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题名: Copper Electrode Fabricated via Pulse Electrodeposition: Toward High Methane Selectivity and Activity for CO2 Electroreduction
作者: Qiu, Yan-Ling1;  Zhong, He-Xiang1, 3;  Zhang, Tao-Tao1, 2;  Xu, Wen-Bin1;  Li, Xian-Feng1, 3;  Zhang, Hua-Min1, 3
关键词: carbon dioxide electroreduction ;  methane ;  Faradaic efficiency ;  electrocatalytic activity ;  Cu electrode ;  pulse-electrodeposition
刊名: ACS CATALYSIS
发表日期: 2017-09-01
DOI: 10.1021/acscatal.7b00571
卷: 7, 期:9, 页:6302-6310
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: Electrochemical reduction of CO2 (ERC) to methane has significant economic benefits and represents one promising solution for energy and environmental sustain ability. However, traditional metal electrodes suffer from higher overpotentials, low activities, and poor selectivity. In this article, the pulse electrodeposition (P-ED) method is employed to prepare a copper electrode for ERC. The P-ED method can easily create Cu coatings on carbon paper with a much rougher surface and extended surface area, which is highly beneficial for improving their activity and selectivity. As a result, the prepared Cu electrodes exhibit high faradaic efficiency (of 85% at -2.8 V) and enhanced partial current density (jCH(4) = 38 mA cm(-2)) for methane, which is by far the highest value ever reported at room temperature and ambient pressure. The enhanced activity is attributed to the extended reactive areas with rough morphology and loosened coating structure to ensure CO2 access the reaction sites located at the sublayers of the deposited Cu coatings. The prominent selectivity for CH4 is likely due to the presence of a stepped surface, which is formed by introduction of Cu (100) step into Cu (111) and Cu (220) terraces during the P-ED processes. The lower resistance to the one-electron transfer to CO2, which is a pre equilibrium step prior to the rate-limiting nonelectrochemical step, is another positive factor to improve the ERC activity for CH4. Furthermore, we surprisingly find that the activity and selectivity of the Cu electrode can be easily recovered through continuous CO2 bubbling. This paper provides a facile method to prepare highly effective electrodes for electrochemical conversion of CO2.
关键词[WOS]: ELECTROCHEMICAL REDUCTION ;  CARBON-DIOXIDE ;  CU NANOPARTICLES ;  SINGLE-CRYSTAL ;  HYDROCARBONS ;  CONVERSION ;  NANOWIRES ;  SURFACES ;  ETHYLENE ;  FILMS
语种: 英语
WOS记录号: WOS:000410005700084
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/150033
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Div Energy Storage, Zhongshan Rd 457, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Collaborat Innovat Ctr Chem Energy Mat iChEM, Dalian 116023, Peoples R China

Recommended Citation:
Qiu, Yan-Ling,Zhong, He-Xiang,Zhang, Tao-Tao,et al. Copper Electrode Fabricated via Pulse Electrodeposition: Toward High Methane Selectivity and Activity for CO2 Electroreduction[J]. ACS CATALYSIS,2017,7(9):6302-6310.
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