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Recent progress and strategies of cathodes toward polysulfides shuttle restriction for lithium-sulfur batteries

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Abstract

Lithium-sulfur batteries (LSBs) have already developed into one of the most promising new-generation high-energy density electrochemical energy storage systems with outstanding features including high-energy density, low cost, and environmental friendliness. However, the development and commercialization path of LSBs still presents significant limitations and challenges, particularly the notorious shuttle effect triggered by soluble long-chain lithium polysulfides (LiPSs), which inevitably leads to low utilization of cathode active sulfur and high battery capacity degradation, short cycle life, etc. Substantial research efforts have been conducted to develop various sulfur host materials capable of effectively restricting the shuttle effect. This review firstly introduces the fundamental electrochemical aspects of LSBs, followed by a comprehensive analysis of the mechanism underlying the shuttle effect in Li–S batteries and its profound influence on various battery components as well as the overall battery performance. Subsequently, recent advances and strategies are systematically reviewed, including physical confinement, chemisorption, and catalytic conversion of sulfur hosts for restricting LiPSs shuttle effects. The interplay mechanisms of sulfur hosts and LiPSs are discussed in detail and the structural advantages of different host materials are highlighted. Furthermore, key insights for the rational design of advanced host materials for LSBs are provided, and the upcoming challenges and the prospects for sulfur host materials in lithium-sulfur batteries are also explored.

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摘要

锂硫电池（LSBs）由于具有高能量密度、低成本和环境友好等突出特点已发展成为最有前途的新一代高能量密度电化学储能系统之一。然而，LSBs 的发展和商业化道路仍然面临着巨大的限制和挑战，尤其是可溶性长链多硫化锂（LiPSs）引发的穿梭效应，不可避免地导致**极活性硫利用率低、电池容量衰减大、循环寿命短等问题。为了开发能够有效限制穿梭效应的各种硫主材料，研究人员进行了大量的研究工作。本综述首先介绍了 LSBs 的基本电化学方面，然后全面分析了锂-硫电池中穿梭效应的机制及其对各种电池组件和电池整体性能的深远影响。随后，系统回顾了相关最**的研究进展和策略，包括物理限制，化学吸附，和硫宿主的催化转化限制LiPSs穿梭效应。详细讨论了硫和LiPSs的相互作用机理，**调了不同宿主材料的结构优势。此外，还为合理设计先进的锂-硫电池**极宿主材料提供了关键见解，并探讨了锂硫电池中硫主体材料即将面临的挑战和前景。

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Fig. 1

(Source: Web of Science Core Collection, with search results: (“lithium sulfur batteries” or “Li–S batteries” or “LSBs”) and (“Shuttle effect” or “polysulfide shuttling” or “shuttle”), retrieved June 26, 2023)

Fig. 2
Fig. 3

Reproduced with permission from Ref. [35]. Copyright 2020, Wiley–VCH. b Polysulfide shuttle effect in lithium-sulfur batteries. Reproduced with permission from Ref. [36]. Copyright 2015, Royal Society of Chemistry

Fig. 4

Reproduced with permission from Ref. [74]. Copyright 2012, Wiley–VCH. b Schematic illustration of AGNs@S composites confining polysulfides and undergoing electrochemical reactions. Reproduced with permission from Ref. [75]. Copyright 2013, Royal Society of Chemistry. c Synthesis of F-GS@S sandwich composites. Reproduced with permission from Ref. [76]. Copyright 2020, IOP Publishing Ltd. d Graphite chemically modified to graphene, where CMG is chemically modified graphite, EG is edge-cleaved graphite. Reproduced with permission from Ref. [81]. Copyright 2016, Wiley–VCH

Fig. 6

Reproduced with permission from Ref. [86]. Copyright 2017, Wiley–VCH. c Calculated binding energy of Li2S with various functional groups (R) in context of vinyl polymers -(CH2-CHR)n-; d ab initio simulations investigating Li2S binding configurations and energies with various R groups in vinyl polymers and Li–O interaction between Li2S and >C=O groups. Reproduced with permission from Ref. [93]. Copyright 2013, Royal Society of Chemistry

Fig. 7

Reproduced with permission from Ref. [94]. Copyright 2013, Royal Society of Chemistry. c Voltage profiles of DIXPS and DIXDS during cycling at 0.1C (1C = 672 mA·g−1 for DIXPS; 1C = 198 mA·g−1 for DIXDS); d cyclic voltammograms (CV) of the initial cycle for DIXPS and DIXDS at a scanning rate of 0.05 mV·s−1. Reproduced with permission from Ref. [100]. Copyright 2020, Wiley–VCH. e Synthesis process of phenyl polysulfide. Reproduced with permission from Ref. [101]. Copyright 2018, American Chemical Society. f Synthesis process and proposed chemical structure of STI. Reproduced with permission from Ref. [117]. Copyright 2019, Elsevier. d Preparation of TCD-TCS and TCD-TCS/S and evolution of active materials during discharge process for e conventional C/S cathodes and f TC-100/S cathodes; g XPS spectra of discharge products for TC-100 at DoD of 72% and 100%; h charge–discharge voltage curves of TC-60/S, TC-80/S, and TC-100/S electrodes at an areal loading of 1.8 mg·cm−2. Reproduced with permission from Ref. [129]. Copyright 2021, MDPI

Fig. 10

Reproduced with permission from Ref. [142]. Copyright 2019, American Chemical Society. g Spatial charge density of SATi and Li2S, illustrating distinctive d-orbital and p-orbital distribution pattern, highlighting d-p orbital hybridization scenario between SAC and Li2S; h SAC-S and Li–S bond strengths in (Li2S)8-SAC adsorption system assessed by integrated-COHP (–ICOHP) and (inset) adsorption structure; i energy barrier for delithiation during oxidation process of (Li2S)8. Reproduced with permission from Ref. [147]. Copyright 2021, Wiley–VCH

Fig. 11

Reproduced with permission from Ref. [158]. Copyright 2020, Wiley–VCH. f Free energy change of Li2S nucleation; current response during PITT testing at constant potentials of g 2.0 V during discharge and h 2.4 V during charge; i schematic illustration of a unidirectional catalyst with a single type of defect (DN or VSe), and a bidirectional catalyst combining both DN and VSe; j operando Raman spectra of S@N-MoSe2-x/C electrode electrolyte during the initial cycle at a scan rate of 0.2 mV·s−1. Reproduced with permission from Ref. [161]. Copyright 2020, Wiley–VCH

Fig. 12

Reproduced with permission from Ref. [163]. Copyright 2021, Wiley–VCH. e Proposed redox reaction pathways for LSBs based on sulfur-vacancy heterojunction materials; f excessive adsorption of liquid-phase LiPSs on traditional Co9S8/MoS2 heterostructure (orange-yellow liquid spheres of Co9S8); g coordination of chemisorption and catalytic conversion achieved by introducing sulfur vacancies in Co9S8/MoS2 heterostructure; h CV curves of CMG-H at various sweep rates within voltage range of 1.6–2.8 V. Reproduced with permission from Ref. [165]. Copyright 2022, Royal Society of Chemistry

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 52105575 & 52205593), the Fundamental Research Funds for the Central Universities (No. QTZX23063), the Proof of Concept Foundation of **dian University Hangzhou Institute of Technology (Nos. GNYZ2023YL0302 & GNYZ2023QC0401), and the Aeronautical Science Foundation of China (No. 2022Z073081001).

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  1. **ng-You Rao and Shuang-Fei **ang have contributed equally to this work.

Authors and Affiliations

  1. School of Energy Sciences and Engineering, Nan**g Tech University, Nan**g, 211816, China

    **ng-You Rao, Jian Zhou, Zhen Zhang, **ang-Yu Xu, Yuan-Yuan Xu, **n-Chi Zhou, Zheng-Dao Pan, Su-Chong Tan, Zhou-Lu Wang, Yu-Tong Wu, **ang Liu & Yi Zhang

  2. School of Materials Science and Engineering and Institute of Smart Fiber Materials, Zhejiang Sci-Tech University, Hangzhou, 310018, China

    Shuang-Fei **ang

  3. JiangSu Sailboat Petrochemical Co.,Ltd, Lianyungang, 222000, China

    Shi-**ng Dong

  4. Hangzhou Institute of Technology, **dian University, Hangzhou, 311200, China

    Yun-Lei Zhou & Shan Jiang

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Rao, XY., **ang, SF., Zhou, J. et al. Recent progress and strategies of cathodes toward polysulfides shuttle restriction for lithium-sulfur batteries. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02708-7

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