Preparation of ZnO@BD-g-C3N4 Nanoplate Catalysts Mediating Green and Efficient CO2–Epoxide Cycloaddition Reactions for the Synthesis of Cyclic Carbonates

Ahmet Kılıç

doi:10.1021/acs.energyfuels.5c05187

Preparation of ZnO@BD-g-C3N4 Nanoplate Catalysts Mediating Green and Efficient CO2–Epoxide Cycloaddition Reactions for the Synthesis of Cyclic Carbonates

2025-11-26

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Ahmet Kılıç *

E

Eyyup Yasar

H

Halil İbrahim Önal

F

Filiz Koyuncu

M

Murat Aydemir

F

Feyyaz Durap *

DOI：10.1021/acs.energyfuels.5c05187

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The production of green and economically attractive cyclic carbonates from CO2 as an alternative to the highly toxic and expensive method of phosgene gas is a well-established synthetic route in green chemistry. It is also consistent with achieving net-zero emissions and promoting 100% atom economy. This study presents the preparation and characterization of reusable ZnO@BD-g-C3N4 nanoplate catalysts (1–9), which feature abundant active sites and a dynamic oscillating active architecture and demonstrate a catalytic role in enhancing the fixation of CO2 to cyclic carbonates under ambient pressure conditions. The structure of the most active ZnO@BD-g-C3N4 nanoplate catalyst (1) was characterized by using FTIR spectroscopy, UV–DR spectroscopy, XRD, SEM-EDS, TEM, XPS, and BET techniques. The ZnO@BD-g-C3N4 nanoplate catalyst (1) showed the best catalytic activity with 98% conversion for epichlorohydrin (ECH) and 99% selectivity toward epichlorohydrin carbonate (ECHC) under appropriate conditions (ambient pressure, 100 °C, 4 h) without the need for any solvent. The ZnO@BD-g-C3N4 nanoplate catalyst (1) has been successfully tested with various terminal and internal epoxides under the same reaction conditions. Additionally, the synergic effect of Lewis acidic active centers resulted in an efficiency of over 93% and a selectivity of about 99% without a significant decrease in catalytic activity during five consecutive reaction cycles in the recyclability test for the ZnO@BD-g-C3N4/PPNCl catalytic system. In addition, kinetic studies of this cycloaddition reaction revealed that the reaction was pseudo-first-order under similar conditions. The rate constant at 100 °C was 0.8684 h 1, and the activation energy was 45.16 ± 2 kJ/mol.

Preparation of ZnO@BD-g-C3N4 Nanoplate Catalysts Mediating Green and Efficient CO2–Epoxide Cycloaddition Reactions for the Synthesis of Cyclic Carbonates

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