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Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres

Tang, Cheng ; Chen, Ling ; Li, Haijing ; Li, Laiquan ; Jiao, Yan ; Zheng, Yao ; Xu, Haolan ; Davey, Kenneth ; Qiao, Shi-Zhang

Journal of the American Chemical Society, 2021-05, Vol.143 (20), p.7819-7827 [Periódico revisado por pares]

United States: American Chemical Society

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  • Título:
    Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres
  • Autor: Tang, Cheng ; Chen, Ling ; Li, Haijing ; Li, Laiquan ; Jiao, Yan ; Zheng, Yao ; Xu, Haolan ; Davey, Kenneth ; Qiao, Shi-Zhang
  • É parte de: Journal of the American Chemical Society, 2021-05, Vol.143 (20), p.7819-7827
  • Notas: ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
  • Descrição: Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback is the limited understanding of actual catalytic active sites. Here, using as a prototype single-atom catalysts (SACs) in acidic oxygen reduction reaction (ORR), we report the structure–property relationship of catalysts and show for the first time that molecular-level local structure, including first and second coordination spheres (CSs), rather than individual active atoms, synergistically determines the electrocatalytic response. ORR selectivity on Co-SACs can be tailored from a four-electron to a two-electron pathway by modifying first (N or/and O coordination) and second (C–O–C groups) CSs. Using combined theoretical predictions and experiments, including X-ray absorption fine structure analyses and in situ infrared spectroscopy, we confirm that the unique selectivity change originates from the structure-dependent shift of active sites from the center Co atom to the O-adjacent C atom. We show this optimizes the electronic structure and *OOH adsorption behavior on active sites to give the present “best” activity and selectivity of >95% for acidic H2O2 electrosynthesis.
  • Editor: United States: American Chemical Society
  • Idioma: Inglês
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  • Realização: ABCD-USP USP   Logos de Redes Sociais: Freepik

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