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Integrated preservation of water activity as key to intensified chemoenzymatic synthesis of bio-based styrene derivatives
Citation Link: https://doi.org/10.15480/882.9485
Publikationstyp
Journal Article
Publikationsdatum
2024-12-01
Sprache
English
Enthalten in
Volume
7
Issue
1
Article Number
57
Citation
Communications Chemistry 7 (1): 57 (2024)
Publisher DOI
Scopus ID
Publisher
Macmillan
The valorization of lignin-derived feedstocks by catalytic means enables their defunctionalization and upgrading to valuable products. However, the development of productive, safe, and low-waste processes remains challenging. This paper explores the industrial potential of a chemoenzymatic reaction performing the decarboxylation of bio-based phenolic acids in wet cyclopentyl methyl ether (CPME) by immobilized phenolic acid decarboxylase from Bacillus subtilis, followed by a base-catalyzed acylation. Key-to-success is the continuous control of water activity, which fluctuates along the reaction progress, particularly at high substrate loadings (triggered by different hydrophilicities of substrate and product). A combination of experimentation, thermodynamic equilibrium calculations, and MD simulations revealed the change in water activity which guided the integration of water reservoirs and allowed process intensification of the previously limiting enzymatic step. With this, the highly concentrated sequential two-step cascade (400 g·L–1) achieves full conversions and affords products in less than 3 h. The chemical step is versatile, accepting different acyl donors, leading to a range of industrially sound products. Importantly, the finding that water activity changes in intensified processes is an academic insight that might explain other deactivations of enzymes when used in non-conventional media.
DDC Class
660: Chemistry; Chemical Engineering
Publication version
publishedVersion
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main article
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