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Tailoring Oxygen Reduction Reaction Kinetics of Fe-N-C Catalyst via Spin Manipulation for Efficient Zinc-Air Batteries.
Zhang, Huiwen; Chen, Hsiao-Chien; Feizpoor, Solmaz; Li, Linfeng; Zhang, Xia; Xu, Xuefei; Zhuang, Zechao; Li, Zhishan; Hu, Wenyu; Snyders, Rony; Wang, Dingsheng; Wang, Chundong.
Afiliación
  • Zhang H; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
  • Chen HC; Center for Reliability Science and Technologies, Center for Sustainability and Energy Technologies, Chang Gung University, Taoyuan, 33302, Taiwan.
  • Feizpoor S; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
  • Li L; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
  • Zhang X; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
  • Xu X; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
  • Zhuang Z; Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
  • Li Z; Faculty of Metallurgical and Energy Engineering, State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming, 650093, P. R. China.
  • Hu W; Department of Physics, Southern University of Science and Technology, ShenZhen, 518055, P. R. China.
  • Snyders R; Chimie des Interactions Plasma Surfaces (ChIPS), University of Mons, 7000 Mons, Belgium; Materia Nova Research Center, Mons, B-7000, Belgium.
  • Wang D; Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China.
  • Wang C; School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
Adv Mater ; 36(25): e2400523, 2024 Jun.
Article en En | MEDLINE | ID: mdl-38594481
ABSTRACT
The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the oxygen reduction reaction (ORR) kinetics. Herein, a new approach for boosting the inherent ORR activity of atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. The as-prepared catalyst delivers excellent ORR activity with half-wave potentials of 0.78 and 0.90 V in acidic and alkaline solutions, respectively. The decent ORR activity can also be validated from the high-performance rechargeable Zn-air battery. The experiments and density functional theory calculations reveal that the electron spin-state of monodispersed Fe active sites is transferred from the low spin (LS, t2g 6 eg 0) to the medium spin (MS, t2g 5 eg 1) due to the involvement of Fe atomic clusters, leading to the spin electron filling in σ∗ orbit, by which it favors OH- desorption and in turn boosts the reaction kinetics of the rate-determining step. This work paves a solid way for rational design of high-performance Fe-based single atom catalysts through spin manipulation.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article Pais de publicación: Alemania
Texto completo
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XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article Pais de publicación: Alemania