Abstract
Developing an effective catalyst for converting CO2 into high-value chemicals is greatly desirable but remains a big hurdle. Herein, Zr-MOF derivative-bearing hydrazino groups were synthesized by mixing the ligands of terephthalic acid and 4-hydrazinobenzoic acid (HBA), resulting in UiO-66-HBA as heterocatalyst for epoxide cycloaddition with CO2. Compared to UiO-66, the optimal UiO-66-HBA0.2 displayed outstanding activity for epichlorohydrin cycloaddition, with 96.03 % cyclocarbonate yield under 0.1 MPa CO2 at 70 ℃. The great activity of UiO-66-HBA0.2 was attributed to the synergistic cooperation of Lewis base offered by HBA moiety and Lewis acid originated from Zr6 clusters, which was affirmed by NH3/CO2-temperature-programmed desorption experiments and CO2 adsorption isotherms. Moreover, UiO-66-HBA0.2 exhibited excellent stability and great substrate compatibility. In addition, a possible mechanism for catalyzing CO2 conversion into cyclocarbonate was suggested. This study provides an effective way to design functionalized MOFs-based heterocatalysts for CO2 utilization.
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