Publication: One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade
Issued Date
2019-02-18
Resource Type
ISSN
15213773
14337851
14337851
Other identifier(s)
2-s2.0-85060784297
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Mahidol University
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SCOPUS
Bibliographic Citation
Angewandte Chemie - International Edition. Vol.58, No.8 (2019), 2428-2432
Suggested Citation
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. Angewandte Chemie - International Edition. Vol.58, No.8 (2019), 2428-2432. doi:10.1002/anie.201814219 Retrieved from: https://repository.li.mahidol.ac.th/handle/20.500.14594/50521
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Title
One-Pot Bioconversion of l-Arabinose to l-Ribulose in an Enzymatic Cascade
Abstract
© 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.