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We evaluated bismuth doped cerium oxide catalysts for the continuous synthesis of dimethyl carbonate (DMC) from methanol and carbon dioxide in the absence of a dehydrating agent. Bi  x  Ce 1− x  O  δ   nanocomposites of various compositions ( x  = 0.06–0.24) were coated on a ceramic honeycomb and their structural and catalytic properties were examined. The incorporation of Bi species into the CeO 2  lattice facilitated controlling of the surface population of oxygen vacancies, which is shown to play a crucial role in the mechanism of this reaction and is an important parameter for the design of ceria-based catalysts. The DMC production rate of the Bi  x  Ce 1− x  O  δ   catalysts was found to be strongly enhanced with increasing O v  concentration. The concentration of oxygen vacancies exhibited a maximum for Bi 0.12 Ce 0.88 O  δ  , which afforded the highest DMC production rate. Long-term tests showed stable activity and selectivity of this catalyst over 45 h on-stream at 140 °C and a gas-hourly space velocity of 2,880 mL·g cat  −1 ·h −1 .  In-situ  modulation excitation diffuse reflection Fourier transform infrared spectroscopy and first-principle calculations indicate that the DMC synthesis occurs through reaction of a bidentate carbonate intermediate with the activated methoxy (−OCH 3 ) species. The activation of CO 2  to form the bidentate carbonate intermediate on the oxygen vacancy sites is identified as highest energy barrier in the reaction pathway and thus is likely the rate-determining step.

nano research

Continuous dimethyl carbonate synthesis from CO2 and methanol over BixCe1−xOδ monoliths: Effect of bismuth doping on population of oxygen vacancies, activity, and reaction pathway