Inducing Fe 3d Electron Delocalization and Spin-State Transition of FeN4 Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery

Chen，Shengmei1; Liang，Xiongyi1; Hu，Sixia2; Li，Xinliang1; Zhang，Guobin4; Wang，Shuyun1; Ma，Longtao3; Wu，Chi Man Lawrence1; Zhi，Chunyi1; Zapien，Juan Antonio1

2023-12-01

10.1007/s40820-023-01014-8

Nano-Micro Letters   Impact Factor & Quartile

2311-6706

2150-5551

Abstract: Transition metal–nitrogen–carbon materials (M–N–Cs), particularly Fe–N–Cs, have been found to be electroactive for accelerating oxygen reduction reaction (ORR) kinetics. Although substantial efforts have been devoted to design Fe–N–Cs with increased active species content, surface area, and electronic conductivity, their performance is still far from satisfactory. Hitherto, there is limited research about regulation on the electronic spin states of Fe centers for Fe–N–Cs electrocatalysts to improve their catalytic performance. Here, we introduce TiC MXene with sulfur terminals to regulate the electronic configuration of FeN species and dramatically enhance catalytic activity toward ORR. The MXene with sulfur terminals induce the spin-state transition of FeN species and Fe 3d electron delocalization with d band center upshift, enabling the Fe(II) ions to bind oxygen in the end-on adsorption mode favorable to initiate the reduction of oxygen and boosting oxygen-containing groups adsorption on FeN species and ORR kinetics. The resulting FeN–TiCS exhibits comparable catalytic performance to those of commercial Pt-C. The developed wearable ZABs using FeN–TiCS also exhibit fast kinetics and excellent stability. This study confirms that regulation of the electronic structure of active species via coupling with their support can be a major contributor to enhance their catalytic activity. [Figure not available: see fulltext.].

Fe 3d electron delocalization Oxygen reduction reaction Spin-state transition Wearable zinc–air batteries

SCI

English

Others

Grant of the Innovation and Technology Commission of Hong Kong[ITS/461/18] ; City University of Hong Kong[9678179]

Science & Technology - Other Topics ; Materials Science ; Physics

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied

WOS:000935642000001

SHANGHAI JIAO TONG UNIV PRESS

2-s2.0-85148237871

Scopus

1.Department of Materials Science and Engineering,City University of Hong Kong,999077,Hong Kong
2.Sustech Core Research Facilities,Southern University of Science and Technology,Shenzhen,1088 Xueyuan Blvd, Guangdong,518055,China
3.Frontiers Science Center for Flexible Electronics,Institute of Flexible Electronics,Northwestern Polytechnical University,Xi’an,710072,China
4.Tsinghua Shenzhen International Graduate School,Tsinghua University,Shenzhen, Guangdong, 518055,China

Chen，Shengmei,Liang，Xiongyi,Hu，Sixia,等. Inducing Fe 3d Electron Delocalization and Spin-State Transition of FeN4 Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery[J]. Nano-Micro Letters,2023,15(1).

Chen，Shengmei.,Liang，Xiongyi.,Hu，Sixia.,Li，Xinliang.,Zhang，Guobin.,...&Zapien，Juan Antonio.(2023).Inducing Fe 3d Electron Delocalization and Spin-State Transition of FeN4 Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery.Nano-Micro Letters,15(1).

Chen，Shengmei,et al."Inducing Fe 3d Electron Delocalization and Spin-State Transition of FeN4 Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery".Nano-Micro Letters 15.1(2023).