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In the transition to a clean-energy future, CO 2 separations will play a critical role in mitigating current greenhouse gas emissions and facilitating conversion to cleaner-burning and renewable fuels. New materials with high selectivities for CO 2 adsorption, large CO 2 removal capacities, and low regeneration energies are needed to achieve these separations efficiently at scale. Here, we present a detailed investigation of nine diamine-appended variants of the metal-organic framework Mg 2 (dobpdc) (dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) that feature step-shaped CO 2 adsorption isotherms resulting from cooperative and reversible insertion of CO 2 into metal-amine bonds to form ammonium carbamate chains. Small modifications to the diamine structure are found to shift the threshold pressure for cooperative CO 2 adsorption by over 4 orders of magnitude at a given temperature, and the observed trends are rationalized on the basis of crystal structures of the isostructural zinc frameworks obtained from in situ single-crystal X-ray diffraction experiments. The structure-activity relationships derived from these results can be leveraged to tailor adsorbents to the conditions of a given CO 2 separation process. The unparalleled versatility of these materials, coupled with their high CO 2 capacities and low projected energy costs, highlights their potential as next-generation adsorbents for a wide array of CO 2 separations.

Controlling Cooperative CO2 Adsorption in Diamine-Appended Mg2(dobpdc) Metal–Organic Frameworks

Controlling Cooperative CO₂ Adsorption in Diamine-Appended Mg₂(dobpdc) Metal–Organic Frameworks