Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction
Yan, CC; Li, HB; Ye, YF; Wu, HH; Cai, F; Si, R; Xiao, JP; Miao, S; Xie, SH; Yang, F; Li, YS; Wang, GX; Bao, XH
2018
发表期刊ENERGY & ENVIRONMENTAL SCIENCE
ISSN1754-5692
卷号11期号:5页码:1204-1210
文章类型期刊论文
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.
关键词X-ray Photoelectron-spectroscopy Electrochemical Co2 Carbon-dioxide Reduction Nanoparticles Graphene Oxygen
DOI10.1039/c8ee00133b
收录类别SCI
语种英语
WOS记录号WOS:000432599100007
引用统计
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/28950
专题中科院上海应用物理研究所2011-2018年
作者单位1.Yan, CC
2.Li, HB
3.Ye, YF
4.Wu, HH
5.Cai, F
6.Si, R
7.Xiao, JP
8.Miao, S
9.Xie, SH
10.Yang, F
11.Li, YS
12.Wang, GX
13.Bao, XH
推荐引用方式
GB/T 7714
Yan, CC,Li, HB,Ye, YF,et al. Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction[J]. ENERGY & ENVIRONMENTAL SCIENCE,2018,11(5):1204-1210.
APA Yan, CC.,Li, HB.,Ye, YF.,Wu, HH.,Cai, F.,...&Bao, XH.(2018).Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction.ENERGY & ENVIRONMENTAL SCIENCE,11(5),1204-1210.
MLA Yan, CC,et al."Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction".ENERGY & ENVIRONMENTAL SCIENCE 11.5(2018):1204-1210.
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