Dendrite growth is a long-standing challenge that has limited the applications of rechargeable lithium metal electrodes. Here, we have developed a grand potential-based nonlinear phase-field model to study the electrodeposition of lithium as relevant for a lithium metal anode, using open-source software package MOOSE. The dynamic morphological evolution under a large/small overpotential is studied in two dimensions, revealing important dendrite growth/stable deposition patterns. The corresponding temporal–spatial distributions of ion concentration, overpotential, and driving force are studied, which demonstrate an intimate, dynamic competition between ion transport and electrochemical reactions, resulting in vastly different growth patterns. On the basis of the understanding from this model, we propose a “compositionally graded electrolyte” with higher local ion concentration as a way to potentially suppress dendrite formation. Given the importance of morphological evolution for lithium metal electrodes, widespread applications of phase-field models have been limited in part due to in-house or proprietary software. In order to spur growth of this field, we make all files available to enable future studies to study the many unsolved aspects related to morphology evolution of lithium metal electrodes.

中文翻译：

---

开源软件对锂枝晶生长的相场模拟

树突生长是一项长期的挑战，它限制了可充电锂金属电极的应用。在这里，我们使用开源软件包MOOSE，开发了一个基于宏电位的非线性相场模型来研究与锂金属阳极相关的锂电沉积。在二维上研究了大/小超电势下的动态形态演化，揭示了重要的枝晶生长/稳定的沉积模式。研究了离子浓度，超电势和驱动力的相应时空分布，结果表明离子迁移与电化学反应之间存在密切的动态竞争，从而导致了截然不同的生长方式。根据对模型的了解，我们提出了一种具有较高局部离子浓度的“成分梯度电解质”，以潜在地抑制枝晶形成。考虑到形态演变对锂金属电极的重要性，由于内部或专有软件的存在，相场模型的广泛应用受到了限制。为了促进该领域的发展，我们提供了所有文件，以使将来的研究能够研究与锂金属电极的形态演变有关的许多未解决的方面。