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The catalytic conversion of methanol to hydrocarbons is an important way to prepare liquid fuels and chemicals from non-petroleum routes. Since the discovery of molecular sieves as effective catalysts in the 1970s, significant progress has been made in the targeted conversion of methanol to hydrocarbons, and the methanol selective olefins (MTG/O/P) technology has achieved industrialization. However, the catalytic conversion of methanol is extremely complicated and the reaction mechanism has not been clearly understood. Although the "hydrocarbon pool" mechanism is generally considered to play a leading role, it cannot explain the origin of the "hydrocarbon pool" species. Therefore, the formation mechanism of the initial CC bond is considered to be one of the most challenging topics in the field of heterogeneous catalysis in the past 40 years.
Recently, the 603 Group of the Institute of Coal Chemistry, Chinese Academy of Sciences, China, through the pulse reaction, on-line spectral characterization and isotope labeling experiments, combined with the density functional theory calculations thoroughly explored the initial reaction process of methanol conversion, and effectively confirmed the existence of direct reaction mechanism. intermediate active species CH3OCH2 +, discloses the initial reaction of dimethyl ether, the initial formation mechanism of CH 4 and olefin products, the CO bond to clarify the mechanism of CC bonds transition proposed reasonably practicable direct reaction mechanism - methoxymethyl The positive ion mechanism clearly explained the origin of the CC bond and found that the initial olefin product was propylene, which was the source of the “hydrocarbon pool†species, and achieved a perfect connection between the direct reaction mechanism and the “hydrocarbon pool†mechanism. This achievement lays the foundation for deep understanding of the evolution and action mechanism of "hydrocarbon pool" species and its organic relationship with catalytic performance, and also provides a strong theoretical support for the design and development of highly selective methanol catalysts with high stability.
Related research results were published in J. Catal., 2014, 317, 277–283; Chem. Soc. Rev., 2015, 44, 7155–7176; J. Phys. Chem. C, 2016, 120, 6075–6087; Catal Sci. Technol., 2016, DOI: 10.1039/C6CY00506C.
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