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Fast Depolymerization of PET Bottle Mediated by Microwave Pre-Treatment and An Engineered PETase
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab.ORCID iD: 0000-0001-5510-1392
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab.ORCID iD: 0000-0002-4708-9861
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Polymer Technology.ORCID iD: 0000-0002-7968-1691
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2023 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 16, no 18, article id e202300742Article in journal (Refereed) Published
Abstract [en]

Recycling plastics is the key to reaching a sustainable materials economy. Biocatalytic degradation of plastics shows great promise by allowing selective depolymerization of man-made materials into constituent building blocks under mild aqueous conditions. However, insoluble plastics have polymer chains that can reside in different conformations and show compact secondary structures that offer low accessibility for initiating the depolymerization reaction by enzymes. In this work, we overcome these shortcomings by microwave irradiation as a pre-treatment process to deliver powders of polyethylene terephthalate (PET) particles suitable for subsequent biotechnology-assisted plastic degradation by previously generated engineered enzymes. An optimized microwave step resulted in 1400 times higher integral of released terephthalic acid (TPA) from high-performance liquid chromatography (HPLC), compared to original untreated PET bottle. Biocatalytic plastic hydrolysis of substrates originating from PET bottles responded to 78 % yield conversion from 2 h microwave pretreatment and 1 h enzymatic reaction at 30 °C. The increase in activity stems from enhanced substrate accessibility from the microwave step, followed by the administration of designer enzymes capable of accommodating oligomers and shorter chains released in a productive conformation.

Place, publisher, year, edition, pages
Wiley , 2023. Vol. 16, no 18, article id e202300742
Keywords [en]
enzyme engineering, microwave pre-treatment, plastic biodegradation, polyesterase, polyethylene terephthalate recycling
National Category
Polymer Chemistry Food Science
Identifiers
URN: urn:nbn:se:kth:diva-338514DOI: 10.1002/cssc.202300742ISI: 001044462900001PubMedID: 37384425Scopus ID: 2-s2.0-85167360099OAI: oai:DiVA.org:kth-338514DiVA, id: diva2:1811893
Note

QC 20231114

Available from: 2023-11-14 Created: 2023-11-14 Last updated: 2024-05-21Bibliographically approved
In thesis
1. Chemoenzymatic Synthesis and Degradation of Plastics
Open this publication in new window or tab >>Chemoenzymatic Synthesis and Degradation of Plastics
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The development of a carbon-based bioeconomy for synthesis and degradation of polymers has gained importance over the years. Research efforts have been made to develop green routes to produce bio-based material from biomass as well as environmentally friendly ways to synthesize and degrade polymers. Enzymes are biocatalysts that are capable of performing reactions beyond their intended purpose. The work presented in this thesis focused on using biocatalysts for novel reactions to produce bio-plastics as well as degrade synthetic polymers. In Paper I, a decarboxylase was used to perform the fixation of CO2 under mild conditions to produce the platform chemical 2,5-furandicarboxylic acid (FDCA). In Paper II, a closed-loop approach for the production of bio-based polyesters and their enzymatic degradation was investigated. Moreover, the difference of catalytic activity towards different polymer conformations was noted and further investigated in Paper III. Here, the conformational landscape to match enzyme to substrate was explored. The model substrate for this project was post-consumer PET bottles since is one of the most used polymer worldwide. The substrate conformation affected the catalytic activity of the enzymes significantly hence, in Paper IV, the physical and chemical characteristics of various PET-based substrates was investigated to better understand the factors that will yield a high reaction efficiency for polymer depolymerization. Finally, the results obtained so far were used in Paper V to show that plastic degrading enzymes can be used for microplastic degradation in human blood as a proof-of-concept. In summary, the work in this thesis showed the potential of using enzymes as catalysts for the production of platform chemicals through CO2 fixation and for polymer degradation initiating an attractive path to close the loop in a bio-economy for polymer materials.

Abstract [sv]

Utvecklingen av en kolbaserad bioekonomi för syntes och återvinning av polymerer har blivit allt viktigare under åren. Forskningsinsatser har genomförts för att utveckla grönare alternativ för att producera biobaserade material samt miljövänliga sätt att syntetisera och bryta ner polymerer. Enzymer är biokatalysatorer som kan utföra reaktioner utöver deras avsedda syfte. Arbetet som presenteras i denna avhandling fokuserade på att använda biokatalysatorer för nya reaktioner för att producera bioplaster och bryta ner syntetiska polymerer. I Artikel I användes ett dekarboxylas för att fixera CO2 under milda förhållanden för att producera plattformskemikalien 2,5-furandikarboxylsyra (FDCA). I Artikel II undersöktes en sluten loop-metod för produktion av biobaserade polyester och deras enzymatiska nedbrytning. Dessutom noterades skillnaden i katalytisk aktivitet mot olika polymerkonformationer och undersöktes vidare i Artikel III. Här studerades det konformationella landskapet för att matcha enzym mot substrat. Modellsubstratet för detta projekt var PET-flaskor eftersom det är den mest använda polymeren världen över. Substratkonformationen påverkade enzymernas katalytiska aktivitet signifikant, varför de fysikaliska och kemiska egenskaperna hos olika PET-baserade substrat undersöktes i Artikel IV för att bättre förstå de faktorer som ger en hög reaktionseffektivitet för depolymerisering. Slutligen användes de hittills erhållna resultaten i Artikel V för att visa att plastnedbrytande enzymer kan användas för nedbrytning av mikroplast i humanblod som en proof-of-concept. Sammanfattningsvis visade arbetet i denna avhandling potentialen att använda enzymer som katalysatorer för produktion av plattformskemikalier genom CO2 -fixering och för polymernedbrytning vilket initierar en attraktiv väg för att sluta kretsloppet i en bioekonomi för polymera material. 

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2024. p. 81
Series
TRITA-CBH-FOU ; 2024:19
Keywords
Bio-based materials, Bioeconomy, Biomass, CO2, Conformational selection, Enzyme- engineering, Microwave pre-treatment, Plastic degradation, Polyester, Recycling., Biobaserade material, Bioekonomi, Biomassa, Konformationsselektion, Enzymingenejörskonst, Mikrovågsförbehandling, Plastnedbrytning, Polyester, Återvinning.
National Category
Biocatalysis and Enzyme Technology
Research subject
Fibre and Polymer Science
Identifiers
urn:nbn:se:kth:diva-346252 (URN)978-91-8040-920-9 (ISBN)
Public defence
2024-06-05, F3, Lindstedtsvägen 26, https://kth-se.zoom.us/j/62551057307, Stockholm, 10:00 (English)
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Supervisors
Note

QC 20240508

Available from: 2024-05-08 Created: 2024-05-08 Last updated: 2024-05-29Bibliographically approved

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Guo, BoyangLopez-Lorenzo, XimenaFang, YuanBäckström, EvaCapezza, Antonio JoseVanga, Sudarsana ReddyFuro, IstvanHakkarainen, MinnaSyrén, Per-Olof

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Guo, BoyangLopez-Lorenzo, XimenaFang, YuanBäckström, EvaCapezza, Antonio JoseVanga, Sudarsana ReddyFuro, IstvanHakkarainen, MinnaSyrén, Per-Olof
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