Electroplating is one of the most common processes to create smooth surfaces and thin coatings, but achieving smooth lithium (Li) plating without Li dendrite growth remains a challenge for developing next-generation Li-ion batteries based on Li metal anodes. One of the main reasons is our inability to directly model and predict the atomistic and mesoscale mechanisms underlying the complex electroplating process involving concurrent ionic transport, redox reactions, and development of morphological instability. Here we report a multiscale model integrating atomistic calculations of charge transfer physics with the mesoscale phase-field model to understand and predict morphological evolution for general metal electrodeposition processes. The results reveal that the difference in cation desolvation-induced exchange current is mainly responsible for the dramatically different dendritic Li plating and smooth magnesium (Mg) plating. This study provides a strategy for designing dendrite-free Li-ion battery anodes guided by a multiscale model integrating the phase-field method and atomistic calculations.

电镀是创建光滑表面和薄涂层的最常见方法之一，但是在开发不基于Li树枝状晶体的情况下实现光滑的锂（Li）电镀仍然是开发基于锂金属阳极的下一代锂离子电池的挑战。主要原因之一是我们无法直接建模和预测复杂电镀过程所涉及的原子和中尺度机理，该过程涉及同时发生的离子迁移，氧化还原反应和形态不稳定性的发展。在这里，我们报告了一个多尺度模型，该模型将电荷转移物理学的原子计算与中尺度相场模型结合在一起，以了解和预测一般金属电沉积过程的形态演变。结果表明，阳离子去溶剂化引起的交换电流的差异主要是导致树枝状Li镀层和平滑镁（Mg）镀层显着不同的原因。这项研究提供了一种设计多相模型的无树突状锂离子电池阳极的策略，该模型结合了相场法和原子计算。