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Silver-doped nickel thiolates as electrocatalysts for heterogeneous CO2 reduction

银掺杂镍的硫醇盐类团簇用于非均相电催化二氧化碳还原

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摘要

精细调控具有原子尺度精确的团簇结构并将其应用于非均相催化研究, 对于从分子水平阐明催化反应机制, 明确催化反应活性位具有重要意义. 本文基于环已硫醇保护的Ni4团簇体系, 成功制备了一种全新的Ni3Ag2双金属团簇, 该团簇为Ni4团簇中一个Ni原子被两个Ag原子取代的结果. 研究发现将该团簇用于非均相电催化二氧化碳还原, Ni3Ag2双金属团簇催化二氧化碳还原产生一氧化碳的法拉第效率可达90%以上, 而母体结构Ni4团簇的催化产物主要为氢气. 对照实验与DFT理论计算结果表明, 电解中去配体过程对于Ni3Ag2团簇的高选择性催化具有重要作用. 其催化二氧化碳选择性还原的主要活性位为去配体后暴露出的Ni原子而非Ag原子.

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Acknowledgements

This work was supported by the Major Program of National Natural Science Foundation of China (92161110), the Natural Science Foundation of Hubei Province of China (2021CFB174), the Open Research Project of State key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2021006) and the Opening Fund of Hubei Key Laboratory of Bioinorganic Chemistry & Mate-ria Medica (BCMM202104).

Author information

Authors and Affiliations

  1. School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan, 430205, China

    Fan Tian  (田凡), Wangxuan Li  (李旺轩), Wenjin Guo  (郭文锦) & Rong Chen  (陈嵘)

  2. State Key Laboratory of New Textile Materials and Advanced Processing Technologies, Wuhan Textile University, Wuhan, 430200, China

    Rong Chen  (陈嵘)

  3. Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Guangfang Li  (李广芳)

Authors
  1. Fan Tian  (田凡)
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  2. Wangxuan Li  (李旺轩)
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  3. Wenjin Guo  (郭文锦)
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  4. Guangfang Li  (李广芳)
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  5. Rong Chen  (陈嵘)
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Contributions

Author contributions Chen R supervised the project. Tian F designed the study, conducted the experiments and DFT calculations, and analyzed the results. Li W prepared the clusters. Guo W performed the electrochemical measurement. Li G assisted in the characterizations. All authors participated in the discussion of the results and organization of the manuscript.

Corresponding author

Correspondence to Rong Chen  (陈嵘).

Additional information

Conflict of interest The authors declare that they have no conflict of interest.

Fan Tian obtained his BSc (2013), MSc (2016), and PhD (2020) degrees from Wuhan Institute of Technology under the supervision of prof. Rong Chen. Currently, he is a chair associate professor at Wuhan Institute of Technology. His research interests focus on the development of nanoclusters and cluster-related DFT calculations.

Rong Chen received his PhD degree from the University of Hong Kong in 2006 under the supervision of prof. Chi-Ming Che and prof. Hongzhe Sun. After that, he worked at Wuhan Institute of Technology as a full professor from 2007 to 2021. Since 2022, he has been working at Wuhan Textile University as a full professor in the State Key Laboratory of New Textile Materials and Advanced Processing Technologies. His current research interests focus on the precise synthesis of micro-/nanostructured inorganic functional materials and their applications in environmental catalysis and adsorption, textiles and biomedicine.

Supplementary information Experimental details and supporting data are available in the online version of the paper.

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Tian, F., Li, W., Guo, W. et al. Silver-doped nickel thiolates as electrocatalysts for heterogeneous CO2 reduction. Sci. China Mater. 66, 407–412 (2023). https://doi.org/10.1007/s40843-022-2230-6

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  • DOI: https://doi.org/10.1007/s40843-022-2230-6

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