Details of Grant 

EPSRC Reference:	GR/S20598/01
Title:	Synthesis and Reactivity of Biomimetic Monocopper Peroxo Complexes
Principal Investigator:	Halcrow, Professor MA
Other Investigators:	McGowan, Professor P
Researcher Co-Investigators:
Project Partners:
Department:	Sch of Chemistry
Organisation:	University of Leeds
Scheme:	Standard Research (Pre-FEC)
Starts:	01 October 2003	Ends:	31 December 2006	Value (£):	183,301
EPSRC Research Topic Classifications:	Biological & Medicinal Chem. Chemical Biology Co-ordination Chemistry
EPSRC Industrial Sector Classifications:	Manufacturing Chemicals Pharmaceuticals and Biotechnology No relevance to Underpinning Sectors
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Summary on Grant Application Form
The two best-understood copper monooxygenase enzyme systems are: tyrosinase, which employs a dicopper active site to bind and activate dioxygen; and dopamine-b-monooxygenase (DbM) and peptidylglycine a-hydroxylating monooxygenase (PHM), which contain identical monocopper active sites. The chemical mechanism of tyrosinase is well-established, largely thanks to model chemistry studies. However, there are no biochemical data, or relevant model chemistry, to establish how the monocopper centre in DbM and PHM can activate dioxygen, to do the same chemistry that requies two copper ions in tyrosinase.An important feature of DbM and PHM is a second copper ion, remote from the active site but which can donate an electron to the dioxygen substrate during catalysis. Hence, to model these enzymes we must design a monocopper complex capable of two-electron oxidation. We will synthesise new derivatives of ligands that have been previously shown to support dicopper/dioxygen reactivity, but containing oxidisable ferrocenyl or nitroxyl pendant substituents. Reaction of Cu(I) complexes of these ligands with dioxygen will form mononuclear Cu(II)/peroxo products, with concomitant oxidation of the bound ligand. The structures of these species, and their reactivity towards intramolecular monooxygenation, will be elucidated in a much detail as possible. Similar studies will also be preformed on Cu(I) complexes of otherwise identical ligands that lack the oxidisable substituent. In this way, the influence of an exogenous electron donor on the dioxygen chemistry of a monocopper centre would be probed.
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Organisation Website:	http://www.leeds.ac.uk