| Texto completo | |
| Autor(es): |
dos Santos, Alberto M.
;
da Costa, Clauber H. S.
;
Silva, Pedro H. A.
;
Skaf, Munir S.
;
Lameira, Jeronimo
Número total de Autores: 5
|
| Tipo de documento: | Artigo Científico |
| Fonte: | Journal of Physical Chemistry B; v. 128, n. 31, p. 14-pg., 2024-07-29. |
| Resumo | |
The enzyme PETase fromIdeonella sakaiensis (IsPETase) strain 201-F6 can catalyze the hydrolysis of polyethylene terephthalate (PET), mainly converting it into mono(2-hydroxyethyl) terephthalic acid (MHET). In this study, we used quantum mechanics/molecular mechanics (QM/MM) simulations to explore the molecular details of the catalytic reaction mechanism of IsPETase in the formation of MHET. The QM region was described with AM1d/PhoT and M06-2X/6-31+G(d,p) potential. QM/MM simulations unveil the complete enzymatic PET hydrolysis mechanism and identify two possible reaction pathways for acylation and deacylation steps. The barrier obtained at M06-2X/6-31+G(d,p)/MM potential for the deacylation step corresponds to 20.4 kcal/mol, aligning with the experimental value of 18 kcal/mol. Our findings indicate that deacylation is the rate-limiting step of the process. Furthermore, per-residue interaction energy contributions revealed unfavorable contributions to the transition state of amino acids located at positions 200-230, suggesting potential sites for targeted mutations. These results can contribute to the development of more active and selective enzymes for PET depolymerization. (AU) | |
| Processo FAPESP: | 13/08293-7 - CECC - Centro de Engenharia e Ciências Computacionais |
| Beneficiário: | Munir Salomao Skaf |
| Modalidade de apoio: | Auxílio à Pesquisa - Centros de Pesquisa, Inovação e Difusão - CEPIDs |
| Processo FAPESP: | 22/04703-5 - Simulações de dinâmica molecular de enzimas de interesse biotecnológico |
| Beneficiário: | Clauber Henrique Souza da Costa |
| Modalidade de apoio: | Bolsas no Brasil - Pós-Doutorado |
| Processo FAPESP: | 22/04695-2 - Mecanismos de reação de enzimas e aprimoramento catalítico com base em estados de transição e algoritmos de aprendizado de máquina |
| Beneficiário: | Alberto Monteiro dos Santos |
| Modalidade de apoio: | Bolsas no Brasil - Pós-Doutorado |