Gelation-Assisted Assembly of Large-Area, Highly Aligned, and Environmentally Stable MXene Films with an Excellent Trade-Off between Mechanical and Electrical Properties

Layered MXene films have shown enormous potential for wide applications due to their high electrical conductivity and unique laminated microstructure. However, the intrinsic susceptibility to oxidation and the mechanical fragility of MXene films are the two major bottlenecks that prevent their widespread industrial applications. Here, a facile yet efficient assembly strategy is proposed to address these issues by increasing the alignment and compactness of MXene layers as well as strengthening the interlayer interactions. This method involves the gelation of MXene flakes with a multifunctional inorganic "mortar" polymer (ammonium polyphosphate, APP) followed by quasi-solid-state assembly enabled by a mechanical rolling process, by which the 3D gel network is transformed into 2D freestanding MXene films with unprecedented flake alignment and compactness. Besides, due to the multiple molecular-level interactions (hydrogen bonding, coordination bonding, and electrostatic force) between APP and MXene flakes, the resultant MXene-APP film (MAF) displays high mechanical strength (286.4 +/- 20.3 MPa) and excellent electrical conductivity (8012.4 +/- 325.6 S cm(-1)), along with remarkable environmental stability. As an application demonstration, MAF exhibits outstanding electromagnetic interference shielding effectiveness with long-term durability, highlighting the great potential of this gelation-assisted assembly strategy in fabricating large-area, high-performance MXene films for diverse real-world applications.