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Elaboration of Aggregated Polysulfide Phases: From Molecules to Large Clusters and Solid Phases

Cite this: Nano Lett. 2019, 19, 10, 7487–7493
Publication Date (Web):September 11, 2019
https://doi.org/10.1021/acs.nanolett.9b03297
Copyright © 2019 American Chemical Society

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    Abstract

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    With the increasing strategies aimed at repressing shuttle problems in the lithium–sulfur battery, dissolved contents of polysulfides are significantly reduced. Except for solid-state Li2S2 and Li2S, aggregated phases of polysulfides remain unexplored, especially in well confined cathode material systems. Here, we report a series of nanosize polysulfide clusters and solid phases from an atomic perspective. The calculated phase diagram and formation energy evolution process demonstrate their stabilities and cohesive tendency. It is interesting to find that Li2S6 can stay in the solid state and contains short S3 chains, further leading to the unique stability and dense structure. Simulated electronic properties indicate reduced band gaps when polysulfides are aggregated, especially for solid phase Li2S6 with a band gap as low as 0.47 eV. Their dissolution behavior and conversion process are also investigated, which provides a more realistic model and gives further suggestions on the future design of the lithium–sulfur battery.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.9b03297.

    • Detailed description of computational methods; Geometric structures, dynamic stabilities and electronic structure of polysulfide clusters and solid phases; Additional simulations for dissolved polysulfides in DOL and DME electrolyte; Simulated Raman spectra; Binding strength of graphene toward different phases of polysulfides (PDF)

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    Cited By

    This article is cited by 12 publications.

    1. Jinhao Zhang, Qingshan Fu, Peng Li, Ruibo Linghu, Xiaozhong Fan, Haibin Lin, Juncao Bian, Songbai Han, Gengzhi Sun, Long Kong. Lithium polysulfide solvation and speciation in the aprotic lithium-sulfur batteries. Particuology 2024, 89 , 238-245. https://doi.org/10.1016/j.partic.2023.11.006
    2. Yi Guo, Qian Niu, Fei Pei, Qian Wang, Yun Zhang, Liyu Du, Yin Zhang, Yunsheng Zhang, Yueying Zhang, Ling Fan, Qianyu Zhang, Lixia Yuan, Yunhui Huang. Interface engineering toward stable lithium–sulfur batteries. Energy & Environmental Science 2024, 17 (4) , 1330-1367. https://doi.org/10.1039/D3EE04183B
    3. Chao Ye, Jieqiong Shan, Huan Li, Chun‐Chuan Kao, Qinfen Gu, Shi‐Zhang Qiao. Reducing Overpotential of Solid‐State Sulfide Conversion in Potassium‐Sulfur Batteries. Angewandte Chemie 2023, 135 (22) https://doi.org/10.1002/ange.202301681
    4. Chao Ye, Jieqiong Shan, Huan Li, Chun‐Chuan Kao, Qinfen Gu, Shi‐Zhang Qiao. Reducing Overpotential of Solid‐State Sulfide Conversion in Potassium‐Sulfur Batteries. Angewandte Chemie International Edition 2023, 62 (22) https://doi.org/10.1002/anie.202301681
    5. Tianshuai Wang, Xiang Feng, Chao Lin, Qianfan Zhang. Rational design of the cathode catalysts for high performance lithium–sulfur batteries. Chemical Physics Reviews 2023, 4 (1) https://doi.org/10.1063/5.0110449
    6. Xiang Feng, Qianfan Zhang, Zhi Wei Seh. Toward Automated Computational Discovery of Battery Materials. Advanced Materials Technologies 2023, 8 (3) https://doi.org/10.1002/admt.202200616
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    8. Tong Shi, Huiqing Guo, Yue Liu, Long Wang, Yanqiu Lei, Haigang Hao, fenrong liu. Dft Combined with Xanes to Investigate the Sulfur Fixation Mechanisms of H2s on Different Cao Surfaces. SSRN Electronic Journal 2022, 154 https://doi.org/10.2139/ssrn.4045358
    9. Zhiyuan Han, Shiyong Zhao, Jiewen Xiao, Xiongwei Zhong, Jinzhi Sheng, Wei Lv, Qianfan Zhang, Guangmin Zhou, Hui‐Ming Cheng. Engineering d‐p Orbital Hybridization in Single‐Atom Metal‐Embedded Three‐Dimensional Electrodes for Li–S Batteries. Advanced Materials 2021, 33 (44) https://doi.org/10.1002/adma.202105947
    10. Yongliang Cui, Sufu Liu, Donghuang Wang, Xiuli Wang, Xinhui Xia, Changdong Gu, Jiangping Tu. A Facile Way to Construct Stable and Ionic Conductive Lithium Sulfide Nanoparticles Composed Solid Electrolyte Interphase on Li Metal Anode. Advanced Functional Materials 2021, 31 (3) https://doi.org/10.1002/adfm.202006380
    11. Sanket Bhoyate, Junyoung Kim, Eunho Lee, Bumsu Park, Eunji Lee, Juhong Park, Sang Ho Oh, Jeongyong Kim, Wonbong Choi. Mixed phase 2D Mo 0.5 W 0.5 S 2 alloy as a multi-functional electrocatalyst for a high-performance cathode in Li–S batteries. Journal of Materials Chemistry A 2020, 8 (25) , 12436-12445. https://doi.org/10.1039/D0TA04354K
    12. Eunho Cha, Mumukshu Patel, Sanket Bhoyate, Vish Prasad, Wonbong Choi. Nanoengineering to achieve high efficiency practical lithium–sulfur batteries. Nanoscale Horizons 2020, 5 (5) , 808-831. https://doi.org/10.1039/C9NH00730J

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