The growth of lithium dendrites severely restricts the development of lithium metal batteries. In order to achieve the goal of dendrites-free lithium in principle, it is crucial and urgent to control nucleation and growth of lithium. Here, a functional organic layer of perylene-3, 4, 9, 10-tetracarboxydiimide-lithium (PTCDI-Li) is built on the lithium anode surface by in-situ chemical reaction of PTCDI and Li metal. PTCDI-Li, with high surface energy (-10.19 eV) and low diffusion barrier (0.89 eV), efficiently promotes disk-shaped high-dimensional nucleation by regulation of lithium ion flux upon lithium plating, leading to a dendrites-free morphology. When operating under a relatively high current density of 10 mA cm⁻², the Li | Li symmetrical cells with PTCDI-Li exhibit outstanding cyclic stability for 300 hours with ultralow overpotential of 400 mV, superior to the most of the reported lithium anode. The corresponding PTCDI-Li batteries show high specific capacity and enhanced cycle life. We anticipate that this strategy of regulation of lithium deposition from one-dimensional to high-dimensional opens a new horizon in the development of dendrites-free Li anodes.

锂树枝状晶体的生长严重限制了锂金属电池的发展。为了原则上实现无树枝状锂的目标，控制锂的成核和生长是至关重要和紧迫的。在此，通过PTCDI和Li金属的原位化学反应，在锂阳极表面上构建per-3、4、9、10-四羧基二酰亚胺锂（PTCDI-Li）的功能有机层。具有高表面能（-10.19 eV）和低扩散势垒（0.89 eV）的PTCDI-Li通过调节镀锂时的锂离子通量来有效地促进盘状高维成核，从而导致无枝晶形貌。在10 mA cm ^-2的较高电流密度下运行时，李| 具有PTCDI-Li的Li对称电池在300小时内表现出出色的循环稳定性，超低过电势为400 mV，优于大多数报道的锂阳极。相应的PTCDI-Li电池显示出高比容量和更长的循环寿命。我们预计，这种从一维到高维的锂沉积调节策略将为无枝状锂阳极的发展开辟新的视野。