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Theoretically endured defect-engineered antimony selenide nanocrystals grafted within three-dimensional reduced graphene oxide hollow microspheres with large open cavities as polysulfide barrier for robust sulfur kinetics

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Abstract

Defect engineering techniques have gained significant attention worldwide as a promising strategy to amend the electronic and atomic arrangements of nanomaterials. By introducing defects such as dislocations or vacancies in polar materials, it is possible to create electrophilic adsorption sites that can effectively trap polysulfide species by lowering the energy transfer barrier for electrons. In this study, non-stoichiometric antimony selenide (Sb2Se2.2) nanocrystals embedded in a three-dimensional hollow microsphere composed of a reduced graphene oxide (rGO) matrix (H-Sb2Se2.2@rGO‒600) were synthesized by precisely controlling the heating conditions. Density functional theory (DFT) calculations revealed that thermally induced anionic Se-defects caused atomic disorder in the crystal structure, altering the electronic structure and in turn enhancing the adsorption strength of polysulfide through improved electrophilic coupling interactions between \(\mathrm{Sb}^{\delta+}-\mathrm S_x^{2-}\) and \(\mathrm{Li}^+-\mathrm{Se}^{\delta-}\). Lithium–sulfur (Li–S) batteries incorporating H-Sb2Se2.2@rGO‒600-coated separator and a typical sulfur electrode (≈2.0 mg cm–2) exhibited excellent high-rate capability, with a discharge rate of up to 4.0 C, and exceptional cycling stability. After 1300 continuous charge‒discharge cycles at 4.0 C, the cell showed a capacity retention of 90.4%, with an average capacity decay rate of only 0.007% per cycle. The impressive performance was maintained under more demanding cell conditions, such as high effective S content (66%), high S loading (6.0 mg cm–2), and a low electrolyte-to-sulfur ratio (4.3 µL mg–1). The Li–S cell demonstrates excellent cycling stability (120 cycles at 0.1 C) and maintains feasible rate performance up to 0.3 C.

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The data are available from the corresponding author upon reasonable request.

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Funding

This work was supported by the National Research Foundation of Korea (NRF) and funded by the Korean Government (MSIP) (grant numbers No. RS-2023-00217581 and NRF-2021R1I1A3057700). This work was partly supported by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) (20224000000070, Human Resource Training for Smart Energy New Industry Cluster). This research was supported by the “Regional Innovation Strategy (RIS)” through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (MOE) (2021RIS-001).

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  1. Rakesh Saroha, Dong Yun Shin, and Jae Seob Lee contributed equally to this work.

Authors and Affiliations

  1. Department of Engineering Chemistry, Chungbuk National University, Chungbuk, 361-763, Republic of Korea

    Rakesh Saroha, Jae Seob Lee, Sung Woo Cho & Jung Sang Cho

  2. Department of Environmental Engineering, Chungbuk National University, Chungbuk, 361-763, Republic of Korea

    Dong Yun Shin & Dong-Hee Lim

  3. Department of Materials Science and Engineering, Korea University, Anam-Dong, Seongbuk-Gu, Seoul, 136-713, Republic of Korea

    Jae Seob Lee

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  1. Rakesh Saroha
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Contributions

Rakesh Saroha—designed the idea, performed experiments, and prepared the initial blueprint. Dong Yun Shin—DFT calculations and analysis. Jae Seob Lee and Sung Woo Cho—performed experiments and data accumulation. Dong-Hee Lim—DFT analysis, review and editing. Jung Sang Cho—supervision, writing, review and editing.

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Correspondence to Dong-Hee Lim or Jung Sang Cho.

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Saroha, R., Shin, D.Y., Lee, J.S. et al. Theoretically endured defect-engineered antimony selenide nanocrystals grafted within three-dimensional reduced graphene oxide hollow microspheres with large open cavities as polysulfide barrier for robust sulfur kinetics. Adv Compos Hybrid Mater 7, 93 (2024). https://doi.org/10.1007/s42114-024-00892-9

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