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Tuning the electrocatalytic properties of a Cu electrode with organic additives containing amine group for CO2 reduction
Qiu, Yanling1; Zhong, Hexiang1,2; Xu, Wenbin1; Zhang, Taotao1,3; Li, Xianfeng1,2; Zhang, Huamin1,2
Corresponding AuthorLi, Xianfeng(lixianfeng@dicp.ac.cn) ; Zhang, Huamin(zhanghm@dicp.ac.cn)
Source PublicationJOURNAL OF MATERIALS CHEMISTRY A
2019-03-14
ISSN2050-7488
DOI10.1039/c9ta00039a
Volume7Issue:10Pages:5453-5462
Funding ProjectNational Natural Science Foundation of China[21577141] ; National Natural Science Foundation of China[21576255]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
WOS SubjectChemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS Research AreaChemistry ; Energy & Fuels ; Materials Science
WOS KeywordCARBON-DIOXIDE ELECTROREDUCTION ; TOTAL-ENERGY CALCULATIONS ; ELECTROCHEMICAL REDUCTION ; COPPER ; SELECTIVITY ; HYDROCARBONS ; TRANSITION ; EFFICIENCY ; CATALYSTS ; NANOCRYSTALS
AbstractThe conversion of CO2 into value-added chemicals by employing renewable energy via an electrochemical process has received increasing attention. However, the low reaction rate and efficiency, as well as poor selectivity, have limited its further development. The low solubility of CO2 in an aqueous solution is one of the main factors that limit the reaction rate and selectivity of the electroreduction of CO2 (ERC) at a high overpotential. In this study, an organic additive containing an -NH2 group (methyl carbamate, MC) was incorporated into the ERC electrolyte for the first time. By utilizing the affinity interaction between a Lewis acid (the -NH3+ group formed by protonation of the -NH2 group) and a Lewis base (CO2), the ERC reaction rate was increased by 17%, and the faradaic efficiency for the production of CH4 reached 81.6%, which represented a large increase of 34% and surpassed that of most reported Cu electrodes. Furthermore, the partial current density for the production of CH4 was 31 mA cm(-2) at -2.13 V (vs. RHE), which represents an increase of 30% in comparison with that in the blank system. In addition, the competitive hydrogen evolution reaction was substantially inhibited, and the decline in faradaic efficiency increased from 38.5% to 48.1% when the potential decreased gradually from -1.63 V to -1.98 V (vs. RHE). DFT calculations further indicate that the -NH3+ group can significantly promote the adsorption of CO* and CHO* on the Cu surface and increase the surface coverage of both intermediates. CHO* can be further stabilized by the -NH3+ group via the facilitation of partial electron transfer from Cu to C and the formation of H-bonds, which is favorable for further hydrogenation to form hydrocarbons. These results provide a simple and powerful way to increase the reaction rate and product selectivity of the reduction of CO2.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
WOS IDWOS:000463824300035
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/165651
Collection中国科学院大连化学物理研究所
Corresponding AuthorLi, Xianfeng; Zhang, Huamin
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Div Energy Storage, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Collaborat Innovat Ctr Chem Energy Mat iChEM, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Beying 100039, Peoples R China
Recommended Citation
GB/T 7714
Qiu, Yanling,Zhong, Hexiang,Xu, Wenbin,et al. Tuning the electrocatalytic properties of a Cu electrode with organic additives containing amine group for CO2 reduction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2019,7(10):5453-5462.
APA Qiu, Yanling,Zhong, Hexiang,Xu, Wenbin,Zhang, Taotao,Li, Xianfeng,&Zhang, Huamin.(2019).Tuning the electrocatalytic properties of a Cu electrode with organic additives containing amine group for CO2 reduction.JOURNAL OF MATERIALS CHEMISTRY A,7(10),5453-5462.
MLA Qiu, Yanling,et al."Tuning the electrocatalytic properties of a Cu electrode with organic additives containing amine group for CO2 reduction".JOURNAL OF MATERIALS CHEMISTRY A 7.10(2019):5453-5462.
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