This project aims to develop cascade catalytic methods to convert CO₂ into commercially relevant chemicals. Specifically, we are working to develop panels of catalysts that work in concert to promote the selective reduction of CO₂ to alcohols under mild conditions. Research has focused on two areas: (a) refining cascade catalysis through improved understanding of catalyst compatibility; and (b) discovery of new catalysts for specific steps in proposed cascade sequences. Building on our report of the first cascade catalytic conversion of CO₂ to CH₃ OH using three homogeneous catalysts, ¹ mechanistic studies have elucidated deactivation pathways, such as co-catalyst incompatibility and substrate inhibition of specific co-catalyst. This information has been used to guide the design of three second-generation catalyst systems.
Another focus of this project is use of homogeneous and heterogeneous catalysts in tandem. In addition to broadening the scope of available catalytic options, the heterogeneous materials tend to be more robust than their homogeneous counterparts. Also, to push towards more valuable chemicals, especially C₂ or higher organics, individual reaction steps are also being developed or improved.
Reference ¹: Huff, C. A.; Sanford, M. S. "Cascade Catalysis for the Homogeneous Hydrogenation of Carbon Dioxide to Methanol", J. Am. Chem. Soc., 2011, 133, 18122-18125. (DOI: 10.1021/ja208760j)
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This work was supported by NSF under the CCI Center for Enabling New Technologies Through Catalysis, CHE-1205189. Any opinions, findings, and conclusions or recommendations expressed here are those of the authors and do not necessarily reflect the views of the National Science Foundation (NSF).