Implanting Mo Atoms into Surface Lattice of Pt3Mn Alloys Enclosed by High-Indexed Facets: Promoting Highly Active Sites for Ethylene Glycol Oxidation

被引:95
作者
Wang, Yao [1 ]
Zhuo, Hongying [1 ]
Sun, Hui [1 ]
Zhang, Xin [1 ]
Dai, Xiaoping [1 ]
Luan, Chenglong [1 ]
Qin, Congli [1 ]
Zhao, Huihui [1 ]
Li, Jun [2 ,3 ]
Wang, Meiling [4 ]
Ye, Jin-Yu [5 ]
Sun, Shi-Gang [5 ]
机构
[1] China Univ Petr, Coll Chem Engn, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[2] Tsinghua Univ, Minist Educ, Dept Chem, Beijing 100084, Peoples R China
[3] Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
[4] Natl Inst Metrol, Beijing 100013, Peoples R China
[5] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
关键词
Pt-based alloy catalysts; high-indexed facets; Mo decoration; electronic effect; ethylene glycol oxidation; OXYGEN REDUCTION REACTION; PT-M M; HYDROGEN-EVOLUTION REACTION; TIME FTIR SPECTROSCOPY; METHANOL OXIDATION; CATALYTIC-ACTIVITY; NI ALLOY; PLATINUM NANOCRYSTALS; ASSISTED SYNTHESIS; NICKEL-HYDROXIDE;
D O I
10.1021/acscatal.8b04447
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 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.
引用
收藏
页码:442 / 455
页数:27
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