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Chemo-enzymatic Synthesis of Functional Bio-Based Polyesters

Chemo-enzymatic Synthesis of Functional Bio-Based Polyesters

Alessandro Pellis (ORCID: 0000-0003-3711-3087)
  • Grant DOI 10.55776/J4014
  • Funding program Erwin Schrödinger
  • Status ended
  • Start October 1, 2017
  • End October 31, 2020
  • Funding amount € 160,210

Disciplines

Chemistry (40%); Industrial Biotechnology (60%)

Keywords

    Circular economy, Green Chemistry, Biocatalyzed Synthesis, Polycondensation Reactions, Chemo-Enzymatic Processings, Functional Materials

Abstract Final report

Since the 1980s, industry and academia have investigated the possibility to improve efficiency, selectivity and sustainability of industrial processes by developing suitable enzyme catalysts as competitive alternatives to traditional stoichiometric synthesis or metallo- catalysis. Some processes and products are nowadays already implemented in industry but further research work is indeed needed in order to optimize and upscale a wide range of sustainable processes and products, especially in the field of bio-based plastics. This proposal aims at the sustainable synthesis of functional plant-derived plastics, which are not accessible by traditional chemical routes. These linear pre-polymers will be chemically post-processed in a 2nd reaction step in order to produce innovative advanced materials with unique properties and targeted at a variety of applications. Such polyesters will be of further inspiration for the next generation of scientists and be of industrial relevance in a timely manner, as they demonstrate how the proposed green synthesis techniques can be used to leave valuable functionality in plant-derived plastics for use in further downstream chemical processing, allowing modification towards a variety of target applications. Based on the solid experience of the researcher on the enzymatic synthesis and functionalization of bio-based polyesters developed during his Masters and continued during his PhD, and to the deep knowledge of the host, Prof. James H. Clark developed during the last 30 years of work in the field of green chemical synthesis, post- polymerization functionalization strategies and sustainable bio-derived monomers, the overall CESBP project strategy will be successfully implemented. In order to develop such innovative materials, this proposal will use a multidisciplinary approach combining traditional polymer chemistry with novel sustainable and green synthetic routes. The described research will not only address sustainability, but also pursue the competitiveness of the produced polymers in terms of their superior technological and functional properties. Greener and environmentally-friendly chemical modifications of the isolated bio-plastics will be investigated targeting diverse structures and broaden potential applications. Innovations in the field of bio-plastics are a paradigm of the increasingly intimate integration between biotechnologies and sustainable chemistry, which responds to the pressing challenges of a circular economy.

Since over 50 years, both industry and academia have investigated the possibility to improve efficiency, selectivity and sustainability of industrial processes by developing suitable enzyme catalysts as competitive alternatives to traditional stoichiometric synthesis or metal-based catalysis. Some processes and products are nowadays already implemented in industry, but further work is needed in order to optimize and upscale a wide range of sustainable processes and products, especially in the field of bio-based plastics. In this work, the sustainable synthesis of functional, plant-derived plastics, which are not accessible by traditional chemical routes was developed. Polymers having highly controlled structures were synthesized using natural catalysts using a variety of building blocks obtainable from fermentative processes. These polymers were also chemically post- processed in a 2nd reaction step in order to produce innovative advanced materials with unique properties and targeted at a variety of applications. Finally, the synthesized and functionalized materials were recycled and/or upcycled therefore closing the materials carbon cycle. The materials and technologies developed in the frame of the CESBP project will be of further inspiration for the next generation of scientists and be of high relevance for todays society that urges to undergo a green plastic revolution in order to preserve the environment we all live in. Innovations in the field of bio-plastics are a paradigm of the increasingly intimate integration between biotechnologies and sustainable chemistry, which responds to the pressing challenges of developing a self-sustaining circular economy.

Research institution(s)
  • University of York - 100%
  • Universität für Bodenkultur Wien - 100%
International project participants
  • Lucia Gardossi, University of Trieste - Italy

Research Output

  • 1111 Citations
  • 30 Publications
Publications
  • 2019
    Title Lysozyme-Responsive Spray-Dried Chitosan Particles for Early Detection of Wound Infection
    DOI 10.1021/acsabm.9b00023
    Type Journal Article
    Author Tallian C
    Journal ACS Applied Bio Materials
    Pages 1331-1339
    Link Publication
  • 2019
    Title Enzymatic synthesis of unsaturated polyesters: functionalization and reversibility of the aza-Michael addition of pendants
    DOI 10.1039/c8py01655k
    Type Journal Article
    Author Pellis A
    Journal Polymer Chemistry
    Pages 843-851
    Link Publication
  • 2019
    Title Laminaria digitata and Palmaria palmata Seaweeds as Natural Source of Catalysts for the Cycloaddition of CO2 to Epoxides
    DOI 10.3390/molecules24020269
    Type Journal Article
    Author Comerford J
    Journal Molecules
    Pages 269
    Link Publication
  • 2019
    Title Sustainable Galactarate-Based Polymers: Multi-Enzymatic Production of Pectin-Derived Polyesters
    DOI 10.1002/marc.201900361
    Type Journal Article
    Author Vastano M
    Journal Macromolecular Rapid Communications
    Link Publication
  • 2019
    Title Improving the Post-polymerization Modification of Bio-Based Itaconate Unsaturated Polyesters: Catalyzing Aza-Michael Additions With Reusable Iodine on Acidic Alumina
    DOI 10.3389/fchem.2019.00501
    Type Journal Article
    Author Moore O
    Journal Frontiers in Chemistry
    Pages 501
    Link Publication
  • 2019
    Title Solvent Applications of Short-Chain Oxymethylene Dimethyl Ether Oligomers
    DOI 10.1021/acssuschemeng.9b02895
    Type Journal Article
    Author Zhenova A
    Journal ACS Sustainable Chemistry & Engineering
    Pages 14834-14840
    Link Publication
  • 2019
    Title Integrating computational and experimental methods for efficient biocatalytic synthesis of polyesters
    DOI 10.1016/bs.mie.2019.07.040
    Type Book Chapter
    Author Pellis A
    Publisher Elsevier
    Pages 23-55
  • 2019
    Title Environmentally friendly covalent coupling of proteins onto oxidized cellulosic materials
    DOI 10.1039/c9nj03077h
    Type Journal Article
    Author Haske-Cornelius O
    Journal New Journal of Chemistry
    Pages 14536-14545
  • 2019
    Title Enzymatic hydrolysis of poly(1,4-butylene 2,5-thiophenedicarboxylate) (PBTF) and poly(1,4-butylene 2,5-furandicarboxylate) (PBF) films: A comparison of mechanisms
    DOI 10.1016/j.envint.2019.05.046
    Type Journal Article
    Author Gigli M
    Journal Environment International
    Pages 104852
    Link Publication
  • 2019
    Title Safer bio-based solvents to replace toluene and tetrahydrofuran for the biocatalyzed synthesis of polyesters
    DOI 10.1039/c8gc03567a
    Type Journal Article
    Author Pellis A
    Journal Green Chemistry
    Pages 1686-1694
    Link Publication
  • 2018
    Title Insights into post-polymerisation modification of bio-based unsaturated itaconate and fumarate polyesters via aza-michael addition: Understanding the effects of C?C isomerisation
    DOI 10.1002/pola.29079
    Type Journal Article
    Author Farmer T
    Journal Journal of Polymer Science Part A: Polymer Chemistry
    Pages 1935-1945
    Link Publication
  • 2018
    Title Elucidating enzymatic polymerisations: Chain-length selectivity of Candida antarctica lipase B towards various aliphatic diols and dicarboxylic acid diesters
    DOI 10.1016/j.eurpolymj.2018.07.009
    Type Journal Article
    Author Pellis A
    Journal European Polymer Journal
    Pages 79-84
    Link Publication
  • 2018
    Title Spatially confined lignin nanospheres for biocatalytic ester synthesis in aqueous media
    DOI 10.1038/s41467-018-04715-6
    Type Journal Article
    Author Sipponen M
    Journal Nature Communications
    Pages 2300
    Link Publication
  • 2018
    Title Immobilization of Myceliophthora thermophila laccase on poly(glycidyl methacrylate) microspheres enhances the degradation of azinphos-methyl
    DOI 10.1002/app.47417
    Type Journal Article
    Author Vera M
    Journal Journal of Applied Polymer Science
  • 2018
    Title Post-polymerization modification of bio-based polymers: maximizing the high functionality of polymers derived from biomass
    DOI 10.1002/pi.5573
    Type Journal Article
    Author Farmer T
    Journal Polymer International
    Pages 775-789
    Link Publication
  • 2020
    Title Enzymatic synthesis and tailoring lignin properties: A systematic study on the effects of plasticizers
    DOI 10.1016/j.polymer.2020.122725
    Type Journal Article
    Author Bartolome M
    Journal Polymer
    Pages 122725
  • 2020
    Title Work-hardening Photopolymer from Renewable Photoactive 3,3’-(2,5-Furandiyl)bisacrylic Acid
    DOI 10.1002/cssc.202000842
    Type Journal Article
    Author Lie Y
    Journal ChemSusChem
    Pages 4140-4150
    Link Publication
  • 2020
    Title Enzymatic synthesis of biobased polyesters utilizing aromatic diols as the rigid component
    DOI 10.1016/j.eurpolymj.2020.109680
    Type Journal Article
    Author Pellis A
    Journal European Polymer Journal
    Pages 109680
    Link Publication
  • 2020
    Title Harnessing the Power of Enzymes for Tailoring and Valorizing Lignin
    DOI 10.1016/j.tibtech.2020.03.010
    Type Journal Article
    Author Weiss R
    Journal Trends in Biotechnology
    Pages 1215-1231
  • 2020
    Title High Throughput Screening for New Fungal Polyester Hydrolyzing Enzymes
    DOI 10.3389/fmicb.2020.00554
    Type Journal Article
    Author Weinberger S
    Journal Frontiers in Microbiology
    Pages 554
    Link Publication
  • 2020
    Title Effects of Methyl Branching on the Properties and Performance of Furandioate-Adipate Copolyesters of Bio-Based Secondary Diols
    DOI 10.1021/acssuschemeng.0c04513
    Type Journal Article
    Author Little A
    Journal ACS Sustainable Chemistry & Engineering
    Pages 14471-14483
    Link Publication
  • 2020
    Title Renewable polymers and plastics: Performance beyond the green
    DOI 10.1016/j.nbt.2020.10.003
    Type Journal Article
    Author Pellis A
    Journal New Biotechnology
    Pages 146-158
  • 2020
    Title Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters
    DOI 10.3390/ma13020368
    Type Journal Article
    Author Comerford J
    Journal Materials
    Pages 368
    Link Publication
  • 2018
    Title Efficient Physisorption of Candida Antarctica Lipase B on Polypropylene Beads and Application for Polyester Synthesis
    DOI 10.3390/catal8090369
    Type Journal Article
    Author Weinberger S
    Journal Catalysts
    Pages 369
    Link Publication
  • 2018
    Title Highly Selective Enzymatic Recovery of Building Blocks from Wool-Cotton-Polyester Textile Waste Blends
    DOI 10.3390/polym10101107
    Type Journal Article
    Author Quartinello F
    Journal Polymers
    Pages 1107
    Link Publication
  • 2019
    Title Enzymatic synthesis of lignin derivable pyridine based polyesters for the substitution of petroleum derived plastics
    DOI 10.1038/s41467-019-09817-3
    Type Journal Article
    Author Pellis A
    Journal Nature Communications
    Pages 1762
    Link Publication
  • 2019
    Title Recent Advances on Enzymatic Catalysis as a Powerful Tool for the Sustainable Synthesis of Bio-Based Polyesters
    DOI 10.1007/978-3-030-10961-5_23
    Type Book Chapter
    Author Pellis A
    Publisher Springer Nature
    Pages 555-570
  • 2019
    Title Enzymatic Processing of Technical Lignins into Materials
    DOI 10.1007/978-3-030-10961-5_24
    Type Book Chapter
    Author Guebitz G
    Publisher Springer Nature
    Pages 571-592
  • 2019
    Title Functionalization of Enzymatically Synthesized Rigid Poly(itaconate)s via Post-Polymerization Aza-Michael Addition of Primary Amines
    DOI 10.1002/adsc.201900055
    Type Journal Article
    Author Guarneri A
    Journal Advanced Synthesis & Catalysis
    Pages 2559-2573
    Link Publication
  • 2019
    Title Smart textiles in wound care: functionalization of cotton/PET blends with antimicrobial nanocapsules
    DOI 10.1039/c9tb01474h
    Type Journal Article
    Author Quartinello F
    Journal Journal of Materials Chemistry B
    Pages 6592-6603

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