Enhanced lithium polysulfide adsorption and reaction with cobalt-doped spinel additives for robust lithium-sulfur batteries
Chacón Borrero, Jesús (Institut de Recerca en Energia de Catalunya)
Qi, Xuede (Chongqing University of Technology. College of Chemistry and Chemical Engineering)
Zhang, Xuesong (Institut de Ciència de Materials de Barcelona)
Berlanga-Vázquez, Armando (Institut de Recerca en Energia de Catalunya)
Chang, Xingqi (Universitat de Barcelona. Facultat de Química)
Montaña-Mora, Guillem (Institut de Recerca en Energia de Catalunya)
Mejía-Centeno, Karol V. (Universitat de Barcelona. Facultat de Química)
Rabelo Freitas, Helena (Institut Català de Nanociència i Nanotecnologia)
Spadaro, Maria Chiara (Institut Català de Nanociència i Nanotecnologia)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)
Llorca, Jordi (Universitat Politècnica de Catalunya. Centre de Recerca en Ciencia i Enginyeria Multiescala de Barcelona)
Guardia, Pablo (Institut de Ciència de Materials de Barcelona)
Qi, Xueqiang (Chongqing University of Technology. College of Chemistry and Chemical Engineering)
Zhang, Chao Yue (Lanzhou University. School of Physical Science & Technology China)
Cabot, Andreu (Institut de Recerca en Energia de Catalunya)

Date:	2025
Abstract:	Sulfur-based cathodes offer a promising high-energy-density alternative to conventional lithium-ion batteries. However, their commercial viability is hindered by limited stability due to the gradual loss of active sulfur during cycling. This study addresses this challenge by introducing a cobalt-doped spinel oxide as a catalytic additive, designed to enhance the performance and stability of sulfur cathodes with minimized cobalt usage. Small amounts of cobalt doping improve the adsorption of sulfur species through stronger electronic interactions with antibonding orbitals and accelerate charge transfer, thereby promoting more efficient sulfur redox reactions. Cobalt also lowers the energy barrier for LiS formation, a critical step in the cycling process. Specifically, Co-doped MnFeO with 2. 4 wt % Co demonstrates a remarkable initial capacity of 1302 mAh/g at 0. 1C, excellent rate capability with 700 mAh/g at 4C, and stable cycling performance with an average capacity decay of just 0. 03 % per cycle at 0. 5C over 200 cycles. Overall, this work underscores the potential of cobalt-doped spinel structures as catalytic additives to mitigate the limitations of sulfur cathodes, paving the way for more stable and high-performance lithium-sulfur batteries.
Grants:	Agencia Estatal de Investigación CEX2023-001300-M Agencia Estatal de Investigación PID2023-149158OB-C43 Agencia Estatal de Investigación PID2022-136883OB-C22 Agencia Estatal de Investigación CEX2021-001214-S Agencia Estatal de Investigación PID2021-124572OB-C31 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-01061
Note:	Altres ajuts: this study is part of the Advanced Materials program and was supported by MCIN with funding from the European Union Next Generation EU (PRTR-C17.I1) and by Generalitat de Catalunya (In-CAEM Project). ICN2 is funded by the CERCA Program / Generalitat de Catalunya.
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.
Language:	Anglès
Document:	Article ; recerca ; Versió acceptada per publicar
Subject:	Lithium-sulfur battery ; Spinel structure ; Cobalt doping ; Lithium polysulfide
Published in:	Energy storage materials, Vol. 77 (April 2025) , art. 104207, ISSN 2405-8297

DOI: 10.1016/j.ensm.2025.104207

Available from: 2027-04-30 Postprint

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Research literature > UAB research groups literature > Research Centres and Groups (research output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
Articles > Research articles
Articles > Published articles