Journal
CHINESE CHEMICAL LETTERS
Volume 34, Issue 7, Pages -Publisher
ELSEVIER SCIENCE INC
DOI: 10.1016/j.cclet.2022.107814
Keywords
Non-3d metal modulation; Metal-organic framework; CO 2 fixation; Flue gas; Cycloaddition reaction
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Two new Zn(II) imidazolate frameworks incorporating MoO4 2- or WO4 2- units were reported, which can catalyze the cycloaddition of CO2 and epichlorohydrin at room temperature and atmospheric pressure, achieving high yields. The modulation mechanisms of the MoO4 2- unit in optimizing the electronic structure of Zn(II) center were revealed.
Cycloaddition of CO2 and epoxide into cyclic carbonate is one of the most efficient ways for CO2 conver-sion with 100% atom-utilization. Metal-organic frameworks are a kind of potential heterogeneous cata-lysts, however, high temperature, high pressure, and high-purity CO2 are still required for the reaction. Here, we report two new Zn(II) imidazolate frameworks incoporating MoO4 2- or WO4 2- units, which can catalyse cycloaddition of CO2 and epichlorohydrin at room temperature and atomospheric pressure, giv-ing 95% yield after 24 h in pure CO2 and 98% yield after 48 h in simulated flue gas (15% CO2 + 85% N 2 ), respectively. For comparison, the analogic Zn(II) imidazolate framework MAF-6 without non-3d metal ox-ide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO4 2- unit in optimizing the electronic structure of Zn(II) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations. (c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
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