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Promoting electrocatalytic CO2 reduction to CO via Sulfur-Doped Co-N-C Single-Atom Catalyst
  • +3
  • Zhiming Wei,
  • Yuhang Liu,
  • Jie Ding,
  • Qinye He,
  • Qiao Zhang,
  • Yueming Zhai
Zhiming Wei
Wuhan University
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Yuhang Liu
Suzhou University of Science and Technology
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Jie Ding
Wuhan University
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Qinye He
Wuhan University
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Qiao Zhang
Wuhan University
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Yueming Zhai
Wuhan University

Corresponding Author:[email protected]

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Abstract

Electrocatalytic reduction of CO2 to fuels and chemicals possesses huge potential to alleviate current environmental crisis. Heteroatom doping in metal-nitrogen-carbon (M-N-C) single-atom catalysts (SACs) has been found capable to promote the electrocatalytic CO2 reduc-tion reaction (CO2RR). However, the origin of the enhanced activity is still elusive. Here, we report that sulfur-doped cobalt-nitrogen-carbon single-atom catalyst (Co1-SNC) exhibits superior CO2RR performance compared to sulfur-free counterpart (Co1-NC). On the basis of in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), kinetic isotope effect (KIE) and theoretical calculation, it is demonstrated that sulfur doping can promote water activation, elevate the d-band center of Co active site, and reduce the free energy of *COOH intermediate formation. This work deepens the understanding of the CO2RR chemistry over heteroatom-doped SACs for designing efficient CO2RR processes.
20 Jul 20231st Revision Received
21 Jul 2023Submission Checks Completed
21 Jul 2023Assigned to Editor
21 Jul 2023Review(s) Completed, Editorial Evaluation Pending
23 Jul 2023Reviewer(s) Assigned
11 Aug 2023Editorial Decision: Accept