Electrochemical CO2 reduction on copper nanoparticles-dispersed carbon aerogels

被引:55
作者
Xiao, Xinxin [1 ]
Xu, Yongliang [2 ]
Lv, Xiaomeng [1 ]
Xie, Jimin [1 ]
Liu, Jun [2 ]
Yu, Changlin [3 ]
机构
[1] Jiangsu Univ, Sch Chem & Chem Engn, Zhenjiang 212013, Jiangsu, Peoples R China
[2] Jiangsu Univ, Sch Environm & Safety Engn, Zhenjiang 212013, Jiangsu, Peoples R China
[3] Guangdong Univ Petrochem Technol, Fac Environm Sci & Engn, Maoming 525000, Guangdong, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2 electrochemical reduction; Cu nanoparticles; Carbon aerogel; CO2; activation; N-2; THEORETICAL INSIGHTS; ELECTROREDUCTION; DIOXIDE; CU; ELECTROCATALYSTS; EVOLUTION; AU; HYDROCARBONS; CATALYSIS; ELECTRODE;
D O I
10.1016/j.jcis.2019.03.005
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
The conversion of CO2 into carbon-based fuels via electrochemical reduction is a promising approach to realizing the termination of carbon cycling. Copper (Cu-0) is considered to be an effective electrochemical catalyst for such purpose. However, it is limited by its instability and low selectivity. In this work, Cu2+ was embedded into a polycondensation structure of resorcinol (R) and formaldehyde (F) via sol-gel reaction, and the complex was then calcined at high temperature to obtain copper nanoparticles-dispersed carbon aerogels (Cu/CA). The samples were further activated sequentially under CO2 and N-2 atmosphere. The final products under different activation temperature of secondary N-2 atmosphere were obtained and marked as Cu/CA-CO2-N-2-T. The existence of highly dispersed Cu-0 on the carbon aerogels was confirmed by XPS and HRTEM, which exhibited attractive activity towards electrochemical CO2 reduction reaction (CO2RR) forming carbon product in 0.1 M KHCO3 aqueous media. Furthermore, the CO2 RR product distribution varied under different samples. The sample activated under 700 degrees C (Cu/CA-CO2-N-2-700) with Cu loading c.a. 5.13 wt% showed remarkable CO faradaic efficiency (FE) (75.6%) at low overpotential of -0.49 V. Further calcination led to more exposure of copper, and CO dimerization to C2 product. The high selectivity toward CO by Cu/CA-CO2-N-2-700 maybe attributed to their excellent stability in maintaining the metallic nature of Cu component within the hydrophobic carbon aerogels during electrocatalysis, which further prevents the adsorption and reduction of CO on the catalyst. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:1 / 7
页数:7
相关论文
共 46 条
[1]   Active Sites of Au and Ag Nanoparticle Catalysts for CO2 Electroreduction to CO [J].
Back, Seoin ;
Yeom, Min Sun ;
Jung, Yousung .
ACS CATALYSIS, 2015, 5 (09) :5089-5096
[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]   Mechanistic Studies of the Oxygen Evolution Reaction Mediated by a Nickel-Borate Thin Film Electrocatalyst [J].
Bediako, D. Kwabena ;
Surendranath, Yogesh ;
Nocera, Daniel G. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (09) :3662-3674
[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]   Fabrication of novel shape Cu and Cu/Cu2O nanoparticles modified electrode for the determination of dopamine and paracetamol [J].
Devaraj, Manoj ;
Saravanan, R. ;
Deivasigamani, RanjithKumar ;
Gupta, Vinod Kumar ;
Gracia, F. ;
Jayadevan, Santhanalakshmi .
JOURNAL OF MOLECULAR LIQUIDS, 2016, 221 :930-941
[7]   CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface [J].
Dinh, Cao-Thang ;
Burdyny, Thomas ;
Kibria, Md Golam ;
Seifitokaldani, Ali ;
Gabardo, Christine M. ;
de Arquer, F. Pelayo Garcia ;
Kiani, Amirreza ;
Edwards, Jonathan P. ;
De Luna, Phil ;
Bushuyev, Oleksandr S. ;
Zou, Chengqin ;
Quintero-Bermudez, Rafael ;
Pang, Yuanjie ;
Sinton, David ;
Sargent, Edward H. .
SCIENCE, 2018, 360 (6390) :783-787
[8]   Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel [J].
Gao, Shan ;
Lin, Yue ;
Jiao, Xingchen ;
Sun, Yongfu ;
Luo, Qiquan ;
Zhang, Wenhua ;
Li, Dianqi ;
Yang, Jinlong ;
Xie, Yi .
NATURE, 2016, 529 (7584) :68-+
[9]   Recycling of carbon dioxide to methanol and derived products - closing the loop [J].
Goeppert, Alain ;
Czaun, Miklos ;
Jones, John-Paul ;
Prakash, G. K. Surya ;
Olah, George A. .
CHEMICAL SOCIETY REVIEWS, 2014, 43 (23) :7995-8048
[10]   Identification of Possible Pathways for C-C Bond Formation during Electrochemical Reduction of CO2: New Theoretical Insights from an Improved Electrochemical Model [J].
Goodpaster, Jason D. ;
Bell, Alexis T. ;
Head-Gordon, Martin .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2016, 7 (08) :1471-1477