First-Principles Study of C-C Coupling Pathways for CO2 Electrochemical Reduction Catalyzed by Cu(110)

被引：34

作者：

Kuo, Tung-Chun ^{[1
]}

Chou, Jia-Wei ^{[1
]}

Shen, Min-Hsiu ^{[1
]}

Hong, Zih-Siang ^{[1
]}

Chao, Tzu-Hsuan ^{[1
]}

Lu, Qi ^{[2
]}

Cheng, Mu-Jeng ^{[1
]}

机构：

[1] Natl Cheng Kung Univ, Dept Chem, Tainan 701, Taiwan

[2] Tsinghua Univ, Dept Chem Engn, State Key Lab Chem Engn, Beijing 10084, Peoples R China

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2021年 / 125卷 / 04期

基金：

中国国家自然科学基金;

关键词：

COPPER SINGLE-CRYSTAL; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; CARBON-DIOXIDE REDUCTION; THEORETICAL INSIGHTS; SELECTIVE FORMATION; REACTION-MECHANISMS; STRAIN CONTROL; ELECTRODE; SURFACE;

D O I：

10.1021/acs.jpcc.0c10736

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：

To build a carbon-neutral energy cycle, the development of electrocatalysts that can reduce CO2 into products containing at least two carbon atoms (C2+) is crucial. This process would require at least one C-C coupling of two C-1 intermediates. The (110) facet of copper is known for its ability to reduce CO2 to C2+ products in high quantities (Faradaic efficiency >= 65%). In this study, we used constant electrode potential density functional theory calculations to determine the dominant C-C coupling pathways for CO2 electrochemical reduction (CO2ER) on Cu(110). By studying the mechanism of CO2ER to methane, we identified *CO and *CH as high-concentration C-1 species due to their high Delta G* for further hydrogenation. Based on this result, 26 C-C coupling reactions that contain at least one high-concentration C-1 intermediate were selected for investigation. The most important ones responsible for C2+ formation on Cu(110) were identified, and the influence of strain on the rates of these reactions was also investigated.

引用

页码：2464 / 2476

页数：13

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[1] PROJECTOR AUGMENTED-WAVE METHOD [J].