Rodrigues, R.M.S.; Spinace, E.V.; Oliveira Neto, A.

2010-01-01

PtRu/C electrocatalyst was prepared in a single step, while that PtRu/85%C-15%Ce, PtRu/85%C-15%La, PtRu/85%C-15%Nd and PtRu/85%C-15%Er electrocatalyst were prepared in a two step. In the first step a Carbon Vulcan XC72 + rare earth supports were prepared. In the second step PtRu electrocatalyst were prepared by an alcohol-reduction process using ethylene glycol as solvent and reducing agent and supported on Vulcan XC72 + earth rare. The obtained electrocatalysts were characterized by EDAX, XRD and chronoamperometry. The electro-oxidation of ethanol was studied by chronoamperometry at room temperature. PtRu/85%C- 15%Ce electrocatalyst showed a significant increase of performance for ethanol oxidation compared to PtRu/C electrocatalyst. (author)

Mixed phase Pt-Ru catalyst for direct methanol fuel cell anode by flame aerosol synthesis

DEFF Research Database (Denmark)

Chakraborty, Debasish; Bischoff, H.; Chorkendorff, Ib

2005-01-01

A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst wa......Ru1/Vulcan carbon. The kinetics of methanol oxidation on the mixed phase catalyst was also explored by electrochemical impedance spectroscopy. (c) 2005 The Electrochemical Society.......A spray-flame aerosol catalyzation technique was studied for producing Pt-Ru anode electrodes for the direct methanol fuel cell. Catalysts were produced as aerosol nanoparticles in a spray-flame reactor and deposited directly as a thin layer on the gas diffusion layer. The as-prepared catalyst...... was found to be a mixture of nanocrystalline, mostly unalloyed Pt and an amorphous phase mostly of Ru and to a lesser extent of Pt oxides on top of the crystalline phase. The flame-produced Pt1Ru1 demonstrated similar onset potential but similar to 60% higher activity compared to commercially available Pt1...

Highly effective and CO-tolerant PtRu electrocatalysts supported on poly(ethyleneimine) functionalized carbon nanotubes for direct methanol fuel cells

International Nuclear Information System (INIS)

Cheng, Yi; Jiang, San Ping

2013-01-01

A highly efficient and CO tolerant PtRu electrocatalysts supported on amino-rich, cationic poly(ethyleneimine) polyelectrolyte functionalized multi-walled carbon nanotubes (PtRu/PEI-MWCNTs) has been developed. The catalysts were characterized by thermogravimetric analysis, Raman spectroscopy, cyclic voltammograms, CO stripping, chronoamperometry, transmission electron microscopy (TEM) and X-ray diffraction (XRD). The PtRu particles with average size ∼2.5 nm are well dispersed on PEI-MWCNTs. The peak current for the methanol oxidation reaction on 40% PtRu/PEI-MWCNTs is 636mAmg Pt −1 , 5.7 times higher than 112mA mg Pt −1 measured on the 40% PtRu supported on acid treated MWCNTs (PtRu/AO-MWCNTs) under identical conditions. PtRu/PEI-MWCNTs catalysts exhibit a superior electrocatalytic activity and stability for the methanol oxidation reaction due to its high tolerance toward CO poisoning as compared with PtRu/AO-MWCNTs for direct methanol fuel cells

Characterization and evaluation of Pt-Ru catalyst supported on multi-walled carbon nanotubes by electrochemical impedance

Energy Technology Data Exchange (ETDEWEB)

Ocampo, A.L.; Miranda-Hernandez, M.; Sebastian, P.J. [Centro de Investigacion en Energia-UNAM, Temixco, 62580 Morelos (Mexico); Morgado, J.; Montoya, J.A. [IMP, Eje Central Lazaro Cardenas 152, 07730 D.F. Mexico (Mexico)

2006-10-06

In this work the authors present the results of a systematic characterization and evaluation of the carbon nanotube supported Pt-Ru (Pt-Ru/CNT) for its use as methanol oxidation catalyst. Its activity was compared with that of Pt and Pt-Ru catalysts supported on Vulcan and synthesized from carbonyl precursors, and another commercial Pt-Ru catalyst. The cyclic voltammetry, CO stripping and electrochemical impedance techniques were employed to determine the electrocatalytic activity of the catalysts. The electrochemical studies were performed in 0.5M H{sub 2}SO{sub 4} containing different concentrations of methanol (0.05-1M). The results showed a noticeable influence of the catalyst support (CNT) on the performance of the catalyst for CO oxidation. The electrochemical impedance studies allowed us to separate the different steps in the methanol oxidation reaction and to control these steps or reactions by varying the applied potential and the methanol concentration. At low methanol concentration and potentials the de-hydrogenation of methanol predominated. But, at high potential and methanol concentrations, the CO oxidation predominated. These results allowed us to clearly describe at what potential and concentration ranges the bi-functional effect of Ru becomes evident. Our results indicated that the CO oxidation occurs both on Pt and Ru. Compared to other catalysts, Pt-Ru supported on carbon nanotubes showed superior catalytic activity for CO and methanol oxidation. (author)

Derivation of the liquidus surface projection for the Al-Pt-Ru system from as-cast samples

CSIR Research Space (South Africa)

Prins, SN

2005-11-10

Full Text Available -rich corner. Two new ternary phases similar to Ru12Pt15Al73 and similar to Ru18Pt28Al64 were observed near the Al-corner. The similarity to Ru12Pt15Al73 phase has a primitive cubic structure, lattice parameter of similar to 0.7721 nm, and is stable to room...

Electronic Structure of the fcc Transition Metals Ir, Rh, Pt, and Pd

DEFF Research Database (Denmark)

Andersen, O. Krogh

1970-01-01

We give a complete description of a relativistic augmented-plane-wave calculation of the band structures of the paramagnetic fcc transition metals Ir, Rh, Pt, and Pd. The width and position of the d band decrease in the sequence Ir, Pt, Rh, Pd; and N(EF)=13.8,23.2,18.7, and 32.7 (states/atom)/Ry,......We give a complete description of a relativistic augmented-plane-wave calculation of the band structures of the paramagnetic fcc transition metals Ir, Rh, Pt, and Pd. The width and position of the d band decrease in the sequence Ir, Pt, Rh, Pd; and N(EF)=13.8,23.2,18.7, and 32.7 (states....../atom)/Ry, respectively. Spin-orbit coupling is important for all four metals and the coupling parameter varies by 30% over the d bandwidth. Detailed comparisons with de Haas—van Alphen Fermi-surface dimensions have previously been presented and the agreement was very good. Comparison with measured electronic specific...

Electrooxidation of ethanol on Pt and PtRu surfaces investigated by ATR surface-enhanced infrared absorption spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Silva, Marcio F.; Camara, Giuseppe A., E-mail: giuseppe.silva@ufms.br [Departamento de Quimica, Universidade Federal do Mato Grosso do Sul, Campo Grande-MS (Brazil); Batista, Bruno C.; Boscheto, Emerson [Instituto de Quimica de Sao Carlos, Universidade de Sao Paulo, Sao Carlos-SP, (Brazil); Varela, Hamilton, E-mail: varela@iqsc.usp.br [Ertl Center for Electrochemistry and Catalysis, Gwangju Institute of Science and Technology (GIST), Gwangju (Korea, Republic of)

2012-05-15

Herein, it was investigated for the first time the electro-oxidation of ethanol on Pt and PtRu electrodeposits in acidic media by using in situ surface enhanced infrared absorption spectroscopy with attenuated total reflection (ATR-SEIRAS). The experimental setup circumvents the weak absorbance signals related to adsorbed species, usually observed for rough, electrodeposited surfaces, and allows a full description of the CO coverage with the potential for both catalysts. The dynamics of adsorption-oxidation of CO was accessed by ATR-SEIRAS experiments (involving four ethanol concentrations) and correlated with expressions derived from a simple kinetic model. Kinetic analysis suggests that the growing of the CO adsorbed layer is nor influenced by the presence of Ru neither by the concentration of ethanol. The results suggest that the C-C scission is not related to the presence of Ru and probably happens at Pt sites. (author)

Electrooxidations of ethanol, acetaldehyde and acetic acid using PtRuSn/C catalysts prepared by modified alcohol-reduction process

Energy Technology Data Exchange (ETDEWEB)

Wu, Gang [Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208 (United States); Swaidan, Raja [Department of Chemical Engineering, Cooper Union, New York, NY 10003 (United States); Cui, Guofeng [School of Chemistry and Chemical Engineering, Sun-Yat Sen University, Guangzhou 510275 (China)

2007-10-11

Well-dispersed ternary PtRuSn catalysts of various atomic ratios (60:30:10, 60:20:20 and 60:10:30) were deposited onto carbon using modified alcohol-reduction process for electrochemical oxidation of ethanol. The alloy phase structure and surface morphology for each variation of the PtRuSn/C catalysts were determined by XRD and HRTEM. In order to evaluate the contributions of Ru and Sn in the different stages of ethanol oxidation, electrochemical oxidations of adsorbed CO, ethanol, acetaldehyde and acetic acid were performed on each PtRuSn/C catalyst. The results indicated that the Ru-rich PtRuSn/C catalyst (60:30:10) exhibited the lowest onset potential for the electrooxidations of adsorbed CO, ethanol and acetaldehyde, revealing that the removal through oxidation of the intermediate C{sub 1} and C{sub 2} species from Pt sites is primarily attributed to the Ru and Pt{sub 3}Sn alloy structures. However, for the overall oxidation of ethanol, the Sn-rich PtRuSn/C catalyst (60:10:30) containing PtSn phase and SnO{sub 2} structure is favorable for the activation of C-C bond breaking, thereby generating higher current density (mass activity) at higher potentials. Moreover, in the electrooxidation of acetic acid, a remarkable improvement for oxidizing acetic acid to C{sub 1} species was observed in the Sn-rich PtRuSn/C catalyst (60:10:30), while the Ru-rich PtRuSn/C catalyst (60:30:10) was almost incapable of breaking the C-C bond to further oxidize acetic acid. The possible reasons for the different reactivities on the studied PtRuSn/C catalysts were discussed based on the removal of intermediates and activation of the C-C bonds on the different surfaces. (author)

Low Pt content Pt-Ru-Ir-Sn quaternary catalysts for anodic methanol oxidation in DMFC

Energy Technology Data Exchange (ETDEWEB)

Neburchilov, Vladimir; Wang, Haijiang; Zhang, Jiujun [Institute for Fuel Cell Innovation, National Research Council (Canada)

2007-07-15

In this communication we report our research work on low Pt content Pt-Ru-Ir-Sn quaternary catalysts for use in DMFC anodes. The carbon-supported quaternary metal alloy catalyst was synthesized according to the solution reduction method and was deposited onto a carbon fiber paper or a carbon aerogel nanofoam to form the anode for direct methanol fuel cells. The Pt loading of the electrode is 0.1 mg/cm{sup 2}. The testing results from a three-electrode electrochemical cell show that the simultaneous use of higher Ir (25-35 wt.%) and Sn (10 wt.%) content gives satisfactory stability and higher activity for methanol oxidation than the commercially available E-TEK anode (80%[0.5Pt 0.5Ru]/C on carbon cloth). Energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), scanning electron microscope (SEM), and Bruner-Emmett-Teller method (BET) measurements were carried out to characterize the composition, structure, morphology, and surface area of the developed catalysts. (author)

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.

Separation of [Rh-103m]-rhodocene-derivatives from the parent [103Ru]ruthenocen-derivatives and their organ distribution

International Nuclear Information System (INIS)

Wenzel, M.; Wu, Y.

1987-01-01

The radioactive decay of [ 103 Ru]ruthenocene derivatives leads to sup(103m)Rh labelled rhodocinium derivatives, which can be separated by the extraction of a lipophilic solution of the ruthenocen derivate with water. The separation factor sup(103m)Rh/ 103 Ru reaches values of 32:1 Rh 3+ ions are not liberated and extracted. The organ distribution of the sup(103m)Rh labelled rhodocinium derivatives gained from ruthenocene and from N-isopropyl-ruthenocene amphetamine is different from the distribution of the parent ruthenocene compound. The liver and kidney uptake of the rhodocinium-amphetamine is much higher than the uptake with ruthenocene amphetamine. (author)

Carbon-Supported PtRuMo Electrocatalysts for Direct Alcohol Fuel Cells

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José L.G. Fierro

2013-10-01

Full Text Available The review article discusses the current status and recent findings of our investigations on the synthesis and characterization of carbon-supported PtRuMo electrocatalysts for direct alcohol fuel cells. In particular, the effect of the carbon support and the composition on the structure, stability and the activity of the PtRuMo nanoparticles for the electrooxidation of CO, methanol and ethanol have been studied. Different physicochemical techniques have been employed for the analysis of the catalysts structures: X-ray analytical methods (XRD, XPS, TXRF, thermogravimetry (TGA and transmission electron microscopy (TEM, as well as a number of electrochemical techniques like CO adsorption studies, current-time curves and cyclic voltammetry measurements. Furthermore, spectroscopic methods adapted to the electrochemical systems for in situ studies, such as Fourier transform infrared spectroscopy (FTIRS and differential electrochemical mass spectrometry (DEMS, have been used to evaluate the oxidation process of CO, methanol and ethanol over the carbon-supported PtRuMo electrocatalysts.

Effects of the Electrodeposition Time in the Synthesis of Carbon-Supported Pt(Cu and Pt-Ru(Cu Core-Shell Electrocatalysts for Polymer Electrolye Fuel Cells

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Griselda Caballero-Manrique

2016-08-01

Full Text Available Pt(Cu/C and Pt-Ru(Cu/C electrocatalysts with core-shell structure supported on Vulcan Carbon XC72R have been synthesized by potentiostatic deposition of Cu nanoparticles on the support, galvanic exchange with Pt and spontaneous deposition of Ru species. The duration of the electrodeposition time of the different species has been modified and the obtained electrocatalysts have been characterized using electrochemical and structural techniques. The High Resolution Transmission Electron Microscopy (HRTEM, Fast Fourier Transform (FFT and Energy Dispersive X-ray (EDX microanalyses allowed the determining of the effects of the electrodeposition time on the nanoparticle size and composition. The best conditions identified from Cyclic Voltammetry (CV corresponded to onset potentials for CO and methanol oxidation on Pt-Ru(Cu/C of 0.41 and 0.32 V vs. the Reversible Hydrogen Electrode (RHE, respectively, which were smaller by about 0.05 V than those determined for Ru-decorated commercial Pt/C. The CO oxidation peak potentials were about 0.1 V smaller when compared to commercial Pt/C and Pt-Ru/C. The positive effect of Cu was related to its electronic effect on the Pt shells and also to the generation of new active sites for CO oxidation. The synthesis conditions to obtain the best performance for CO and methanol oxidation on the core-shell Pt-Ru(Cu/C electrocatalysts were identified. When compared to previous results in literature for methanol, ethanol and formic acid oxidation on Pt(Cu/C catalysts, the present results suggest an additional positive effect of the deposited Ru species due to the introduction of the bifunctional mechanism for CO oxidation.

Ni2P Makes Application of the PtRu Catalyst Much Stronger in Direct Methanol Fuel Cells.

Science.gov (United States)

Chang, Jinfa; Feng, Ligang; Liu, Changpeng; Xing, Wei

2015-10-12

PtRu is regarded as the best catalyst for direct methanol fuel cells, but the performance decay resulting from the loss of Ru seriously hinders commercial applications. Herein, we demonstrated that the presence of Ni2 P largely reduces Ru loss, which thus makes the application of PtRu much stronger in direct methanol fuel cells. Outstanding catalytic activity and stability were observed by cyclic voltammetry. Upon integrating the catalyst material into a practical direct methanol fuel cell, the highest maximum power density was achieved on the PtRu-Ni2P/C catalyst among the reference catalysts at different temperatures. A maximum power density of 69.9 mW cm(-2) at 30 °C was obtained on PtRu-Ni2P/C, which is even higher than the power density of the state-of-the-art commercial PtRu catalyst at 70 °C (63.1 mW cm(-2)). Moreover, decay in the performance resulting from Ru loss was greatly reduced owing to the presence of Ni2 P, which is indicative of very promising applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fabrication and performance of the Pt-Ru/Ni-P/FTO counter electrode for dye-sensitized solar cells

International Nuclear Information System (INIS)

Ma, Huanmei; Tian, Jianhua; Bai, Shuming; Liu, Xiaodong; Shan, Zhongqiang

2014-01-01

Highlights: • Pt-Ru alloy acts as the catalyst of counter electrodes in dye-sensitized solar cell. • Ni-P/FTO (fluorine-doped SnO 2 ) substrate is prepared by electroless plating method. • Pt-Ru/Ni-P/FTO counter electrode is fabricated by electrodeposition method. • The Ni-P sublayer improves the conductivity and light reflectance of FTO substrate. • The cell with Pt-Ru/Ni-P/FTO counter electrode exhibits an improved efficiency. - Abstract: In this paper, Pt-Ru/Ni-P/FTO has been designed and fabricated as the counter electrode for dye-sensitized solar cells. The Pt-Ru catalytic layer and Ni-P alloy sublayer are prepared by traditional electrodeposition method and a simple electroless plating method, respectively, and the preparation conditions have been optimized. The scanning electron microscopy (SEM) images show that the Pt-Ru particles are evenly distributed on FTO and Ni-P/FTO substrate. By X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), it is confirmed that the Ni-P amorphous alloy has been formed, and no other compounds involved Ni and P have been formed. The electrochemical measurement results reveal that the Pt-Ru electrode has higher catalytic activity and stability towards tri-iodine reduction reaction than Pt electrode in the organic medium. The Ni-P sublayer deposited on FTO glasses increases the conductivity and light-reflection ability of the counter electrode, and this contributes to lowering the inner resistance of the cell and improving the light utilization efficiency. Through the photovoltaic test, it is confirmed that the energy conversion efficiency of a single DSSC with the optimized Pt-Ru/Ni-P/FTO counter electrode is increased by 29% compared with that of the cell based on the Pt/FTO counter electrode under the same conditions

In situ Ru K-edge EXAFS of CO adsorption on a Ru modified Pt/C fuel cell catalyst

International Nuclear Information System (INIS)

Rose, Abigail; Bilsborrow, Robert; King, Colin R.; Ravikumar, M.K.; Qian Yangdong; Wiltshire, Richard J.K.; Crabb, Eleanor M.; Russell, Andrea E.

2009-01-01

The Ru-CO bond of CO adsorbed on a Ru modified Pt/C fuel cell catalyst has been directly probed by in situ EXAFS at the Ru K-edge, providing evidence of a CO:metal surface atom ratio greater than 1:1 and that CO is adsorbed at bridging sites associated with Ru atoms at the surface of the catalyst nanoparticles. This result illustrates the limitations of single crystal models as representations of the bonding of adsorbed species at nanoparticle surfaces.

Radiolytic Synthesis of Pt-Ru Catalysts Based on Functional Polymer-Grafted MWNT and Their Catalytic Efficiency for CO and MeOH

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Dae-Soo Yang

2011-01-01

Full Text Available Pt-Ru catalysts based on functional polymer-grafted MWNT (Pt-Ru@FP-MWNT were prepared by radiolytic deposition of Pt-Ru nanoparticles on functional polymer-grafted multiwalled carbon nanotube (FP-MWNT. Three different types of functional polymers, poly(acrylic acid (PAAc, poly(methacrylic acid (PMAc, and poly(vinylphenyl boronic acid (PVPBAc, were grafted on the MWNT surface by radiation-induced graft polymerization (RIGP. Then, Pt-Ru nanoparticles were deposited onto the FP-MWNT supports by the reduction of metal ions using γ-irradiation to obtain Pt-Ru@FP-MWNT catalysts. The Pt-Ru@FP-MWNT catalysts were then characterized by XRD, XPS, TEM ,and elemental analysis. The catalytic efficiency of Pt-Ru@FP-MWNT catalyst was examined for CO stripping and MeOH oxidation for use in a direct methanol fuel cell (DMFC. The Pt-Ru@PVPBAc-MWNT catalyst shows enhanced activity for electro-oxidation of CO and MeOH oxidation over that of the commercial E-TEK catalyst.

Magnetic and structural characterizations on nanoparticles of FePt, FeRh and their composites

International Nuclear Information System (INIS)

Ko, Hnin Yu Yu; Suzuki, Takao; Nam, Nguyen T.; Phuoc, Nguyen N.; Cao Jiangwei; Hirotsu, Yoshihiko

2008-01-01

The various compositions of FePt and FeRh nanoparticles, and their composite particles have been fabricated by the solution-phase chemical method and their magnetic properties characterized. High-resolution transmission electron microscopic observations indicate that mono-dispersed FeRh and FePt/FeRh nanoparticles are fabricated with the average size of 3-5 nm. However, larger size particles are distributed in the annealed state. From X-ray diffraction results, the as-deposited FeRh nanoparticles reveal a chemically disordered fcc structure which can be transformed into CsCl-type structure through thermal annealing. Similarly, the annealed FePt nanoparticles show the L1 0 -phase fct structure although the fcc structure is apparent in the as-deposited state. It is also found that the first time in the exchange bias effect in the composite of ferromagnetic (FePt) and anti-ferromagnetic (FeRh) nanoparticles; result in a shift of the hysteresis loop after field cooling process

Energy barriers for interlayer diffusion in Pt/Pt(111) and Rh/Rh(111) homoepitaxy: small islands

Czech Academy of Sciences Publication Activity Database

Máca, František; Kotrla, Miroslav; Trushin, O. S.

1999-01-01

Roč. 49, č. 11 (1999), s. 1591-1596 ISSN 0011-4626. [Symposium on Surface Physics /8./. Třešť, 28.06.1999-02.07.1999] R&D Projects: GA MŠk OC P3.80 Institutional research plan: CEZ:AV0Z1010914 Keywords : molecular statics * energy barriers * Pt and Rh Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 0.328, year: 1999

Novel Pt-Ru nanoparticles formed by vapour deposition as efficient electrocatalyst for methanol oxidation

International Nuclear Information System (INIS)

Sivakumar, Pasupathi; Tricoli, Vincenzo

2006-01-01

The methods developed and described in paper-part I are employed to prepare nanometer size Pt-Ru particles on a Vulcan[reg] XC72R substrate with controlled metal loading. Transmission Electron Microscopy (TEM) confirmed uniform particles size (average diameter 2 nm) and homogeneous dispersion of the particles over the substrate. Energy Dispersive X-ray absorption (EDX) analysis confirmed the compositional homogeneity. The catalytic activity of these supported nanoparticles with regard to methanol electrooxidation is investigated using cyclic voltammetry (CV), chronoamperometry (CA) and CO-stripping voltammetry techniques at temperatures between 25 and 60 deg. C. Such investigation concerns supported catalysts prepared with ca. 10 and 18 wt.% overall metal loading (Pt + Ru) onto the Vulca[reg] XC72R substrate. Comparative testing of our catalysts and a commercial Pt-Ru/Vulcan reveals markedly superior activity for our catalysts. In fact, we observe for the latter a five-fold increase of the oxidation current as compared to a commercial Pt-Ru/Vulcan with equal metal loading. One of the reasons for the greater activity is found to be the very high dispersion of the metals over the substrate, i.e. the large surface area of the active phase. Other reasons are plausibly ascribable to the varied Pt/Ru composition and/or reduced presence of contaminants at the catalyst surface

Electrocatalytic Activity for CO, MeOH, and EtOH Oxidation on the Surface of Pt-Ru Nanoparticles Supported by Metal Oxide

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Kwang-Sik Sim

2011-01-01

Full Text Available This paper describes the electrocatalytic activity for CO, MeOH, and EtOH oxidation on the surface of Pt-Ru nanoparticles supported by metal oxide (Nb-TiO2-H prepared for use in a fuel cell. To prepare Nb-TiO2-supported Pt-Ru nanoparticles, first, the Nb-TiO2 supports were prepared by sol-gel reaction of titanium tetraisopropoxide with a small amount of the niobium ethoxide in polystyrene (PS colloids. Second, Pt-Ru nanoparticles were then deposited by chemical reduction of the Pt4+ and Ru3+ ions onto Nb-TiO2 supports (Pt-Ru@Nb-TiO2-CS. Nb element was used to reduce electrical resistance to facilitate electron transport during the electrochemical reactions on a fuel cell electrode. Finally, the Pt-Ru@Nb-TiO2-H catalysts were formed by the removal of core-polystyrene ball from Pt-Ru@TiO2-CS at 500∘C. The successfully prepared Pt-Ru electrocatalysts were confirmed via TEM, XPS, and ICP analysis. The electrocatalytic efficiency of Pt-Ru nanoparticles was evaluated via CO, MeOH, and EtOH oxidation for use in a direct methanol fuel cell (DMFC. As a result, the Pt-Ru@Nb-TiO2-H electrodes showed high electrocatalytic activity for the electrooxidation of CO, MeOH, and EtOH.

SiO2 decoration dramatically enhanced the stability of PtRu electrocatalysts with undetectable deterioration in fuel cell performance

Science.gov (United States)

Yu, Xinxin; Xu, Zejun; Yang, Zehui; Xu, Sen; Zhang, Quan; Ling, Ying; Zhang, Yunfeng; Cai, Weiwei

2018-06-01

Prevention of Ru dissolution is essential for steady CO tolerance of anodic electrocatalysts in direct methanol fuel cells. Here, we demonstrate a facile way to stabilize Ru atoms by decorating commercial CB/PtRu with SiO2, which shows a six-fold higher stability and similar activity toward a methanol oxidation reaction leading to no discernible degradation in fuel cell performance compared to commercial CB/PtRu electrocatalysts. The higher stability and stable CO tolerance of SiO2-decorated electrocatalysts originate from the SiO2 coating, since Ru atoms are partially ionized during SiO2 decorating, resulting in difficulties in dissolution; while, in the case of commercial CB/PtRu, the dissolved Ru offers active sites for Pt coalescences and CO species resulting in the rapid decay of the electrochemical surface area and fuel cell performance. To the best of our knowledge, this is the first study about the stabilization of Ru atoms by SiO2. The highest stability is obtained for a PtRu electrocatalyst with negligible effect on the electrochemical properties.

Separation of (Rh-103m)-rhodocene-derivatives from the parent (/sup 103/Ru)ruthenocen-derivatives and their organ distribution

Energy Technology Data Exchange (ETDEWEB)

Wenzel, M.; Wu, Y.

1987-01-01

The radioactive decay of (/sup 103/Ru)ruthenocene derivatives leads to sup(103m)Rh labelled rhodocinium derivatives, which can be separated by the extraction of a lipophilic solution of the ruthenocen derivate with water. The separation factor sup(103m)Rh//sup 103/Ru reaches values of 32:1 Rh/sup 3 +/ ions are not liberated and extracted. The organ distribution of the sup(103m)Rh labelled rhodocinium derivatives gained from ruthenocene and from N-isopropyl-ruthenocene amphetamine is different from the distribution of the parent ruthenocene compound. The liver and kidney uptake of the rhodocinium-amphetamine is much higher than the uptake with ruthenocene amphetamine.

The Effect of PtRuIr Nanoparticle Crystallinity in Electrocatalytic Methanol Oxidation

Directory of Open Access Journals (Sweden)

Vladimir Linkov

2013-04-01

Full Text Available Two structural forms of a ternary alloy PtRuIr/C catalyst, one amorphous and one highly crystalline, were synthesized and compared to determine the effect of their respective structures on their activity and stability as anodic catalysts in methanol oxidation. Characterization techniques included TEM, XRD, and EDX. Electrochemical analysis using a glassy carbon disk electrode for cyclic voltammogram and chronoamperometry were tested in a solution of 0.5 mol L−1 CH3OH and 0.5 mol L−1 H2SO4. Amorphous PtRuIr/C catalyst was found to have a larger electrochemical surface area, while the crystalline PtRuIr/C catalyst had both a higher activity in methanol oxidation and increased CO poisoning rate. Crystallinity of the active alloy nanoparticles has a big impact on both methanol oxidation activity and in the CO poisoning rate.

A determination method of Ru, Rh and Pd in high-level liquid waste (HLLW) by cation exchange separation and ICP-AES measurement

International Nuclear Information System (INIS)

Cao Desheng; Duan Shirong; Qin Fengzhou; Li Jinying; Zhang Huaili

1992-01-01

The authors describe a determination method of Ru, Rh and Pd in HLLW with cation-exchange separation and ICP-AES measurement. A sample of HLLW was treated with the hydrochloride acid containing enough sodium chloride, then passed through a strongly acidic cation-exchange resin column, the Ru, Rh and Pd as chloro-complexes go to the eluate while the interference elements are absorbed on the resins in the column. The Ru, Rh and Pd are collected and determined by ICP-AES. The obtained results show that the recovery is 90% and the relative standard deviation is 6% as the Ru content within the range (35-230) x 10 -6 ; the recovery is 106% and RSD is 10% as the Rh content within (2-20) x 10 -6 ; and the recovery of Pd is 72% as its content less than 2 x 10 -6

Preparation of PtRu/C anode electrocatalysts using gamma radiation for methanol electro-oxidation; Preparacao de eletrocatalisadores PtRu/C utilizando radiacao gama para aplicacao como anodo na oxidacao direta de metanol

Energy Technology Data Exchange (ETDEWEB)

Silva, Dionisio Fortunato da

2006-07-01

Pt Ru/C (carbon-supported Pt Ru nanoparticles) anode electrocatalysts were prepared using radiolytic process (gamma radiation) and tested for methanol electro-oxidation. In this process, water/2-propanol and water/ethylene glycol solutions containing the metallic ions and the carbon support were submitted to gamma radiation under stirring. The water/alcohol ratio (v/v) and the total dose (kGy) were studied. A nominal Pt Ru atomic ratio of 50:50 were used in all experiments. The electrocatalysts were characterized by energy dispersive X-ray analysis (EDX), X-ray diffraction (XRD), transmission electron microscopy (TEM) and cyclic voltammetry (CV). The electro-oxidation of methanol was studied by cyclic voltammetry using the thin porous coating technique. The electrocatalysts prepared in water/2-propanol showed crystallite size in the range of 3-5 nm and Pt Ru atomic ratio of 50:50. The electrocatalysts prepared in water/ethylene glycol showed crystallite size (2-3 nm) smaller than the ones obtained in water/2-propanol, however, the Pt Ru atomic ratios obtained were approximately 80:20, showing that only part of ruthenium ions were reduced. For methanol oxidation the electrocatalytic activity depends on the water/2-propanol and water/ethylene glycol ratio used in the reaction medium. The electrocatalysts prepared in water/2-propanol showed inferior performance to the ones prepared in water/ethylene glycol, which showed similar or superior performances (amperes per gram of platinum) to the commercial electrocatalyst from E-TEK. (author)

Effect of heat treatment on stability of gold particle modified carbon supported Pt-Ru anode catalysts for a direct methanol fuel cell

International Nuclear Information System (INIS)

Li Xiaowei; Liu Juanying; Huang Qinghong; Vogel, Walter; Akins, Daniel L.; Yang Hui

2010-01-01

Carbon supported Au-PtRu (Au-PtRu/C) catalysts were prepared as the anodic catalysts for the direct methanol fuel cell (DMFC). The procedure involved simple deposition of Au particles on a commercial Pt-Ru/C catalyst, followed by heat treatment of the resultant composite catalyst at 125, 175 and 200 o C in a N 2 atmosphere. High-resolution transmission electron microscopy (HR-TEM) measurements indicated that the Au nanoparticles were attached to the surface of the Pt-Ru nanoparticles. We found that the electrocatalytic activity and stability of the Au-PtRu/C catalysts for methanol oxidation is better than that of the PtRu/C catalyst. An enhanced stability of the electrocatalyst is observed and attributable to the promotion of CO oxidation by the Au nanoparticles adsorbed onto the Pt-Ru particles, by weakening the adsorption of CO, which can strongly adsorb to and poison Pt catalyst. XPS results show that Au-PtRu/C catalysts with heat treatment lead to surface segregation of Pt metal and an increase in the oxidation state of Ru, which militates against the dissolution of Ru. We additionally find that Au-PtRu/C catalysts heat-treated at 175 o C exhibit the highest electrocatalytic stability among the catalysts prepared by heat treatment: this observation is explained as due to the attainment of the highest relative concentration of gold and the highest oxidation state of Ru oxides for the catalyst pretreated at this temperature.

Ethanol electrooxidation using Ti/(RuO2)(x) Pt(1-x) electrodes prepared by the polymeric precursor method

Energy Technology Data Exchange (ETDEWEB)

Freitas, R.G.; Marchesi, L.F.Q.P.; Forim, M.R.; Pereira, E.C. [Departamento de Quimica, Universidade Federal de Sao Carlos, Sao Carlos, SP (Brazil); Bulhoes, L.O.S [CENIP, Centro Universitario Central Paulista, Sao Carlos, SP (Brazil); Santos, M.C. [LEMN, Centro de Ciencias Naturais e Humanas, Universidade Federal do ABC, Santo Andre, SP (Brazil); Oliveira, R.T.S., E-mail: robson@icbn.uftm.edu.br [Instituto de Ciencias Biologicas e Naturais, Universidade Federal do Triangulo Mineiro, Uberaba, MG (Brazil)

2011-09-15

This work describes a detailed study of the ethanol electrooxidation on Ti/(RuO{sub 2}){sub (x)}Pt{sub (1-x)} electrodes using several compositions prepared by the polymeric precursor method. The results obtained using cyclic voltammetry and chronoamperometry showed that the best composition of Ti/(RuO{sub 2}){sub (x)}Pt{sub (1-x)} electrodes for CO and ethanol oxidation processes is Ti/(RuO{sub 2}){sub 0.50}Pt{sub 0.50}. On this electrode composition the onset of CO and the ethanol oxidation occurred at 380 mV and 220 mV more negative than on Ti/Pt, respectively. Besides, there was an increase of 2.5-fold in the current density for ethanol electrooxidation under constant potential polarization. The Ti/(RuO{sub 2}){sub 0.50}Pt{sub 0.50}. electrodes produced lower amount of acetic acid compared to Ti/Pt and polycrystalline Pt electrodes using in situ HPLC spectrometric analysis. Also, a non common product from ethanol oxidation could be observed on higher RuO{sub 2} loads: ethyl acetate. Finally, the impedance data showed that Ti/(RuO{sub 2}){sub 0.50}Pt{sub 0.50}. electrode composition had the smallest charge transfer resistance for ethanol oxidation among those compositions investigated. (author)

STUDY OF THE Pt/Ru(0001) INTERFACE

DEFF Research Database (Denmark)

Godowski, P.J.; Li, Zheshen; Bork, J.

2007-01-01

to the different stages of the deposition were analyzed. Up to ca. two adsorbate monolayers, the intensity changes of the peaks indicated layer-by-layer growth mode. The surface core level shifts of Ru and Pt levels were evaluated as -0.33 and -0.476 eV, respectively. The valence band spectra show a rather weak...

Promotion of Pt-Ru/C catalysts driven by heat treated induced surface segregation for methanol oxidation reaction

International Nuclear Information System (INIS)

Wei Yuchen; Liu Chenwei; Chang Weijung; Wang Kuanwen

2011-01-01

Research highlights: → Thermal treatments on the Pt-Ru/C induce different extents of surface segregation. → O 2 treatment results in obvious Ru segregation and formation of RuO 2 . → Catalysts treated in H 2 have the excellent CO de-poisoning ability. → N 2 treatment suppresses the surface Pt depletion and hence promotes the MOR. - Abstract: Carbon supported Pt-Ru/C (1:1) alloy catalysts supplied by E-TEK are widely used for fuel cell research. Heat treatments in various atmospheres are conducted for the promotion of the methanol oxidation reaction (MOR) and the investigation of the structure-activity relationship (SAR) of the catalysts. The alloy structures, surface compositions, surface species, and electro-catalytic activities of the alloy catalysts are characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV), respectively. The as-received Pt-Ru/C catalysts have a Ru rich in the inner core and Pt rich on the outer shell structure. Thermal treatments on the catalysts induce Ru surface segregation in different extents and thereby lead to their alteration of the alloying degrees. O 2 treatment results in obvious Ru segregation and formation of RuO 2 . Catalysts treated in H 2 have the highest I f /I b value in the CV scans among all samples, indicating the catalysts have the excellent CO de-poisoning ability as evidenced by anodic CO stripping experiments. N 2 treatment may serve as an adjustment process for the surface composition and structure of the catalysts, which can suppress the surface Pt depletion (∼60% Pt on the surface), make the components stable and hence promote the MOR significantly.

Promotion of Pt-Ru/C catalysts driven by heat treated induced surface segregation for methanol oxidation reaction

Energy Technology Data Exchange (ETDEWEB)

Wei Yuchen; Liu Chenwei; Chang Weijung [Institute of Materials Science and Engineering, National Central University, Taoyuan 32001, Taiwan (China); Wang Kuanwen, E-mail: kuanwen.wang@gmail.com [Institute of Materials Science and Engineering, National Central University, Taoyuan 32001, Taiwan (China)

2011-01-12

Research highlights: > Thermal treatments on the Pt-Ru/C induce different extents of surface segregation. > O{sub 2} treatment results in obvious Ru segregation and formation of RuO{sub 2}. > Catalysts treated in H{sub 2} have the excellent CO de-poisoning ability. > N{sub 2} treatment suppresses the surface Pt depletion and hence promotes the MOR. - Abstract: Carbon supported Pt-Ru/C (1:1) alloy catalysts supplied by E-TEK are widely used for fuel cell research. Heat treatments in various atmospheres are conducted for the promotion of the methanol oxidation reaction (MOR) and the investigation of the structure-activity relationship (SAR) of the catalysts. The alloy structures, surface compositions, surface species, and electro-catalytic activities of the alloy catalysts are characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV), respectively. The as-received Pt-Ru/C catalysts have a Ru rich in the inner core and Pt rich on the outer shell structure. Thermal treatments on the catalysts induce Ru surface segregation in different extents and thereby lead to their alteration of the alloying degrees. O{sub 2} treatment results in obvious Ru segregation and formation of RuO{sub 2}. Catalysts treated in H{sub 2} have the highest I{sub f}/I{sub b} value in the CV scans among all samples, indicating the catalysts have the excellent CO de-poisoning ability as evidenced by anodic CO stripping experiments. N{sub 2} treatment may serve as an adjustment process for the surface composition and structure of the catalysts, which can suppress the surface Pt depletion ({approx}60% Pt on the surface), make the components stable and hence promote the MOR significantly.

Synthesis of Pt-Ru PSB-Py catalysis by {gamma}-irradiation and their electrocatalytic efficiency for methanol oxidation

Energy Technology Data Exchange (ETDEWEB)

Yoon, Jung Ah; Sim, Kwang Sik; Choi, Seong Ho [Hannam University, Daejeon (Korea, Republic of); Jung, Sung Hee [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

2009-09-15

We report here that deposition of Pt-Ru catalysis on the surface of core-shell conductive balls by radiation-chemical reduction of Pt and Ru ions, in order to use as catalysis in a fuel cell. The poly(styrene-co-4-vinylphenylboronic acid)-pyrrole (PSB-Py) with core-shell structure was obtained by in situ polymerization of pyrrole in the presence of the poly(styrene-co-4-vinylphenylboronic acid) (PSB). Subsequently, Pt-Ru catalysis were deposited onto PSB-Py ball by {gamma}-irradiation, in the presence/absence of poly(vinypyrolidone) (PVP) to prepare electrocatalysis for a fuel cell. The catalytic efficiency of Pt-Ru PSB-Py catalyst was examined for carbon monoxide (CO) stripping and methanol oxidation.

Synthesis of Pt-Ru PSB-Py catalysis by γ-irradiation and their electrocatalytic efficiency for methanol oxidation

International Nuclear Information System (INIS)

Yoon, Jung Ah; Sim, Kwang Sik; Choi, Seong Ho; Jung, Sung Hee

2009-01-01

We report here that deposition of Pt-Ru catalysis on the surface of core-shell conductive balls by radiation-chemical reduction of Pt and Ru ions, in order to use as catalysis in a fuel cell. The poly(styrene-co-4-vinylphenylboronic acid)-pyrrole (PSB-Py) with core-shell structure was obtained by in situ polymerization of pyrrole in the presence of the poly(styrene-co-4-vinylphenylboronic acid) (PSB). Subsequently, Pt-Ru catalysis were deposited onto PSB-Py ball by γ-irradiation, in the presence/absence of poly(vinypyrolidone) (PVP) to prepare electrocatalysis for a fuel cell. The catalytic efficiency of Pt-Ru PSB-Py catalyst was examined for carbon monoxide (CO) stripping and methanol oxidation

Co-catalytic effect of Ni in the methanol electro-oxidation on Pt-Ru/C catalyst for direct methanol fuel cell

International Nuclear Information System (INIS)

Wang, Z.B.; Yin, G.P.; Zhang, J.; Sun, Y.C.; Shi, P.F.

2006-01-01

This research is aimed to improve the utilization and activity of anodic catalysts, thus to lower the contents of noble metals loading in anodes for methanol electro-oxidation. The direct methanol fuel cell anodic catalysts, Pt-Ru-Ni/C and Pt-Ru/C, were prepared by chemical reduction method. Their performances were tested by using a glassy carbon working electrode through cyclic voltammetric curves, chronoamperometric curves and half-cell measurement in a solution of 0.5 mol/L CH 3 OH and 0.5 mol/L H 2 SO 4 . The composition of the Pt-Ru-Ni and Pt-Ru surface particles were determined by EDAX analysis. The particle size and lattice parameter of the catalysts were determined by means of X-ray diffraction (XRD). XRD analysis showed that both of the catalysts exhibited face-centered cubic structures and had smaller lattice parameters than Pt-alone catalyst. Their sizes are small, about 4.5 nm. No significant differences in the methanol electro-oxidation on both electrodes were found by using cyclic voltammetry, especially regarding the onset potential for methanol electro-oxidation. The electrochemically active-specific areas of the Pt-Ru-Ni/C and Pt-Ru/C catalysts are almost the same. But, the catalytic activity of the Pt-Ru-Ni/C catalyst is higher for methanol electro-oxidation than that of the Pt-Ru/C catalyst. Its tolerance performance to CO formed as one of the intermediates of methanol electro-oxidation is better than that of the Pt-Ru/C catalyst

Preparation of PtRu/C anode electrocatalysts using gamma radiation for methanol electro-oxidation

International Nuclear Information System (INIS)

Silva, Dionisio Fortunato da

2006-01-01

Pt Ru/C (carbon-supported Pt Ru nanoparticles) anode electrocatalysts were prepared using radiolytic process (gamma radiation) and tested for methanol electro-oxidation. In this process, water/2-propanol and water/ethylene glycol solutions containing the metallic ions and the carbon support were submitted to gamma radiation under stirring. The water/alcohol ratio (v/v) and the total dose (kGy) were studied. A nominal Pt Ru atomic ratio of 50:50 were used in all experiments. The electrocatalysts were characterized by energy dispersive X-ray analysis (EDX), X-ray diffraction (XRD), transmission electron microscopy (TEM) and cyclic voltammetry (CV). The electro-oxidation of methanol was studied by cyclic voltammetry using the thin porous coating technique. The electrocatalysts prepared in water/2-propanol showed crystallite size in the range of 3-5 nm and Pt Ru atomic ratio of 50:50. The electrocatalysts prepared in water/ethylene glycol showed crystallite size (2-3 nm) smaller than the ones obtained in water/2-propanol, however, the Pt Ru atomic ratios obtained were approximately 80:20, showing that only part of ruthenium ions were reduced. For methanol oxidation the electrocatalytic activity depends on the water/2-propanol and water/ethylene glycol ratio used in the reaction medium. The electrocatalysts prepared in water/2-propanol showed inferior performance to the ones prepared in water/ethylene glycol, which showed similar or superior performances (amperes per gram of platinum) to the commercial electrocatalyst from E-TEK. (author)

Electrooxidation of C{sub 1} to C{sub 3} alcohols with Pt and Pt-Ru sputter deposited interdigitated array electrodes

Energy Technology Data Exchange (ETDEWEB)

Lee, Choong-Gon [Department of Chemical Engineering, Faculty of Engineering, Hanbat National University, San 16-1, Dukmyeong-dong, Yuseong-gu, Daejeon 305-719 (Korea, Republic of)], E-mail: leecg@hanbat.ac.kr; Ojima, Hiroyuki [Department of Applied Chemistry, Graduate School of Engineering, Tohoku University, Aramaki-Aoba 07, Aoba-ku, Sendai 980-8579 (Japan); Umeda, Minoru [Department of Materials Science and Technology, Faculty of Engineering, Nagaoka University of Technology, Kamitomioka 1603-1, Nagaoka, Niigata 940-2188 (Japan)], E-mail: mumeda@vos.nagaokaut.ac.jp

2008-02-25

The electrooxidation of methanol, ethanol, and 2-propanol was investigated with interdigitated array electrodes (IDAEs). The IDAE oxidizes alcohol at the generator and reduces the reaction intermediates produced by the oxidation process at the collector. Thus, the reaction intermediates can be estimated with the IDAE. The IDAE in the present work was made of sputter deposited Pt and Pt-Ru. The use of Ru free and added electrodes provides information on the effect of Ru addition on the alcohol oxidation. Cyclic voltammetric analyses revealed that Ru addition enhances the oxidation currents and reduces the E{sub onset} of the alcohols. The detectable reaction intermediate at the methanol and ethanol oxidation was proton, while the intermediate species was acetone in 2-propnaol oxidation.

Electrochemical characterization of Pt-Ru-Pd catalysts for methanol oxidation reaction in direct methanol fuel cells.

Science.gov (United States)

Choi, M; Han, C; Kim, I T; An, J C; Lee, J J; Lee, H K; Shim, J

2011-01-01

PtRuPd nanoparticles on carbon black were prepared and characterized as electrocatalysts for methanol oxidation reaction in direct methanol fuel cells. Nano-sized Pd (2-4 nm) particles were deposited on Pt/C and PtRu/C (commercial products) by a simple chemical reduction process. The structural and physical information of the PtRuPd/C were confirmed by TEM and XRD, and their electrocatalytic activities were measured by cyclic voltammetry and linear sweep voltammetry. The catalysts containing Pd showed higher electrocatalytic activity for methanol oxidation reaction than the other catalysts. This might be attributed to an increase in the electrochemical surface area of Pt, which is caused by the addition of Pd; this results in increased catalyst utilization.

Activity of PtSnRh/C nanoparticles for the electrooxidation of C1 and C2 alcohols

International Nuclear Information System (INIS)

Teran, Freddy E.; Santos, Deise M.; Ribeiro, Josimar; Kokoh, Kouakou B.

2012-01-01

A systematic investigation of alcohol adsorption and oxidation on binary and ternary electrocatalysts in acid medium was performed. Binary (PtRh) and ternary (PtRhSn) were prepared by the Pechini modified method on carbon Vulcan XC-72, and different nominal compositions were characterized by energy dispersive X-ray and X-ray diffraction (XRD) techniques. The XRD results showed that the Pt 80 Rh 20 /C and Pt 70 Sn 10 Rh 20 /C electrocatalysts consisted of the Pt displaced phase, suggesting the formation of a solid solution between the metals Pt/Rh and Pt/Sn. Electrochemical investigations on these different electrode materials were carried out as a function of the electrocatalyst composition, in acid medium (0.5 mol dm −3 H 2 SO 4 ), and in the absence and presence of different alcohols (methanol, ethanol and ethylene glycol). The electrochemical results obtained at room temperature have shown that the Pt 70 Sn 10 Rh 20 /C catalyst display better catalytic activity for alcohol oxidation compared with the binary catalyst. In situ reflectance infrared spectroscopy measurements have shown that the oxidation of alcohols mentioned produced CO 2 at low potentials indicating that the materials synthesized could be used as efficient anodes in the fuel cell applications. - Highlights: ► Pt-based catalysts were synthesized by thermal decomposition polymeric precursors. ► Pt 70 Sn 10 Rh 20 /C displays better catalytic activity for the oxidation of alcohols. ► The co-catalysts tin and rhodium promote the removal of CO to CO 2 at low potentials. ► Ethylene glycol is oxidizing strongly to CO 2 at low potentials. ► Pt 70 Sn 10 Rh 20 /C catalyst is an efficient anode material for a direct alcohol fuel cell.

A durable PtRu/C catalyst with a thin protective layer for direct methanol fuel cells.

Science.gov (United States)

Shimazaki, Yuzuru; Hayasaka, Sho; Koyama, Tsubasa; Nagao, Daisuke; Kobayashi, Yoshio; Konno, Mikio

2010-11-15

A methanol oxidation catalyst with improved durability in acidic environments is reported. The catalyst consists of PtRu alloy nanoparticles on a carbon support that were stabilized with a silane-coupling agent. The catalyst was prepared by reducing ions of Pt and Ru in the presence of a carbon support and the silane-coupling agent. The careful choice of preparatory conditions such as the concentration of the silane-coupling agent and solution pH resulted in the preparation of catalyst in which the PtRu nanoparticles were dispersively adsorbed onto the carbon support. The catalytic activity was similar to that of a commercial catalyst and was unchanged after immersion in sulfuric acid solution for 1000 h, suggesting the high durability of the PtRu catalyst for the anode of direct methanol fuel cells. Copyright © 2010 Elsevier Inc. All rights reserved.

Emission Spectroscopy as a Probe into Photoinduced Intramolecular Electron Transfer in Polyazine Bridged Ru(II,Rh(III Supramolecular Complexes

Directory of Open Access Journals (Sweden)

Karen J. Brewer

2010-08-01

Full Text Available Steady-state and time-resolved emission spectroscopy are valuable tools to probe photochemical processes of metal-ligand, coordination complexes. Ru(II polyazine light absorbers are efficient light harvesters absorbing in the UV and visible with emissive 3MLCT excited states known to undergo excited state energy and electron transfer. Changes in emission intensity, energy or band-shape, as well as excited state lifetime, provide insight into excited state dynamics. Photophysical processes such as intramolecular electron transfer between electron donor and electron acceptor sub-units may be investigated using these methods. This review investigates the use of steady-state and time-resolved emission spectroscopy to measure excited state intramolecular electron transfer in polyazine bridged Ru(II,Rh(III supramolecular complexes. Intramolecular electron transfer in these systems provides for conversion of the emissive 3MLCT (metal-to-ligand charge transfer excited state to a non-emissive, but potentially photoreactive, 3MMCT (metal-to-metal charge transfer excited state. The details of the photophysics of Ru(II,Rh(III and Ru(II,Rh(III,Ru(II systems as probed by steady-state and time-resolved emission spectroscopy will be highlighted.

Functional separation of oxidation–reduction reactions and electron transport in PtRu/ND and conductive additive hybrid electrocatalysts during methanol oxidation

Energy Technology Data Exchange (ETDEWEB)

Zhang, Yan; Wang, Yanhui [State Key Laboratory of Metastable Materials Science and Technology, College of Materials Science and Engineering, Yanshan University, Qinhuangdao 066004 (China); Bian, Linyan [College of Physics and Chemistry, Henan Polytechnic University, Jiaozuo, Henan 454000 (China); Lu, Rui [State Key Laboratory of Metastable Materials Science and Technology, College of Materials Science and Engineering, Yanshan University, Qinhuangdao 066004 (China); Zang, Jianbing, E-mail: jbzang@ysu.edu.cn [State Key Laboratory of Metastable Materials Science and Technology, College of Materials Science and Engineering, Yanshan University, Qinhuangdao 066004 (China)

2016-02-28

Graphical abstract: - Highlights: • Functional separation of reactions and electron transport in PtRu/ND + AB (or CNT). • A conductive network was formed after the addition of AB or CNT. • PtRu/ND + AB (or CNT) exhibited enhanced activity and stability than PtRu/ND. - Abstract: Undoped nanodiamond (ND) supported PtRu (PtRu/ND) electrocatalyst for methanol oxidation reactions (MOR) in direct methanol fuel cells was prepared by a microwave-assisted polyol reduction method. Sp{sup 3}-bonded ND possesses high electrochemical stability but low conductivity, while sp{sup 2}-bonded carbon nanomaterials with high conductivity are prone to oxidation. Therefore, the functions of the supporting material were separated in this study. ND (sp{sup 3}), as a support, and AB or CNTs (sp{sup 2}), as a conductive additive, were combined to form the hybrid electrocatalysts PtRu/ND + AB and PtRu/ND + CNT for MOR. The morphology of the electrocatalysts was characterized by scanning electron microscopy and electrochemical measurements were performed using an electrochemical workstation. The results indicated that the electrocatalytic activity of PtRu/ND for MOR was improved with the addition of AB or CNTs as a conductive additive. Moreover, adding CNTs to PtRu/ND as a conductive additive showed better electrocatalytic activities than adding AB, which can be ascribed to the better electron-transfer ability of CNTs.

Metal-insulator transition and superconductivity induced by Rh doping in the binary pnictides RuPn (Pn=P, As, Sb)

Science.gov (United States)

Hirai, Daigorou; Takayama, Tomohiro; Hashizume, Daisuke; Takagi, Hidenori

2012-04-01

Binary ruthenium pnictides, RuP and RuAs, with an orthorhombic MnP structure, were found to show a metal to a nonmagnetic insulator transition at TMI = 270 and 200 K, respectively. In the metallic region above TMI, a structural phase transition, accompanied with a weak anomaly in the resistivity and the magnetic susceptibility, indicative of a pseudogap formation, was identified at Ts = 330 and 280 K, respectively. These two transitions were suppressed by substituting Ru with Rh. We found superconductivity with a maximum Tc = 3.7 and 1.8 K in a narrow composition range around the critical point for the pseudogap phase, Rh content xc = 0.45 and 0.25 for Ru1-xRhxP and Ru1-xRhxAs, respectively, which may provide us with a nonmagnetic route to superconductivity at a quantum critical point.

Nitrogen Doped Ordered Mesoporous Carbon as Support of PtRu Nanoparticles for Methanol Electro-Oxidation

Directory of Open Access Journals (Sweden)

David Sebastián

2018-04-01

Full Text Available The low oxidation kinetics of alcohols and the need for expensive platinum group metals are still some of the main drawbacks for the commercialization of energy efficient direct alcohol fuel cells. In this work, we investigate the influence of nitrogen doping of ordered mesoporous carbon (CMK as support on the electrochemical activity of PtRu nanoparticles. Nitrogen doping procedures involve the utilization of pyrrole as both nitrogen and carbon precursor by means of a templating method using mesoporous silica. This method allows obtaining carbon supports with up to 14 wt. % nitrogen, with an effective introduction of pyridinic, pyrrolic and quaternary nitrogen. PtRu nanoparticles were deposited by sodium formate reduction method. The presence of nitrogen mainly influences the Pt:Ru atomic ratio at the near surface, passing from 50:50 on the bare (un-doped CMK to 70:30 for the N-doped CMK catalyst. The electroactivity towards the methanol oxidation reaction (MOR was evaluated in acid and alkaline electrolytes. The presence of nitrogen in the support favors a faster oxidation of methanol due to the enrichment of Pt at the near surface together with an increase of the intrinsic activity of PtRu nanoparticles.

A comprehensive study on the effect of Ru addition to Pt electrodes ...

Indian Academy of Sciences (India)

Administrator

The electro-oxidation of ethanol was studied over nanosized Pt and different compositions of ... The onset potential of ethanol electro-oxidation is lowered on bimetallic PtRu ..... Hogarth M P and Ralph T R 2002 Platinum Metals Review 46.

Improvements of electrocatalytic activity of PtRu nanoparticles on multi-walled carbon nanotubes by a H2 plasma treatment in methanol and formic acid oxidation

International Nuclear Information System (INIS)

Jiang Zhongqing; Jiang Zhongjie

2011-01-01

Graphical abstract: A H 2 plasma, that aims at reducing the fraction of the oxidized species at the outermost perimeter of metal particles, has been used to treat the PtRu nanoparticles supported on the plasma functionalized multi-walled carbon nanotubes (PtRu/PS-MWCNTs). The plasma treated PtRu/PS-MWCNTs exhibit increased electrochemically active surface area, reduced charge transfer resistance, improved electrocatalytic activity and long term stability toward methanol and formic acid oxidation, and enhanced tolerance to carbonaceous species relative to the sample untreated with the H 2 plasma. Highlights: → A H 2 plasma technique is used to treat the PtRu nanoparticles. → The H 2 plasma treated PtRu/PS-MWCNTs exhibit improved electrocatalytic activity. → The H 2 plasma treated PtRu/PS-MWCNTs have significantly reduced charge transfer resistance. → The H 2 plasma treated PtRu/PS-MWCNTs show the increased stability. → The Pt:Ru atomic ratio of PtRu nanoparticles has a significant effect on the electrochemical activity. - Abstract: A H 2 plasma has been used to treat the PtRu nanoparticles supported on the plasma functionalized multi-walled carbon nanotubes (PtRu/PS-MWCNTs). The plasma treatment does not change the size and crystalline structure of PtRu nanoparticles, but reduces the fraction of the oxidized species at the outermost perimeter of particles. The electrochemical results show that these plasma treated PtRu/PS-MWCNTs exhibit increased electrochemically active surface area, improved electrocatalytic activity and long term stability toward methanol and formic acid oxidation, and enhanced tolerance to carbonaceous species relative to the sample untreated with the H 2 plasma. The electrocatalytic activities of the plasma treated PtRu/PS-MWCNTs are found to be dependent upon the Pt:Ru atomic ratios of PtRu nanoparticles. The catalysts with a Pt:Ru atomic ratio close to 1:1 show superior properties in the electrooxidation of methanol and formic acid

High activity PtRu/C catalysts synthesized by a modified impregnation method for methanol electro-oxidation

International Nuclear Information System (INIS)

Ma Liang; Liu Changpeng; Liao Jianhui; Lu Tianhong; Xing Wei; Zhang Jiujun

2009-01-01

A modified impregnation method was used to prepare highly dispersive carbon-supported PtRu catalyst (PtRu/C). Two modifications to the conventional impregnation method were performed: one was to precipitate the precursors ((NH 4 ) 2 PtCl 6 and Ru(OH) 3 ) on the carbon support before metal reduction; the other was to add a buffer into the synthetic solution to stabilize the pH. The prepared catalyst showed a much higher activity for methanol electro-oxidation than a catalyst prepared by the conventional impregnation method, even higher than that of current commercially available, state-of-the-art catalysts. The morphology of the prepared catalyst was characterized using TEM and XRD measurements to determine particle sizes, alloying degree, and lattice parameters. Electrochemical methods were also used to ascertain the electrochemical active surface area and the specific activity of the catalyst. Based on XPS measurements, the high activity of this catalyst was found to originate from both metallic Ru (Ru 0 ) and hydrous ruthenium oxides (RuO x H y ) species on the catalyst surface. However, RuO x H y was found to be more active than metallic Ru. In addition, the anhydrous ruthenium oxide (RuO 2 ) species on the catalyst surface was found to be less active.

Activity of PtSnRh/C nanoparticles for the electrooxidation of C1 and C2 alcohols

Energy Technology Data Exchange (ETDEWEB)

Teran, Freddy E. [Universite de Poitiers, IC2MP UMR CNRS 7285, ' Equipe E-lyse' , 4 rue Michel Brunet-B27, BP 633, 86022 Poitiers cedex (France); Santos, Deise M. [Departamento de Quimica, CCE-UFES, Av. Fernando Ferrari, 514, Goiabeiras-Vitoria, ES (Brazil); Ribeiro, Josimar, E-mail: josimar.ribeiro@ufes.br [Universite de Poitiers, IC2MP UMR CNRS 7285, ' Equipe E-lyse' , 4 rue Michel Brunet-B27, BP 633, 86022 Poitiers cedex (France); Departamento de Quimica, CCE-UFES, Av. Fernando Ferrari, 514, Goiabeiras-Vitoria, ES (Brazil); Kokoh, Kouakou B. [Universite de Poitiers, IC2MP UMR CNRS 7285, ' Equipe E-lyse' , 4 rue Michel Brunet-B27, BP 633, 86022 Poitiers cedex (France)

2012-07-01

A systematic investigation of alcohol adsorption and oxidation on binary and ternary electrocatalysts in acid medium was performed. Binary (PtRh) and ternary (PtRhSn) were prepared by the Pechini modified method on carbon Vulcan XC-72, and different nominal compositions were characterized by energy dispersive X-ray and X-ray diffraction (XRD) techniques. The XRD results showed that the Pt{sub 80}Rh{sub 20}/C and Pt{sub 70}Sn{sub 10}Rh{sub 20}/C electrocatalysts consisted of the Pt displaced phase, suggesting the formation of a solid solution between the metals Pt/Rh and Pt/Sn. Electrochemical investigations on these different electrode materials were carried out as a function of the electrocatalyst composition, in acid medium (0.5 mol dm{sup -3} H{sub 2}SO{sub 4}), and in the absence and presence of different alcohols (methanol, ethanol and ethylene glycol). The electrochemical results obtained at room temperature have shown that the Pt{sub 70}Sn{sub 10}Rh{sub 20}/C catalyst display better catalytic activity for alcohol oxidation compared with the binary catalyst. In situ reflectance infrared spectroscopy measurements have shown that the oxidation of alcohols mentioned produced CO{sub 2} at low potentials indicating that the materials synthesized could be used as efficient anodes in the fuel cell applications. - Highlights: Black-Right-Pointing-Pointer Pt-based catalysts were synthesized by thermal decomposition polymeric precursors. Black-Right-Pointing-Pointer Pt{sub 70}Sn{sub 10}Rh{sub 20}/C displays better catalytic activity for the oxidation of alcohols. Black-Right-Pointing-Pointer The co-catalysts tin and rhodium promote the removal of CO to CO{sub 2} at low potentials. Black-Right-Pointing-Pointer Ethylene glycol is oxidizing strongly to CO{sub 2} at low potentials. Black-Right-Pointing-Pointer Pt{sub 70}Sn{sub 10}Rh{sub 20}/C catalyst is an efficient anode material for a direct alcohol fuel cell.

[Determination of ru, rh and Pd in 30% trialkyl phosphine oxide (TRPO)-kerosene by inductively coupled plasma-atomic emission spectrum (ICP-AES)].

Science.gov (United States)

Wang, Jian-Chen; Zhang, Lin

2013-07-01

The determination method of Ru, Rh and Pd in 30% TRPO-kerosene ICP-AES was studied by using aqueous calibration reference solution and choosing ethanol as diluent. The effects of the contents of 30% TRPO-kerosene and aqueous solution and the concentration of HNO3 in 30% TRPO-kerosene on the intensities of Ru, Rh and Pd were described. The optimized condition for preparing samples and calibration solutions was chosen as follows: The contents of 30% TRPO-kerosene and aqueous phase were 10% (V/V) and 5% (V/V) respectively and the concentration of HNO3 30% TRPO-kerosene was 0.20 mol x L(-1). The determination method of Au, Ru and Pd was set up according to the above condition. The detection limit, precision and recovery ratio of Ru, Rh and Pd are well. The method is not only used in determination of Au, Ru and Pd in 30% TRPO-kerosene, but also used in other organic phases.

Assessment for the role of rare earth oxide in the R2O3 - RuO2 - Pt composite electrode

International Nuclear Information System (INIS)

Do Ngoc Lien; Nguyen Van Sinh

2004-01-01

Our work has showed several results related to assessment for the role of rare earth oxide in the R 2 O 3 - RuO 2 - Pt composite electrode. The precursor method was used for preparing composite electrode in the following forms: a- RuO 2 - Pt electrode b- La 2 O 3 (55%) - RuO 2 (45%) - Pt electrode c- CeO 2 (60%) - RuO 2 (40%) - Pt electrode By measurements of anodic polarization and cyclic potential for the types of a, b, c electrodes we can see that the La 2 O 3 (55%) - 45% RuO 2 - Pt electrode will be the best anodic electrode. It means that the partial replacement of ruthenium oxide by lanthanum oxide in composite oxide electrode will be an effective one. (author)

Ru-decorated Pt surfaces as model fuel cell electrocatalysts for CO electrooxidation.

Science.gov (United States)

Maillard, F; Lu, G-Q; Wieckowski, A; Stimming, U

2005-09-01

This feature article concerns Pt surfaces modified (decorated) by ruthenium as model fuel cell electrocatalysts for electrooxidation processes. This work reveals the role of ruthenium promoters in enhancing electrocatalytic activity toward organic fuels for fuel cells, and it particularly concerns the methanol decomposition product, surface CO. A special focus is on surface mobility of the CO as it is catalytically oxidized to CO(2). Different methods used to prepare Ru-decorated Pt single crystal surfaces as well as Ru-decorated Pt nanoparticles are reviewed, and the methods of characterization and testing of their activity are discussed. The focus is on the origin of peak splitting involved in the voltammetric electrooxidation of CO on Ru-decorated Pt surfaces, and on the interpretative consequences of the splitting for single crystal and nanoparticle Pt/Ru bimetallic surfaces. Apparently, screening through the literature allows formulating several models of the CO stripping reaction, and the validity of these models is discussed. Major efforts are made in this article to compare the results reported by the Urbana-Champaign group and the Munich group, but also by other groups. As electrocatalysis is progressively more and more driven by theory, our review of the experimental findings may serve to summarize the state of the art and clarify the roads ahead. Future studies will deal with highly dispersed and reactive nanoscale surfaces and other more advanced catalytic materials for fuel cell catalysis and related energy applications. It is expected that the metal/metal and metal/substrate interactions will be increasingly investigated on atomic and electronic levels, with likewise increasing participation of theory, and the structure and reactivity of various monolayer catalytic systems involving more than two metals (that is ternary and quaternary systems) will be interrogated.

Magnetic spin configuration in Fe{sub 50}Pt{sub 50-x}Rh{sub x} alloys

Energy Technology Data Exchange (ETDEWEB)

Fenske, J.; Lott, D.; Schreyer, A. [GKSS Research Centre (Germany); Mankey, G.J. [University of Alabama, MINT Center (United States); Schmidt, W.; Schmalzl, K. [Juelich Research Centre (Germany); Tartakowskaya, E. [Institute for Magnetism, National Ukrainian Accademy of Science (Ukraine)

2010-07-01

FePt-based alloys are typically the material of choice for magnetic information storage media. The high magnetic moment of Fe gives a large magnetization and the large atomic number of Pt results in a high magnetic anisotropy. This combination enables the written bits to be smaller than ever before. One way to control the magnetic properties in these materials is through the introduction of a third element into the crystal matrix e.g. Rh. When Rh is added to replace Pt in the equiatomic alloy, new magnetic phases emerge. Bulk samples of Fe{sub 50}Pt{sub 50-x}Rh{sub x} studied by magnetization measurements refer to three different phase transitions with increasing temperature: (I) An antiferromagnetic (AF)-paramagnetic (PM) transition for 30Pt{sub 50-x}Rh{sub x} films with different Rh concentrations. These films were examined by neutron diffraction in dependence of temperature and magnetic field. By the use of polarized and unpolarized neutron diffraction we could develop a detailed model of the magnetic spin structure in these thin films.

Ternary Pt/Rh/SnO2 electrocatalysts for oxidizing ethanol to CO2.

Science.gov (United States)

Kowal, A; Li, M; Shao, M; Sasaki, K; Vukmirovic, M B; Zhang, J; Marinkovic, N S; Liu, P; Frenkel, A I; Adzic, R R

2009-04-01

Ethanol, with its high energy density, likely production from renewable sources and ease of storage and transportation, is almost the ideal combustible for fuel cells wherein its chemical energy can be converted directly into electrical energy. However, commercialization of direct ethanol fuel cells has been impeded by ethanol's slow, inefficient oxidation even at the best electrocatalysts. We synthesized a ternary PtRhSnO(2)/C electrocatalyst by depositing platinum and rhodium atoms on carbon-supported tin dioxide nanoparticles that is capable of oxidizing ethanol with high efficiency and holds great promise for resolving the impediments to developing practical direct ethanol fuel cells. This electrocatalyst effectively splits the C-C bond in ethanol at room temperature in acid solutions, facilitating its oxidation at low potentials to CO(2), which has not been achieved with existing catalysts. Our experiments and density functional theory calculations indicate that the electrocatalyst's activity is due to the specific property of each of its constituents, induced by their interactions. These findings help explain the high activity of Pt-Ru for methanol oxidation and the lack of it for ethanol oxidation, and point to the way to accomplishing the C-C bond splitting in other catalytic processes.

High activity of cubic PtRh alloys supported on graphene towards ethanol electrooxidation.

Science.gov (United States)

Rao, Lu; Jiang, Yan-Xia; Zhang, Bin-Wei; Cai, Yuan-Rong; Sun, Shi-Gang

2014-07-21

Cubic PtRh alloys supported on graphene (PtxRhy/GN) with different atomic ratio of Pt and Rh were directly synthesized for the first time using the modified polyol method with Br(-) for the shape-directing agents. The process didn't use surface-capping agents such as PVP that easily occupy the active sites of electrocatalysts and are difficult to remove. Graphene is the key factor for cubic shape besides Br(-) and keeping catalysts high-dispersed. The X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM) were used to characterize the structure and morphology of these electrocatalysts. The results showed that they were composed of homogeneous cubic PtRh alloys. Traditional electrochemical methods, such as cyclic voltammetry and chronoamperometry, were used to investigate the electrocatalytic properties of PtxRhy/GN towards ethanol electrooxidation. It can be seen that PtxRhy/GN with all atomic ratios exhibited high catalytic activity, and the most active one has a composition with Pt : Rh = 9 : 1 atomic ratio. Electrochemical in situ FTIR spectroscopy was used to evaluate the cleavage of C-C bond in ethanol at room temperature in acidic solutions, the results illustrated that Rh in an alloy can promote the split of C-C bond in ethanol, and the alloy catalyst with atomic ratio Pt : Rh = 1 : 1 showed obviously better performance for the C-C bond breaking in ethanol and higher selectivity for the enhanced activity of ethanol complete oxidation to CO2 than alloys with other ratios of Pt and Rh. The investigation indicates that high activity of PtxRhy/GN electrocatalyst towards ethanol oxidation is due to the specific shape of alloys and the synergistic effect of two metal elements as well as graphene support.

Comparing Pt/SrTiO3 to Rh/SrTiO3 for hydrogen photocatalytic production from ethanol

KAUST Repository

Wahab, A. K.; Odedairo, T.; Labis, J.; Hedhili, Mohamed N.; Delavar, A.; Idriss, H.

2013-01-01

Photocatalytic hydrogen production from ethanol as an example of biofuel is studied over 0.5 wt% Rh/SrTiO3 and 0.5 wt% Pt/SrTiO3 perovskite materials. The rate of hydrogen production, rH2, over Pt/SrTiO3 is found to be far higher than that observed over Rh/SrTiO3 (4 × 10−6 mol of H2 g catal. −1 min−1 (1.1 × 10−6 mol of H2 m catal. −2 min−1) compared to 0.7 × 10−6 mol of H2 g catal. −1 min−1 (5.5 × 10−8 mol of H2 m catal. −2 min−1), respectively, under UV excitation with a flux equivalent to that from the sun light (ca. 1 mW cm−2). Analyses of the XPS Rh3d and XPS Pt4f indicate that Rh is mainly present in its ionic form (Rh3+) while Pt is mainly present in its metallic form (Pt0). A fraction of the non-metallic state of Rh in the catalyst persisted even after argon ion sputtering. The tendency of Rh to be oxidized compared to Pt might be the reason behind the lower activity of the former compared to the later. On the contrary, a larger amount of methane are formed on the Rh containing catalyst compared to that observed on the Pt containing catalyst due to the capacity of Rh to break the carbon–carbon bond of the organic compound.

Comparing Pt/SrTiO3 to Rh/SrTiO3 for hydrogen photocatalytic production from ethanol

KAUST Repository

Wahab, A. K.

2013-08-13

Photocatalytic hydrogen production from ethanol as an example of biofuel is studied over 0.5 wt% Rh/SrTiO3 and 0.5 wt% Pt/SrTiO3 perovskite materials. The rate of hydrogen production, rH2, over Pt/SrTiO3 is found to be far higher than that observed over Rh/SrTiO3 (4 × 10−6 mol of H2 g catal. −1 min−1 (1.1 × 10−6 mol of H2 m catal. −2 min−1) compared to 0.7 × 10−6 mol of H2 g catal. −1 min−1 (5.5 × 10−8 mol of H2 m catal. −2 min−1), respectively, under UV excitation with a flux equivalent to that from the sun light (ca. 1 mW cm−2). Analyses of the XPS Rh3d and XPS Pt4f indicate that Rh is mainly present in its ionic form (Rh3+) while Pt is mainly present in its metallic form (Pt0). A fraction of the non-metallic state of Rh in the catalyst persisted even after argon ion sputtering. The tendency of Rh to be oxidized compared to Pt might be the reason behind the lower activity of the former compared to the later. On the contrary, a larger amount of methane are formed on the Rh containing catalyst compared to that observed on the Pt containing catalyst due to the capacity of Rh to break the carbon–carbon bond of the organic compound.

Ultrasonically treated multi-walled carbon nanotubes (MWCNTs) as PtRu catalyst supports for methanol electrooxidation

Energy Technology Data Exchange (ETDEWEB)

Yang, Chunwei; Hu, Xinguo; Wang, Dianlong; Dai, Changsong [Department of Applied Chemistry, Harbin Institute of Technology, Harbin 150001 (China); Zhang, Liang; Jin, Haibo [School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081 (China); Agathopoulos, Simeon [Department of Materials Science and Engineering, University of Ioannina, GR-451 10 Ioannina (Greece)

2006-09-29

In the quest of fabricating supported catalysts, experimental results of transmission electron microscopy, Raman and infrared spectroscopy indicate that ultrasonic treatment effectively functionalizes multi-walled carbon nanotubes (MWCNTs), endowing them with groups that can act as nucleation sites which can favor well-dispersed depositions of PtRu clusters on their surface. Ultrasonic treatment seems to be superior than functionalization via regular refluxing. This is confirmed by the determination of the electrochemistry active surface area (ECA) and the CO-tolerance performance of the PtRu catalysts, measured by adsorbed CO-stripping voltammetry in 0.5M sulfuric acid solution, and the real surface area of the PtRu catalysts, evaluated by Brunauer-Emmett-Teller (BET) measurements. Finally, the effectiveness for methanol oxidation is assessed by cyclic voltammetry (CV) in a sulfuric acid and methanol electrolyte. (author)

Novel Electronic Structures of Ru-pnictides RuPn (Pn = P, As, Sb)

Science.gov (United States)

Goto, H.; Toriyama, T.; Konishi, T.; Ohta, Y.

Density-functional-theory-based electronic structure calculations are made to consider the novel electronic states of Ru-pnictides RuP and RuAs where the intriguing phase transitions and superconductivity under doping of Rh have been reported. We find that there appear nearly degenerate flat bands just at the Fermi level in the high-temperature metallic phase of RuP and RuAs; the flat-band states come mainly from the 4dxy orbitals of Ru ions and the Rh doping shifts the Fermi level just above the flat bands. The splitting of the flat bands caused by their electronic instability may then be responsible for the observed phase transition to the nonmagnetic insulating phase at low temperatures. We also find that the band structure calculated for RuSb resembles that of the doped RuP and RuAs, which is consistent with experiment where superconductivity occurs in RuSb without Rh doping.

{sup 96}Ru(p,{gamma}){sup 97}Rh measurement at the GSI storage ring

Energy Technology Data Exchange (ETDEWEB)

Zhong, Q; Aumann, T; Boretzky, K; Bosch, F; Braeuning, H; Brandau, C; Ershova, O; Geissel, H; Heil, M; Kelic, A; Kozhuharov, C; Langer, C; Bleis, T Le; Litvinov, Y A [GSI Helmholtzzentrum fuer Schwerionenforschung GmbH, Darmstadt, 64291 (Germany); Bishop, S; Dillmann, I [Technische Universitaet Muenchen, 85748 Garching (Germany); Blaum, K [Max-Planck-Institut fuer Kernphysik, 69117 Heidelberg (Germany); Davinson, T [University of Edinburgh, Edinburgh (United Kingdom); Gyuerky, G [Institute of Nuclear Research of the Hungarian Academy of Sciences (Hungary); Kaeppeler, F, E-mail: r.reifarth@gsi.d [Forschungszentrum Karlsruhe, Institut fuer Kernphysik, Karlsruhe (Germany)

2010-01-01

A pioneering experiment was recently performed at the Experimental Storage Ring (ESR) at GSI. Fully stripped ions of {sup 96}Ru were injected into the storage ring and slowed down to a few MeV per nucleon. The {sup 97}Rh ions from the {sup 96}Ru(p,{gamma}) reaction at a newly developed hydrogen jet target were detected with Double Sided Silicon Strip Detectors (DSSSD) mounted inside a pocket. The experiment and the status of the analysis at a beam energy of 11 MeV per nucleon will be presented.

Estimates of relative doses of {sup 106}Ru/{sup 106}Rh of spherical applicators used in ophthalmic brachytherapy; Estimativas de doses relativas de aplicadores esfericos de {sup 106}Ru/{sup 106}Rh usados em braquiterapia oftalmologica

Energy Technology Data Exchange (ETDEWEB)

Paiva, Eduardo de, E-mail: edup2112@gmail.com, E-mail: epaiva@ird.gov.br [Instituto de Radioprotecao e Dosimetria (IRD/CNEN-RJ), Rio de Janeiro, RJ (Brazil). Div. de Fisica Medica

2016-11-01

Spherical ophthalmic applicators containing the beta emitter {sup 106}Ru / {sup 106}Rh are much used in brachytherapy for the treatment of various eye diseases. However, there is great difficulty in dosimetry these sources because of its geometric shape, the short range of the beta particles and the large dose gradient, and because of that calculation methods of dose distributions around these sources take on a great importance. In this work an analytical / numerical method is used to estimate the dose rates for a function of depth for spherical sources containing {sup 106}Ru / {sup 106}Rh. The results of the doses on along the central axis for applicators models CXS, CCX, CCY, CCZ, CCD and CGD and CCC are compared with published values calculated by Monte Carlo simulation and measurement results.

Methanol oxidation reaction on Ti/RuO{sub 2(x)}Pt{sub (1-x)} electrodes prepared by the polymeric precursor method

Energy Technology Data Exchange (ETDEWEB)

Freitas, R.G.; Marchesi, L.F.; Mattos-Costa, F.I.; Pereira, E.C. [Laboratorio Interdisciplinar de Eletroquimica e Ceramica, Centro Multidisciplinar para o Desenvolvimento de Materiais Ceramicos, Departamento de Quimica, Universidade Federal de Sao Carlos, Caixa Postal 676, 13560-905 Sao Carlos, SP (Brazil); Oliveira, R.T.S. [Laboratorio Interdisciplinar de Eletroquimica e Ceramica, Centro Multidisciplinar para o Desenvolvimento de Materiais Ceramicos, Departamento de Quimica, Universidade Federal de Sao Carlos, Caixa Postal 676, 13560-905 Sao Carlos, SP (Brazil); Grupo de Materiais Eletroquimicos e Metodos Eletroanaliticos, Instituto de Quimica de Sao Carlos, Universidade de Sao Paulo, Caixa Postal 780, 13566-590 Sao Carlos, SP (Brazil); LEMN, Laboratorio de Eletroquimica e Materiais Nanoestruturados, CCNH-Centro de Ciencias Naturais e Humanas, UFABC-Universidade Federal do ABC, CEP 09.210-170, Rua Santa Adelia 166, Bairro Bangu, Santo Andre, SP (Brazil); Bulhoes, L.O.S. [Laboratorio Interdisciplinar de Eletroquimica e Ceramica, Centro Multidisciplinar para o Desenvolvimento de Materiais Ceramicos, Departamento de Quimica, Universidade Federal de Sao Carlos, Caixa Postal 676, 13560-905 Sao Carlos, SP (Brazil); CENIP, Centro Universitario Central Paulista, UNICEP, Rua Miguel Petroni, 5111, CEP 13563-470, Sao Carlos, SP (Brazil); Santos, M.C. [Laboratorio Interdisciplinar de Eletroquimica e Ceramica, Centro Multidisciplinar para o Desenvolvimento de Materiais Ceramicos, Departamento de Quimica, Universidade Federal de Sao Carlos, Caixa Postal 676, 13560-905 Sao Carlos, SP (Brazil); LEMN, Laboratorio de Eletroquimica e Materiais Nanoestruturados, CCNH-Centro de Ciencias Naturais e Humanas, UFABC-Universidade Federal do ABC, CEP 09.210-170, Rua Santa Adelia 166, Bairro Bangu, Santo Andre, SP (Brazil)

2007-09-27

In this work, ruthenium oxide films containing platinum nanoparticles were prepared using the polymeric precursor method on Ti substrates with several molar ratios. This paper aims at presenting the characterization of the Pt content effect in the methanol electrochemical oxidation reaction. The films were physically characterized using X-ray diffraction and both Pt and RuO{sub 2} (rutile) phases were observed. The mean crystallite sizes were 6 nm for Pt and 25 nm for RuO{sub 2}. The X-ray photoelectronic results indicated that on the electrodes surfaces, depending on the substrate, there was RuO{sub 2}, Ru metal and Pt metal. Besides, it was not observed the formation of PtRu alloys. The atomic force microscopy images of the films showed highly rough surfaces. A decrease in the roughness mean square values is observed as the Pt content increases. These last results are similar to electroactive surface area values calculated by redox-couple (K{sub 4}FeCN{sub 6}/K{sub 3}FeCN{sub 6}). There was an increase in the globular size observed on the electrode surface and lower particle dispersion as the Pt content is increased from 12.5 to 75 mol%. Regarding the eletrode electrocatalytical behavior for methanol oxidation, it was observed that the onset oxidation overpotential is displaced towards more negative values as Pt content is decreased. Besides, an increase has been shown in the current density for methanol oxidation of 600% using a Ti/RuO{sub 2}-Pt (87.5:12.5) electrode compared to polycrystalline Pt. (author)

Preparation of ternary Pt/Rh/SnO2 anode catalysts for use in direct ethanol fuel cells and their electrocatalytic activity for ethanol oxidation reaction

Science.gov (United States)

Higuchi, Eiji; Takase, Tomonori; Chiku, Masanobu; Inoue, Hiroshi

2014-10-01

Pt, Rh and SnO2 nanoparticle-loaded carbon black (Pt/Rh/SnO2/CB) catalysts with different contents of Pt and Rh were prepared by the modified Bönnemann method. The mean size and size distribution of Pt, Rh and SnO2 for Pt-71/Rh-4/SnO2/CB (Pt : Rh : Sn = 71 at.%: 4 at.%: 25 at.%) were 3.8 ± 0.7, 3.2 ± 0.7 and 2.6 ± 0.5 nm, respectively, indicating that Pt, Rh and SnO2 were all nanoparticles. The onset potential of ethanol oxidation current for the Pt-65/Rh-10/SnO2/CB and Pt-56/Rh-19/SnO2/CB electrodes was ca. 0.2 V vs. RHE which was ca. 0.2 V less positive than that for the Pt/CB electrode. The oxidation current at 0.6 V for the Pt/Rh/SnO2/CB electrode (ca. 2% h-1) decayed more slowly than that at the Pt/SnO2/CB electrode (ca. 5% h-1), indicating that the former was superior in durability to the latter. The main product of EOR in potentiostatic electrolysis at 0.6 V for the Pt-71/Rh-4/SnO2/CB electrode was acetic acid.

A general approach for the synthesis of bimetallic M–Sn (M = Ru, Rh and Ir) catalysts for efficient hydrogenolysis of ester

KAUST Repository

Samal, Akshaya Kumar

2016-11-24

A versatile synthetic method was applied for the preparation of Sn containing bimetallic catalysts. The synthesis was performed by simply mixing the super hydride [LiB(C2H5)(3)H], with a metal (Ru, Rh or Ir) salt and an organotin complex in tetrahydrofuran solvent without using any surfactant. This leads to the formation of monodispersed M-Sn (M = Ru, Rh or Ir) bimetallic nanoparticles (NPs). These bimetallic catalysts show high performances in the hydrogenolysis of ester to the corresponding alcohol.

Magnetic properties and configuration of Fe{sub 50}Pt{sub 50*x}Rh{sub x} films

Energy Technology Data Exchange (ETDEWEB)

Fenske, Jochen; Lott, Dieter; Schreyer, Andreas [Helmholt-Zentrum, Geesthacht (Germany); Schmidt, Wolfgang; Schmalzl, Karin [IFF Forschungszentrum, Juelich (Germany); JCNS at ILL (France); Mankey, Gary J. [MINT Center, University of Alabama (United States); Klose, Frank [Ansto, Bragg Institute (Australia); Tartakowskaya, Helena [Institute for Magnetism, National Accademy of Scinece (Ukraine)

2011-07-01

Ordered FePt alloys with L1{sub 0} structure are known as materials with FM order and a high magnetic moment of Fe providing a large magnetization. The large atomic number of Pt on the other hand results in a high magnetic anisotropy. If grown in thin films, the high anisotropy often results in perpendicular magnetization which is the preferred orientation for current magnetic recording media. One way to control the magnetic properties in these materials is through the introduction of a third element into the crystal matrix e.g. Rh. When Rh is added to replace Pt in the equiatomic alloy, new magnetic phases emerge. Here we present neutron diffraction studies on the magnetic properties of different 200nm thick Fe{sub 50}Pt{sub 50*x}Rh{sub x} films in dependence of the temperature and external magnetic fields. Additional resonant x-ray measurements on the Fe and Pt absorption edges provide additional information about the magnetic moments on these sites.

Influence of alcohol additives in the preparation of electrodeposited Pt-Ru catalysts on oxidized graphite cloths

International Nuclear Information System (INIS)

Sieben, Juan Manuel; Duarte, Marta M.E.; Mayer, Carlos E.

2011-01-01

Research highlights: → Pt-Ru catalysts were prepared by potential pulse electrodeposition from solutions containing EtOH or EG at pH 2 and 5. → The catalyst particle size, loading and dispersion were influenced by solution pH and alcohol addition. → The deposits prepared at pH 2 exhibited large irregular agglomerates while those prepared at pH 5 presented smaller globular particles. → Pt-Ru system prepared using EG at pH 5 exhibited the best performance for CH 3 OH oxidation. - Abstract: Carbon supported Pt-Ru catalysts were prepared by multiple cycles of potentiostatic pulses from aqueous diluted chloroplatinic acid and ruthenium chloride solutions in the presence of ethanol or ethylene glycol at pH 2 and 5. SEM images showed that the metallic deposit prepared at pH 2 consisted of large irregular agglomerates, whereas smaller globular particles were obtained at pH 5. In addition, the average particle size was considerably decreased in the presence of the stabilizers. The supported Pt-Ru alloys were tested as catalysts for methanol electro-oxidation in acid media. Electrocatalytic activity measurements indicated that the most active electrode was obtained with ethylene glycol as additive at pH 5.

Surface and electrochemical characterization of electrodeposited PtRu alloys

Science.gov (United States)

Richarz, Frank; Wohlmann, Bernd; Vogel, Ulrich; Hoffschulz, Henning; Wandelt, Klaus

1995-07-01

PtRu alloys of different compositions were electrodeposited on Au. Twelve alloys between 0% and 100% Pt were characterized with surface sensitive spectroscopies (XPS, LEIS) after transfer from an electrochemical cell to an ultra high vaccum chamber without contact to air. The composition of the thus prepared alloys showed a linear dependence on the concentrations of the deposition solution, but was Pt-enriched both in the bulk and (even more so) at the surface. During the electrochemical reduction of the metal cations, sulfur from the supporting electrolyte 1N H 2SO 4 was found to be incorporated into the electrodes. Cyclic voltammetry was used for the determination of the electrocatalytic activity of the electrodes for the oxidation of carbon monoxide. The highest activity for this oxidation as measured by the (peak) potential of the CO oxidation cyclovoltammograms was found for a surface concentration of ˜ 50%Pt. The asymmetry of this "activity curve" (oxidation potential versus Pt surface concentration) is tentatively explained in terms of a surface structural phase separation.

Quaternary Pt{sub 2}Ru{sub 1}Fe{sub 1}M{sub 1}/C (M=Ni, Mo, or W) catalysts for methanol electro-oxidation reaction

Energy Technology Data Exchange (ETDEWEB)

Jeon, Min Ku; Lee, Ki Rak; Kang, Kweon Ho; Park, Geun Il [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Jeon, Hyung Joon [Kyoto University, Kyoto (Japan); McGinn, Paul J. [University of Notre Dame, Indiana (United States)

2015-02-15

Quaternary Pt{sub 2}Ru{sub 1}Fe{sub 1}M{sub 1}/C (M=Ni, Mo, or W) catalysts were investigated for the methanol electro-oxidation reaction (MOR). Electrocatalytic activities of the quaternary catalysts for CO electro-oxidation were studied via CO stripping experiments, and the Pt{sub 2}Ru{sub 1}Fe{sub 1}Ni{sub 1}/C and Pt{sub 2}Ru{sub 1}Fe{sub 1}W{sub 1}/C catalysts exhibited lowered on-set potential compared to that of a commercial PtRu/C catalyst. MOR activities of the quaternary catalysts were determined by linear sweep voltammetry (LSV) experiments, and the Pt{sub 2}Ru{sub 1}Fe{sub 1}W{sub 1}/C catalyst outperformed the commercial PtRu/C catalyst by 170 and 150% for the mass and specific activities, respectively. X-ray photoelectron spectroscopy (XPS) was employed to analyze surface oxidation states of constituent atoms, and it was identified that the structure of the synthesized catalysts are close to a nano-composite of Pt and constituent metal hydroxides and oxides. In addition, the XPS results suggested that the bi-functional mechanism accounts for the improved performance of the Pt{sub 2}Ru{sub 1}Fe{sub 1}Ni{sub 1}/C and Pt{sub 2}Ru{sub 1} Fe{sub 1}W{sub 1}/C catalysts.

Electrical enhancement of direct methanol fuel cells by metal-plasma ion implantation Pt-Ru/C multilayer catalysts.

Science.gov (United States)

Weng, Ko-Wei; Chen, Yung-Lin; Chen, Ya-Chi; Lin, Tai-Nan

2009-02-01

Direct methanol fuel cells (DMFC) have been widely studied owing to their simple cell configuration, high volume energy density, short start-up time, high operational reliability and other favorable characteristics. However, major limitations include high production cost, poisoning of the catalyst and methanol crossover. This study adopts a simple technique for preparing Pt-Ru/C multilayer catalysts, including magnetron sputtering (MS) and metal-plasma ion implantation (MPII). The Pt catalysts were sputtered onto the gas diffusion layer (GDL), followed by the implantation of Ru catalysts using MPII (at an accelerating voltage of 20 kV and an implantation dose of 1 x 10(16) ions/cm2). Pt-Ru is repeatedly processed to prepare Pt-Ru/C multilayer catalysts. The catalyst film structure and microstructure were analyzed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electronic microscopy (SEM), respectively. The cell performance was tested using a potential stat/galvano-stat. The results reveal that the membrane electrode assembly (MEA) of four multilayer structures enhances the cell performance of DMFC. The measured power density is 2.2 mW/cm2 at a methanol concentration of 2 M, with an OCV of 0.493 V.

In Situ Synthesis and Characterization of Polyethyleneimine-Modified Carbon Nanotubes Supported PtRu Electrocatalyst for Methanol Oxidation

Directory of Open Access Journals (Sweden)

Xi Geng

2015-01-01

Full Text Available PtRu bimetallic nanoparticles were successfully synthesized on polyethyleneimine- (PEI- functionalized multiwalled carbon nanotubes (MWCNTs via an effective and facile polyol reduction approach. Noncovalent surface modification of MWCNTs with PEI was confirmed by FTIR and zeta potential measurements. The morphology, crystalline structure, and composition of the hybrid material were characterized by transmission electron microscopy (TEM, scanning electron microscopy (SEM, X-ray powder diffraction (XRD, and energy dispersive X-ray spectroscopy (EDX, respectively. According to SEM and TEM observations, PtRu nanoparticles with narrow size distribution were homogeneously deposited on PEI-MWCNTs. Cyclic voltammetry tests demonstrated that the as-prepared PtRu/PEI-MWCNTs nanocomposite had a large electrochemical surface area and exhibited enhanced electrocatalytic activity towards methanol oxidation in comparison with oxidized MWCNTs as catalyst support. PEI-functionalized CNTs, as useful building blocks for the assembly of Pt-based electrocatalyst, may have great potential for applications such as direct methanol fuel cell (DMFC.

Analysis of the kinetics of methanol oxidation in a porous Pt-Ru anode

Energy Technology Data Exchange (ETDEWEB)

Sun, Yan-Ping; Xing, Lei [Chemical Engineering Department, Taiyuan University of Technology, Shanxi 030024 (China); Scott, Keith [School of Chemical Engineering and Advanced Materials, Merz Court, University of Newcastle, Newcastle upon Tyne NE1 7RU (United Kingdom)

2010-01-01

A kinetic model of a porous Pt-Ru anode for methanol oxidation is presented. It was based on the dual-site mechanism for methanol oxidation and used to predict anode performance and the influence of species adsorption on the overall oxidation (macro-) kinetics. The performance of the porous Pt-Ru anode depended on the parameters of the intrinsic chemical kinetics of methanol oxidation and physical parameters such as electrode thickness, surface area, effective diffusion and charge transfer coefficients and concentration of methanol and temperature. The model was solved by using the finite difference method with a subroutine for solving a set of nonlinear algebraic equations in each step. Surface coverage ratio distributions of adsorbed species, effectiveness of the porous electrode and macro-polarisation curves were obtained. The simulated polarisation curves were compared to experimental polarisation data for methanol oxidation on Pt-Ru porous anodes at different temperatures and methanol concentrations. The intrinsic kinetic parameters were regressed from the corresponding experimental data. The predicted polarisation curves calculated by the model, were consistent with experimental polarisation data at lower current densities. The departure of experimental data from the predicted polarisation curves at high concentration and high apparent current densities was believed to be due to two-phase flow in the electrode. (author)

The kinetics and mechanism of methanol oxidation on Pt and PtRu catalysts in alkaline and acid media

Directory of Open Access Journals (Sweden)

JELENA LOVIC

2007-07-01

Full Text Available The kinetic of methanol electrochemical oxidation for a series of platinum and platinum–ruthenium catalysts was investigated. A correlation between the beginning of OHad adsorption and methanol oxidation was demonstarated on Pt single crystals and Pt nanocatalyst. The activity of the nano-structured Pt catalyst was compared with single crystal platinum electrodes assuming the Kinoshita model of nanoparticles. The ruthenium-containing catalysts shifted the onset of methanol oxidation to more negative potentials. The effect was more pronounced in acid than in alkaline media. Based on the established diagnostic criteria, the reaction between COad and OHad species according to the Langmuir–Hinshelwood mechanism was proposed as the rate determining step in alkaline and acid media on Pt and PtRu catalysts.

Novel Pt-Ru nanoparticles formed by vapour deposition as efficient electrocatalyst for methanol oxidation

International Nuclear Information System (INIS)

Sivakumar, Pasupathi; Ishak, Randa; Tricoli, Vincenzo

2005-01-01

Bimetallic Pt-Ru nanoparticles supported on carbon substrates have been prepared reproducibly by a simple method that utilizes commercially available metal-organic precursors at low temperature in vacuum. Particles morphology, composition and structure have been investigated using HRTEM, EDX, selected area electron diffraction (SAED) and powder XRD analysis. TEM shows that the obtained nanoparticles are homogeneously dispersed on the substrate surface and exhibit narrow size distribution, the average diameter being ca. 2 nm. Point resolved EDX analysis demonstrates co-presence of both Pt and Ru in each particle, thereby indicating that truly bimetallic nanoparticles have been obtained. Moreover, EDX performed on several areas of the sample evidences uniform particles composition. The latter can be controlled very easily and effectively by regulating the operation temperature during particles preparation. HRTEM imaging shows that the particles possess crystalline structure. Both SAED and XRD analyses indicate presence of nanoparticles exhibiting structure consistent with that of an f.c.c. Pt-Ru alloy. Besides the f.c.c. alloy, an additional crystalline phase might also be present as noticed by SAED. These nanoparticles display electrocatalytic activity with regard to methanol oxidation as evidenced by cyclic voltammetry (CV)

Barrier characteristics of Pt/Ru Schottky contacts on n-type GaN ...

Indian Academy of Sciences (India)

Pt/Ru Schottky rectifiers; n-type GaN; temperature–dependent electrical properties; inhomogeneous barrier heights .... a 2 μm thick Si-doped GaN films which were grown by .... ted values of ap using (9) for two Gaussian distributions of bar-.

Pt-Ni and Pt-M-Ni (M = Ru, Sn Anode Catalysts for Low-Temperature Acidic Direct Alcohol Fuel Cells: A Review

Directory of Open Access Journals (Sweden)

Ermete Antolini

2017-01-01

Full Text Available In view of a possible use as anode materials in acidic direct alcohol fuel cells, the electro-catalytic activity of Pt-Ni and Pt-M-Ni (M = Ru, Sn catalysts for methanol and ethanol oxidation has been widely investigated. An overview of literature data regarding the effect of the addition of Ni to Pt and Pt-M on the methanol and ethanol oxidation activity in acid environment of the resulting binary and ternary Ni-containing Pt-based catalysts is presented, highlighting the effect of alloyed and non-alloyed nickel on the catalytic activity of these materials.

Ru-decorated Pt nanoparticles on N-doped multi-walled carbon nanotubes by atomic layer deposition for direct methanol fuel cells

DEFF Research Database (Denmark)

Johansson, Anne-Charlotte Elisabeth Birgitta; Yang, R.B.; Haugshøj, K.B.

2013-01-01

We present atomic layer deposition (ALD) as a new method for the preparation of highly dispersed Ru-decorated Pt nanoparticles for use as catalyst in direct methanol fuel cells (DMFCs). The nanoparticles were deposited onto N-doped multi-walled carbon nanotubes (MWCNTs) at 250 °C using trimethyl......(methylcyclopentadienyl)platinum MeCpPtMe3, bis(ethylcyclopentadienyl)ruthenium Ru(EtCp)2 and O2 as the precursors. Catalysts with 5, 10 and 20 ALD Ru cycles grown onto the CNT-supported ALD Pt nanoparticles (150 cycles) were prepared and tested towards the electro-oxidation of CO and methanol, using cyclic voltammetry...... and chronoamperometry in a three-electrode electrochemical set-up. The catalyst decorated with 5 ALD Ru cycles was of highest activity in both reactions, followed by the ones with 10 and 20 ALD Ru cycles. It is demonstrated that ALD is a promising technique in the field of catalysis as highly dispersed nanoparticles...

Preparation and characterization of Pt Sn / C-rare earth and PtRu / C-rare earth using an alcohol reduction process for ethanol electron-oxidation

International Nuclear Information System (INIS)

Rodrigues, Rita Maria de Sousa

2011-01-01

The electro catalyst PtRu / C-rare earth and PtSn/C-rare earth (20 wt%) were prepared by alcohol reduction method using H 2 PtCl 6 .6H 2 O Ru Cl xH 2 O, SnCl 2 .2H 2 O as a source of metals 85 % Vulcan - 15 % rare earth as a support and, finally, ethylene glycol as reducing agent. The electrocatalysts were characterized physically by X-ray diffraction (XRD), energy dispersive X-ray (EDX), and transmission electron microscopy (TEM). Analyses by EDX showed that the atomic ratios of different electrocatalysts, prepared by alcohol reduction method are similar to the nominal starting compositions indicating that this methodology is promising for the preparation of electrocatalysts. In all the XRD patterns for the prepared electrocatalysts there is a broad peak at about 2θ = 25 o , which is associated with the carbon support and four additional diffraction peaks at approximately 2θ = 40 o , 47 o , 67 o e 82 o , which in turn are associated with the plans (111), (200), (220) e (311), respectively, of face-centered cubic structure (FCC) platinum. The results of X-ray diffraction also showed average crystallite sizes between 2.0 and 4.0 nm for PtSn e 2,0 a 3,0 para PtRu. The studies for the electrochemical oxidation of ethanol in acid medium were carried out using the technique of chronoamperometry in a solution 0,5 mol.L-1 H 2 SO 4 , + 1,0 mol.L-1 de C 2 H 5 OH. The polarization curves obtained in the fuel cell unit, powered directly by ethanol, are in agreement with the results of voltammetry and chronoamperometry noting the beneficial effect of rare earths in the preparation of electrocatalysts and attesting that the electrocatalysts PtSn/C are more effective than PtRu/C for the oxidation of ethanol.

Electrochemical promotion of catalytic reactions with Pt/C (or Pt/Ru/C)//PBI catalysts

DEFF Research Database (Denmark)

Petrushina, Irina; Bjerrum, Niels; Bandur, Viktor

2007-01-01

The paper is an overview of the results of the investigation on electrochemical promotion of three catalytic reactions: methane oxidation with oxygen, NO reduction with hydrogen at 135 degrees C and Fischer-Tropsch synthesis (FTS) at 170 degrees C in the [CH4/O-2(or NO/H-2 or CO/H-2)/Ar//Pt(or Pt....../Ru)//PBI(H3PO4)/H-2, Ar] fuel cell. It has been shown that the partial methane oxidation to C2H2 and the C-2 selectivity were electrochemically promoted by the negative catalyst polarization. This was also the case in NO reduction with hydrogen for low NO and H-2 partial pressures. In both cases the catalytic...... reactions have been promoted by the electrochemically produced hydrogen. It has been found that the NO reduction with hydrogen on the Pt/PBI strongly depends on NO and hydrogen partial pressures in the working gas mixture. At higher NO and H-2 partial pressures the catalysis is promoted...

Epitaxial growth of unusual 4H hexagonal Ir, Rh, Os, Ru and Cu nanostructures on 4H Au nanoribbons

KAUST Repository

Fan, Zhanxi; Chen, Ye; Zhu, Yihan; Wang, Jie; Li, Bing; Zong, Yun; Han, Yu; Zhang, Hua

2016-01-01

Metal nanomaterials normally adopt the same crystal structure as their bulk counterparts. Herein, for the first time, the unusual 4H hexagonal Ir, Rh, Os, Ru and Cu nanostructures have been synthesized on 4H Au nanoribbons (NRBs) via solution-phase epitaxial growth under ambient conditions. Interestingly, the 4H Au NRBs undergo partial phase transformation from 4H to face-centered cubic (fcc) structures after the metal coating. As a result, a series of polytypic 4H/fcc bimetallic Au@M (M = Ir, Rh, Os, Ru and Cu) core-shell NRBs has been obtained. We believe that the rational crystal structure-controlled synthesis of metal nanomaterials will bring new opportunities for exploring their phase-dependent physicochemical properties and promising applications.

Epitaxial growth of unusual 4H hexagonal Ir, Rh, Os, Ru and Cu nanostructures on 4H Au nanoribbons

KAUST Repository

Fan, Zhanxi

2016-09-12

Metal nanomaterials normally adopt the same crystal structure as their bulk counterparts. Herein, for the first time, the unusual 4H hexagonal Ir, Rh, Os, Ru and Cu nanostructures have been synthesized on 4H Au nanoribbons (NRBs) via solution-phase epitaxial growth under ambient conditions. Interestingly, the 4H Au NRBs undergo partial phase transformation from 4H to face-centered cubic (fcc) structures after the metal coating. As a result, a series of polytypic 4H/fcc bimetallic Au@M (M = Ir, Rh, Os, Ru and Cu) core-shell NRBs has been obtained. We believe that the rational crystal structure-controlled synthesis of metal nanomaterials will bring new opportunities for exploring their phase-dependent physicochemical properties and promising applications.

Ionic Liquid Gating Control of RKKY Interaction in FeCoB/Ru/FeCoB and (Pt/Co)₂/Ru/(Co/Pt)₂ Multilayers.

Energy Technology Data Exchange (ETDEWEB)

Yang, Qu; Wang, Lei; Zhou, Ziyao; Wang, Liqian; Zhang, Yijun; Zhao, Shishun; Dong, Guohua; Cheng, Yuxin; Min, Tai; Hu, Zhongqiang; Chen, Wei; Xia, Ke; Liu, Ming

2018-03-07

To overcome the fundamental challenge of the weak natural response of antiferromagnetic materials under a magnetic field, voltage manipulation of antiferromagnetic interaction is developed to realize ultrafast, high-density, and power efficient antiferromagnetic spintronics. Here, we report a low voltage modulation of Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction via ionic liquid gating in synthetic antiferromagnetic multilayers of FeCoB/Ru/FeCoB and (Pt/Co)₂/Ru/(Co/Pt)₂. At room temperature, the distinct voltage control of transition between antiferromagnetic and ferromagnetic ordering is realized and up to 80% of perpendicular magnetic moments manage to switch with a small-applied voltage bias of 2.5 V. We related this ionic liquid gating-induced RKKY interaction modification to the disturbance of itinerant electrons inside synthetic antiferromagnetic heterostructure and the corresponding change of its Fermi level. Voltage tuning of RKKY interaction may enable the next generation of switchable spintronics between antiferromagnetic and ferromagnetic modes with both fundamental and practical perspectives.

Pulse electrodeposition of Pt and Pt–Ru methanol-oxidation nanocatalysts onto carbon nanotubes in citric acid aqueous solutions

Energy Technology Data Exchange (ETDEWEB)

Chou, Huei-Yu [Department of Engineering and System Science, National Tsing Hua University, Hsinchu 30013, Taiwan, ROC (China); Hsieh, Chien-Kuo [Department of Materials Engineering, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC (China); Tsai, Ming-Chi; Wei, Yu-Hsuan; Yeh, Tsung-Kuang [Department of Engineering and System Science, National Tsing Hua University, Hsinchu 30013, Taiwan, ROC (China); Tsai, Chuen-Horng, E-mail: tsai@aec.gov.tw [Department of Engineering and System Science, National Tsing Hua University, Hsinchu 30013, Taiwan, ROC (China)

2015-06-01

In this study, platinum nanoparticle/carbon nanotube (Pt NP/CNT) and platinum–ruthenium nanoparticle (Pt–Ru NP/CNT) hybrid nanocatalysts were prepared by the pulse-electrodeposition method in different aqueous solutions containing citric acid (CA) or sulfuric acid (SA). The electrocatalytic properties of the Pt NP/CNT and Pt–Ru NP/CNT electrodes prepared using different aqueous solutions were investigated for methanol oxidation. The results show that the electrochemical mass activities of these hybrid nanocatalysts prepared in the CA aqueous solution were increased by factors of 1.46 and 2.77 for Pt NPs and Pt–Ru NPs, respectively, compared with those prepared in SA aqueous solutions using the same procedure. These increased mass activities are attributed to the CA playing dual roles as both a stabilizing agent and a particle size reducing agent in the aqueous solutions. The approach developed in this work enables further reductions in the particle sizes of noble-metal nanocatalysts. - Highlights: • Pulse-electrodeposition of Pt or Pt–Ru nanoparticles on carbon nanotubes • Carbon nanotubes used as a catalyst-supporting material • Citric acid used as reducing agent in the aqueous electrodeposition solutions • Electrochemical activity for methanol oxidation improved by a factor of 1.46 to 2.77.

Improved reaction kinetics and selectivity by the TiO2-embedded carbon nanofiber support for electro-oxidation of ethanol on PtRu nanoparticles

Science.gov (United States)

Nakagawa, Nobuyoshi; Ito, Yudai; Tsujiguchi, Takuya; Ishitobi, Hirokazu

2014-02-01

The electro-oxidation of ethanol by the catalyst of PtRu nanoparticles supported on a TiO2-embedded carbon nanofiber (PtRu/TECNF), which has recently been proposed by the authors as a highly active catalyst for methanol oxidation, is investigated by cyclic voltammetry using a glassy carbon electrode and by operating a direct ethanol fuel cell (DEFC) with the catalyst. The mass activity obtained from the cyclic voltammogram for the ethanol oxidation is compared to that for the methanol oxidation reported in our recent paper. The mass activity for the ethanol oxidation is comparable or slightly higher than that for the methanol oxidation, and the relationship between the TECNF composition, i.e., the Ti/C mass ratio, and the activity are also similar to that for the methanol oxidation. A DEFC fabricated with the PtRu/TECNF shows a higher power output compared to that with the commercial PtRu/C catalyst. An analysis of the reaction products by a simple two-step reaction model reveals that the PtRu/TECNF increases the rate constant for the reaction steps from ethanol to acetaldehyde and subsequently to CO2, but decreases that from acetaldehyde to acetic acid. This means that the PtRu/TECNF improves not only the kinetics, but also the selectivity to acetaldehyde.

Heat flux measurements of Tb{sub 3}M series (M=Co, Rh and Ru): Specific heat and magnetocaloric properties

Energy Technology Data Exchange (ETDEWEB)

Monteiro, J.C.B., E-mail: jolmiui@gmail.com [Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin, Campinas, SP 13083-859 (Brazil); Lombardi, G.A. [Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin, Campinas, SP 13083-859 (Brazil); Reis, R.D. dos [Max-Planck Institute for Chemical Physics of Solids, Nöthnitzer Str. 40, 01187 Dresden (Germany); Freitas, H.E.; Cardoso, L.P.; Mansanares, A.M.; Gandra, F.G. [Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin, Campinas, SP 13083-859 (Brazil)

2016-12-15

We report on the magnetic properties and magnetocaloric effect (MCE) for the Tb{sub 3}M series, with M=Co, Rh and Ru, obtained using a heat flux technique. The specific heat of Tb{sub 3}Co and Tb{sub 3}Rh are very similar, with a first order type transition occurring around 6 K below the magnetic ordering temperature without any corresponding feature on the magnetization. The slightly enhanced electronic specific heat, the Debye temperature around 150 K and the presence of the magnetic specific heat well above the ordering temperature are also characteristic of many other compounds of the R{sub 3}M family (R=Rare Earth). The specific heat for Tb{sub 3}Ru, however, presents two peaks at 37 K and 74 K. The magnetization shows that below the first peak the system presents an antiferromagnetic behavior and is paramagnetic above 74 K. We obtained a magnetocaloric effect for M=Co and Rh, −∆S=12 J/kg K, but for Tb{sub 3}Ru it is less than 3 J/kg K (μ{sub 0}∆H=5 T). We believe that the experimental results show that the MCE is directly related with the process of hybridization of the (R)5d-(M)d electrons that occurs in the R{sub 3}M materials.

Electrodeposition of mesoscopic Pt-Ru on reticulated vitreous carbon from reverse emulsions and microemulsions: Application to methanol electro-oxidation

International Nuclear Information System (INIS)

Cheng, Tommy T.; Gyenge, Elod L.

2006-01-01

High surface area Pt-Ru (between 120 and 400 cm 2 mg -1 ) meso-sized particles and mesoporous coatings were electrodeposited on reticulated vitreous carbon (RVC) three-dimensional electrodes using reverse emulsions and microemulsions. The organic phase of the colloidal media was composed of cyclohexane, Triton X-100 non-ionic surfactant and tetrabutylammonium perchlorate (for ionic conductivity) while the aqueous phase contained H 2 PtCl 6 and RuCl 3 (or (NH 4 ) 2 RuCl 6 ). For microemulsification to occur isopropanol was also added as co-surfactant. The catalytic activity for the electro-oxidation of methanol was assessed by cyclic voltammetry and chronopotentiometry in conjunction with surface area measurement by Cu underpotential deposition. The composition and morphology of the Pt-Ru deposit was analyzed by inductively coupled plasma atomic emission spectroscopy and scanning electron microscopy, respectively. The effects on the catalytic activity of the deposition current density, temperature, RVC pretreatment and plating bath composition are presented. It was found that the electrodeposition of Pt-Ru in reverse microemulsion yielded the highest specific surface area (400 cm 2 mg -1 ) and catalytic activity toward CH 3 OH electro-oxidation as shown, for example, by a 50-200 mV more negative anode potential determined by chronopotentiometry compared to a catalyst obtained by pure aqueous and emulsion electroplating

Electrodeposition of mesoscopic Pt-Ru on reticulated vitreous carbon from reverse emulsions and microemulsions: Application to methanol electro-oxidation

Energy Technology Data Exchange (ETDEWEB)

Cheng, Tommy T. [2360 East Mall, Department of Chemical and Biological Engineering, University of British Columbia, Vancouver, BC, V6T 1Z3 (Canada); Gyenge, Elod L. [2360 East Mall, Department of Chemical and Biological Engineering, University of British Columbia, Vancouver, BC, V6T 1Z3 (Canada)]. E-mail: egyenge@chml.ubc.ca

2006-05-20

High surface area Pt-Ru (between 120 and 400 cm{sup 2} mg{sup -1}) meso-sized particles and mesoporous coatings were electrodeposited on reticulated vitreous carbon (RVC) three-dimensional electrodes using reverse emulsions and microemulsions. The organic phase of the colloidal media was composed of cyclohexane, Triton X-100 non-ionic surfactant and tetrabutylammonium perchlorate (for ionic conductivity) while the aqueous phase contained H{sub 2}PtCl{sub 6} and RuCl{sub 3} (or (NH{sub 4}){sub 2}RuCl{sub 6}). For microemulsification to occur isopropanol was also added as co-surfactant. The catalytic activity for the electro-oxidation of methanol was assessed by cyclic voltammetry and chronopotentiometry in conjunction with surface area measurement by Cu underpotential deposition. The composition and morphology of the Pt-Ru deposit was analyzed by inductively coupled plasma atomic emission spectroscopy and scanning electron microscopy, respectively. The effects on the catalytic activity of the deposition current density, temperature, RVC pretreatment and plating bath composition are presented. It was found that the electrodeposition of Pt-Ru in reverse microemulsion yielded the highest specific surface area (400 cm{sup 2} mg{sup -1}) and catalytic activity toward CH{sub 3}OH electro-oxidation as shown, for example, by a 50-200 mV more negative anode potential determined by chronopotentiometry compared to a catalyst obtained by pure aqueous and emulsion electroplating.

Revisiting anomalous B(E2;41+→21+)/B(E2;21+→01+) values in 98Ru and 180Pt

International Nuclear Information System (INIS)

Williams, E.; Plettner, C.; McCutchan, E. A.; Levine, H.; Casten, R. F.; Ai, H.; Heinz, A.; Qian, J.; Meyer, D. A.; Werner, V.; Zamfir, N. V.; Cakirli, R. B.; Beausang, C. W.; Guerdal, G.; Pietralla, N.

2006-01-01

Recently, a set of nine nonmagic nuclei with anomalous values of the B(E2) ratio B 4/2 ≡B(E2;4 1 + →2 1 + )/B(E2;2 1 + →0 1 + ) 1 + →2 1 + ) values for two of these nuclei, 98 Ru and 180 Pt, were re-measured to determine if the current literature values for these nuclei are correct. 98 Ru was studied in a 27 Al( 98 Ru, 98 Ru*) Coulomb excitation experiment in inverse kinematics, while the lifetime of the 4 1 + state in 180 Pt was measured in a 122 Sn( 62 Ni, 4n) 180 Pt recoil distance method (RDM) experiment. For both nuclei, the remeasured B 4/2 values are well above 1, removing the deviations from collective models

Synergistic effects for the TiO2/RuO2/Pt photodissociation of water

Energy Technology Data Exchange (ETDEWEB)

Blondel, G; Harriman, A; Williams, D

1983-07-01

Compressed discs of naked TiO2 or TiO2 coated with a thin film of a noble metal (e.g. Pt) do not photodissociate water upon illumination with UV light, but small amounts of H2 are generated if the TiO2 has been reduced in a stream of H2 at 600 C. Discs prepared from mixtures of TiO2/RuO2 facilitate the UV photodissociation of water into H2 and O2 although the yields are very low. When a thin (about 9 nm) film of Pt is applied to the TiO2/RuO2 discs, the yields of H2 and O2 observed upon irradiation with UV light are improved drastically. 25 references.

Tetrapropylammonium ion influence on the synthesis of Pt Ru/carbon hybrids by hydrothermal carbonization

International Nuclear Information System (INIS)

Tusi, M.M.; Polanco, N.S.O.; Brandalise, M.; Correa, O.V.; Silva, A.C.; Oliveira Neto, A.; Linardi, M.; Spinace, E.V.

2010-01-01

PtRu/Carbon hybrid materials were prepared by hydrothermal carbonization using starch as carbon source and reducing agent and H 2 PtCl 6 .6H 2 O e RuCl 3 .xH 2 O as metals source and catalyst of the carbonization process. The materials were prepared in the following conditions: without pH adjustment, in the absence and in the presence of tetrapropylammonium chloride (TPACl), and adjusting the pH using potassium hydroxide (KOH) or tetrapropylammonium hydroxide (TPAOH). The obtained materials were treated under argon atmosphere at 900 deg C and characterized by SEM/EDX, BET isotherm, XRD and TEM. The electro-oxidation of methanol was studied by chronoamperometry. The material prepared using TPAOH showed the best performance for methanol electro-oxidation. (author)

Energy deposition by a 106Ru/106Rh eye applicator simulated using LEPTS, a low-energy particle track simulation

International Nuclear Information System (INIS)

Fuss, M.C.; Munoz, A.; Oller, J.C.; Blanco, F.; Williart, A.; Limao-Vieira, P.; Borge, M.J.G.; Tengblad, O.; Huerga, C.; Tellez, M.; Garcia, G.

2011-01-01

The present study introduces LEPTS, an event-by-event Monte Carlo programme, for simulating an ophthalmic 106 Ru/ 106 Rh applicator relevant in brachytherapy of ocular tumours. The distinctive characteristics of this code are the underlying radiation-matter interaction models that distinguish elastic and several kinds of inelastic collisions, as well as the use of mostly experimental input data. Special emphasis is placed on the treatment of low-energy electrons for generally being responsible for the deposition of a large portion of the total energy imparted to matter. - Highlights: → We present the Monte Carlo code LEPTS, a low-energy particle track simulation. → Carefully selected input data from 10 keV to 1 eV. → Application to an electron emitting Ru-106/Rh-106 plaque used in brachytherapy.

Incorporation of metals (Pt-Ni-Ru) in the zeolite ZSM-5 through ion exchange competitive: synthesis and characterization

International Nuclear Information System (INIS)

Barbosa, A.S.; Rodrigues, M.G.F.

2012-01-01

Zeolites are very important materials due to their high specific surface area. Moreover, they are suitable for use as catalyst support. Noble metals supported on zeolites have been widely used as catalysts in the petrochemical industry. This paper was prepared and characterized, a powder aiming its use in heterogeneous catalysis. Support was used as ZSM-5 and the method of incorporation of the metals (Ru-PtNi) was competitive ion exchange. The materials (ZSM-5 and Pt-Ni-Ru/ZSM-5) were characterized by spectrophotometry Energy Dispersive X-ray (EDX), X-Ray Diffraction (XRD) and nitrogen physisorption (BET method). Based on the results of X-ray diffraction, it is possible to demonstrate the preservation of the structure of zeolite ZSM-5 after the competitive ion Exchange with metals (Ru-Pt-Ni) and calcination. The dispersion of metals on ZSM-5 did not change the textural characteristics of the zeolite. (author)

Chemometric study of the effects of PtRu:BH4-molar ratio and solvent used in the preparation of PtRu/C electrocatalysts for for direct methanol fuel cell anodes

Energy Technology Data Exchange (ETDEWEB)

Polanco, N.S.O.; Neto, A.O.; Spinace, E.V. [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil); Tusi, M.M. [Universidade Regional Integrada do Alto Uruguai e das Missoes (URI), Santiago, RS (Brazil); Brandalise, M. [Instituto Federal Fluminense (IFF), Campos dos Goyracazes, RJ (Brazil)

2014-07-01

PtRu/C electrocatalysts were prepared by borohydride reduction method and a chemometric study was performed to evaluate the influence of the solvent (water and isopropyl alcohol) and amount of reducing agent (PtRu:BH4- molar ratios of 5 and 15) in maximum power density. In borohydride reduction method, a solution containing sodium hydroxide and sodium borohydride (NaBH4) is added to a mixture containing water, isopropyl alcohol, metallic precursors and the carbon support Vulcan XC72. The obtained materials were characterized by energy-dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD) and transmission electron microscopy (TEM). Membrane Electrode Assemblies (MEA's) were produced and tests in single direct methanol fuel cells were performed. The amount of sodium borohydride used in the reduction showed more influence on the maximum power density than the change of solvent of the reaction. (author)

Influence of method of preparation of Pt Ru/C electrocatalysts on the catalytic activity for the ethanol oxidation reaction in acidic medium; Influencia do metodo de preparacao de eletrocatalisadores PtRu/C sobre a atividade catalitica frente a reacao de oxidacao de etanol em meio acido

Energy Technology Data Exchange (ETDEWEB)

Gomes, Walber dos Santos; Silva, Uriel Lean Valente; Souza, Jose Pio Iudice de, E-mail: jpio@ufpa.br [Universidade Federal do Para, (UFPA), Belem, PA (Brazil). Instituto de Ciencias Exatas e Naturais. Faculdade de Quimica

2013-09-01

In this work the influence of variations in the borohydrate reduction method on the properties of Pt Ru/C electrocatalysts was investigated. The electrocatalysts were prepared using 1:1 ; 2:1; 5:1; 50:1 and 250:1 molar ratios of NaBH{sub 4} to metals. The reduction was also performed by dripping or by fast addition of the solution. The results showed that Pt Ru nanoparticles obtained by fast addition had the smallest crystallite sizes. It was also noted that the catalytic activity increased as the borohydrate:metal molar ratio increased. The Pt Ru/C electrocatalysts (50:1) obtained by fast addition presented the best catalytic activity for ethanol electro-oxidation. (author)

Electrodeposition of Pt-Ru nanoparticles on fibrous carbon substrates in the presence of nonionic surfactant: Application for methanol oxidation

International Nuclear Information System (INIS)

Bauer, Alex; Gyenge, Elod L.; Oloman, Colin W.

2006-01-01

Liquid crystalline and micellar aqueous solutions of the nonionic surfactant Triton X-100 were used to direct the electrodeposition of Pt-Ru nanoparticles onto graphite felts, which were investigated as novel anodes for the direct methanol fuel cell. The effects of surfactant concentration, current density and deposition time in the preparation of these three-dimensional electrodes were studied in a factorial experiment and the electrodes were characterized by SEM and ICP-AES. Cyclic voltammetry, chronoamperometry and chronopotentiometry were carried out to assess the activity of the catalyzed felts for methanol oxidation. The presence of Triton X-100 (40-60 wt.%) coupled with an acidic plating solution were essential for the efficient co-electrodeposition of Ru in the presence of Pt to yield approximately a 1:1 Pt:Ru atomic ratio in the deposit. The highest mass specific activity, 24 A g -1 at 298 K (determined by chronoamperometry after 180 s at 0 V versus Hg/Hg 2 SO 4 , K 2 SO 4std ), was obtained for the Pt-Ru electrodeposited in the presence of 40 wt.% Triton X-100 at 60 A m -2 , 298 K for 90 min. Surfactant mediated electrodeposition is a promising method for meso-scale (ca. 10-60 nm diameter) catalyst particle preparation on three-dimensional electrodes

Three dimensional PtRh alloy porous nanostructures: tuning the atomic composition and controlling the morphology for the application of direct methanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Zhang, Yuan [Department of Chemistry, Shanghai University, Shanghai 200444 (China); Department of Chemical Engineering, Case Western Reserve University, Cleveland, OH 44106 (United States); Janyasupab, Metini; Liu, Chung-Chiun [Department of Chemical Engineering, Case Western Reserve University, Cleveland, OH 44106 (United States); Liu, Chen-Wei [Institute of Material Sciences and Engineering, National Central University, Chung-Li 320 (China); Li, Xinxin [State Key Laboratory of Transducer Technology, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050 (China); Xu, Jiaqiang [Department of Chemistry, Shanghai University, Shanghai 200444 (China)

2012-09-11

A strategy for the synthesis of PtRh alloy 3D porous nanostructures by controlled aggregation of nanoparticles in oleylamine is presented. The atomic ratio between the two components (Pt and Rh) is tuned by varying the concentration of precursor salts accommodating the oxidation of methanol. The morphology of PtRh alloy nanostructure is controlled by elevating the temperature of the reaction system to 240 C. The prepared 3D porous nanostructures provide a high degree of electrochemical activity and good durability toward the methanol oxidation reaction compared to those of the commercial Pt/C (E-TEK) and PtRh nanoparticles. Therefore, the 3D alloy porous nanostructures provide a good opportunity to explore their catalytic properties for methanol oxidation. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

In Silico Switch from Second- to First-Row Transition Metals in Olefin Metathesis: From Ru to Fe and from Rh to Co

Directory of Open Access Journals (Sweden)

Jesús Antonio Luque-Urrutia

2017-12-01

Full Text Available Density functional theory (DFT calculations have been used to investigate the behavior of different transition metals from Groups 8 (Fe and Ru and 9 (Co and Rh in an already well-known catalytic mechanism, which is based on an Ru(SIMes(PPh3Cl2=CH(Ph complex. As expected, Ru has proven to perform better than their Fe, Co, and Rh counterparts. Even though the topographic steric maps analysis shows no difference in sterical hindrance for any of the metal centers, geometrically, the Fe-based species show a high rigidity with shorter and stronger bonds confirmed by Mayer Bond Orders. The systems bearing Co as a metallic center might present a reactivity that is, surprisingly, too high according to conceptual DFT, which would consequently be a drawback for the formation of the fundamental species of the reaction pathway: the metallacycle intermediate.

Ferrocene, ruthenocene or rhodocene analogues of Haloperidol. Synthesis and organ distribution after labelling with 103Ru or 103mRh

International Nuclear Information System (INIS)

Wenzel, M.; Wu, Y.

1988-01-01

Ferrocene-Haloperidol was synthesized by N-alkylation of 4-(4'-chlorophenyl)-4-hydroxypiperidine with 1-ferrocenyl-4-chlor-butan-1-on. By heating the ferrocene-haloperidol with 103 RuCl 3 the 103 Ru-labelled ruthenocene-haloperidol was obtained. This compound showed a high affinity for lung but not for brain in rats and mice. The decay of the 103 Ru labelled compound results in the formation of the 103m Rh labelled rhodocene-haloperidol, which is rapidly oxidized by air to the corresponding rhodocinium-haloperidol. This compound can be separated by extraction and TLC. (author)

Influence of ceria on the thermally durability of Pt/Rh automotive catalyst

International Nuclear Information System (INIS)

Muraki, H.; Zhang, G.

1998-01-01

Full text: The use of cerium oxide as an oxygen storage component in automotive three-way catalysts has been well established. More recently the requirement of the three-way catalysts against the increase of the severity in emission standards has focused attention on the development of more active, durable catalysts. The thermally durability of Pt/Rh catalyst can be achieved by the utilization of thermally stable ceria as well as optimization of washcoat composition and structure in order to control the extent of interaction between PGM and ceria. In the present paper, we describe the influence of newly developed washcoat components and PGM interaction with ceria on catalytic performance. First, to clear that the interaction between PGM and ceria contributes to catalytic performance, several kinds of catalysts which have the varied interactions between PGM and ceria were prepared using engineered washcoat techniques and evaluated in the model gas reactor. It was obvious that the difference in performance among them after aging derived from a diversity of interactions between Pt, Rh, and ceria. Second, for the purpose of determining the thermally durability of the developed Pt/Rh catalyst, the catalysts including the current catalyst were aged under three different temperatures and evaluated on engine dynamometer. Result of engine dynamometer evaluation revealed that significant improvement in the thermal durability can be achieved by optimizing the PGM-ceria interaction. In conclusion, we recognize that a thermal durability of a three-way catalyst can be improved by the stabilization of proper PGM-ceria interaction after aging as well as the utilization of thermally durable ceria material

Synthesis, single-crystal structure refinement and Fe/T site preference in the ternary borides Fe {sub x}T{sub 7-x}B{sub 3} (T = Ru, Rh; 0 < x {<=} 1.5)

Energy Technology Data Exchange (ETDEWEB)

Fokwa, Boniface P.T. [Institut fuer Anorganische Chemie, Rheinisch-Westfaelische Technische Hochschule Aachen, D-52056 Aachen (Germany); Dronskowski, Richard [Institut fuer Anorganische Chemie, Rheinisch-Westfaelische Technische Hochschule Aachen, D-52056 Aachen (Germany)]. E-mail: drons@HAL9000.ac.rwth-aachen.de

2007-01-31

Single crystals of the borides Fe {sub x}Rh{sub 7-x}B{sub 3} (1 < x < 1.5) and Fe {sub x}Ru{sub 7-x}B{sub 3} (0 < x < 1) have been synthesized by arc-melting the elements in a water-cooled copper crucible under argon atmosphere. The silver-like products, structurally characterized by single-crystal X-ray analysis, adopt the hexagonal Th{sub 7}Fe{sub 3} structure type (space group P6{sub 3} mc, no. 186) with Z = 2. Their structures consist of layers of boron-centered trigonal prisms of rhodium or ruthenium (Rh;Ru) and iron on the one side, and one-dimensional channels of face-sharing octahedral (Rh;Ru){sub 6} clusters on the other. Unlike in FeRh{sub 6}B{sub 3}, the iron substitution takes place at two (6c and 2b) of the three available rhodium/ruthenium positions, with a preference for the 6c site in the case of the Fe {sub x}Rh{sub 7-x}B{sub 3} compounds but not for Fe {sub x}Ru{sub 7-x}B{sub 3}.

Pt-Rh alloys. Investigation of creep rate and rupture time at high temperatures

Energy Technology Data Exchange (ETDEWEB)

Trumic, Biserka; Gomidzelovic, Lidija; Marjanovic, Sasa; Ivanovic, Aleksandra; Dimitrijevic, Silvana [Belgrade Univ., Bor (Serbia). Inst. of Mining and Metallurgy; Krstic, Vesna

2013-02-01

The results of experimental investigation of creep rate and rupture time of the alloys of Pt-Rh system are presented in this paper. Selected alloys with 7-40 wt.-% Rh content were examined using a universal device for tensile testing of materials at high temperatures, and monitoring structure changes of the samples by electron microscopy. Investigations were performed in the temperature range between 1200 C and 1700 C at a stress between 2 MPa and 15 MPa. (orig.)

Cyclic voltammetric analysis of C 1-C 4 alcohol electrooxidations with Pt/C and Pt-Ru/C microporous electrodes

Science.gov (United States)

Lee, Choong-Gon; Umeda, Minoru; Uchida, Isamu

The effect of temperature on methanol, ethanol, 2-propanol, and 2-butanol electrooxidation is investigated with Pt/C and Pt-Ru/C microporous electrodes. Cyclic voltammetry is employed in temperatures ranging from 25 to 80 °C to provide quantitative and qualitative information on the kinetics of alcohol oxidation. Methanol displays the greatest activity atom alcohols. The addition of ruthenium reduces the poisoning effect, although it is ineffective with secondary alcohols. Secondary alcohols undergo a different oxidation mechanism at higher temperatures. Microporous electrodes provide detailed information on alcohol oxidation.

Structure and magnetic properties of L10-FePt thin films on TiN/RuAl underlayers

International Nuclear Information System (INIS)

Yang En; Ratanaphan, Sutatch; Zhu Jiangang; Laughlin, David E.

2011-01-01

Highly ordered L1 0 FePt-oxide thin films with small grains were prepared by using a RuAl layer as a grain size defining seed layer along with a TiN barrier layer. Different HAMR (Heat Assisted Magnetic Recording) favorable underlayers were studied to encourage perpendicular texture and preferred microstructure. It was found that the epitaxial and small grain growth from the RuAl/TiN underlayer results in small and uniform grains in the FePt layer with perpendicular texture. By introducing the grain size defining underlayers, the FePt grain size can be reduced from 30 to 6 nm with the same volume fraction (9%) of SiO 2 in the film, excellent perpendicular texture, and very high order parameter at 520 deg. C.

Electrodeposition of Pt-Ru nanoparticles on fibrous carbon substrates in the presence of nonionic surfactant: Application for methanol oxidation

Energy Technology Data Exchange (ETDEWEB)

Bauer, Alex; Gyenge, Elod L.; Oloman, Colin W. [Department of Chemical and Biological Engineering, University of British Columbia, 2360 East Mall, Vancouver, BC (Canada)

2006-07-28

Liquid crystalline and micellar aqueous solutions of the nonionic surfactant Triton X-100 were used to direct the electrodeposition of Pt-Ru nanoparticles onto graphite felts, which were investigated as novel anodes for the direct methanol fuel cell. The effects of surfactant concentration, current density and deposition time in the preparation of these three-dimensional electrodes were studied in a factorial experiment and the electrodes were characterized by SEM and ICP-AES. Cyclic voltammetry, chronoamperometry and chronopotentiometry were carried out to assess the activity of the catalyzed felts for methanol oxidation. The presence of Triton X-100 (40-60wt.%) coupled with an acidic plating solution were essential for the efficient co-electrodeposition of Ru in the presence of Pt to yield approximately a 1:1 Pt:Ru atomic ratio in the deposit. The highest mass specific activity, 24Ag{sup -1} at 298K (determined by chronoamperometry after 180s at 0V versus Hg/Hg{sub 2}SO{sub 4}, K{sub 2}SO{sub 4std}), was obtained for the Pt-Ru electrodeposited in the presence of 40wt.% Triton X-100 at 60Am{sup -2}, 298K for 90min. Surfactant mediated electrodeposition is a promising method for meso-scale (ca. 10-60nm diameter) catalyst particle preparation on three-dimensional electrodes. (author)

Preparation of Pt Ru/C electrocatalysts using gamma radiation for application as anode in direct methanol fuel cell

International Nuclear Information System (INIS)

Spinace, Estevam V.; Silva, Dionisio F. da; Cruz, Victor A. da; Oliveira Neto, Almir; Machado, Luci D.B.; Pino, Eddy S.; Linardi, Marcelo

2005-01-01

PtRu nanoparticles supported on carbon (PtRu/C electrocatalysts) were prepared submitting a water/2-propanol mixture containing the metal ions and the carbon support to gamma radiation. The water/2-propanol (v/v) and the total dose (kGy) were studied. The electrocatalysts were characterized by EDX, XRD and cyclic voltammetry. The methanol electro-oxidation was studied by cyclic voltammetry using the thin porous coating. In the studied conditions, the electrocatalytic activity of the prepared electrocatalysts depend on the water/2-propanol ratio used in the reaction medium. (author)

A re-examination of thermodynamic modelling of U-Ru binary phase diagram

Energy Technology Data Exchange (ETDEWEB)

Wang, L.C.; Kaye, M.H., E-mail: matthew.kaye@uoit.ca [University of Ontario Institute of Technology, Oshawa, ON (Canada)

2015-07-01

Ruthenium (Ru) is one of the more abundant fission products (FPs) both in fast breeder reactors and thermal reactors. Post irradiation examinations (PIE) show that both 'the white metallic phase' (MoTc-Ru-Rh-Pd) and 'the other metallic phase' (U(Pd-Rh-Ru)3) are present in spent nuclear fuels. To describe this quaternary system, binary subsystems of uranium (U) with Pd, Rh, and Ru are necessary. Presently, only the U-Ru system has been thermodynamically described but with some problems. As part of research on U-Ru-Rh-Pd quaternary system, an improved consistent thermodynamic model describing the U-Ru binary phase diagram has been obtained. (author)

Energy deposition by a {sup 106}Ru/{sup 106}Rh eye applicator simulated using LEPTS, a low-energy particle track simulation

Energy Technology Data Exchange (ETDEWEB)

Fuss, M.C. [Instituto de Fisica Fundamental, Consejo Superior de Investigaciones Cientificas (CSIC), Serrano 113-bis, 28006 Madrid (Spain); Munoz, A.; Oller, J.C. [Centro de Investigaciones Energeticas, Medioambientales y Tecnologicas (CIEMAT), Avenida Complutense 22, 28040 Madrid (Spain); Blanco, F. [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad Complutense de Madrid, Avenida Complutense, 28040 Madrid (Spain); Williart, A. [Departamento de Fisica de los Materiales, Universidad Nacional de Educacion a Distancia, Senda del Rey 9, 28040 Madrid (Spain); Limao-Vieira, P. [Laboratorio de Colisoes Atomicas e Moleculares, Departamento de Fisica, CEFITEC, FCT-Universidade Nova de Lisboa, Quinta da Torre, 2829-516 Caparica (Portugal); Borge, M.J.G.; Tengblad, O. [Instituto de Estructura de la Materia, Consejo Superior de Investigaciones Cientificas (CSIC), Serrano 113-bis, 28006 Madrid (Spain); Huerga, C.; Tellez, M. [Hospital Universitario La Paz, Paseo de la Castellana 261, 28046 Madrid (Spain); Garcia, G., E-mail: g.garcia@iff.csic.es [Instituto de Fisica Fundamental, Consejo Superior de Investigaciones Cientificas (CSIC), Serrano 113-bis, 28006 Madrid (Spain); Departamento de Fisica de los Materiales, Universidad Nacional de Educacion a Distancia, Senda del Rey 9, 28040 Madrid (Spain)

2011-09-15

The present study introduces LEPTS, an event-by-event Monte Carlo programme, for simulating an ophthalmic {sup 106}Ru/{sup 106}Rh applicator relevant in brachytherapy of ocular tumours. The distinctive characteristics of this code are the underlying radiation-matter interaction models that distinguish elastic and several kinds of inelastic collisions, as well as the use of mostly experimental input data. Special emphasis is placed on the treatment of low-energy electrons for generally being responsible for the deposition of a large portion of the total energy imparted to matter. - Highlights: > We present the Monte Carlo code LEPTS, a low-energy particle track simulation. > Carefully selected input data from 10 keV to 1 eV. > Application to an electron emitting Ru-106/Rh-106 plaque used in brachytherapy.

Scanning tunneling microscopy and spectroscopy investigation of graphene on Ru(0001) and (CO+O) on Rh(111)

International Nuclear Information System (INIS)

Marchini, Stefano

2007-01-01

In this work STM was employed to investigate fundamental aspects of catalyst poisoning and deactivation on two model systems, namely the Ru(0001) and the Rh(111) surfaces. The structure of graphene on the Ru(0001) surface was investigated in detail with STM and LEED. The lattice mismatch between graphene and Ru(0001) results in the formation of an (11x11) superstructure. The two lattices come into coincidence every 11 metal unit cells and every 12 graphene cells, corresponding to a periodicity of 3 nm. The superstructure is characterized by a pronounced apparent corrugation of up to ∝1.5 Aa. Graphene has a preferential orientation aligned along the [10 anti 1 0] direction of the ruthenium lattice. Only in few cases a slight rotation of 1 between the two lattices was observed which nevertheless does not affect the 3 mn periodicity of the superstructure. The Ru surface restructures during the C segregation process so that the metal steps are aligned along the main directions of the overlayer. (orig.)

Influence of polymolybdate adsorbates on electrooxidation of ethanol at PtRu nanoparticles: Combined electrochemical, mass spectrometric and X-ray photoelectron spectroscopic studies

Science.gov (United States)

Gralec, Barbara; Lewera, Adam; Kulesza, Pawel J.

2016-05-01

The role Keggin-type phosphomolybdate (PMo12O403-) ions (adsorbed on carbon-supported PtRu, PtRu/C) on electrooxidation of ethanol is addressed here. The combined results obtained using Differential Electrochemical Mass Spectrometry, X-ray Photoelectron Spectroscopy and Cyclic Voltammetry are consistent with the view that presence of the Keggin-type polyoxometallate, phosphomolybdate, ions (adsorbates) leads to enlargement of the current densities associated with electrooxidation of ethanol at potentials greater than 700 mV vs. RHE. This increase of the anodic currents is correlated with the higher acetaldehyde yield which is likely to reflect changes in the reaction kinetics (e.g. more dynamic dehydrogenation of ethanol leading to acetaldehyde) or in the reaction mechanism defined by the preferential surface modification resulting not only in faster kinetics but also in higher selectivity with respect to acetaldehyde production. It is apparent from the spectroscopic data that modification of PtRu/C nanoparticles with phosphomolybdate ions leads to suppression of the formation of Ru surface oxides.

Electrocatalysis of the hydrogen oxidation in the presence of CO on RhO{sub 2}/C-supported Pt nanoparticles

Energy Technology Data Exchange (ETDEWEB)

Freitas, K.S.; Lopes, P.P. [Instituto de Quimica de Sao Carlos, USP, C.P. 780, Sao Carlos, SP 13560-970 (Brazil); Ticianelli, E.A., E-mail: edsont@iqsc.usp.b [Instituto de Quimica de Sao Carlos, USP, C.P. 780, Sao Carlos, SP 13560-970 (Brazil)

2010-12-15

This work presents a study on the kinetics of the hydrogen oxidation reaction (HOR) in the absence and in the presence of CO in ultra thin porous layer and in PEM fuel cell electrodes formed with Pt supported on RhO{sub 2}/C substrates. Together with the electrochemical measurements, the structural and electronic properties of these catalysts were characterized, enabling to correlate their structural and electronic properties with the HOR kinetics. The results show that the presence of Rh oxides leads to an emptying of the Pt 5d band and a consequent reduction of the back-donation of electrons from Pt to CO, weakening the Pt-CO bond and diminishing the CO degree of coverage on Pt, leaving more sites available to HOR. These changes in the electronic spectra do not lead to any perceptible change in the kinetics or the reaction of pure hydrogen. Also, the formation of CO{sub 2} monitored by the MS experiments in the fuel cell anode outlet indicates that the bifunctional mechanism is also operative, but the major CO tolerance is achieved by the electronic effect induced by the RhO{sub 2} support.

Gamma-gamma angular correlation measurement in the 100 Ru

International Nuclear Information System (INIS)

Kenchian, G.

1990-01-01

An angular correlation automatic spectrometer with two Ge(Li) detectors has been developed. The spectrometer moves automatically, controlled by a microcomputer. The gamma-gamma directional angular correlations of coincidence transitions have been measured in 100 Ru nuclide, following the β + and electron capture of 100 Rh. The 100 Rh source has been produced with 100 Ru(p,n) 100 Rh reaction, using the proton beam of the Cyclotron Accelerator insiding in 100 Ru isotope. (author)

Development of a database for the prediction of phases in Pt-Al-Cr-Ru alloys for high-temperature and corrosive environments: Al-Cr-Ru

International Nuclear Information System (INIS)

Suess, R.; Watson, A.; Cornish, L.A.; Compton, D.N.

2009-01-01

Platinum-based alloys for high-temperature corrosive environments are being developed which have microstructures that are analogous to the γ/γ' microstructure of the nickel-based superalloys. The need for a predictive thermodynamic database for these alloys was identified. Because experimental studies suggested that such a database should be based on Pt-Al-Cr-Ru, the Al-Cr-Ru system is of importance in this research programme. Using the CALPHAD method and Thermo-Calc software, existing binary data were used to optimise a ternary database for Al-Cr-Ru against available experimental ternary data. The database gives good predictions with regards to phase equilibria in the system as well as the nature of the primary solidification phases.

Ferrocene, ruthenocene or rhodocene analogues of Haloperidol. Synthesis and organ distribution after labelling with /sup 103/Ru or /sup 103m/Rh

Energy Technology Data Exchange (ETDEWEB)

Wenzel, M; Wu, Y

1988-01-01

Ferrocene-Haloperidol was synthesized by N-alkylation of 4-(4'-chlorophenyl)-4-hydroxypiperidine with 1-ferrocenyl-4-chlor-butan-1-on. By heating the ferrocene-haloperidol with /sup 103/RuCl/sub 3/ the /sup 103/Ru-labelled ruthenocene-haloperidol was obtained. This compound showed a high affinity for lung but not for brain in rats and mice. The decay of the /sup 103/Ru labelled compound results in the formation of the /sup 103m/Rh labelled rhodocene-haloperidol, which is rapidly oxidized by air to the corresponding rhodocinium-haloperidol. This compound can be separated by extraction and TLC.

Hydrogen Production by Steam Reforming of Ethanol on Rh-Pt Catalysts: Influence of CeO2, ZrO2, and La2O3 as Supports

Directory of Open Access Journals (Sweden)

Bernay Cifuentes

2015-11-01

Full Text Available CeO2-, ZrO2-, and La2O3-supported Rh-Pt catalysts were tested to assess their ability to catalyze the steam reforming of ethanol (SRE for H2 production. SRE activity tests were performed using EtOH:H2O:N2 (molar ratio 1:3:51 at a gaseous space velocity of 70,600 h−1 between 400 and 700 °C at atmospheric pressure. The SRE stability of the catalysts was tested at 700 °C for 27 h time on stream under the same conditions. RhPt/CeO2, which showed the best performance in the stability test, also produced the highest H2 yield above 600 °C, followed by RhPt/La2O3 and RhPt/ZrO2. The fresh and aged catalysts were characterized by TEM, XPS, and TGA. The higher H2 selectivity of RhPt/CeO2 was ascribed to the formation of small (~5 nm and stable particles probably consistent of Rh-Pt alloys with a Pt surface enrichment. Both metals were oxidized and acted as an almost constant active phase during the stability test owing to strong metal-support interactions, as well as the superior oxygen mobility of the support. The TGA results confirmed the absence of carbonaceous residues in all the aged catalysts.

Thermochemical investigations on intermetallic UMe3 compounds (Me=Ru,Rh,Pd)

International Nuclear Information System (INIS)

Wijbenga, G.

1981-10-01

The subject of this thesis is the determination of the thermodynamic properties of the intermetallic compounds of uranium with the light platinum metals, ruthenium, rhodium and palladium. These intermetallics are formed as very stable compounds during fission in nuclear fuel by the reaction of the fission products Ru, Rh and Pd with the matrix. Methods for the preparation of URu 3 , URh 3 and UPd 3 , experiments showing the chemical reactivities of these compounds, and studies of the stoichiometry of hexagonal UPd 3 by X-ray diffraction of solubility experiments of UN and palladium in UPd 3 , are described. Thermodynamic properties of the UMe 3 compounds have been obtained using several experimental thermodynamic techniques: fluorine bomb calorimetry, low-temperature cryogenic calorimetry, high-temperature drop calorimetry and EMF measurements of reversible cells. (Auth.)

High-quality graphene grown on polycrystalline PtRh{sub 20} alloy foils by low pressure chemical vapor deposition and its electrical transport properties

Energy Technology Data Exchange (ETDEWEB)

Yang, He; Shen, Chengmin, E-mail: cmshen@iphy.ac.cn; Tian, Yuan; Bao, Lihong; Chen, Peng; Yang, Rong; Yang, Tianzhong; Li, Junjie; Gu, Changzhi; Gao, Hong-Jun [Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190 (China)

2016-02-08

High-quality continuous uniform monolayer graphene was grown on polycrystalline PtRh{sub 20} alloy foils by low pressure chemical vapor deposition. The morphology of graphene was investigated by Raman spectroscopy, scanning electron microscopy, and atomic force microscopy. Analysis results confirm that high quality single-layer graphene was fabricated on PtRh{sub 20} foil at 1050 °C using a lower flux of methane under low pressure. Graphene films were transferred onto the SiO{sub 2}/Si substrate by the bubbling transfer method. The mobility of a test field effect transistor made of the graphene grown on PtRh{sub 20} was measured and reckoned at room temperature, showing that the carrier mobility was about 4000 cm{sup 2} V{sup −1} s{sup −1}. The results indicate that desired quality of single-layer graphene grown on PtRh{sub 20} foils can be obtained by tuning reaction conditions.

Cyclic voltammetric analysis of C{sub 1}-C{sub 4} alcohol electrooxidations with Pt/C and Pt-Ru/C microporous electrodes

Energy Technology Data Exchange (ETDEWEB)

Lee, Choong-Gon [Department of Chemical Engineering, Hanbat National University, San 16-1 Dukmyung-dong, Yusong-gu, Daejon (Korea); Umeda, Minoru [Department of Chemistry, Nagaoka University of Technology, Kamitomioka, Nagaoka (Japan); Uchida, Isamu [Department of Applied Chemistry, Tohoku University, Aramaki-aoba, Aoba-ku, Sendai (Japan)

2006-09-29

The effect of temperature on methanol, ethanol, 2-propanol, and 2-butanol electrooxidation is investigated with Pt/C and Pt-Ru/C microporous electrodes. Cyclic voltammetry is employed in temperatures ranging from 25 to 80{sup o}C to provide quantitative and qualitative information on the kinetics of alcohol oxidation. Methanol displays the greatest activity atom alcohols. The addition of ruthenium reduces the poisoning effect, although it is ineffective with secondary alcohols. Secondary alcohols undergo a different oxidation mechanism at higher temperatures. Microporous electrodes provide detailed information on alcohol oxidation. (author)

Magnetic properties of Co and Fe on Pt(111), Rh(111) and Pd(111): From single atoms to ultrathin films

Energy Technology Data Exchange (ETDEWEB)

Lehnert, Anne; Rusponi, Stefano; Etzkorn, Markus; Moulas, Geraud; Brune, Harald [IPN, EPF-Lausanne (Switzerland); Gambardella, Pietro [CREA, Catalan Institute of Nanotechnology (Spain); Bencok, Peter [ESRF, Grenoble (France)

2009-07-01

Single atoms of Co on Pt(111) are known to have a giant magnetic anisotropy energy (MAE) of 9.3 meV/atom. This is due to the reduced coordination and the strong spin-orbit coupling of the Pt 5d-states. In order to study the contribution of a highly polarizable substrate to the MAE, we investigated single Co atoms on Pd(111) and Rh(111) using X-ray magnetic circular dichroism (XMCD). We find a decreasing MAE moving from a 5d-substrate (Pt) to 4d-substrates (Pd and Rh). Co has a large orbital moment L of about 0.7 independent of the substrate. The easy axis is out-of-plane for Pt(111) and Pd(111) whereas it is in-plane for Co/Rh(111). Fe has on all substrates an out-of-plane easy axis, a very small anisotropy energy, and a L/S ratio of about 0.1. With increasing coverage the coordination number of the adatom increases and generally leads to a reduced MAE and orbital moment compared to the single atom. We measure one monolayer of Co and Fe on Pt(111) and Rh(111) and find MAE values <0.5 meV/atom. For 1 ML Co we find a substantial decrease in the L/S ratio to 0.19. However, the L/S ratio for 1 ML Fe on both substrates does not change much compared with the Fe single atom.

Bifunctional electrodes with ir and Ru oxide mixtures and pt for unified regenerative cells; Electrodos bifuncionales basados en mezclas de oxidos de Ir y Ru con Pt para celdas regenerativas unificadas

Energy Technology Data Exchange (ETDEWEB)

Duron-Torres, S.M.; Escalante-Garcia, I.L. [Universidad Autonoma de Zacatecas, Zacatecas (Mexico); Cruz, J. C.; Arriaga-Hurtado; L.G. [Centro de Investigacion y Desarrollo Tecnologico en Electroquimica, Pedro Escobedo, Queretaro (Mexico)]. E-mail: duronsm@prodigy.net.mx

2009-09-15

Unified regenerative fuel cells (URFC) represent an attractive option to obtain hydrogen and generate energy using a compact device. Nevertheless, the fusion of a fuel cell (PEMFC) and a water electrolyzer continue to be a challenge because of the wide range of conditions to which this type of device is subject. Because of its kinetic characteristics, oxygen reduction reaction (ORR) in PEMFC and oxygen evolution reaction (OER) in PEMWE are the limiting stages of the URFC depending on the mode of operation. The primary focus of research related to URFC is the obtainment of bifunctional electrocatalysts that satisfactorily perform in both oxygen reactions and support the different working conditions found in a fuel cell and an electrolyzer. The present work contributes to the research on bifunctional electrocatalysts and shows some preliminary results from the electrochemical study of different Pt gcc, IrO{sub 2} and RuO{sub 2} mixtures supported in Ebonex® as oxygen electrodes. The electrochemical characterization with cyclic voltamperometry (CV), linear voltamperometry (LV) and electrochemical impedance spectroscopy (EIS) in H{sub 2}SO{sub 4} 0.5 M, in the absence and present of oxygen shows that Ebonex®-supported bifunctional electrodes IrO{sub 2}-Pt and RuO{sub 2}-Pt present reasonable electrocatalytic properties for oxygen evolution and reduction reactions and present the possibility of their use in an URFC. The Ir- based oxide electrodes show greater stability than ruthenium-oxide electrodes. [Spanish] Las celdas de combustible regenerativas unificadas (URFC) representan una atractiva opcion para la obtencion de hidrogeno y generacion de energia en un dispositivo compacto. Sin embargo, la fusion de una celda de combustible (PEMFC) y un electrolizador de agua (PEMWE) sigue siendo un reto por la amplia gama de condiciones a que se sujeta un dispositivo de este tipo. Por sus caracteristicas cineticas, la reaccion de reduccion de oxigeno (ORR) en la PEMFC y la

Electrocatalytical activity of Pt, SnO2 and RuO2 mixed electrodes for the electrooxidation of formic acid and formaldehyde

International Nuclear Information System (INIS)

Profeti, L.P.R.; Profeti, D.; Olivi, P.

2005-01-01

The electrocatalytical activity of binary electrodes of Pt and SnO 2 and ternary electrodes of Pt and SnO 2 and RuO 2 for the electrooxidation of formic acid and formaldehyde was investigated by cyclic voltammetry and chronoamperometry techniques. The electrode materials were prepared by the thermal decomposition of polymeric precursors at 400 deg C. The cyclic voltammetry results showed that the methanol electrooxidation process presents peak potentials for those electrodes approximately 100 mV lower than the values obtained for metallic platinum electrodes. The Pt 0.6 Ru 0.2 Sn 0.2 O y electrodes presented the highest current density values for potentials lower than the peak potential values. The chronoamperometric experiments also showed that the addition of SnO 2 and RuO 2 contributed for the enhancement of the electrode activity in low potential values. The preparation method was found to be useful to obtain high active materials. (author)

CoFeRh alloys

Energy Technology Data Exchange (ETDEWEB)

Tabakovic, Ibro [Seagate Technology, Research and Development, Bloomington, MN 55435 (United States)], E-mail: ibro.m.tabakovic@seagate.com; Qiu Jiaoming; Riemer, Steve; Sun Ming; Vas' ko, Vlad; Kief, Mark [Seagate Technology, Research and Development, Bloomington, MN 55435 (United States)

2008-01-01

The electrochemical behavior of Rh(III) species in CoFe solution containing RhCl{sub 3}, NH{sub 4}Cl, H{sub 3}BO{sub 3}, CoSO{sub 4}, FeSO{sub 4}, saccharin, and NaLS (Na lauryl sulfate) has been investigated. The electrochemistry of Rh(III) species is influenced by each of the compounds present in CoFe plating solution, but especially by addition of saccharin and H{sub 3}BO{sub 3} to the RhCl{sub 3}-NH{sub 4}Cl solution. The nucleation and growth of Rh on GC (glassy carbon), Ru, and Cu electrodes from NH{sub 4}Cl solution was studied using the potentiostatic current-transient methods. The results support a predominantly progressive nucleation of Rh on all three-electrode surfaces. The nucleation kinetic parameters ANo (steady state nucleation rate) and Ns (saturation nuclear number density) were found to vary with potential and are electrode-dependent in order: GC > Ru{approx}Cu. The electrodeposited Rh films obtained from NH{sub 4}Cl solution and nonmagnetic CoFeRh film obtained from CoFe solution were characterized in terms of the following properties: morphology, surface roughness, crystal structure and chemical composition. The origin of light elements found in Rh and CoFeRh films (O, Cl, S, C, N) was discussed.

Roadside Accumulation of Pt, Pd, Rh and Other Trace Elements From Automobiles: Catalytic Converter Attrition and Platinum-Group Element Mobility in the Roadside Environment.

Science.gov (United States)

Ely, J. C.; Dahlheimer, S. R.; Neal, C. R.

2003-12-01

Elemental abundances of Pt, Pd and Rh have been documented across the industrialized world in roadside environments due to attrition of automotive catalytic converters (Zereini and Alt, 2000, Anthropogenic PGE Emissions, Springer, 308pp; Ely et al., 2001, EnvSci&Tech, 35:3816-3822; Whiteley and Murray, 2003, SciTotEnv, in press). In our ongoing study, the highest reported roadside Pt abundance 1.8 ppm has been found immediately adjacent to the road at a field site in South Bend, IN, USA. Furthermore, initial studies show positive correlations of Pt, Pd and Rh with some trace elements (Ni, Cu, Zn and Pb), which has been confirmed by further analysis for these and other elements (Ce, Cr). It has been demonstrated that elements such as Ce are present in catalytic converters at concentrations of 100's ppm to 3-wt.%. These elements are also being attrited with Pt, Pd and Rh and aerially transported and deposited. Our field site was established next to US-933 adjacent to the Notre Dame campus. Areas were cleared of the top 2-4 cm of soil (removing surficial Pt, Pd and Rh) at 1, 5, 10 and 50 meters from the roadside. Within 3 months the 1-meter site contained 67% of the initial Rh and Pt concentrations and 100% of the initial Pd concentration. The sites at 5, 10 and 50 meters showed similar results, in some cases exceeding the initial concentrations. After 6 months the concentrations of Pt, Pd and Rh were all within error of the initial concentrations, indicating steady state abundances had probably been reached. Grass samples from each site showed that washed vs. unwashed samples were within error of each other, and there may be a slight enrichment (approx. 1 ppb) in the grasses of Pd and Pt, but this enrichment was independent of distance from the road. The steady-state situation suggests that the PGEs are being removed from the immediate roadside environment, which requires that the metals are being oxidized and/or complexed in such a way to facilitate transport. The

Synthesis, crystal structure investigation and magnetism of the complex metal-rich boride series Cr{sub x}(Rh{sub 1-y}Ru{sub y}){sub 7-x}B{sub 3} (x=0.88-1; y=0-1) with Th{sub 7}Fe{sub 3}-type structure

Energy Technology Data Exchange (ETDEWEB)

Misse, Patrick R.N.; Mbarki, Mohammed [Institute of Inorganic Chemistry, RWTH Aachen University, 52066 Aachen (Germany); Fokwa, Boniface P.T., E-mail: boniface.fokwa@ac.rwth-aachen.de [Institute of Inorganic Chemistry, RWTH Aachen University, 52066 Aachen (Germany)

2012-08-15

Powder samples and single crystals of the new complex boride series Cr{sub x}(Rh{sub 1-y}Ru{sub y}){sub 7-x}B{sub 3} (x=0.88-1; y=0-1) have been synthesized by arc-melting the elements under purified argon atmosphere on a water-cooled copper crucible. The products, which have metallic luster, were structurally characterized by single-crystal and powder X-ray diffraction as well as EDX measurements. Within the whole solid solution range the hexagonal Th{sub 7}Fe{sub 3} structure type (space group P6{sub 3}mc, no. 186, Z=2) was identified. Single-crystal structure refinement results indicate the presence of chromium at two sites (6c and 2b) of the available three metal Wyckoff sites, with a pronounced preference for the 6c site. An unexpected Rh/Ru site preference was found in the Ru-rich region only, leading to two different magnetic behaviors in the solid solution: The Rh-rich region shows a temperature-independent (Pauli) paramagnetism whereas an additional temperature-dependent paramagnetic component is found in the Ru-rich region. - Graphical abstract: The new complex boride series Cr{sub x}(Rh{sub 1-y}Ru{sub y}){sub 7-x}B{sub 3} (x=0.88-1; y=0-1) has been synthesized by arc melting the elements under purified argon atmosphere. Beside the 3d/4d site preference within the whole solid solution, an unexpected Rh/Ru site preference was found in the Ru-rich region only, leading to two different magnetic behaviors: The Rh-rich region shows a temperature-independent (Pauli) paramagnetism whereas an additional temperature-dependent paramagnetic component is found in the Ru-rich region. Highlights: Black-Right-Pointing-Pointer Synthesis of a new boride series fulfilling Vegard Acute-Accent s rule. Black-Right-Pointing-Pointer 3d/4d site preference. Black-Right-Pointing-Pointer Unexpected Ru/Rh site preference. Black-Right-Pointing-Pointer Rh-rich region is Pauli paramagnetic. Black-Right-Pointing-Pointer Ru-rich region is Pauli and temperature-dependent paramagnetic.

Monitoring Pt and Rh in urban aerosols from Buenos Aires, Argentina

Energy Technology Data Exchange (ETDEWEB)

Bocca, Beatrice; Caimi, Stefano; Caroli, Sergio [Istituto Superiore di Sanita, Viale Regina Elena 299, 00161, Rome (Italy); Smichowski, Patricia; Gomez, Dario [Comision Nacional de Energia Atomica, Unidad de Actividad Quimica, Centro Atomico Constituyentes, Av. Gral. Paz 1499, B1650KNA-San Martin, Pcia. de Buenos Aires (Argentina)

2006-04-01

Vehicular traffic is the main source of platinum group elements (PGEs) in highly populated urban areas like Buenos Aires where a traffic density of 1,500,000 vehicles day{sup -1} (corresponding to 7500 vehicles km{sup -2}) is estimated. Since there is no information on the levels of PGEs in Buenos Aires, a pilot study was undertaken to ascertain the amount of two major PGEs, namely Pt and Rh, in the atmosphere of this city. To this end, 49 samples of PM-10 particulate matter were collected during 7 days in seven representative sampling sites located downtown Buenos Aires and spread over an area of about 30 km{sup 2}. The collection of particulate matter was performed on ash-free glass-fiber filters using high volume samplers with PM-10 sampling heads. Filters loaded with the particulate matter were subjected to microwave (MW)-assisted acid digestion using a combination of HNO{sub 3}, HF and HClO{sub 4}. The resulting solutions were evaporated and then diluted with 0.1 mol l{sup -1} HCl. Analyses were performed by sector field inductively coupled plasma-mass spectrometry (SF-ICP-MS) and special attention was paid to the control of mass interferences. Statistical analysis was performed on the experimental data obtained for the element concentrations taking also into account local meteorological data for the monitored period. The highest concentrations of Pt and Rh were detected at two sites (Hospital Aleman and Casa Rapallini) located in streets with traffic consisting mostly of passenger cars. The Pt content (in pg m{sup -3}) in airborne particulate matter was found to vary from 2.3 to 47.7, with a mean value of 12.9+/-7, and that of Rh from 0.3 to 16.8, with a mean value of 3.9+/-2.8. These concentrations are by far below the levels for which adverse health effects might be expected to occur, i.e., around 100 ng m{sup -3}. On the other hand, monitoring of PGEs should be carried out in a systematic fashion to detect possible dramatic increases from today

Metamorphosis of the mixed phase PtRu anode catalyst for direct methanol fuel cells after exposure of methanol: In situ and ex situ characterizations

Energy Technology Data Exchange (ETDEWEB)

Chakraborty, Debasish [Center for Individual Nanoparticle Functionality (CINF), Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Aerosol Laboratory, Nano.DTU, Department of Chemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Chorkendorff, Ib [Center for Individual Nanoparticle Functionality (CINF), Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Johannessen, Tue [Aerosol Laboratory, Nano.DTU, Department of Chemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark)

2007-11-08

The change in the mixed phase heavily oxidized PtRu anode with the exposure of methanol in a direct methanol fuel cell (DMFC) has been investigated by electrochemical impedance spectroscopy (EIS) and X-ray diffraction (XRD). The investigation had two major objectives: (i) to explore the original state of the active catalyst and (ii) to understand if alloying of Pt and Ru is a requirement for higher methanol oxidation activity. It was found that the methanol oxidation activity gradually improved for {proportional_to}2 h of exposure. The impedance spectra were taken at different times within this time of improvement of activity. The impedance spectra were deconvoluted in different contributions like membrane resistance (R{sub m}), charge transfer resistance (R{sub Ct}), adsorption resistance (R{sub ad}), and oxidation resistance (R{sub ox}). The improvement of the activity was explained in terms of the effect of the pretreatment on different contributions. XRD was done on the virgin and methanol exposed sample as a possible mean to identify the difference. It was postulated that the reduction of the as prepared PtRu after exposure was responsible for the activity improvement. Also, it was shown that bulk alloy formation is not a necessary condition for higher methanol activity of PtRu catalysts. (author)

Stability and ordering properties of fcc alloys based on Rh, Ir, Pd, and Pt

Czech Academy of Sciences Publication Activity Database

Turchi, P. E. A.; Drchal, Václav; Kudrnovský, Josef

2006-01-01

Roč. 74, č. 6 (2006), 064202/1-064202/12 ISSN 1098-0121 Institutional research plan: CEZ:AV0Z10100520; CEZ:AV0Z1010914 Keywords : alloy phase stability * ordering in alloys * fcc alloys of Rh, Ir, Pd, Pt Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.107, year: 2006

PENGARUH KUALITAS KEHIDUPAN KERJA DAN KEPUASAN KERJA TERHADAP KINERJA KARYAWAN PT PERTAMINA PERSERO RU IV CILACAP

Directory of Open Access Journals (Sweden)

Astrianditya Januar Ristanti

2017-04-01

These results indicate that the quality of work life has significant influence but not the performance, job satisfaction has a significant impact on performance, while the quality of work life and job satisfaction has a significant impact on employee performance remains part of PT Pertamina Persero shift RU Cilacap.

Diastereoselective formation of metallamacrocyclic (arene)Ru(II) and CpRh(III) complexes.

Science.gov (United States)

Lehaire, Marie-Line; Scopelliti, Rosario; Herdeis, Lorenz; Polborn, Kurt; Mayer, Peter; Severin, Kay

2004-03-08

The reaction of [(arene)RuCl(2)](2) (arene = cymene, 1,3,5-C(6)H(3)Me(3)) and [CpRhCl(2)](2) half-sandwich complexes with tridentate heterocyclic ligands in the presence of base has been investigated. In all cases, the chloro-ligands were substituted to give metallacyclic products with ring sizes between 4 and 18 atoms. The cyclization occurs in a highly diastereoselective fashion with chiral recognition between the different metal fragments. The complexes were comprehensively characterized by elemental analysis, NMR spectroscopy, and single crystal X-ray crystallography. For 2-hydroxy-nicotinic acid and 2-amino-nicotinic acid, dinuclear structures were obtained (15-17) whereas for 2,3-dihydroxyquinoline, 2,3-dihydroxyquinoxaline, and 6-methyl-2,3-phenazinediol, trimeric assemblies were found (19-22), and for 4-imidazolecarboxylic acid, a tetrameric assembly (18) was found.

Mixed valent noble metal perovskites Ba/sub 3/B/sup 3 +/Pt/sub x/Ru/sub 2-x//sup 4. 5+/O/sub 9/

Energy Technology Data Exchange (ETDEWEB)

Moessner, B; Kemmler-Sack, S; Ehmann, A [Tuebingen Univ. (Germany, F.R.). Lehrstuhl fuer Anorganische Chemie 2

1982-04-01

In perovskites of type Ba/sub 3/B/sup 3 +/Pt/sub x/Ru/sub 2-x//sup 4.5+/O/sub 9/ the ruthenium can be substituted by platinum up to x = 1. The compounds crystallize in a 1:2 ordered hexagonal BaTiO/sub 3/ structure (sequence (hcc)/sub 2/) with face connected Pt/sub x/Ru/sub 2-x/O/sub 9/ double octahedra. Intensity calculations on powder data of Ba/sub 3/YPt/sub 1/2/Ru/sub 3/2/O/sub 9/ (space group P6/sub 3//mmc) gave a refined, intensity related R' value of 8.6%. The vibrational spectroscopic and catalytic properties are reported.

Electrochemical oxidation of ethanol using PtRh/C electrocatalysts in alkaline medium and synthesized by sodium borohydride and alcohol reduction

International Nuclear Information System (INIS)

Fontes, Eric Hossein

2017-01-01

PtRh/C were prepared by the following atomic proportions: (100,0), (0,100), (90,10), (70,30) and (50,50). The methods employed in the synthesis of these materials were reduction by sodium borohydride and reduction by alcohol. The metal salts used were H 2 PtCl 6 3•6H 2 0 and (RhNO 3 ) 3 , the support used was Carbon black XC72 and the bulk metal composition was 20% and 80% of support. The electrocatalysts were characterized by Energy Dispersive X-ray spectroscopy, X-ray diffraction and Transmission electron microscopy. The ethanol electrochemical oxidation mechanism was investigated by in situ Fourier Transform Infrared Spectroscopy couple to an Attenuated Total Reflection technique. The electrocatalytic activity were evaluated by Cyclic Voltammetry, Linear Sweep Voltammetry and Chronoamperometry techniques. The Fuel Cells tests were made in a single direct alcohol fuel cell with alkaline membrane. The working electrodes were prepared by a thin porous coating technique. X-ray diffraction allowed to verify metallic alloys, segregate phases and to calculate the percentage of metallic alloys. It was else possible to identify crystallographic phases. Infrared Spectroscopy allowed to verify that the electrochemical oxidation of ethanol was carried out by an incomplete mechanism. PtRh(70:30)/C prepared by sodium borohydride produced large amounts of carbon dioxide and acetaldehyde. Rh/C showed electrocatalytic activity when compared with other materials studied.

Performance PtSnRh electrocatalysts supported on carbon-Sb2O5.SbO2 for the electro-oxidation of ethanol, prepared by an alcohol-reduction process

International Nuclear Information System (INIS)

Castro, Jose Carlos

2013-01-01

PtSnRh electrocatalysts supported on carbon-Sb 2 O 5 .SnO 2 , with metal loading of 20 wt%, were prepared by an alcohol-reduction process, using H 2 PtCl 6 .6H 2 O (Aldrich), RhCl 3 .xH 2 O (Aldrich) and SnCl 2 .2H 2 O (Aldrich), as source of metals; Sb 2 O 5 .SnO 2 (ATO) and carbon Vulcan XC72, as support; and ethylene glycol as reducing agent. The electrocatalysts obtained were characterized physically by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The diffractograms showed which PtSnRh/C-ATO electrocatalysts had FCC structure of Pt and Pt alloys, besides several peaks associated with SnO 2 and ATO. The average sizes of crystallites were between 2 and 4 nm. TEM micrographs showed a good distribution of the nanoparticles on the support. The average sizes of particles were between 2 and 3 nm, with good agreement for the average size of the crystallites. The performances of the electrocatalysts were analyzed by electrochemical techniques and in real conditions of operation using single direct ethanol fuel cell. In the chronoamperometry at 50 deg C, the electrocatalysts with carbon (85 wt%) and ATO (15 wt%) support, showed the best activity, and the atomic proportions which achieved the best results were PtSnRh(70:25:05) e (90:05:05). PtSnRh(70:25:05)/85C+15ATO electrocatalysts showed the best performance in a direct ethanol fuel cell. (author)

First-principle calculations for electronic properties of PuX3 (X=Rh, Pd, Pt)

International Nuclear Information System (INIS)

Tatetsu, Yasutomi; Maehira, Takahiro

2012-01-01

Energy band structures of PuX 3 (X=Rh, Pd, and Pt) are investigated by a relativistic linear augmented-plane-wave method with the exchange-correlation potential in a local density approximation. It is found in common that the energy bands in the vicinity of the Fermi level are mainly due to the hybridization between Pu 5f and X d electrons.

On new ternary equiatomic scandium transition metal aluminum compounds ScTAl with T = Cr, Ru, Ag, Re, Pt, and Au

Energy Technology Data Exchange (ETDEWEB)

Radzieowski, Mathis; Janka, Oliver [Muenster Univ. (Germany). Inst. fuer Anorganische und Analytische Chemie; Benndorf, Christopher [Muenster Univ. (Germany). Inst. fuer Anorganische und Analytische Chemie; Muenster Univ. (Germany). Inst. fuer Physikalische Chemie; Haverkamp, Sandra [Muenster Univ. (Germany). Inst. fuer Physikalische Chemie; Eckert, Hellmut [Muenster Univ. (Germany). Inst. fuer Physikalische Chemie; University of Sao Paulo, Sao Carlos, SP (Brazil). Inst. of Physics

2016-08-01

The new equiatomic scandium transition metal aluminides ScTAl for T = Cr, Ru, Ag, Re, Pt, and Au were obtained by arc-melting of the elements followed by subsequent annealing for crystal growth. The samples were studied by powder and single crystal X-ray diffraction. The structures of three compounds were refined from single crystal X-ray diffractometer data: ScCrAl, MgZn{sub 2} type, P6{sub 3}/mmc, a = 525.77(3), c = 858.68(5) pm, R{sub 1} = 0.0188, wR{sub 2} = 0.0485, 204 F{sup 2} values, 13 variables, ScPtAl, TiNiSi type, Pnma, a = 642.83(4), b = 428.96(2), c = 754.54(5) pm, R{sub 1} = 0.0326, wR{sub 2} = 0.0458, 448 F{sup 2} values, 20 variables and ScAuAl, HfRhSn type, P anti 62c, a = 722.88(4), c = 724.15(4) pm, R{sub 1} = 0.0316, wR{sub 2} = 0.0653, 512 F{sup 2} values, 18 variables. Phase pure samples of all compounds were furthermore investigated by magnetic susceptibility measurements, and Pauli-paramagnetism but no superconductivity was observed down to 2.1 K for all of them. The local structural features and disordering phenomena have been characterized by {sup 27}Al and {sup 45}Sc magic angle spinning (MAS) and static NMR spectroscopic investigations.

Effect of Ni and noble metals (Ru, Pd and Pt) on performance of bifunctional MoP/SiO2 for hydroconversion of methyl laurate

Science.gov (United States)

Nie, Ziyang; Zhang, Zhena; Chen, Jixiang

2017-10-01

SiO2 supported bifunctional MoP catalysts modified with different metal promoters (Ni, Ru, Pd, Pt), where Mo/Ni and Mo/M(M = Ru, Pd and Pt) atomic ratios was respectively 10 and 40, were prepared by TPR method from the phosphate precursors. It was found that the introduction of metal promoters facilitated the reduction of phosphate precursor and enhanced the dispersion of MoP. However, the MoP catalyst acidity was scarcely influenced by the small amount of metal promoters. In the hydroconversion of methyl laurate, the promoters enhanced the MoP catalyst activity for conversion of methyl laurate and hydrogenation of alkenes (intermediate), but reduced isomerization ability. Among the promoters, Ru was an optimum to decrease selectivity to alkenes while maintain high selectivity to iso-alkanes, and Mo40RuP showed better stability than MoP. At 380 °C and 3.0 MPa, the conversion of methyl laurate, the total selectivity to C11 and C12 hydrocarbons and the selectivity to iso-alkanes maintained at 100%, ∼94% and ∼30% on Mo40RuP during 102 h, respectively. The good stability of Mo40RuP is ascribed to that the presence of Ru prevented the sintering of MoP particles and suppressed carbon deposition.

A first-principles study on the interaction of biogas with noble metal (Rh, Pt, Pd) decorated nitrogen doped graphene as a gas sensor: A DFT study

Science.gov (United States)

Zhao, Chunjiang; Wu, Huarui

2018-03-01

Density functional theory calculations are carried out to investigate the adsorption characteristics of methane (CH4), carbon dioxide (CO2), hydrogen (H2), hydrogen sulfide (H2S), nitrogen (N2), and oxygen (O2) on the surface of pyridine-like nitrogen doped graphene (PNG) as well as noble metal (Rh, Pt, Pd) decorated PNG to elaborate their potentials as gas sensors. The adsorption intensities of biogas on noble metal (Rh, Pt, Pd) decorated PNG are in the order of O2> H2S> N2> CH4> CO2> H2, which are corresponded to the order of their sensitivity on surface. Compared with biogas adsorption on pristine PNG, there exist higher adsorption ability, higher charge transfer and higher orbital hybridization upon adsorption on noble metal (Rh, Pt, Pd) decorated PNG. Consequently, the noble metal (Rh, Pt, Pd) decorated PNG can transform the existence of CH4, CO2, H2, H2S, N2, and O2 molecules into electrical signal and they could potentially be used as ideal sensors for detection of biogas in ambient situation.

Assessment of ocular beta radiation dose distribution due to 106Ru/106Rh brachytherapy applicators using MCNPX Monte Carlo code

Directory of Open Access Journals (Sweden)

Nilseia Aparecida Barbosa

2014-08-01

Full Text Available Purpose: Melanoma at the choroid region is the most common primary cancer that affects the eye in adult patients. Concave ophthalmic applicators with 106Ru/106Rh beta sources are the more used for treatment of these eye lesions, mainly lesions with small and medium dimensions. The available treatment planning system for 106Ru applicators is based on dose distributions on a homogeneous water sphere eye model, resulting in a lack of data in the literature of dose distributions in the eye radiosensitive structures, information that may be crucial to improve the treatment planning process, aiming the maintenance of visual acuity. Methods: The Monte Carlo code MCNPX was used to calculate the dose distribution in a complete mathematical model of the human eye containing a choroid melanoma; considering the eye actual dimensions and its various component structures, due to an ophthalmic brachytherapy treatment, using 106Ru/106Rh beta-ray sources. Two possibilities were analyzed; a simple water eye and a heterogeneous eye considering all its structures. Two concave applicators, CCA and CCB manufactured by BEBIG and a complete mathematical model of the human eye were modeled using the MCNPX code. Results and Conclusion: For both eye models, namely water model and heterogeneous model, mean dose values simulated for the same eye regions are, in general, very similar, excepting for regions very distant from the applicator, where mean dose values are very low, uncertainties are higher and relative differences may reach 20.4%. For the tumor base and the eye structures closest to the applicator, such as sclera, choroid and retina, the maximum difference observed was 4%, presenting the heterogeneous model higher mean dose values. For the other eye regions, the higher doses were obtained when the homogeneous water eye model is taken into consideration. Mean dose distributions determined for the homogeneous water eye model are similar to those obtained for the

Investigation of the behavior of Pt-Ru mixtures with nafion in the oxygen reduction reaction; Investigacion del comportamiento de mezclas de Pt-Ru con nafion en la reaccion de reduccion de oxigeno

Energy Technology Data Exchange (ETDEWEB)

Enriquez M, O

2005-07-01

In this work the electrochemical study for the reduction reaction of oxygen (RRO) of ruthenium, platinum and two mixtures of Pt-Ru (10:90) and Pt-Ru (50:50); to this last its were determined the kinetic and electrochemical parameters. The platinum used was analytical platinum and the ruthenium it was obtained of the decarboxylation of 200 mg of ruthenium dode carbonyl with 200 ml of 1-2 dichlorobenzene under a reflux system by 20 hours with agitation. Decanted and centrifuged by 30 minutes, the obtained ruthenium was washed with ether and it was evaporated for it later use. The material was characterized by means of X-ray diffraction, elementary analysis, scanning electron microscopy and infrared spectroscopy. To determine the optimum quantity of nafion to be deposited on the catalytic material, they were carried out tests with different quantities deposited on the electrodes with 1, 2, 4 and 8 {mu}L, giving better result 2 {mu}L for that it was opted for to work with this proportion in the mixtures. The electrochemical performance of 2 ruthenium relationships and platinum 0.05 mg - 0.45 mg and 0.25 mg - 0.25 mg respectively were studied with a potentiostat galvanostat EG and G Princeton Applied Research model 273a; it was found that the electrode with the mixture of 0.25 mg of platinum with 0.25 mg of ruthenium has a bigger response of current intensity after to deposit the nafion in the surface. The electro active area was determined carrying out recurrent voltametry to different scanning velocities (5, 10, 20, 30, 40, 50, 60, 70 and 80 mV/s) in the non faraday region with a value of 0.2082 cm{sup 2}. The mixture Pt-Ru (50:50) it presents a first order kinetics for the RRO and it is carried out via 4 electrons; the study of current density in function of the temperature presents values of 0.47 {+-} 0.3 for the charge transfer coefficient, of 118 mV/decade for the Tafel slope and it has an activation energy of 0.39 eV. (Author)

Gama-gama angular correlations in the 105Rh nucleus

International Nuclear Information System (INIS)

Esteves, V.A.P.

1979-01-01

The Directional Correlation of γ transitions in 105 Rh have been measured from the β - decay of 105 Ru using a Ge(Li) - Nal(Tl) spectrometers. The measurements were carried out for the (316-469), (500-469), (845-499), (875-469), (878-499), (907-469), (1017-469), (350-326), (393-263), (413-263), (489-149) and (575-149) KeV gama cascades. The present results confirm the spin assignments to several levels in 105 Rh obtained in previous studies. The multipole mixing ratios Δ(E2/M1) for several gama transitions have been calculated from the measured angular correlations. The results are Δ(149)=0.34+-0.01,Δ(262)=-1.27+-0.02 or -0.14+-0.01,Δ(326)=-1.79+-0.01 or 0.014+-0.002, Δ(393)=-7.1+-0.3 or -0.36+-0.01, Δ(489)=0.25+-0.002, Δ(500)=0.7+-0.3 and Δ(907)=-21.7 +8 -31.1 or 0.21+-0.03. The structure of nuclear levels in 105 Rh is discussed briefly in terms of models applicable for nuclide in this mass region [pt

The sticking probability for H-2 on some transition metals at a hydrogen pressure of 1 bar

DEFF Research Database (Denmark)

Johansson, Martin; Lytken, Ole; Chorkendorff, Ib

2008-01-01

The sticking probability for hydrogen on films of Co, Ni, Cu, Ru, Rh, Pd, Ir, and Pt supported on graphite has been measured at a hydrogen pressure of 1 bar in the temperature range 40–200 °C. The sticking probability is found to increase in the order Ni, Co, Ir, Pd, Pt, Rh, and Ru at temperature...

Diamond nanoparticles as a support for Pt and PtRu catalysts for direct methanol fuel cells.

Science.gov (United States)

La-Torre-Riveros, Lyda; Guzman-Blas, Rolando; Méndez-Torres, Adrián E; Prelas, Mark; Tryk, Donald A; Cabrera, Carlos R

2012-02-01

Diamond in nanoparticle form is a promising material that can be used as a robust and chemically stable catalyst support in fuel cells. It has been studied and characterized physically and electrochemically, in its thin film and powder forms, as reported in the literature. In the present work, the electrochemical properties of undoped and boron-doped diamond nanoparticle electrodes, fabricated using the ink-paste method, were investigated. Methanol oxidation experiments were carried out in both half-cell and full fuel cell modes. Platinum and ruthenium nanoparticles were chemically deposited on undoped and boron doped diamond nanoparticles through the use of NaBH(4) as reducing agent and sodium dodecyl benzene sulfonate (SDBS) as a surfactant. Before and after the reduction process, samples were characterized by electron microscopy and spectroscopic techniques. The ink-paste method was also used to prepare the membrane electrode assembly with Pt and Pt-Ru modified undoped and boron-doped diamond nanoparticle catalytic systems, to perform the electrochemical experiments in a direct methanol fuel cell system. The results obtained demonstrate that diamond supported catalyst nanomaterials are promising for methanol fuel cells.

Performance PtSnRh electrocatalysts supported on carbon-Sb{sub 2}O{sub 5}.SbO{sub 2} for the electro-oxidation of ethanol, prepared by an alcohol-reduction process; Desempenho de eletrocatalisadores PtSnRh suportados em carbono-Sb{sub 2}O{sub 5}.SnO{sub 2} para a oxidacao eletroquimica do etanol, preparados pelo metodo de reducao por alcool

Energy Technology Data Exchange (ETDEWEB)

Castro, Jose Carlos

2013-07-01

PtSnRh electrocatalysts supported on carbon-Sb{sub 2}O{sub 5}.SnO{sub 2}, with metal loading of 20 wt%, were prepared by an alcohol-reduction process, using H{sub 2}PtCl{sub 6}.6H{sub 2}O (Aldrich), RhCl{sub 3}.xH{sub 2}O (Aldrich) and SnCl{sub 2}.2H{sub 2}O (Aldrich), as source of metals; Sb{sub 2}O{sub 5}.SnO{sub 2} (ATO) and carbon Vulcan XC72, as support; and ethylene glycol as reducing agent. The electrocatalysts obtained were characterized physically by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The diffractograms showed which PtSnRh/C-ATO electrocatalysts had FCC structure of Pt and Pt alloys, besides several peaks associated with SnO{sub 2} and ATO. The average sizes of crystallites were between 2 and 4 nm. TEM micrographs showed a good distribution of the nanoparticles on the support. The average sizes of particles were between 2 and 3 nm, with good agreement for the average size of the crystallites. The performances of the electrocatalysts were analyzed by electrochemical techniques and in real conditions of operation using single direct ethanol fuel cell. In the chronoamperometry at 50 deg C, the electrocatalysts with carbon (85 wt%) and ATO (15 wt%) support, showed the best activity, and the atomic proportions which achieved the best results were PtSnRh(70:25:05) e (90:05:05). PtSnRh(70:25:05)/85C+15ATO electrocatalysts showed the best performance in a direct ethanol fuel cell. (author)

Mixed-valent perovskites of the type Ba/sub 3/Bsup(III)PtRuO/sub 9/

Energy Technology Data Exchange (ETDEWEB)

Kemmler-Sack, S; Ehmann, A; Herrmann, M [Tuebingen Univ. (Germany, F.R.). Lehrstuhl fuer Anorganische Chemie 2

1981-08-01

Compounds of type Ba/sub 3/Bsup(III)PtRuO/sub 9/ - with a mean oxydation state of the noble metals of +4.5 - crystallize with Bsup(III) = Gd-Lu, Y in a variant of hexagonal BaTiO/sub 3/ type with ordered cationic distribution. Intensity calculations on powder data of Ba/sub 3/YPtRuO/sub 9/ (a = 5.88/sub 8/; c = 14.7/sub 0/ A) gave in the space group P6/sub 3//mmc (sequence (hcc)/sub 2/) a refined, intensity related R' value of 5.9%. With Bsup(III) = Eu the lattice is monoclinic and for Bsup(III) = Sm, Nd, La triclinic distorted.

Dynamics of electrocatalytic oxidation of ethylene glycol, methanol and formic acid at MWCNT platform electrochemically modified with Pt/Ru nanoparticles

CSIR Research Space (South Africa)

Maxakato, NW

2010-03-01

Full Text Available Comparative electrocatalytic behavior of functionalized multiwalled carbon nanotubes (fMWCNTs) electrodecorated with Pt/Ru nanoparticles towards the oxidation of methanol (MeOH), ethylene glycol (EG) and formic acid (FA) has been investigated...

Nano-composite of PtRu alloy electrocatalyst and electronically conducting polymer for use as the anode in a direct methanol fuel cell

Energy Technology Data Exchange (ETDEWEB)

Jongho Choi; Kyungwon Park; Hyekyung Lee; Youngmin Kim; Jaesuk Lee; Yungeun Sung [Kwangju Inst. of Science and Technology, Dept. of Materials Science and Engineering, Gwangju (Korea)

2003-08-15

Nano-composites comprised of PtRu alloy nanoparticles and an electronically conducting polymer for the anode electrode in direct methanol fuel cell (DMFC) were prepared. Two conducting polymers of poly(N-vinyl carbazole) and poly(9-(4-vinyl-phenyl)carbazole) were used for the nano-composite electrodes. Structural analyses were carried out using Fourier transform nuclear magnetic resonance spectroscopy, AC impedance spectroscopy, X-ray diffraction (XRD), and transmission electron microscopy (TEM). Electrocatalytic activities were investigated by voltammetry and chronoamperometry in a 2 M CH{sub 3}OH/{sub 0.5} M H{sub 2}SO{sub 4} solution and the data compared with a carbon-supported PtRu electrode. XRD patterns indicated good alloy formation and nano-composite formation was confirmed by TEM. Electrochemical measurements and DMFC unit-cell tests indicate that the nano-composites could be useful in a DMFC, but its performance would be slightly lower than that of a carbon-supported electrode. The interfacial property between the PtRu-polymer nano-composite anode and the polymer electrolyte was good, as evidenced by scanning electron microscopy. For better performance in a DMFC, a higher electric conductivity of the polymer and a lower catalyst loss are needed in nano-composite electrodes. (Author)

Inelastic scattering on 100Ru

International Nuclear Information System (INIS)

Sirota, S.

1987-01-01

Aspects of the nuclear structure of 100 Ru whe investigated by means of the scattering of 100 Ru (p,p') 100 Ru* with 16 MeV protons, where 21 states were investigated. The emergent protons were analysed by a magnetic spectrograph, of the enge type with a typical resolution of ≅ 9 KeV. (A.C.A.S.) [pt

New determination of the half-lives of 57Co, 103Ru, sup(103m)Rh, 103Pd, and 109Cd

International Nuclear Information System (INIS)

Vaninbroukx, R.; Grosse, G.; Zehner, W.

1981-01-01

The half-lives of five radionuclides were redetermined by photon-counting techniques using NaI(Tl)- and Si(Li) detectors. The results are: 57 Co: (271.90 +- 0.09)d, 103 Ru: (39.260 +- 0.020)d, sup(103m)Rh: (56.114 +- 0.020)m, 103 Pd: (16.991 +- 0.019)d, and 109 Cd: (461.90 +- 0.30)d. The quoted uncertainties, corresponding to a lσ level, take into account random and systematic uncertainties. (author)

γ - γ angular correlation in sup(100)Ru

International Nuclear Information System (INIS)

Kenchian, G.; Leljbman, I.D.G.; Cruz, M.T.F.

1990-01-01

The gamma-gamma directional angular correlations of coincident transitions have been measured in sup(100)Ru nuclide, following the β sup(+) and electron capture of sup(100)Rh using an angular correlation automatic spectrometer with two Ge(Li) detectors. The sup(100)Rh source has been produced with sup(100)Ru(p,n) sup(100)Rh reaction, using the proton beam of the Cyclotron Acelerator and enriched sup(100)Ru isotope. We have measured 30 direct cascades and 11 triple cascades. The spin and the parity of the 1865 KeV, 1881 KeV, 2099 KeV, 2167 KeV, 2241 KeV, 2517 KeV, and 3070 KeV levels have been established and multipole mixing ratios (δ) for 21 transitions have been obtained, 12 for the first time. Multipole mixing ratios Q sup(2)(E0/E2) has been also measured in the 2 sup(+) sub(2) → 2 sup(+) sub(1) transition. (author)

Conductivity study of thermally stabilized RuO2/polythiophene nanocomposites

Science.gov (United States)

Hebbar, Vidyashree; Bhajantri, R. F.

2018-04-01

The polymer nanocomposites of Ruthenium oxide (RuO2) filled polythiophene (PT) were synthesized by polymerization using chemical method. The purity of the synthesized polymer composite is verified using X-Ray diffraction (XRD). The structural discrepancies of the RuO2 filled PT composites are studied by Fourier transform infrared (FT-IR) spectroscopy. The phase transition and thermal stability of the prepared composite is revised by thermal characterization such as differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA). The DC conductivity of RuO2 filled PT composite in the form of pellets is calculated using current-voltage (I-V) characterization by two-probe method. The enhancement in conductivity with increased RuO2 content in PT matrix is examined, which is the required property for electrical and electronic applications in supercapacitors.

Fabrication of Nonenzymatic Glucose Sensors Based on Multiwalled Carbon Nanotubes with Bimetallic Pt-M (M = Ru and Sn Catalysts by Radiolytic Deposition

Directory of Open Access Journals (Sweden)

Sun-Young Kwon

2012-01-01

Full Text Available Nonenzymatic glucose sensors employing multiwalled carbon nanotubes (MWNTs with highly dispersed Pt-M (M = Ru and Sn nanoparticles (Pt-M@PVP-MWNTs were fabricated by radiolytic deposition. The Pt-M nanoparticles on the MWNTs were characterized by transmittance electron microscopy, elemental analysis, and X-ray diffraction. They were found to be well dispersed and to exhibit alloy properties on the MWNT support. Electrochemical testing showed that these nonenzymatic sensors had larger currents (mA than that of a bare glassy carbon (GC electrode and one modified with MWNTs. The sensitivity (A mM−1, linear range (mM, and detection limit (mM (S/N = 3 of the glucose sensor with the Pt-Ru catalyst in NaOH electrolyte were determined as 18.0, 1.0–2.5, 0.7, respectively. The corresponding data of the sensor with Pt-Sn catalyst were 889.0, 1.00–3.00, and 0.3, respectively. In addition, these non-enzymatic sensors can effectively avoid interference arising from the oxidation of the common interfering species ascorbic acid and uric acid in NaOH electrolyte. The experimental results show that such sensors can be applied in the detection of glucose in commercial red wine samples.

Investigation of nano Pt and Pt-based alloys electrocatalysts for direct methanol fuel cells and their properties

Directory of Open Access Journals (Sweden)

Chunguang Suo

2014-03-01

Full Text Available The electrocatalysts used in micro direct methanol fuel cell (μDMFC, such as Pt/C and Pt alloy/C, prepared by liquid-phase NaBH4 reduction method have been investigated. XC-72 (Cobalt corp. Company, U.S.A is chosen as the activated carrier for the electrocatalysts to keep the catalysts powder in the range of several nanometers. The XRD, SEM, EDX analyses indicated that the catalysts had small particle size in several nanometers, in excellent dispersed phase and the molar ratio of the precious metals was found to be optimal. The performances of the DMFCs using cathodic catalyst with Pt percentage of 30wt% and different anodic catalysts (Pt-Ru, Pt-Ru-Mo were tested. The polarization curves and power density curves of the cells were measured to determine the optimal alloy composition and condition for the electrocatalysts. The results showed that the micro direct methanol fuel cell with 30wt% Pt/C as the cathodic catalyst and n(Pt:n(Ru:n(Mo = 3:2:2 PtRuMo/C as the anodic catalyst at room temperature using 2.0mol/L methanol solution has the best performances.

X = Pt, Os, Ru, Ir, Rh

African Journals Online (AJOL)

Timothy Ademakinwa

The compressibility of five compounds in the stoichiometry X Al was evaluated from 0K to 2000K using the. 3 ... atom model framework, using the Sutton and Chen potentials. Keywords: ... However, alloys based on these ... computer code (Turodov et al., 2006). DL-POLY is a molecular dynamics (MD) simulation package.

The Effect of Surface Site Ensembles on the Activity and Selectivity of Ethanol Electrooxidation by Octahedral PtNiRh Nanoparticles.

Science.gov (United States)

Erini, Nina; Beermann, Vera; Gocyla, Martin; Gliech, Manuel; Heggen, Marc; Dunin-Borkowski, Rafal E; Strasser, Peter

2017-06-01

Direct ethanol fuel cells are attractive power sources based on a biorenewable, high energy-density fuel. Their efficiency is limited by the lack of active anode materials which catalyze the breaking of the C-C bond coupled to the 12-electron oxidation to CO 2 . We report shape-controlled PtNiRh octahedral ethanol oxidation electrocatalysts with excellent activity and previously unachieved low onset potentials as low as 0.1 V vs. RHE, while being highly selective to complete oxidation to CO 2 . Our comprehensive characterization and in situ electrochemical ATR studies suggest that the formation of a ternary surface site ensemble around the octahedral Pt 3 Ni 1 Rh x nanoparticles plays a crucial mechanistic role for this behavior. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electrochemical oxidation of methanol on Pt/(RuxSn1-xO2 nanocatalyst

Directory of Open Access Journals (Sweden)

Krstajić Mila N.

2013-01-01

Full Text Available The Ru-doped SnO2 powder, (RuxSn1-xO2, with the Sn:Ru atomic ratio of 9:1 was synthesized and used as a support for Pt nanoparticles (30 mass% loading. The (RuxSn1-xO2 support and Pt/(RuxSn1-xO2 catalyst were characterized by X-ray diffraction, energy dispersive X-ray spectroscopy and transmission electron microscopy (TEM. (RuxSn1-xO2 was found to be two-phase material consisting of probably solid solution of RuO2 in SnO2 and pure RuO2. The average Pt particle size determined by TEM was 5.3 nm. Cyclic voltammetry of Pt/(RuxSn1-xO2 indicated good conductivity of the sup-port and displayed usual features of Pt. The results of the electrochemical oxidation of COads and methanol on Pt/(RuxSn1-xO2 were compared with those on commercial Pt/C and PtRu/C catalysts. Oxidation of COads on Pt/(RuxSn1-xO2 starts at less positive potentials than on PtRu/C and Pt/C. Potentiodynamic polarization curves and chronoamperometric curves of methanol oxidation indicated higher initial activity of Pt/(RuxSn1-xO2 catalyst compared to PtRu/C, but also a greater loss in the current density over time. Potentiodynamic stability test of the catalysts revealed that deactivation of the Pt/(RuxSn1-xO2 and Pt/C was primarily caused by the poisoning of Pt surface by the methanol oxidation residues, which mostly occurred during the first potential cycle. In the case of PtRu/C the poisoning of the surface was minor and deactivation was caused by the PtRu surface area loss. [Projekat Ministarstva nauke Republike Srbije, br. ON-172054

Superconductivity and Competing Ordered Phase in RuPn (Pn = As, P)

Science.gov (United States)

Hirai, Daigorou; Takayama, Tomohiro; Hashizume, Daisuke; Yamamoto, Ayako; Takagi, Hidenori

2011-03-01

Unconventional superconductivity likely manifests itself when some competing electronic phases are suppressed down to zero temperature such as cuprates and iron-pnictide superconductors. Therefore, the correlated metallic state neighboring a competing electronic ordering can be a promising playground for unconventional superconductivity. Here we report superconductivity emerging adjacent to electronically ordered phases of RuPn (Pn = As, P). We found that RuAs(P) exhibits phase transitions at 240 (265) K, which is discerned as a drop of magnetic susceptibility or a resistivity upturn. Such anomalies can be suppressed by substituting Rh to the Ru site. Accompanied by the disappearance of the electronic order, superconductivity was found to emerge below 1.8 K and 3.8 K for RuAs and RuP, respectively. The superconductivity in Rh substituted RuPn, which neighbors a competing electronic order, might exhibit an exotic pairing state as seen in the unconventional superconductors known to date.

Room temperature magnetism of few-nanometers-thick Fe{sub 3}O{sub 4}(111) films on Pt(111) and Ru(0001) studied in ambient conditions

Energy Technology Data Exchange (ETDEWEB)

Lewandowski, M., E-mail: lewandowski@amu.edu.pl [NanoBioMedical Centre, Adam Mickiewicz University, Umultowska 85, 61-614 Poznań (Poland); Institute of Molecular Physics, Polish Academy of Sciences, M. Smoluchowskiego 17, 60-179 Poznań (Poland); Miłosz, Z.; Michalak, N.; Ranecki, R. [Institute of Molecular Physics, Polish Academy of Sciences, M. Smoluchowskiego 17, 60-179 Poznań (Poland); Sveklo, I.; Kurant, Z.; Maziewski, A. [Faculty of Physics, University of Białystok, Lipowa 41, 15-424 Białystok (Poland); Mielcarek, S. [Faculty of Physics, Adam Mickiewicz University, Umultowska 85, 61-614 Poznań (Poland); Luciński, T. [Institute of Molecular Physics, Polish Academy of Sciences, M. Smoluchowskiego 17, 60-179 Poznań (Poland); Jurga, S. [NanoBioMedical Centre, Adam Mickiewicz University, Umultowska 85, 61-614 Poznań (Poland)

2015-09-30

Few-nanometers-thick Fe{sub 3}O{sub 4}(111) films were epitaxially grown on Pt(111) and Ru(0001) single crystal supports by sequential iron deposition and oxidation in an ultra-high vacuum chamber. The growth of well-ordered magnetite films was confirmed by low energy electron diffraction. The films were covered with a protective Au layer and subjected to magnetic and structural studies in ambient conditions. Magnetic hysteresis loops, recorded using magneto-optical Kerr effect apparatus, confirmed magnetic ordering in both films at room temperature. The Kerr measurements indicated in-plane orientation of magnetization, which was supported by the lack of magnetic contrast in magnetic force microscopy images. Atomic force microscopy revealed significant differences in morphology of the films, tentatively attributed to different lattice mismatch with Pt(111) and Ru(0001) single crystal supports. - Highlights: • Few-nanometers-thick Fe{sub 3}O{sub 4}(111) films were grown on Pt(111) and Ru(0001). • Magnetic properties were studied using MOKE and AFM/MFM in ambient conditions. • The films exhibited in-plane magnetic ordering at room temperature. • Differences in magnetic properties were tentatively assigned to structural differences.

NO reduction by CO over noble-metal catalysts under cycled feedstreams

International Nuclear Information System (INIS)

Muraki, H.; Fujitani, Y.

1986-01-01

The reduction of NO with CO was studied over α-Al/sub 2/O/sub 3/-supported Pt, Pd, Rh, Ru, and Ir catalysts. The activities were measured by using cycled feeds and steady noncycled feed. The activity sequence of the catalysts tested was Rh > Ru > Ir > Pd > Pt. The activities of Pt and Pd catalysts were increased under the cycled feed. The periodic operation effect on the Pt catalyst was more predominant than that on the Pd catalyst. The order of periodic operation effect corresponded to the order of their susceptibility to CO self-poisoning

Preparation of Pb(Zr0.52Ti0.48)O3 thin films on Pt/RuO2 double electrode by a new sol-gel route

International Nuclear Information System (INIS)

Kim, S.; Choi, Y.; Kim, C.; Oh, Y.

1997-01-01

Pb(Zr 0.52 Ti 0.48 )O 3 (PZT) thin film on Pt/RuO 2 double electrode was successfully prepared by using new alkoxide endash alkanolamine, sol-gel method. It was observed that the use of Pt/RuO 2 double electrode reduced leakage current, resulting in a marked improvement in the leakage characteristics and more reliable capacitors. Typical P-E hysteresis behavior was observed even at low applied voltage of 5 V, manifesting greatly improved remanance and coercivity. Fatigue and breakdown characteristic, measured at 5 V, showed stable behavior and no degradation in polarization was observed up to 10 11 cycles.copyright 1997 Materials Research Society

Determination of Pt, Pd and Rh in Brassica Napus using solid sampling electrothermal vaporization inductively coupled plasma optical emission spectrometry

International Nuclear Information System (INIS)

Nischkauer, Winfried; Herincs, Esther; Puschenreiter, Markus; Wenzel, Walter; Limbeck, Andreas

2013-01-01

Conventional approaches for the analysis of platinum group elements (PGEs) in plant material suffer from sample digestion which results in sample dilution and therefore requires high sample intakes to maintain the sensitivity. The presented solid-sampling method avoids sample digestion while improving sensitivity when compared to digestion-based inductively coupled plasma optical emission spectrometry (ICP-OES) methods and allows the analysis of sample masses of 5 mg or less. Detection limits of 0.38 μg g −1 , 0.14 μg g −1 and 0.13 μg g −1 were obtained for Pt, Pd and Rh, respectively using a sample intake of 5 mg. The reproducibility of the procedure ranged between 4.7% (Pd) relative standard deviation (RSD, n = 7) and 7.1% (Rh) RSD for 25 ng analytes. For quantification, aqueous standards were applied on paper filter strips and dried. Only the dried filters were introduced into the electrothermal vaporization unit. This approach successfully removed memory-effects observed during analysis of platinum which occurred only if liquid standards came into contact with the graphite material of the furnace. The presented method for overcoming the Pt-memory-effects may be of further interest for the analysis of other carbide-forming analytes as it does not require any technical modification of the graphite furnace (e.g., metal inlays, pyrolytic coating). Owing to lack of suitable certified reference materials, the proposed method was compared with conventional ICP-OES analysis of digested samples and a good agreement was obtained. As a result of the low sample consumption, it was possible to determine the spatial distribution of PGEs within a single plant. Significant differences in PGE concentrations were observed between the shoots (stem, leaves) and the roots. Pd was mainly found in the roots, whereas Pt and Rh were also found in higher concentrations in the shoots. - Highlights: • The uptake of Pt, Pd and Rh by hydroponically grown plants was investigated

Determination of Pt, Pd and Rh in Brassica Napus using solid sampling electrothermal vaporization inductively coupled plasma optical emission spectrometry

Energy Technology Data Exchange (ETDEWEB)

Nischkauer, Winfried [Vienna University of Technology, Institute of Chemical Technologies and Analytics, Division of Instrumental Analytical Chemistry, Getreidemarkt 9/164-IAC, A-1060 Vienna (Austria); Herincs, Esther [Vienna University of Technology, Institute of Chemical Technologies and Analytics, Division of Instrumental Analytical Chemistry, Getreidemarkt 9/164-IAC, A-1060 Vienna (Austria); University of Natural Resources and Life Sciences, Department of Forest and Soil Sciences, Institute of Soil Research, Konrad Lorenz Straße 24, A-3430 Tulln (Austria); Puschenreiter, Markus; Wenzel, Walter [University of Natural Resources and Life Sciences, Department of Forest and Soil Sciences, Institute of Soil Research, Konrad Lorenz Straße 24, A-3430 Tulln (Austria); Limbeck, Andreas, E-mail: A.Limbeck@tuwien.ac.at [Vienna University of Technology, Institute of Chemical Technologies and Analytics, Division of Instrumental Analytical Chemistry, Getreidemarkt 9/164-IAC, A-1060 Vienna (Austria)

2013-11-01

Conventional approaches for the analysis of platinum group elements (PGEs) in plant material suffer from sample digestion which results in sample dilution and therefore requires high sample intakes to maintain the sensitivity. The presented solid-sampling method avoids sample digestion while improving sensitivity when compared to digestion-based inductively coupled plasma optical emission spectrometry (ICP-OES) methods and allows the analysis of sample masses of 5 mg or less. Detection limits of 0.38 μg g{sup −1}, 0.14 μg g{sup −1} and 0.13 μg g{sup −1} were obtained for Pt, Pd and Rh, respectively using a sample intake of 5 mg. The reproducibility of the procedure ranged between 4.7% (Pd) relative standard deviation (RSD, n = 7) and 7.1% (Rh) RSD for 25 ng analytes. For quantification, aqueous standards were applied on paper filter strips and dried. Only the dried filters were introduced into the electrothermal vaporization unit. This approach successfully removed memory-effects observed during analysis of platinum which occurred only if liquid standards came into contact with the graphite material of the furnace. The presented method for overcoming the Pt-memory-effects may be of further interest for the analysis of other carbide-forming analytes as it does not require any technical modification of the graphite furnace (e.g., metal inlays, pyrolytic coating). Owing to lack of suitable certified reference materials, the proposed method was compared with conventional ICP-OES analysis of digested samples and a good agreement was obtained. As a result of the low sample consumption, it was possible to determine the spatial distribution of PGEs within a single plant. Significant differences in PGE concentrations were observed between the shoots (stem, leaves) and the roots. Pd was mainly found in the roots, whereas Pt and Rh were also found in higher concentrations in the shoots. - Highlights: • The uptake of Pt, Pd and Rh by hydroponically grown plants was

Electrochemical oxidation of ethanol using PtRh/C electrocatalysts in alkaline medium and synthesized by sodium borohydride and alcohol reduction; Oxidação eletroquímica do etanol utilizando eletrocatalisadores PtRh/C em meio alcalino e sintetizados via borohidreto de sódio e redução por álcool

Energy Technology Data Exchange (ETDEWEB)

Fontes, Eric Hossein

2017-07-01

PtRh/C were prepared by the following atomic proportions: (100,0), (0,100), (90,10), (70,30) and (50,50). The methods employed in the synthesis of these materials were reduction by sodium borohydride and reduction by alcohol. The metal salts used were H{sub 2}PtCl{sub 6}3•6H{sub 2}0 and (RhNO{sub 3}){sub 3}, the support used was Carbon black XC72 and the bulk metal composition was 20% and 80% of support. The electrocatalysts were characterized by Energy Dispersive X-ray spectroscopy, X-ray diffraction and Transmission electron microscopy. The ethanol electrochemical oxidation mechanism was investigated by in situ Fourier Transform Infrared Spectroscopy couple to an Attenuated Total Reflection technique. The electrocatalytic activity were evaluated by Cyclic Voltammetry, Linear Sweep Voltammetry and Chronoamperometry techniques. The Fuel Cells tests were made in a single direct alcohol fuel cell with alkaline membrane. The working electrodes were prepared by a thin porous coating technique. X-ray diffraction allowed to verify metallic alloys, segregate phases and to calculate the percentage of metallic alloys. It was else possible to identify crystallographic phases. Infrared Spectroscopy allowed to verify that the electrochemical oxidation of ethanol was carried out by an incomplete mechanism. PtRh(70:30)/C prepared by sodium borohydride produced large amounts of carbon dioxide and acetaldehyde. Rh/C showed electrocatalytic activity when compared with other materials studied.

CoFeRh alloys

International Nuclear Information System (INIS)

Tabakovic, Ibro; Qiu Jiaoming; Riemer, Steve; Sun Ming; Vas'ko, Vlad; Kief, Mark

2008-01-01

The electrochemical behavior of Rh(III) species in CoFe solution containing RhCl 3 , NH 4 Cl, H 3 BO 3 , CoSO 4 , FeSO 4 , saccharin, and NaLS (Na lauryl sulfate) has been investigated. The electrochemistry of Rh(III) species is influenced by each of the compounds present in CoFe plating solution, but especially by addition of saccharin and H 3 BO 3 to the RhCl 3 -NH 4 Cl solution. The nucleation and growth of Rh on GC (glassy carbon), Ru, and Cu electrodes from NH 4 Cl solution was studied using the potentiostatic current-transient methods. The results support a predominantly progressive nucleation of Rh on all three-electrode surfaces. The nucleation kinetic parameters ANo (steady state nucleation rate) and Ns (saturation nuclear number density) were found to vary with potential and are electrode-dependent in order: GC > Ru∼Cu. The electrodeposited Rh films obtained from NH 4 Cl solution and nonmagnetic CoFeRh film obtained from CoFe solution were characterized in terms of the following properties: morphology, surface roughness, crystal structure and chemical composition. The origin of light elements found in Rh and CoFeRh films (O, Cl, S, C, N) was discussed

Pt-Rh/g Al2O3 Influence of Catalyst Preparation Methods on Metallic Particle Dispersion and Size Distribution

Directory of Open Access Journals (Sweden)

N.M. da Fonseca

1998-06-01

Full Text Available - Pt-Rh/Al2O3 catalysts were prepared by successive incipient impregnations or coimpregnation. Characterization was achieved by H2 chemisorption and transmission electron microscopy. It was verified that method of preparation, ratio of metal weights and sequence of deposition are factors that result in very distinct catalysts.

Isolation and X-ray structures of four Rh(PCP) complexes including a Rh(I) dioxygen complex with a short O-O bond

KAUST Repository

Hayashi, Yukiko

2013-07-01

The reaction of RhCl3·H2O with tBu2P(CH2)5PtBu 2 afforded several complexes including [RhIII(H)Cl{ tBu2- P(CH2)2CH(CH2) 2PtBu2}] (1), [RhIIIHCl 2{tBu2P(CH2)5P tBu2}]2 (2), [RhICl{ tBu2P(CH2)2CH=CHCH2P tBu2}] (3) and [RhICl{tBu 2PCH2C(O)CH=CHCH2PtBu2}] (4). X-ray crystal structures of 3 and 4 showed that the C=C bond on the C 5 unit of tBu2P(CH2) 5PtBu2 is bound to Rh(I) in a η2 configuration. In 4, the Rh atom has a trigonal pyramidal coordination geometry. The X-ray crystal structure of 2 consists of two rhodium( III) centers bridged by two tBu2P(CH2)5P tBu2 ligands with two phosphorus atoms, one from each ligand, trans to one another. The crystal structure of the rhodium oxygen adduct with 1,3-bis(di-t-butylphosphinomethyl) benzene [RhO2{ tBu2PCH2(C6H3)CH 2PtBu2}] (5) was also investigated. In this species the O2 is η2 coordinated to the Rh(I) center with asymmetric Rh-O bond lengths (2.087(7) and 1.998(8) Å). The O-O bond distance is short (1.337(11) Å) with νO-O of 990.5 cm -1. DFT calculations on complex 5 yielded two η2- O2 structures that differed in energy by only 0.76 kcal/mol. The lower energy one (5a) had near C2 symmetry, and had nearly equal Rh-O bond lengths, while the higher energy structure (5b) had near Cs symmetry and generally good agreement with the experimental structure. The calculated UV-Vis and IR spectra of complex 5 are in excellent agreement with experiment. © 2012 Elsevier Ltd. All rights reserved.

Isolation and X-ray structures of four Rh(PCP) complexes including a Rh(I) dioxygen complex with a short O-O bond

KAUST Repository

Hayashi, Yukiko; Szalda, David J.; Grills, David C.; Hanson, Jonathan C.; Huang, Kuo-Wei; Muckerman, James T.; Fujita, Etsuko

2013-01-01

The reaction of RhCl3·H2O with tBu2P(CH2)5PtBu 2 afforded several complexes including [RhIII(H)Cl{ tBu2- P(CH2)2CH(CH2) 2PtBu2}] (1), [RhIIIHCl 2{tBu2P(CH2)5P tBu2}]2 (2), [RhICl{ tBu2P(CH2)2CH=CHCH2P tBu2}] (3) and [RhICl{tBu 2PCH2C(O)CH=CHCH2PtBu2}] (4). X-ray crystal structures of 3 and 4 showed that the C=C bond on the C 5 unit of tBu2P(CH2) 5PtBu2 is bound to Rh(I) in a η2 configuration. In 4, the Rh atom has a trigonal pyramidal coordination geometry. The X-ray crystal structure of 2 consists of two rhodium( III) centers bridged by two tBu2P(CH2)5P tBu2 ligands with two phosphorus atoms, one from each ligand, trans to one another. The crystal structure of the rhodium oxygen adduct with 1,3-bis(di-t-butylphosphinomethyl) benzene [RhO2{ tBu2PCH2(C6H3)CH 2PtBu2}] (5) was also investigated. In this species the O2 is η2 coordinated to the Rh(I) center with asymmetric Rh-O bond lengths (2.087(7) and 1.998(8) Å). The O-O bond distance is short (1.337(11) Å) with νO-O of 990.5 cm -1. DFT calculations on complex 5 yielded two η2- O2 structures that differed in energy by only 0.76 kcal/mol. The lower energy one (5a) had near C2 symmetry, and had nearly equal Rh-O bond lengths, while the higher energy structure (5b) had near Cs symmetry and generally good agreement with the experimental structure. The calculated UV-Vis and IR spectra of complex 5 are in excellent agreement with experiment. © 2012 Elsevier Ltd. All rights reserved.

Pt{sub X}Ru{sub Y}Ir{sub Z} as a bifunctional electrocatalyst for oxygen reduction reaction in a PEM fuel cell; Pt{sub X}Ru{sub Y}Ir{sub Z} como electrocatalizador bifuncional para la reaccion redox del oxigeno en una celda tipo PEM

Energy Technology Data Exchange (ETDEWEB)

Morales, L.; Fernandez, A.M. [Centro de Investigacion en Energia, Universidad Nacional Autonoma de Mexico, Temixco, Morelos (Mexico)]. E-mail: limos@cie.unam.mx; Cano, U. [Instituto de Investigaciones Electricas, Cuernavaca, Morelos (Mexico)

2009-09-15

This work presents the synthesis and characterization of the ternary material Pt{sub X}Ru{sub Y}Ir{sub Z}, obtained by chemical reduction with NaBH{sub 4}. Two different atomic compositions were developed (sample A and B) in order to observe the kinetic effect, as suggested by the combinatorial libraries. The main objective of this synthesis is to study the oxygen reduction reaction (ORR and OER) and its potential use in the construction of a bifunctional catalyst. In addition, each of the metals are synthesized separately using the same technique in order to make the corresponding comparison. The compounds obtained were characterized by sweep electron microscopy, x-ray diffraction and composition using fluorescence and energy-dispersive x-ray spectroscopy. The results showed a displacement of the x-ray diffraction peaks for Ir and Pt in sample A, and displacement in sample B for Ru and Ir peaks. These changes suggest the possible formation of a solid solution substitution. Separate cyclic and linear voltamperometry studies were performed for the oxygen reduction and release reactions. The electrochemical analysis showed improved kinetic behavior when combining the three metals according to the composition of sample B. [Spanish] En este trabajo se presenta la sintesis y caracterizacion del material ternario Pt{sub X}Ru{sub Y}Ir{sub Z}, elaborado por la tecnica de Reduccion Quimica utilizando al NaBH{sub 4}. Se elaboraron dos composiciones atomicas diferentes (Muestra A y B) con el fin de observar el efecto cinetico, como lo sugieren las librerias combinatorias. El objetivo principal de esta sintesis es para el estudio de la Reaccion Redox del Oxigeno (RRO y REO) y su potencial uso para la construccion de un catalizador bifuncional. Asi mismo, se realiza la sintesis de cada uno de los metales por separado empleando la misma tecnica, con el proposito de realizar la comparacion correspondiente. Los compuestos obtenidos se caracterizaron por Microscopia Electronica de

PALLADIUM, PLATINUM, RHODIUM, RUTHENIUM AND IRIDIUM IN PERIDOTITES AND CHROMITITES FROM OPHIOLITE COMPLEXES IN NEWFOUNDLAND.

Science.gov (United States)

Page, Norman J; Talkington, Raymond W.

1984-01-01

Samples of spinel lherzolite, harzburgite, dunite, and chromitite from the Bay of Islands, Lewis Hills, Table Mountain, Advocate, North Arm Mountain, White Hills Periodite Point Rousse, Great Bend and Betts Cove ophiolite complexes in Newfoundland were analyzed for the platinum-group elements (PGE) Pd, Pt, Rh, Ru and Ir. The ranges of concentration (in ppb) observed for all rocks are: less than 0. 5 to 77 (Pd), less than 1 to 120 (Pt), less than 0. 5 to 20 (Rh), less than 100 to 250 (Ru) and less than 20 to 83 (Ir). Chondrite-normalized PGE ratios suggest differences between rock types and between complexes. Samples of chromitite and dunite show relative enrichment in Ru and Ir and relative depletion in Pt and Pd.

Photoemission study of 5f localization in UPd/sub 3-x/(Pt,Rh)/sub x/

International Nuclear Information System (INIS)

Arko, A.J.; Koelling, D.D.; Dunlap, B.D.; Mitchell, A.W.

1987-10-01

Photoemission measurements in the two systems UPd/sub 3-x/(Pt,Rh)/sub x/ show that the 5f spectra are consistent with localized 5f electrons (peak in spectral weight is below E/sub F/ for all x within the double hexagonal DO 24 phase) while at both phase transitions the 5f peaks lock in at E/sub F/ consistent with intinerancy. A satellite 5f peak representative of d-screening is observed in both localized and itinerant systems. 17 refs., 3 figs

Effect of the solvent in the catalyst ink preparation on the properties and performance of unsupported PtRu catalyst layers in direct methanol fuel cells

International Nuclear Information System (INIS)

Alcaide, Francisco; Álvarez, Garbiñe; Cabot, Pere L.; Genova-Koleva, Radostina; Grande, Hans-Jürgen; Miguel, Oscar

2017-01-01

The effect of the organic solvent polarity on the properties of unsupported PtRu catalyst inks and on the performance of the catalyst layers prepared with them for the methanol electrooxidation, has been studied. The light scattering results indicate that the PtRu-Nafion ® aggregates in the inks prepared with n-butyl acetate (NBA) are larger than those prepared with 2-propanol (IPA). The lower polarity of the former favours the aggregation of Nafion ® and nanoparticles. The electron microscopy images and porosimetry measurements of the catalyst layers show that the secondary pore volume between the agglomerates is larger for NBA. The linear sweep voltammetry and eis results for the methanol electrooxidation in the three-electrode cell denote the higher active surface area for NBA and comparable specific oxidation rates of the intermediates in both catalysts layers. The current densities for PtRu anode catalyst layers in single DMFC are higher when the solvent is NBA, the mass transport limitations being much more apparent with IPA. The adapted transmission line equivalent circuit to interpret the impedance results in single DMFC indicates that the proton resistance for NBA is significantly lower than for IPA, thus suggesting that the greater number of accessible active sites for methanol oxidation in the former are well connected to the Nafion ® ionomers and easier transported to the membrane.

Investigation of the problems associated with the Pt-20 Rh clads of the viking heat sources VF-3 and VF-7

International Nuclear Information System (INIS)

Zielinski, R.E.

1975-01-01

The investigation was undertaken to determine why the emissive coatings of the Viking Heat Sources VF-3 and VF-7 had flaked off the Pt-20 Rh clad material. During the course of the investigation, two additional, unusual phenomena were observed: a surface reaction zone on the uncoated Pt-20 Rh surfaces and grain boundary reactions in the weld zone of the clad. It seems that all three phenomena were the result of a complicated reaction couple that involved the heat source materials, storage container materials, and environment. Vapor transport mechanisms were responsible for the phenomena which were observed. The vapor transport mechanisms were probably initiated because of the impurities that were in both the heat source and storage container materials. The mechanisms resulted in significant changes in these heat sources because vapor transport was allowed to continue in a static environment for an unusually long period of time. (U.S.)

The sticking probability for H-2 in presence of CO on some transition metals at a hydrogen pressure of 1 bar

DEFF Research Database (Denmark)

Johansson, Martin; Lytken, Ole; Chorkendorff, Ib

2008-01-01

The sticking probability for H-2 on Ni, Co, Cu, Rh, Ru, Pd, it and Pt metal films supported on graphite has been investigated in a gas mixture consisting of 10 ppm carbon monoxide in hydrogen at a total pressure of 1 bar in the temperature range 40-200 degrees C. Carbon monoxide inhibits the stic......The sticking probability for H-2 on Ni, Co, Cu, Rh, Ru, Pd, it and Pt metal films supported on graphite has been investigated in a gas mixture consisting of 10 ppm carbon monoxide in hydrogen at a total pressure of 1 bar in the temperature range 40-200 degrees C. Carbon monoxide inhibits...... the sticking probability significantly for all the metals, even at 200 degrees C. In the presence of 10 ppm CO, the sticking probability increases in the order It, Pt, Ni, Co, Pd, Rh, Ru, whereas for Cu, it is below the detection limit of the measurement, even in pure H2. The sticking probability for H2...

Comparison of radiation detector performance for different metal contacts on CdZnTe deposited by electroless deposition method

Energy Technology Data Exchange (ETDEWEB)

Zheng, Q.; Dierre, F.; Crocco, J.; Bensalah, H.; Dieguez, E. [Crystal Growth Laboratory, Department of Materials Physics, Universidad Autonoma de Madrid, 28049 Madrid (Spain); Ayoub, M. [Durham Scientific Crystals Laboratory, Netpark, Thomas Wright Way, Sedgefield, TS21, 3FD (United Kingdom); Corregidor, V.; Alves, E. [Unidade de Fisica e Aceleradores, LFI, ITN, E.N.10, 2686-953, Sacavem (Portugal); Fernandez-Ruiz, R. [Servicio Interdepartamental de Investigacion. Laboratorio de TXRF/Laue-XRD. Facultad de Ciencias, Universidad Autonoma de Madrid, 28049 Madrid (Spain); Perez, J.M. [CIEMAT, Edificio 22, Avda Complutense 22, 28040 Madrid (Spain)

2011-11-15

A comparative study of four different metals gold (Au), platinum (Pt), ruthenium (Ru) and rhodium (Rh) deposited on CdZnTe(CZT) by the electroless deposition method has been carried out. Two of these materials, Ru and Rh, have been deposited for the first time by this method. In contrast to the Pt deposition, the deposition of Ru and Rh were not carried out under the optimal conditions. The metals deposited on the samples were identified by Total reflection X-ray Fluorescence (TXRF). Rutherford Backscattering Spectrometry (RBS) analyses show that Au forms the thickest layer ({proportional_to}160 nm) for the experimental conditions of this work. Current-voltage measurements show that Pt forms a more linear ohmic contact with the lowest leakage current. A {sup 57}Co gamma ray spectrum gave a better detector performance with a FWHM 11 keV at 122 keV. (copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

Lipid solubility of the platinum group metals Pt, Pd and Rh in dependence on the presence of complexing agents

International Nuclear Information System (INIS)

Zimmermann, Sonja; Menzel, Christoph M.; Stueben, Doris; Taraschewski, Horst; Sures, Bernd

2003-01-01

All complexing agents had a significant influence on octanol solubility of PGM. - Investigations on the bioaccumulation of the platinum group metals (PGM) Pt, Pd and Rh in aquatic organisms are of growing interest in environmental research due to the increasing emission of these metals by motor vehicles with catalytic converters. Until now, nothing is known about the possible influence of complexing agents on the bioaccumulation capacity of these precious metals. According to the partition coefficient between 1-octanol and water (P OW ) as a measure of bioaccumulation, in this study a simple shaking method was performed in order to investigate the effects of different complexing agents (L-methionine, thio urea, EDTA, humic substances, bile compounds) on the octanol solubility of the PGM. The results demonstrated a significant influence of all agents used. L-Methionine and thio urea decreased the lipid solubility. In contrast, the presence of EDTA, humic substances and especially bile caused a higher transfer of metals in the octanol phase. For most complexing agents tested, the transfer of Pd to the lipid phase was significantly higher compared with Rh and Pt, except for bile acid where the highest octanol solubility was found for Pt. Recent experimental results on PGM accumulation in zebra mussels confirm a high bioaccumulation of Pd which could be predicted from the lipid solubility

Lipid solubility of the platinum group metals Pt, Pd and Rh in dependence on the presence of complexing agents

Energy Technology Data Exchange (ETDEWEB)

Zimmermann, Sonja; Menzel, Christoph M.; Stueben, Doris; Taraschewski, Horst; Sures, Bernd

2003-07-01

All complexing agents had a significant influence on octanol solubility of PGM. - Investigations on the bioaccumulation of the platinum group metals (PGM) Pt, Pd and Rh in aquatic organisms are of growing interest in environmental research due to the increasing emission of these metals by motor vehicles with catalytic converters. Until now, nothing is known about the possible influence of complexing agents on the bioaccumulation capacity of these precious metals. According to the partition coefficient between 1-octanol and water (P{sub OW}) as a measure of bioaccumulation, in this study a simple shaking method was performed in order to investigate the effects of different complexing agents (L-methionine, thio urea, EDTA, humic substances, bile compounds) on the octanol solubility of the PGM. The results demonstrated a significant influence of all agents used. L-Methionine and thio urea decreased the lipid solubility. In contrast, the presence of EDTA, humic substances and especially bile caused a higher transfer of metals in the octanol phase. For most complexing agents tested, the transfer of Pd to the lipid phase was significantly higher compared with Rh and Pt, except for bile acid where the highest octanol solubility was found for Pt. Recent experimental results on PGM accumulation in zebra mussels confirm a high bioaccumulation of Pd which could be predicted from the lipid solubility.

[Zn(NH3)4][PtCl6] and [Cd(NH3)4][PtCl6] as precursors for intermetallic compounds PtZn and PtCd

International Nuclear Information System (INIS)

Zadesenets, A.V.; Venediktov, A.B.; Shubin, Yu.V.; Korenev, S.V.

2007-01-01

Double complex salts (tetraamminezinc and tetraamminecadmium hexachloroplatinates) have been synthesized. Their thermal properties have been studied, as well as the products of their degradation in hydrogen and helium atmospheres. Optimal thermolysis schedules have been determined. Thermolysis under hydrogen yields intermetallic compounds PtZn and PtCd [ru

Low-Temperature Preparation of (111)-oriented Pb(Zr,Ti)O3 Films Using Lattice-Matched (111)SrRuO3/Pt Bottom Electrode by Metal-Organic Chemical Vapor Deposition

Science.gov (United States)

Kuwabara, Hiroki; Sumi, Akihiro; Okamoto, Shoji; Hoko, Hiromasa; Cross, Jeffrey S.; Funakubo, Hiroshi

2009-04-01

Pb(Zr0.35Ti0.65)O3 (PZT) films 170 nm thick were prepared at 415 °C by pulsed metal-organic chemical vapor deposition. The (111)-oriented PZT films with local epitaxial growth were obtained on (111)SrRuO3/(111)Pt/TiO2/SiO2/Si substrates and their ferroelectricities were ascertained. Ferroelectricity was improved by postannealing under O2 gas flow up to 550 °C. Larger remanent polarization and better fatigue endurance were obtained using a SrRuO3 top electrode compared to a Pt top electrode for PZT films after annealing at 500 °C.

London penetration depth measurements in Ba (Fe_1-xT_x)₂As₂(T=Co,Ni,Ru,Rh,Pd,Pt,Co+Cu) superconductors

Energy Technology Data Exchange (ETDEWEB)

Gordon, Ryan T. [Iowa State Univ., Ames, IA (United States)

2011-01-01

The London penetration depth has been measured in various doping levels of single crystals of Ba(Fe_1-xT_x)₂As₂ (T=Co,Ni,Ru,Rh,Pd,Pt,Co+Cu) superconductors by utilizing a tunnel diode resonator (TDR) apparatus. All in-plane penetration depth measurements exhibit a power law temperature dependence of the form Δλ_ab(T) = CTⁿ, indicating the existence of low-temperature, normal state quasiparticles all the way down to the lowest measured temperature, which was typically 500 mK. Several different doping concentrations from the Ba(Fe_1-xT_x)₂As₂ (T=Co,Ni) systems have been measured and the doping dependence of the power law exponent, n, is compared to results from measurements of thermal conductivity and specific heat. In addition, a novel method has been developed to allow for the measurement of the zero temperature value of the in-plane penetration depth, λ_ab(0), by using TDR frequency shifts. By using this technique, the doping dependence of λ_ab(0) has been measured in the Ba(Fe_1-xCo_x)₂As₂ series, which has allowed also for the construction of the doping-dependent superfluid phase stiffness, ρ_s(T) = [λ(0)/λ(T)]². By studying the effects of disorder on these superconductors using heavy ion irradiation, it has been determined that the observed power law temperature dependence likely arises from pair-breaking impurity scattering contributions, which is consistent with the proposed s±-wave symmetry of the superconducting gap in the dirty scattering limit. This hypothesis is supported by the measurement of an exponential temperature dependence of the penetration depth in the intrinsically clean LiFeAs, indicative of a nodeless superconducting gap.

Salt-induced phase separation for the determination of metals as their diethyldithiocarbamate complexes by high-performance liquid chromatography

International Nuclear Information System (INIS)

Mueller, B.J.; Lovett, R.J.

1987-01-01

Reversed-phase high-performance liquid chromatography with ultraviolet detection can be used to determine trace levels of Pt(II), Pd(II), Rh(III), Co(III), Ru(III), and Ir in aqueous solution following complexation with diethyldithiocarbamate. The metal complexes are extracted into acetonitrile from aqueous solution by the addition of a saturated salt solution. Quantitative metal recovery from aqueous solution is achievable for most metals for a wide solution pH range. Detection limits for the metals are <3 ng of metal/mL of original aqueous sample. Analyses of real samples are highly reproducible and sensitive. Ir an interfere in the determination of Pt(II) and Rh(III). A general protocol for chromatographic separation and determination of Pt(II), Pd(II), Rh(III), Ru(III), and Ir in aqueous solution is presented

The influence of methanol on the chemical state of PtRu anodes in a high-temperature direct methanol fuel cell studied in situ by synchrotron-based near-ambient pressure x-ray photoelectron spectroscopy

International Nuclear Information System (INIS)

Saveleva, Viktoriia A; Savinova, Elena R; Daletou, Maria K

2017-01-01

Synchrotron radiation-based near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) has recently become a powerful tool for the investigation of interfacial phenomena in electrochemical power sources such as batteries and fuel cells. Here we present an in situ NAP-XPS study of the anode of a high-temperature direct methanol fuel cell with a phosphoric acid-doped hydrocarbon membrane, which reveals an enhanced flooding of the Pt 3 Ru anode with phosphoric acid in the presence of methanol. An analysis of the electrode surface composition depending on the cell voltage and on the presence of methanol reveals the strong influence of the latter on the extent of Pt oxidation and on the transformation of Ru into Ru (IV) hydroxide. (paper)

The influence of methanol on the chemical state of PtRu anodes in a high-temperature direct methanol fuel cell studied in situ by synchrotron-based near-ambient pressure x-ray photoelectron spectroscopy

Science.gov (United States)

Saveleva, Viktoriia A.; Daletou, Maria K.; Savinova, Elena R.

2017-01-01

Synchrotron radiation-based near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) has recently become a powerful tool for the investigation of interfacial phenomena in electrochemical power sources such as batteries and fuel cells. Here we present an in situ NAP-XPS study of the anode of a high-temperature direct methanol fuel cell with a phosphoric acid-doped hydrocarbon membrane, which reveals an enhanced flooding of the Pt3Ru anode with phosphoric acid in the presence of methanol. An analysis of the electrode surface composition depending on the cell voltage and on the presence of methanol reveals the strong influence of the latter on the extent of Pt oxidation and on the transformation of Ru into Ru (IV) hydroxide.

High pressure stability of the monosilicides of cobalt and the platinum group elements

International Nuclear Information System (INIS)

Hernandez, J.A.; Vočadlo, L.; Wood, I.G.

2015-01-01

Highlights: • We model the high-pressure phases of cobalt- and platinum-group-monosilicides. • CoSi, RuSi, OsSi transform with pressure from the ε-FeSi to the CsCl structure. • RhSi and IrSi transform with pressure from the MnP structure to the ε-FeSi structure. • PdSi and PtSi transform with pressure from the MnP structure to the CuTi structure. - Abstract: The high pressure stability of CoSi, RuSi, RhSi, PdSi, OsSi, IrSi and PtSi was investigated by static first-principles calculations up to 300 GPa at 0 K. As found experimentally, at atmospheric pressure, CoSi, RuSi and OsSi were found to adopt the cubic ε-FeSi structure (P2 1 3) whereas RhSi, PdSi, IrSi and PtSi were found to adopt the orthorhombic MnP (Pnma) structure. At high pressure, CoSi, RuSi and OsSi show a phase transition to the CsCl structure (Pm3 ¯ m) structure at 270 GPa, 7 GPa and 6 GPa respectively. RhSi and IrSi were found to transform to an ε-FeSi structure at 10 GPa and 25 GPa. For PdSi and PtSi, a transformation from the MnP structure to the tetragonal CuTi structure (P4/nmm) occurs at 13 GPa and 20 GPa. The pressure dependence of the electronic density of states reveals that RuSi and OsSi are semiconductors in the ε-FeSi structure and become metallic in the CsCl structure. RhSi and IrSi are metals in the MnP structure and become semimetals in their high pressure ε-FeSi form. CoSi in the ε-FeSi configuration is a semimetal. PdSi and PtSi remain metallic throughout up to 300 GPa

Investigation of the magnetic phase transition in thin Fe{sub 50}Pt{sub 50-x}Rh{sub x} films by neutron diffraction

Energy Technology Data Exchange (ETDEWEB)

Fenske, Jochen; Lott, Dieter; Schreyer, Andreas [GKSS Research Centre, Geesthacht (Germany); Mankey, Gary J. [MINT Center, The University of Alabama, Tuscaloosa, AL (United States); Schmidt, Wolfgang; Schmalzl, Karin [JCNS, Juelich (Germany)

2008-07-01

In the last years perpendicular recording plays a major role in the development of novel magnetic data storage. Here, materials with high anisotropy are used which delivers good thermal stability. However in order to write the bits a high magnetic field is necessary. By the use of soft underlayers the write field can be significant reduced. Fe{sub 50}Pt{sub 50-x}Rh{sub x} is a promising candidate for such an underlayer. Magnetization measurements of the bulk samples for x=10 refer to a antiferromagnetic (AF)/ferromagnetic (FM) phase transition at about 150 K when heated. Additional magnetostriction measurements indicate that the phase transition could also be induced by applying a magnetic field. The FM state lowers the high anisotropy and therefore the high write field. The AF state helps to stabilize the recording media via exchange interaction. For technical applications the use of thin films are essential to save space and costs for the next generation of magnetic storage devices. Here we present results on several thin Fe{sub 50}Pt{sub 50-x}Rh{sub x} films with different concentration of Rh. The films were examined by polarized and unpolarized neutron diffraction in dependence of temperature and magnetic field.

Use of Dendrimers during the Synthesis of Pt-Ru Electrocatalysts for PEM Fuel Cells: Effects on the Physical and Electrochemical Properties

Directory of Open Access Journals (Sweden)

J. C. Calderón

2011-01-01

Full Text Available In this work, Pt-Ru catalysts were synthesized by a novel methodology which includes the use as encapsulating molecules of dendrimers of different generation: zero (DN-0, one (DN-1, two (DN-2, and three (DN-3. Synthesized catalysts were heat-treated at 350°C, and the effects of this treatment was established from the physical (X-ray dispersive energy (XDE and X-ray diffraction (XRD and electrochemical characterization (cyclic voltammetry and chronoamperometry. Results showed that the heat-treatment benefits the catalytic properties of synthesized materials in terms of CO and methanol electrochemical oxidation. The curves for CO stripping were more defined for heat-treated catalysts, and methanol oxidation current densities were higher for these materials. These changes are principally explained from the removal of organic residues remaining on the surface of the Pt-Ru nanoparticles after the synthesis procedure. After the activation of the catalysts by heating at 350°C, the real importance of the use of these encapsulating molecules and the effect of the generation of the dendrimer become visible. From these results, it can be concluded that synthesized catalysts are good catalytic anodes for direct methanol fuel cells (DMFCs.

Metal induced B-Y activation in semisandwich Cp*Rh-, Cp*Ir-, (p-cumene)Ru-, and (p-cumene)Os complexes containing 1,2-dicarba-closo-dodecaborane(12)-1,2-dichalcogenide ligand

International Nuclear Information System (INIS)

Bernd Vrakmejer; Khong Yan; Vol'fgang Milius; Maks Kherberkhol'd

2001-01-01

Reactivity of 16e-semisandwich Cp*M[E 2 C 2 (B 10 H 10 )] and (p-cumene) M' [S 2 C 2 (B 10 H 10 )] complexes (Cp = cyclopentadienyl-ion; M = Rh, Ir; M' Ru, Os; E = S, Se) towards various alkynes was studied using data of NMR and X-ray diffraction analyses of intermediate and final products of the reactions. It is shown that the reactions initiate from introduction of alkyne molecule in one of metal-E bonds, then intramolecular metal-induced B-H activation occurs along with metal-B bond formation, followed by simultaneous hydrogen atom transfer from boron atom through metal atom to alkyne [ru

Surface noble metal modified PdM/C (M = Ru, Pt, Au) as anode catalysts for direct ethanol fuel cells

International Nuclear Information System (INIS)

Mao, Han; Huang, Tao; Yu, Aishui

2016-01-01

In this article, we studied the surface noble metal modification on Pd nanoparticles, other than the homogeneous or core-shell structure. The surface modification will lead to the uneven constitution within the nanoparticles and thus more obvious optimization effect toward the catalyst brought by the lattice deformation. The surface of the as-prepared Pd nanoparticles was modified with Ru, Pt or Au by a moderate and green approach, respectively. XPS results confirm the interactive electron effects between Pd and the modified noble metal. Electrochemical measurements show that the surface noble metal modified catalysts not only show higher catalytic activity, but also better stability and durability. The PdM/C catalysts all exhibit good dispersion and very little agglomeration after long-term potential cycles toward ethanol oxidation. With only 10% metallic atomic ratio of Au, PdAu/C catalyst shows extraordinary catalytic activity and stability, the peak current reaches 1700 mA mg"−"1 Pd, about 2.5 times that of Pd/C. Moreover, the PdAu/C maintains 40% of the catalytic activity after 4500 potential cycles. - Highlights: • Pd-based catalysts with complicated exposed facets. • Much enhanced electrocatalytic activity and stability with about 10% noble metal M (M = Ru, Pt, Au) on Pd nanoparticles. • The outstanding electrocatalytic performance of PdAu/C towards ethanol oxidation after the Au modification.

Surface noble metal modified PdM/C (M = Ru, Pt, Au) as anode catalysts for direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Mao, Han; Huang, Tao, E-mail: huangt@fudan.edu.cn; Yu, Aishui, E-mail: asyu@fudan.edu.cn

2016-08-15

In this article, we studied the surface noble metal modification on Pd nanoparticles, other than the homogeneous or core-shell structure. The surface modification will lead to the uneven constitution within the nanoparticles and thus more obvious optimization effect toward the catalyst brought by the lattice deformation. The surface of the as-prepared Pd nanoparticles was modified with Ru, Pt or Au by a moderate and green approach, respectively. XPS results confirm the interactive electron effects between Pd and the modified noble metal. Electrochemical measurements show that the surface noble metal modified catalysts not only show higher catalytic activity, but also better stability and durability. The PdM/C catalysts all exhibit good dispersion and very little agglomeration after long-term potential cycles toward ethanol oxidation. With only 10% metallic atomic ratio of Au, PdAu/C catalyst shows extraordinary catalytic activity and stability, the peak current reaches 1700 mA mg{sup −1} Pd, about 2.5 times that of Pd/C. Moreover, the PdAu/C maintains 40% of the catalytic activity after 4500 potential cycles. - Highlights: • Pd-based catalysts with complicated exposed facets. • Much enhanced electrocatalytic activity and stability with about 10% noble metal M (M = Ru, Pt, Au) on Pd nanoparticles. • The outstanding electrocatalytic performance of PdAu/C towards ethanol oxidation after the Au modification.

Stacking reactions of the borole complex Cp*Rh(η5-C4H4BPh) with the dicationic fragments [Cp*M]2+ (M = Rh or Ir)

International Nuclear Information System (INIS)

Loginov, D.A.; Muratov, D.V.; Starikova, Z.A.; Petrovskij, P.V.; Kudinov, A.R.

2006-01-01

The reaction of the (borole)rhodium iodide complex [(η-C 4 H 4 BPh)RhI] 4 with Cp*Li afforded the sandwich compound Cp*Rh(η-C 4 H 4 BPh) (1). The reactions of compound 1 with the solvated complexes [Cp*M(MeNO 2 ) 3 ] 2+ (BF 4 - ) 2 gave triple-decker cationic complexes with the central borole ligand [Cp*Rh(μ-η 5 :η 5 -C 4 H 4 BPh)MCp*] 2+ (BF 4 - ) 2 (M = Rh or Ir). The structure of complex 1 was established by X-ray diffraction [ru

A Reactive Oxide Overlayer on Rh Nanoparticles during CO Oxidation and Its Size Dependence Studied by in Situ Ambient Pressure XPS

International Nuclear Information System (INIS)

Grass, Michael E.; Zhang, Yawen; Butcher, Derek R.; Park, Jeong Y.; Li, Yimin; Bluhm, Hendrik; Bratlie, Kaitlin M.; Zhang, Tianfu; Somorjai, Gabor A.

2008-01-01

CO oxidation is one of the most studied heterogeneous reactions, being scientifically and industrially important, particularly for removal of CO from exhaust streams and preferential oxidation for hydrogen purification in fuel cell applications. The precious metals Ru, Rh, Pd, Pt, and Au are most commonly used for this reaction because of their high activity and stability. Despite the wealth of experimental and theoretical data, it remains unclear what is the active surface for CO oxidation under catalytic conditions for these metals. In this communication, we utilize in situ synchrotron ambient pressure X-ray photoelectron spectroscopy (APXPS) to monitor the oxidation state at the surface of Rh nanoparticles during CO oxidation and demonstrate that the active catalyst is a surface oxide, the formation of which is dependent on particle size. The amount of oxide formed and the reaction rate both increase with decreasing particle size.

Cerium valence change in the solid solutions Ce(Rh1-xRux)Sn

International Nuclear Information System (INIS)

Niehaus, Oliver; Riecken, Jan F.; Winter, Florian; Poettgen, Rainer; Muenster Univ.; Abdala, Paula M.; Chevalier, Bernard

2013-01-01

The solid solutions Ce(Rh 1-x Ru x )Sn were investigated by means of susceptibility measurements, specific heat, electrical resistivity, X-ray absorption spectroscopy (XAS), and 119 Sn Moessbauer spectroscopy. Magnetic measurements as well as XAS data show a cerium valence change in dependence on the ruthenium content. Higher ruthenium content causes an increase from 3.22 to 3.45 at 300 K. Furthermore χ and χ -1 data indicate valence fluctuation for cerium as a function of temperature. For example, Ce(Rh 0.8 Ru 0.2 )Sn exhibits valence fluctuations between 3.42 and 3.32 in the temperature range of 10 to 300 K. This could be proven by using the interconfiguration fluctuation (ICF) model introduced by Sales and Wohlleben. Cerium valence change does not influence the tin atoms as proven by 119 Sn Moessbauer spectroscopy, but it influences the electrical properties. Ce(Rh 0.9 Ru 0.1 )Sn behaves like a typical valence fluctuating compound, and higher ruthenium content causes an increase of the metallic behavior. (orig.)

Functional toxicity and tolerance patterns of bioavailable Pd(II), Pt(II), and Rh(III) on suspended Saccharomyces cerevisiae cells assayed in tandem by a respirometric biosensor

Energy Technology Data Exchange (ETDEWEB)

Frazzoli, Chiara; Mantovani, Alberto [Istituto Superiore di Sanita, Department of Food Safety and Veterinary Public Health and WHO/FAO Collaborating Centre for Veterinary Public Health, Rome (Italy); Dragone, Roberto [Consiglio Nazionale delle Ricerche, Institute for Complex Systems, Rome (Italy); Massimi, Cristiana [Istituto Superiore di Sanita, Department of Food Safety and Veterinary Public Health and WHO/FAO Collaborating Centre for Veterinary Public Health, Rome (Italy); University ' La Sapienza' , Department of Chemistry, Rome (Italy); Campanella, Luigi [University ' La Sapienza' , Department of Chemistry, Rome (Italy)

2007-12-15

Toxicological implications of exposure to bioavailable platinum group metals, here Pd, Pt, and Rh, are still to be clarified. This study obtained by a biosensor-based method preliminary information on potential effects on cellular metabolism as well as on possible tolerance mechanisms. Aerobic respiration was taken as the toxicological end point to perform tandem tests, namely functional toxicity test and tolerance test. Cells were suspended in the absence of essential constituents for growth. The dose-response curves obtained by exposure (2 h) to the metals (nanogram per gram range) suggested the same mechanisms of action, with Rh showing the greatest curve steepness and the lowest EC{sub 50} value. Conservative (95% lower confidence interval) EC{sub 10} values were 187, 85 and 51 ng g{sup -1} for Pt, Pd, and Rh respectively. Tolerance patterns were tested during the same runs. The full tolerance obtained after 12 h of exposure to each metal suggested mitochondrial inhibition of aerobic respiration as a target effect. The hazard rating of the metals in the tolerance test changed in the Rh EC{sub 50} range, where Rh showed the lowest toxicity. The observed tolerance might suggest a protective mechanism such as metallothionein induction at concentrations around the EC{sub 50} values. The performance of the bioassay was satisfactory, in terms of the limit of detection, repeatability, reproducibility, roboustness, sensibility, and stability; the method's critical uncertainty sources were identified for improvements. (orig.)

Adsorption and oxidation of acetaldehyde on carbon supported Pt, PtSn and PtSn-based trimetallic catalysts by in situ Fourier transform infrared spectroscopy

Science.gov (United States)

Beyhan, Seden; Léger, Jean-Michel; Kadırgan, Figen

2013-11-01

The adsorption and oxidation of acetaldehyde on carbon supported Pt, Pt90Sn10 and Pt80Sn10M10 (M = Ni, Co, Rh, Pd) catalysts have been investigated by using in situ Fourier transform infrared (FTIR) spectroscopy. The result revealed that Pt90Sn10/C catalyst is not very efficient for the conversion of acetaldehyde to CO2 due to the weak adsorption of acetaldehyde in the presence of Sn. However, the addition of a third metal to Pt--Sn facilitates the C-C bond cleavage of acetaldehyde. It seems that acetaldehyde is adsorbed dissociatively on the surface of Pt80Sn10Ni10/C, Pt80Sn10Co10/C, Pt80Sn10Rh10/C catalysts, producing CH3 and CHO adsorbate species, which can be further oxidized to CO2. However, the pathway forming CO2 for Pt80Sn10Pd10/C catalyst mainly originates from the oxidation of CH3CO species. Thus, the presence of third metal in the PtSn catalyst has a strong impact upon the acetaldehyde adsorption behaviour and its reaction products.

Noble metal catalyzed aqueous phase hydrogenation and hydrodeoxygenation of lignin-derived pyrolysis oil and related model compounds.

Science.gov (United States)

Mu, Wei; Ben, Haoxi; Du, Xiaotang; Zhang, Xiaodan; Hu, Fan; Liu, Wei; Ragauskas, Arthur J; Deng, Yulin

2014-12-01

Aqueous phase hydrodeoxygenation of lignin pyrolysis oil and related model compounds were investigated using four noble metals supported on activated carbon. The hydrodeoxygenation of guaiacol has three major reaction pathways and the demethylation reaction, mainly catalyzed by Pd, Pt and Rh, produces catechol as the products. The presence of catechol and guaiacol in the reaction is responsible for the coke formation and the catalysts deactivation. As expected, there was a significant decrease in the specific surface area of Pd, Pt and Rh catalysts during the catalytic reaction because of the coke deposition. In contrast, no catechol was produced from guaiacol when Ru was used so a completely hydrogenation was accomplished. The lignin pyrolysis oil upgrading with Pt and Ru catalysts further validated the reaction mechanism deduced from model compounds. Fully hydrogenated bio-oil was produced with Ru catalyst. Copyright © 2014 Elsevier Ltd. All rights reserved.

Improvement of energy conversion efficiency and power generation in direct borohydride-hydrogen peroxide fuel cell: The effect of Ni-M core-shell nanoparticles (M = Pt, Pd, Ru)/Multiwalled Carbon Nanotubes on the cell performance

Science.gov (United States)

Hosseini, M. G.; Mahmoodi, R.

2017-12-01

In this study, core@shell nanoparticles with Ni as a core material and Pt, Pd and Ru as shell materials are synthesized on multiwalled carbon nanotube (MWCNT) as catalyst support using the sequence reduction method. The influence of Ni@Pt, Ni@Pd and Ni@Ru core@shell nanoparticles on MWCNT toward borohydride oxidation in alkaline solution is investigated by various three-electrode electrochemical techniques. Also, the impact of these anodic electrocatalysts on the performance of direct borohydride-hydrogen peroxide fuel cell (DBHPFC) is evaluated. The structural and morphological properties of electrocatalysts are studied by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS). The results of three electrode investigations show that Ni@Pd/MWCNT has excellent catalytic activity since borohydride oxidation current density on Ni@Pd/MWCNT (34773.27 A g-1) is 1.37 and 9.19 times higher than those of Ni@Pt/MWCNT (25347.27 A g-1) and Ni@Ru/MWCNT (3782.83 A g-1), respectively. Also, the energy conversion efficiency and power density of DBHPFC with Ni@Pd/MWCNT (246.82 mW cm-2) increase to 34.27% and 51.53% respect to Ni@Pt/MWCNT (162.24 mW cm-2) and Ni@Ru/MWCNT (119.62 mW cm-2), respectively. This study reveals that Ni@Pd/MWCNT has highest activity toward borohydride oxidation and stability in fuel cell.

Isotope dilution inductively coupled plasma quadrupole mass spectrometry in connection with a chromatographic separation for ultra trace determinations of platinum group elements (Pt, Pd, Ru, Ir) in environmental samples.

Science.gov (United States)

Müller, M; Heumann, K G

2000-09-01

An isotope dilution inductively coupled plasma quadrupole mass spectrometric (ID-ICP-QMS) method was developed for the simultaneous determination of the platinum group elements Pt, Pd, Ru, and Ir in environmental samples. Spike solutions, enriched with the isotopes 194Pt, 108Pd, 99Ru, and 191Ir, were used for the isotope dilution step. Interfering elements were eliminated by chromatographic separation using an anion-exchange resin. Samples were dissolved with aqua regia in a high pressure asher. Additional dissolution of possible silicate portions by hydrofluoric acid was usually not necessary. Detection limits of 0.15 ng x g(-1), 0.075 ng x g(-1), and 0.015 ng x g(-1) were achieved for Pt, Pd, Ru, and Ir, respectively, using sample weights of only 0.2 g. The reliability of the ID-ICP-QMS method was demonstrated by analyzing a Canadian geological reference material and by participating in an interlaboratory study for the determination of platinum and palladium in a homogenized road dust sample. Surface soil, sampled at different distances from a highway, showed concentrations in the range of 0.1-87 ng x g(-1). An exponential decrease of the platinum and palladium concentration with increasing distance and a small anthropogenic contribution to the natural background concentration of ruthenium and iridium was found in these samples.

Pt20RuxSny nanoparticles dispersed on mesoporous carbon CMK-3 and their application in the oxidation of 2-carbon alcohols and fermentation effluent

International Nuclear Information System (INIS)

Lo, An-Ya; Chung, Yi-Chen; Hung, Wei-Hsuan; Hsu, Yun-Chi; Tseng, Chuan-Ming; Zhang, Wei-Lun; Wang, Fu-Kai; Lin, Chiu-Yue

2017-01-01

Highlights: • Pt 20 Ru x Sn y @C catalysts are formed by dispersing Pt-Sn and Pt-Ru-Sn NPs on CMK-3. • They are tested in fuel cells using ethanol, ethylene glycol, and CFHPE as fuels. • Higher Sn contents improve catalytic efficiency of Pt 20 Ru x Sn y when x = 0 or x = 10. • Role of Sn in C−C bond cleavage and improving poisoning tolerance is explained. • Pt 20 Ru 10 Sn 15 @C is used to show feasibility of using bioalcohol from CFHPE as fuel. - Abstract: We report the synthesis of Pt-Sn binary and Pt-Ru-Sn ternary alloy nanoparticles (NPs) dispersed on mesoporous carbon CMK-3 for bioalcohol fuel cell applications where ethanol, ethylene glycol, and fermentative hydrogen production effluent were used as the fuels. The proposed alloy electrocatalysts, denoted as Pt 20 Ru x Sn y @C (where 20, x, and y represent the weight fractions of Pt, Ru, and Sn, respectively), were examined using scanning electron microscopy, energy-dispersive X-ray spectroscopy mapping, transmission electron microscopy, Brunauer-Emmett-Teller measurements, X-ray diffraction analysis, and electrochemical measurements, in order to determine their morphologies, microstructures, compositions, phase structures, and electrochemical characteristics. The effects of the Sn content on the following factors were examined: 1) average particle size of the alloy NPs, 2) mesoporosity, 3) electrochemically active surfaces of Pt 20 Ru x Sn y @C, and 4) ethanol oxidation reaction and ethylene glycol oxidation reaction activities. Higher Sn contents improved the catalytic efficiency of Pt 20 Ru x Sn y when x = 0 or x = 10, with the optimized compositions being Pt 20 Sn 30 and Pt 20 Ru 10 Sn 15 for the binary and ternary alloys, respectively. Based on the ethanol and ethylene glycol oxidation reactions, we explain the role of Sn in promoting C−C bond cleavage and in improving catalyst tolerance against poisoning. Overall, for both the ethanol system and the ethylene glycol system, the catalytic

Applications Ni59Nb40Pt(1-x) Xx (X= Sn,Sby and Ru) amorphous alloy as anodes for direct methanol (DMFC) fuel cells

International Nuclear Information System (INIS)

Rodriguez Pierna, A

2005-01-01

The search of new anode materials of amorphous nature for methanol fuel cells is one of the aims of this work.The main problem that fuel cells present is related to the catalytic material and its distribution in a suitable matrix.Amorphous alloys are particularly attractive materials as catalyst supports because of their high conductivity, high corrosion resistance in sulphuric acid, as well as the possibility of a good distribution of the electrocatalytic particles, mainly platinum and platinum-tin, on a conducting matrix.The electrooxidation of methanol, in percloric acid medium, has been used as probe to evaluate the performance of metallic amorphous electrodes, with compositions Ni 5 9Nb 4 0Pt 1 , Ni 5 9Nb 4 0Pt 0 .6Sn0.4, Ni 5 9Nb 4 0Pt 0 .6Sb 0 .4 and Ni 5 9Nb 4 0Pt 0 .6Ru 0 .4.The electrocatalytic activity of the alloyed ribbons of compositions (x = 0.6, 1% at. in platinum) is improved considerably, so much for the change in their composition, as for the roughness degree that the catalytic surfaces present. The increase of the tolerance to adsorbed species, and better resistance to the poisoning of their catalytic centers, can be observed by means of voltammetric experiments at different activation times with HF 48%. The electrooxidation of methanol in the amorphous alloy of composition Ni 5 9Nb 4 0Pt 1 , is influenced by the nature of the used electrolyte, presenting smaller values of current density in solutions 1M H 2 SO 4 than in 1M of HClO 4 .This behavior is not observed in the alloy Ni 5 9Nb 4 0Pt 0 .6Sn 0 .4, Ni 5 9Nb 4 0Pt 0 .6Sb 0 .4 and Ni 5 9Nb 4 0Pt 0 .6Ru 0 .4which does not present a poisoning of the catalytic centers depending on the used electrolyte.Adding tin to the alloys showed the existence of a synergetic effect in the methanol electrooxidation process, attaining to a descent of 20 mV vs Ag/AgCl in the onset potential, and about 200 mV in the maximun peak potential

Electrochemical oxidation of ammonia-containing wastewater using Ti/RuO2-Pt electrode

Directory of Open Access Journals (Sweden)

Wei-wu Hu

2009-12-01

Full Text Available The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current densities, space sizes between the two electrodes, and amounts of added NaCl on ammonia-containing wastewater treatment. It was shown that, after a 30-min treatment under the optimal conditions, which were a current density of 20 mA/cm2, a space size between the two electrodes of 1 cm, and an added amount of 0.5 g/L of NaCl, the COD concentration in municipal wastewater was 40 mg/L, a removal rate of 90%; and the NH3-N concentration was 7 mg/L, a removal rate of 88.3%. The effluent of municipal wastewater qualified for Class A of the Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant (GB18918-2002.

Determination of the half-life of sup 1 sup 0 sup 5 sup m Rh

CERN Document Server

Kronenberg, A K; Weber, R; Esterlund, R A; Patzelt, P

1998-01-01

Following a fast chemical separation of Ru isotopes from a fission-product mixture, sup 1 sup 0 sup 5 sup m Rh was periodically extracted from its precursor (4.44-h sup 1 sup 0 sup 5 Ru) for measurements of its half-life. The new value for the T sub 1 sub / sub 2 of sup 1 sup 0 sup 5 sup m Rh of (43.0+-0.3) s resolves the long-standing conflict in the literature between the two earlier measured values of 45 and 30 s.

Analisis Bahaya Fisik: Hubungan Tingkat Pencahayaan dan Keluhan Mata Pekerja pada Area Perkantoran Health, Safety, and Environmental (HSE PT. Pertamina RU VI Balongan

Directory of Open Access Journals (Sweden)

Dina Rahmayanti

2016-04-01

Full Text Available The eyes are part of the body that must be protected workers safety and health. Sufficient light is one of the most important aspects that determine the health of the eye, excellent lighting intensity affects the eyes. This study was performed at PT Pertamina RU VI Balongan, based on observation in the work area, it is necessary to evaluate the intensity of light and eye strain workers in a unit of PT. Pertamina Refinery Unit VI Balongan.Be collected from primary and secondary data and processing in the form of statistical testing using Microsoft Excel and SPSS Software 2.0. Tests conducted on four types of questionnaires and data variables intensity lighting in the office area of HSE unit RU VI Balongan.There are 12 rooms which have the following illumination standard (under 300 lux. Based on a statistical test between the variable quality of the lighting of the eye complaints get results there are two variables that have a relationship. In addition, all respondents had complaints of eye fatigue that varies with the highest percentage of 80% with complaints of eye feel sleepy and 63% of workers feel pain in the neck or shoulder.

Low Pt content direct methanol fuel cell anode catalyst: nanophase PtRuNiZr

Science.gov (United States)

Narayanan, Sekharipuram R. (Inventor); Whitacre, Jay F. (Inventor)

2010-01-01

A method for the preparation of a metallic material having catalytic activity that includes synthesizing a material composition comprising a metal content with a lower Pt content than a binary alloy containing Pt but that displays at least a comparable catalytic activity on a per mole Pt basis as the binary alloy containing Pt; and evaluating a representative sample of the material composition to ensure that the material composition displays a property of at least a comparable catalytic activity on a per mole Pt basis as a representative binary alloy containing Pt. Furthermore, metallic compositions are disclosed that possess substantial resistance to corrosive acids.

Influence of hydrogen on the thermoelectric power of palladium alloyed with neighbouring elements: I. Pd/Ru/H and Pd/Rh/H alloys

CERN Document Server

Szafranski, A W

2003-01-01

Pd/Ru and Pd/Rh alloys have been loaded with hydrogen in high-pressure conditions. The resulting hydrogen contents were close to the stoichiometric composition, H/(Pd + Me) = 1. Lower hydrogen contents have been obtained by successive partial desorptions. The thermoelectric power and electrical resistance of one- and two-phase alloys have been measured simultaneously in the temperature range between 80 and 300 K. A Nordheim-Gorter type correlation of the two quantities has been observed in many cases and the partial thermopowers corresponding to electron-phonon scattering and lattice disorder could be determined. The observed anomalous behaviour of the total and partial thermopowers is attributed to virtual bound states of ruthenium or rhodium.

Pt based anode catalysts for direct ethanol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Zhou, Weijiang; Zhou, Zhenhua; Song, Shuqin; Li, Wenzhen; Sun, Gongquan; Xin, Qin [Direct Alcohol Fuel Cell Laboratory, Dalian Institute of Chemical Physics, CAS, P.O. Box 110, Dalian 116023 (China); Tsiakaras, Panagiotis [Department of Mechanical and Industrial Engineering, University of Thessalia, Pedion Areos, GR 38334 Volos (Greece) 7

2003-11-10

In the present work several Pt-based anode catalysts supported on carbon XC-72R were prepared with a novel method and characterized by means of XRD, TEM and XPS analysis. It was found that all these catalysts are consisted of uniform nanosized particles with sharp distribution and Pt lattice parameter decreases with the addition of Ru or Pd and increases with the addition of Sn or W. Cyclic voltammetry (CV) measurements and single direct ethanol fuel cell (DEFC) tests jointly showed that the presence of Sn, Ru and W enhances the activity of Pt towards ethanol electro-oxidation in the following order: Pt{sub 1}Sn{sub 1}/C>Pt{sub 1}Ru{sub 1}/C>Pt{sub 1}W{sub 1}/C>Pt{sub 1}Pd{sub 1}/C>Pt/C. Moreover, Pt{sub 1}Ru{sub 1}/C further modified by W and Mo showed improved ethanol electro-oxidation activity, but its DEFC performance was found to be inferior to that measured for Pt{sub 1}Sn{sub 1}/C. Under this respect, several PtSn/C catalysts with different Pt/Sn atomic ratio were also identically prepared and characterized and their direct ethanol fuel cell performances were evaluated. It was found that the single direct ethanol fuel cell having Pt{sub 1}Sn{sub 1}/C or Pt{sub 3}Sn{sub 2}/C or Pt{sub 2}Sn{sub 1}/C as anode catalyst showed better performances than those with Pt{sub 3}Sn{sub 1}/C or Pt{sub 4}Sn{sub 1}/C. It was also found that the latter two cells exhibited higher performances than the single cell using Pt{sub 1}Ru{sub 1}/C, which is exclusively used in PEMFC as anode catalyst for both methanol electro-oxidation and CO-tolerance. This distinct difference in DEFC performance between the catalysts examined here would be attributed to the so-called bifunctional mechanism and to the electronic interaction between Pt and additives. It is thought that an amount of -OH{sub ads}, an amount of surface Pt active sites and the conductivity effect of PtSn/C catalysts would determine the activity of PtSn/C with different Pt/Sn ratios. At lower temperature values or at low

Low-Pt-Content Anode Catalyst for Direct Methanol Fuel Cells

Science.gov (United States)

Narayanan, Sekharipuram; Whitacre, Jay

2008-01-01

Combinatorial experiments have led to the discovery that a nanophase alloy of Pt, Ru, Ni, and Zr is effective as an anode catalyst material for direct methanol fuel cells. This discovery has practical significance in that the electronic current densities achievable by use of this alloy are comparable or larger than those obtained by use of prior Pt/Ru catalyst alloys containing greater amounts of Pt. Heretofore, the high cost of Pt has impeded the commercialization of direct methanol fuel cells. By making it possible to obtain a given level of performance at reduced Pt content (and, hence, lower cost), the discovery may lead to reduction of the economic impediment to commercialization.

The influence of alizarin and fluorescein on the photoactivity of Ni, Pt and Ru-doped TiO2 layers

International Nuclear Information System (INIS)

Rosu, Marcela-Corina; Suciu, Ramona-Crina; Lazar, Mihaela D.; Bratu, I.

2013-01-01

Highlights: ► The Ni, Pt, Ru-doped TiO 2 materials and sensitized with alizarin and fluorescein dyes were prepared by wet chemical route. ► The samples were characterized by: UV–vis spectroscopy, spectrofluorimetry, FT/IR spectroscopy and microscopy, X-ray diffraction and N 2 physisorption measurements. ► A combined influence of the dopants and dyes was observed, leading to a beneficial effect to TiO 2 photoactivity. -- Abstract: The doping with different metal ions and sensitization with organic compounds are two well known methods used to improve the photoactivity of TiO 2 . In this respect, the metallic ions-doped TiO 2 samples were prepared by embedding Ni, Pt and Ru ions into TiO 2 crystalline network and then, each sample was sensitized with alizarin and fluorescein dyes. The qualitative evaluation of prepared TiO 2 -based materials was made by: UV–vis spectroscopy, spectrofluorimetry, FT/IR spectroscopy and microscopy, X-ray diffraction and N 2 physisorption measurements. The optoelectronic properties investigated by UV–vis spectroscopy show that the optical response of Ni-doped TiO 2 layer shifts to visible. The X-ray spectra do not show peaks of nickel, platinum and ruthenium oxide crystals or pure metals. The FT/IR spectra proved the presence of dye molecules adsorbed on titania nanoparticles surface. These results demonstrated that the studied dopants and dyes have potential to promote modified TiO 2 -based materials as good candidates to be used in photolectrocatalytic processes

Balance of Nanostructure and Bimetallic Interactions in Pt Model Fuel Cell Catalysts

DEFF Research Database (Denmark)

Friebel, Daniel; Viswanathan, Venkatasubramanian; Miller, Daniel J.

2012-01-01

We have studied the effect of nanostructuring in Pt monolayer model electrocatalysts on a Rh(111) single-crystal substrate on the adsorption strength of chemisorbed species. In situ high energy resolution fluorescence detection X-ray absorption spectroscopy at the Pt L3 edge reveals characteristic...... changes of the shape and intensity of the “white-line” due to chemisorption of atomic hydrogen (Had) at low potentials and oxygen-containing species (O/OHad) at high potentials. On a uniform, two-dimensional Pt monolayer grown by Pt evaporation in ultrahigh vacuum, we observe a significant destabilization...... of both Had and O/OHad due to strain and ligand effects induced by the underlying Rh(111) substrate. When Pt is deposited via a wet-chemical route, by contrast, three-dimensional Pt islands are formed. In this case, strain and Rh ligand effects are balanced with higher local thickness of the Pt islands...

Application of the Auger and X-ray photoelectron electronic spectroscopies to the study of superficial segregation in the system Pt-Rh

International Nuclear Information System (INIS)

Volpe, M.A.; Castellani, N.J.; Leroy, D.B.

1987-01-01

The Auger and X-ray photoelectron spectroscopies are applied to the study of the superficial segregation in the system of the binary alloy Pt-Rh. The methodology for the cleaning of the samples, which is essential for the obtainment of reproducible results, has been established. The spectra qualitative analysis allows to identify the element segregated. The application of the Gallon model permits to develop a quantitative study of the phenomenon. (S.M.) [es

Reforming of Ethanol to Produce Hydrogen over PtRuMg/ZrO2 Catalyst

Directory of Open Access Journals (Sweden)

Josh Y. Z. Chiou

2012-01-01

Full Text Available A modified PtRu/ZrO2 catalyst with Mg is evaluated for the oxidative steam reforming of ethanol (OSRE and the steam reforming of ethanol (SRE. In order to understand the variation in the reaction mechanism on OSRE and SRE, further analysis of both fresh and used catalyst is concentrated on for TEM, TG, Raman, and TPR characterization. The results show that the OSRE reaction requires a higher temperature (∼390°C to achieve 100% ethanol conversion than the SRE reaction (∼2500°C. The distribution of CO is minor for both reactions (< 5% for OSRE, < 1% for SRE. This demonstrates that the water gas shift (WGS reaction is an important side-reaction in the reforming of ethanol to produce H2 and CO2. A comparison of the temperature of WGS (WGS shows it is lower for the SRE reaction (WGS∼250°C for SRE, ~340°C for OSRE.

Theoretical insights into the interaction between RunPt13-n (n=4, 7 and 9) clusters and [BMIM]+ based ionic liquids: Effect of anion.

Science.gov (United States)

Cheng, Ping; Yang, Yongpeng; Huang, Shiping

2017-06-01

Density functional theory has been performed to systematically study the interactions between Ru n Pt 13-n (n=4, 7 and 9) clusters and [BMIM] + based ionic liquids. Ionic liquids [BMIM][Br], [BMIM][BF 4 ], [BMIM][PF 6 ], [BMIM][CF 3 SO 3 ], and [BMIM][NTf 2 ] have different effects on the stability of Ru 7 Pt 6 . Ionic liquids with median size anions of PF 6 - and CF 3 SO 3 - can better improve the stability of Ru 7 Pt 6 than those with the small anions of Br - and BF 4 - and large anion of NTf 2 - . Based on negative relaxation energies, the stabilities of Ru 4 Pt 9 , Ru 7 Pt 6 , and Ru 9 Pt 4 are all enhanced after interacting with [BMIM][CF 3 SO 3 ]. The stability enhanced degree is in agreement with the interaction strength. For Ru 7 Pt 6 -n{[BMIM][CF 3 SO 3 ]} (n=1, 2, 3, 4), the interaction between ionic liquid and cluster plays the primary role in stabilizing the cluster in Ru 7 Pt 6 -[BMIM][CF 3 SO 3 ]. With the increase of the number of [BMIM][CF 3 SO 3 ], the role of the interaction in stabilizing the cluster is getting weaker, while the role of steric protection is getting more important. Copyright © 2017 Elsevier Inc. All rights reserved.

Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts

KAUST Repository

Krier, James M.

2015-01-14

© 2014 American Chemical Society. 1,3-Butadiene (1,3-BD) hydrogenation was performed on 4 nm Pt, Pd, and Rh nanoparticles (NPs) encapsulated in SiO2 shells at 20, 60, and 100 °C. The core-shells were grown around polyvinylpyrrolidone (PVP) coated NPs (Stöber encapsulation) prepared by colloidal synthesis. Sum frequency generation (SFG) vibrational spectroscopy was performed to correlate surface intermediates observed in situ with reaction selectivity. It is shown that calcination is effective in removing PVP, and the SFG signal can be generated from the metal surface. Using SFG, it is possible to compare the surface vibrational spectrum of Pt@SiO2 (1,3-BD is hydrogenated through multiple paths and produces butane, 1-butene, and cis/trans-2-butene) to Pd@SiO2 (1,3-BD favors one path and produces 1-butene and cis/trans-2-butene). In contrast to Pt@SiO2 and Pd@SiO2, SFG and kinetic experiments of Rh@SiO2 show a permanent accumulation of organic material.

A possible in vivo generator 103Pd/103mRh-Recoil considerations

International Nuclear Information System (INIS)

Rooyen, Johann van; Szucs, Zoltan; Rijn Zeevaart, Jan

2008-01-01

The use of Auger emitters as potential radiopharmaceuticals is increasingly investigated. One such radionuclide of interest is 103m Rh. This can be produced from 103 Ru or from 103 Pd in an in vivo generator. A potential problem with this concept is the recoil of the 103m Rh out of the carrier molecule and even out of the target cell. In order to determine whether this would happen in the 103 Pd/ 103m Rh case calculations were done to prove that this does not happen. From theoretical considerations it seems that the 103 Pd/ 103m Rh in vivo generator system would be possible

Fuel cycle integration issues associated with P/T technology

International Nuclear Information System (INIS)

Michaels, G.E.; Ludwig, S.B.

1992-01-01

The three primary interfaces between a generic partitioning and transmutation (P/T) technology and the existing United States fuel cycle are the light-water reactor (LWR) spent fuel inventory, the reprocessed uranium (RU) stream, and the high-level waste stream. The features and implications of these three interfaces are reviewed and their implications for P/T system design and for waste management are assessed. The variability of transuranic nuclide composition in the LWR spent fuel is calculated and its potential implications for transmutation system core design are discussed. The radiological characteristics of the RU stream are presented, and options for disposition of the stream are reviewed. Most P/T scenarios assume that RU will be recycled to LWRs. This study demonstrates, however, that LWR recycle cannot totally consume the reprocessed stream, and disposal of a waste uranium steam with high levels of radiologically-significant isotopes will still be necessary. The radioactivity of the tails stream for enrichment plants resulting from a dedicated RU campaign is calculated. The tendency of gaseous diffusion plant enrichment technology to deplete the tails stream of minor uranium isotopes is seen as a benefit and an advantage over Atomic Vapor Laser Isotope Separation-type technology. Finally, the implications of P/T on LWR-origin wastes reporting to the repository is discussed, and several significant differences between LWR-origin waste originating from transmutation systems are assessed

The influence of alizarin and fluorescein on the photoactivity of Ni, Pt and Ru-doped TiO{sub 2} layers

Energy Technology Data Exchange (ETDEWEB)

Rosu, Marcela-Corina, E-mail: marcela.rosu@itim-cj.ro [National Institute for Research and Development of Isotopic and Molecular Technologies, 65-103 Donath Street, 400293, Cluj-Napoca (Romania); Suciu, Ramona-Crina; Lazar, Mihaela D.; Bratu, I. [National Institute for Research and Development of Isotopic and Molecular Technologies, 65-103 Donath Street, 400293, Cluj-Napoca (Romania)

2013-04-20

Highlights: ► The Ni, Pt, Ru-doped TiO{sub 2} materials and sensitized with alizarin and fluorescein dyes were prepared by wet chemical route. ► The samples were characterized by: UV–vis spectroscopy, spectrofluorimetry, FT/IR spectroscopy and microscopy, X-ray diffraction and N{sub 2} physisorption measurements. ► A combined influence of the dopants and dyes was observed, leading to a beneficial effect to TiO{sub 2} photoactivity. -- Abstract: The doping with different metal ions and sensitization with organic compounds are two well known methods used to improve the photoactivity of TiO{sub 2}. In this respect, the metallic ions-doped TiO{sub 2} samples were prepared by embedding Ni, Pt and Ru ions into TiO{sub 2} crystalline network and then, each sample was sensitized with alizarin and fluorescein dyes. The qualitative evaluation of prepared TiO{sub 2}-based materials was made by: UV–vis spectroscopy, spectrofluorimetry, FT/IR spectroscopy and microscopy, X-ray diffraction and N{sub 2} physisorption measurements. The optoelectronic properties investigated by UV–vis spectroscopy show that the optical response of Ni-doped TiO{sub 2} layer shifts to visible. The X-ray spectra do not show peaks of nickel, platinum and ruthenium oxide crystals or pure metals. The FT/IR spectra proved the presence of dye molecules adsorbed on titania nanoparticles surface. These results demonstrated that the studied dopants and dyes have potential to promote modified TiO{sub 2}-based materials as good candidates to be used in photolectrocatalytic processes.

Activity and Stability of Dispersed Multi Metallic Pt-based Catalysts for CO Tolerance in Proton Exchange Membrane Fuel Cell Anodes.

Science.gov (United States)

Hassan, Ayaz; Ticianelli, Edson A

2018-01-01

Studies aiming at improving the activity and stability of dispersed W and Mo containing Pt catalysts for the CO tolerance in proton exchange membrane fuel cell (PEMFC) anodes are revised for the following catalyst systems: (1) a carbon supported PtMo electrocatalyst submitted to heat treatments; (2) Pt and PtMo nanoparticles deposited on carbon-supported molybdenum carbides (Mo2C/C); (3) ternary and quaternary materials formed by PtMoFe/C, PtMoRu/C and PtMoRuFe/C and; (4) Pt nanoparticles supported on tungsten carbide/carbon catalysts and its parallel evaluation with carbon supported PtW catalyst. The heat-treated (600 oC) Pt-Mo/C catalyst showed higher hydrogen oxidation activity in the absence and in the presence of CO and better stability, compared to all other Mo-containing catalysts. PtMoRuFe, PtMoFe, PtMoRu supported on carbon and Pt supported on Mo2C/C exhibited similar CO tolerances but better stability, as compared to as-prepared PtMo supported on carbon. Among the tungsten-based catalysts, tungsten carbide supported Pt catalyst showed reasonable performance and reliable stability in comparison to simple carbon supported PtW catalyst, though an uneven level of catalytic activity towards H2 oxidation in presence of CO is observed for the former as compared to Mo containing catalyst. However, a small dissolution of Mo, Ru, Fe and W from the anodes and their migration toward cathodes during the cell operation is observed. These results indicate that the fuel cell performance and stability has been improved but not yet totally resolved.

Activity and Stability of Dispersed Multi Metallic Pt-based Catalysts for CO Tolerance in Proton Exchange Membrane Fuel Cell Anodes

Directory of Open Access Journals (Sweden)

AYAZ HASSAN

2018-04-01

Full Text Available ABSTRACT Studies aiming at improving the activity and stability of dispersed W and Mo containing Pt catalysts for the CO tolerance in proton exchange membrane fuel cell (PEMFC anodes are revised for the following catalyst systems: (1 a carbon supported PtMo electrocatalyst submitted to heat treatments; (2 Pt and PtMo nanoparticles deposited on carbon-supported molybdenum carbides (Mo2C/C; (3 ternary and quaternary materials formed by PtMoFe/C, PtMoRu/C and PtMoRuFe/C and; (4 Pt nanoparticles supported on tungsten carbide/carbon catalysts and its parallel evaluation with carbon supported PtW catalyst. The heat-treated (600 oC Pt-Mo/C catalyst showed higher hydrogen oxidation activity in the absence and in the presence of CO and better stability, compared to all other Mo-containing catalysts. PtMoRuFe, PtMoFe, PtMoRu supported on carbon and Pt supported on Mo2C/C exhibited similar CO tolerances but better stability, as compared to as-prepared PtMo supported on carbon. Among the tungsten-based catalysts, tungsten carbide supported Pt catalyst showed reasonable performance and reliable stability in comparison to simple carbon supported PtW catalyst, though an uneven level of catalytic activity towards H2 oxidation in presence of CO is observed for the former as compared to Mo containing catalyst. However, a small dissolution of Mo, Ru, Fe and W from the anodes and their migration toward cathodes during the cell operation is observed. These results indicate that the fuel cell performance and stability has been improved but not yet totally resolved.

Synthesis and electrochemical study of Pt-based nanoporous materials

International Nuclear Information System (INIS)

Wang Jingpeng; Holt-Hindle, Peter; MacDonald, Duncan; Thomas, Dan F.; Chen Aicheng

2008-01-01

In the present work, a variety of Pt-based bimetallic nanostructured materials including nanoporous Pt, Pt-Ru, Pt-Ir, Pt-Pd and Pt-Pb networks have been directly grown on titanium substrates via a facile hydrothermal method. The as-fabricated electrodes were characterized by scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and electrochemical methods. The active surface areas of these nanoporous Pt-based alloy catalysts are increased by over 68 (Pt-Pd), 69 (Pt-Ru) and 113 (Pt-Ir) fold compared to a polycrystalline Pt electrode. All these synthesized nanoporous electrodes exhibit superb electrocatalytic performance towards electrochemical oxidation of methanol and formic acid. Among the five nanoporous Pt-based electrodes, the Pt-Ir shows the highest peak current density at +0.50 V, with 68 times of enhancement compared to the polycrystalline Pt for methanol oxidation, and with 86 times of enhancement in formic acid oxidation; whereas the catalytic activity of the nanoporous Pt-Pb electrode outperforms the other materials in formic acid oxidation at the low potential regions, delivering an enhanced current density by 280-fold compared to the polycrystalline Pt at +0.15 V. The new approach described in this study is suitable for synthesizing a wide range of bi-metallic and tri-metallic nanoporous materials, desirable for electrochemical sensor design and potential application in fuel cells

Synthesis and electrochemical study of Pt-based nanoporous materials

Energy Technology Data Exchange (ETDEWEB)

Wang Jingpeng [Department of Chemistry, Lakehead University, Thunder Bay, Ontario P7B 5E1 (Canada); Department of Chemistry, University of Guelph, Guelph, Ontario N1G 2W1 (Canada); Holt-Hindle, Peter; MacDonald, Duncan [Department of Chemistry, Lakehead University, Thunder Bay, Ontario P7B 5E1 (Canada); Thomas, Dan F. [Department of Chemistry, University of Guelph, Guelph, Ontario N1G 2W1 (Canada); Chen Aicheng [Department of Chemistry, Lakehead University, Thunder Bay, Ontario P7B 5E1 (Canada)], E-mail: aicheng.chen@lakeheadu.ca

2008-10-01

In the present work, a variety of Pt-based bimetallic nanostructured materials including nanoporous Pt, Pt-Ru, Pt-Ir, Pt-Pd and Pt-Pb networks have been directly grown on titanium substrates via a facile hydrothermal method. The as-fabricated electrodes were characterized by scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and electrochemical methods. The active surface areas of these nanoporous Pt-based alloy catalysts are increased by over 68 (Pt-Pd), 69 (Pt-Ru) and 113 (Pt-Ir) fold compared to a polycrystalline Pt electrode. All these synthesized nanoporous electrodes exhibit superb electrocatalytic performance towards electrochemical oxidation of methanol and formic acid. Among the five nanoporous Pt-based electrodes, the Pt-Ir shows the highest peak current density at +0.50 V, with 68 times of enhancement compared to the polycrystalline Pt for methanol oxidation, and with 86 times of enhancement in formic acid oxidation; whereas the catalytic activity of the nanoporous Pt-Pb electrode outperforms the other materials in formic acid oxidation at the low potential regions, delivering an enhanced current density by 280-fold compared to the polycrystalline Pt at +0.15 V. The new approach described in this study is suitable for synthesizing a wide range of bi-metallic and tri-metallic nanoporous materials, desirable for electrochemical sensor design and potential application in fuel cells.0.

Synthesis and electrochemical study of Pt-based nanoporous materials

Energy Technology Data Exchange (ETDEWEB)

Wang, Jingpeng [Department of Chemistry, Lakehead University, Thunder Bay, Ontario P7B 5E1 (Canada); Department of Chemistry, University of Guelph, Guelph, Ontario N1G 2W1 (Canada); Holt-Hindle, Peter; MacDonald, Duncan; Chen, Aicheng [Department of Chemistry, Lakehead University, Thunder Bay, Ontario P7B 5E1 (Canada); Thomas, Dan F. [Department of Chemistry, University of Guelph, Guelph, Ontario N1G 2W1 (Canada)

2008-10-01

In the present work, a variety of Pt-based bimetallic nanostructured materials including nanoporous Pt, Pt-Ru, Pt-Ir, Pt-Pd and Pt-Pb networks have been directly grown on titanium substrates via a facile hydrothermal method. The as-fabricated electrodes were characterized by scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction and electrochemical methods. The active surface areas of these nanoporous Pt-based alloy catalysts are increased by over 68 (Pt-Pd), 69 (Pt-Ru) and 113 (Pt-Ir) fold compared to a polycrystalline Pt electrode. All these synthesized nanoporous electrodes exhibit superb electrocatalytic performance towards electrochemical oxidation of methanol and formic acid. Among the five nanoporous Pt-based electrodes, the Pt-Ir shows the highest peak current density at +0.50 V, with 68 times of enhancement compared to the polycrystalline Pt for methanol oxidation, and with 86 times of enhancement in formic acid oxidation; whereas the catalytic activity of the nanoporous Pt-Pb electrode outperforms the other materials in formic acid oxidation at the low potential regions, delivering an enhanced current density by 280-fold compared to the polycrystalline Pt at +0.15 V. The new approach described in this study is suitable for synthesizing a wide range of bi-metallic and tri-metallic nanoporous materials, desirable for electrochemical sensor design and potential application in fuel cells. (author)

Investigation of energy band alignments and interfacial properties of rutile NMO2/TiO2 (NM = Ru, Rh, Os, and Ir) by first-principles calculations.

Science.gov (United States)

Yang, Chen; Zhao, Zong-Yan

2017-11-08

In the field of photocatalysis, constructing hetero-structures is an efficient strategy to improve quantum efficiency. However, a lattice mismatch often induces unfavorable interfacial states that can act as recombination centers for photo-generated electron-hole pairs. If the hetero-structure's components have the same crystal structure, this disadvantage can be easily avoided. Conversely, in the process of loading a noble metal co-catalyst onto the TiO 2 surface, a transition layer of noble metal oxides is often formed between the TiO 2 layer and the noble metal layer. In this article, interfacial properties of hetero-structures composed of a noble metal dioxide and TiO 2 with a rutile crystal structure have been systematically investigated using first-principles calculations. In particular, the Schottky barrier height, band bending, and energy band alignments are studied to provide evidence for practical applications. In all cases, no interfacial states exist in the forbidden band of TiO 2 , and the interfacial formation energy is very small. A strong internal electric field generated by interfacial electron transfer leads to an efficient separation of photo-generated carriers and band bending. Because of the differences in the atomic properties of the components, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures demonstrate band dividing, while RhO 2 /TiO 2 and IrO 2 /TiO 2 hetero-structures have a pseudo-gap near the Fermi energy level. Furthermore, NMO 2 /TiO 2 hetero-structures show upward band bending. Conversely, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures present a relatively strong infrared light absorption, while RhO 2 /TiO 2 and IrO 2 /TiO 2 hetero-structures show an obvious absorption edge in the visible light region. Overall, considering all aspects of their properties, RuO 2 /TiO 2 and OsO 2 /TiO 2 hetero-structures are more suitable than others for improving the photocatalytic performance of TiO 2 . These findings will provide useful information

Effect of HCl Concentration on the Oxidation of LIX 63 and the Subsequent Separation of Pd(II), Pt(IV), Ir(IV) and Rh(III) by Solvent Extraction

Energy Technology Data Exchange (ETDEWEB)

Nguyen, Thi Hong; Lee, Man Seung [Mokpo National University, Jeollanamdo (Korea, Republic of)

2016-10-15

During the selective extraction of Pd(II) by LIX 63 from 6 M HCl solutions containing platinum group metals, an oxidation-reduction reaction occurs between the LIX 63 and Ir(IV). Since the reduced Ir(III) cannot be extracted by solvating and amine extractants, the oxidation-reduction reaction has a significant effect on the separation of Pt(IV), Ir(IV) and Rh(III). Therefore, the effect of HCl concentration on the reduction of Ir(IV) during the extraction with LIX 63 was investigated at 3 and 6 M HCl solutions. The extraction behavior of Iridium by Aliquat 336 from the Pd(II) free raffinate showed that the percentage of iridium extraction rapidly decreased when HCl concentration was increased from 3 to 6 M, indicating that more Ir(IV) was reduced to Ir(III). Extraction schemes for the separation of Pt(IV), iridium and Rh(III) by Aliquat 336 from 3 and 6 M HCl solutions were investigated.

Effects of microstructure and composition of anode Pt based electrocatalysts on performance of direct alcohol fuel cells

Energy Technology Data Exchange (ETDEWEB)

Jiang, L.; Li, H.; Yan, S.; Sun, G. [Dalian Inst. of Chemical Physics, Dalian (China). Direct Alcohol Fuel Cell Lab; Xin, Q. [Dalian Inst. of Chemical Physics, Dalian (China). Direct Alcohol Fuel Cell Lab; Dalian Inst. of Chemical Physics, Dalian (China). State Key Laboratory of Catalysis

2008-07-01

This paper reported on a study in which platinum (Pt)-based electrocatalysts were synthesized and characterized by XRD, TEM and EDS. The focus of the study was on the relationship between the microstructure and components of PtRu and PtSn catalysts and the performance of direct alcohol fuel cells (DAFCs). All of the Pt-based electrocatalysts were prepared by a modified polyol method. XRD patterns of the 2 catalysts showed that both catalysts have an fcc pattern of Pt. This was also confirmed by the shift of diffraction peaks of Pt in both catalysts. Electrochemical measurements were carried out using an EG and G model 273A potentiostat/galvanostat and a three-electrode test cell at room temperature. Membrane electrode assemblies (MEAs) were fabricated with a pair of stainless steel plates with parallel flow-fields. The MEAs were activated by 1 M methanol/ethanol at 75 degrees C for 3 hours before all the data were collected. The study showed that PtRu is active to methanol electrooxidation while PtSn is active to ethanol electrooxidation. Based on the above experimental analysis, it was determined that the dilatation of Pt lattice parameter is favourable for ethanol adsorption, while the suitable contract of Pt lattice parameter is favorable for methanol electrooxidation. Since Pt is more electronegative than Sn, the partial electrons of Sn atom could be transferred to Pt atom leading to filling of Pt d band. Although Ru is as electronegative as Pt, the electric effect of Pt and Ru may not be as pronounced. 4 refs., 4 figs.

Acetylene and carbon monoxide oxidation over a Pt/Rh/CeO2/γ-Al2O3 automotive exhaust gas catalyst: kinetic modelling of transient experiments

NARCIS (Netherlands)

Harmsen, J.M.A.; Hoebink, J.H.B.J.; Schouten, J.C.

2001-01-01

The transient kinetics of acetylene (C2H2) conversion by oxygen over a commercial Pt/Rh/CeO2/¿-Al2O3 three-way catalyst have been modelled. Experiments to validate the model were carried out in a fixed-bed reactor with two separate inlets, enabling alternate feeding of acetylene and oxygen.

Hydrogen production from bio-fuels using precious metal catalysts

Science.gov (United States)

Pasel, Joachim; Wohlrab, Sebastian; Rotov, Mikhail; Löhken, Katrin; Peters, Ralf; Stolten, Detlef

2017-11-01

Fuel cell systems with integrated autothermal reforming unit require active and robust catalysts for H2 production. Thus, an experimental screening of catalysts for autothermal reforming of commercial biodiesel fuel was performed. Catalysts consisted of a monolithic cordierite substrate, an oxide support (γ-Al2O3) and Pt, Ru, Ni, PtRh and PtRu as active phase. Experiments were run by widely varying the O2/C and H2O/C molar ratios at different gas hourly space velocities. Fresh and aged catalysts were characterized by temperature programmed methods and thermogravimetry to find correlations with catalytic activity and stability.

Successful treatment of Rh alloimmunization in a twin pregnancy: case report

Directory of Open Access Journals (Sweden)

Rahimi Sharbaf F

2008-09-01

Full Text Available "n Normal 0 false false false EN-US X-NONE AR-SA MicrosoftInternetExplorer4 /* Style Definitions */ table.MsoNormalTable {mso-style-name:"Table Normal"; mso-tstyle-rowband-size:0; mso-tstyle-colband-size:0; mso-style-noshow:yes; mso-style-priority:99; mso-style-qformat:yes; mso-style-parent:""; mso-padding-alt:0in 5.4pt 0in 5.4pt; mso-para-margin-top:0in; mso-para-margin-right:0in; mso-para-margin-bottom:10.0pt; mso-para-margin-left:0in; line-height:115%; mso-pagination:widow-orphan; font-size:11.0pt; font-family:"Calibri","sans-serif"; mso-ascii-font-family:Calibri; mso-ascii-theme-font:minor-latin; mso-fareast-font-family:"Times New Roman"; mso-fareast-theme-font:minor-fareast; mso-hansi-font-family:Calibri; mso-hansi-theme-font:minor-latin;} Background: The prevalence of Rh alloimmunization has decreased following the use of anti-D immunoglobulin. With serial amniocentesis, Doppler sonography of the middle cerebral artery and treatment of anemia with intrauterine blood transfusion, perinatal mortality has declined. However, Rh alloimmunization in twin pregnancies poses a diagnostic and therapeutic challenge."n"n Case report: We are reporting, for the first time in Iran, the successful treatment of severe Rh alloimmunization in a dichorionic- diamnionic twin pregnancy leading to the live births of both neonates. Before treatment, the fetal hemoglobin levels were 3.1g/dL and 3.9g/dL, with ascites in both fetuses. The fetuses were treated with several IUTs."n"n Results: After treatment, the neonates were delivered, weighing 2200 and 2300g, with good Apgar scores, at a gestational age of 34 weeks. "n"n Conclusion: 10% of population in Iran is Rh-negative, although Prophylaxis for Rh alloimmunization is universal, as other part of the world it cannot irrigated. For the best management of these cases, we need a well-equipped referral center."n"n Keywords: Twin, pregnancy, Rh alloimmunization, intrauterine blood transfusion, Doppler, middle cerebral

Improving The Efficiency Of Ammonia Electrolysis For Hydrogen Production

Science.gov (United States)

Palaniappan, Ramasamy

Given the abundance of ammonia in domestic and industrial wastes, ammonia electrolysis is a promising technology for remediation and distributed power generation in a clean and safe manner. Efficiency has been identified as one of the key issues that require improvement in order for the technology to enter the market phase. Therefore, this research was performed with the aim of improving the efficiency of hydrogen production by finding alternative materials for the cathode and electrolyte. 1. In the presence of ammonia the activity for hydrogen evolution reaction (HER) followed the trend Rh>Pt>Ru>Ni. The addition of ammonia resulted in lower rates for HER for Pt, Ru, and Ni, which have been attributed to competition from the ammonia adsorption reaction. 2. The addition of ammonia offers insight into the role of metal-hydrogen underpotential deposition (M-Hupd) on HER kinetics. In addition to offering competition via ammonia adsorption it resulted in fewer and weaker M-Hupd bonds for all metals. This finding substantiates the theory that M-Hupd bonds favor HER on Pt electrocatalyst. However, for Rh results suggest that M-Hupd bond may hinder the HER. In addition, the presence of unpaired valence shell electrons is suggested to provide higher activity for HER in the presence of ammonia. 3. Bimetals PtxM1-x (M = Ir, Ru, Rh, and Ni) offered lower overpotentials for HER compared to the unalloyed metals in the presence of ammonia. The activity of HER in the presence of ammonia follows the trend Pt-Ir>Pt-Rh>Pt-Ru>Pt-Ni. The higher activity of HER is attributed to the synergistic effect of the alloy, where ammonia adsorbs onto the more electropositive alloying metal leaving Pt available for Hupd formation and HER to take place. Additionally, this supports the theory that the presence of a higher number of unpaired electrons favors the HER in the presence of ammonia. 4. Potassium polyacrylate (PAA-K) was successfully used as a substitute for aqueous KOH for ammonia

Characterization and methanol electrooxidation studies of Pt(111)/Os surfaces prepared by spontaneous deposition.

Science.gov (United States)

Johnston, Christina M; Strbac, Svetlana; Lewera, Adam; Sibert, Eric; Wieckowski, Andrzej

2006-09-12

Catalytic activity of the Pt(111)/Os surface toward methanol electrooxidation was optimized by exploring a wide range of Os coverage. Various methods of surface analyses were used, including electroanalytical, STM, and XPS methods. The Pt(111) surface was decorated with nanosized Os islands by spontaneous deposition, and the Os coverage was controlled by changing the exposure time to the Os-containing electrolyte. The structure of Os deposits on Pt(111) was characterized and quantified by in situ STM and stripping voltammetry. We found that the optimal Os surface coverage of Pt(111) for methanol electrooxidation was 0.7 +/- 0.1 ML, close to 1.0 +/- 0.1 Os packing density. Apparently, the high osmium coverage Pt(111)/Os surface provides more of the necessary oxygen-containing species (e.g., Os-OH) for effective methanol electrooxidation than the Pt(111)/Os surfaces with lower Os coverage (vs e.g., Ru-OH). Supporting evidence for this conjecture comes from the CO electrooxidation data, which show that the onset potential for CO stripping is lowered from 0.53 to 0.45 V when the Os coverage is increased from 0.2 to 0.7 ML. However, the activity of Pt(111)/Os for methanol electrooxidation decreases when the Os coverage is higher than 0.7 +/- 0.1 ML, indicating that Pt sites uncovered by Os are necessary for sustaining significant methanol oxidation rates. Furthermore, osmium is inactive for methanol electrooxidation when the platinum substrate is absent: Os deposits on Au(111), a bulk Os ingot, and thick films of electrodeposited Os on Pt(111), all compare poorly to Pt(111)/Os. We conclude that a bifunctional mechanism applies to the methanol electrooxidation similarly to Pt(111)/Ru, although with fewer available Pt sites. Finally, the potential window for methanol electrooxidation on Pt(111)/Os was observed to shift positively versus Pt(111)/Ru. Because of the difference in the Os and Ru oxophilicity under electrochemical conditions, the Os deposit provides fewer

Electrochemical evaluation of Pt-Based binary catalysts on various supports for the direct methanol fuel cell

CSIR Research Space (South Africa)

Khotseng, L

2016-01-01

Full Text Available Ru/MoO(sub2) > PtSn/TiO(sub2) > PtRu/TiO(sub2). It was also observed that catalysts supported on MWCNTs were more active than those supported on metal oxides. Furthermore, catalysts supported on MWCNTs proved to be more stable than all the other supported...

Direct determination of platinum group elements and their distributions in geological and environmental samples at the ng g{sup -1} level using LA-ICP-IDMS

Energy Technology Data Exchange (ETDEWEB)

Boulyga, Sergei F.; Heumann, Klaus G. [Johannes Gutenberg-University Mainz, Institute of Inorganic Chemistry and Analytical Chemistry, Mainz (Germany)

2005-10-01

Laser ablation inductively coupled plasma isotope dilution mass spectrometry (LA-ICP-IDMS) was applied to the direct and simultaneous determination of the platinum group elements (PGEs) Pt, Pd, Ru, and Ir in geological and environmental samples. A special laser ablation system with high ablation rates was used, along with sector field ICP-MS. Special attention was paid to deriving the distributions of PGEs in the pulverized samples. IDMS could not be applied to the (mono-isotopic) Rh, but the similar ablation behavior of Ru and Rh allowed Rh to be simultaneously determined via relative sensitivity coefficients. The laser ablation process produces hardly any oxide ions (which usually cause interference in PGE analysis with liquid sample injection), so the ICP-MS can be run in its low mass resolution but high-sensitivity mode. The detection limits obtained for the geological samples were 0.16 ng g{sup -1}, 0.14 ng g{sup -1}, 0.08 ng g{sup -1}, 0.01 ng g{sup -1} and 0.06 ng g{sup -1} for Ru, Rh, Pd, Ir and Pt, respectively. LA-ICP-IDMS was applied to different geological reference materials (TDB-1, WGB-1, UMT-1, WMG-1, SARM-7) and the road dust reference material BCR-723, which are only certified for some of the PGEs. Comparisons with certified values as well as with indicative values from the literature demonstrated the validity of the LA-ICP-IDMS method. The PGE concentrations in subsamples of the road dust reference material correspond to a normal distribution, whereas the distributions in the geological reference materials TDB-1, WGB-1, UMT-1, WMG-1, and SARM-7 are more complex. For example, in the case of Ru, a logarithmic normal distribution best fits the analyzed concentrations in TDB-1 subsamples, whereas a pronounced nugget effect was found for Pt in most geological samples. (orig.)

Direct determination of platinum group elements and their distributions in geological and environmental samples at the ng g(-1) level using LA-ICP-IDMS.

Science.gov (United States)

Boulyga, Sergei F; Heumann, Klaus G

2005-10-01

Laser ablation inductively coupled plasma isotope dilution mass spectrometry (LA-ICP-IDMS) was applied to the direct and simultaneous determination of the platinum group elements (PGEs) Pt, Pd, Ru, and Ir in geological and environmental samples. A special laser ablation system with high ablation rates was used, along with sector field ICP-MS. Special attention was paid to deriving the distributions of PGEs in the pulverized samples. IDMS could not be applied to the (mono-isotopic) Rh, but the similar ablation behavior of Ru and Rh allowed Rh to be simultaneously determined via relative sensitivity coefficients. The laser ablation process produces hardly any oxide ions (which usually cause interference in PGE analysis with liquid sample injection), so the ICP-MS can be run in its low mass resolution but high-sensitivity mode. The detection limits obtained for the geological samples were 0.16 ng g(-1), 0.14 ng g(-1), 0.08 ng g(-1), 0.01 ng g(-1) and 0.06 ng g(-1) for Ru, Rh, Pd, Ir and Pt, respectively. LA-ICP-IDMS was applied to different geological reference materials (TDB-1, WGB-1, UMT-1, WMG-1, SARM-7) and the road dust reference material BCR-723, which are only certified for some of the PGEs. Comparisons with certified values as well as with indicative values from the literature demonstrated the validity of the LA-ICP-IDMS method. The PGE concentrations in subsamples of the road dust reference material correspond to a normal distribution, whereas the distributions in the geological reference materials TDB-1, WGB-1, UMT-1, WMG-1, and SARM-7 are more complex. For example, in the case of Ru, a logarithmic normal distribution best fits the analyzed concentrations in TDB-1 subsamples, whereas a pronounced nugget effect was found for Pt in most geological samples.

Kinetic study of the ethene oxidation by oxygen in the presence of carbon dioxide and steam over Pt/Rh/CeO2/g-Al2O3

NARCIS (Netherlands)

Nibbelke, R.H.; Kreijveld, R.J.M.; Hoebink, J.H.B.J.; Marin, G.B.M.M.; Kruse, N.

1998-01-01

The oxidation of ethene by oxygen in the presence of steam and carbon dioxide over a commercially available Pt/Rh/CeO2/¿-Al2O3 three-way automotive catalyst was studied. Experiments were carried out in a fixed-bed micro reactor under intrinsic conditions, i.e. in the absence of external and internal

Rare earth-rich cadmium compounds RE{sub 10}TCd{sub 3} (RE = Y, Tb, Dy, Ho, Er, Tm, Lu; T = Rh, Pd, Ir, Pt) with an ordered Co{sub 2}Al{sub 5}-type structure

Energy Technology Data Exchange (ETDEWEB)

Block, Theresa; Klenner, Steffen; Heletta, Lukas; Poettgen, Rainer [Muenster Univ. (Germany). Inst. fuer Anorganische und Analytische Chemie

2018-04-01

Eighteen new rare earth-rich intermetallic phases RE{sub 10}TCd{sub 3} (RE = Y, Tb, Dy, Ho, Er, Tm, Lu; T = Rh, Pd, Ir, Pt) were obtained by induction melting of the elements in sealed niobium ampoules followed by annealing in muffle furnaces. All samples were characterized by X-ray powder diffraction. The structures of four representatives were refined from single-crystal X-ray diffractometer data: ordered Co{sub 2}Al{sub 5} type, P6{sub 3}/mmc, a = 951.2(1), c = 962.9(2) pm, wR = 0.0460, 595 F{sup 2} values, 20 parameters for Er{sub 10}RhCd{sub 3}; a = 945.17(4), c = 943.33(4), wR = 0.0395, 582 F{sup 2} values, 21 parameters for Lu{sub 9.89}PdCd{sub 3.11}; a = 964.16(6), c = 974.93(6) pm, wR = 0.0463, 614 F{sup 2} values, 21 parameters for Y{sub 10}Ir{sub 1.09}Cd{sub 2.91}; a = 955.33(3), c = 974.56(3) pm, wR = 0.0508, 607 F{sup 2} values, 22 refined parameters for Dy{sub 9.92}IrCd{sub 3.08}. Refinements of the occupancy parameters revealed small homogeneity ranges resulting from RE/Cd, respectively T/Cd mixing. The basic building units of the RE{sub 10}TCd{sub 3} phases are transition metal-centered RE{sub 6} trigonal prisms (TP) that are condensed with double-pairs of empty RE{sub 6} octahedra via common triangular faces. A second type of rods is formed by slightly distorted RE3 rate at Cd{sub 6}RE{sub 6} icosahedra which are condensed via Cd{sub 3} triangular faces. The shortest interatomic distances occur for RE-T, compatible with strong covalent bonding interactions. Temperature dependent magnetic susceptibility measurements were performed for RE{sub 10}RhCd{sub 3} (RE = Dy-Tm, Lu), RE{sub 10}IrCd{sub 3} (RE = Er, Tm, Lu) and RE{sub 10}PtCd{sub 3} (RE = Y, Lu). While Y{sub 10}PtCd{sub 3} and Lu{sub 10}TCd{sub 3} (T = Rh, Ir, Pt) show Pauli paramagnetic behavior, the compounds containing paramagnetic rare earth elements show Curie-Weiss behavior (the experimental magnetic moments indicate stable trivalent RE{sup 3+}) and magnetic ordering at low temperatures

Gibbs Free Energy of Formation for Selected Platinum Group Minerals (PGM

Directory of Open Access Journals (Sweden)

Spiros Olivotos

2016-01-01

Full Text Available Thermodynamic data for platinum group (Os, Ir, Ru, Rh, Pd and Pt minerals are very limited. The present study is focused on the calculation of the Gibbs free energy of formation (ΔfG° for selected PGM occurring in layered intrusions and ophiolite complexes worldwide, applying available experimental data on their constituent elements at their standard state (ΔG = G(species − ΔG(elements, using the computer program HSC Chemistry software 6.0. The evaluation of the accuracy of the calculation method was made by the calculation of (ΔGf of rhodium sulfide phases. The calculated values were found to be ingood agreement with those measured in the binary system (Rh + S as a function of temperature by previous authors (Jacob and Gupta (2014. The calculated Gibbs free energy (ΔfG° followed the order RuS2 < (Ir,OsS2 < (Pt, PdS < (Pd, PtTe2, increasing from compatible to incompatible noble metals and from sulfides to tellurides.

Electrocatalytic activity of atomic layer deposited Pt–Ru catalysts onto N-doped carbon nanotubes

DEFF Research Database (Denmark)

Johansson, Anne-Charlotte Elisabeth Birgitta; Larsen, Jackie Vincent; Verheijen, Marcel A.

2014-01-01

(ethylcyclopentadienyl)ruthenium (Ru(EtCp)2), respectively. O2 was used as the reactant in both processes. The composition of the catalysts was easily tuned by varying the Pt-to-Ru ALD cycle ratio. The catalysts were tested toward the CO oxidation and methanol oxidation reaction (MOR) in a three-electrode electrochemical set...

Hydrogen production from bio-fuels using precious metal catalysts

Directory of Open Access Journals (Sweden)

Pasel Joachim

2017-01-01

Full Text Available Fuel cell systems with integrated autothermal reforming unit require active and robust catalysts for H2 production. Thus, an experimental screening of catalysts for autothermal reforming of commercial biodiesel fuel was performed. Catalysts consisted of a monolithic cordierite substrate, an oxide support (γ-Al2O3 and Pt, Ru, Ni, PtRh and PtRu as active phase. Experiments were run by widely varying the O2/C and H2O/C molar ratios at different gas hourly space velocities. Fresh and aged catalysts were characterized by temperature programmed methods and thermogravimetry to find correlations with catalytic activity and stability.

Novel RuCoSe as non-platinum catalysts for oxygen reduction reaction in microbial fuel cells

Science.gov (United States)

Rozenfeld, Shmuel; Schechter, Michal; Teller, Hanan; Cahan, Rivka; Schechter, Alex

2017-09-01

Microbial electrochemical cells (MECs) are explored for the conversion of acetate directly to electrical energy. This device utilizes a Geobacter sulfurreducens anode and a novel RuCoSe air cathode. RuCoSe synthesized in selected compositions by a borohydride reduction method produces amorphous structures of powdered agglomerates. Oxygen reduction reaction (ORR) was measured in a phosphate buffer solution pH 7 using a rotating disc electrode (RDE), from which the kinetic current (ik) was measured as a function of potential and composition. The results show that ik of RuxCoySe catalysts increases in the range of XRu = 0.25 > x > 0.7 and y < 0.15 for all tested potentials. A poisoning study of RuCoSe and Pt catalysts in a high concentration acetate solution shows improved tolerance of RuCoSe to this fuel at acetate concentration ≥500 mM. MEC discharge plots under physiological conditions show that ∼ RuCo2Se (sample S3) has a peak power density of 750 mW cm-2 which is comparable with Pt 900 mW cm-2.

Experimental investigation of air relative humidity (RH) cycling tests on MEA/cell aging in PEMFC. Pt. I. Study of high RH cycling test with air RH at 62%/100%

Energy Technology Data Exchange (ETDEWEB)

Huang, B.T.; Chatillon, Y.; Bonnet, C.; Lapicque, F. [Laboratoire Reactions et Genie des Procedes, CNRS-Nancy University, Nancy (France); Leclerc, S. [Laboratoire d' Energetique et de Mecanique Theorique et Appliquee, CNRS-Nancy University, Vandoeuvre-les-Nancy (France); Hinaje, M.; Rael, S. [Groupe de Recherche en Electrotechnique et Electronique de Nancy, CNRS-Nancy University, Vandoeuvre-les-Nancy (France)

2012-06-15

The effect of high air relative humidity (RH) cycling (RH{sub C} 62%/100%) on the degradation mechanisms of a single (5 x 5 cm{sup 2}) proton exchange membrane fuel cells was investigated. The cell performance was compared to a cell operated at constant humidification (RH{sub C} = 62%). Runs were conducted over approximately 1,500 h at 0.3 A cm{sup -2}. The overall loss in cell performance for the high RH cycling test was 12 {mu}V h{sup -1} whereas it was at 3 {mu}V h{sup -1} under constant humidification. Impedance spectroscopy reveals that the ohmic and charge transfer resistances were little modified in both runs. H{sub 2} crossover measurement indicated that both high RH cycling and constant RH test did not promote serious effect on gas permeability. The electroactive surface loss for anode and cathode during high air RH cycling was more significant than at constant RH operation. The water uptake determined by {sup 1}H nuclear magnetic resonance within the membrane electrode assembly (MEA) after high RH cycling was reduced by 12% in comparison with a fresh MEA. Transmission electron microscopy showed bubbles and pinholes formation in the membrane, catalyst particles agglomeration (also observed by X-ray diffraction), catalyst particles migration in the membrane and thickness reduction of the catalytic layers. Scanning electron microscopy was conducted to observe the changes in morphology of gas diffusion layers after the runs. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

First principles study on the interfacial properties of NM/graphdiyne (NM = Pd, Pt, Rh and Ir): The implications for NM growing

Energy Technology Data Exchange (ETDEWEB)

Lu, Zhansheng; Li, Shuo; Lv, Peng [College of Physics and Electronic Engineering, Henan Normal University, Xinxiang 453007 (China); He, Chaozheng, E-mail: hecz2013@nynu.edu.cn [College of Physics and Electronic Engineering, Nanyang Normal University, Nanyang 473061 (China); Ma, Dongwei [School of Physics, Anyang Normal University, Anyang 455000 (China); Yang, Zongxian, E-mail: yzx@henannu.edu.cn [College of Physics and Electronic Engineering, Henan Normal University, Xinxiang 453007 (China); Collaborative Innovation Center of Nano Functional Materials and Applications, Kaifeng (China)

2016-01-01

Graphical abstract: - Highlights: • The NM adatoms belong to embedded adsorption in 18C-hexagon of GDY. • The Rh and Ir/GDY can be applied to single metal catalysts or sensors. • A simple linear relationship between E{sub e-ads} and E{sub b} is presented. • The linear relationship can be used in the noble metal modified GDY. - Abstract: Based on the dispersion-corrected density functional calculations (DFT-D), we systematically studied the adsorption of noble metals (NM), Pd, Pt, Rh and Ir, on graphdiyne (GDY). We present a systematic study on the geometry, embedded adsorption energy and electronic structure of four different adatoms adsorbed on the GDY. The strong interaction between the NM adatoms and the GDY substrate is found with the NM embedded in the 18C-hexagon of the GDY. We investigated the mobility of the NM adatoms on the GDY, and found that the mobility barrier energy increases along with the increasing of the embedded adsorption energy. We present the NM adatoms growth of high concentrations on the GDY. Upon the analysis of the electronic structure and the frontier molecular orbitals, Rh and Ir adatoms of low concentrations (about 1.37 at%) on the GDY have the potential to be applied as single metal catalysts or gas molecule sensors.

Adsorption of Ruthenium, Rhodium and Palladium from Simulated High-Level Liquid Waste by Highly Functional Xerogel - 13286

Energy Technology Data Exchange (ETDEWEB)

Onishi, Takashi [Fukushima Fuels and Materials Department O-arai Research and Development Center Japan Atomic Energy Agency, Narita-cho 4002, O-arai-machi, Ibaraki, 311-1393 (Japan); Koyama, Shin-ichi [Fukushima Fuels and Materials Department O-arai Research and Development Center Japan Atomic Energy Agency, Narita-cho 4002, O-arai-machi, Ibaraki, 311-1393 (Japan); Mimura, Hitoshi [Dept. of Quantum Science and Energy Engineering, Graduate School of Engineering, Tohoku University Aramaki-Aza-Aoba 6-6-01-2,Aoba-ku, Sendai-shi, Miyagi-ken, 980-8579 (Japan)

2013-07-01

Fission products are generated by fission reactions in nuclear fuel. Platinum group (Pt-G) elements, such as palladium (Pd), rhodium (Rh) and ruthenium (Ru), are also produced. Generally, Pt-G elements play important roles in chemical and electrical industries. Highly functional xerogels have been developed for recovery of these useful Pt-G elements from high - level radioactive liquid waste (HLLW). An adsorption experiment from simulated HLLW was done by the column method to study the selective adsorption of Pt-G elements, and it was found that not only Pd, Rh and Ru, but also nickel, zirconium and tellurium were adsorbed. All other elements were not adsorbed. Adsorbed Pd was recovered by washing the xerogel-packed column with thiourea solution and thiourea - nitric acid mixed solution in an elution experiment. Thiourea can be a poison for automotive exhaust emission system catalysts, so it is necessary to consider its removal. Thermal decomposition and an acid digestion treatment were conducted to remove sulfur in the recovered Pd fraction. The relative content of sulfur to Pd was decreased from 858 to 0.02 after the treatment. These results will contribute to design of the Pt-G element separation system. (authors)

A novel binary Pt 3Te x/C nanocatalyst for ethanol electro-oxidation

Science.gov (United States)

Huang, Meihua; Wang, Fei; Li, Lirong; Guo, Yonglang

The Pt 3Te x/C nanocatalyst was prepared and its catalytic performance for ethanol oxidation was investigated for the first time. The Pt 3Te/C nanoparticles were characterized by an X-ray diffractometer (XRD), transmission electron microscope (TEM) and energy dispersive X-ray spectroscopy equipped with TEM (TEM-EDX). The Pt 3Te/C catalyst has a typical fcc structure of platinum alloys with the presence of Te. Its particle size is about 2.8 nm. Among the synthesized catalysts with different atomic ratios, the Pt 3Te/C catalyst has the highest anodic peak current density. The cyclic voltammograms (CV) show that the anodic peak current density for the Pt 3Te/C, commercial PtRu/C and Pt/C catalysts reaches 1002, 832 and 533 A g -1, respectively. On the current-time curve, the anodic current on the Pt 3Te/C catalyst was higher than those for the catalysts reported. So, these findings show that the Pt 3Te/C catalyst has uniform nanoparticles and the best activity among the synthesized catalysts, and it is better than commercial PtRu/C and Pt/C catalysts for ethanol oxidation at room temperature.

Eletroxidação de etanol em eletrodos de platina modificados por ródio - estudos empregando eletrodos dispersos e eletrodos monocristalinos

OpenAIRE

Melina D\\'Villa Silva

2010-01-01

No presente trabalho foi estudado catalisadores dispersos em carbono contendo Pt, PtRh e PtRhRu para eletroxidação de etanol. Os catalisadores foram preparados em ultra-som e caracterizados por EDX, DRX e MET e sua atividade catalítica estudada através das técnicas de voltametria cíclica e DEMS. Os resultados experimentais indicaram que a adição de ródio diminui o potencial de início de oxidação de etanol, embora também diminua a corrente faradáica. Os estudos de DEMS mostraram que com a pres...

Copper-based alloys, crystallographic and crystallochemical parameters of alloys in binary systems Cu-Me (Me=Co, Rh, Ir, Cu, Ag, Au, Ni, Pd, Pt)

Energy Technology Data Exchange (ETDEWEB)

Porobova, Svetlana, E-mail: porobova.sveta@yandex.ru; Loskutov, Oleg, E-mail: lom58@mail.ru [Tomsk State University of Architecture and Building, Russia, Tomsk, 2 Solyanaya sq, Tomsk, 634003 (Russian Federation); Markova, Tat’jana, E-mail: patriot-rf@mail.ru [Siberian State Industrial University. 42 Kirov St., Novokuznetsk, 654007 (Russian Federation); Klopotov, Vladimir, E-mail: vdklopotov@mail.ru [Research Tomsk Polytechnic University, 30 Lenin Ave., Tomsk, 634050 (Russian Federation); Klopotov, Anatoliy, E-mail: klopotovaa@tsuab.ru [Tomsk State University of Architecture and Building, Russia, Tomsk, 2 Solyanaya sq, Tomsk, 634003 (Russian Federation); National Research Tomsk State University, 36, Lenin Ave., Tomsk, 634050 (Russian Federation); Vlasov, Viktor, E-mail: vik@tsuab.ru [Tomsk State University of Architecture and Building, Russia, Tomsk, 2 Solyanaya sq, Tomsk, 634003 (Russian Federation); Research Tomsk Polytechnic University, 30 Lenin Ave., Tomsk, 634050 (Russian Federation)

2016-01-15

The article presents the results of the analysis of phase equilibrium of ordered phases in binary systems based on copper Cu- Me (where Me - Co, Rh, Ir, Ag, Au, Ni, Pd, Pt) to find correlations of crystallochemical and crystallographic factors. It is established that the packing index in disordered solid solutions in binary systems based on copper is close to the value of 0.74 against the background of an insignificant deviation of atomic volumes from the Zen’s law.

Standard enthalpies of formation of selected Rh2YZ Heusler compounds

International Nuclear Information System (INIS)

Yin, Ming; Nash, Philip

2015-01-01

The standard enthalpies of formation (Δ f H°) of selected ternary Rh-based Rh 2 YZ (Y = Cu, Fe, Mn, Ni, Ru, Ti, V; Z = Al, Ga, In, Si, Ge, Sn) compounds were measured using high temperature direct reaction calorimetry. The measured standard enthalpies of formation (in kJ/mol of atoms) are, for the Heusler compound Rh 2 MnSn (−40.1 ± 3.6), for the B2-structured compounds: Rh 2 FeAl (−48.5 ± 2.9); Rh 2 MnAl (−72.4 ± 2.7); Rh 2 MnGa (−55.3 ± 2.0); Rh 2 MnIn (−35.3 ± 1.9), for the tetragonal compounds: Rh 2 FeSn (−28.9 ± 1.3); Rh 2 TiAl (−97.6 ± 2.2); Rh 2 TiGa (−79.0 ± 1.8); Rh 2 TiSn (−74.7 ± 3.1). Values are compared with those from first principles calculations in published papers and the Open Quantum Materials Database (OQMD). Lattice parameters of these compounds are determined using X-ray diffraction analysis (XRD). Microstructures were characterized using scanning electron microscopy (SEM) and Energy Dispersive Spectroscopy (EDS). - Highlights: • Standard enthalpies of formation of Rh 2 YZ were measured using a drop calorimeter. • Measured enthalpies agree with first principles data in general. • Lattice parameters and related phase relationships were consistent with literature data. • Rh 2 TiSn of tI8 structure were reported for the first time.

Electrochemical CO2 and CO reduction on metal-functionalized porphyrin-like graphene

DEFF Research Database (Denmark)

Tripkovic, Vladimir; Vanin, Marco; Karamad, Mohammedreza

2013-01-01

Porphyrin-like metal-functionalized graphene structures have been investigated as possible catalysts for CO2 and CO reduction to methane or methanol. The late transition metals (Cu, Ag, Au, Ni, Pd, Pt, Co, Rh, Ir, Fe, Ru, Os) and some p (B, Al, Ga) and s (Mg) metals comprised the center of the po......Porphyrin-like metal-functionalized graphene structures have been investigated as possible catalysts for CO2 and CO reduction to methane or methanol. The late transition metals (Cu, Ag, Au, Ni, Pd, Pt, Co, Rh, Ir, Fe, Ru, Os) and some p (B, Al, Ga) and s (Mg) metals comprised the center...... instead of CO2. Volcano plots were constructed on the basis of scaling relations of reaction intermediates, and from these plots the reaction steps with the highest overpotentials were deduced. The Rh-porphyrin-like functionalized graphene was identified as the most active catalyst for producing methanol...... from CO, featuring an overpotential of 0.22 V. Additionally, we have also examined the hydrogen evolution and oxidation reaction, and in their case, too, Rh-porphyrin turned out to be the best catalyst with an overpotential of 0.15 V. © 2013 American Chemical Society....

Identification of a Catalytically Highly Active Surface Phase for CO Oxidation over PtRh Nanoparticles under Operando Reaction Conditions

Science.gov (United States)

Hejral, U.; Franz, D.; Volkov, S.; Francoual, S.; Strempfer, J.; Stierle, A.

2018-03-01

Pt-Rh alloy nanoparticles on oxide supports are widely employed in heterogeneous catalysis with applications ranging from automotive exhaust control to energy conversion. To improve catalyst performance, an atomic-scale correlation of the nanoparticle surface structure with its catalytic activity under industrially relevant operando conditions is essential. Here, we present x-ray diffraction data sensitive to the nanoparticle surface structure combined with in situ mass spectrometry during near ambient pressure CO oxidation. We identify the formation of ultrathin surface oxides by detecting x-ray diffraction signals from particular nanoparticle facets and correlate their evolution with the sample's enhanced catalytic activity. Our approach opens the door for an in-depth characterization of well-defined, oxide-supported nanoparticle based catalysts under operando conditions with unprecedented atomic-scale resolution.

Excitation function and yield for the 103Rh(d,2n)103Pd nuclear reaction: Optimization of the production of palladium-103

International Nuclear Information System (INIS)

Manenti, Simone; Alí Santoro, María del Carmen; Cotogno, Giulio; Duchemin, Charlotte; Haddad, Ferid; Holzwarth, Uwe; Groppi, Flavia

2017-01-01

Deuteron-induced nuclear reactions for the generation of 103 Pd were investigated using the stacked-foil activation technique on rhodium targets at deuteron energies up to E d = 33 MeV. The excitation functions of the reactions 103 Rh(d,xn) 101,103 Pd, 103 Rh(d,x) 100g,cum,101m,g,102m,g Rh and 103 Rh(d,2p) 103 Ru have been measured, and the Thick-Target Yield for 103 Pd has been calculated.

Steam reforming of methane over Pt/Rh based wire mesh catalyst in single channel reformer for small scale syngas production

DEFF Research Database (Denmark)

Sigurdsson, Haftor Örn; Kær, Søren Knudsen

2012-01-01

of a catalytic parallel plate type heat exchanger (CPHE) reformer stack, where coated Pt/Rh based wire mesh is used as a catalyst. Heat is supplied to the endothermic reaction with infrared electric heaters. All the experiments were performed under atmospheric pressure and at stable operating conditions......The purpose of this study is to investigate a small scale steam methane reformer for syngas production for a micro combined heat and power (mCPH) unit under different operational conditions. The study presents an experimental analysis of the performance of a specially built single channel...... to evaluate the effect of flow maldistribution in a CPHE reformer stack on the CH4 conversion and H2 yield....

Discovery of fuel cell anode electrocatalysts and dehydrogenation catalysts using combinatorial techniques

Science.gov (United States)

Chan, Benny Chun Wai

A gas diffusion optical screening method was developed for the discovery of catalysts for the electro-oxidation of reformate gas (H2 with 100 ppm CO). The screening cell was designed to accommodate a gas diffusion layer, 715 member catalyst array, and an electrolyte container. Since protons are generated during H2 oxidation, a pH sensitive fluorphore was used to identify active compositions. The cell showed no detectable iR drop across the array and ranked activity of two commercial PtRu and one Pt catalysts. Over 95% of a given catalyst fluoresced at the initial onset potential and a 5 mV difference in onset potential of two different catalysts was statistically different. A gas diffusion half cell was designed similar to the optical screening cell to obtain current-potential curves of bulk catalysts. The screening results correlated with half cell and fuel cell data, internally validating the method. The combinatorial method was then applied to search for catalysts in the PtRuMoIrRh composition space. The catalysts on the array were prepared by hydrogen reduction of the metals salts on carbon. The most active catalysts were from the Pt enriched regions of the PtRuMoRh quaternary. Bulk catalysts were prepared from the active regions and tested in the gas diffusion half cell. The most active catalysts in the optical screening were also the most active catalysts in the half cell. When any homemade catalysts were compared to commercial PtRu, however, the performance was worse. A high surface area, high catalyst activity synthetic method is the most important factor to reliably screen catalysts for "real world" fuel cell application. High surface area catalysts were tested for direct methanol oxidation activity. The optical screening method was compared with disk electrode, high throughput fuel cell testing, and fuel cell testing. Six catalysts examined included two commercial PtRu catalysts, a Pt catalyst, and three homemade PtRu catalysts of varying activity

Metal-isonitrile adducts for preparing radionuclide complexes

International Nuclear Information System (INIS)

Carpenter, A.P.; Linder, K.E.; Maheu, L.J.; Patz, M.A.; Thompson, J.S.; Tulip, T.H.; Subramanyam, V.

1988-01-01

An method for preparing a coordination complex of isonitrile ligand and a radioisotope of Te, Ru, Co, Pt, Re, Os, Ir, W, Re, Cr, Mo, Mn, Ni, Rh, Nb and Ta from a non-radioactive metal adduct of the isonitrile

Experimental investigation of air relative humidity (RH) cycling tests on MEA/cell aging in PEMFC. Pt. II. Study of low RH cycling test with air RH at 62%/0%

Energy Technology Data Exchange (ETDEWEB)

Huang, B.T.; Chatillon, Y.; Bonnet, C.; Lapicque, F. [Laboratoire Reactions et Genie des Procedes, CNRS-Nancy University, Nancy (France); Leclerc, S. [Laboratoire d' Energetique et de Mecanique Theorique et Appliquee, CNRS-Nancy University, Vandoeuvre-les-Nancy (France); Hinaje, M.; Rael, S. [Groupe de Recherche en Electrotechnique et Electronique de Nancy, Nancy University, Vandoeuvre-les-Nancy (France)

2012-06-15

The effect of low relative humidity (RH) cycling (RH{sub C} 62%/0%) on the degradation mechanisms of a single proton exchange membrane fuel cell (5 x 5 cm{sup 2}) was investigated and compared to a cell operated at constant humidification (RH{sub C} = 62%). The overall cell performance loss was near 33 {mu}V h{sup -1}, which is greater than the voltage decay under constant RH condition near 3 {mu}V h{sup -1}. The electroactive surface was reduced but to an acceptable level. Impedance spectroscopy revealed that the ohmic and charge transfer resistances were reduced by the likely improved hydration of the ionomeric layer at the catalyst due to hydrogen crossover. This was so important that H{sub 2} starvation was finally responsible for the collapse of the cell after 650 h. Transmission electron microscopy showed occurrence of various phenomena, e.g., bubbles and pinholes formation in the membrane due to local overheat from hydrogen combustion at the cathode, and thickness reduction of catalytic layers. The water up take obtained by {sup 1}H NMR within the membrane electrode assembly (MEA) after low RH cycling reduced by 24% compared to a fresh MEA. Observations are also compared to those obtained at high RH cycling (RH{sub C} 62%/100%) presented in Part I of this study [1]. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Crystal phase-based epitaxial growth of hybrid noble metal nanostructures on 4H/fcc Au nanowires

Science.gov (United States)

Lu, Qipeng; Wang, An-Liang; Gong, Yue; Hao, Wei; Cheng, Hongfei; Chen, Junze; Li, Bing; Yang, Nailiang; Niu, Wenxin; Wang, Jie; Yu, Yifu; Zhang, Xiao; Chen, Ye; Fan, Zhanxi; Wu, Xue-Jun; Chen, Jinping; Luo, Jun; Li, Shuzhou; Gu, Lin; Zhang, Hua

2018-03-01

Crystal-phase engineering offers opportunities for the rational design and synthesis of noble metal nanomaterials with unusual crystal phases that normally do not exist in bulk materials. However, it remains a challenge to use these materials as seeds to construct heterometallic nanostructures with desired crystal phases and morphologies for promising applications such as catalysis. Here, we report a strategy for the synthesis of binary and ternary hybrid noble metal nanostructures. Our synthesized crystal-phase heterostructured 4H/fcc Au nanowires enable the epitaxial growth of Ru nanorods on the 4H phase and fcc-twin boundary in Au nanowires, resulting in hybrid Au-Ru nanowires. Moreover, the method can be extended to the epitaxial growth of Rh, Ru-Rh and Ru-Pt nanorods on the 4H/fcc Au nanowires to form unique hybrid nanowires. Importantly, the Au-Ru hybrid nanowires with tunable compositions exhibit excellent electrocatalytic performance towards the hydrogen evolution reaction in alkaline media.

Electronic and magnetic properties of infinite 1D chains of paddlewheel carboxylates M2(COOR)4 (M = Mo, W, Ru, Rh, Ir, Cu)

KAUST Repository

Peskov, Maxim

2013-03-14

Dinuclear complexes of transition metals bridged by four carboxylate-groups are examples of stable atomic configurations serving as fundamental building blocks of catalysts and prototypical molecular electronic devices. The electronic structure and magnetic properties of many molecular tetracarboxylate complexes were meticulously studied; however, the properties of the one-dimensional (1D) polymeric chain of associated tetracarboxylates have so far evaded much attention. Using periodic density-functional theory calculations, we analyze the electronic structure of condensed tetracarboxylates Mo(II), W(II), Ru(II), Rh(II), Ir(II), and Cu(II). The relationship between crystal structure of the polymerized tetracarboxylates and the electronic properties of the metal-metal bond in the M24+ core is studied. The electronic effects emanating from the association of dinuclear transition metal tetracarboxylates are important for designing molecular electronic devices. In this study, its influence on both direct and indirect metal-metal interactions, and the electronic structure, in particular transport properties, is discussed. © 2013 American Chemical Society.

Annealing-temperature-dependent voltage-sign reversal in all-oxide spin Seebeck devices using RuO2

Science.gov (United States)

Kirihara, Akihiro; Ishida, Masahiko; Yuge, Ryota; Ihara, Kazuki; Iwasaki, Yuma; Sawada, Ryohto; Someya, Hiroko; Iguchi, Ryo; Uchida, Ken-ichi; Saitoh, Eiji; Yorozu, Shinichi

2018-04-01

Thermoelectric converters based on the spin Seebeck effect (SSE) have attracted great attention due to their potential to offer novel applications such as energy harvesting and heat-flow sensing. For converting a SSE-induced spin current into an electric current, a transition metal film such as Pt, which exhibits large inverse spin-Hall effect (ISHE), has been typically used. In this work, we show an all-oxide SSE device using ruthenium oxide (RuO2) as a conductive film. We found that both the sign and magnitude of the SSE-induced ISHE voltage V appearing in the RuO2 film changes depending on the post annealing temperature, and that the magnitude can become larger than that of a standard SSE device using Pt. The similar sign change was also observed in Hall-resistance measurements of the RuO2 films. X-ray absorption fine structure (XAFS) spectra of as-deposited and annealed RuO2 revealed that the annealing process substantially improved the long-range crystalline order in RuO2. This suggests that change in the crystalline order may modify the dominant ISHE mechanism or electronic states in RuO2, leading to the sign reversal of V as well as the Hall coefficient. Our result demonstrates that RuO2 is an interesting material not only as a practical ISHE film but also as a testbed to study physics of spin-to-charge converters that depend on their crystalline order.

Microwave irradiation for the facile synthesis of transition-metal nanoparticles (NPs) in ionic liquids (ILs) from metal-carbonyl precursors and Ru-, Rh-, and Ir-NP/IL dispersions as biphasic liquid-liquid hydrogenation nanocatalysts for cyclohexene.

Science.gov (United States)

Vollmer, Christian; Redel, Engelbert; Abu-Shandi, Khalid; Thomann, Ralf; Manyar, Haresh; Hardacre, Christopher; Janiak, Christoph

2010-03-22

Stable chromium, molybdenum, tungsten, manganese, rhenium, ruthenium, osmium, cobalt, rhodium, and iridium metal nanoparticles (M-NPs) have been reproducibly obtained by facile, rapid (3 min), and energy-saving 10 W microwave irradiation (MWI) under an argon atmosphere from their metal-carbonyl precursors [M(x)(CO)(y)] in the ionic liquid (IL) 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIm][BF(4)]). This MWI synthesis is compared to UV-photolytic (1000 W, 15 min) or conventional thermal decomposition (180-250 degrees C, 6-12 h) of [M(x)(CO)(y)] in ILs. The MWI-obtained nanoparticles have a very small (TED), and dynamic light scattering (DLS)). The ruthenium, rhodium, or iridium nanoparticle/IL dispersions are highly active and easily recyclable catalysts for the biphasic liquid-liquid hydrogenation of cyclohexene to cyclohexane with activities of up to 522 (mol product) (mol Ru)(-1) h(-1) and 884 (mol product) (mol Rh)(-1) h(-1) and give almost quantitative conversion within 2 h at 10 bar H(2) and 90 degrees C. Catalyst poisoning experiments with CS(2) (0.05 equiv per Ru) suggest a heterogeneous surface catalysis of Ru-NPs.

Hydrothermal synthesis of highly crystalline RuS2 nanoparticles as cathodic catalysts in the methanol fuel cell and hydrochloric acid electrolysis

International Nuclear Information System (INIS)

Li, Yanjuan; Li, Nan; Yanagisawa, Kazumichi; Li, Xiaotian; Yan, Xiao

2015-01-01

Highlights: • Highly crystalline RuS 2 nanoparticles have been first synthesized by a “one-step” hydrothermal method. • The product presents a pure cubic phase of stoichiometric ratio RuS 2 with average particle size of 14.8 nm. • RuS 2 nanoparticles were used as cathodic catalysts in methanol fuel cell and hydrochloric acid electrolysis. • The catalyst outperforms commercial Pt/C in methanol tolerance and stability towards Cl − . - Abstract: Highly crystalline ruthenium sulfide (RuS 2 ) nanoparticles have been first synthesized by a “one-step” hydrothermal method at 400 °C, using ruthenium chloride and thiourea as reactants. The products were characterized by powder X-ray diffraction (XRD), scanning electron microscopy/energy disperse spectroscopy (SEM/EDS), thermo gravimetric-differential thermal analyze (TG-DTA), transmission electron microscopy equipped with selected area electron diffraction (TEM/SAED). Fourier transform infrared spectra (IR), and X-ray photoelectron spectroscopy (XPS). XRD result illustrates that the highly crystalline product presents a pure cubic phase of stoichiometric ratio RuS 2 and the average particle size is 14.8 nm. SEM and TEM images display the products have irregular shape of 6–25 nm. XPS analyst indicates that the sulfur exists in the form of S 2 2− . Cyclic voltammetry (CV), rotating disk electrode (RDE), chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS) measurements are conducted to evaluate the electrocatalytic activity and stability of the highly crystalline RuS 2 nanoparticles in oxygen reduction reaction (ORR) for methanol fuel cell and hydrochloric acid electrolysis. The results illustrate that RuS 2 is active towards oxygen reduction reaction. Although the activity of RuS 2 is lower than that of Pt/C, the RuS 2 catalyst outperforms commercial Pt/C in methanol tolerance and stability towards Cl −

Estudo do efeito de tratamentos térmicos em catalisadores de PtRu/C frente à reação de oxidação de hidrogênio na presença de CO Study of the effect of thermal treatments of PtRu/C catalysts on the hydrogen oxidation reaction in the presence of CO

Directory of Open Access Journals (Sweden)

Pietro Papa Lopes

2007-10-01

Full Text Available In this work the effects of time and temperature of thermal treatments under reducing atmosphere (H2 on PtRu/C catalysts for the hydrogen oxidation reaction (HOR in the presence of CO on a proton exchange membrane fuel cell (PEMFC single cells have been studied. It can be seen that the increase of the treatment temperature leads to an increasing sintering of the catalyst particles with reduction of the active area, although the catalyst treated at 550 ºC presents more CO tolerance for the HOR.

Investigation of the magnetic properties in thin Fe50Pt50-xRhx films by neutron diffraction

Energy Technology Data Exchange (ETDEWEB)

Fenske, J.; Lott, D.; Schreyer, A. [GKSS Research Centre (Germany); Mankey, G.J. [University of Alabama, MINT Center (United States); Schmidt, W.; Schmalzl, K. [Juelich Research Centre (Germany); Tartakowskaya, E. [Institute for Magnetism, National Accademy of Science (United States)

2009-07-01

FePt-based alloys are typically the material of choice for magnetic information storage media. The high magnetic moment of Fe gives a large magnetization and the large atomic number of Pt results in a high magnetic anisotropy. This combination enables the written bits to be smaller than ever before, since magnetic grains with a high magnetic anisotropy are more thermally stable. One way to control the magnetic properties in these materials is through the introduction of a third element into the crystal matrix, e.g. Rh. When Rh is added to replace Pt in the equiatomic alloy, new magnetic phases emerge. Bulk samples of Fe{sub 50}Pt{sub 40}Rh{sub 10} for example, studied by magnetization measurements refer to an antiferromagnetic (AF)/ferromagnetic (FM) phase transition at about 150 K when heated. Additional magnetostriction measurements indicate that the phase transition could also be induced by applying a magnetic field. Here we present results on several Fe{sub 50}Pt{sub 50-x}Rh{sub x} films. These films were examined by neutron diffraction in dependence of temperature and magnetic field. The observed magnetic behaviours differ significant from the behaviour of the bulk system.

Dispersion of Pt, Pd and Rh produced by catalytic converters into the roadside and urban environment. Element speciation study; Dispersion dans l'environnement routier et urbain de Pt, Pd, et Rh emis par les pots d'echappement catalytiques. Etude de la speciation des elements

Energy Technology Data Exchange (ETDEWEB)

Amosse, J.; Delbos, V. [Centre National de la Recherche Scientifique (CNRS), Lab. de Geodynamique des Chaines Alpines, LGCA, UMR 5025, 38 - Grenoble (France)

2002-09-01

This study highlights the dispersion into the French urban environment of platinum group elements (PGEs) used in catalytic converters. Differences were observed between Pt and Rh on the one hand, and Pd on the other one. One experiment, consisting in passing the corrosive gas emissions from engines over the metals heated to 1000 deg. C, showed that Pd was severely corroded by nitrogen oxides. It was concluded that Pd is emitted in nitrate form. Hydrolysis of this nitrate form leads to the formation of soluble species. In situ pH and E{sub h} measurements in the soils concerned confirm this theory when the results are compared with the Pd species predominance diagram. (authors)

Palladium, platinum, rhodium, ruthenium, and iridium in chromitites from the Massif du Sud and Tiebaghi massif, New Caledonia.

Science.gov (United States)

Page, N.J.; Cassard, D.; Haffty, J.

1982-01-01

The massive and disseminated podiform chromitites from 43 mines and other occurrences in the area contain up to (in ppb) Pd 9, Pt 45, Rh 31, Ir 410 and Ru 1300. The possble origins of the chromitites are discussed. -K.A.R.

Magnetic and electronic properties in CeTSi3 and CeTGe3 (T: transition metal)

International Nuclear Information System (INIS)

Shimoda, T.; Okuda, Y.; Takeda, Y.; Ida, Y.; Miyauchi, Y.; Kawai, T.; Fujie, T.; Sugitani, I.; Thamizhavel, A.; Matsuda, T.D.; Haga, Y.; Takeuchi, T.; Nakashima, M.; Settai, R.; Onuki, Y.

2007-01-01

We investigated the magnetic properties of CeTSi 3 (T: Ru, Os, Co, Rh, Ir, Pd and Pt) and CeTGe 3 (T: Co, Rh and Ir) by measuring their electrical resistivity and magnetic susceptibility. CeRuSi 3 , CeOsSi 3 and CeCoSi 3 do not order magnetically, with a large Kondo temperature of about 200K. The other compounds order antiferromagnetically, and are very similar to each other in their magnetic and electronic properties, which is related to a large crystalline electric field (CEF) splitting energy of the 4f electron, about 500K in CeIrSi 3

Size dependent reactivity of metal nanoparticles and alloys supported on HOPG, probed by the H-D exchange and the NH3 decomposition reactions

DEFF Research Database (Denmark)

Fiordaliso, Elisabetta Maria

this investigation have been summarized in a scientific article which has been submitted to the Journal of Physical Chemistry. The second reaction investigated in this thesis is the NH3 decomposition reaction, relevant for hydrogen storage and production in a COx free environment, which has been performed on Ru, Ir......, Rh and Pt thin films, on Ru nanoparticles and on Ir/Ru alloys. Preliminary results indicated that Ru is the most active among the selected metals, but no definitive conclusions can be drawn on the effect of the particle diameter on the decomposition rate. In the case of the Ru/Ir alloys, it is found...

Inhibition of ammonia poisoning by addition of platinum to Ru/α-Al2 O3 for preferential CO oxidation in fuel cells.

Science.gov (United States)

Sato, Katsutoshi; Yagi, Sho; Zaitsu, Shuhei; Kitayama, Godai; Kayada, Yuto; Teramura, Kentaro; Takita, Yusaku; Nagaoka, Katsutoshi

2014-12-01

In polymer electrolyte fuel cell (PEFC) systems, small amounts of ammonia (NH3 ) present in the reformate gas deactivate the supported ruthenium catalysts used for preferential oxidation (PROX) of carbon monoxide (CO). In this study, we investigated how the addition of a small amount of platinum to a Ru/α-Al2 O3 catalyst (Pt/Ru=1:9 w/w) affected the catalyst's PROX activity in both the absence and the presence of NH3 (130 ppm) under conditions mimicking the reformate conditions during steam reforming of natural gas. The activity of undoped Ru/α-Al2 O3 decreased sharply upon addition of NH3 , whereas Pt/Ru/α-Al2 O3 exhibited excellent PROX activity even in the presence of NH3 . Ruthenium K-edge X-ray absorption near-edge structure (XANES) spectra indicated that in the presence of NH3 , some of the ruthenium in the undoped catalyst was oxidized in the presence of NH3 , whereas ruthenium oxidation was not observed with Pt/Ru/α-Al2 O3 . These results suggest that ruthenium oxidation is retarded by the platinum, so that the catalyst shows high activity even in the presence of NH3 . © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Standard enthalpies of formation of selected Rh{sub 2}YZ Heusler compounds

Energy Technology Data Exchange (ETDEWEB)

Yin, Ming, E-mail: myin1@hawk.iit.edu; Nash, Philip

2015-11-25

The standard enthalpies of formation (Δ{sub f}H°) of selected ternary Rh-based Rh{sub 2}YZ (Y = Cu, Fe, Mn, Ni, Ru, Ti, V; Z = Al, Ga, In, Si, Ge, Sn) compounds were measured using high temperature direct reaction calorimetry. The measured standard enthalpies of formation (in kJ/mol of atoms) are, for the Heusler compound Rh{sub 2}MnSn (−40.1 ± 3.6), for the B2-structured compounds: Rh{sub 2}FeAl (−48.5 ± 2.9); Rh{sub 2}MnAl (−72.4 ± 2.7); Rh{sub 2}MnGa (−55.3 ± 2.0); Rh{sub 2}MnIn (−35.3 ± 1.9), for the tetragonal compounds: Rh{sub 2}FeSn (−28.9 ± 1.3); Rh{sub 2}TiAl (−97.6 ± 2.2); Rh{sub 2}TiGa (−79.0 ± 1.8); Rh{sub 2}TiSn (−74.7 ± 3.1). Values are compared with those from first principles calculations in published papers and the Open Quantum Materials Database (OQMD). Lattice parameters of these compounds are determined using X-ray diffraction analysis (XRD). Microstructures were characterized using scanning electron microscopy (SEM) and Energy Dispersive Spectroscopy (EDS). - Highlights: • Standard enthalpies of formation of Rh{sub 2}YZ were measured using a drop calorimeter. • Measured enthalpies agree with first principles data in general. • Lattice parameters and related phase relationships were consistent with literature data. • Rh{sub 2}TiSn of tI8 structure were reported for the first time.

Recoil effect on β-decaying in vivo generators, interpreted for 103Pd/103mRh

International Nuclear Information System (INIS)

Szucs, Zoltan; Rooyen, Johann van; Zeevaart, Jan Rijn

2009-01-01

The use of Auger emitters as potential radiopharmaceuticals is being increasingly investigated. One of the radionuclides of interest is 103m Rh, which can be produced from 103 Ru or 103 Pd in an in vivo generator. A potential problem, however, is the recoil of the 103m Rh out of the carrier molecule and even out of the target cell. In order to determine the likelihood of this happening in the 103 Pd/ 103m Rh, case calculations were made to prove that this does not happen. The equations were generalised for all radionuclides with an atomic mass of 10-240 as a tool for determining the recoil threshold of any β-emitting radionuclide.

Isobaric yields and radiochemistry of near-target residues in the interaction of 12C and 16O with 103Rh at an incident energy of 400 MeV

International Nuclear Information System (INIS)

Buthelezi, E.Z.; Steyn, G.F.; Walt, T.N. Van der; Aardaneh, K.; Gadioli, E.; Albertini, F.; Cerutti, F.; Connell, S.H.; Cowley, A.A.; Nortier, F.M.

2003-01-01

Production cross sections of residues with mass near to that of the target were measured in 12 C and 16 O induced reactions on Rh at an incident energy of 400 MeV. An ion-exchange method has been developed for the separation of Rh, Pd and Ag nuclides from all other produced activities. Rh and Ag nuclides were separated from elements such as Pd, Ru, and Tc, amongst others, on an AG1-X8 anion exchange resin in 6M HCl. The Ag nuclides were then removed from the effluent using a precipitation technique so that only Rh remained in the final solution. The Pd was afterwards separated from Ru and Tc by eluting it from the resin with 5% ammonia solution. This procedure made it possible to accurately measure production cross sections for 103m Rh and 103 Pd. Cross sections for the production of various other observed residues are also presented. The results are consistent with an enhanced isobaric yield in the near-target mass region. The radiochemical separation technique is also suitable for the routine production of Pd and Rh nuclides, e.g., 103 Pd and 101m Rh, in proton-induced reactions on Rh targets. (author)

Characterization of highly (110)- and (111)-oriented Pb(Zr,Ti)O3 films on BaPbO3 electrode using Ru conducting barrier

International Nuclear Information System (INIS)

Liang, C.-S.; Wu, J.-M.

2005-01-01

Highly non-(001)-oriented Pb(Zr,Ti)O 3 (PZT) films have been fabricated by rf-magnetron sputtering. The preferential (110)-oriented BaPbO 3 (BPO) deposited on Ru buffer layer induces the growth of (110)-oriented PZT film. With the aid of self-organized growth of PZT, the orientation of the film deposited on random-oriented BPO/Pt(111)/Ru(002) is (111)-preferred. The insertion of Pt layer between BPO and Ru changes the orientation of PZT from (110) to (111) and prevents the oxygen diffusion. These non-(001)-oriented PZT films possess more superior ferroelectric, fatigue, and retention properties than those of (001)-oriented PZT films

A novel binary Pt{sub 3}Te{sub x}/C nanocatalyst for ethanol electro-oxidation

Energy Technology Data Exchange (ETDEWEB)

Huang, Meihua; Wang, Fei; Li, Lirong; Guo, Yonglang [College of Chemistry and Chemical Engineering, Fuzhou University, Fuzhou 350002 (China)

2008-03-15

The Pt{sub 3}Te{sub x}/C nanocatalyst was prepared and its catalytic performance for ethanol oxidation was investigated for the first time. The Pt{sub 3}Te/C nanoparticles were characterized by an X-ray diffractometer (XRD), transmission electron microscope (TEM) and energy dispersive X-ray spectroscopy equipped with TEM (TEM-EDX). The Pt{sub 3}Te/C catalyst has a typical fcc structure of platinum alloys with the presence of Te. Its particle size is about 2.8 nm. Among the synthesized catalysts with different atomic ratios, the Pt{sub 3}Te/C catalyst has the highest anodic peak current density. The cyclic voltammograms (CV) show that the anodic peak current density for the Pt{sub 3}Te/C, commercial PtRu/C and Pt/C catalysts reaches 1002, 832 and 533 A g{sup -1}, respectively. On the current-time curve, the anodic current on the Pt{sub 3}Te/C catalyst was higher than those for the catalysts reported. So, these findings show that the Pt{sub 3}Te/C catalyst has uniform nanoparticles and the best activity among the synthesized catalysts, and it is better than commercial PtRu/C and Pt/C catalysts for ethanol oxidation at room temperature. (author)

Characterization of RuO sub 2 electrodes for ferroelectric thin films prepared by metal-organic chemical-vapor deposition using Ru(C sub 1 sub 1 H sub 1 sub 9 O sub 2) sub 3

CERN Document Server

Lee, J M; Shin, J C; Hwang, C S; Kim, H J; Suk, C G

1999-01-01

Pure and conducting RuO sub 2 thin films were deposited on Si substrates at 250 approx 450 .deg. C using Ru(C sub 1 sub 1 H sub 1 sub 9 O sub 2) sub 3 as a precursor by low-pressure metal-organic chemical-vapor deposition (LP-MOCVD). At a lower deposition temperature,smoother and denser RuO sub 2 thin films were deposited. The RuO sub 2 thin films, which were crack free, adhered well onto the substrates and showed very low resistivities around 45 approx 60 mu OMEGA cm. RuO sub 2 thin films on (Ba, Sr)/TiO sub 3 /Pt/SiO sub 2 /Si showed good properties, indicating that MOCVD RuO sub 2 thin films from Ru(C sub 1 sub 1 H sub 1 sub 9 O sub 2) sub 3 can be applied as electrodes of high-dielectric thin films for capacitors in ultra-large-scale DRAMs.

Study of reactivities of electro-catalytic oxidation of organic substrates with Ru(IV) complex

International Nuclear Information System (INIS)

Madurro, J.M.; Oliveira, S.M. de; Campos, J.L.

1988-01-01

An electrocatalytic procedure for the oxidation of olefines, ketones, heterocycles and ethers using the Ru IV oxidant RuO (bpy) (trpy) 2+ (bpy is 2,2 - bipyridine; trpy is 2,2', 2''' - terpyridine), is described. The relative reactivities of the substrates are determined by analysis of the exponential i x t curves, using simple linear and exponential least-square programme. Mechanistics considerations based on the observed relative reactivities are discussed. (M.J.C.) [pt

Concentrations of Platinum Group Elements (Pt, Pd, Rh) in Airborne Particulate Matter (PM2.5 and PM10-2.5) Collected at Selected Canadian Urban Sites: a Case Study

OpenAIRE

Celo V.; Zhao J. J.; Dabek-Zlotorzynska E.

2013-01-01

Increasing environmental concentrations of platinum group elements (PGEs), in particular platinum (Pt), palladium (Pd) and rhodium (Rh), from catalytic converters has been reported worldwide. Initially it was believed that the emitted PGEs remain in the roadside environment, but recent studies have shown that fine PGE-containing particles can be transported and distributed at regional and long-range levels. Therefore, the monitoring of PGEs in airborne particulate matter (PM) is important for...

RuO4-mediated oxidation of secondary amines 2. imines as main reaction intermediates

Directory of Open Access Journals (Sweden)

Florea Cristina A.

2017-01-01

Full Text Available Oxidation by RuO4 (generated in situ from RuO2 and NaIO4 of secondary amines such as Bn–NH–CH2R (1; R=H, Me gave complex reaction mixtures, but mainly amides. In the presence of cyanide, the leading products were α-aminonitriles. Comparison of the oxidation products of 1 with those from the corresponding imines PhCH=N–CH2R and Bn–N=CH–R showed that formation of the indicated imines is the first main step in the oxidation of 1. A detailed mechanism is proposed.

Preparação e caracterização de eletrocatalisadores PtRu/C e PtSn/C via redução química por ácido cítrico para oxidação direta de alcoóis em células a combustível tipo PEM

OpenAIRE

Roberto Willyan Ramon Verjulio-Silva

2008-01-01

Neste trabalho, os sistemas de eletrocatalisadores platina-rutênio (PtRu/C) e platina-estanho (PtSn/C) suportados em carbono de alta área superficial XC72R (Cabot) foram preparados pela redução química de precursores metálicos em solução usando o ácido cítrico como agente redutor. Os eletrocatalisadores foram preparados em diferentes valores de pH, com o objetivo de obter as condições de sínteses mais otimizadas para cada um dos sistemas preparados. O método otimizado mostrou-se eficiente na ...

Rapid evaluation of the electrooxidation of fuel compounds with a multiple-electrode setup for direct polymer electrolyte fuel cells

Energy Technology Data Exchange (ETDEWEB)

Fujiwara, Naoko; Siroma, Zyun; Ioroi, Tsutomu; Yasuda, Kazuaki [Research Institute for Ubiquitous Energy Devices, National Institute of Advanced Industrial Science and Technology (AIST), 1-8-31 Midorigaoka, Ikeda, Osaka 563-8577 (Japan)

2007-02-10

Electrochemical oxidation of fuel compounds in acidic media was examined on eight electrodes (Pt, Ru, PtRu, Rh, Ir, Pd, Au, and glassy carbon) simultaneously by multiple cyclic voltammetry (CV) with an electrochemical cell equipped with an eight-electrode configuration. Direct-type polymer electrolyte fuel cells (PEFCs), in which aqueous solutions of the fuel compounds are directly supplied to the anode, were also evaluated. The performances of direct PEFCs with various anode catalysts could be roughly estimated from the results obtained with multiple CV. This multiple evaluation may be useful for identifying novel fuels or electrocatalysts. Methanol, ethanol, ethylene glycol, 2-propanol, and D-glucose were oxidized selectively on Pt or PtRu, as reported previously. However, several compounds that are often used as reducing agents show electrochemical oxidation with unique characteristics. Large current was obtained for the oxidation of formic acid, hypophosphorous acid, and phosphorous acid on a Pd electrode. L-Ascorbic acid and sulfurous acid were oxidized on all of the electrodes used in the present study. (author)

Strong Metal Support Interaction of Pt and Ru Nanoparticles Deposited on HOPG Probed by the H-D Exchange Reaction

DEFF Research Database (Denmark)

Fiordaliso, Elisabetta M.; Dahl, Søren; Chorkendorff, Ib

2012-01-01

The interaction between metals and support is investigated in the case of 50 Å Pt and 50 Å Ru films deposited on a HOPG substrate. The films are prepared by electron beam physical vapor deposition and annealed in UHV to temperatures up to 700 °C. The equilibrium hydrogen exchange rate between...... adsorbed and gas phase at 1 bar is measured before and after annealing. The rate is measured in the temperature range of 40–200 °C at 1 bar, by utilization of the H-D exchange reaction. Experiments are performed on fresh cleaved and sputtered HOPG, which give similar results. We find that annealing...... the films from 150 up to 700 °C increases the amount of carbon present in the films up to 95%, as derived by surface analysis, indicating the formation of a carbon layer on top of the metal films. The exchange rate decreases dramatically with increasing carbon content on the films for both metals, pointing...

Platinum-Group Elements in Soils and Street Dust of the Southeastern Administrative District of Moscow

Science.gov (United States)

Ladonin, D. V.

2018-03-01

The contents of five platinum-group metals (Ru, Rh, Pd, Ir, and Pt) in soils and street dust of the Southeastern administrative district (SEAD) of Moscow have been determined. The contents of these elements in soils may considerably exceed their natural abundances in the lithosphere and are characterized by considerable variability and asymmetric frequency distribution. A close correlation between Rh, Pd, and Pt contents in soils and street dust has been shown. The data on the contents of the elements and the ratios between them suggest that motor vehicles are the major source of pollution of soils and street dust in the studied district.

Fabrication of ultra-thin cerium oxide layers on Ru(0001) single crystal surfaces. Scanning tunneling microscopic and photoelectron spectroscopic studies on growth, structure and properties; Herstellung ultraduenner Ceroxidschichten auf Ru(0001)-Einkristallflaechen. Rastertunnelmikroskopische und photoelektronenspektroskopische Untersuchungen zu Wachstum, Struktur und Eigenschaften

Energy Technology Data Exchange (ETDEWEB)

Bouchtaoui, Mustapha

2016-12-07

The thesis at hand aims at a study of structure and properties of well-defined ultrathin CeO{sub 2} films supported on Ru(0001). Such systems may serve as model systems in heterogenous catalysis. The epitaxial growth of ceria films on Ru(0001) surface has been achieved by electron beam evaporation of metal Cer at low background oxygen pressure of 10{sup -6} mbar under ultrahigh-vacuum conditions at room temperature. Cerium oxide qualifies for proper oxygen-storage in oxidation reactions, and hence it widely used in heterogenous catalysis. The oxidation begins with the adsorption of CO on the CeO{sub 2}(111) surface, and it ends with participation of lattice oxygen leading to vacancy formation and CO{sub 2} desorption. We investigate the geometric structure by means of scanning tunneling microscopy and low energy electron diffraction. The coverage of 2.5 monolayers (ML) was sufficient to cover the substrate almost completely. We further analysed the interaction of CO with the CeO{sub 2}/Ru(0001) and the Pt/CeO{sub 2}/Ru(0001) systems. During the interaction process the ratio of Ce{sup 4+} and Ce{sup 3+} changes significantly. This ratio change as well as the effect of Pt evaporated onto the surface with respect to the reducibility of CeO{sub 2}/Ru(0001) in CO environment has been studied by X-ray photoemission spectroscopy and it has been confirmed with thermal desorption spectroscopy. It is revealed that the Pt-Nanoparticles with a height from 7.15 Aa to 9.73 Aa clearly enhances the reducibility of CeO{sub 2}.

Quasi-two-dimensional Fermi-liquid state in Sr2RhO4-δ

International Nuclear Information System (INIS)

Nagai, Ichiro; Shirakawa, Naoki; Umeyama, Norio; Ikeda, Shin-ichi

2010-01-01

Single crystals of layered perovskite Sr 2 RhO 4-δ (δ=0.0 and 0.1) are successfully grown by the floating-zone method. Stoichiometric single crystals (Sr 2 RhO 4.0 ) are obtained by O 2 -annealing the as-grown crystals (Sr 2 RhO 3.9 ). Sr 2 RhO 4.0 and Sr 2 RhO 3.9 show quasi-two-dimensional Fermi-liquid behavior at low temperatures, whereas there are large differences in the anisotropy of electrical resistivity ρ c (3 K)/ρ ab (3 K) and Wilson ratio R w between Sr 2 RhO 4.0 and Sr 2 RhO 3.9 : ρ c (3 K)/ρ ab (3 K)=2400 (19000) and R w =3.8 (6.4) for Sr 2 RhO 4.0 (Sr 2 RhO 3.9 ). The differences observed between the temperature dependence of the in-plane electrical resistivity (T 2 RhO 4.0 and Sr 2 RhO 3.9 are mainly derived from those between the density of states and band structure near the corresponding Fermi level. This indicates that the changes in these physical properties, which are accompanied by oxygen defects in the Sr 2 RhO 4-δ system, can be explained by the rigid band model. Moreover, these results suggest that t 2g band-filling can be controlled by adjusting the oxygen defect content δ in the Sr 2 RhO 4-δ system. Although many similarities are observed in this study between the physical properties of Sr 2 RhO 4.0 and Sr 2 RuO 4 . Sr 2 RhO 4.0 does not exhibit superconductivity down to 36 mK. (author)

Hydrothermal synthesis of highly crystalline RuS{sub 2} nanoparticles as cathodic catalysts in the methanol fuel cell and hydrochloric acid electrolysis

Energy Technology Data Exchange (ETDEWEB)

Li, Yanjuan [Key Laboratory of Marine Chemistry Theory and Technology, Minisry of Education Ocean University of China, Qingdao, 266100 (China); College of Material Science and Engineering, Key Laboratory of Automobile Materials of Ministry of Education, Jilin University, 2699 Qianjin Street, Changchun 130012 (China); Li, Nan, E-mail: lin@jlu.edu.cn [College of Material Science and Engineering, Key Laboratory of Automobile Materials of Ministry of Education, Jilin University, 2699 Qianjin Street, Changchun 130012 (China); Yanagisawa, Kazumichi [Research Laboratory of Hydrothermal Chemistry, Kochi University, Kochi 780-8520 (Japan); Li, Xiaotian [College of Material Science and Engineering, Key Laboratory of Automobile Materials of Ministry of Education, Jilin University, 2699 Qianjin Street, Changchun 130012 (China); Yan, Xiao [Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), College of Physics, Jilin University, Changchun 130012 (China)

2015-05-15

Highlights: • Highly crystalline RuS{sub 2} nanoparticles have been first synthesized by a “one-step” hydrothermal method. • The product presents a pure cubic phase of stoichiometric ratio RuS{sub 2} with average particle size of 14.8 nm. • RuS{sub 2} nanoparticles were used as cathodic catalysts in methanol fuel cell and hydrochloric acid electrolysis. • The catalyst outperforms commercial Pt/C in methanol tolerance and stability towards Cl{sup −}. - Abstract: Highly crystalline ruthenium sulfide (RuS{sub 2}) nanoparticles have been first synthesized by a “one-step” hydrothermal method at 400 °C, using ruthenium chloride and thiourea as reactants. The products were characterized by powder X-ray diffraction (XRD), scanning electron microscopy/energy disperse spectroscopy (SEM/EDS), thermo gravimetric-differential thermal analyze (TG-DTA), transmission electron microscopy equipped with selected area electron diffraction (TEM/SAED). Fourier transform infrared spectra (IR), and X-ray photoelectron spectroscopy (XPS). XRD result illustrates that the highly crystalline product presents a pure cubic phase of stoichiometric ratio RuS{sub 2} and the average particle size is 14.8 nm. SEM and TEM images display the products have irregular shape of 6–25 nm. XPS analyst indicates that the sulfur exists in the form of S{sub 2}{sup 2−}. Cyclic voltammetry (CV), rotating disk electrode (RDE), chronoamperometry (CA) and electrochemical impedance spectroscopy (EIS) measurements are conducted to evaluate the electrocatalytic activity and stability of the highly crystalline RuS{sub 2} nanoparticles in oxygen reduction reaction (ORR) for methanol fuel cell and hydrochloric acid electrolysis. The results illustrate that RuS{sub 2} is active towards oxygen reduction reaction. Although the activity of RuS{sub 2} is lower than that of Pt/C, the RuS{sub 2} catalyst outperforms commercial Pt/C in methanol tolerance and stability towards Cl{sup −}.

Structure and composition of single Pt–Ru electrocatalyst nanoparticles supported on multiwall carbon nanotubes

International Nuclear Information System (INIS)

Paraguay-Delgado, Francisco; Malac, Marek; Alonso-Nuñez, Gabriel

2014-01-01

Individual Pt-Ru nanoparticles (NPs) supported on multiwall carbon nanotubes (MWCNTs) synthesized by microemulsion method were characterized by nano beam diffraction (NBD) and high resolution imaging in transmission electron microscopy (TEM). Comparing the TEM images and NBD to simulations provided insight into particle composition, structure and morphology in three dimensions. In particular, the NBD allowed us to detect various components of the individual NPs that would be difficult to observe otherwise. We find that the NPs contain four different components: Pt–RuO 2 , Pt–Ru, RuO 2 and metallic Pt. Often an individual NP is composed of more than one component. The most frequently encountered external morphology is close to a spherical shape and ∼3.7 nm in diameter. The collective properties of NPs’ assemblies were studied by thermogravimetry, differential thermal analysis and x-ray diffraction. The results allowed us to gain some insight into the relation of the NPs’ structure and composition with their catalytic performance, and revealed the presence of components not detectable by bulk methods. The electrocatalytic properties were evaluated by CO stripping, methanol oxidation and oxygen reduction. Bulk characterization methods miss many properties and structures present in the sample due to low volume fraction and due to overlap of reflections. Single NPs should be analyzed to obtain reliable indication of sample composition. (paper)

Surface enrichment of Pt in stable Pt-Ir nano-alloy particles on MgAl 2 O 4 spinel in oxidizing atmosphere

Energy Technology Data Exchange (ETDEWEB)

Li, Weizhen; Nie, Lei; Chen, Ying; Kovarik, Libor; Liu, Jun; Wang, Yong

2017-04-01

With the capability of MgAl2O4 spinel {111} nano-facets in stabilizing small Rh, Ir and Pt particles, bimetallic Ir-Pt catalysts on the same support were investigated, aiming at further lowering the catalyst cost by substituting expensive Pt with cheaper Ir in the bulk. Small Pt-Ir nano-alloy particles (< 2nm) were successfully stabilized on the spinel {111} nano-facets as expected. Interestingly, methanol oxidative dehydrogenation (ODH) rate on the surface Pt atoms increases with oxidizing aging but decreases upon reducing treatment, where Ir is almost inactive under the same reaction conditions. Up to three times enhancement in Pt exposure was achieved when the sample was oxidized at 800 °C in air for 1 week and subsequently reduced by H2 for 2 h, demonstrating successful surface enrichment of Pt on Pt-Ir nano-alloy particles. A dynamic stabilization mechanism involving wetting\

Study on oxidization of Ru and its application as electrode of PZT capacitor for FeRAM

International Nuclear Information System (INIS)

Jia Ze; Ren Tianling; Liu Tianzhi; Hu Hong; Zhang Zhigang; Xie Dan; Liu Litian

2007-01-01

Oxidization for Ru through anneal with plenteous oxygen atmosphere and its application as the top electrode of sol-gel PZT capacitor are investigated in this study. PZT capacitor with RuO 2 or oxygen-doped Ru as top electrode can be obtained from Ru/PZT/Pt capacitor through slow-rate anneal at 650 deg. C for 20 min in cannulation furnace. It has larger remanent polarization, better rectangle shape, better fatigue properties and lower leakage current than the other capacitors with PZT film prepared by the same process and different top electrodes in this study. Plenteous oxygen atmosphere and 650 deg. C in cannulation furnace are important conditions for the oxidation of Ru and renewed crystallization of PZT in this capacitor. Plenteous oxygen at interface can compensate the oxygen vacancies at PZT/electrode interface, which results in the above good characteristics

Infrared and swelling study of wet-spun films of DNA\\cdot[(bipy)Pt(en)]^2+ as a function of hydration

Science.gov (United States)

Kuebler, A.; Whitson, K. B.; Marlowe, R. L.; Lee, S. A.; Rupprecht, A.

1997-11-01

A ladder-like conformation of DNA has been induced by the binding of bipyridyl-Pt(II)-ethylenediamine (denoted as [(bipy)Pt(en)]^2+) at a relative humidity (RH) of 75%.(Arnott et al.,) Nature 287, (1980) 561. We report the first study of oriented films of this complex as a function of hydration by using Fourier transform infrared (IR) spectroscopy and optical microscopy. Vibrational modes between 800 and 1000 cm-1 are localized in the phosphodiester backbone and are sensitive to changes in the geometry of the molecule. The IR spectrum of this region is substantially different at 59% RH than at higher humidities, implying that a conformational change occurs as the RH is lowered below 75%. Optical microscopy measurements of small pieces of films of the complex also show changes at low RH. These trends are consistent with an order-disorder transition occurring as the RH is lowered The measurements also show that the DNA\\cdot[(bipy)Pt(en)]^2+) are very stable at the highest humidities.

High-Performance Rh ₂ P Electrocatalyst for Efficient Water Splitting

Energy Technology Data Exchange (ETDEWEB)

Duan, Haohong [Department; Chemistry; Li, Dongguo [Materials; Tang, Yan [Department; amp, Molecular; He, Yang [Department; Ji, Shufang [Department; Wang, Rongyue [Materials; Lv, Haifeng [Materials; Lopes, Pietro P. [Materials; Paulikas, Arvydas P. [Materials; Li, Haoyi [Department; amp, Molecular; Mao, Scott X. [Department; Wang, Chongmin [Environmental; Markovic, Nenad M. [Materials; Li, Jun [Department; amp, Molecular; Stamenkovic, Vojislav R. [Materials; Li, Yadong [Department

2017-04-05

The search for active, stable, and cost-efficient electrocatalysts for hydrogen production via water splitting could make a substantial impact on energy technologies that do not rely on fossil fuels. Here we report the synthesis of rhodium phosphide electrocatalyst with low metal loading in the form of nanocubes (NCs) dispersed in high-surface-area carbon (Rh2P/C) by a facile solvo-thermal approach. The Rh2P/C NCs exhibit remarkable performance for hydrogen evolution reaction and oxygen evolution reaction compared to Rh/C and Pt/C catalysts. The atomic structure of the Rh2P NCs was directly observed by annular dark-field scanning transmission electron microscopy, which revealed a phosphorus-rich outermost atomic layer. Combined experimental and computational studies suggest that surface phosphorus plays a crucial role in determining the robust catalyst properties.

One-Pot and Facile Fabrication of Hierarchical Branched Pt-Cu Nanoparticles as Excellent Electrocatalysts for Direct Methanol Fuel Cells.

Science.gov (United States)

Cao, Yanqin; Yang, Yong; Shan, Yufeng; Huang, Zhengren

2016-03-09

Hierarchical branched nanoparticles are one promising nanostructure with three-dimensional open porous structure composed of integrated branches for superior catalysis. We have successfully synthesized Pt-Cu hierarchical branched nanoparticles (HBNDs) with small size of about 30 nm and composed of integrated ultrathin branches by using a modified polyol process with introduction of poly(vinylpyrrolidone) and HCl. This strategy is expected to be a general strategy to prepare various metallic nanostructures for catalysis. Because of the special open porous structure, the as-prepared Pt-Cu HBNDs exhibit greatly enhanced specific activity toward the methanol oxidation reaction as much as 2.5 and 1.7 times compared with that of the commercial Pt-Ru and Pt-Ru/C catalysts, respectively. Therefore, they are potentially applicable as electrocatalysts for direct methanol fuel cells.

Spectroscopy of 96-98Ru and neighboring nuclei: shell model calculations and lifetime measurements

International Nuclear Information System (INIS)

Kharraja, B.; Garg, U.; Ghugre, S.S.

1997-01-01

High Spin states in 94,95 Mo, 94-96 Tc, 96-98 Ru and 97,98 Rh were populated via the 65 Cu( 36 S,xpyn) reactions at 142 MeV. Level schemes of these nuclei have been extended up to a spin of J ∼ 20ℎ and an excitation energy of E x ∼12 -14 MeV. Information on the high spin structure for 96 Tc and 98 Rh has been obtained for the first time. Spherical shell model calculations have been performed and compared with the experimental excitation energies. The level structures of the N=51, 52 isotones exhibit single-particle nature even at the highest spins and excitation energies. A fragmentation of intensity into several branches after breaking of the N = 50 core has been observed. There are indications for the onset of collectivity around neutron number N = 53 in this mass region. A sequence of E2 transitions, reminiscent of vibrational degree of freedom, were observed in 98 Ru at spins just above the observed N = 50 core breaking. RDM lifetime measurements have been performed to ascertain the intrinsic structures of these level sequences. (author)

Adsorption of Rh(III) complexes from chloride solutions obtained by leaching chlorinated spent automotive catalysts on ion-exchange resin Diaion WA21J

International Nuclear Information System (INIS)

Shen Shaobo; Pan Tonglin; Liu Xinqiang; Yuan Lei; Wang Jinchao; Zhang Yongjian; Guo Zhanchen

2010-01-01

It was found that Rh, Pd and Pt contained in the spent ceramic automotive catalysts could be effectively extracted by dry chlorination with chlorine. In order to concentrate Rh(III) ions contained in the chloride solutions obtained, thermodynamic and kinetics studies for adsorption of Rh(III) complexes from the chloride solutions on an anionic exchange resin Diaion WA21J were carried out. Rh, Pd, Pt, Al, Fe, Si, Zn and Pb from the chloride solution could be adsorbed on the resin. The distribution coefficients (K d ) of Rh(III) decreased with the increase in initial Rh(III) concentration or in adsorption temperature. The isothermal adsorption of Rh(III) was found to fit Langmuir, Freundlich and Dubinin-Kaganer-Radushkevich models under the adsorption conditions. The maximum monolayer adsorption capacities Q max based on Langmuir adsorption isotherms were 6.39, 6.61 and 5.81 mg/g for temperatures 18, 28 and 40 deg. C, respectively. The apparent adsorption energy of Rh was about -7.6 kJ/mol and thus Rh(III) adsorption was a physical type. The experimental data obtained could be better simulated by pseudo-first-order kinetic model and the activation energy obtained was 6.54 J/mol. The adsorption rate of Rh(III) was controlled by intraparticle diffusion in most of time of adsorption process.

Indides RE{sub 3}T{sub 2}In{sub 4} (RE = Y, Gd-Tm, Lu; T = Ni, Ru, Rh) with a ZrNiAl superstructure

Energy Technology Data Exchange (ETDEWEB)

Heying, Birgit; Niehaus, Oliver; Rodewald, Ute C.; Poettgen, Rainer [Univ. Muenster (Germany). Inst. fuer Anorganische und Analytische Chemie

2016-07-01

Three series of rare earth-transition metal-indides RE{sub 3}T{sub 2}In{sub 4} (RE=Y, Gd-Tm, Lu; T=Ni, Ru, Rh) were synthesized from arc-melted RE{sub 3}T{sub 2} precursor compounds and indium tear shot in sealed niobium ampoules using different annealing sequences. The new indides crystallize with the hexagonal Lu{sub 3}Co{sub 2}In{sub 4}-type structure, space group P anti 6. All samples were characterized on the basis of Guinier powder patterns and six structures were refined from single crystal X-ray diffractometer data. The RE{sub 3}T{sub 2}In{sub 4} structures are derived from the ZrNiAl type through RE/In ordering, paralleled by a symmetry reduction from P anti 62m to P anti 6. This induces twinning for some of the investigated crystals. The main crystal chemical motifs of the RE{sub 3}T{sub 2}In{sub 4} structures are trigonal prisms of rare earth, respectively indium atoms that are filled by the transition metals.

Creation of Novel Solid-Solution Alloy Nanoparticles on the Basis of Density-of-States Engineering by Interelement Fusion.

Science.gov (United States)

Kobayashi, Hirokazu; Kusada, Kohei; Kitagawa, Hiroshi

2015-06-16

Currently 118 known elements are represented in the periodic table. Of these 118 elements, only about 80 elements are stable, nonradioactive, and widely available for our society. From the viewpoint of the "elements strategy", we need to make full use of the 80 elements to bring out their latent ability and create innovative materials. Furthermore, there is a strong demand that the use of rare or toxic elements be reduced or replaced while their important properties are retained. Advanced science and technology could create higher-performance materials even while replacing or reducing minor or harmful elements through the combination of more abundant elements. The properties of elements are correlated directly with their electronic states. In a solid, the magnitude of the density of states (DOS) at the Fermi level affects the physical and chemical properties. In the present age, more attention has been paid to improving the properties of materials by means of alloying elements. In particular, the solid-solution-type alloy is advantageous because the properties can be continuously controlled by tuning the compositions and/or combinations of the constituent elements. However, the majority of bulk alloys are of the phase-separated type under ambient conditions, where constituent elements are immiscible with each other. To overcome the challenge of the bulk-phase metallurgical aspects, we have focused on the nanosize effect and developed methods involving "nonequilibrium synthesis" or "a process of hydrogen absorption/desorption". We propose a new concept of "density-of-states engineering" for the design of materials having the most desirable and suitable properties by means of "interelement fusion". In this Account, we describe novel solid-solution alloys of Pd-Pt, Ag-Rh, and Pd-Ru systems in which the constituent elements are immiscible in the bulk state. The homogeneous solid-solution alloys of Pd and Pt were created from Pd core/Pt shell nanoparticles using a

RuO4-mediated oxidation of secondary amines: Part 1. Are hydroxylamines main intermediates?

Directory of Open Access Journals (Sweden)

Florea Cristina A.

2016-01-01

Full Text Available The RuO4-catalyzed oxidation of secondary amines Bn-NH-CH2R (1a-b; R=H, Me gave mainly amides, but minute amounts of nitrones PhCH=N(O-CH2R (9a-b and traces of Bn-N(OH-CH2R (R=H, 4a were also detected. In the presence of cyanide, up to 22 reaction products were identified, but mainly α-aminonitriles. Comparison of the oxidation products of 1a-b with those of 4a-b, 9a-b, and Bn-N(O=CHR (10a-b showed that 4a-b cannot be main reaction intermediates formed from 1a-b.

Preparation and electrocatalytic properties of Pt-SiO2 nanocatalysts for ethanol electrooxidation.

Science.gov (United States)

Liu, B; Chen, J H; Zhong, X X; Cui, K Z; Zhou, H H; Kuang, Y F

2007-03-01

Due to their high stability in general acidic solutions, SiO(2) nanoparticles were selected as the second catalyst for ethanol oxidation in sulfuric acid aqueous solution. Pt-SiO(2) nanocatalysts were prepared in this paper. The micrography and elemental composition of Pt-SiO(2) nanoparticles were characterized by scanning electron microscopy and energy dispersive X-ray spectroscopy, respectively. The electrocatalytic properties of Pt-SiO(2) nanocatalysts for ethanol oxidation were investigated by cyclic voltammetry. Under the same Pt loading mass and experimental conditions for ethanol oxidation, Pt-SiO(2) nanocatalysts show higher activity than PtRu/C (E-Tek), Pt/C (E-Tek), and Pt catalysts. Additionally, Pt-SiO(2) nanocatalysts possess good anti-poisoning ability. The results indicate that Pt-SiO(2) nanocatalysts may have good potential applications in direct ethanol fuel cells.

Growth and maturational changes in dense fibrous connective tissue following 14 days of rhGH supplementation in the dwarf rat

Science.gov (United States)

Kyparos, Antonios; Orth, Michael W.; Vailas, Arthur C.; Martinez, Daniel A.

2002-01-01

The purpose of this study was to investigate the impact of recombinant human growth hormone (rhGH) on patella tendon (PT), medial collateral ligament (MCL), and lateral collateral ligament (LCL) on collagen growth and maturational changes in dwarf GH-deficient rats. Twenty male Lewis mutant dwarf rats, 37 days of age, were randomly assigned to Dwarf + rhGH (n = 10) and Dwarf + vehicle (n = 10) groups. The GH group received 1.25 mg rhGH/kg body wt twice daily for 14 days. rhGH administration stimulated dense fibrous connective tissue growth, as demonstrated by significant increases in hydroxyproline specific activity and significant decreases in the non-reducible hydroxylysylpyridinoline (HP) collagen cross-link contents. The increase in the accumulation of newly accreted collagen was 114, 67, and 117% for PT, MCL, and LCL, respectively, in 72 h. These findings suggest that a short course rhGH treatment can affect the rate of new collagen production. However, the maturation of the tendon and ligament tissues decreased 18-25% during the rapid accumulation of de novo collagen. We conclude that acute rhGH administration in a dwarf rat can up-regulate new collagen accretion in dense fibrous connective tissues, while causing a reduction in collagen maturation. Copyright 2002 Elsevier Science Ltd.

Direct hydrodeoxygenation of cellulose and xylan to lower alkanes on ruthenium catalysts in subcritical water

International Nuclear Information System (INIS)

Osaka, Yuriko; Ikeda, Yoichi; Hashizume, Daisuke; Iwamoto, Masakazu

2013-01-01

Nano particles of Ru, Rh, Pd, Ir, Pt, and Au, protected by polyvinyl pyrrolidone (PVP), were applied to the hydrodeoxygenation of cellulose and xylan in water and 5 MPa H 2 at 543 K. The distributions of products generated from cellulose and xylan were roughly similar to each other under the present reaction conditions, and therefore, the former was intensively studied. The Ru-PVP catalyst afforded mainly methane and lower alkanes, rather than producing water soluble organic compounds, such as diols and alcohols, that were formed with the use of the other catalysts. The changes in the product distributions with reaction temperature and time indicated that the reaction consisted of two consecutive reactions: cellulose or xylan → water soluble compounds → hydrogenolysis. The first transformation was promoted in subcritical water, and the second step was catalyzed by the Ru catalyst. The Ru catalyst that was supported on CeO 2 , γ-Al 2 O 3 , or activated carbon yielded a similar product distribution to that on Ru-PVP; however, the loading of Ru on TiO 2 , ZrO 2 , SiO 2 –Al 2 O 3 , or SiO 2 resulted in the increment of diols. After the reaction a small portion of the CeO 2 and most of the SiO 2 –Al 2 O 3 and SiO 2 were dissolved in water, and a portion of the Al 2 O 3 was transformed to boehmite AlO(OH) from the γ-alumina. Little change in the catalytic activity however was observed upon the reuse of Ru/Al 2 O 3 in the second run. Highlights: •One-path hydrodeoxygenation of cellulose and xylan to methane and lower alkanes was studied. •Ru-PVP catalysts gave the best yields among Ru-, Rh-, Pd-, Ir-, Pt-, and Au-PVP. •The reaction pathways were cellulose → water soluble compounds → hydrogenolysis. •The catalytic activity of Ru was greatly dependent on the supports

Concentrations of Platinum Group Elements (Pt, Pd, Rh in Airborne Particulate Matter (PM2.5 and PM10-2.5 Collected at Selected Canadian Urban Sites: a Case Study

Directory of Open Access Journals (Sweden)

Celo V.

2013-04-01

Full Text Available Increasing environmental concentrations of platinum group elements (PGEs, in particular platinum (Pt, palladium (Pd and rhodium (Rh, from catalytic converters has been reported worldwide. Initially it was believed that the emitted PGEs remain in the roadside environment, but recent studies have shown that fine PGE-containing particles can be transported and distributed at regional and long-range levels. Therefore, the monitoring of PGEs in airborne particulate matter (PM is important for the estimation of potential risks to human health and to the ecosystem. The aim of this study is to present the first results from an analysis on the concentration and distribution of Pt, Pd and Rh in PM collected on Teflon filters at two selected urban sites (Toronto, Ontario; Edmonton, Alberta collected within the Canadian National Air Pollution Surveillance (NAPS network. In this work, a quadruple inductively coupled plasma mass spectrometry (ICP-MS, combined with microwave assisted acid digestion using aqua regia was used. A cation exchange separation was used to alleviate the matrix-induced spectral and nonspectral interferences prior to ICP-MS analysis. To obtain sufficient material needed for PGEs analysis, fine PM (particles with aerodynamic diameter less than 2.5 mm; PM2.5 and coarse PM (with aerodynamic diameter between 2.5 and 10 mm; PM10-2.5 samples were combined into composite samples on a seasonal basis. The obtained results will be discussed and compared with literature data.

Identification of short-lived neutron-rich ruthenium and rhodium isotopes in fission

International Nuclear Information System (INIS)

Franz, G.; Herrmann, G.

1975-01-01

Short-lived ruthenium and rhodium isotopes ( 107 Ru, 108 Ru, 108 Rh, 109 Ru, 109 Rh, 110 Ru, 110 Rh, 111 Ru, 111 Rh, 112 Ru, 112 Rh, 113 Ru) have been separated from fission products by a rapid chemical procedure and identified by means of γ-ray spectroscopy. Nuclides with half-lives down to 3 sec were accessible. Ruthenium isotopes up to mass number 113 have been identified. (author)

Synthesis, crystal structure investigation and magnetism of the complex metal-rich boride series Crx(Rh1-yRuy)7-xB3 (x=0.88-1; y=0-1) with Th7Fe3-type structure

Science.gov (United States)

Misse, Patrick R. N.; Mbarki, Mohammed; Fokwa, Boniface P. T.

2012-08-01

Powder samples and single crystals of the new complex boride series Crx(Rh1-yRuy)7-xB3 (x=0.88-1; y=0-1) have been synthesized by arc-melting the elements under purified argon atmosphere on a water-cooled copper crucible. The products, which have metallic luster, were structurally characterized by single-crystal and powder X-ray diffraction as well as EDX measurements. Within the whole solid solution range the hexagonal Th7Fe3 structure type (space group P63mc, no. 186, Z=2) was identified. Single-crystal structure refinement results indicate the presence of chromium at two sites (6c and 2b) of the available three metal Wyckoff sites, with a pronounced preference for the 6c site. An unexpected Rh/Ru site preference was found in the Ru-rich region only, leading to two different magnetic behaviors in the solid solution: The Rh-rich region shows a temperature-independent (Pauli) paramagnetism whereas an additional temperature-dependent paramagnetic component is found in the Ru-rich region.