Reactive separations couples separation and conversion processes in the same medium in order to increase the energy efficiency of CO2 capture and conversion. The last step of reactive separations, the conversion of CO2, involves the design of new reactive landscapes for which molecular-level control is crucial. Hence, we evaluate the feasibility of cycloadditions of CO2 bound to various carbon-capture solvents, where the CO2-loaded solvent serves as the dienophile. While these reactions are widely applied for the synthesis of various products, historically, they have not been applied to CO2 that is chemically fixated in solution. Here, we particularly focus on water-lean solvents for CO2 capture, due to their promising improvements in energy efficiency for post-combustion capture from power plants. Through a synergistic cycle of quantum chemical calculations, machine learning techniques, and experimental validation, we are able to i) identify whether a given carbon-capture solvent prefers the inverse or normal demand reaction and ii) select the most promising diene functional groups for reducing the activation energy.

Computational screening of cycloaddition reactions for the reactive separation of CO2

ACS Spring 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.