First-Principles Investigation of the Formation of Pt Nanorafts on a Mo2C Support and Their Catalytic Activity for Oxygen Reduction Reaction

被引:34
作者
Krishnamurthy, Chethana B. [1 ]
Lori, Oran [1 ]
Elbaz, Lior [1 ]
Grinberg, Ilya [1 ]
机构
[1] Bar Ilan Univ, Dept Chem, IL-52900 Ramat Gan, Israel
关键词
MOLYBDENUM CARBIDE; TRANSITION-METALS; FUEL-CELLS; PLATINUM; CO; ELECTROCATALYSTS; STABILITY; AG; HYDROGENATION; SURFACES;
D O I
10.1021/acs.jpclett.8b00949
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
We use first-principles calculations to study the formation of Pt nanorafts and their oxygen reduction reaction (ORR) catalytic activity on Mo2C. Due to the high Pt binding energy on C atoms, Pt forms sheet-like structures on the Mo2C surface instead of agglomerating into particles. We find that the disordered Mo2C surface carbon arrangement limits the Pt sheet growth, leading to the formation of 4-6 atom Pt nanorafts. The O-O repulsion between the O atoms on the Mo2C and O adsorbate enhances the ORR activity by weakening the O adsorption energy. We find a significant change from the usual scaling of the energies of the intermediates in the ORR pathway and a strong interaction between the nanoraft and water that lead to a high activity of the Pt nanorafts. Fundamentally, our work demonstrates that the activity of metal catalysts can be strongly affected by manipulation of the atomic arrangement of the supporting carbide surface.
引用
收藏
页码:2229 / 2234
页数:11
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