Abstract
This study explores the catalytic efficacy of fluorine-modified 1 wt% copper oxide on MCM-41 (F-1Cu/MCM-41) in carbon dioxide cycloaddition reactions. It delves into reaction mechanisms, active sites, and the practical applicability of the catalyst. Comprehensive examination through in situ diffuse reflectance infrared Fourier transform spectroscopy and other analytical methods substantiated the role of halogen-modified mono-dispersed copper species in carbon dioxide activation and silicon hydroxide sites in epoxide activation, while underscoring the role of Lewis bases and Brønsted acids. Kinetic studies and density functional theory calculations pinpointed carbon dioxide activation as the pivotal step. Furthermore, the catalyst exhibited robust stability and efficiency in continuous flow experiments, sustaining a 99% selectivity towards cyclic carbonate over 150 h. An eco-friendly evaluation confirmed the sustainability of the process, emphasizing its minimal environmental footprint and high efficiency. These results establish fluorine-modified 1 wt% copper oxide on MCM-41 as a formidable candidate for industrial-scale cyclic carbonate production, due to its promising performance and sustainability.
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