Hydroiodic‐Acid‐Initiated Dense yet Porous Ti3C2Tx MXene Monoliths toward Superhigh Areal Energy Storage

Abstract The assembly of 3D structured materials from 2D units paves a royal road for building thick and dense electrodes, which are long sought after for practical energy‐storage devices. 2D transitional metal carbides (MXene) are promising for this due to their capabilities of solution‐based assembly and intrinsic high density, yet face huge challenges in yielding high areal capacitance electrodes owing to the absence of porous ion‐transport paths. Here, a gelation–densification process initiated by hydroiodide acids (HI) is proposed, where the protons break the electrostatic balance of MXene nanosheets to trigger gelation, while HI serves as a spacer to prevent nanosheets from restacking during capillary shrinkage. More promising, the controlled evaporation of reductive HI leaves superiorly shrinking yet porous network for ion transport, and the produced monoliths exhibit a high density of 2.74 g cm −3 and an unprecedented areal capacitance of 18.6 F cm −2 .