Ferromagnetic Atomic d‐p Orbital Hybridization for Promoting Al‐S Batteries

Yu, Guobin; Liu, Xiaoya; Huang, Weiyuan; Wang, Shixin; Zhan, Jiqiang; Ma, Lu; Li, Hongpeng; Lin, Xiaojing; Liu, Tongchao; Amine, Khalil; Li, Hongsen

doi:10.1002/adma.202418784

Ferromagnetic Atomic d‐p Orbital Hybridization for Promoting Al‐S Batteries

Journal Article · Fri Apr 11 00:00:00 EDT 2025 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202418784· OSTI ID:2570563

Yu, Guobin ^[1]; Liu, Xiaoya ^[1]; Huang, Weiyuan ^[2]; Wang, Shixin ^[1]; Zhan, Jiqiang ^[1]; Ma, Lu ^[3]; Li, Hongpeng ^[4]; Lin, Xiaojing ^[1]; Liu, Tongchao ^[2]; ^[2]; Li, Hongsen ^[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)

Rechargeable aluminum‐sulfur batteries (Al‐S) are emerging as a promising alternative energy storage system beyond lithium‐ion batteries due to their high energy density, abundant material resources, and economic efficiency. However, their practical application remains challenged by sluggish conversion kinetics, polysulfide shuttling, and low sulfur cathode utilization. While extensive studies have focused on enhancing polysulfide adsorption through catalytic strategies, the roles of electronic structure in dictating catalytic performance remain underexplored. Here, this work unveils the critical effect of unpaired electronic structure on the catalytic performance of single atom ferromagnetic transition metals through a systematic evaluation of three typical atomically dispersed ferromagnetic single atoms—Fe, Co, and Ni—supported on porous carbon (denoted as PC‐SAFAs). Comprehensive characterizations and density functional theory (DFT) calculations reveal that the PC‐SAFe catalysts, exhibiting the highest spin polarization arising from unpaired electrons, demonstrate the strongest interactions with polysulfide, thereby facilitating rapid and reversible polysulfide conversion reactions. Consequently, Al‐S batteries incorporating the optimized PC‐SAFe cathode achieve an impressive specific capacity of 508.8 mAh g⁻¹ at 1.0 A g⁻¹ after 500 cycles, along with much improved rate capability. In conclusion, this work provides a deeper understanding of the role of electronic structure in catalytic chemistry, and offers new insights for developing high‐performance Al‐S batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: 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:: 2570563

Alternate ID(s):: OSTI ID: 2583988

Report Number(s):: BNL--228362-2025-JAAM

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 24 Vol. 37; ISSN 1521-4095; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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