Hierarchically Porous and Interconnected Ti ₃ C ₂ T _<i>x</i> MXene Networks via Interface-Directed Functionalization for Lithium–Sulfur Batteries

MXene networks, enabled by interface-directed functionalization and organized assembly at water-nonpolar heterointerface. Rational control of MXene flakes wettability through solution phase functionalization unfolds large tunability of MXene assembled structure, successfully addressing key design requirements for lithium-sulfur batteries. Interconnected hierarchical porosity facilitates electron/ion transport as well as polysulfide conversion, contributing to high sulfur utilization and excellent rate capability. In-depth microstructural characterization along with density functional theory simulations reveals that local lattice strain in the MXene plane enforced by nonplanar interfacial geometry boosts polysulfide adsorption. The proposed interface-directed functionalization strategy and the resulting hierarchical network structure offer a versatile framework for judicious microstructural tuning of MXene-based electrodes beyond typical energy storage applications.