Water-stable direct air capture of CO₂ with microcapsules of task-specific ionic liquid and their electrothermal regeneration

Microcapsules of the task specific ionic liquid (TSIL) 1-ethyl-3-methylimidazolium 2-cyanopyrrolide [EMIM][2CNpyr] with composite polydimethylsiloxane (PDMS) shells were fabricated for use in CO₂ direct air capture (DAC) conditions. The TSIL was encapsulated using an oil-in-oil emulsion as a templating procedure through two different approaches. In the first approach, a PDMS-polyurea (PU) shell was constructed by interfacial polymerization, while in the second approach, a graphene oxide (GO)-PDMS shell was constructed by cross-linking GO sheets. The composition and structure of both capsule types were fully characterized, and their CO₂ DAC performance was evaluated by gravimetric and breakthrough analysis. Both capsules exhibited competitive capacities, with the PDMS-PU capsules and the GO-PDMS capsules reaching 0.75 mol kg⁻¹ and 0.66 mol kg⁻¹, respectively. We further demonstrate that both capsule systems can be regenerated with complementary electrothermal methods. Microwave (MW) regeneration was used for the PDMS-PU capsules, effectively releasing absorbed CO₂ in less than an hour. Owing to the electrical conductivity of GO, GO-PDMS capsules were regenerated via radio frequency heating (RF). This work highlights the importance and opportunity of tuning solid–liquid composite performance for advanced applications, including direct air capture of carbon dioxide.