Single-Atom Catalysts with Unsaturated Co-N2 Active Sites Based on a C2N 2D-Organic Framework for Efficient Sulfur Redox Reaction
Yang, Dawei (Institut de Recerca en Energia de Catalunya)
Wang, Jiaao (The University of Texas at Austin. Oden Institute for Computational Engineering and Sciences)
Lou, Chenjie (Center for High Pressure Science and Technology Advanced Research (China))
Li, Mengyao (Zhengzhou University)
Zhang, Chaoqi (Institut de Recerca en Energia de Catalunya)
Ramon, Alberto (Institut de Recerca en Energia de Catalunya)
Li, Canhuang (Institut de Recerca en Energia de Catalunya)
Tang, Mingxue (Center for High Pressure Science and Technology Advanced Research (China))
Henkelman, Graeme (The University of Texas at Austin. Oden Institute for Computational Engineering and Sciences)
Xu, Ming (Beijing University of Chemical Technology)
Li, Junshan (Chengdu University. Institute for Advanced Study)
Llorca, Jordi (Universitat Politècnica de Catalunya. Centre de Recerca en Ciencia i Enginyeria Multiescala de Barcelona)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)
Mitlin, David (The University of Texas at Austin. Texas Materials Institute)
Zhou, Guangmin (Tsinghua University. Shenzhen Geim Graphene Center)
Cabot i Codina, Andreu (Institut de Recerca en Energia de Catalunya)

Date:	2024
Abstract:	The lithium-sulfur battery (LSB) is a viable option for the next generation of energy storage systems. However, the shuttle effect of lithium polysulfides (LiPS) and the poor electrical conductivity of sulfur and lithium sulfides limit its deployment. Here, we report on a 2D-organic framework, C2N, with a high loading of low-coordination cobalt single atoms (Co-SAs/C2N) as an effective sulfur host in LSB cathodes. Experimental and computational results reveal that unsaturated Co-N2 active sites with an asymmetric electron distribution act as effective polysulfide traps, accommodating electrons from polysulfide ions to form strong Sx2--Co-N bonds. Additionally, charge transfer between LiPS and unsaturated Co-N2 active sites endows immobilized LiPS with low free energy and low electrochemical decomposition energy barriers, thus accelerating the kinetic conversion of LiPS. As a result, S@Co-SAs/C2N-based cathodes exhibit superior rate performance, impressive cycling stability, and good areal capacity at high sulfur loading, 2-fold that of commercial lithium-ion batteries. This work emphasizes the potential capabilities and promising prospects of single-atom catalysts with unsaturated coordination in LSBs.
Grants:	Agencia Estatal de Investigación ENE2016-77798-C4-3-R Agencia Estatal de Investigación PID2020-116093RB-C43 Ministerio de Ciencia e Innovación CEX2021-001214-S Agencia Estatal de Investigación PID2021-124572OB-C31 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-01061 European Commission 823717 Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-00457
Rights:	Aquest material està protegit per drets d'autor i/o drets afins. Podeu utilitzar aquest material en funció del que permet la legislació de drets d'autor i drets afins d'aplicació al vostre cas. Per a d'altres usos heu d'obtenir permís del(s) titular(s) de drets.
Language:	Anglès
Document:	Article ; recerca ; Versió acceptada per publicar
Subject:	2D organic framework (C2N) ; Co-N2 active sites ; Single-atom catalysts ; Catalytic conversion ; Lithium-sulfur batteries ; Active site ; Electrical conductivity ; High loadings ; Low coordination ; Organics ; Polysulphides ; Single-atoms ; Storage systems ; ]+ catalyst
Published in:	ACS energy letters, Vol. 9, Issue 5 (May 2024) , p. 2083-2091, ISSN 2380-8195

DOI: 10.1021/acsenergylett.4c00771

Postprint 38 p, 1.7 MB

The record appears in these collections:
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