Electrooxidation of Ethanol on Pt. An in Situ and Time-Resolved XANES Study

被引：19
|
作者：
Melke, J. [1 ,2 ]
Schoekel, A. [2 ]
Gerteisen, D. [1 ]
Dixon, D. [2 ]
Ettingshausen, F. [2 ]
Cremers, C. [3 ]
Roth, C. [2 ]
Ramaker, D. E. [4 ]
机构：
[1] Fraunhofer Inst Solar Energy Syst ISE, Freiburg, Germany
[2] Tech Univ Darmstadt, Inst Mat Sci, Darmstadt, Germany
[3] Fraunhofer Inst Chem Technol ICT, Pfinztal, Germany
[4] George Washington Univ, Dept Chem, Washington, DC 20052 USA
来源：
JOURNAL OF PHYSICAL CHEMISTRY C | 2012年 / 116卷 / 04期
关键词：
RAY-ABSORPTION SPECTROSCOPY; SINGLE-CRYSTAL ELECTRODES; FUEL-CELL; ELECTROCHEMICAL OXIDATION; FINE-STRUCTURE; ELEMENTARY STEPS; ACETIC-ACID; PLATINUM; ACETALDEHYDE; METHANOL;
D O I：
10.1021/jp206295h
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：
The ethanol oxidation reaction is studied using X-ray absorption spectroscopy during chronoamperometric cell operation with a carbon-supported Pt catalyst. The analysis of the MANES region of the Pt L-3 edge by the Delta mu-technique allows the coverage of the Pt surface with OH-, n-fold O-, and C-species to be determined. The current voltage characteristics and the coverage is modeled by means of a multistep reaction mechanism based on a modified Butler-Volmer approach that additionally includes adsorbate adsorbate lateral interactions. The model is validated against experimental current and surface coverage data over time. With the model, the importance of acetaldehyde formation via initial C-alpha-H vs O-H bond cleavage is examined, the latter dominating at higher potentials on vacant sites remaining in the oxygen coverage coming from water activation.
引用
收藏
页码：2838 / 2849
页数：12
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