Improving the Biodesulfurization of Crude Oil and Derivatives: A QM/MM Investigation of the Catalytic Mechanism of NADH-FMN Oxidoreductase (DszD)

• Tipo: Artigo em Revista Científica Internacional
• Data: 2016

Autores

Sergio Filipe Sousa (Autor) FCUP; Sousa, JFM (Autor) Outra; Barbosa, ACC (Autor) Outra; Ferreira, CE (Autor) Outra; Neves, RPP (Autor) Outra; Ribeiro, AJM (Autor) Outra; Pedro A Fernandes (Autor) FCUP; Ramos, MJ (Autor) FCUP

Revista

Título: Journal of Physical Chemistry A

Vol. 120

Páginas: 5300-5306

ISSN: 1089-5639

Editora: American Chemical Society

Indexação

ISI Web of Knowledge - 19 Citações

Scopus - 16 Citações

Outras Informações

ID Authenticus: P-00K-N69

DOI: 10.1021/acs.jpca.6b01536

Abstract (EN): The development of biocatalytic desulfurization strategies of petroleum and its derivatives could result in more economic alternatives than the widely used chemical desulfurization. The organism Rhodococcus erythropolis IGTS8 has been shown to metabolize organic sulfur compounds through a mechanism known as 4S pathway, which involves four enzymes (DszA, DszB, DszC, and DszD) and has been explored in biodesulfurization. Here we have applied QM/MM methods to study the catalytic mechanism of the enzyme DszD, a NADH-FMN oxidoreductase that occupies a central place on the 4S pathway by catalyzing the formation of the FMNH2 that is used by the two monooxynases in the cycle: DszA and DszC. In addition, to clarify the catalytic mechanism of this enzyme, this study analyzed in detail the role played by the active site Thr residue and of Asn and Ala enzyme mutants. The results help to explain previous experimental evidence and suggest new strategies for improving biodesulfurization through an increase in the activity of DszD.

Idioma: Inglês

Tipo (Avaliação Docente): Científica

Nº de páginas: 7