Lin Jin-Xia, Dai Peng, Hu Sheng-Nan, Zhou Shiyuan, Park Gyeong-Su, Shi Chen-Guang, Shen Jun-Fei, Xie Yu-Xiang, Zheng Wei-Chen, Chen Hui, Liu Shi-Shi, Huang Hua-Yu, Zhong Ying, Li Jun-Tao, Oh Rena, Huang Xiaoyang Jerry, Lin Wen-Feng, Huang Ling, Sun Shi-Gang
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Institute of Next-Generation Semiconductor Convergence Technology, Daegu Gyeongbuk Institute of Science and Technology (DGIST), Daegu, Republic of Korea.
Nat Commun. 2025 Apr 1;16(1):3130. doi: 10.1038/s41467-025-57572-5.
Controlling nucleation and growth of Li is crucial to avoid dendrite formation for practical applications of lithium metal batteries. LiS 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 LiS, and reveal that the LiS(111) plane exhibits the highest Li affinity and the lowest diffusion barrier, leading to dense Li deposition. Using sulfur defect engineering for LiS crystal orientation control, we construct three-dimensional vertically oriented LiS(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 LiS(111)@Cu substrate when paired with two positive electrodes: achieving an initial discharge capacity of 138.8 mAh g with 88% capacity retention after 400 cycles at 83.5 mA g with LiFePO, and an initial discharge capacity of 181 mAh g with 80% capacity retention after 160 cycles at 60 mA g with commercial LiNiCoMnO positive electrode (4 mAh cm).
对于锂金属电池的实际应用而言，控制锂的成核和生长对于避免枝晶形成至关重要。硫化锂已被证明可促进锂的传输，但其晶体取向会显著影响锂的沉积行为。在此，我们研究了锂与硫化锂各种表面结构之间的相互作用，并揭示出硫化锂（111）面表现出最高的锂亲和力和最低的扩散势垒，从而导致锂致密沉积。通过对硫化锂晶体取向控制进行硫缺陷工程，我们构建了三维垂直取向的硫化锂（111）@铜纳米棒阵列作为锂金属电极基底，并确定了基底依赖的锂成核过程和面依赖的生长模式。此外，我们展示了硫化锂（111）@铜基底与两种正极配对时的通用性：与磷酸铁锂配对时，在83.5 mA g下循环400次后，初始放电容量为138.8 mAh g，容量保持率为88%；与商用锂镍钴锰氧化物正极（4 mAh cm）配对时，在60 mA g下循环160次后，初始放电容量为181 mAh g，容量保持率为80%。
