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

被引:80
|
作者
Wu, Gang [1 ]
Swaidan, Raja
Cui, Guofeng
机构
[1] Univ S Carolina, Dept Chem Engn, Columbia, SC 29208 USA
[2] Cooper Union Adv Sci & Art, Dept Chem Engn, New York, NY 10003 USA
[3] Sun Yat Sen Univ, Sch Chem & Chem Engn, Guangzhou 510275, Peoples R China
关键词
PtRuSn/C ethanol electrooxidation; acetaldehyde electrooxidation; acetic acid electrooxidation; direct ethanol fuel cell;
D O I
10.1016/j.jpowsour.2007.07.034
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
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 acohol-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 Sri 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-1 and C-2 species from Pt sites is primarily attributed to the Ru and Pt3Sn alloy structures. However, for the overall oxidation of ethanol, the Sn-rich PtRuSn/C catalyst (60:10:30) containing PtSn phase and SnO2 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, 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. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:180 / 188
页数:9
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