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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. 

Solid–liquid composites (SLCs) combine the properties of solids and liquids, enhancing functionalities and expanding potential applications. Traditional methods for creating SLCs often face challenges such as low mass transfer efficiency, difficulty in controlling separation behavior, and substantial waste production. Herein, we report a new approach to solve these challenges by using disulfide-based responsive polymeric capsule shells to make liquid-filled monoliths for carbon capture. The capsules are prepared through interfacial polymerization and contain either non-polar poly(α-olefin)432 or highly polar 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([HMIM][TFSI]) at 74–82 wt%. Upon gentle heating, the dynamic disulfide bonds of the isolated capsules undergo bond exchange, leading to the fusion of capsule shells into free-standing monoliths that retain >89 wt% of their liquid core and remain stable for at least two weeks. These monoliths demonstrate CO2 absorption rates and capacities comparable to their capsule counterparts; further, in response to radiofrequency (RF), they reach the CO2 desorption temperature in only ∼31 s. This innovative system addresses the limitations of conventional SLC fabrication techniques, offering a versatile and practical approach to fusing polymer capsule shells for applications across separation, energy storage, and carbon capture applications.