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Biomimetic synthesis, iron-sulfur clusters, metal-organic frameworks, molecular electronics
We focus on four research areas: iron-sulfur clusters, heterometal paddlewheel complexes, metal-organic frameworks, and molecular electronics. The first two projects are both aimed at modeling or imitating the metal-containing active sites of various enzymes. Iron-sulfur clusters are ubiquitous in nature and commonly provide electron transport and storage – our research in this area has made great progress in synthesizing iron-sulfur clusters in highly reduced states. We also are interesting in synthesizing MFe3S4 clusters as analogues of the P-cluster and FeMo-cofactors of nitrogenase. Heterometal Pt-M paddlewheels are seen as models of square-planar / square pyramidal porphyrin-containing enzymes. We have developed a novel hard-soft synthetic scheme to reliably create these paddlewheels with a variety of metals, and have demonstrated binding of nitrogenous ligands.
Metal-organic frameworks (MOFs) reside at the interface of inorganic chemistry and materials science: MOFs are zeolite-like networks containing metal ions or clusters linked by large organic ligands. We use novel ligands to create frameworks with high porosity, high gas sorption, functionalized channels, or chiral channels; each of these have many interesting potential applications. We eventually envision creating MOFs which can serve as supports for biomimetic clusters, thus creating a “nanostructured artificial enzyme”.
Our molecular electronics project, a collaborative effort involving synthetic chemistry, analytical chemistry, and physics, aims to synthesize single-molecule “wires” containing metal-metal multiple bonds, in order to measure conductivity and electron transport at the atomic and molecular level.
Inorganic as well as organic synthetic techniques, both in solution and solvothermal methods, are regularly used. An array of physical methods, including CV, EPR, IR, Mössbauer, NMR, UV/Vis and particularly X-ray crystallography, are utilized.
Selected Publications
"An interweaving MOF with high hydrogen uptake." D. Sun, S. Ma, Y. Ke, D. J. Collins, and H.-C. Zhou. J. Amer. Chem. Soc. 2006, in press.
"Construction of metal-organic frameworks based on pre-designed carboxylate isomers: From achiral to chiral nets." D. Sun, D. J. Collins, Y. Ke, J.-L. Zuo, and H.-C. Zhou. Chem. Eur. J., 2006, in press.
A (10,3)-a non-interpenetrated network built from a Piedford ligand pair." Y. Ke, D. J. Collins, D. Sun, and H.-C. Zhou. Inorg. Chem. 2006, 45, 1897.
"Temperature-dependent supramolecular stereoisomerism in porous copper coordination networks based on a designed carboxylate ligand." D. Sun, Y. Ke, T. M. Mattox, B. A. Ooro, and H.-C. Zhou. Chem. Commun. 2005, 5447.
"Iron-sulfur models of protein active sites." D. J. Collins and H.-C. Zhou. In Encyclopedia of Inorganic Chemistry, 2nd Ed. Wiley: New York, 2005.
"Initial synthesis and structure of an all-ferrous analogue of the fully reduced [Fe4S4]0 cluster of the nitrogenase iron protein." T. A. Scott, C. P. Berlinguette, R. H. Holm, and H.-C. Zhou. PNAS 2005, 102, 9741.
"Syntheses, characterization, and photoluminescence of isostructural Mn, Co, and Zn MOFs having a diamondoid structure with large tetrahedral cages and high thermal stability." D. Sun, S. Ma, Y. Ke, T. M. Petersen, and H.-C. Zhou. Chem. Commun. 2005, 2663.
"Synthesis and structure of cuboctahedral and anticuboctahedral cages containing 12 quadruply bonded dimolybdenum units." Y. Ke, D. J. Collins, and H.-C. Zhou. Inorg. Chem. 2005, 44, 4154.
"Synthesis, structure and properties of mercury complexes with a new extended tetrathiafulvalene 4,5-dithiolate ligand." H.-R. Wen, J.-L. Zuo, T. A. Scott, H.-C. Zhou, and X.-Z. You. Polyhedron. 2005, 24, 671.
"Two cyano-bridged heterotrinuclear complexes built from [(Tp)Fe(CN)3]- (Tp=hydrotris(pyrazolyl)borate): synthesis, crystal structures and magnetic properties." S. Wang, J.-L. Zuo, H.-C. Zhou, Y. Song, and X.-Z. You. Inorg. Chim. Acta. 2005, 358, 2101.
"The first all-cyanide Fe4S4 cluster, [Fe4S4(CN)4]3-." T. A. Scott and H.-C. Zhou. Angew. Chem., Int. Ed. 2004, 43, 5628.
“Crystallographic evidence for chromium-platinum interaction." T. A. Scott, B. Abbaoui, and H.-C. Zhou. Inorg. Chem. 2004, 43, 2459.
"[(Tp)8(H2O)6CuII6FeIII8(CN)24]4+: A cyanide-bridged face-centered-cubic cluster with single-molecule-magnet behavior." S. Wang, J.-L. Zuo, H.-C. Zhou, H. J. Choi, Y. Ke, J. R. Long, and X.-Z. You. Angew. Chem., Int. Ed. 2004, 43, 5940.
"Heterobimetallic complexes based on [(Tp)Fe(CN)3]-: Syntheses, crystal structures and magnetic properties." S. Wang, J.-L. Zuo, H.-C. Zhou, Y. Song, S. Gao, and X.-Z. You. Eur. J. Inorg. Chem. 2004, 3681.
"The observation of superparamagnetic behavior in molecular nanowires." S. Wang, J.-L. Zuo, S. Gao, Y. Song, H.-C. Zhou, Y.-Z. Zhang, and X.-Z. You. J. Am. Chem. Soc. 2004, 126, 8900.
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