Cultivating a self-reinforcing solid-electrolyte interphase for negative fading enhancement in CH3NH3PbBr3 perovskite anodes

Abstract

The practical deployment of MAPbBr3 perovskite anodes in photovoltaic cells and battery applications is hindered by interfacial instability and poor initial Coulombic efficiency (ICE).This study demonstrates a modular interfacial engineering strategy to cultivate a selfreinforcing solid-electrolyte interphase (SEI) into a source of exceptional stability. Combined theoretical and experimental analyses reveal that the initial SEI (containing inorganic components LiBr and PbBr2 ) via mechanical prelithiation process effectively improves the ICE to 84.6%; the continuous interfacial optimization in the tailored ether-electrolyte unlocks exceptional stability in the MAPbBr3 -based anode over 1000 cycles via an enhanced negativefading phenomenon. Notably, the optimized ether-based electrolyte T-DME/DOL creates a unique solvation structure with low anion coordination and high solvation energy, initiating a self-reinforcing SEI during cycling. Consequently, the pre-lithiated MAPbBr3 -based anode achieves exceptional lithium storage performance, particularly maintaining 96% capacity retention after 1000 cycles at 1.0 A g-1 . Beyond lithium-ion batteries, this dynamic interfacial stabilization strategy provides crucial insights for enhancing durability of perovskite materials in photovoltaics and optoelectronics where interface-dominated degradation mechanisms prevail.