Controlled assembly of Cu nanoparticles on pyridinic-N rich graphene for electrochemical reduction of CO2 to ethylene

被引:210
作者
Li, Qing [1 ,3 ]
Zhu, Wenlei [1 ]
Fu, Jiaju [1 ]
Zhang, Hongyi [1 ]
Wu, Gang [2 ]
Sun, Shouheng [1 ]
机构
[1] Brown Univ, Dept Chem, Providence, RI 02912 USA
[2] SUNY Buffalo, Univ Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
[3] Huazhong Univ Sci & Technol, Sch Mat Sci & Engn, Wuhan 430074, Peoples R China
基金
美国国家科学基金会;
关键词
Cu nanoparticles; Self-assembly; Graphene; Nitrogen doping; CO2; reduction; Electrocatalysis; SELECTIVE ELECTROCATALYTIC REDUCTION; CARBON-DIOXIDE; ELECTROREDUCTION; COPPER; ELECTRODES; CATALYSTS; FORMATE;
D O I
10.1016/j.nanoen.2016.03.024
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
Monodisperse Cu nanoparticles (NPs) assembled on a pyridinic-N rich graphene (p-NG) support show a Cu NP mass- and size-dependent catalysis for the selective electrochemical reduction of CO2 to ethylene (C2H4). For the 7 nm Cu NPs assembled on the p-NG with the p-NG/Cu mass ratio of 1:1, the C2H4 formation Faradaic efficiency and hydrocarbon selectivity reach 19% and 79% respectively at -0.9 V (vs reversible hydrogen electrode). The p-NG itself can catalyze the CO2 reduction to formate, but in the composite p-NG-Cu structure, the pyridinic-N functions as a CO2 and proton absorber, facilitating hydrogenation and carbon-carbon coupling reactions on Cu for the formation of C2H4. The work demonstrates a new strategy to improve Cu NP catalytic activity and selectivity for the electrochemical reduction of CO2 for sustainable chemistry and energy applications. (C) 2016 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1 / 9
页数:9
相关论文
共 30 条
[1]   Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2 Fixation [J].
Appel, Aaron M. ;
Bercaw, John E. ;
Bocarsly, Andrew B. ;
Dobbek, Holger ;
DuBois, Daniel L. ;
Dupuis, Michel ;
Ferry, James G. ;
Fujita, Etsuko ;
Hille, Russ ;
Kenis, Paul J. A. ;
Kerfeld, Cheal A. ;
Morris, Robert H. ;
Peden, Charles H. F. ;
Portis, Archie R. ;
Ragsdale, Stephen W. ;
Rauchfuss, Thomas B. ;
Reek, Joost N. H. ;
Seefeldt, Lance C. ;
Thauer, Rudolf K. ;
Waldrop, Grover L. .
CHEMICAL REVIEWS, 2013, 113 (08) :6621-6658
[2]   CO2 Electroreduction to Hydrocarbons on Carbon-Supported Cu Nanoparticles [J].
Baturina, Olga A. ;
Lu, Qin ;
Padilla, Monica A. ;
Xin, Le ;
Li, Wenzhen ;
Serov, Alexey ;
Artyushkova, Kateryna ;
Atanassov, Plamen ;
Xu, Feng ;
Epshteyn, Albert ;
Brintlinger, Todd ;
Schuette, Mike ;
Collins, Greg E. .
ACS CATALYSIS, 2014, 4 (10) :3682-3695
[3]   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
[4]   Electrocatalytic reduction of dioxygen at platinum particles dispersed in a polyaniline film [J].
Coutanceau, C ;
Croissant, MJ ;
Napporn, T ;
Lamy, C .
ELECTROCHIMICA ACTA, 2000, 46 (04) :579-588
[5]   Anodized Indium Metal Electrodes for Enhanced Carbon Dioxide Reduction in Aqueous Electrolyte [J].
Detweiler, Zachary M. ;
White, James L. ;
Bernasek, Steven L. ;
Bocarsly, Andrew B. .
LANGMUIR, 2014, 30 (25) :7593-7600
[6]   Room-Temperature Formation of Hollow Cu2O Nanoparticles [J].
Hung, Ling-I ;
Tsung, Chia-Kuang ;
Huang, Wenyu ;
Yang, Peidong .
ADVANCED MATERIALS, 2010, 22 (17) :1910-+
[7]   Rapid Selective Electrocatalytic Reduction of Carbon Dioxide to Formate by an Iridium Pincer Catalyst Immobilized on Carbon Nanotube Electrodes [J].
Kang, Peng ;
Zhang, Sheng ;
Meyer, Thomas J. ;
Brookhart, Maurice .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (33) :8709-8713
[8]   Electrochemical CO2 reduction on Cu2O-derived copper nanoparticles: controlling the catalytic selectivity of hydrocarbons [J].
Kas, Recep ;
Kortlever, Ruud ;
Milbrat, Alexander ;
Koper, Marc T. M. ;
Mul, Guido ;
Baltrusaitis, Jonas .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (24) :12194-12201
[9]  
Kim D., 2014, NAT COMMUN, V5
[10]   Controlling H+ vs CO2 Reduction Selectivity on Pb Electrodes [J].
Lee, Chang Hoon ;
Kanan, Matthew W. .
ACS CATALYSIS, 2015, 5 (01) :465-469