Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO2 Reduction

被引：123

作者：

Cao, Zhi ^{[1
,2
,3
]}

Zacate, Samson B. ^{[4
]}

Sun, Xiaodong ^{[1
,2
]}

Liu, Jinjia ^{[1
,2
]}

Hale, Elizabeth M. ^{[4
]}

Carson, William P. ^{[4
]}

Tyndall, Sam B. ^{[4
]}

Xu, Jun ^{[3
]}

Liu, Xingwu ^{[1
,2
]}

Liu, Xingchen ^{[1
,2
]}

Song, Chang ^{[1
,2
]}

Luo, Jheng-hua ^{[5
]}

Cheng, Mu-Jeng ^{[5
]}

Wen, Xiaodong ^{[1
,2
]}

Liu, Wei ^{[4
]}

机构：

[1] Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Shanxi, Peoples R China

[2] Synfuels China Technol Co Ltd, Natl Energy Ctr Coal Liquids, Beijing 101400, Peoples R China

[3] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[4] Miami Univ, Dept Chem & Biochem, Oxford, OH 45056 USA

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

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2018年 / 57卷 / 39期

基金：

中国国家自然科学基金;

关键词：

chelate effect; CO2; reduction; electrocatalysis; gold nanoparticles; porphyrins; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; FORMIC-ACID; SURFACE; SIZE; ELECTROREDUCTION; CONVERSION; PLANET;

D O I：

10.1002/anie.201805696

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Capped chelating organic molecules are presented as a design principle for tuning heterogeneous nanoparticles for electrochemical catalysis. Gold nanoparticles (AuNPs) functionalized with a chelating tetradentate porphyrin ligand show a 110-fold enhancement compared to the oleylamine-coated AuNP in current density for electrochemical reduction of CO2 to CO in water at an overpotential of 340 mV with Faradaic efficiencies (FEs) of 93%. These catalysts also show excellent stability without deactivation (<5% productivity loss) within 72 hours of electrolysis. DFT calculation results further confirm the chelation effect in stabilizing molecule/NP interface and tailoring catalytic activity. This general approach is thus anticipated to be complementary to current NP catalyst design approaches.

引用

页码：12675 / 12679

页数：5

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