QM/MM MD studies of polyester synthesis/hydrolysis
The world is suffering the consequences of plastic pollution, however modern societies remain heavily reliant on plastics. More sustainable alternatives are actively being sought-after. Enzymatic synthesis can offer a more sustainable route for polyester synthesis. Nevertheless, there are still limi...
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fteci:oai:dc.engconfintl.org:enzyme_xxv-1059 2023-05-15T14:04:06+02:00 QM/MM MD studies of polyester synthesis/hydrolysis Carvalho, Alexandra T. P. Figueiredo, Pedro Almeida, Beatriz C. 2019-09-16T07:00:00Z https://dc.engconfintl.org/enzyme_xxv/90 unknown ECI Digital Archives https://dc.engconfintl.org/enzyme_xxv/90 Enzyme Engineering XXV Biodegradable polyesters polycaprolactone enzymatic synthesis AfEST lipase carboxylesterase CaLB QM/MM MD sim-ulations Engineering text 2019 fteci 2022-12-27T14:51:37Z The world is suffering the consequences of plastic pollution, however modern societies remain heavily reliant on plastics. More sustainable alternatives are actively being sought-after. Enzymatic synthesis can offer a more sustainable route for polyester synthesis. Nevertheless, there are still limitations, such as limited activity and selectivity for some monomers, unfavorable compatibility in chemoenzymatic reactions and low stability under harsh reactions conditions. We have studied the catalytic mechanisms for polycaprolactone hydrolysis/synthesis by the wildtype enzymes Archaeoglobus fulgidus carboxylesterase (AfEST) and Candida antarctica lipase B (CaLB) and respective enzyme variants by performing Quantum Mechanics/Molecular Mechanics Molecular Dynamics simulations [1-3]. Our results give important insights towards the design of new enzyme variants combining good activity with high thermostability. [1] Almeida, B., Figueiredo, P., Carvalho, A. PCL enzymatic hydrolysis: a mechanistic study. ACS Omega. Doi:10.1021/acsomega.9b00345. [2] Carvalho, A. T. P., Dourado, D. F. A. R., Skvortsov, T., de Abreu M., Ferguson, L. J., Quinn, D. J., Moody, T. S. Huang, M. Spatial requirement for PAMO for transformation of non-native linear substrates. Phys. Chem. Chem. Phys. 2018. [3] Dourado D. F. A. R., Swart M., Carvalho A. T. P. Why the flavin dinucleotide cofactor needs to be covalently linked to Complex II of the electron transport chain for conversion of FADH2 to FAD. Chem. – Eur J. 2018. Text Antarc* Antarctica Engineering Conferences International: ECI Digital Archives Ferguson ENVELOPE(-168.583,-168.583,-84.933,-84.933) |
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Engineering Conferences International: ECI Digital Archives |
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topic |
Biodegradable polyesters polycaprolactone enzymatic synthesis AfEST lipase carboxylesterase CaLB QM/MM MD sim-ulations Engineering |
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Biodegradable polyesters polycaprolactone enzymatic synthesis AfEST lipase carboxylesterase CaLB QM/MM MD sim-ulations Engineering Carvalho, Alexandra T. P. Figueiredo, Pedro Almeida, Beatriz C. QM/MM MD studies of polyester synthesis/hydrolysis |
topic_facet |
Biodegradable polyesters polycaprolactone enzymatic synthesis AfEST lipase carboxylesterase CaLB QM/MM MD sim-ulations Engineering |
description |
The world is suffering the consequences of plastic pollution, however modern societies remain heavily reliant on plastics. More sustainable alternatives are actively being sought-after. Enzymatic synthesis can offer a more sustainable route for polyester synthesis. Nevertheless, there are still limitations, such as limited activity and selectivity for some monomers, unfavorable compatibility in chemoenzymatic reactions and low stability under harsh reactions conditions. We have studied the catalytic mechanisms for polycaprolactone hydrolysis/synthesis by the wildtype enzymes Archaeoglobus fulgidus carboxylesterase (AfEST) and Candida antarctica lipase B (CaLB) and respective enzyme variants by performing Quantum Mechanics/Molecular Mechanics Molecular Dynamics simulations [1-3]. Our results give important insights towards the design of new enzyme variants combining good activity with high thermostability. [1] Almeida, B., Figueiredo, P., Carvalho, A. PCL enzymatic hydrolysis: a mechanistic study. ACS Omega. Doi:10.1021/acsomega.9b00345. [2] Carvalho, A. T. P., Dourado, D. F. A. R., Skvortsov, T., de Abreu M., Ferguson, L. J., Quinn, D. J., Moody, T. S. Huang, M. Spatial requirement for PAMO for transformation of non-native linear substrates. Phys. Chem. Chem. Phys. 2018. [3] Dourado D. F. A. R., Swart M., Carvalho A. T. P. Why the flavin dinucleotide cofactor needs to be covalently linked to Complex II of the electron transport chain for conversion of FADH2 to FAD. Chem. – Eur J. 2018. |
format |
Text |
author |
Carvalho, Alexandra T. P. Figueiredo, Pedro Almeida, Beatriz C. |
author_facet |
Carvalho, Alexandra T. P. Figueiredo, Pedro Almeida, Beatriz C. |
author_sort |
Carvalho, Alexandra T. P. |
title |
QM/MM MD studies of polyester synthesis/hydrolysis |
title_short |
QM/MM MD studies of polyester synthesis/hydrolysis |
title_full |
QM/MM MD studies of polyester synthesis/hydrolysis |
title_fullStr |
QM/MM MD studies of polyester synthesis/hydrolysis |
title_full_unstemmed |
QM/MM MD studies of polyester synthesis/hydrolysis |
title_sort |
qm/mm md studies of polyester synthesis/hydrolysis |
publisher |
ECI Digital Archives |
publishDate |
2019 |
url |
https://dc.engconfintl.org/enzyme_xxv/90 |
long_lat |
ENVELOPE(-168.583,-168.583,-84.933,-84.933) |
geographic |
Ferguson |
geographic_facet |
Ferguson |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_source |
Enzyme Engineering XXV |
op_relation |
https://dc.engconfintl.org/enzyme_xxv/90 |
_version_ |
1766275100164751360 |