A Stable Zn-Based Metal–Organic Framework as an Efficient Catalyst for Carbon Dioxide Cycloaddition and Alcoholysis at Mild Conditions
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Developing highly efficient heterogeneous catalysts for cycloaddition of CO2 and epoxides to produce cyclic carbonates is promising but challenging. In this work, a novel three-dimensional metal organic framework (MOF) with cylinder pore systems and unsaturated Zn sites has been demonstrated as potent candidate in CO2 fixation at mild and solvent-free conditions. The Zn(atz)(bdc)0.5, where atz = aminotriazole and H2bdc = terephthalic, exhibits microporous nature that can regulate the catalytic interaction of active centers and substrates. The structure stability has been systematically investigated and proven to be sufficient for practical application. Furthermore, the cooperative effects of porosity, CO2 binding affinity, activation centers, and synergism with co-catalyst have been deeply investigated. Moreover, high propylene epoxide conversion (97%) and selectivity (> 99%) have been achieved at mild conditions (60 °C and 1 MPa) with excellent cycle stability. Owing to the well-defined pore system, an obvious substrates selectivity has been clearly observed. A possible catalytic mechanism has been proposed and verified by DFT calculations. Furthermore, the prepared Zn-MOF can also be used as an efficient heterogeneous catalyst for the reaction of epoxides with alcohols to produce β-alkoxy alcohol.
KeywordsMetal organic frameworks Cycloaddition CO2 conversion Alcoholysis
This research work is partially supported by the National Natural Science Foundation of China (No.51672186 and 21908090), Natural Science Foundation of Jiangxi Province (No.20192ACB21015), and the start-up funds of Nanchang University and Arizona State University.
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Conflict of interest
The authors declare that they have no conflict of interests.