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 |
推荐引用方式 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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