School of Integrative Biological & Chemical Sciences Faculty Publications

Atomic d-d Orbital Coupling Drives Interfacial Spin-Related Electronic Redistribution for Accelerated Sulfur Redox Kinetics

Document Type

Article

Publication Date

7-2026

Abstract

Heteronuclear Ni-Co dual-atom catalysts anchored on nitrogen-doped carbon (NiCo DACs/NC) are constructed to clarify the relationship between intermetallic d-d orbital coupling and bidirectional sulfur redox kinetics in lithium-sulfur batteries. Combining spin-resolved density functional theory, spin-density mapping, and potential-dependent magnetic measurements, we demonstrate that d-oupling reconstructs the local 3d electronic structure, induces interfacial spin-related electronic redistribution, and undergoes reversible dynamic evolution during sulfur reduction and Li2S oxidation. This regulation enhances polysulfide conversion, Li─S bond activation, and Li2S nucleation/deposition as well as oxidation/decomposition. Consequently, the NiCo DACs/NC-based Li-S battery delivers a discharge capacity of 1129.6 mAh g−1 at 1C and retains 864.6 mAh g−1 after 500 cycles (0.034% decay per cycle). Under a high sulfur loading of 9.12 mg cm−2 and lean electrolyte (3.5 µL mg−1 an areal capacity of 7.69 mAh cm−2 is achieved. A pouch cell delivers a component-level energy density of 321.2 Wh kg−1 with 88.7% retention after 50 cycles. This work provides mechanistic insight into spin-related electronic dynamics for designing high-performance dual-atom catalysts in Li-S batteries.

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© 2026 Wiley-VCH GmbH.

https://advanced.onlinelibrary.wiley.com/share/CPV8IHN2SCTPXAUSTHCS?target=10.1002/adfm.76531

Publication Title

Advanced Functional Materials

DOI

10.1002/adfm.76531

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