气候变化领域集成服务门户(CCPortal): Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction

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DOI	10.1039/c8ee00133b
	Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction
	Yan C.; Li H.; Ye Y.; Wu H.; Cai F.; Si R.; Xiao J.; Miao S.; Xie S.; Yang F.; Li Y.; Wang G.; Bao X.
发表日期	2018
ISSN	17545692
起始页码	1204
结束页码	1210
卷号	11 期号:5
英文摘要	High Faradaic efficiency and appreciable current density are essential for future applications of the electrochemical CO2 reduction reaction (CO2RR). However, these goals are difficult to achieve simultaneously due to the severe side reaction-the hydrogen evolution reaction (HER). Herein, we successfully synthesized coordinatively unsaturated nickel-nitrogen (Ni-N) sites doped within porous carbon with a nickel loading as high as 5.44 wt% by pyrolysis of Zn/Ni bimetallic zeolitic imidazolate framework-8. Over the Ni-N composite catalysts, the CO current density increases with the overpotential and reaches 71.5 ± 2.9 mA cm-2 at -1.03 V (vs. a reversible hydrogen electrode, RHE), while maintaining a high CO Faradaic efficiency of 92.0-98.0% over a wide potential range of -0.53 to -1.03 V (vs. the RHE). Density functional theory calculations suggest that the CO2RR occurs more easily than the HER over the coordinatively unsaturated Ni-N site. Therefore, highly doped and coordinatively unsaturated Ni-N sites achieve high current density and Faradaic efficiency of the CO2RR simultaneously, breaking current limits in metal-nitrogen composite catalysts. © 2018 The Royal Society of Chemistry.
英文关键词	Carbon dioxide; Catalysts; Current density; Density functional theory; Efficiency; Electrolytic reduction; Hydrogen; Nickel; Nitrogen; Porous materials; Co-ordinatively unsaturated; Composite catalysts; Faradaic efficiencies; Future applications; High current densities; Hydrogen evolution reactions; Reversible hydrogen electrodes; Zeolitic imidazolate framework-8; Nickel compounds; carbon dioxide; catalyst; chemical reaction; composite; electrical method; electrode; energy efficiency; nickel; nitrogen; pyrolysis; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190250
作者单位	State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China; University of Chinese Academy of Sciences, Beijing, 100039, China; Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China; Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai, 200433, China; School of Material Science and Chemical Engineering, Department of Chemistry, Ningbo University, Ningbo, 315211, China
推荐引用方式 GB/T 7714	Yan C.,Li H.,Ye Y.,et al. Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction[J],2018,11(5).
APA	Yan C..,Li H..,Ye Y..,Wu H..,Cai F..,...&Bao X..(2018).Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction.Energy & Environmental Science,11(5).
MLA	Yan C.,et al."Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction".Energy & Environmental Science 11.5(2018).