Ternary Sn-Ti-O Electrocatalyst Boosts the Stability and Energy Efficiency of CO2Reduction

被引：84

作者：

Wen, Guobin ^{[1
,2
]}

Ren, Bohua ^{[2
]}

Park, Moon G. ^{[2
]}

Yang, Jie ^{[3
,4
]}

Dou, Haozhen ^{[2
]}

Zhang, Zhen ^{[2
]}

Deng, Ya-Ping ^{[2
]}

Bai, Zhengyu ^{[1
]}

Yang, Lin ^{[1
]}

Gostick, Jeff ^{[2
]}

Botton, Gianluigi A. ^{[3
,4
,5
]}

Hu, Yongfeng ^{[5
]}

Chen, Zhongwei ^{[2
]}

机构：

[1] Henan Normal Univ, Sch Chem & Chem Engn, Key Lab Green Chem Media & React, Minist Educ, Xinxiang 453007, Henan, Peoples R China

[2] Waterloo Inst Nano, Dept Chem Engn, Waterloo Inst Sustainable Energy, Waterloo, ON N2L 3G1, Canada

[3] McMaster Univ, Dept Mat Sci & Engn, 1280 Main St West, Waterloo, ON L8S 4M1, Canada

[4] McMaster Univ, Canadian Ctr Elect Microscopy, 1280 Main St West, Waterloo, ON L8S 4M1, Canada

[5] Univ Saskatchewan, Canadian Light Source, Saskatoon, SK S7N 0X4, Canada

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 31期

基金：

加拿大自然科学与工程研究理事会; 中国国家自然科学基金; 加拿大健康研究院;

关键词：

carbon dioxide fixation; electrochemistry; interfaces; materials science; mesoporous materials; LOW-OVERPOTENTIAL ELECTROREDUCTION; CARBON-DIOXIDE CONVERSION; CO2; ELECTROREDUCTION; ELECTROCHEMICAL REDUCTION; MECHANISTIC INSIGHTS; CATALYST; SITES; GOLD; ELECTRODES; VALENCE;

D O I：

10.1002/anie.202004149

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO(2)conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn(0.3)Ti(0.7)O(2)achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.5 % Faradaic efficiency for CO at an overpotential as low as 430 mV. DFT and X-ray absorption fine structure analyses reveal an electron density reconfiguration in the Sn-Ti-O system. A downshift of the orbital band center of Sn and a charge depletion of Ti collectively facilitate the dissociative adsorption of the desired intermediate COOH* for CO formation. It is also beneficial in maintaining a local alkaline environment to suppress H(2)and formate formation, and in stabilizing oxygen atoms to prolong durability. These findings provide a new strategy in materials design for efficient CO(2)conversion and beyond.

引用

页码：12860 / 12867

页数：8

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