Structure‐Guided Engineering of a Versatile Urethanase Improves Its Polyurethane Depolymerization Activity

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Polyurethane (PUR), the fifth most prevalent synthetic polymer, substantially contributes to global plastic waste problem. Biotechnology-based recycling methods have recently emerged as innovative solutions disposal and sparked interest among scientific communities industrial stakeholders in discovering designing highly active plastic-degrading enzymes. Here, ligand-free crystal structure of UMG-SP2, a metagenome-derived urethanase with depolymerization activities, at 2.59 Å resolution, well its (co-)structures bound suicide hydrolase inhibitor short-chain carbamate substrate 2.16 2.40 resolutions, respectively, is reported. Structural analysis molecular dynamics simulations reveal that flexible loop L3 consisting residues 219-226 crucial for regulating hydrolytic activity UMG-SP2. The semi-rational redesign UMG-SP2 reveals superior variants, A141G Q399A, exhibiting over 30.7- 7.4-fold increased activities on polyester-PUR methylene diamine derivative PUR, compared wild-type enzyme. These findings advance understanding structure-function relationship PUR-hydrolyzing enzymes, which hold great promise developing effective PUR processes mitigating environmental footprint waste.

Language: Английский

---

Quantitative nylon monomerization by the combination of chemical pretreatment and enzymatic hydrolysis using nylon hydrolases

PLoS ONE, Journal Year: 2025, Volume and Issue: 20(2), P. e0318641 - e0318641

Published: Feb. 10, 2025

Nylons, derived from fossil fuels, are widely used for their toughness and flexibility, but they pose environmental concerns due to low biodegradability. This study explored an efficient method the monomerization of polymeric nylons, specifically nylon-6 nylon-6,6, through a combination chemical pretreatment enzymatic hydrolysis using two kinds nylon hydrolases, NylB NylC (Nyl series enzymes). To break down strong intermolecular hydrogen bonding between polymer chains nylon, methods were investigated: homogeneous dispersion soluble oligomerization induced by acid treatment. Homogeneous enhances water solubility, while reduces molecular weight. These pretreatments significantly increased enzyme sensitivity resulting in nearly complete conversion into monomers Nyl series. Finally convincing toward market products such as fishing nets was also achieved. highlights potential this methodology recycling, offering promising solution reducing impacts achieving circular economy products.

Language: Английский

---

Exploring biotechnology for plastic recycling, degradation and upcycling for a sustainable future

Biotechnology Advances, Journal Year: 2025, Volume and Issue: unknown, P. 108544 - 108544

Published: Feb. 1, 2025

Language: Английский

---

High Salt-Resistant Urethanase Degrades Ethyl Carbamate in Soy Sauce

Journal of Agricultural and Food Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 13, 2024

Urethanase is a promising biocatalyst for degrading carcinogen ethyl carbamate (EC) in fermented foods. However, their vulnerability to high ethanol and/or salt and acidic conditions severely limits applications. In this study, novel urethanase from

Language: Английский

---

Process insights for harnessing biotechnology for plastic depolymerization

Nature Chemical Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 17, 2025

Language: Английский

---

A self-assembly strategy for fabricating tough and magneto-responsive scaffolds to promote osteogenesis with enhanced vascularization

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 163129 - 163129

Published: April 1, 2025

Language: Английский

---

Enzymatic recycling and microbial upcycling for a circular plastics bioeconomy

Current Opinion in Biotechnology, Journal Year: 2025, Volume and Issue: 93, P. 103307 - 103307

Published: May 1, 2025

Since the 1950s, plastics have become commodity materials that are present in virtually every aspect of our daily lives. However, current economic model is fundamentally linear, with less than 10% returning to value chain at their end life. In recent years, efforts been dedicated develop new technologies can change this a circular economy for plastics, including enzymatic recycling and biological upcycling value-added products. Here, we will review advances made rapidly evolving field discuss how further development these could contribute reduce share postconsumer plastic waste diverted toward landfilling incineration.

Language: Английский

---

Maßgeschneiderte Biokatalysatoren für industrielle Anwendungen

BIOspektrum, Journal Year: 2025, Volume and Issue: 31(3), P. 340 - 341

Published: May 1, 2025

---

The Catalytic Mechanism of the Plastic-Degrading Enzyme Urethanase UMG-SP2

Published: Aug. 6, 2024

The recently discovered metagenomic urethanases UMG-SP1, UMG-SP2, and UMG-SP3 have emerged as promising tools to improve existing chemical processes for polyurethane (PU) waste recycling. These enzymes are capable of breaking down urethane bonds in low molecular weight dicarbamates using the Ser-Sercis-Lys triad catalysis, similar other members amidase signature protein superfamily. Understanding catalytic mechanism these is crucial enhancing their enzymatic activity improving PU bio-recycling processes. In this study, we employed hybrid quantum mechanics/molecular mechanics methods delve into machinery UMG-SP2 urethanase a model substrate. Our results indicate that reaction proceeds two stages: STAGE 1 acylation, which enzyme becomes covalently bound substrate, releasing an alcohol-leaving group; 2 - deacylation, water hydrolyzes enzyme:ligand covalent adduct, product form highly unstable carbamic acid, expected rapidly decompose amine carbon dioxide. We found comprises rate-limiting step overall reaction, consisting cleavage substrate’s bond by its ester moiety release group (overall Gibbs activation energy 20.8 kcal·mol-1). Lastly, identified point mutations enhance enzyme's turnover hydrolysis stabilizing macrodipole transition state. findings expand our current knowledge homolog from superfamily, paving way future research on depolymerization plastic materials.

Language: Английский

---

Biosensor‐Guided Engineering of a Baeyer‐Villiger Monooxygenase for Aliphatic Ester Production

ChemBioChem, Journal Year: 2024, Volume and Issue: 26(1)

Published: Sept. 25, 2024

Abstract Esters are valuable aroma compounds and can be produced enzymatically by Baeyer‐Villiger monooxygenases (BVMOs) from (aliphatic) ketone precursors. However, a genetically encoded biosensor system for the assessment of BVMO activity detection reaction products is missing. In this work, we assembled synthetic enzyme cascade – featuring an esterase, alcohol dehydrogenase, LuxAB in heterologous host Escherichia coli . Target esters BVMO, subsequently cleaved, corresponding oxidized through artificial pathway. Ultimately, aldehyde detected vivo LuxAB, luciferase Photorhabdus luminescens that emits bioluminescence upon oxidation aldehydes to carboxylates. This greatly accelerated screening selection active variants focused library, omitting commonly used low‐throughput chromatographic analysis. Engineered enzymes accepted linear aliphatic ketones such as 2‐undecanone 2‐dodecanone exhibited improved ester formation.

Language: Английский

---