Design Principles for Heterointerfacial Alloying Kinetics at Metallic Anodes in Rechargeable Batteries

Abstract

How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest. Here we consider the relation between the surface chemistry at such interfaces and the reversibility of electrochemical transformations at rechargeable battery electrodes. Using Zn as a model system, we report that a moderate strength of chemical interaction between the deposit and the substrate—neither too weak nor too strong—enables highest reversibility and stability of the plating/stripping redox processes. Focused-ion-beam and electron microscopy were used to directly probe the morphology, chemistry and crystallography of the heterointerfaces of distinct natures. Analogous to the empirical Sabatier principle for chemical heterogeneous catalysis, our finding arises from the confluence of competing interfacial processes. Using full batteries with stringent N:P ratios, we show that such knowledge provides a powerful tool for designing key materials in highly reversible battery systems based on earth-abundant, low-cost metals such as Zn and Na.Reference: Zheng, Jingxu, et al. "Design principles for heterointerfacial alloying kinetics at metallic anodes in rechargeable batteries." Science Advances 8.44 (2022): eabq6321.