Journal
INORGANICA CHIMICA ACTA
Volume 363, Issue 3, Pages 601-604Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.ica.2009.02.001
Keywords
Transfer hydrogenation; Artificial enzyme; Streptavidin; Biotin; Ruthenium complexes; Piano-stool; Evolution; Mutagenesis; Enantioselectivity
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Funding
- Swiss National Science Foundation [FN 200021-105192, 200020-113348]
- Roche Foundation
- FP6 Marie Curie Research Training network [MRTNCT-2003-505020]
- Canton of Neuchatel
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Artificial metalloenzymes based on the incorporation of biotinylated ruthenium piano-stool complexes within streptavidin can be readily optimized by chemical or genetic means. We performed genetic modifications of such artificial metalloenzymes for the transfer hydrogenation of aromatic ketones, by combining targeted point mutations of the host protein. Upon using the P64G-L124V double mutant of streptavidin in combination with the [eta(6)-(p-cymene)Ru(Biot-p-L)Cl] complex, the enantioselectivity can be increased up to 98% ee (R) for the reduction of p-methylacetophenone, which is the highest selectivity obtained up to date with an artificial transfer hydrogenase. (C) 2009 Elsevier B.V. All rights reserved.
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