Electrochemical promotion of the CO2 hydrogenation reaction using thin Rh, Pt and Cu films in a monolithic reactor at atmospheric pressure

摘要

A monolithic electropromoted reactor (MEPR) with up to 22 thin Rh/YSZ/Pt or Cu/TiO2/YSZ/Au plate cells was used to investigate the hydrogenation of CO2 at atmospheric pressure and temperatures 220-380 °C. The Rh/YSZ/Pt cells lead to CO and CH4 formation and the open-circuit selectivity to CH4 is less than 5%. Both positive and negative applied potentials enhance significantly the total hydrogenation rate but the selectivity to CH4 remains below 12%. The Cu/TiO2/YSZ/Au cells produce CO, CH4 and C2H4 with selectivities to CH4 and C2H4 up to 80% and 2%. Both positive and negative applied potential significantly enhance the hydrogenation rate and the selectivity to C2H4. It was found that the addition of small (~0.5 kPa) amounts of CH3OH in the feed has a pronounced promotional effect on the reaction rate and selectivity of the Cu/Ti02/YSZ/Au cells. The selective reduction of CO2 to CH4 starts at 220 °C (vs 320 °C in absence of CH3OH) with near 100% CH4 selectivity at open-circuit and under polarization conditions at temperatures 220-380 °C. The results show the possibility of direct CO2 conversion to useful products in a MEPR via electrochemical promotion at atmospheric pressure.