Single-Atom Catalysts with Unsaturated Co-N2 Active Sites Based on a C2N 2D-Organic Framework for Efficient Sulfur Redox Reaction

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,...

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Detalles Bibliográficos
Autores: Yang, Dawei|||0000-0002-3842-8286, Wang, Jiaao|||0000-0002-4944-4951, Lou, Chenjie, Li, Mengyao|||0000-0002-9082-7938, Zhang, Chaoqi|||0000-0002-0357-235X, Ramon, Alberto, Li, Canhuang, Tang, Mingxue|||0000-0002-7282-4100, Henkelman, Graeme|||0000-0002-0336-7153, Xu, Ming, Li, Junshan|||0000-0002-1482-1972, Llorca, Jordi|||0000-0002-7447-9582, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Mitlin, David, Zhou, Guangmin|||0000-0002-3629-5686, Cabot i Codina, Andreu|||0000-0002-7533-3251
Tipo de recurso: artículo
Fecha de publicación:2024
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:302102
Acceso en línea:https://ddd.uab.cat/record/302102
https://dx.doi.org/urn:doi:10.1021/acsenergylett.4c00771
Access Level:acceso abierto
Palabra clave: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
Descripción
Sumario: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.

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