Spatially resolved modulation of the electrode-electrolyte interface in high Li-stoichiometric battery anodes

Abstract

High Li-stoichiometric battery anodes (e.g., Si, Ge, Sn, P, Sb, Bi) with exceptional theoretical capacities and favorable lithiation potentials are promising to surpass the energy limitations of existing rechargeable batteries. Yet, these anodes suffer from large volume fluctuations, unstable interfacial reactions, and the difficulty of maintaining an intact solid electrolyte interphase layer, all of which hinder their practical application. Numerous strategies have been developed to stabilize the electrode-electrolyte interface to overcome these challenges. In fact, these approaches can be systematically categorized according to their spatial proximity to the interface, ranging from surface-level modifications to bulk-level structural designs. The continued advancement of such spatially resolved strategies offers an attractive pathway to achieve durable and high-performance electroarchitectures. In this review, we first discuss the fundamental aspects, encompassing the spatial structures and functional roles that emerge at the electrode-electrolyte interface. Thereafter, interfacial strategies are presented in terms of their spatial location, spanning from the electrode subsurface to the bulk, while addressing both liquid electrolyte and solid-state electrolyte systems. By presenting a spatial framework for interfacial engineering, this review provides new insights and future research directions for constructing more stable interfaces in Li-alloying anodes.

Keywords

High Li-stoichiometric anodes / electrode-electrolyte interface / spatial architecture / solid electrolyte interphase layer / interfacial strategies

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