Spin State Modulation via Magnetic Fields in Fe Single Atom Catalysts for High-Performance Aqueous Zinc–Sulfur Batteries

Dai, Penghao; Lang, Jian; Huang, Weiyuan; Ma, Lu; Zhao, Xueru; Lin, Xiaojing; Li, Qiang; Li, Hongpeng; Liu, Tongchao; Amine, Khalil; Li, Hongsen

doi:10.1021/acsnano.5c05185

Spin State Modulation via Magnetic Fields in Fe Single Atom Catalysts for High-Performance Aqueous Zinc–Sulfur Batteries

Journal Article · Thu May 29 00:00:00 EDT 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5c05185· OSTI ID:2570566

Dai, Penghao ^[1]; Lang, Jian ^[1]; Huang, Weiyuan ^[2]; Ma, Lu ^[3]; Zhao, Xueru ^[1]; Lin, Xiaojing ^[1]; ^[1]; ^[4]; ^[2]; ^[2]; ^[1]

Qingdao Univ. (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Yangzhou Univ., Jiangsu (China)

Aqueous zinc–sulfur battery has garnered significant attention as a high-energy, low-cost, and safe energy storage system. However, the multielectron transfer kinetics of sulfur cathodes are relatively slow, presenting challenges such as limited sulfur utilization and lower discharge voltage, which significantly hinder their practical applications. Here, in this study, we explored a comprehensive design approach for high-performance, long-cycle aqueous zinc–sulfur batteries. The simultaneous introduction of ZnI₂ and Fe single atoms (Fe-SAs) as catalytically active agents decouples the redox reactions, effectively facilitating ZnS oxidation and S reduction separately. The application of an external magnetic field regulates the spin state of Fe-SAs, further enhancing their catalytic activity and electron transfer capability. Electrochemical tests demonstrate that the S@Fe-NC HS/ZnI₂ cathode assembled under a magnetic field exhibits excellent rate performance, achieving an impressive specific capacity of 1399 mAh g^–1 at a high current density of 5 A g^–1 and good cycling stability over 300 cycles, representing the highest reported high-current discharge capacity to date. This study provides a comprehensive design framework for optimizing zinc–sulfur (Zn–S) battery performance and elucidates the influence of magnetic field-induced spin state modulation on catalytic behavior.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Excellent Youth Science Fund Project of Shandong China; National Natural Science Foundation of China (NSFC); Outstanding Youth Innovation Team of Universities in Shandong Province; Shandong Provincial Program for Enhancing Innovation Capacity of Technology-Based Small and Medium-Sized Enterprises; Taishan Scholar Project of Shandong Province; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2570566

Report Number(s):: BNL--228368-2025-JAAM

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 22 Vol. 19; ISSN 1936-086X; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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