Confinement effects facilitate low-concentration carbon dioxide capture with zeolites

• Published in: Proceedings of the National Academy of Sciences - PNAS Vol. 119; no. 39; pp. 1 - e2211544119
• Main Authors: Fu, Donglong, Park, Youngkyu, Davis, Mark E.
• Format: Journal Article
• Language: English
• Published: Washington National Academy of Sciences 27.09.2022
• Subjects: Adsorbents; Adsorption; Aluminum; Carbon dioxide; Carbon dioxide concentration; Carbon sequestration; Cations; Heat of adsorption; Low concentrations; Physical Sciences; Topology; Zeolites
• ISSN: 0027-8424; 1091-6490
• DOI: 10.1073/pnas.2211544119

Engineered systems designed to remove CO 2 from the atmosphere need better adsorbents. Here, we report on zeolite-based adsorbents for the capture of low-concentration CO 2 . Synthetic zeolites with the mordenite (MOR)-type framework topology physisorb CO 2 from low concentrations with fast kinetics, low heat of adsorption, and high capacity. The MOR-type zeolites can have a CO 2 capacity of up to 1.15 and 1.05 mmol/g for adsorption from 400 ppm CO 2 at 30 °C, measured by volumetric and gravimetric methods, respectively. A structure–performance study demonstrates that Na + cations in the O33 site located in the side-pocket of the MOR-type framework, that is accessed through a ring of eight tetrahedral atoms (either Si 4+ or Al 3+ : eight-membered ring [8MR]), is the primary site for the CO 2 uptake at low concentrations. The presence of N 2 and O 2 shows negligible impact on CO 2 adsorption in MOR-type zeolites, and the capacity increases to ∼2.0 mmol/g at subambient temperatures. By using a series of zeolites with variable topologies, we found the size of the confining pore space to be important for the adsorption of trace CO 2 . The results obtained here show that the MOR-type zeolites have a number of desirable features for the capture of CO 2 at low concentrations.