Dual-Axis Interfacial Engineering of Carbon Paper Hosts for Stable Anode-Less Lithium Metal Batteries

Abstract

Anode-less lithium (Li) metal batteries (LMBs) offer exceptional energy density but suffer from rapid capacity degradation caused by unstable Li plating and electrolyte decomposition on bare current collectors. Here, we address these challenges using a dual-functionalized three-dimensional (3D) carbon paper (CP) host. We convert the inherent PTFE coating of commercial CP into an inorganic pre-formed solid electrolyte interphase (pre-SEI) while simultaneously integrating lithiophilic MgO nanoparticles via a single-step co-annealing process, creating a MgO-preSEI-CP composite. The pre-SEI layer passivates the interface and suppresses parasitic reactions, while MgO nanoparticles provide uniformly distributed nucleation sites that enhance surface lithiophilicity. By simultaneously reducing electronic conductivity at the surface and improving electrolyte wettability, this dual-functional design establishes an internal potential gradient, directing Li plating into the host interior rather than forming surface dendrites. This synergistic approach demonstrates a generalizable design strategy for 3D hosts that enable stable operation of anode-less LMBs.