Balancing Electronic Spin State via Atomically-Dispersed Heteronuclear Fe–Co Pairs for High-Performance Sodium–Sulfur Batteries
Room-temperature sodium-sulfur (Na-S) batteries are emerging as a promising next-generation energy storage technology, offering high energy densities at low cost and utilizing abundant elements. However, their practical application is hindered by the shuttle effect of sodium-polysulfides and the sluggish kinetics of sulfur redox reactions. In this study, we demonstrate a heteronuclear diatomic catalyst featuring Fe and Co bimetallic sites embedded in nitrogen-doped hollow carbon nanospheres (Fe-Co/NC) as an effective sulfur host at the cathode of Na-S batteries. Aberration-corrected high-angle annular dark field scanning transmission electron microscopy demonstrates the presence of isolated Fe-Co atomic pairs, while synchrotron radiation X-ray absorption fine structure analysis confirms the (Fe-Co-N<sub>6</sub>) coordination structure. Density functional theory calculations show that the introduction of Fe atoms induces electron delocalization in Co(II), shifting the electronic configuration from a low-spin to a higher-spin state. This shift enhances the hybridization of the Co dz<sup>2</sup> orbitals with the antibonding π orbitals of sulfur atoms within the sodium sulfide species that accelerates their catalytic conversion. As a result, Fe-Co/NC-based cathodes exhibit excellent cycling stability (378 mAh g<sup>-1</sup> after 2000 cycles) and impressive rate performance (341.1 mAh g<sup>-1</sup> under 5 A g<sup>-1</sup>).
Authors
- Dawei Yang (ORCID: https://orcid.org/0000-0002-3842-8286)
- Jordi Arbiol (ORCID: https://orcid.org/0000-0002-0695-1726)
- Sen Xin (ORCID: https://orcid.org/0000-0002-0546-0626)
- Canhuang Li (ORCID: https://orcid.org/0000-0002-9746-9483)
- Jing Yu (ORCID: https://orcid.org/0000-0002-0500-1980)
- Jiachen Ma (ORCID: https://orcid.org/0000-0002-5553-2464)
- Ruirui Zhao (ORCID: https://orcid.org/0000-0002-6016-5275)
- Yingtang Zhou (ORCID: https://orcid.org/0000-0002-8678-295X)
- Yuchuan Ren (ORCID: https://orcid.org/0000-0002-6870-4149)
- Junshan Li (ORCID: https://orcid.org/0000-0002-1482-1972)
- Andreu Cabot (ORCID: https://orcid.org/0000-0002-7533-3251)
- Ivan Pinto‐Huguet (ORCID: https://orcid.org/0000-0002-2275-4861)
- Chen Huang (ORCID: https://orcid.org/0000-0003-2934-8118)
- Xiaoyu Bi (ORCID: https://orcid.org/0000-0001-6428-5250)
- Yapeng Cheng (ORCID: https://orcid.org/0000-0002-9218-9095)
- Haining Zhang (ORCID: https://orcid.org/0000-0002-5546-2347)
- Hao Li (ORCID: https://orcid.org/0000-0002-7577-1366)
- Jian Wang (ORCID: https://orcid.org/0000-0002-7945-0826)
Institutions
- Institució Catalana de Recerca i Estudis Avançats (ES)
- Henan University (CN)
- South China Normal University (CN)
- Wuhan University of Technology (CN)
- Chinese Academy of Sciences (CN)
- Chemnitz University of Technology (DE)
- Zhejiang Ocean University (CN)
- Quantum (Australia) (AU)
- Institut Català de Nanociència i Nanotecnologia (ES)
- Beijing National Laboratory for Molecular Sciences (CN)
- Chengdu University (CN)
- Institut de Recerca en Energia de Catalunya (ES)
- Helmholtz-Institute Ulm (DE)
- Molecular Sciences Institute (US)
- Universitat de Barcelona (ES)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-02-28
- DOI
- https://doi.org/10.1021/jacs.4c15408
- Citations
- 59
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 43.10
Funders
- Ministerio de Ciencia, Innovación y Universidades
- Centres de Recerca de Catalunya
- National Natural Science Foundation of China
- Generalitat de Catalunya
- China Scholarship Council
- Natural Science Foundation of Sichuan Province
- Agencia Estatal de Investigación