Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives

Hydroxylated amino acids and their derivatives, including those found in proteins, are important in biology and medicinal chemistry. Incubation of N-acetyl-l-arginine with clavaminic acid synthase, a key oxygenase in clavulanic acid biosynthesis, affords a (3R)-hydroxylated product that is identical...

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Main Authors: Ye Zheng, Zhenyu Chen, Guy J. Clarkson, Stephen A. Marshall, Jianliang Xiao, Christopher J. Schofield, Martin Wills, Andrew V. Stachulski
Format: Article
Language:English
Published: The Royal Society 2025-02-01
Series:Royal Society Open Science
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Online Access:https://royalsocietypublishing.org/doi/10.1098/rsos.241607
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author Ye Zheng
Zhenyu Chen
Guy J. Clarkson
Stephen A. Marshall
Jianliang Xiao
Christopher J. Schofield
Martin Wills
Andrew V. Stachulski
author_facet Ye Zheng
Zhenyu Chen
Guy J. Clarkson
Stephen A. Marshall
Jianliang Xiao
Christopher J. Schofield
Martin Wills
Andrew V. Stachulski
author_sort Ye Zheng
collection DOAJ
description Hydroxylated amino acids and their derivatives, including those found in proteins, are important in biology and medicinal chemistry. Incubation of N-acetyl-l-arginine with clavaminic acid synthase, a key oxygenase in clavulanic acid biosynthesis, affords a (3R)-hydroxylated product that is identical to material obtained by total synthesis from Boc-beta alanine. The key step employed dynamic kinetic resolution (DKR) of a β-ketoester precursor, achieved in high diastereomeric and enantiomeric excess using an (R)-SEGPHOS/Ru(II) catalyst. The results highlight the utility of DKR for the preparation of C-3 hydroxylated amino acid derivatives.
format Article
id doaj-art-4460ca8ab8384b5d81567d8a0e964e80
institution DOAJ
issn 2054-5703
language English
publishDate 2025-02-01
publisher The Royal Society
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series Royal Society Open Science
spelling doaj-art-4460ca8ab8384b5d81567d8a0e964e802025-08-20T03:02:06ZengThe Royal SocietyRoyal Society Open Science2054-57032025-02-0112210.1098/rsos.241607Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivativesYe Zheng0Zhenyu Chen1Guy J. Clarkson2Stephen A. Marshall3Jianliang Xiao4Christopher J. Schofield5Martin Wills6Andrew V. Stachulski7Department of Chemistry, University of Warwick, Coventry CV4 7AL, UKDepartment of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, UKDepartment of Chemistry, University of Warwick, Coventry CV4 7AL, UKDepartment of Chemistry, Chemistry Research Laboratory, University of Oxford, Mansfield Road, Oxford OX1 3TA, UKDepartment of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, UKDepartment of Chemistry, Chemistry Research Laboratory, University of Oxford, Mansfield Road, Oxford OX1 3TA, UKDepartment of Chemistry, University of Warwick, Coventry CV4 7AL, UKDepartment of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, UKHydroxylated amino acids and their derivatives, including those found in proteins, are important in biology and medicinal chemistry. Incubation of N-acetyl-l-arginine with clavaminic acid synthase, a key oxygenase in clavulanic acid biosynthesis, affords a (3R)-hydroxylated product that is identical to material obtained by total synthesis from Boc-beta alanine. The key step employed dynamic kinetic resolution (DKR) of a β-ketoester precursor, achieved in high diastereomeric and enantiomeric excess using an (R)-SEGPHOS/Ru(II) catalyst. The results highlight the utility of DKR for the preparation of C-3 hydroxylated amino acid derivatives.https://royalsocietypublishing.org/doi/10.1098/rsos.241607asymmetric synthesisbiotransformationhydroxy amino-acidsantibioticscatalysis
spellingShingle Ye Zheng
Zhenyu Chen
Guy J. Clarkson
Stephen A. Marshall
Jianliang Xiao
Christopher J. Schofield
Martin Wills
Andrew V. Stachulski
Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
Royal Society Open Science
asymmetric synthesis
biotransformation
hydroxy amino-acids
antibiotics
catalysis
title Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
title_full Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
title_fullStr Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
title_full_unstemmed Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
title_short Dynamic kinetic resolution-mediated synthesis of C-3 hydroxylated arginine derivatives
title_sort dynamic kinetic resolution mediated synthesis of c 3 hydroxylated arginine derivatives
topic asymmetric synthesis
biotransformation
hydroxy amino-acids
antibiotics
catalysis
url https://royalsocietypublishing.org/doi/10.1098/rsos.241607
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