Sulfur defect engineering controls Li2S crystal orientation towards dendrite-free lithium metal batteries
Controlling nucleation and growth of Li is crucial to avoid dendrite formation for practical applications of lithium metal batteries. Li<sub>2</sub>S has been exemplified to promote Li transport, but its crystal orientation significantly influences the Li deposition behaviors. Here, we investigate the interactions between Li and various surface structures of Li<sub>2</sub>S, and reveal that the Li<sub>2</sub>S(111) plane exhibits the highest Li affinity and the lowest diffusion barrier, leading to dense Li deposition. Using sulfur defect engineering for Li<sub>2</sub>S crystal orientation control, we construct three-dimensional vertically oriented Li<sub>2</sub>S(111)@Cu nanorod arrays as a Li metal electrode substrate and identify a substrate-dependent Li nucleation process and a facet-dependent growth mode. Furthermore, we demonstrate the versatility of the Li<sub>2</sub>S(111)@Cu substrate when paired with two positive electrodes: achieving an initial discharge capacity of 138.8 mAh g<sup>-1</sup> with 88% capacity retention after 400 cycles at 83.5 mA g<sup>-1</sup> with LiFePO<sub>4</sub>, and an initial discharge capacity of 181 mAh g<sup>-1</sup> with 80% capacity retention after 160 cycles at 60 mA g<sup>-1</sup> with commercial LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> positive electrode (4 mAh cm<sup>-2</sup>).
Authors
- Wei‐Chen Zheng (ORCID: https://orcid.org/0009-0008-1359-1344)
- Chenguang Shi (ORCID: https://orcid.org/0000-0003-3024-8667)
- Shiyuan Zhou (ORCID: https://orcid.org/0000-0002-9270-2573)
- Xiaoyang Huang (ORCID: https://orcid.org/0000-0002-7221-2075)
- Ling Huang (ORCID: https://orcid.org/0000-0003-2403-1170)
- Yuxiang Xie (ORCID: https://orcid.org/0000-0002-8528-7922)
- Jin‐Xia Lin (ORCID: https://orcid.org/0000-0003-0407-3867)
- Wen‐Feng Lin
- Hua-yu Huang
- Shi-Shi Liu
- Gyeong‐Su Park (ORCID: https://orcid.org/0000-0002-5820-8280)
- Rena Oh (ORCID: https://orcid.org/0000-0001-9729-0398)
- Hui Chen (ORCID: https://orcid.org/0000-0001-7619-3425)
- Juntao Li (ORCID: https://orcid.org/0000-0003-1399-9792)
- Shi‐Gang Sun (ORCID: https://orcid.org/0000-0003-2327-4090)
- Peng Dai (ORCID: https://orcid.org/0000-0002-5973-9155)
- Jun-Fei Shen
- Shengnan Hu (ORCID: https://orcid.org/0000-0002-7771-7339)
- Ying Zhong (ORCID: https://orcid.org/0000-0001-9041-3172)
Institutions
- Seoul National University (KR)
- Loughborough University (GB)
- Chongqing University (CN)
- Xiamen University (CN)
- Daegu Gyeongbuk Institute of Science and Technology (KR)
- Advanced Energy (United States) (US)
- Quzhou University (CN)
- Collaborative Innovation Center of Chemistry for Energy Materials (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-04-01
- DOI
- https://doi.org/10.1038/s41467-025-57572-5
- Citations
- 12
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 8.77
Funders
- National Research Foundation
- National Natural Science Foundation of China
- Ministry of Science, ICT and Future Planning
- National Research Foundation of Korea
- Engineering and Physical Sciences Research Council
- National Key Research and Development Program of China
- Beijing Synchrotron Radiation Facility