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Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers

Atropisomeric biaryls carrying ortho-hydroxymethyl and formyl groups were made enantioselectively by desymmetrisation of dialdehyde or diol substrates. The oxidation of the symmetrical diol substrates was achieved using a variant of galactose oxidase (GOase), and the reduction of the dialdehydes usi...

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Autores principales: Staniland, Samantha, Yuan, Bo, Giménez-Agulló, Nelson, Marcelli, Tommaso, Willies, Simon C, Grainger, Damian M, Turner, Nicholas J, Clayden, Jonathan
Formato: Online Artículo Texto
Lenguaje:English
Publicado: WILEY-VCH Verlag 2014
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4497317/
https://www.ncbi.nlm.nih.gov/pubmed/25156181
http://dx.doi.org/10.1002/chem.201404509
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author Staniland, Samantha
Yuan, Bo
Giménez-Agulló, Nelson
Marcelli, Tommaso
Willies, Simon C
Grainger, Damian M
Turner, Nicholas J
Clayden, Jonathan
author_facet Staniland, Samantha
Yuan, Bo
Giménez-Agulló, Nelson
Marcelli, Tommaso
Willies, Simon C
Grainger, Damian M
Turner, Nicholas J
Clayden, Jonathan
author_sort Staniland, Samantha
collection PubMed
description Atropisomeric biaryls carrying ortho-hydroxymethyl and formyl groups were made enantioselectively by desymmetrisation of dialdehyde or diol substrates. The oxidation of the symmetrical diol substrates was achieved using a variant of galactose oxidase (GOase), and the reduction of the dialdehydes using a panel of ketoreductases. Either M or P enantiomers of the products could be formed, with absolute configurations assigned by time-dependent DFT calculations of circular dichroism spectra. The differing selectivities observed with different biaryl structures offer an insight into the detailed structure of the active site of the GOase enzyme.
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spelling pubmed-44973172015-07-10 Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers Staniland, Samantha Yuan, Bo Giménez-Agulló, Nelson Marcelli, Tommaso Willies, Simon C Grainger, Damian M Turner, Nicholas J Clayden, Jonathan Chemistry Communications Atropisomeric biaryls carrying ortho-hydroxymethyl and formyl groups were made enantioselectively by desymmetrisation of dialdehyde or diol substrates. The oxidation of the symmetrical diol substrates was achieved using a variant of galactose oxidase (GOase), and the reduction of the dialdehydes using a panel of ketoreductases. Either M or P enantiomers of the products could be formed, with absolute configurations assigned by time-dependent DFT calculations of circular dichroism spectra. The differing selectivities observed with different biaryl structures offer an insight into the detailed structure of the active site of the GOase enzyme. WILEY-VCH Verlag 2014-10-06 2014-08-22 /pmc/articles/PMC4497317/ /pubmed/25156181 http://dx.doi.org/10.1002/chem.201404509 Text en © 2014 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. http://creativecommons.org/licenses/by-nc-nd/4.0/ This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Communications
Staniland, Samantha
Yuan, Bo
Giménez-Agulló, Nelson
Marcelli, Tommaso
Willies, Simon C
Grainger, Damian M
Turner, Nicholas J
Clayden, Jonathan
Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title_full Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title_fullStr Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title_full_unstemmed Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title_short Enzymatic Desymmetrising Redox Reactions for the Asymmetric Synthesis of Biaryl Atropisomers
title_sort enzymatic desymmetrising redox reactions for the asymmetric synthesis of biaryl atropisomers
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4497317/
https://www.ncbi.nlm.nih.gov/pubmed/25156181
http://dx.doi.org/10.1002/chem.201404509
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