Atomic and molecular layer deposition (ALD/MLD) coatings are promising solutions for preventing dendrite formation in aqueous and non-aqueous Li/Na/Zn metal batteries. Notably, alumina and alucone coatings have emerged as highly effective against dendrite formation in Zn anodes. Despite their demonstrated efficacy, a comprehensive understanding of their chemo-mechanical impact on anodes remains elusive. In this study, we take a bottom-up framework to these coatings on Zn foils, employing an approach that integrates ab initio simulations with continuum theories to elucidate lattice misfit and chemical bonding. We use this insight to develop a macroscopic model to predict the epitaxial residual stresses generated during thin-film deposition. Our findings reveal a robust chemical bonding between the hydroxylated Zn surface and the thin film. This, in turn, generates large misfit strains that result in significant interfacial stresses during deposition. These results are then compared to experiments by measuring the curvature of the coated thin films, finding good agreement between experiments and theory. This novel understanding sheds light on the fundamental mechanisms underpinning the development of chemo-mechanical stresses in thin films, which impact dendrite suppression in anodes, offering valuable insights for the design of new coatings.

中文翻译：

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通过原子层和分子层沉积在晶格失配外延薄膜中的残余应力发展


原子和分子层沉积 （ALD/MLD） 涂层是防止水/Na/Na/Zn 金属电池中形成枝晶的有前途的解决方案。值得注意的是，氧化铝和明铝涂层对 Zn 阳极中枝晶的形成非常有效。尽管它们已被证明是有效的，但对其对阳极的化学机械影响的全面了解仍然难以捉摸。在这项研究中，我们对 Zn 箔上的这些涂层采用自下而上的框架，采用一种将 ab initio 模拟与连续体理论相结合的方法来阐明晶格失配和化学键合。我们利用这一见解开发了一个宏观模型来预测薄膜沉积过程中产生的外延残余应力。我们的研究结果揭示了羟基化 Zn 表面和薄膜之间强大的化学键。这反过来又会产生较大的 misfit 应变，从而在沉积过程中产生显着的界面应力。然后通过测量涂层薄膜的曲率将这些结果与实验进行比较，发现实验和理论之间有很好的一致性。这种新颖的理解阐明了支撑薄膜中化学机械应力发展的基本机制，这些应力会影响阳极中的枝晶抑制，为新涂层的设计提供了有价值的见解。