Roles of Surface Steps on Pt Nanoparticles in Electro-oxidation of Carbon Monoxide and Methanol

被引:172
作者
Lee, Seung Woo [2 ,5 ]
Chen, Shuo [1 ,5 ]
Sheng, Wenchao [3 ,5 ]
Yabuuchi, Naoaki [1 ,5 ]
Kim, Yong-Tae [1 ,5 ,6 ]
Mitani, Tadaoki [6 ]
Vescovo, Elio [7 ]
Shao-Horn, Yang [1 ,4 ,5 ]
机构
[1] MIT, Dept Mech Engn, Cambridge, MA 02139 USA
[2] MIT, Dept Chem Engn, Cambridge, MA 02139 USA
[3] MIT, Dept Chem, Cambridge, MA 02139 USA
[4] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA
[5] MIT, Electrochem Energy Lab, Cambridge, MA 02139 USA
[6] Japan Adv Inst Sci & Technol, Sch Mat Sci, Kanazawa, Ishikawa 9231292, Japan
[7] Brookhaven Natl Lab, Upton, NY 11973 USA
基金
美国国家科学基金会; 新加坡国家研究基金会;
关键词
CO MONOLAYER OXIDATION; PARTICLE-SIZE; OXYGEN REDUCTION; PLATINUM; CATALYSTS; ELECTROCATALYSIS; ELECTRODES; MECHANISM; SITES; ADSORPTION;
D O I
10.1021/ja9025648
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Design of highly active nanoscale catalysts for electro-oxidation of small organic molecules is of great importance to the development of efficient fuel cells. Increasing steps on single-crystal Pt surfaces is shown to enhance the activity of CO and methanol electro-oxidation up to several orders of magnitude. However, little is known about the surface atomic structure of nanoparticles with sizes of practical relevance, which limits the application of fundamental understanding in the reaction mechanisms established on single-crystal surfaces to the development of active, nanoscale catalysts. In this study, we reveal the surface atomic structure of Pt nanoparticles supported on multiwall carbon nanotubes, from which the amount of high-index surface facets on Pt nanoparticles is quantified. Correlating the surface steps on Pt nanoparticles with the electrochemical activity and stability clearly shows the significant role of surface steps in enhancing. intrinsic activity for CO and methanol electro-oxidation. Here, we show that increasing surface steps on Pt nanoparticles of similar to 2 nm can lead to enhanced intrinsic activity up to similar to 200% (current normalized to Pt surface area) for electro-oxidation of methanol.
引用
收藏
页码:15669 / 15677
页数:9
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