Conformational Selection in Enzyme-Catalyzed Depolymerization of Bio-based Polyesters.

Autor: Lopez-Lorenzo X; KTH Royal Institute of Technology, Department of Fibre and Polymer Technology, SWEDEN., Ranjani G; KTH Royal Institute of Technology, Department of Fibre and Polymer Technology, SWEDEN., Syrén PO; KTH Royal Institute of Technology, School of Chemical Science and Engineering, Science for Life Laboratory, Tomtebodavägen 23B, 171 65, Solna, 17165, Stockholm, SWEDEN.
Jazyk: angličtina
Zdroj: Chembiochem : a European journal of chemical biology [Chembiochem] 2024 Jul 22, pp. e202400456. Date of Electronic Publication: 2024 Jul 22.
DOI: 10.1002/cbic.202400456
Abstrakt: Enzymatic degradation of polymers holds promise for advancing towards a bio-based economy. However, bulky polymers presents challenges in accessibility for biocatalysts, hindering depolymerization reactions. Beyond the impact of crystallinity, polymer chains can reside in different conformations affecting binding efficiency to the enzyme. We previously showed that the gauche and trans chain conformers associated with crystalline and amorphous regions of the synthetic polyethylene terephthalate (PET) display different affinity to PETase, thus affecting the depolymerization rate. However, structural-function relationships for biopolymers remain poorly understood in biocatalysis. In this study, we explored biodegradation of by-us previously synthesized bio-polyesters made from a rigid bicyclic chiral terpene-based diol and copolymerized with various renewable diesters. Herein, four of those polyesters spanning from semi-aromatic to aliphatic were subjected to enzymatic degradations in concert with induced-fit docking (IFD) analyses. Our findings demonstrate the importance of conformational selection in enzymatic depolymerization of biopolymers. A straight or twisted conformation of the polymer chain is crucial in biocatalytic degradation by showing different affinities to enzyme ground-state conformers. This work highlights the importance of considering the conformational match between the polymer and the enzyme to optimize the biocatalytic degradation efficiency of biopolymers, providing valuable insights for the development of sustainable bioprocesses.
(© 2024 Wiley‐VCH GmbH.)
Databáze: MEDLINE
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