One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim This work reports the one-pot enzymatic cascade that completely converts l-arabinose to l-ribulose using four reactions catalyzed by pyranose 2-oxidase (P2O), xylose reductase, formate dehydrogenase, and catalase. As wild-type P2O is specific f...
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th-cmuir.6653943832-636052019-03-18T02:21:49Z One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade Litavadee Chuaboon Thanyaporn Wongnate Pangrum Punthong Cholpisit Kiattisewee Narin Lawan Chia Yi Hsu Chun Hung Lin Uwe T. Bornscheuer Pimchai Chaiyen Chemical Engineering Chemistry © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim This work reports the one-pot enzymatic cascade that completely converts l-arabinose to l-ribulose using four reactions catalyzed by pyranose 2-oxidase (P2O), xylose reductase, formate dehydrogenase, and catalase. As wild-type P2O is specific for the oxidation of six-carbon sugars, a pool of P2O variants was generated based on rational design to change the specificity of the enzyme towards the oxidation of l-arabinose at the C2-position. The variant T169G was identified as the best candidate, and this had an approximately 40-fold higher rate constant for the flavin reduction (sugar oxidation) step, as compared to the wild-type enzyme. Computational calculations using quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) showed that this improvement is due to a decrease in the steric effects at the axial C4-OH of l-arabinose, which allows a reduction in the distance between the C2-H and flavin N5, facilitating hydride transfer and enabling flavin reduction. 2019-03-18T02:21:37Z 2019-03-18T02:21:37Z 2019-02-18 Journal 15213773 14337851 2-s2.0-85060784297 10.1002/anie.201814219 https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85060784297&origin=inward http://cmuir.cmu.ac.th/jspui/handle/6653943832/63605 |
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Chemical Engineering Chemistry Litavadee Chuaboon Thanyaporn Wongnate Pangrum Punthong Cholpisit Kiattisewee Narin Lawan Chia Yi Hsu Chun Hung Lin Uwe T. Bornscheuer Pimchai Chaiyen One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
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© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim This work reports the one-pot enzymatic cascade that completely converts l-arabinose to l-ribulose using four reactions catalyzed by pyranose 2-oxidase (P2O), xylose reductase, formate dehydrogenase, and catalase. As wild-type P2O is specific for the oxidation of six-carbon sugars, a pool of P2O variants was generated based on rational design to change the specificity of the enzyme towards the oxidation of l-arabinose at the C2-position. The variant T169G was identified as the best candidate, and this had an approximately 40-fold higher rate constant for the flavin reduction (sugar oxidation) step, as compared to the wild-type enzyme. Computational calculations using quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) showed that this improvement is due to a decrease in the steric effects at the axial C4-OH of l-arabinose, which allows a reduction in the distance between the C2-H and flavin N5, facilitating hydride transfer and enabling flavin reduction. |
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Litavadee Chuaboon Thanyaporn Wongnate Pangrum Punthong Cholpisit Kiattisewee Narin Lawan Chia Yi Hsu Chun Hung Lin Uwe T. Bornscheuer Pimchai Chaiyen |
author_facet |
Litavadee Chuaboon Thanyaporn Wongnate Pangrum Punthong Cholpisit Kiattisewee Narin Lawan Chia Yi Hsu Chun Hung Lin Uwe T. Bornscheuer Pimchai Chaiyen |
author_sort |
Litavadee Chuaboon |
title |
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
title_short |
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
title_full |
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
title_fullStr |
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
title_full_unstemmed |
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade |
title_sort |
one-pot bioconversion of l-arabinose to l-ribulose in an enzymatic cascade |
publishDate |
2019 |
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https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=85060784297&origin=inward http://cmuir.cmu.ac.th/jspui/handle/6653943832/63605 |
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1681425926342049792 |