Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 9, Issue 16, Pages 4255-4261Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy00739c
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Funding
- National Science Foundation of China [21777149]
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A zinc 2-N-methyl N-confused porphyrin (Zn(NCP)Cl) catalyst was developed for the solvent-free synthesis of cyclic carbonates from epoxides and CO2. Zn(NCP)Cl exhibited very high catalytic activity. Using this catalyst, a series of epoxides have been converted into the corresponding cyclic carbonates in high yields and selectivity (>99%). The turnover frequency (TOF) value reached 266 667 h(-1) for the conversion of CO2 with epichlorohydrin into cyclic carbonate at 120 degrees C and an initial CO2 pressure of 1.7 MPa within 3 h. Furthermore, an almost quantitative cyclic carbonate product was achieved under atmospheric CO2 within 24 h. X-ray structural analysis of Zn(NCP)Cl reveals that the Zn2+ ion is four-coordinate, surrounded by three nitrogen atoms from the N-confused porphyrin and a chlorine atom. Due to the strong electron-withdrawing ability of chloride, zinc shows strong acidity, thereby enhancing its ability to activate epoxide. Density functional theory calculations (DFT) suggest that the ring-opening of epoxide is the rate-determining step of the catalytic cycle.
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