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Fluorine-doped Carbon Support Enables Superfast Oxygen Reduction Kinetics by Breaking the Scaling Relationship.
Liang, Jinhui; Liang, Lecheng; Zeng, Binwen; Feng, Binbin; Du, Li; Qiu, Xiaoyi; Wang, Yian; Song, Huiyu; Liao, Shijun; Shao, Minhua; Cui, Zhiming.
Afiliación
  • Liang J; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Liang L; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Zeng B; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Feng B; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Du L; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Qiu X; Hong Kong University of Science and Technology, Department of Chemical and Biological Engineering, HONG KONG.
  • Wang Y; The Hong Kong University of Science and Technology, Department of Chemical and Biological Engineering, HONG KONG.
  • Song H; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Liao S; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
  • Shao M; The Hong Kong University of Science and Technology, Chemical and Biomolecular Engineering, Clear Water Bay, Kowloon, Hong Kong, CHINA.
  • Cui Z; South China University of Technology, School of Chemistry and Chemical Engineering, CHINA.
Angew Chem Int Ed Engl ; : e202412825, 2024 Aug 09.
Article en En | MEDLINE | ID: mdl-39119836
ABSTRACT
It is well-established that Pt-based catalysts suffer from the unfavorable linear scaling relationship (LSR) between *OOH and *OH (ΔG(*OOH) = ΔG(*OH) + 3.2 ± 0.2 eV) for the oxygen reduction reaction (ORR), resulting in a great challenge to significantly reduced ORR overpotentials. Herein, we propose a universal and feasible strategy of fluorine-doped carbon supports, which optimize interfacial microenvironment of Pt-based catalysts and thus significantly enhance their reactive kinetics. The introduction of C-F bonds not only weakens the *OH binding energy, but also stabilizes the *OOH intermediate, resulting in a break of LSR. Furthermore, fluorine-doped carbon constructs a local super-hydrophobic interface that facilitates the diffusion of H2O and the mass transfer of O2. Electrochemical tests show that the F-doped carbon-supported Pt catalysts exhibit over 2-fold higher mass activities than those without F modification. More importantly, those catalysts also demonstrate excellent stability in both rotating disk electrode (RDE) and membrane electrode assembly (MEA) tests. This study not only validates the feasibility of tuning the electrocatalytic microenvironment to improve mass transport and to break the scaling relationship, but also provides a universal catalyst design paradigm for other gas-involving electrocatalytic reactions.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania