Su Ben, Wang Xingyu, Chai Lei, Huo Sida, Qiu Jingyi, Huang Qiang, Li Shuang, Wang Yue, Xue Wendong
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China.
School of Microelectronics, Dalian University of Technology, Dalian, Liaoning, 116024, China.
Adv Sci (Weinh). 2024 Jun;11(23):e2308939. doi: 10.1002/advs.202308939. Epub 2024 Apr 10.
Lithium metal, with ultrahigh theoretical specific capacity, is considered as an ideal anode material for the lithium-ion batteries. However, its practical application is severely plagued by the uncontrolled formation of dendritic Li. Here, a cation-loaded porous Mg-Zeolite layer is proposed to enable the dendrite-free deposition on the surface of Li metal anode. The skeleton channels of zeolite provide the low coordinated Li-solvation groups, leading to the faster desolvation process at the interface. Meanwhile, anions-involved solvation sheath induces a stable, inorganic-rich SEI, contributing to the uniform Li flux through the interface. Furthermore, the co-deposition of sustained release Mg realizes a new faster migration pathway, which proactively facilitates the uniform diffusion of Li on the lithium substrate. The synergistic modulation of these kinetic processes facilitates the homogeneous Li plating/stripping behavior. Based on this synergistic mechanism, the high-efficiency deposition with cyclic longevity exceeding 2100 h is observed in the symmetric Li/Li cell with Mg-Zeolite modified anode at 1 mA cm. The pouch cell matched with LiFePO cathode fulfills a capacity retention of 88.4% after 100 cycles at a severe current density of 1 C charge/discharge. This synergistic protective mechanism can give new guidance for realizing the safe and high-performance Li metal batteries.
锂金属具有超高的理论比容量,被认为是锂离子电池理想的负极材料。然而,其实际应用受到枝晶锂无控制生长的严重困扰。在此,提出了一种阳离子负载的多孔镁-沸石层,以实现锂金属负极表面无枝晶沉积。沸石的骨架通道提供低配位的锂溶剂化基团,导致界面处的去溶剂化过程更快。同时,涉及阴离子的溶剂化鞘层诱导形成稳定的、富含无机成分的固体电解质界面(SEI),有助于锂通量均匀通过界面。此外,持续释放的镁的共沉积实现了一条新的更快迁移路径,主动促进锂在锂基底上的均匀扩散。这些动力学过程的协同调节促进了锂的均匀沉积/剥离行为。基于这种协同机制,在1 mA cm²的电流密度下,具有镁-沸石改性负极的对称锂/锂电池中观察到循环寿命超过2100小时的高效沉积。与磷酸铁锂正极匹配的软包电池在1 C充/放电的严苛电流密度下经过100次循环后容量保持率为88.4%。这种协同保护机制可为实现安全高性能锂金属电池提供新的指导。