LAUSR

Abstract Various porous solid sorbents in the form of powder or monoliths have been developed over the last years, as a promising solution for reducing CO2 emissions. Although powder sorbents, due to higher porosities and efficient mass transport, exhibit higher capacities compared with monoliths, several factors limit their suitability for practical application. The most prominent is their low bulk density, which makes them difficult to handle and poses health risks due to dust inhalation. In this work, we prepared robust hierarchically porous carbon-based monoliths based on a simple three-step approach with the focus on combining efficient CO2 adsorption and transport with easy handling for practical applications. The approach is based on incorporation of polystyrene nanoparticles (PS NPs) and expanded graphite (EG) into a nitrogen-rich precursor, which is polymerized to form 3D monoliths. Incorporation of thermally unstable PS NPs or thermally stable EG enables us to control the formation of macropores during a precarbonization step, while variation of KOH concentration and mixing intensity during a subsequent activation step controls the formation of micropores. The resulting hierarchically porous monoliths with high nitrogen contents exhibited CO2 uptake capacities reaching 6.52 mmol g−1 at 273.15 K and 1 bar, which is among the highest reported for porous carbon monoliths. In addition, the materials also exhibited good reversibility of CO2 adsorption over several cycles with simple regeneration under mild conditions. Considering the high CO2 capture performance together with improvements in sorbent properties such as easy handling and reusability, the presented sorbents are promising candidates for practical applications.