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Research Article | Online first | Published: 15 May 2024

Electron delocalization-enhanced sulfur reduction kinetics on an MXene-derived heterostructured electrocatalyst

Show Author's Information Yunmeng Li1,  Yinze Zuo2,  Xiang Li1,  Yongzheng Zhang1( ),  Cheng Ma3,  Xiaomin Cheng4,  Jian Wang4,5,  Jitong Wang1( ),  Hongzhen Lin4,  Licheng Ling1( )
State Key Laboratory of Chemical Engineering, Key Laboratory of Specially Functional Polymeric Materials and Related Technology (Ministry of Education), East China University of Science and Technology, Shanghai 200237, China
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China
Key Laboratory of Specially Functional Polymeric Materials and Related Technology (Ministry of Education), School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
i-Lab & CAS Key Laboratory of Nanophotonic Materials and Device Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China
Helmholtz Institute Ulm (HIU), D89081 Ulm, Germany
Keywords:
lithium sulfur batteries, delocalized electron, MXene-based heterostructures, catalytic desolvation, multi-catalytic sites
Topics:
ElectrocatalystsLithium sulfur batteries
Cite this article:
Li Y, Zuo Y, Li X, et al. Electron delocalization-enhanced sulfur reduction kinetics on an MXene-derived heterostructured electrocatalyst. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6682-6
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Abstract Full text Electronic supplementary material About this article

Lithium-sulfur (Li-S) batteries mainly rely on the reversible electrochemical reaction of between lithium ions (Li+) and sulfur species to achieve energy storage and conversion, therefore, increasing the number of free Li+ and improving the Li+ diffusion kinetics will effectively enhance the cell performance. Here, Mo-based MXene heterostructure (MoS2@Mo2C) was developed by partial vulcanization of Mo2C MXene, in which the introduction of similar valence S into Mo-based MXene (Mo2C) can create an electron delocalization effect. Through theoretical simulations and electrochemical characterisation, it is demonstrated that the MoS2@Mo2C heterojunction can effectively promote ion desolvation, increase the amount of free Li+, and accelerate Li+ transport for more efficient polysulfide conversion. In addition, the MoS2@Mo2C material is also capable of accelerating the oxidation and reduction of polysulfides through its sufficient defects and vacancies to further enhance the catalytic efficiency. Consequently, the Li-S battery with the designed MoS2@Mo2C electrocatalyst performed for 500 cycles at 1 C and still maintained the ideal capacity (664.7 mAh·g−1), and excellent rate performance (567.6 mAh·g−1 at 5 C). Under the extreme conditions of high loading, the cell maintained an excellent capacity of 775.6 mAh·g−1 after 100 cycles. It also retained 838.4 mAh·g−1 for 70 cycles at a low temperature of 0 °C, and demonstrated a low decay rate (0.063%). These results indicate that the delocalized electrons effectively accelerate the catalytic conversion of lithium polysulfide, which is more practical for enhancing the behaviour of Li-S batteries.


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Abstract
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Electronic supplementary material
About this article

Electron delocalization-enhanced sulfur reduction kinetics on an MXene-derived heterostructured electrocatalyst

Show Author's information Yunmeng Li1, Yinze Zuo2, Xiang Li1, Yongzheng Zhang1( ), Cheng Ma3, Xiaomin Cheng4, Jian Wang4,5, Jitong Wang1( ), Hongzhen Lin4, Licheng Ling1( )
State Key Laboratory of Chemical Engineering, Key Laboratory of Specially Functional Polymeric Materials and Related Technology (Ministry of Education), East China University of Science and Technology, Shanghai 200237, China
Institute of New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China
Key Laboratory of Specially Functional Polymeric Materials and Related Technology (Ministry of Education), School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
i-Lab & CAS Key Laboratory of Nanophotonic Materials and Device Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China
Helmholtz Institute Ulm (HIU), D89081 Ulm, Germany

Abstract

Lithium-sulfur (Li-S) batteries mainly rely on the reversible electrochemical reaction of between lithium ions (Li+) and sulfur species to achieve energy storage and conversion, therefore, increasing the number of free Li+ and improving the Li+ diffusion kinetics will effectively enhance the cell performance. Here, Mo-based MXene heterostructure (MoS2@Mo2C) was developed by partial vulcanization of Mo2C MXene, in which the introduction of similar valence S into Mo-based MXene (Mo2C) can create an electron delocalization effect. Through theoretical simulations and electrochemical characterisation, it is demonstrated that the MoS2@Mo2C heterojunction can effectively promote ion desolvation, increase the amount of free Li+, and accelerate Li+ transport for more efficient polysulfide conversion. In addition, the MoS2@Mo2C material is also capable of accelerating the oxidation and reduction of polysulfides through its sufficient defects and vacancies to further enhance the catalytic efficiency. Consequently, the Li-S battery with the designed MoS2@Mo2C electrocatalyst performed for 500 cycles at 1 C and still maintained the ideal capacity (664.7 mAh·g−1), and excellent rate performance (567.6 mAh·g−1 at 5 C). Under the extreme conditions of high loading, the cell maintained an excellent capacity of 775.6 mAh·g−1 after 100 cycles. It also retained 838.4 mAh·g−1 for 70 cycles at a low temperature of 0 °C, and demonstrated a low decay rate (0.063%). These results indicate that the delocalized electrons effectively accelerate the catalytic conversion of lithium polysulfide, which is more practical for enhancing the behaviour of Li-S batteries.

Keywords: lithium sulfur batteries, delocalized electron, MXene-based heterostructures, catalytic desolvation, multi-catalytic sites

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Publication history

Received: 19 February 2024
Revised: 26 March 2024
Accepted: 03 April 2024
Published: 15 May 2024

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© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. U1710252), the Natural Science Foundation of Jiangsu Province (BK. 20210130), Innovative and Entrepreneurial Doctor in Jiangsu Province (No. JSSCBS20211428), China Postdoctoral Science Foundation (No. 2023M731084), Shanghai Sailing Program of China (No. 23YF1408900) and the Fundamental Research Funds for the Central Universities (No. JKD01231701). J. W. acknowledged the funding provided by the Alexander von Humboldt Foundation and the basic funding of the Helmholtz Association. Dr. Y. Z. Z. thanks the Shanghai Super Postdoctoral Incentive Program. We also thank the support from Nano-X, Suzhou Institute of Nano-tech and Nano-bionics, Chinese Academy of Sciences.

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