Carbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation-Resistant Cyclodextrin-Based Metal-Organic Frameworks.
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Publication Date
2022-05-17Journal Title
Angew Chem Int Ed Engl
ISSN
1433-7851
Publisher
Wiley
Type
Article
This Version
AM
Physical Medium
Print-Electronic
Metadata
Show full item recordCitation
Zick, M. E., Pugh, S. M., Lee, J., Forse, A., & Milner, P. J. (2022). Carbon Dioxide Capture at Nucleophilic Hydroxide Sites in Oxidation-Resistant Cyclodextrin-Based Metal-Organic Frameworks.. Angew Chem Int Ed Engl https://doi.org/10.1002/anie.202206718
Abstract
Carbon 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.
Keywords
NMR spectroscopy, adsorption, carbon storage, hydrogen bonds, metal-organic framework
Sponsorship
Leverhulme Trust (RPG-2020-337)
MRC (MR/T043024/1)
Embargo Lift Date
2023-05-17
Identifiers
External DOI: https://doi.org/10.1002/anie.202206718
This record's URL: https://www.repository.cam.ac.uk/handle/1810/337327
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