With ever growing concerns over increased anthropogenic carbon dioxide concentrations, we have developed a catalytic system to convert carbon dioxide to methanol. In this system, carbon dioxide, a greenhouse gas, can be converted into methanol, an important building block for the generation of other commodity and fine chemicals. This system utilizes a PNP-based ruthenium catalyst to hydrogenate carbon dioxide to formic acid, which then undergoes an amidation reaction with cocatalytic amine to form the corresponding amide. The amide can finally be hydrogenated by the same ruthenium catalyst to generate methanol and regenerate the amine. Current research efforts aim to develop better catalysts, both in terms of reactivity and stability, by investigating electronically and sterically different substituents on the phosphorous atoms. A suite of five different catalysts were synthesized and tested in amide hydrogenation, amide hydrogenation in the presence of carbon dioxide, carbon dioxide hydrogenation, and finally, conversion of carbon dioxide to methanol. In addition, in-situ high pressure Raman monitoring was used to gain important kinetic information for each of the catalysts, as well as aid in elucidating a mechanism for the conversion of carbon dioxide to methanol operable in this system. The catalytic, kinetic, and mechanistic information gained has resulted in an overall better understanding of the system, ultimately resulting in higher yields of methanol.

Cascade conversion of carbon dioxide to methanol: New catalytic, kinetic, and mechanistic insights

251st National Meeting (2016)

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