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MES research with energy-systems focus on energy. Living systems provide a promising approach to chemical synthesis, having been optimized by evolution to convert renewab...

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not_BES

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Abstract

Living systems provide a promising approach to chemical synthesis, having been optimized by evolution to convert renewable carbon sources such as glucose to an enormous range of small molecules. However, a large number of synthetic structures can still be difficult to obtain solely from cells, such as unsubstituted hydrocarbons. In this work, we demonstrate the use of a hybrid cellular-heterogeneous catalytic strategy to produce olefins from glucose, using a selective hydrolase to generate an activated intermediate that is readily deoxygenated. Using a new family of iterative thiolase enzymes, we have genetically engineered a microbial strain that produces 4.3 ± 0.4 g L⁻¹ of fatty acid from glucose with 86% captured as 3-hydroxyoctanoic and 3-hydroxydecanoic acids. This 3-hydroxy substituent serves as a leaving group enabling heterogeneous tandem decarboxylation-dehydration routes to olefinic products on Lewis acidic catalysts without the additional redox input required for enzymatic or chemical deoxygenation of simple fatty acids.

Keywords

DecarboxylationCatalysisDeoxygenationCombinatorial chemistryOrganic chemistry

Identifiers

Journal
bioRxiv (Cold Spring Harbor Laboratory)
Year
2020