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author:

Duan, X. (Duan, X..) [1] | Xu, J. (Xu, J..) [2] | Cong, Y. (Cong, Y..) [3] | Geng, H. (Geng, H..) [4] | Chen, K. (Chen, K..) [5] | Xu, T. (Xu, T..) [6] | Zhang, Y. (Zhang, Y..) [7] | Zhang, F. (Zhang, F..) [8] | Zhu, J. (Zhu, J..) [9] | Zhang, L. (Zhang, L..) [10] | Zhao, W. (Zhao, W..) [11] | Sun, Y. (Sun, Y..) [12] | Xiong, H. (Xiong, H..) [13]

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Abstract:

The electrochemical reduction of CO2 to formate is an effective approach to achieving carbon neutrality. However, the instability of catalyst remains a significant limitation. Doping heteroatoms is a recognized method for tuning the coordination environment to enhance both electrochemical performance and stability. Herein, we report a facile and mild hydrothermal method employing sulfur doping to tune the coordination environment of bismuth active sites. Sulfur doping modifies the coordination environment of active sites by partially substituting O atoms bonded with bismuth active sites and simultaneously creating an abundance of oxygen vacancies, which effectively stabilize the active sites. This results in notably improved stability, reaching 110 h with a significant FEHCOOH (around 100 %). The bismuth-based catalyst modified with sulfur exhibits an impressive FEHCOOH over 95 % across a wide applied potential range of −0.7 to −1.4 VRHE. The flower-like structure increases the electrochemical surface area, promoting greater exposure of bismuth active sites. This leads to a high formate production rate of 1248 mmol∙h-1∙cm-2 for the Cu-BiS catalyst, which is 1.7 times that of the Cu-Bi catalyst. This strategy provides an effective way to tune the coordination environment of active sites and stabilize them. © 2024 Elsevier B.V.

Keyword:

Coordination environment Electroreduction Oxygen vacancy Sulfur doping

Community:

  • [ 1 ] [Duan X.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 2 ] [Duan X.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 3 ] [Xu J.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 4 ] [Xu J.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 5 ] [Cong Y.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 6 ] [Cong Y.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 7 ] [Geng H.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 8 ] [Chen K.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 9 ] [Chen K.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 10 ] [Xu T.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 11 ] [Xu T.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 12 ] [Zhang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 13 ] [Zhang F.]Institute for Advanced Study, Shenzhen University, Shenzhen, 518060, China
  • [ 14 ] [Zhang F.]Department of Chemistry, Colgate University, 13 Oak Drive, Hamilton, 13346, NY, United States
  • [ 15 ] [Zhu J.]Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800, China
  • [ 16 ] [Zhang L.]Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800, China
  • [ 17 ] [Zhao W.]Institute for Advanced Study, Shenzhen University, Shenzhen, 518060, China
  • [ 18 ] [Sun Y.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 19 ] [Sun Y.]Institute for Advanced Study, Shenzhen University, Shenzhen, 518060, China
  • [ 20 ] [Sun Y.]Shenzhen Research Institute of Xiamen University, Shenzhen, 518057, China
  • [ 21 ] [Xiong H.]State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • [ 22 ] [Xiong H.]Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen, 361102, China
  • [ 23 ] [Xiong H.]College of Energy, Xiamen University, Xiamen, 361102, China

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Source :

Chemical Engineering Journal

ISSN: 1385-8947

Year: 2024

Volume: 501

1 3 . 4 0 0

JCR@2023

Cited Count:

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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