金属阳极的形态稳定性：固态电解质界面（SEI）和去溶剂化动力学的作用
Morphological Stability of Metal Anodes: Roles of Solid Electrolyte Interphases (SEIs) and Desolvation Kinetics
AI总结：
本研究通过理论框架分析SEI和去溶剂化动力学对锂金属阳极形态稳定性的影响，提出表观Damköhler数以指导稳定阳极设计。
摘要：
实现稳定的锂金属阳极需要对固态电解质界面（SEI）和去溶剂化动力学进行控制。在这里，我们开发了一个统一的理论框架，整合了离子传输、去溶剂化、电荷转移和SEI破裂，以预测电沉积过程中的形态不稳定性。通过线性稳定性分析，我们识别出六个无量纲参数，这些参数决定了不稳定性的发展和演变。我们证明SEI传输和去溶剂化速率有效调节了表观反应动力学，使系统向稳定、受反应速率限制的区域转变。在经典极限电流概念的基础上，我们展示出厚而导电性差的SEI和缓慢的去溶剂化显著降低了极限电流。我们引入了一个表观Damköhler数来量化关键平衡：通过降低反应速率来抑制扩散受限的不稳定性，同时保持较高的极限电流。我们的理论使能够预测电沉积形态在多种材料和操作条件下的映射，指导稳定锂金属阳极的合理设计。
英文摘要：
Achieving stable lithium metal anodes requires control over the solid-electrolyte interphase (SEI) and desolvation kinetics. Here, we develop a unified theoretical framework integrating ion transport, desolvation, charge transfer, and SEI breakdown to predict morphological instabilities during electrodeposition. Using linear stability analysis, we identify six dimensionless parameters that govern the onset and evolution of instabilities. We show that SEI transport and desolvation rate effectively modulate apparent reaction kinetics, shifting the system toward a stable, reaction-limited regime. Extending the classical limiting current concept, we demonstrate that a thick, poorly conductive SEI and sluggish desolvation significantly reduce the limiting current. We introduce an apparent Damköhler number to quantify the critical balance: suppressing diffusion-limited instabilities by reaction rate reduction, while maintaining a high limiting current. Our theory enables predictive mapping of electrodeposition morphologies across diverse materials and operating conditions, guiding the rational design of stable lithium metal anodes.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
