Transformation of CO2 and glycerol to glycerol carbonate over CeO2ZrO2 solid solution —— effect of Zr doping
Ce 1-x Zr x O 2 (0 ≤ x ≤ 0.2) solid solutions were prepared by hydrothermal method and applied for the synthesis of glycerol carbonate from glycerol and CO 2 in the presence of 2-cyanopyridine (dehydrant) with dimethyl formamide (DMF) as a solvent. The physicochemical properties of the catalysts were characterized by ICP, XRD , BET, H 2 -TPR, CO 2 /NH 3 -TPD, TEM and XPS . The activation route of CO 2 and glycerol were measured by DRIFTS and FT-IR. Compared to pure CeO 2 , Ce 1-x Zr x O 2 solid solutions exhibited enhanced activity in the present reaction system, and the improved catalytic activity was associated with the BET surface area and the acid-base properties. DRIFTS results showed that the chelating bidentate carbonate species was the main adsorption pattern for CeO 2 and no striking differences between Ce 0·98 Zr 0·02 O 2 and CeO 2 . FT-IR spectra of the spent catalysts revealed that glycerol and 2-cyanopyridine could be activated on CeO 2 -based catalysts, and an ester intermediate was formed for the production of glycerol carbonate. Thus, a plausible mechanism is proposed for the synthesis of glycerol carbonate from glycerol and CO 2 in the presence of 2-cyanopyridine in DMF solvent over CeO 2 -based catalysts. Moreover, the recyclability of Ce 0·98 Zr 0·02 O 2 was measured and the catalysts could be regenerated through a simple calcination process at 400 °C for 5 h in air.
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