Enzymatic Synthesis of Polyesters: A QM/MM Study
Plastic pollution is causing an immeasurable damage to marine and land eco-systems. Better alternatives are actively being sought-after, such as biodegradable polyesters obtained by enzymatic synthesis. However, wild type enzymes still pose fundamental efficiency limitations that can be circumvented...
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cracsoc:10.26434/chemrxiv.9638270 2023-07-30T03:59:28+02:00 Enzymatic Synthesis of Polyesters: A QM/MM Study Figueiredo, Pedro Almeida, Beatriz C. Dourado, Daniel F.A.R. Sousa, Andreia F. Silvestre, Armando J.D. Carvalho, Alexandra 2020 http://dx.doi.org/10.26434/chemrxiv.9638270 https://ndownloader.figshare.com/files/20694354 unknown American Chemical Society (ACS) https://creativecommons.org/licenses/by-nc-nd/4.0/ posted-content 2020 cracsoc https://doi.org/10.26434/chemrxiv.9638270 2023-07-16T23:26:25Z Plastic pollution is causing an immeasurable damage to marine and land eco-systems. Better alternatives are actively being sought-after, such as biodegradable polyesters obtained by enzymatic synthesis. However, wild type enzymes still pose fundamental efficiency limitations that can be circumvented by protein reengineering approaches.Here we compare in detail the catalytic mechanisms for polycaprolactone synthesis by the enzymes <i>Archaeoglobus fulgidus</i> carboxylesterase (AfEST) and <i>Candida antarctica</i> lipase B (CalB) by performing Quantum mechanics calculations and Quantum Mechanics/Molecular Mechanics Molecular Dynamics simulations. We found that bond forming/breaking events are concerted with proton transfer to or from the catalytic histidine in all the transition states, but with different degrees of coupling between the motions of the atoms involved. Our results give important insights towards the design of new enzyme variants combining good activity with high thermostability. Other/Unknown Material Antarc* Antarctica ACS Publications (via Crossref) |
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ACS Publications (via Crossref) |
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description |
Plastic pollution is causing an immeasurable damage to marine and land eco-systems. Better alternatives are actively being sought-after, such as biodegradable polyesters obtained by enzymatic synthesis. However, wild type enzymes still pose fundamental efficiency limitations that can be circumvented by protein reengineering approaches.Here we compare in detail the catalytic mechanisms for polycaprolactone synthesis by the enzymes <i>Archaeoglobus fulgidus</i> carboxylesterase (AfEST) and <i>Candida antarctica</i> lipase B (CalB) by performing Quantum mechanics calculations and Quantum Mechanics/Molecular Mechanics Molecular Dynamics simulations. We found that bond forming/breaking events are concerted with proton transfer to or from the catalytic histidine in all the transition states, but with different degrees of coupling between the motions of the atoms involved. Our results give important insights towards the design of new enzyme variants combining good activity with high thermostability. |
format |
Other/Unknown Material |
author |
Figueiredo, Pedro Almeida, Beatriz C. Dourado, Daniel F.A.R. Sousa, Andreia F. Silvestre, Armando J.D. Carvalho, Alexandra |
spellingShingle |
Figueiredo, Pedro Almeida, Beatriz C. Dourado, Daniel F.A.R. Sousa, Andreia F. Silvestre, Armando J.D. Carvalho, Alexandra Enzymatic Synthesis of Polyesters: A QM/MM Study |
author_facet |
Figueiredo, Pedro Almeida, Beatriz C. Dourado, Daniel F.A.R. Sousa, Andreia F. Silvestre, Armando J.D. Carvalho, Alexandra |
author_sort |
Figueiredo, Pedro |
title |
Enzymatic Synthesis of Polyesters: A QM/MM Study |
title_short |
Enzymatic Synthesis of Polyesters: A QM/MM Study |
title_full |
Enzymatic Synthesis of Polyesters: A QM/MM Study |
title_fullStr |
Enzymatic Synthesis of Polyesters: A QM/MM Study |
title_full_unstemmed |
Enzymatic Synthesis of Polyesters: A QM/MM Study |
title_sort |
enzymatic synthesis of polyesters: a qm/mm study |
publisher |
American Chemical Society (ACS) |
publishDate |
2020 |
url |
http://dx.doi.org/10.26434/chemrxiv.9638270 https://ndownloader.figshare.com/files/20694354 |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_rights |
https://creativecommons.org/licenses/by-nc-nd/4.0/ |
op_doi |
https://doi.org/10.26434/chemrxiv.9638270 |
_version_ |
1772810299568553984 |