Diffusion on a nanoparticle surface as revealed by electrochemical NMR

被引:12
作者
Tong, YY
Oldfield, E
Wieckowski, A
机构
[1] Georgetown Univ, Dept Chem, Washington, DC 20057 USA
[2] Univ Illinois, Dept Chem, Urbana, IL 61801 USA
来源
FARADAY DISCUSSIONS | 2002年 / 121卷
关键词
D O I
10.1039/b110800j
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
Surface diffusion of chemisorbed CO (from MeOH electrochemisorption) on pure and Ru-modified nanoscale Pt electrocatalyst surfaces has been investigated by solid-state electrochemical NMR (EC-NMR) in the presence of supporting electrolyte. Temperature-dependent nuclear spin-spin and spin-lattice relaxation measurements enable the diffusion activation energy, E, to be deduced. It is shown that the activation energy E correlates with the steady state current for MeOH electro-oxidation. A simple two-dimensional collision theory model is proposed to explain this intriguing observation, which may provide new mechanistic insights into the promotion of CO-tolerance in Pt/Ru fuel cell catalysts.
引用
收藏
页码:323 / 330
页数:8
相关论文
共 18 条
[1]   AN NMR-STUDY OF THE GEOMETRY OF A CO LAYER CHEMISORBED ON PT PARTICLES [J].
ANSERMET, JP ;
SLICHTER, CP ;
SINFELT, JH .
JOURNAL OF CHEMICAL PHYSICS, 1988, 88 (09) :5963-5971
[2]   NMR-STUDY OF DIFFUSION OF CO ON ALUMINA-SUPPORTED PT CLUSTERS [J].
BECERRA, LR ;
KLUG, CA ;
SLICHTER, CP ;
SINFELT, JH .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (46) :12014-12019
[3]   PEM fuel cells for transportation and stationary power generation applications [J].
Cleghorn, SJC ;
Ren, X ;
Springer, TE ;
Wilson, MS ;
Zawodzinski, C ;
Zawodzinski, TA ;
Gottesfeld, S .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1997, 22 (12) :1137-1144
[4]   Nuclear magnetic resonance spectroscopic study of the electrochemical oxidation product of methanol on platinum black [J].
Day, JB ;
Vuissoz, PA ;
Oldfield, E ;
Wieckowski, A ;
Ansermet, JP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (51) :13046-13050
[5]  
Engel T., 1979, ADV CATALYSIS VOLUME, V28, P1, DOI DOI 10.1016/S0360-0564(08)60133-9
[6]  
Fukushima E, 1981, Experimental Pulse NMR: A Nuts and Bolts Approach, P125
[7]   METHANOL ELECTROOXIDATION ON WELL-CHARACTERIZED PT-RN ALLOYS [J].
GASTEIGER, HA ;
MARKOVIC, N ;
ROSS, PN ;
CAIRNS, EJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (46) :12020-12029
[8]   TEMPERATURE-DEPENDENT METHANOL ELECTROOXIDATION ON WELL-CHARACTERIZED PT-RU ALLOYS [J].
GASTEIGER, HA ;
MARKOVIC, N ;
ROSS, PN ;
CAIRNS, EJ .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1994, 141 (07) :1795-1803
[9]  
Houston PL., 2001, Chemical Kinetics and Reaction Dynamics
[10]   Lattice gas model for CO electrooxidation on Pt-Ru bimetallic surfaces [J].
Koper, MTM ;
Lukkien, JJ ;
Jansen, APJ ;
van Santen, RA .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (26) :5522-5529