Lithium metal batteries (LMBs) possess outstanding theoretical energy density and have attracted widespread attention as the next generation of energy storage devices for various crucial applications. However, the commercialization of LMBs has to simultaneously overcome numerous challenges, such as inferior Coulombic efficiency and cycling performance, high self-discharge, and complicated interfacial reactions. It has traditionally been an enormous challenge about the uniform deposition of lithium on the surface of current collector to relieve the formation of lithium dendrites. In this study, a novel efficient strategy of plating uniform lithiophilic polythiophene derivatives substrates on Cu foils was developed and the nucleation mechanism of Li ions on polythiophene derivatives substrates was further explored. We first explored the interaction between polythiophene derivatives substrates and Li ions by first-principles calculations, and found shorter side chains of polythiophene derivatives can enhance the adsorption energy and promote the diffusion rate of Li ions. Polythiophene derivatives substrates have a large number of dispersive lipophilic sites and Li ions diffusion channels in the main chain, which can effectively regulate the nucleation and growth stages of Li ions deposition. We further found polythiophene derivatives with different side chains can induce the electrodeposition of Li ions with different morphology, while the polythiophene derivatives with the shortest side chains can contribute to the most excellent cycle efficiency, resulting in a uniform lithium deposition with less lithium dendritic growth experimentally.

锂金属电池（LMB）具有出色的理论能量密度，作为下一代用于各种关键应用的能量存储设备已引起广泛关注。然而，LMB的商业化必须同时克服许多挑战，例如库仑效率和循环性能差，自放电率高以及复杂的界面反应。传统上，关于锂在集电器表面上的均匀沉积以减轻锂枝晶的形成是巨大的挑战。在这项研究中，开发了一种新的有效策略，在铜箔上电镀均匀的亲硫聚噻吩衍生物基质，并进一步探索了锂离子在聚噻吩衍生物基质上的成核机理。我们首先通过第一性原理研究了聚噻吩衍生物底物与锂离子之间的相互作用，发现较短的聚噻吩衍生物侧链可以增强吸附能并促进锂离子的扩散速率。聚噻吩衍生物底物在主链上具有大量的亲脂性分散位点和锂离子扩散通道，可有效调节锂离子沉积的成核和生长阶段。我们进一步发现具有不同侧链的聚噻吩衍生物可以诱导具有不同形态的Li离子的电沉积，而具有最短侧链的聚噻吩衍生物可以提供最佳的循环效率，从而在实验中产生均匀的锂沉积，而锂枝晶的生长较少。