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

共 52 条

[1] Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid [J].

Asadi, Mohammad ;

Kim, Kibum ;

Liu, Cong ;

Addepalli, Aditya Venkata ;

Abbasi, Pedram ;

Yasaei, Poya ;

Phillips, Patrick ;

Behranginia, Amirhossein ;

Cerrato, Jose M. ;

Haasch, Richard ;

Zapol, Peter ;

Kumar, Bijandra ;

Klie, Robert F. ;

Abiade, Jeremiah ;

Curtiss, Larry A. ;

Salehi-Khojin, Amin .

SCIENCE, 2016, 353 (6298) :467-470

[2]

Cao Z., 2018, Angew. Chem, V130, P5075

[3] Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry [J].

Cao, Zhi ;

Derrick, Jeffrey S. ;

Xu, Jun ;

Gao, Rui ;

Gong, Ming ;

Nichols, Eva M. ;

Smith, Peter T. ;

Liu, Xingwu ;

Wen, Xiaodong ;

Coperet, Christophe ;

Chang, Christopher J. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2018, 57 (18) :4981-4985

[4] A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction [J].

Cao, Zhi ;

Kim, Dohyung ;

Hong, Dachao ;

Yu, Yi ;

Xu, Jun ;

Lin, Song ;

Wen, Xiaodong ;

Nichols, Eva M. ;

Jeong, Keunhong ;

Reimer, Jeffrey A. ;

Yang, Peidong ;

Chang, Christopher J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (26) :8120-8125

[5] Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].

Chen, Yihong ;

Li, Christina W. ;

Kanan, Matthew W. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972

[6] Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles [J].

Cheng, Tao ;

Huang, Yufeng ;

Xiao, Hai ;

Goddard, William A., III .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2017, 8 (14) :3317-3320

[7] Reaction Mechanisms for the Electrochemical Reduction of CO2 to CO and Formate on the Cu(100) Surface at 298 K from Quantum Mechanics Free Energy Calculations with Explicit Water [J].

Cheng, Tao ;

Xiao, Hai ;

Goddard, William A., III .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (42) :13802-13805

[8] Catalysis of the electrochemical reduction of carbon dioxide [J].

Costentin, Cyrille ;

Robert, Marc ;

Saveant, Jean-Michel .

CHEMICAL SOCIETY REVIEWS, 2013, 42 (06) :2423-2436

[9]

ELAASAR AMM, 1982, BIOCHEMISTRY-US, V21, P1972

[10] Understanding Selectivity for the Electrochemical Reduction of Carbon Dioxide to Formic Acid and Carbon Monoxide on Metal Electrodes [J].

Feaster, Jeremy T. ;

Shi, Chuan ;

Cave, Etosha R. ;

Hatsukade, Tom T. ;

Abram, David N. ;

Kuhl, Kendra P. ;

Hahn, Christopher ;

Norskov, Jens K. ;

Jaramillo, Thomas F. .

ACS CATALYSIS, 2017, 7 (07) :4822-4827

← 1 2 3 4 5 6 →