Tailoring Oxygen Reduction Reaction Kinetics of Fe-N-C Catalyst via Spin Manipulation for Efficient Zinc-Air Batteries.

Autor: 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.
Jazyk: angličtina
Zdroj: Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2024 Jun; Vol. 36 (25), pp. e2400523. Date of Electronic Publication: 2024 Apr 16.
DOI: 10.1002/adma.202400523
Abstrakt: 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, t 2g 6 e g 0 ) to the medium spin (MS, t 2g 5 e g 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.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
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