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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 CO₂chemisorption 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 KHCO₃CD‐MOF possesses rapid and high‐capacity CO₂uptake, good thermal, oxidative, and cycling stabilities, and selective CO₂capture under mixed gas conditions. Because of its low cost and performance under realistic conditions, KHCO₃CD‐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 CO₂capture.