Generalized Interfacial Assembly of 2D Mesoporous Heterostructures for High‐Energy Solid‐State Micro‐Supercapacitors

Abstract 2D materials have garnered considerable interest in various applications from catalysis to energy storage. However, the self‐stacking and poor air stability of 2D materials (e.g., MXene) leads to serious performance degradation, in particular, of micro‐supercapacitors (MSCs) with narrow working voltage and low energy density. Here, a universal confined interfacial assembly strategy is demonstrated for controllably synthesizing a series of 2D mesoporous heterostructures for high‐voltage and high‐energy ionogel‐based MSCs. This assembly process reveals accurate controllability and extraordinary versatility, endowing the 2D mesoporous heterostructures with highly adjustable mesopore size (7–22 nm), tunable thickness (15–29 nm), variable carbon precursors (including oligochitosan, glucose, and sucrose), and replaceable 2D substrates (e.g., MXene, graphene, BN, and MoS 2 ). As a proof of concept, the 2D mesoporous carbon@MXene based MSCs with ionic liquid ionogel electrolyte deliver ultrahigh voltage of 3.7 V, superior areal energy density of 181.3 µWh cm −2 , excellent flexibility with 99% of capacitance retention at 180°, and excellent modular self‐integration for variable voltage/capacitance output, surpassing most reported MXene based MSCs. Therefore, this work will open a novel available paradigm for scalable fabrication of 2D mesoporous materials to target high‐performance and functional microscale power source.