Abstract
5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold. A key obstacle in transitioning to bio-based plastic production lies in meeting the necessary industrial production efficiency, particularly in the cost-effective conversion of HMF to valuable intermediates. Toward addressing the challenge of developing scalable technology for oxidizing crude HMF to more valuable chemicals, here we report coordinated reaction and enzyme engineering to provide a galactose oxidase (GOase) variant with remarkably high activity toward HMF, improved O2 binding and excellent productivity (>1,000,000 TTN). The biocatalyst and reaction conditions presented here for GOase catalysed selective oxidation of HMF to 2,5-diformylfuran offers a productive blueprint for further development, giving hope for the creation of a biocatalytic route to scalable production of furan-based chemical building blocks from sustainable feedstocks.
Highlights
5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold
The oxidized HMF derivatives 2,5diformylfuran (DFF) and furan-2,5-dicarboxylic acid (FDCA) are both important intermediates in furan based polymer synthesis (Fig. 1), as they can be condensed with other monomers to make poly-imines, -esters, -amides and -urethanes as plastics, resins and porous organic frameworks[2,5,6]
This activity is limited to only a few enzymes[21,22], primarily chloroperoxidases[23], HMF oxidases (HMFO)[24], aryl-alcohol oxidases[25,26], and galactose oxidases (GOase) and related copper radical oxidases[27,28,29]
Summary
5-Hydroxymethylfurfural (HMF) has emerged as a crucial bio-based chemical building block in the drive towards developing materials from renewable resources, due to its direct preparation from sugars and its readily diversifiable scaffold. Reaction engineering for the GOase catalysed oxidation of HMF to DFF was performed alongside the enzyme engineering work, incorporating newly improved variants and substrate formulations as they became available.
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