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.v2 2024-04-07T07:48:10+00:00 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.v2 https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/60c7474e0f50db424e3965a8/original/enzymatic-synthesis-of-polyesters-a-qm-mm-study.pdf 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.v2 2024-03-08T00:19:04Z 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 Archaeoglobus fulgidus carboxylesterase (AfEST) and Candida antarctica 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 |
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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 Archaeoglobus fulgidus carboxylesterase (AfEST) and Candida antarctica 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.v2 https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/60c7474e0f50db424e3965a8/original/enzymatic-synthesis-of-polyesters-a-qm-mm-study.pdf |
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.v2 |
_version_ |
1795662045816815616 |