J.Q. Qin *, H.T. Zhang, T.S. Bai, X.H. Liu, Y.L. Ren, L.X. Xie, X. Wang, S.H. Zheng, F. Zhou * and Z.-S. Wu *

Advanced Functional Materials, 2024, Accepted.

2D materials have been 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) lead to serious performance degradation, in particular, of micro-supercapacitors (MSCs) with narrow working voltage and low energy density. Here, we demonstrate a universal chemically confined interfacial assembly strategy 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 MoS2). 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/cm2, excellent flexibility with 99% of capacitance retention at 180º, 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.