Chemo-enzymatic Synthesis of Functional Bio-Based Polyesters
Chemo-enzymatic Synthesis of Functional Bio-Based Polyesters
Disciplines
Chemistry (40%); Industrial Biotechnology (60%)
Keywords
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Circular economy,
Green Chemistry,
Biocatalyzed Synthesis,
Polycondensation Reactions,
Chemo-Enzymatic Processings,
Functional Materials
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.
- University of York - 100%
- Universität für Bodenkultur Wien - 100%
Research Output
- 1111 Citations
- 30 Publications
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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