Carbon-Supported, Selenium-Modified Ruthenium-Molybdenum Catalysts for Oxygen Reduction in Acidic Media

被引:24
作者
Guinel, Maxime J. -F. [2 ]
Bonakdarpour, Arman [1 ]
Wang, Biao [1 ,3 ]
Babu, Panakkattu K. [1 ]
Ernst, Frank [2 ]
Ramaswamy, Nagappan [4 ]
Mukerjee, Sanjeev [4 ]
Wieckowski, Andrzej [1 ]
机构
[1] Univ Illinois, Dept Chem, Urbana, IL 61801 USA
[2] Case Western Reserve Univ, Dept Mat Sci & Engn, Cleveland, OH 44106 USA
[3] Donghua Univ, Coll Mat Sci & Engn, Shanghai 200051, Peoples R China
[4] Northeastern Univ, Dept Chem & Chem Biol, Boston, MA 02115 USA
关键词
electrochemistry; nanoparticles; reduction; ruthenium; supported catalysts; METHANOL FUEL-CELLS; RU-SE; NANOPARTICLES; ELECTROCATALYSTS; PROTON; DMFC; PERFORMANCE; STRATEGIES; MEMBRANES;
D O I
10.1002/cssc.200800215
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The stability and oxygen reduction activity of two carbon-supported catalyst materials are reported. The catalysts, Se/Ru and Se/(Ru-Mo), were prepared by using a chemical reduction method. The catalyst nanoparticles were evenly dispersed onto globular amorphous carbon supports and their average size was ca. 2.4 nm. Thermal treatment at 500 degrees C for 2 h in an inert argon atmosphere resulted in coarsening of the nanoparticles, and also in some decrease of their activity. A gradual reduction of activity was also observed for Se/Ru during potential-cycle experiments. However, the incorporation of small amounts of Mo into the Se/Ru catalysts considerably improved the stability of the catalyst against dissolution. The Mo-containing samples showed excellent oxygen reduction activities even after cycling the potential 1000 times between 0.7 and 0.9 V. Furthermore, they showed excellent fuel-cell, behavior. The performance of the Se/Ru catalysts is greatly improved by the addition of small amounts of elemental Mo. Possible mechanisms responsible for the improvement of the activity are discussed.
引用
收藏
页码:658 / 664
页数:7
相关论文
共 32 条
[1]   Carbonyl tailored electrocatalysts [J].
Alonso-Vante, N. .
FUEL CELLS, 2006, 6 (3-4) :182-189
[2]   The structure analysis of the active centers of Ru-containing electrocatalysts for the oxygen reduction. An in situ EXAFS study [J].
Alonso-Vante, N ;
Malakhov, IV ;
Nikitenko, SG ;
Savinova, ER ;
Kochubey, DI .
ELECTROCHIMICA ACTA, 2002, 47 (22-23) :3807-3814
[3]   KINETICS STUDIES OF OXYGEN REDUCTION IN ACID-MEDIUM ON NOVEL SEMICONDUCTING TRANSITION-METAL CHALCOGENIDES [J].
ALONSOVANTE, N ;
TRIBUTSCH, H ;
SOLORZAFERIA, O .
ELECTROCHIMICA ACTA, 1995, 40 (05) :567-576
[4]   Selenium becomes metallic in Ru-Se fuel cell catalysts: An EC-NMR and XPS investigation [J].
Babu, Panakkattu K. ;
Lewera, Adam ;
Chung, Jong Ho ;
Hunger, Ralf ;
Jaegermann, Wolfram ;
Alonso-Vante, Nicolas ;
Wieckowski, Andrzej ;
Oldfield, Eric .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (49) :15140-+
[5]  
Campbell S. A., 2006, US Patent, Patent No. [US 7125820 B2, 7125820]
[6]   Oxygen reduction reaction on ruthenium and rhodium nanoparticles modified with selenium and sulfur [J].
Cao, DX ;
Wieckowski, A ;
Inukai, J ;
Alonso-Vante, N .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2006, 153 (05) :A869-A874
[7]   Aqueous-based synthesis of ruthenium-selenium catalyst for oxygen reduction reaction [J].
Delacote, Cyril ;
Bonakdarpour, Arman ;
Johnston, Christina M. ;
Zelenay, Piotr ;
Wieckowski, Andrzej .
FARADAY DISCUSSIONS, 2008, 140 :269-281
[8]   International activities in DMFC R&D:: status of technologies and potential applications [J].
Dillon, R ;
Srinivasan, S ;
Aricò, AS ;
Antonucci, V .
JOURNAL OF POWER SOURCES, 2004, 127 (1-2) :112-126
[9]   Effect of methanol crossover on the cathode behavior of a DMFC: A half-cell investigation [J].
Du, C. Y. ;
Zhao, T. S. ;
Yang, W. W. .
ELECTROCHIMICA ACTA, 2007, 52 (16) :5266-5271
[10]   Surface modified ruthenium nanoparticles: Structural investigation and surface analysis of a novel catalyst for oxygen reduction [J].
Fiechter, Sebastian ;
Dorbandt, Iris ;
Bogdanoff, Peter ;
Zehl, Gerald ;
Schulenburg, Hendrik ;
Tributsch, Helmut ;
Bron, Michael ;
Radnik, Joerg ;
Fieber-Erdmann, Martin .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (01) :477-487