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Novel haem-based catalysts

Objective

The specific objective of this project is to study the factors determining the ability of a haem complex to bind, activate and specifically transform compounds. These factors may be classified as:
1) Structural (e.g. the nature of the available coordination site on the metal, type of donor atoms, electron density at the metal atom, superstructure of ligands, and steric effects);
2) Micro-environmental (e.g. polarity, hydrogen bonding ability of solvent, local pH and dynamics);
3) Mechanistic (e.g. competing and/or subsequent reactions, resistance to radical induced inactivation, relative binding affinities of substrate and inhibitor to the haem site).
- An engineered lignin peroxidase cDNA was overexpressed in E. coli. The mechanism of HRPC was studied.
- Microperoxidases which catalyse peroxidase-type and industrially relevant P450-type bioconversions were obtained.
- The structural effect of calcium in the enzymatic mechanism of LIP and HRP was studied.
- The crystal structure of a protein (cytochrome c6) was for the first time obtained by ab initio methods.
- The first 3D structure in solution of a paramagnetic haem protein was obtained. New NMR methods were developed.
- Electronic to protonic-energy was for the first time achieved in aqueous solution.
- Compounds with specific peroxidase activity were synthesised.
- Project deliverables:
1) New recombinant haem enzymes.
2) Development of first generation biomimetic Mn oxidation compounds.
3) Novel molecular calculation method developed.
4) Development of a model for homotropic (e{-}/e{-}) and heterotropic (e{-}/H{+}) cooperativities.
5) Development of new NMR methods.
6) Development of new methods for X-ray structural determinations.

Topic(s)

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Call for proposal

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Coordinator

Universidade Nova de Lisboa
Address
6,quinta Do Marqués
2780 Oeiras
Portugal

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Participants (5)

CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE
France
Address
Rue Des Saints-pères 45, Université De Paris 5
75270 Paris

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John Innes Centre
United Kingdom
Address
Norwich Research Park Colney
NR4 7UH Norwich

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UNIVERSITY OF FLORENCE
Italy
Address
75/77,via Gino Capponi 9
50121 Firenze

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University of Sussex
United Kingdom
Address
Falmer
BN1 9QG Brighton

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WAGENINGEN UNIVERSITY
Netherlands
Address
3,dreijenlaan 3
6703 HA Wageningen

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