Title: Sulfur defect engineering controls Li2S crystal orientation towards dendrite-free lithium metal batteries

Authors: Jin-Xia Lin, Peng Dai, Sheng-Nan Hu, Shiyuan Zhou, Gyeong-Su Park, Chen-Guang Shi, Jun-Fei Shen, Yu-Xiang Xie, Wei-Chen Zheng, Hui Chen, Shi-Shi Liu, Hua-Yu Huang, Ying Zhong, Jun-Tao Li, Rena Oh, Xiaoyang Jerry Huang, Wen-Feng Lin*, Ling Huang* & Shi-Gang Sun*

Abstract: Controlling nucleation and growth of Li is crucial to avoid dendrite formation for practical applications of lithium metal batteries. Li₂S 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 Li₂S, and reveal that the Li₂S(111) plane exhibits the highest Li affinity and the lowest diffusion barrier, leading to dense Li deposition. Using sulfur defect engineering for Li₂S crystal orientation control, we construct three-dimensional vertically oriented Li₂S(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 Li₂S(111)@Cu substrate when paired with two positive electrodes: achieving an initial discharge capacity of 138.8 mAh g^–1 with 88% capacity retention after 400 cycles at 83.5 mA g^–1 with LiFePO₄, and an initial discharge capacity of 181 mAh g^–1 with 80% capacity retention after 160 cycles at 60 mA g^–1 with commercial LiNi_0.8Co_0.1Mn_0.1O₂ positive electrode (4 mAh cm^–2).

Full-Link: https://www.nature.com/articles/s41467-025-57572-5