Reversible Formation of g‐C3N4 3D Hydrogels through Ionic Liquid Activation: Gelation Behavior and Room‐Temperature Gas‐Sensing Properties

Many unique properties arise when the 3D stacking of layered materials is disrupted, originating nanostructures. Stabilization, and further reorganization of these individual layers into complex 3D structures, can be essential to allow these properties to persist in macroscopic systems. It is demonstrated that a simple hydrothermal process, assisted by ionic liquids (ILs), can convert bulk g‐C3N4 into a stable hydrogel. The gelation occurs through delamination of the layered structure, driven by particular interactions between the IL and the carbon nitride sheets, forming an amphiphilic foam‐like network. This study employs spectroscopic and computational tools to unravel the gelation mechanism, and provides a rational approach toward the stabilization of 2D materials in hydrogels. The solution‐processable hydrogels can also be used as building blocks of complex devices. Chemiresistive gas sensors employing g‐C3N4 3D hydrogels exhibit superior response at room temperature, enabling effective gas sensing under low power conditions.