Size-Dependent Nickel-Based Electrocatalysts for Selective CO2Reduction

被引：181

作者：

Li, Zhida ^{[1
,2
]}

He, Dong ^{[5
,6
]}

Yan, Xingxu ^{[3
]}

Dai, Sheng ^{[3
]}

Younan, Sabrina ^{[2
]}

Ke, Zunjian ^{[2
,5
,6
]}

Pan, Xiaoqing ^{[3
,4
]}

Xiao, Xiangheng ^{[5
,6
]}

Wu, Hongjun ^{[1
,2
]}

Gu, Jing ^{[2
]}

机构：

[1] Northeast Petr Univ, Coll Chem & Chem Engn, Daqing 163318, Peoples R China

[2] San Diego State Univ, Dept Chem & Biochem, 5500 Campanile Dr, San Diego, CA 92182 USA

[3] Univ Calif Irvine, Dept Mat Sci & Engn, Irvine, CA 92697 USA

[4] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA

[5] Wuhan Univ, Inst Technol Sci, Minist Educ, Dept Phys, Wuhan 430072, Peoples R China

[6] Wuhan Univ, Inst Technol Sci, Minist Educ, Key Lab Artificial Micro & Nanostruct, Wuhan 430072, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 42期

基金：

美国国家科学基金会; 中国国家自然科学基金;

关键词：

CO selectivity; CO(2)reduction; DFT calculations; nickel; size dependence; NITROGEN-DOPED GRAPHENE; CO2; REDUCTION; OXYGEN REDUCTION; CATALYTIC SITES; ELECTROREDUCTION; NANOPARTICLES; TRENDS;

D O I：

10.1002/anie.202000318

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Closing the anthropogenic carbon cycle by converting CO(2)into reusable chemicals is an attractive solution to mitigate rising concentrations of CO(2)in the atmosphere. Herein, we prepared Ni metal catalysts ranging in size from single atoms to over 100 nm and distributed them across N-doped carbon substrates which were obtained from converted zeolitic imidazolate frameworks (ZIF). The results show variance in CO(2)reduction performance with variance in Ni metal size. Ni single atoms demonstrate a superior Faradaic efficiency (FE) for CO selectivity (ca. 97 % at -0.8 V vs. RHE), while results for 4.1 nm Ni nanoparticles are slightly lower (ca. 93 %). Further increase the Ni particle size to 37.2 nm allows the H(2)evolution reaction (HER) to compete with the CO(2)reduction reaction (CO2RR). The FE towards CO production decreases to under 30 % and HER efficiency increase to over 70 %. These results show a size-dependent CO(2)reduction for various sizes of Ni metal catalysts.

引用

页码：18572 / 18577

页数：6

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