3D Assembly of MXene Networks using a Ceramic Backbone with Controlled Porosity

Transition metal carbides (MXenes) are novel 2D nanomaterials with exceptional properties, promising significant impact in applications such as energy storage, catalysis, and energy conversion. A major barrier preventing the widespread use of MXenes is the lack of methods for assembling MXene in 3D space without significant restacking, which degrades their performance. Here, this challenge is successfully overcome by introducing a novel material system: a 3D network of MXene formed on a porous ceramic backbone. The backbone dictates the network's 3D architecture while providing mechanical strength, gas/liquid permeability, and other beneficial properties. Freeze casting is used to fabricate a silica backbone with open pores and controlled porosity. Next, capilary flow is used to infiltrate MXene into the backbone from a dispersion. The system is then dried to conformally coat the pore walls with MXene, creating an interconnected 3D‐MXene network. The fabrication approach is reproducible, and the MXene‐infiltrated porous silica (MX‐PS) system is highly conductive (e.g., 340 S m⁻¹). The electrical conductivity of MX‐PS is controlled by the porosity distribution, MXene concentration, and the number of infiltration cycles. Sandwich‐type supercapacitors with MX‐PS electrodes are shown to produce excellent areal capacitance (7.24 F cm⁻²) and energy density (0.32 mWh cm⁻²) with only 6% added MXene mass. This approach of creating 3D architectures of 2D nanomaterials will significantly impact many engineering applications.