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Immobilization of a polar sulfone moiety onto the pore surface of a humid stable MOF for highly efficient CO2 separation under dry and wet environment through direct CO2-sulfone interaction

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dc.contributor.author Pal, Arun
dc.contributor.author Chand, Santanu
dc.contributor.author Madden, David G.
dc.contributor.author Franz, Douglas M.
dc.contributor.author Ritter, Logan
dc.contributor.author Space, Brian
dc.contributor.author Curtin, Teresa
dc.contributor.author Chand Pal, Shyam
dc.contributor.author Das, Madhab C.
dc.date.accessioned 2020-09-17T14:45:37Z
dc.date.issued 2020
dc.identifier.uri http://hdl.handle.net/10344/9231
dc.description peer-reviewed en_US
dc.description.abstract The stability of microporous metal–organic frameworks (MOFs) in moist environments must be taken into consideration for their practical implementations, which has been largely ignored thus far. Herein, we synthesized a new moisture-stable Zn-MOF, {[Zn2(SDB)2(L)2]·2DMA}n, IITKGP-12, by utilizing a bent organic linker 4,4′-sulfonyldibenzoic acid (H2SDB) containing a polar sulfone group (−SO2) and a N, N-donor spacer (L) with a Brunauer–Emmett–Teller surface area of 216 m2 g–1. This material displays greater CO2 adsorption capacity over N2 and CH4 with high IAST selectivity, which is also validated by breakthrough experiments with longer breakthrough times for CO2. Most importantly, the separation performance is largely unaffected in the presence of moisture of simulated flue gas stream. Temperature-programmed desorption (TPD) analysis shows the ease of the regeneration process, and the performance was verified for multiple cycles. In order to understand the structure–function relationship at the atomistic level, grand canonical Monte Carlo (GCMC) calculation was performed, indicating that the primary binding site for CO2 is between the sulfone moieties in IITKGP-12. CO2 is attracted to the bonded structure (V-shape) of the sulfone moieties in a perpendicular fashion, where CCO2 is aligned with S, and the CO2 axis bisects the SO2 axis. Thus, the strategic approach to immobilize the polar sulfone moiety with a high number of inherent stronger M–N coordination and the absence of coordination unsaturation made this MOF potential toward practical CO2 separation applications. en_US
dc.language.iso eng en_US
dc.publisher American Chemical Society en_US
dc.relation.ispartofseries ACS Applied Materials and Interfaces;12 (37), pp. 41177-41184
dc.relation.uri https://doi.org/10.1021/acsami.0c07380
dc.rights © 2020 ACS This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces , copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsami.0c07380 en_US
dc.subject breakthrough selectivity en_US
dc.subject CO2 capture and separations en_US
dc.subject GCMC calculation en_US
dc.subject humid-stable MOF en_US
dc.subject IAST selectivity en_US
dc.title Immobilization of a polar sulfone moiety onto the pore surface of a humid stable MOF for highly efficient CO2 separation under dry and wet environment through direct CO2-sulfone interaction en_US
dc.type info:eu-repo/semantics/article en_US
dc.type.supercollection all_ul_research en_US
dc.type.supercollection ul_published_reviewed en_US
dc.identifier.doi 10.1021/acsami.0c07380
dc.contributor.sponsor National Science Foundation en_US
dc.relation.projectid CRG/2019/001034 en_US
dc.relation.projectid DST/TM/EWO/MI/CCUS/21 en_US
dc.relation.projectid DMR-1607989 en_US
dc.relation.projectid CHE-1531590 en_US
dc.relation.projectid TG-DMR090028 en_US
dc.date.embargoEndDate 2021-08-17
dc.embargo.terms 2021-08-17 en_US
dc.rights.accessrights info:eu-repo/semantics/openAccess en_US


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