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Direct Synthesis of Dimethyl Carbonate from CO2 and Methanol over CaO-CeO2 Catalysts: The Role of Acidic-basic properties and Surface Oxygen Vacancies

Abstract

Direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol was investigated over a series of CeO2 based catalysts promoted by variable amount of CaO. The catalysts were synthesized by co-precipitation method and fully characterized using powder X-ray diffraction (XRD), N2 adsorption, transmission electron microscopy (TEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), NH3-TPD and CO2-TPD techniques. The results demonstrated that the addition of different amounts of CaO could affect the structure and surface properties of the obtained catalysts. The acidic-basic properties and amounts of surface oxygen vacancies of the catalysts were improved by the interaction of CaO and CeO2. The oxygen vacancies enhanced the adsorption of CO2. The DMC synthesis from CO2 and methanol was studied in a slurry bed reactor at 3 MPa and 140 oC. The catalytic results revealed that the acidic-basic properties and oxygen vacancies play a crucial role in improving the DMC formation. Among all the bimetallic and pure CeO2 catalysts, Ca1.5Ce sample showed the maximum DMC yield (2.47 mmol/g) due to the modification of acidic-basic properties of the catalyst and the existence of higher concentration of oxygen vacancies on CeO2 surface.

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Publication details

The article was received on 18 Jul 2017, accepted on 30 Aug 2017 and first published on 30 Aug 2017


Article type: Paper
DOI: 10.1039/C7NJ02606D
Citation: New J. Chem., 2017, Accepted Manuscript
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    Direct Synthesis of Dimethyl Carbonate from CO2 and Methanol over CaO-CeO2 Catalysts: The Role of Acidic-basic properties and Surface Oxygen Vacancies

    B. Liu, L. Congming, G. Zhang, L. Yan and Z. Li, New J. Chem., 2017, Accepted Manuscript , DOI: 10.1039/C7NJ02606D

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