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Direct Oxygen-Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single-atom Electrocatalysts for Efficient Oxygen Reduction Reaction.
Xie, Yuhan; Chen, Xin; Sun, Kaian; Zhang, Jinqiang; Lai, Wei-Hong; Liu, Hao; Wang, Guoxiu.
Afiliación
  • Xie Y; Center for Clean Energy Technology, School of Mathematical and Physical Science, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, 2007, Australia.
  • Chen X; Beijing Advanced Innovation Center for Materials Genome Engineering, Institute of Solid State Chemistry, University of Science and Technology Beijing, Beijing, 100083, China.
  • Sun K; Department of Chemistry, Tsinghua University, Beijing, 100084, China.
  • Zhang J; Center for Clean Energy Technology, School of Mathematical and Physical Science, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, 2007, Australia.
  • Lai WH; Institute for Superconducting & Electronic Materials, University of Wollongong, Innovation Campus, Wollongong, New South Wales, 2500, Australia.
  • Liu H; Center for Clean Energy Technology, School of Mathematical and Physical Science, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, 2007, Australia.
  • Wang G; Center for Clean Energy Technology, School of Mathematical and Physical Science, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, 2007, Australia.
Angew Chem Int Ed Engl ; 62(17): e202301833, 2023 Apr 17.
Article en En | MEDLINE | ID: mdl-36853880
The oxygen reduction reaction (ORR) on transition single-atom catalysts (SACs) is sustainable in energy-conversion devices. However, the atomically controllable fabrication of single-atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O-O cleavage pathway through using a bi-functional ligand-assisted strategy to pre-control the distance of hetero-metal atoms. Concretely, the as-synthesized Fe-Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half-wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe-Zn diatomic pairs with a specific distance range of around 3 Å, which is the key to their ultrahigh activity, average the interaction between hetero-diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Australia Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Australia Pais de publicación: Alemania