Unveiling the autocatalytic growth of Li2S crystals at the solid-liquid interface in lithium-sulfur batteries
Electrocatalysts are extensively employed to suppress the shuttling effect in lithium-sulfur (Li-S) batteries. However, it remains challenging to probe the sulfur redox reactions and mechanism at the electrocatalyst/LiPS interface after the active sites are covered by the solid discharge products Li<sub>2</sub>S/Li<sub>2</sub>S<sub>2</sub>. Here, we demonstrate the intrinsic autocatalytic activity of the Li<sub>2</sub>S (100) plane towards lithium polysulfides on single-atom nickel (SANi) electrocatalysts. Guided by theoretical models and experimental data, it is concluded that LiPS dissociates into Li<sub>2</sub>S<sub>2</sub> and short-chain LiPS on the Li<sub>2</sub>S (100) plane. Subsequently, Li<sub>2</sub>S<sub>2</sub> undergoes further lithiation to Li<sub>2</sub>S on the Li<sub>2</sub>S (100) surface, generating a new Li<sub>2</sub>S (100) layer, thus enabling the autocatalytic formation of a new Li<sub>2</sub>S (100) surface. Benefiting from the autocatalytic growth of Li<sub>2</sub>S, the concentration of LiPS in the electrolyte remains at a lower level, enabling Li-S batteries under high loading and low electrolyte conditions to exhibit superior electrochemical performance.
Authors
- Xiaoping Ouyang (ORCID: https://orcid.org/0000-0001-8474-2869)
- Junfeng Wang (ORCID: https://orcid.org/0000-0002-5720-056X)
- Xueliang Andy Sun (ORCID: https://orcid.org/0000-0003-0374-1245)
- Ali Coşkun (ORCID: https://orcid.org/0000-0002-4760-1546)
- Zhen Wu (ORCID: https://orcid.org/0000-0002-6287-8287)
- Erjun Kan (ORCID: https://orcid.org/0000-0003-0433-4190)
- Fen Qiao (ORCID: https://orcid.org/0000-0002-2661-0937)
- Junwu Zhu (ORCID: https://orcid.org/0000-0002-7518-9683)
- Xin Wang (ORCID: https://orcid.org/0000-0003-4099-4268)
- Mingliang Liu (ORCID: https://orcid.org/0000-0001-9703-2911)
- Wenfeng He
- Wei Tong (ORCID: https://orcid.org/0000-0001-8328-7999)
- Yongsheng Fu (ORCID: https://orcid.org/0000-0002-2224-5610)
- Tong Guo
Institutions
- Jiangsu University (CN)
- Western University (CA)
- University of Fribourg (CH)
- Nanjing University of Science and Technology (CN)
- Ministry of Education (KR)
- Xiangtan University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-11-04
- DOI
- https://doi.org/10.1038/s41467-024-53797-y
- Citations
- 75
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 15.65
Funders
- National Science Foundation
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Government of Jiangsu Province
- Natural Science Foundation of Jiangsu Province