Electrochemical reduction of CO2 on compositionally variant Au-Pt bimetallic thin films

被引:100
|
作者
Ma, Ming [1 ]
Hansen, Heine A. [2 ]
Valenti, Marco [1 ]
Wang, Zegao [3 ]
Cao, Anping [4 ]
Dong, Mingdong [3 ]
Smith, Wilson A. [1 ]
机构
[1] Delft Univ Technol, Fac Appl Sci, Dept Chem Engn, MECS, Van der Maasweg 9, NL-2629 HZ Delft, Netherlands
[2] Tech Univ Denmark, Dept Energy Convers & Storage, DK-2800 Lyngby, Denmark
[3] Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus, Denmark
[4] Eindhoven Univ Technol, Dept Chem Engn & Chem, POB 513, NL-5600 MB Eindhoven, Netherlands
关键词
CO2; conversion; Bimetallic catalysts; Au-Pt alloy thin films; Electrocatalysis; CARBON-DIOXIDE; AQUEOUS CO2; ELECTROCATALYTIC REDUCTION; ALLOY SURFACES; COPPER; ELECTROREDUCTION; NANOPARTICLES; ELECTRODES; NANOWIRES; CATALYSTS;
D O I
10.1016/j.nanoen.2017.09.043
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 electrocatalytic reduction of CO2 on Au-Pt bimetallic catalysts with different compositions was evaluated, offering a platform for uncovering the correlation between the catalytic activity and the surface composition of bimetallic electrocatalysts. The Au-Pt alloy films were synthesized by a magnetron sputtering co-deposition technique with tunable composition. It was found that the syngas ratio (CO:H-2) on the Au-Pt films is able to be tuned by systematically controlling the binary composition. This tunable catalytic selectivity is attributed to the variation of binding strength of COOH and CO intermediates, influenced by the surface electronic structure (d-band center energy) which is linked to the surface composition of the bimetallic films. Notably, a gradual shift of the d-band center away from the Fermi level was observed with increasing Au content, which correspondingly reduces the binding strength of the COOH and CO intermediates, leading to the distinct catalytic activity for the reduction of CO2 on the compositionally variant Au-Pt bimetallic films. In addition, the formation of formic acid in the bimetallic systems at reduced overpotentials and higher yield indicates that synergistic effects can facilitate reaction pathways for products that are not accessible with the individual components.
引用
收藏
页码:51 / 57
页数:7
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