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Research Article

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

Yunmeng Li1Yinze Zuo2Xiang Li1Yongzheng Zhang1( )Cheng Ma3Xiaomin Cheng4Jian Wang4,5Jitong Wang1( )Hongzhen Lin4Licheng 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
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Graphical Abstract

The electron delocalized MXene planar heterojunction electrocatalyst (MoS2@Mo2C) effectively accelerated the desolvation process and increased the number of free Li+, significantly promoted the ion transfer and catalyzed the redox conversion of lithium polysulfides (LiPSs).

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.

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Nano Research
Pages 7153-7162
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, 17(8): 7153-7162. https://doi.org/10.1007/s12274-024-6682-6
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Received: 19 February 2024
Revised: 26 March 2024
Accepted: 03 April 2024
Published: 15 May 2024
© Tsinghua University Press 2024
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