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Carbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation-Resistant Cyclodextrin-Based Metal-Organic Frameworks.

cam.depositDate2022-05-19
cam.issuedOnline2022-06-10
cam.orpheus.success2022-05-19 - Embargo set during processing via Fast-track
dc.contributor.authorZick, Mary E
dc.contributor.authorPugh, Suzi M
dc.contributor.authorLee, Jung-Hoon
dc.contributor.authorForse, Alexander C
dc.contributor.authorMilner, Phillip J
dc.contributor.orcidZick, Mary E [0000-0002-3819-5347]
dc.contributor.orcidForse, Alexander C [0000-0001-9592-9821]
dc.contributor.orcidMilner, Phillip J [0000-0002-2618-013X]
dc.date.accessioned2022-05-19T23:30:37Z
dc.date.available2022-05-19T23:30:37Z
dc.date.issued2022-07-25
dc.date.updated2022-05-19T10:51:55Z
dc.description.abstractCarbon capture and sequestration (CCS) from industrial point sources and direct air capture are necessary to combat global climate change. A particular challenge faced by amine-based sorbents-the current leading technology-is poor stability towards O2 . Here, we demonstrate that CO2 chemisorption in γ-cylodextrin-based metal-organic frameworks (CD-MOFs) occurs via HCO3 - formation at nucleophilic OH- sites within the framework pores, rather than via previously proposed pathways. The new framework KHCO3 CD-MOF possesses rapid and high-capacity CO2 uptake, good thermal, oxidative, and cycling stabilities, and selective CO2 capture under mixed gas conditions. Because of its low cost and performance under realistic conditions, KHCO3 CD-MOF is a promising new platform for CCS. More broadly, our work demonstrates that the encapsulation of reactive OH- sites within a porous framework represents a potentially general strategy for the design of oxidation-resistant adsorbents for CO2 capture.
dc.format.mediumPrint-Electronic
dc.identifier.doi10.17863/CAM.84741
dc.identifier.eissn1521-3773
dc.identifier.issn1433-7851
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/337327
dc.language.isoeng
dc.publisherWiley
dc.publisher.departmentDepartment of Chemistry
dc.publisher.urlhttp://dx.doi.org/10.1002/anie.202206718
dc.rightsAll Rights Reserved
dc.rights.urihttp://www.rioxx.net/licenses/all-rights-reserved
dc.subjectAdsorption
dc.subjectCarbon Storage
dc.subjectHydrogen Bonds
dc.subjectMetal-Organic Frameworks
dc.subjectNMR Spectroscopy
dc.titleCarbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation-Resistant Cyclodextrin-Based Metal-Organic Frameworks.
dc.typeArticle
dcterms.dateAccepted2022-05-17
prism.publicationDate2022
prism.publicationNameAngew Chem Int Ed Engl
pubs.funder-project-idLeverhulme Trust (RPG-2020-337)
pubs.funder-project-idMRC (MR/T043024/1)
pubs.licence-display-nameApollo Repository Deposit Licence Agreement
pubs.licence-identifierapollo-deposit-licence-2-1
rioxxterms.typeJournal Article/Review
rioxxterms.versionAM
rioxxterms.versionofrecord10.1002/anie.202206718

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