Carbon Dioxide as a Direct Chemical Feedstock

Project Details

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)

Senior Investigators 

Cascade Catalytic Process for Carbon Dioxide to Methanol

Recent Publications and Patents

  • Chen, Y.; Choi, S.; Thompson, L. T. "Low-Temperature CO2 Hydrogenation to Liquid Products via a Heterogeneous Cascade Catalytic System", ACS Catal., 2015, 5, 1717-1725.
    (DOI: /10.1021/cs501656x)
  • Pitman, C. L.; Miller, A. J. M. "Molecular Photoelectrocatalysts for Visible Light-Driven Hydrogen Evolution from Neutral Water", ACS Catal., 2014, 4, 2727-2733.
    (DOI: 10.1021/cs500441f)
  • Miller, A. J. M.; Kaminsky, W.; Goldberg, K. I. "Arene Activation at Iridium Facilitates C–O Bond Cleavage of Aryl Ethers", Organometallics, 2014, 33, 1245-1252. (DOI: 0.1021/om5000166)
  • Miller, A. J. M.; Heinekey, D. M.; Mayer, J. M.; Goldberg, K. I. "Catalytic Disproportionation of Formic Acid to Generate Methanol", Angew. Chem. Int. Ed., 2013, 52, 3981-3984. (DOI: 10.1002/anie.201208470)
  • Brewster, T. P.; Miller, A. J. M.; Heinekey, D. M.; Goldberg, K. I. "Hydrogenation of Carboxylic Acids Catalyzed by Half-Sandwich Complexes of Iridium and Rhodium", J. Am. Chem. Soc., 2013, 135, 16022-16025.(DOI: 10.1021/ja408149n) 
  • Huff, C. A.; Sanford, M. S. "Catalysis CO₂Hydrogenation to Formate by a Ruthenium Pincer Complex", ACS Catal., 2013, 3, 2412-2416. (DOI: 10.1021/cs400609u)
  • Huff, C. A.; Kampf, J. W.; Sanford, M. S. "Reversible carbon-carbon bond formation between carbonyl compounds and a ruthenium pincer complex", Chem. Commun., 2013, 49, 7147-7149. (DOI: 10.1039/c3cc43517b)
  • Goldberg, K. I.; Heinekey, D. M.; Mayer, J. M.; Miller, A. J. M.; Brewster, T. P. "Hydrogenation and Disproportionation Catalysis,” International Patent Application PCT/US2014/017465 filed February 20, 2014.

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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).

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