Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters
The enzymatic synthesis of polyesters in solventless systems is an environmentally friendly and sustainable method for synthetizing bio-derived materials. Despite the greenness of the technique, in most cases only short oligoesters are obtained, with limited practical applications or requiring furth...
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ftleedsuniv:oai:eprints.whiterose.ac.uk:155565 2023-05-15T13:34:43+02:00 Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters Comerford, James William Byrne, Fergal Weinberger, Simone Farmer, Thomas James Guebitz, Georg M. Gardossi, Lucia Pellis, Alessandro 2020-01-13 text https://eprints.whiterose.ac.uk/155565/ https://eprints.whiterose.ac.uk/155565/1/materials_13_00368.pdf https://doi.org/10.3390/ma13020368 en eng https://eprints.whiterose.ac.uk/155565/1/materials_13_00368.pdf Comerford, James William orcid.org/0000-0002-9977-5695 , Byrne, Fergal, Weinberger, Simone et al. (4 more authors) (2020) Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters. Materials. 368. pp. 1-9. ISSN 1996-1944 cc_by CC-BY Article PeerReviewed 2020 ftleedsuniv https://doi.org/10.3390/ma13020368 2023-01-30T22:25:52Z The enzymatic synthesis of polyesters in solventless systems is an environmentally friendly and sustainable method for synthetizing bio-derived materials. Despite the greenness of the technique, in most cases only short oligoesters are obtained, with limited practical applications or requiring further chemical processing for their elongation. In this work, we present a catalyst-free thermal upgrade of enzymatically synthesized oligoesters. Dierent aliphatic and aromatic oligoesters were synthesized using immobilized Candida antarctica lipase B (iCaLB) as the catalyst (70 C, 24 h) yielding poly(1,4-butylene adipate) (PBA, Mw = 2200), poly(1,4-butylene isophthalate) (PBI, Mw = 1000), poly(1,4-butylene 2,5-furandicarboxylate) (PBF, Mw = 600), and poly(1,4-butylene 2,4-pyridinedicarboxylate) (PBP, Mw = 1000). These polyesters were successfully thermally treated to obtain an increase in Mw of 8.5, 2.6, 3.3, and 2.7 folds, respectively. This investigation focused on the most successful upgrade, poly(1,4-butylene adipate), then discussed the possible eect of di-ester monomers as compared to di-acids in the thermally driven polycondensation. The herein-described two-step synthesis method represents a practical and cost-eective way to synthesize higher-molecular-weight polymers without the use of toxic metal catalysts such as titanium(IV) tert-butoxide, tin(II) 2-ethylhexanoate, and in particular, antimony(IV) oxide. At the same time, the method allows for the extension of the number of reuses of the biocatalyst by preventing its exposure to extreme denaturating conditions. Article in Journal/Newspaper Antarc* Antarctica White Rose Research Online (Universities of Leeds, Sheffield & York) Materials 13 2 368 |
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Open Polar |
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White Rose Research Online (Universities of Leeds, Sheffield & York) |
op_collection_id |
ftleedsuniv |
language |
English |
description |
The enzymatic synthesis of polyesters in solventless systems is an environmentally friendly and sustainable method for synthetizing bio-derived materials. Despite the greenness of the technique, in most cases only short oligoesters are obtained, with limited practical applications or requiring further chemical processing for their elongation. In this work, we present a catalyst-free thermal upgrade of enzymatically synthesized oligoesters. Dierent aliphatic and aromatic oligoesters were synthesized using immobilized Candida antarctica lipase B (iCaLB) as the catalyst (70 C, 24 h) yielding poly(1,4-butylene adipate) (PBA, Mw = 2200), poly(1,4-butylene isophthalate) (PBI, Mw = 1000), poly(1,4-butylene 2,5-furandicarboxylate) (PBF, Mw = 600), and poly(1,4-butylene 2,4-pyridinedicarboxylate) (PBP, Mw = 1000). These polyesters were successfully thermally treated to obtain an increase in Mw of 8.5, 2.6, 3.3, and 2.7 folds, respectively. This investigation focused on the most successful upgrade, poly(1,4-butylene adipate), then discussed the possible eect of di-ester monomers as compared to di-acids in the thermally driven polycondensation. The herein-described two-step synthesis method represents a practical and cost-eective way to synthesize higher-molecular-weight polymers without the use of toxic metal catalysts such as titanium(IV) tert-butoxide, tin(II) 2-ethylhexanoate, and in particular, antimony(IV) oxide. At the same time, the method allows for the extension of the number of reuses of the biocatalyst by preventing its exposure to extreme denaturating conditions. |
format |
Article in Journal/Newspaper |
author |
Comerford, James William Byrne, Fergal Weinberger, Simone Farmer, Thomas James Guebitz, Georg M. Gardossi, Lucia Pellis, Alessandro |
spellingShingle |
Comerford, James William Byrne, Fergal Weinberger, Simone Farmer, Thomas James Guebitz, Georg M. Gardossi, Lucia Pellis, Alessandro Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
author_facet |
Comerford, James William Byrne, Fergal Weinberger, Simone Farmer, Thomas James Guebitz, Georg M. Gardossi, Lucia Pellis, Alessandro |
author_sort |
Comerford, James William |
title |
Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
title_short |
Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
title_full |
Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
title_fullStr |
Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
title_full_unstemmed |
Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters |
title_sort |
thermal upgrade of enzymatically synthesized aliphatic and aromatic oligoesters |
publishDate |
2020 |
url |
https://eprints.whiterose.ac.uk/155565/ https://eprints.whiterose.ac.uk/155565/1/materials_13_00368.pdf https://doi.org/10.3390/ma13020368 |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_relation |
https://eprints.whiterose.ac.uk/155565/1/materials_13_00368.pdf Comerford, James William orcid.org/0000-0002-9977-5695 , Byrne, Fergal, Weinberger, Simone et al. (4 more authors) (2020) Thermal Upgrade of Enzymatically Synthesized Aliphatic and Aromatic Oligoesters. Materials. 368. pp. 1-9. ISSN 1996-1944 |
op_rights |
cc_by |
op_rightsnorm |
CC-BY |
op_doi |
https://doi.org/10.3390/ma13020368 |
container_title |
Materials |
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13 |
container_issue |
2 |
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368 |
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1766056496991305728 |