In Situ Surface-Enhanced Raman Spectroscopic Evidence on the Origin of Selectivity in CO2 Electrocatalytic Reduction
Shan, Wanyu; Liu, Rui; Zhao, Huachao; He, Zuoliang; Lai, Yujian; Li, Shasha; He, Guangzhi; Liu, Jingfu
刊名ACS NANO
2020-09-22
卷号14期号:9页码:11363-11372
关键词CO2 electrocatalytic reduction in situ SERS nanoporous silver selectivity regulating target
ISSN号1936-0851
英文摘要The electrocatalytic reduction of CO2 (CO2ER) to liquid fuels is important for solving fossil fuel depletion. However, insufficient insight into the reaction mechanisms renders a lack of effective regulation of liquid product selectivity. Here, in situ surface-enhanced Raman spectroscopy (SERS) empowered by C-13/C-12 isotope exchange is applied to probing the CO2ER process on nanoporous silver (np-Ag). Direct spectroscopic evidence of the preliminary intermediates, *COOH and *OCO-, indicates that CO2 is coordinated to the catalyst via diverse adsorption modes. Further, the relative Raman intensities of the above intermediates vary notably on np-Ag modified by Cu or Pd, and the liquid product selectivity also changes accordingly. Combined with density functional theory calculations, this study demonstrates that the CO2 adsorption configuration is a critical factor governing the reaction selectivity. Meanwhile, *COOH and *OCO- are key targets in the initial stage regulating liquid product selectivity, which could facilitate future selective catalyst design.
内容类型期刊论文
源URL[http://ir.rcees.ac.cn/handle/311016/44713]  
专题生态环境研究中心_环境化学与生态毒理学国家重点实验室
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GB/T 7714
Shan, Wanyu,Liu, Rui,Zhao, Huachao,et al. In Situ Surface-Enhanced Raman Spectroscopic Evidence on the Origin of Selectivity in CO2 Electrocatalytic Reduction[J]. ACS NANO,2020,14(9):11363-11372.
APA Shan, Wanyu.,Liu, Rui.,Zhao, Huachao.,He, Zuoliang.,Lai, Yujian.,...&Liu, Jingfu.(2020).In Situ Surface-Enhanced Raman Spectroscopic Evidence on the Origin of Selectivity in CO2 Electrocatalytic Reduction.ACS NANO,14(9),11363-11372.
MLA Shan, Wanyu,et al."In Situ Surface-Enhanced Raman Spectroscopic Evidence on the Origin of Selectivity in CO2 Electrocatalytic Reduction".ACS NANO 14.9(2020):11363-11372.
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