Our Mission
Our research interests lie in developing thermal and photochemical-Bergman cyclization reactivity in inorganic small molecules, porphyrins, and nanoparticle surfaces for carbon-based polymerization reactions, or as nature has taught us, biologically-relevant H-atom abstraction reactivity. While a considerable amount of our effort is devoted to developing fundamental metal-catalyzed cyclization reactions, we have also applied these motifs to a subset of natural biopolymers such as plaques and fibrin clots.
We are also committed to the design and synthesis of novel nanocatalysts for thermal and laser-induced catalytic transformations that require inaccessible thermal temperatures on the benchtop. These studies include probing the mechanism of these turnover reactions involving CO2 and NO3− reduction, as well as C-C coupling reactions using transient and low temperature spectroscopic techniques.
Disease states resulting from metal-mediated biopolymer deposition can arise when the natural cleavage mechanisms become inoperative or function poorly, such as the formation of amyloid plaques which have been connected to the neurodegenerative disease Alzheimer’s, as well as thrombotic disease (atherosclerosis) leading to heart attack or stroke. Current treatment options for amyloid plaque buildup involve inhibition or activation of specific enzymes involved in the disease pathway, while acute arterial thrombosis is combated via the use of anti-platelet agents or anti-coagulants that inhibit the thrombus. In the latter case, side effects associated with such anti-coagulants involve the risk of systemic bleeding which can supersede the benefit of the antithrombotic therapy.
Our approach to these problems involves developing small molecule enediyne ligands that extract metal directly from the plaque (Cu, Zn, of Ca), or incorporation of diradicals-generating ligands into optically-active Au and magnetically responsive Fe3O4 nanoarchitectures. Small molecules with N4-coordination have been developed for disaggregation of amyloid plaques by in situ activation and radical-formation upon chelation of Zn(II) and Cu(II), while larger-payload nanoparticles that can be activated photo-thermally or by magnetic induction hyperthermia are applied to dissolve fibrin clots. We are also committed to the design and synthesis of novel nanocatalysts for thermal and laser-induced catalytic transformations that require inaccessible thermal temperatures on the benchtop. These studies include probing the mechanism of these turnover reactions using transient and low temperature spectroscopic techniques.