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Direct Synthesis of Dimethyl Carbonate from Methanol and Carbon Dioxide Catalyzed by Cerium-Based High-Entropy Oxides

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DOI: 10.1007/s10562-023-04303-4

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High entropy oxide; Catalyst; Dimethyl carbonate; Anchoring method; Oxygen vacancy

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Fluorite high entropy oxides (HEOs) were synthesized and used as catalysts for synthesis of dimethyl carbonate (DMC) from methanol and carbon dioxide. The yield of DMC reached 7.6 mmol/g under specific reaction conditions. The structure of HEOs containing Ce, La, Pr, Sm, and Y elements was characterized and the synergistic effect among these elements improved the reaction rate.
Fluorite high entropy oxides (HEOs) were synthesized by anchoring method and Ce-0.5(LaPrSmY)(0.5)O2-y used as catalysts for synthesis of dimethyl carbonate (DMC) from methanol (CH3OH) and carbon dioxide (CO2), the yield of DMC was up to 7.6 mmol/g at 140 celcius and 8.0 MPa. Under the same reaction conditions, the time to reach reaction equilibrium was reduced by half compared HEOs with CeO2. The structure of HEOs were characterized by X-ray diffraction (XRD), specific surface area and pore size analyzer (BET), high-resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS). The results showed that there are five metal elements of Ce, La, Pr, Sm and Y in the lattice of layered fluorite-type HEOs Ce-x(LaPrSmY)(1-x)O2-y. The synergistic effect among the elements led to the lattice distortion and the generation of a large number of oxygen vacancies, which improved the reaction rate. [GRAPHICS] .

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