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Research Article

High-density/efficient surface active sites on modified separators to boost Li-S batteries via atomic Co3+-Se termination

Shujie Liu1,2,§, Xiaofei Liu1,§, Manfang Chen3, Dong Wang4( ), Xin Ge1, Wei Zhang1, Xiyang Wang5, Chunhui Wang6, Tingting Qin1, Haozhe Qin6, Liang Qiao2, Dan Zhang3, Xing Ou6( ), Weitao Zheng1( )
Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun 130013, China
Key Laboratory of Materials Design and Quantum Simulation, College of Science, Changchun University, Changchun 130022, China
National Base for International Science & Technology Cooperation, School of Chemistry, Xiangtan University, Xiangtan 411105, China
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
Department of Mechanical and Mechatronics Engineering, University of Waterloo, Waterloo, N2L 3G1, Canada
School of Metallurgy and Environment, Central South University, Changsha 410083, China

§ Shujie Liu and Xiaofei Liu contributed equally to this work.

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Graphical Abstract

Single-crystal CoSe2 can exhibit three types of terminated (011) facet, efficiently obtaining the surface with a high-rich Co3+–Se bond termination, in contrast with lots of surface grain boundaries and dangling bonds in polycrystalline CoSe2. As anticipated, it can provide high-density and high-efficient active sites, enormously suppressing the shuttle effect and improving the reaction kinetics via accelerating the conversion and deposition of polysulfides and Li2S during long-term charge/discharge process.

Abstract

Various and critical electrocatalytic processes are involved during the redox reactions in the Li-S batteries, which extremely depend on the surface structure and chemical state. Recently, single-atom concept unlocks a route to maximize the use of surface-active atoms, however, further increasing the density of active site is still strictly limited by the inherent structure that single-atoms are only highly-dispersed on substrate. Herein, we provide a viewpoint that an elaborate facet design with single-crystalline structure engineering can harvest high-density surface active sites, which can significantly boost the electrocatalyst performance for excellent Li-S batteries. Specifically, the single-crystal CoSe2 (scCS) exhibits three-types of terminated (011) facet, efficiently obtaining the surface with a high-rich Co3+–Se bond termination, in contrast with lots of surface grain boundaries and dangling bonds in polycrystalline CoSe2. Surprisingly, the surface active sites concentration can reach more than 69%. As anticipated, it can provide high-density and high-efficient active sites, enormously suppressing the shuttle effect and improving the reaction kinetics via accelerating the conversion and deposition of polysulfides and Li2S. This surface lattice strategy with element terminated mode is a promising approach for designing electrocatalyst effect-based energy system, not merely for Li-S batteries.

Keywords

high-density surface active sitesCo3+–Se covalent bond atomic element terminatedLi-S batteriessingle-crystalline strategy

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Nano Research
Volume 15 Issue 8,
August 2022
Pages 7199-7208
DOI: 10.1007/s12274-022-4381-8
Cite this article:
Liu S, Liu X, Chen M, et al. High-density/efficient surface active sites on modified separators to boost Li-S batteries via atomic Co3+-Se termination. Nano Research, 2022, 15(8): 7199-7208. https://doi.org/10.1007/s12274-022-4381-8
Topics:
Lithium sulfur batteries

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Received: 04 March 2022
Revised: 31 March 2022
Accepted: 31 March 2022
Published: 31 May 2022
© Tsinghua University Press 2022
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