Shape‐Customizable Macro‐/Microporous Carbon Monoliths for Structure‐to‐Functionality CO2 Adsorption and Novel Electrical Regeneration

Abstract Potential of porous carbons for practical applications is often limited by their intrinsic fragility and poor processability. Here, a facile approach to fabricate hierarchically macro‐/microporous carbon monolith (CM) with high strength and integrated structure is developed, which offers great possibilities for structure‐to‐functionality applications. Through a fiber‐reinforced sol–gel process and an ambient pressure drying approach, aerogel‐like CMs can be designed and fabricated in customizable forms. In particular, a novel scroll‐type carbon monolith (S‐CM) is constructed, which can mimic a roll‐to‐roll tube reactor and thus avoid the packing problems arising from the granules or powders of conventional activated carbons. The resulting CM exhibits a high CO 2 adsorption capacity of 15.9 mmol g −1 at 25 bar and a breakthrough capacity of 1 mmol g −1 at 1 bar. Moreover, owing to the integrated structure and good electrical conductivity, the scroll‐type S‐CM can be easily regenerated by employing a low‐energy electrothermal desorption technique. The specialized design of the CMs should fulfill industrial directives and may provide an access route to more efficient porous carbons for structure‐oriented and process‐intensified applications.