This research applies the synthetic model compound approach to cytochrome oxidase in order to deduce molecular level structure at the active site. Using tetraphenylporphyrin derivatives it is planned to synthesize iron (III) porphryrins which are covalently linked to copper (II) complexes. Once definitively characterized, preferably by Xray crystallography, the magnetic and structural properties will be investigated by EPR, MCD, Mossbauer, EXAFS and susceptibility studies as a function of bridging ligand (oxo, hydroxo, cyanide, imidazolate, carboxylate, etc.), spin state at iron, iron-copper distance and magnetic orbital orientation. Derivatives of such complexes will be studied as analogues of the cytochrome oxidase intermediates in the catalytic reduction of dioxygen to water. Iron(IV) oxo species of heme a will be prepared to test various proposals for such states in cytochrome oxidase. The H-bonded dioxygen moiety in oxygemoglobin will also be modelled as part of an investigation of dinuclear versus protic trapping of dioxygen at the active site.
| Nava, Matthew; Stoyanova, Irina V; Cummings, Steven et al. (2014) The strongest Brønsted acid: protonation of alkanes by H(CHB(11)F(11)) at room temperature. Angew Chem Int Ed Engl 53:1131-4 |
| Reed, Christopher A; Stoyanov, Evgenii S; Tham, Fook S (2013) Hydrogen bonding versus hyperconjugation in condensed-phase carbocations. Org Biomol Chem 11:3797-802 |
| Reed, Christopher A (2013) Myths about the proton. The nature of H+ in condensed media. Acc Chem Res 46:2567-75 |
| Stoyanov, Evgenii S; Stoyanova, Irina V; Tham, Fook S et al. (2012) Evidence for C-H hydrogen bonding in salts of tert-butyl cation. Angew Chem Int Ed Engl 51:9149-51 |
| Stoyanov, Evgenii S; Gunbas, Gorkem; Hafezi, Nema et al. (2012) The R3O+···H+ hydrogen bond: toward a tetracoordinate oxadionium(2+) ion. J Am Chem Soc 134:707-14 |
| Nava, Matthew; Reed, Christopher A (2011) Triethylsilyl Perfluoro-Tetraphenylborate, [Et(3)Si][F(20)-BPh(4)], a widely used Non-Existent Compound. Organometallics 30:4798-4800 |
| Nava, Matthew J; Reed, Christopher A (2010) High yield C-derivatization of weakly coordinating carborane anions. Inorg Chem 49:4726-8 |
| Stoyanov, Evgenii S; Stoyanova, Irina V; Reed, Christopher A (2010) The structure of the hydrogen ion (H(aq)+) in water. J Am Chem Soc 132:1484-5 |
| Reed, Christopher A (2010) H(+), CH(3)(+), and R(3)Si(+) carborane reagents: when triflates fail. Acc Chem Res 43:121-8 |
| Stoyanov, Evgenii S; Stoyanova, Irina V; Tham, Fook S et al. (2009) H(aq)+ structures in proton wires inside nanotubes. J Am Chem Soc 131:17540-1 |
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