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

Zhang，Huiwen1; Chen，Hsiao Chien2; Feizpoor，Solmaz1; Li，Linfeng1; Zhang，Xia1; Xu，Xuefei1; Zhuang，Zechao3; Li，Zhishan4; Hu，Wenyu5; Snyders，Rony6; Wang，Dingsheng3; Wang，Chundong1

2024-06-20

10.1002/adma.202400523

Advanced Materials   影响因子和分区

0935-9648

1521-4095

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 e) to the medium spin (MS, t e) 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.

Fe─N─C oxygen reduction reaction reaction kinetics spin-state transition zinc–air batteries

SCI ; EI

英语

其他

MATERIALS SCIENCE

2-s2.0-85190389920

Scopus

1.School of Integrated Circuits,Wuhan National Laboratory for Optoelectronics,Huazhong University of Science and Technology,Wuhan,430074,China
2.Center for Reliability Science and Technologies,Center for Sustainability and Energy Technologies,Chang Gung University,Taoyuan,33302,Taiwan
3.Department of Chemistry,Tsinghua University,Beijing,100084,China
4.Faculty of Metallurgical and Energy Engineering,State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization,Kunming University of Science and Technology,Kunming,650093,China
5.Department of Physics,Southern University of Science and Technology,ShenZhen,518055,China
6.Chimie des Interactions Plasma Surfaces (ChIPS),University of Mons,7000 Mons,Belgium; Materia Nova Research Center,Mons,B-7000,Belgium

Zhang，Huiwen,Chen，Hsiao Chien,Feizpoor，Solmaz,等. Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries[J]. Advanced Materials,2024,36(25).

Zhang，Huiwen.,Chen，Hsiao Chien.,Feizpoor，Solmaz.,Li，Linfeng.,Zhang，Xia.,...&Wang，Chundong.(2024).Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries.Advanced Materials,36(25).

Zhang，Huiwen,et al."Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries".Advanced Materials 36.25(2024).