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"The central theme of our research is to synthesize and structurally
characterize paddlewheel reaction platforms and artificial enzymes that
can perform chemical transformations routinely carried out in nature,
but difficult or impossible to achieve by pure chemical means. This
biomimetic approach may lead to catalysts with high activity and
selectivity, and biomimetic materials that can meet the challenge of
on-board vehicular hydrogen storage."
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Description of Research
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 interested 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 has 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.
Undergraduate researcher's roles in your lab
Undergraduate researchers are engaged in ligand, MOF, and iron-sulfur
cluster syntheses. Some of the students are able to access the state of
the art NMR spectrometer and X-ray diffractometer.
Graduate student's role in your lab
For graduate students, inorganic, organic, and solid-state synthetic
techniques will be used to obtain the target compounds. An array of
physical methods, including CV, EPR, IR, Mössbauer, NMR, UV/Vis, and in
particular, X-ray crystallography, will be utilized during the research
process.
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| Presentations |
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Cox, J.; Wandstradt, M.; Spendel, W.; Templated Nanoscale Sol-Gel Films
as Modifiers for Amperoimetric Detector; ElectroAnalytical Conference
ENSCPB, France June 11-15 (2006)
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| Funding |
$100.000 Grant from the State of Ohio
Nanomaterials in our Environment
$100.000 Grant from the State of Ohio
Nanomaterials in our Environment
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| Publications |
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Burns, C.; Spendel, W. U.; Puckett, S.; Pacey, G. E.; Solution ionic
strength effect on gold
nanoparticle solution color transition; Talanta (2006), 69(4), 873-876.
S. Ma and H.-C. Zhou, A Metal-Organic Framework with Entatic Metal
Centers Exhibiting High Gas-Adsorption Affinity, J. Am. Chem. Soc.
2006, 128, 11734-11735.
D. Sun, Y. Ke, T. M. Mattox, S. Parkin, and H.-C. Zhou, Stability and
Porosity Enhancement Through Concurrent Ligand Extension and SBU
Stabilization, Inorg. Chem. 2006, 45, 7566.
Sun, D.; Ma, S.; Ke, Y.; Collins, D. J.; Zhou, H.-C. "An Interweaving
MOF with High Hydrogen Uptake", J. Am. Chem. Soc. 2006, 128, 3896-3897.
D. Sun, D. J. Collins, Y. Ke, J.-L. Zuo, and H.-C. Zhou, Construction
of metal-organic frameworks based on pre-designed carboxylate isomers:
From achiral to chiral nets, Chem. Eur. J., 2006, 12, 3768-3776.
Ke, Y.; Collins, D. J.; Sun, D.; Zhou, H.-C., (10,3)-a
Noninterpenetrated Network Built from a Piedfort Ligand Pair, Inorg.
Chem. 2006, 45, 1897-1899.
D. Sun, Y. Ke, T. M. Mattox, B. A. Ooro, and H.-C. Zhou,
Temperature-dependent Supramolecular stereoisomerism in porous copper
coordination networks based on a designed carboxylate ligand, Chem.
Commun., 2005, 5447-5449.
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