Carbon dioxide is generated during the combustion of fossil fuels and has been linked to global climate change. CO2 could also be used as a source of carbon for the synthesis of fuels and chemicals. This project explores the possibility of hydrogenating CO2 to methanol, an attractive first product that can be used as a fuel or chemical precursor.The gas phase catalytic hydrogenation of CO2 to methanol has been intensively studied on Cu/ZnO based catalysts, however, the high operating temperature (> 200 �C) limits the selectivity to methanol, which is favored at low temperature. This presentation will describe a low temperature route to selectively produce methanol from CO2 over molybdenum carbide based (Mo2C) catalysts via a liquid phase reaction. Several recent works have identified the cascade system for converting CO2 to methanol through formic acid and alkyl formate intermediates using homogeneous catalysts [1]. The use of heterogeneous catalysts for this type of reaction has been limited [2]. We observed that the high surface area Mo2C (~ 100 m2/g) is highly active for formate hydrogenolysis, the rate determining step in this cascade system. The selectivity to methanol was enhanced, when nanoscale particles of Cu and/or Pd, the species that are active for methanol synthesis, were dispersed onto high surface area Mo2C. There also appeared to be a synergy between the metal and carbide. The results indicated the viability of employing metal supported Mo2C in the tandem conversion of CO2 to methanol. We also observed that these metal/Mo2C catalysts were capable of converting formic acid to methanol without the formate intermediate. This finding will simplify the current 3-step cascade system into a 2-step sequence, increasing the efficiency of the overall process.This work is supported by the NSF under the CCI Center for Enabling New Technologies through Catalysis (CENTC) Phase II Renewal, CHE-1205189.References[1] C. Huff, M. Sanford, J. Am. Chem. Soc. 133 (2011) 18122[2] L. Fan, Y. Sakaiya, K. Fujimoto, Appl. Catal. A-Gen. 180 (1999)  L11.

Liquid phase CO<sub>2</sub> hydrogenation to methanol over Mo<sub>2</sub>C-based catalysts

247th National Meeting (2014)

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Liquid phase CO2 hydrogenation to methanol over Mo2C-based catalysts

Liquid phase CO₂ hydrogenation to methanol over Mo₂C-based catalysts