Sandwich-Structured Ordered Mesoporous Polydopamine/MXene Hybrids as High-Performance Anodes for Lithium-Ion Batteries

Abstract

Organic polymers have attracted significant interest as electrodes for energy storage devices because of their advantages, including molecular flexibility, cost-effectiveness, and environmentally friendly nature. Nevertheless, the real implementation of polymer-based electrodes is restricted by their poor stability, low capacity, and slow electron-transfer/ion diffusion kinetics. In this work, a sandwich-structured composite of ordered mesoporous polydopamine (OMPDA)/Ti₃C₂T_x has been fabricated by in situ polymerization of dopamine on the surface of Ti₃C₂T_x via employing the PS-b-PEO block polymer as a soft template. The OMPDA layers with vertically oriented, accessible nanopores (∼20 nm) provide a continuous pore channel for ion diffusion, while the Ti₃C₂T_x layers guarantee a fast electron-transfer path. The OMPDA/Ti₃C₂T_x composite anode exhibits high reversible capacity, good rate performance, and excellent cyclability for lithium-ion batteries. The in situ transmission electron microscopy analysis reveals that the OMPDA in the composite only shows a small volume expansion and almost preserves the initial morphology during lithiation. Moreover, these in situ experiments also demonstrate the generation of a stable and ultrathin solid electrolyte interphase layer surrounding the active material, which acts as an electrode protective film during cycling. This study demonstrates the method to develop polymer-based electrodes for high-performance rechargeable batteries.