期刊
ACS CATALYSIS
卷 9, 期 1, 页码 442-455出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b04447
关键词
Pt-based alloy catalysts; high-indexed facets; Mo decoration; electronic effect; ethylene glycol oxidation
资金
- NSFC [21572688, 21173269, 21590792, 21573286, U1662104, 91645203]
- Science Foundation of China University of Petroleum, Beijing [2462015YQ0304]
- Specialized Research Fund for the Doctoral Program of Higher Education [20130007110003]
- Ministry of Science and Technology of China [2011BAK15B05]
- State Key Laboratory of Physical Chemistry of Solid Surfaces
The instable structure of Pt-based high-indexed facets (HIFs) facile reconstructed is a key obstacle for further practical applications because of its high surface energy and amounts of undercoordinated surface atoms. Herein, a strategy to advance the fundamental surface study on Pt-based HIFs materials is addressed by implanting non-noble metal or nonmetals as active auxiliaries into the near-surface of noble metal nanocrystals bounded with HIFs to engineer a stable structured catalyst. Then the Mo/Pt3Mn catalysts serving as proof-of-concept examples are designed and show enhanced catalytic performance of ethylene glycol (EG). According to the electrochemical in situ Fourier transform infrared spectroscopy results, the Mo modified Pt3Mn alloys with HIFs promote not only the C-C cleavage of EG but also the direct conversion of COHx to CO2, without the formation of COL poison species. In this case, the Mo/Pt3Mn catalysts show the greatly significant increase of the catalytic activity in copamprison with Pt3Mn CNC and the commercial Pt/C, as well as the enhanced stability. The high-resolution transmission electron microscopy and X-ray photoelectron spectrum assisted by Ar surface etching experiments accompanied by density functional theory calculations are further used to explore the structure-performance relationship of Mo/Pt3Mn CNC for electro-oxidation of EG. This study addresses a promising strategy to fabricate a stable structured catalysts, which will elucidate a very promising methodology for developing Pt-based catalysts for further application of the fuel cell.
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