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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...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
WILEY-VCH Verlag
2014
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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. |
format | Online Article Text |
id | pubmed-4497317 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2014 |
publisher | WILEY-VCH Verlag |
record_format | MEDLINE/PubMed |
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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