Journal of Synthetic Crystals, Volume. 50, Issue 1, 113(2021)
Preparation of MeCeOx(Me=In, Zr) Solid Solution Catalyst for the Application in the Synthesis of Dimethyl Carbonate
MeCeOx (Me=In, Zr) bimetallic oxide catalysts were prepared by liquid-phase co-precipitation method with a matrix of CeO2. The physiochemical properties of MeCeOx were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction(H2-TPR), temperature programmed desorption(CO2-TPD, CH3OH-TPD), and diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) techniques. Based on the systematic investigation of the types and doping amounts of various metal oxides, the structure properties and catalytic behavior of solid solution catalysts prepared by doping CeO2 with different metal oxides were comparatively studied in this paper. The results show that the solid solution structure formed by MeCeOx bimetal oxide catalysts increases the concentration of oxygen vacancy defects. The InCeOx solid solution catalyst exhibit the largest concentration of oxygen vacancy defects, resulting in the improve chemical adsorption for CO2 and CH3OH molecules. Under the condition of reaction pressure 1.0 MPa, reaction temperature 140 ℃, reaction space velocity (GHSV) 3 600 mL/(g·h) and V(CO2)/V(CH3OH)/V(N2)=4∶1∶5, the InCeOx shows the excellent catalytic performance with dimethyl carbonate selectivity of 91.3%, CH3OH conversion of 8.4%, and dimethyl carbonate STY(Space Time Yield) of 0.11 gDMC·h-1·g-1cat. In addition, further in-depth DRIFTS study show that activation of CO2 with oxygen vacancies and the formation of terminal methoxy as the intermediate are the crucial to the enhance selectivity of dimethyl carbonate.
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WANG Yizhou, LIU Fei, ZHAO Tianxiang, CAO Jianxin, XU Fang. Preparation of MeCeOx(Me=In, Zr) Solid Solution Catalyst for the Application in the Synthesis of Dimethyl Carbonate[J]. Journal of Synthetic Crystals, 2021, 50(1): 113
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Received: Aug. 19, 2020
Accepted: --
Published Online: Apr. 15, 2021
The Author Email: Yizhou WANG (1063505411@qq.com)
CSTR:32186.14.