articleACS CatalysisJun 16, 2022Closed access

Probing the Oxygen Reduction Reaction Intermediates and Dynamic Active Site Structures of Molecular and Pyrolyzed Fe–N–C Electrocatalysts by In Situ Raman Spectroscopy

JWJie WeiDXDongsheng XiaYWYinping WeiXZXuya ZhuJLJia Li

Tsinghua–Berkeley Shenzhen Institute · Tsinghua University

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Abstract

While FeN4 species are widely suggested as the active sites of noble-metal-free Fe–N–C oxygen reduction reaction (ORR) electrocatalysts, the ORR mechanism, particularly the rate-determining steps (RDSs) at the Fe centers, and the likely contribution of co-existed C–N active site remain disputed. Moreover, the dynamic structures of the FeN4 active sites during ORR electrocatalysis also remain elusive. By in situ (isotope-labeled) Raman spectroscopy of molecular Fe phthalocyanine (FePc) model catalysts and pyrolyzed Fe–N–C catalysts, we achieve direct, simultaneous spectral identification of the ORR intermediates/RDSs at different active sites under different pH conditions, from which their intrinsic activities…

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Topics & keywords

Topics
Keywords
  • Catalysis
  • Electrocatalyst
  • Chemistry
  • Raman spectroscopy
  • Active site
  • Oxygen reduction reaction
  • Pyrolysis
  • Reaction intermediate
UN Sustainable Development Goals
  • Clean water and sanitation
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