The reaction network of oxidative carbonylation of methanol (CH3OH) over CuY catalyst prepared by solid-state ion exchange of HY zeolite with CuCl was enriched by combination of in-situ diffuse reflectance infrared fourier transform spectroscopy and mass spectrometric. Based on the proposed mechanism of dimethyl carbonate formation on CuY in literature, this study mainly focused on the origin of the O atom in methoxyl and the reaction pathway for by-products formation. The interaction of the catalyst with different reactants and reactant mixtures (CH3OH, CH318OH, HCHO, O2, CH3OH/HCHO and CH318OH/CO/O2) was studied in detail. It was found that in the presence of CuOx or oxygen, methoxide species are generated by breaking of the O–H bond. Reaction of methoxide species with oxygen leads to the formation of formaldehyde (HCHO), followed by the generation of formate species through consecutive oxidation of HCHO.
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The financial supports from the National Natural Science Foundation of China (NSFC) (21406120), the Program of Introducing Talents of Discipline to Universities (BP0618007) and the China Postdoctoral Science Foundation (2019M661021) are gratefully acknowledged.
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Lv, J., Chen, P., Wang, M. et al. Supplementary Mechanism for Oxycarbonylation of Methanol Over CuY Catalyst: Origin of the Oxygen Atom in Methoxyl and Formation of By-Products. Catal Lett (2021). https://doi.org/10.1007/s10562-021-03572-1
- Oxidative carbonylation
- In situ DRIFTS