Mechanistic and nanoarchitectonics insight into Li–host interactions in carbon hosts for reversible Li metal storage

Abstract

Li metal has been regarded as a promising anode for rechargeable batteries with high energy densities. However, the growth of Li dendrites and severe volume changes in the Li anode still hinder its practical use. Three-dimensional (3D) host structures have recently attracted significant attention as an effective strategy to resolving these problems. Herein, we demonstrate reversible Li metal storage in carbon hosts with strong Li–host interactions derived from metal-organic frameworks (MOFs). The combined experimental and computational modeling studies reveal that galvanically displaced Ag enhances Li–host interactions and the spatial distribution characteristics of Ag play a crucial role in controlling Li storage behavior and reversibility. The atomic Ag clusters trigger the outward growth of Li from the internal pores of the host and enables stable battery cycling, whereas the surface-anchored Ag nanoparticles induce uneven Li plating on the outer surface of the carbon host, resulting in a rapid performance drop. This work provides new insights into the development of advanced host materials for reversible Li anodes by utilizing strong Li–host interactions. © 2022 Elsevier Ltd