journal article·2024-05-10Open access

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

Dawei Yang, Jiaao Wang, Chenjie Lou, Mengyao Li, Chaoqi Zhang, Alberto Ramon, Canhuang Li, Mingxue Tang, Graeme Henkelman, Ming Xu, Junshan Li, Jordi Llorca, Jordi Arbiol, David Mitlin, Guangmin Zhou, Andreu Cabot

ACS Energy Letters· Volume 9· Issue 5

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, C 2 N, with a high loading of low-coordination cobalt single atoms (Co-SAs/C 2 N) as an effective sulfur host in LSB cathodes. Experimental and computational results reveal that unsaturated Co–N 2 active sites with an asymmetric electron distribution act as effective polysulfide traps, accommodating electrons from polysulfide ions to form strong S x 2– –Co–N bonds. Additionally, charge transfer between LiPS and unsaturated Co–N 2 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/C 2 N-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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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advanced battery technologies research · Advancements in Battery Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Henan Province Key Laboratory of Photovoltaic Materials, School of Future Technology, Henan University, Kaifeng 475004, P. R. China

Catalonia Institute for Energy Research − IREC, Sant Adrià de Besòs, Barcelona 08930, Spain

Department of Chemistry and the Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, United States

Center for High Pressure Science and Technology Advanced Research, Beijing 100193, P. R. China

School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450052, P. R. China

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China

Institute for Advanced Study, Chengdu University, 610106 Chengdu, P. R. China

Institute of Energy Technologies, Department of Chemical Engineering and Barcelona Research Center in Multiscale Science and Engineering, Universitat Politècnica de Catalunya, EEBE, 08019 Barcelona, Spain

Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST Campus UAB, Bellaterra 08193, Barcelona, Spain

Materials Science and Engineering Program & Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States

Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen, International Graduate School, Tsinghua University, Shenzhen 518055, P. R. China

ICREA, Pg. Lluís Companys 23, 08010 Barcelona, Spain

Funding

European Commission · Ministerio de Ciencia e Innovación · European Regional Development Fund · Ministerio de Economía y Competitividad · Centres de Recerca de Catalunya · H2020 Research Infrastructures · Generalitat de Catalunya · China Scholarship Council · Universitat Autònoma de Barcelona · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China · Institució Catalana de Recerca i Estudis Avançats

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