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
[11]   CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O Films [J].
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (17) :7231-7234
[12]   Recent advances in the organic solution phase synthesis of metal nanoparticles and their electrocatalysis for energy conversion reactions [J].
Li, Qing ;
Sun, Shouheng .
NANO ENERGY, 2016, 29 :178-197
[13]   Graphene and its composites with nanoparticles for electrochemical energy applications [J].
Li, Qing ;
Mahmood, Nasir ;
Zhu, Jinghan ;
Hou, Yanglong ;
Sun, Shouheng .
NANO TODAY, 2014, 9 (05) :668-683
[14]   Nanocarbon Electrocatalysts for Oxygen Reduction in Alkaline Media for Advanced Energy Conversion and Storage [J].
Li, Qing ;
Cao, Ruiguo ;
Cho, Jaephil ;
Wu, Gang .
ADVANCED ENERGY MATERIALS, 2014, 4 (06)
[15]   Nanostructured Metallic Electrocatalysts for Carbon Dioxide Reduction [J].
Lu, Qi ;
Rosen, Jonathan ;
Jiao, Feng .
CHEMCATCHEM, 2015, 7 (01) :38-47
[16]   A selective and efficient electrocatalyst for carbon dioxide reduction [J].
Lu, Qi ;
Rosen, Jonathan ;
Zhou, Yang ;
Hutchings, Gregory S. ;
Kimmel, Yannick C. ;
Chen, Jingguang G. ;
Jiao, Feng .
NATURE COMMUNICATIONS, 2014, 5
[17]   Trace Levels of Copper in Carbon Materials Show Significant Electrochemical CO2 Reduction Activity [J].
Lum, Yanwei ;
Kwon, Youngkook ;
Lobaccaro, Peter ;
Chen, Le ;
Clark, Ezra Lee ;
Bell, Alexis T. ;
Ager, Joel W. .
ACS CATALYSIS, 2016, 6 (01) :202-209
[18]   Insights into CC Coupling in CO2 Electroreduction on Copper Electrodes [J].
Montoya, Joseph H. ;
Peterson, Andrew A. ;
Norskov, Jens K. .
CHEMCATCHEM, 2013, 5 (03) :737-742
[19]   Selectivity of CO2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary Steps [J].
Nie, Xiaowa ;
Esopi, Monica R. ;
Janik, Michael J. ;
Asthagiri, Aravind .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (09) :2459-2462
[20]   How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels [J].
Peterson, Andrew A. ;
Abild-Pedersen, Frank ;
Studt, Felix ;
Rossmeisl, Jan ;
Norskov, Jens K. .
ENERGY & ENVIRONMENTAL SCIENCE, 2010, 3 (09) :1311-1315