PDF(Pubmed)
Abstract：
We introduce an adhesion parameter that enables rapid screening for materials interfaces with high adhesion. This parameter is obtained by density functional theory calculations of individual single-material slabs rather than slabs consisting of combinations of two materials, eliminating the need to calculate all configurations of a prohibitively vast space of possible interface configurations. Cleavage energy calculations are used as an upper bound for electrolyte and coating energies and implemented in an adapted contact angle equation to derive the adhesion parameter. In addition to good adhesion, we impose further constraints in electrochemical stability window, abundance, bulk reactivity, and stability to screen for coating materials for next-generation solid-state batteries. Good adhesion is critical in combating delamination and resistance to lithium diffusivity in solid-state batteries. Here, we identify several promising coating candidates for the Li7La3Zr2O12 and sulfide electrolyte systems including the previously investigated electrode coating materials LiAlSiO4 and Li5AlO8, making them especially attractive for experimental optimization and commercialization.
摘要：
我们引入了一个附着力参数，该参数可以快速筛选具有高附着力的材料界面。该参数是通过单个单一材料板的密度泛函理论计算而获得的，而不是由两种材料的组合组成的板。消除了计算可能的接口配置的巨大空间的所有配置的需要。裂解能计算用作电解质和涂层能量的上限，并以适应的接触角方程实现，以得出粘附参数。除了良好的附着力，我们在电化学稳定性窗口中施加了进一步的限制，丰度,本体反应性,和稳定性，以筛选下一代固态电池的涂层材料。良好的粘附性对于防止固态电池中的分层和对锂扩散性的抗性是关键的。这里,我们确定了Li7La3Zr2O12和硫化物电解质系统的几种有前途的候选涂层，包括先前研究的电极涂层材料LiAlSiO4和Li5AlO8，使它们对于实验优化和商业化特别有吸引力。
