Cell‐Free Biosynthesis of ω‐Hydroxy Acids Boosted by a Synergistic Combination of Alcohol Dehydrogenases

Velasco-Lozano, Susana (Universidad de Zaragoza) ; Santiago-Arcos, Javier ; Grazia Rubanu, Maria ; López-Gallego, Fernando

Resumen: The activity orchestration of an unprecedented cell-free enzyme system with self-sufficient cofactor recycling enables the stepwise transformation of aliphatic diols into ω-hydroxy acids at the expense of molecular oxygen as electron acceptor. The efficiency of the biosynthetic route was maximized when two compatible alcohol dehydrogenases were selected as specialist biocatalysts for each one of the oxidative steps required for the oxidative lactonization of diols. The cell-free system reached up to 100 % conversion using 100 mM of linear C5 diols and performed the desymmetrization of prochiral branched diols into the corresponding ω-hydroxy acids with an exquisite enantioselectivity (ee>99 %). Green metrics demonstrate superior sustainability of this system compared to traditional metal catalysts and even to whole cells for the synthesis of 5-hydroxypetanoic acid. Finally, the cell-free system was assembled into a consortium of heterogeneous biocatalysts that allowed the enzyme reutilization. This cascade illustrates the potential of systems biocatalysis to access new heterofunctional molecules such as ω-hydroxy acids.

Idioma: Inglés

DOI: 10.1002/cssc.202200397

Año: 2022

Publicado en: ChemSusChem 15, 9 (2022)
ISSN: 1864-5631

Factor impacto JCR: 8.4 (2022)

Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 32 / 178 = 0.18 (2022) - Q1 - T1
Categ. JCR: GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY rank: 14 / 46 = 0.304 (2022) - Q2 - T1

Factor impacto CITESCORE: 15.5 - Materials Science (Q1) - Chemical Engineering (Q1) - Energy (Q1) - Environmental Science (Q1)

Factor impacto SCIMAGO: 2.064 - Chemical Engineering (miscellaneous) (Q1) - Materials Science (miscellaneous) (Q1) - Environmental Chemistry (Q1) - Energy (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/MINECO/PCI2018-092984
Financiación: info:eu-repo/grantAgreement/ES/MINECO/RTI2018-094398-B-I00

Tipo y forma: Artículo (Versión definitiva)

Área (Departamento): Área Química Orgánica (Dpto. Química Orgánica)