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Development of late transition metalloenzymes and metallo-DNAzymes for higly efficient catalytic processes


The proposal is to move the group of Dr. Paul Kamer to the School of Chemistry, University of St. Andrews to carry out an exciting range of projects related to sustainable development. Waste-free chemical processes are a must for a sustainable society. In nature, enzymes enable the atom economic synthesis of numerous natural products, but there are no enzymes for the synthesis of the many pharmaceuticals, agrochemicals and fine-chemicals that our society needs. To solve this problem, we seek a paradigm shift in catalysis research by developing transition metal containing "artificial enzymes" for catalytic transformations towards industrial products.

We propose a "de novo" design of transition metalloenzymes, using molecular recognition properties of biomolecules to develop (late) transition-metalloenzymes by functionalising oligonucleotides and proteins with phosphino ligands and binding them to late transition metals. Adjusting the structures of the biomolecule and the phosphine ligand will optimise the catalytic performance of these artificial enzymes. Artificial "metallo-DNAzymes" can be developed by complex formation of transition metal prosthetic groups and DNA aptamers as "apo-DNAzyme", starting from large aptamer libraries. The search for efficient "metallo-DNAzymes" will be aided by complex formation with transition state analogues, starting from large dynamic combinatorial libraries. We will create a new class of highly selective catalysts for demanding transformations, like CO insertion, alkene insertion and (asymmetric) C-C bond forming reactions. The biopolymer part will induce the proper substrate orientation to the metal centre. Encapsulating substrates by these "synthetic biopolymers" will then be exploited to achieve clean conversion of unfunctionalised molecules by C-H activation. These new catalysts, like biological systems, will be able to pick out a single substrate, even when it is present at low concentrations in complex mixtures.

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