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We report an approach for soft-template encapsulation of PCMs vita organocatalyzed photoredox ATRP using silica surfactants with surface-immobilized initiators. 

Microencapsulation of pristine core liquids in polymer shells has critical applications in thermal energy storage and management, targeted drug delivery, and carbon capture, among others. Herein, we report a novel encapsulation approach based on a double emulsion soft-template to produce microcapsules comprised of an ionic liquid (IL) core in a degradable polymer shell. We demonstrate the production of [IL-in-oil1]-in-oil2 (IL/O1/O2) double emulsions, in which the oil interphase (O1) contains a CO2-derived polycarbonate bearing vinyl pendant groups, tetrathiol small molecule crosslinker, and photoinitiator; upon irradiation of the double emulsion under low shear, thiol–ene crosslinking of the loaded species results in the formation of a robust shell around the pure IL droplets. The core–shell structures have enhanced physisorption for CO2 uptake compared to the bulk IL, which is consistent with the combined capacity of the IL/shell alone and demonstrates more rapid uptake due to an enhanced gas–liquid interface. This approach to microencapsulation of functional liquids offers researchers a distinct route to fabricate composite architectures with a pristine core for applications in separations, transport of cargo, and gas uptake.