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Rauchfuss Group

Supramolecular Organometallic Chemistry in Separations and Catalysis

A project supported by the U. S. Department of Energy


Principal Investigator: Thomas B. Rauchfuss

International Collaborators:
Professor Ken Sakai, University of Kyushu

Coworkers:
Bryan Carlson, B.S. Texas Tech University
Wan-Yi (Amy) Chu, National Tawain University
James S. Lansing, B.S. University of Delaware
Dr. Hao Lei, Ph.D. University of California-Davis
Anthony Rohrer, undergraduate researcher
Mark Tokarski, undergraduate researcher
Xiaoyuan Zhou, Ph.D. University of Chicago

Overview.
In this project we apply organometallic chemistry to basic issues related to sustainability, i.e. energy processing and environmental remediation. The coordination chemistry of simple unfunctionalized ligands is mature, and but complexes of functional ligands is filled with opportunities, inspired by supramolecular chemistry, organocatalysis, and nanoscience. Molecules are larger than before and expectations for selectivity and green-ness are high. Synthesis plays a major role guided by in situ methods of analysis.


Representative Recent Publications

"Dioxygen and Hydrogen Peroxide Reduction with Hemocyanin Model Complexes", M. A.. Thorseth, C. S. Letko, T. B. Rauchfuss, A. A. Gewirth, Inorg. Chem. 2011, 50, 6158-6161.

"Coordination Chemistry of the Soft Chiral Lewis Acid [Cp*Ir(TsDPEN)]", C. S. Letko, Z. H. Heiden, T. B. Rauchfuss, Inorg. Chem. 2011, 50, 5558-5566.

"Activation and Deactivation of Cp*Ir(TsDPEN) Hydrogenation Catalysts in Water" C. S. Letko, Z. M. Heiden, T. B. Rauchfuss, Eur. J. Inorg. Chem. 2009, 4927-4930.

"Oxidative Addition of Thioesters to Fe(0): Active-Site Models For Hmd, Nature’s Third Hydrogenase" A. M. Royer, T. B. Rauchfuss, D. L. Gray, Organometallics 2009, 28, 3618-3620.

"Proton-Assisted Activation of Dihydrogen: Mechanistic Aspects of Proton-Catalyzed Addition of H2 to Ru and Ir Amido Complexes," Z. M.Heiden, T. B. Rauchfuss, J. Am Chem. Soc. 2009, 131, 3593-3600.

"Redox-Activation of Alkene Ligands in Platinum Complexes with Non-innocent Ligands," J. L.Boyer, T. R. Cundari, N. J. DeYonker, T. B. Rauchfuss, S. R. Wilson, Inorg. Chem., 2009, 49, 638-645.

"Supramolecular Architectures Based on Organometallic Half-sandwich Complexes", T. B. Rauchfuss, K. Severin, in Molecular Nanostructures, J. Atwood, J. Steed, eds. Wiley-VCH, 2008, 179-201.

"Homogeneous Catalytic Hydrogenation of Dioxygen: a Step Toward an Organometallic Fuel Cell?" Z. M. Heiden, T. B. Rauchfuss, 2007, 129, 14303-14310.

"Cyanometallate Cages with Exchangeable Terminal Ligands", J. L. Boyer, H. Yao, M. L. Kuhlman, T. B. Rauchfuss, S. R. Wilson, Eur. J. Inorg. Chem. (invited paper for 10th anniversary issue) 2007, 2721-2728.

"Evolution of Organo-cyanometallate Cages: Supramolecular Architectures and New Cs+-specific Receptors", J.L. Boyer, M.L. Kuhlman and T.B. Rauchfuss, Accounts of Chemical Research, 2007, 40, 233-242.

"Redox-Switched Complexation/Decomplexation of K+ and Cs+ by Molecular Cyanometalate Boxes", J. L. Boyer, M. Ramesh, H. Yao, T. B. Rauchfuss, S. R. Wilson, J. Am. Chem. Soc. 2007, 129, 1931-1936.

"Proton-induced Lewis Acidity of Unsaturated Iridium Amides", Z. M. Heiden and T. B. Rauchfuss, J. Am. Chem. Soc. 2006, 128, 13048-13049.

"Competing H-H, S-S, and M-M Bond Formation in [Ru4S3(arene)4]z Clusters" M. L. Kuhlman, T. B. Rauchfuss, Angew. Chem. Int. Ed. 2004, 43, 6742-6745.

"Synthesis and Characterization of the Hexagonal Prismatic Cage {THFpart of set[PhB(CN)3]6[Cp*Rh]6}6+", M. L. Kuhlman, H. Yao, T. B. Rauchfuss, Chem. Commun. 2004, 1370-1.

"Hybrid Cluster-Cages Formed via Cyanometallate Condensation: Cspart of setCo4Ru6S2(CN)12, Co4Ru9S6(CN)9, and Rh4Ru9S6(CN)9 Frameworks", M. L. Kuhlman, T. B. Rauchfuss, Inorg. Chem. 2004, 43, 430-435.

"Research on Soluble Metal Sulfides: From Polysulfido Complexes to Functional Models for the Hydrogenases" T. B. Rauchfuss, Inorg. Chem. 2004, 43, 14-26.