Mesoporous Carbon Hosts with Tailored Pore Structure for Lithium Deposition in Anode-Free All-Solid-State Batteries

Abstract

Anode-free sulfide all-solid-state lithium batteries have emerged as a platform for achieving increased energy density. However, their practical operation is limited by heterogeneous interfacial reactions and uneven lithium deposition, which degrade reversibility and cycling stability. Among various approaches, silver−carbon (Ag−C) interlayers have attracted attention owing to their lithiophilicity and alloying behavior. Despite these advances, the role of carbon pore architecture in governing lithium deposition remains unclear. Here, we engineer mesoporous carbon hosts with tailored pore sizes to regulate the spatial distribution of Ag nanoparticles, thereby controlling Ag−C interfacial contact in anode-free sulfide ASSLBs. Systematic pore-size tuning promotes a more uniform distribution of Ag−C interfacial contact sites and enables homogeneous lithium deposition. Consequently, the pore-engineered host delivers enhanced cycling stability. This work establishes a clear structure−function relationship between carbon pore architecture and lithium deposition behavior, providing design guidelines for anode-free solid-state batteries.