Ruthenium-Alloy Electrocatalysts with Tunable Hydrogen Oxidation Kinetics in Alkaline Electrolyte

被引：101
|
作者：
St John, Samuel [1 ]
Atkinson, Robert W., III [1 ]
Unocic, Raymond R. [2 ]
Zawodzinski, Thomas A., Jr. [1 ,3 ]
Papandrew, Alexander B. [1 ]
机构：
[1] Univ Tennessee, Chem & Biomol Engn, Knoxville, TN 37996 USA
[2] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA
[3] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA
来源：
JOURNAL OF PHYSICAL CHEMISTRY C | 2015年 / 119卷 / 24期
关键词：
ACID FUEL-CELLS; OXYGEN REDUCTION; EVOLUTION REACTIONS; PT-RU; PLATINUM; NANOPARTICLES; SURFACES; CO; ELECTROOXIDATION; CATALYSTS;
D O I：
10.1021/acs.jpcc.5b03284
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
High-surface-area ruthenium-based RuxMy (M = Pt or Pd) alloy catalysts supported on carbon black were synthesized to investigate the hydrogen oxidation reaction (HOR) in alkaline electrolytes. The exchange current density for hydrogen oxidation on a Pt-rich Ru0.20Pt0.80 catalyst is 1.42 mA/cm(2), nearly 3 times that of Pt (0.490 mA/cm(2)). Furthermore, RuxPty alloy surfaces in 0.1 M KOH yield a Tafel slope of similar to 30 mV/dec, in contrast with the similar to 125 mV/dec Tafel slope observed for supported Pt, signifying that hydrogen dissociative adsorption is rate-limiting rather than charge-transfer processes. Ru alloying with Pd does not result in modified kinetics. We attribute these disparate results to the interplay of bifunctional and ligand effects. The dependence of the rate-determining step on the choice of alloy element allows for tuning catalyst activity and suggests not only that a low-cost, alkaline anode catalyst is possible but also that it is tantalizingly close to reality.
引用
收藏
页码：13481 / 13487
页数：7
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