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

• Type: Article in International Scientific Journal
• Date: 2016

Authors

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

Journal

Title: Journal of Physical Chemistry A

Vol. 120

Pages: 5300-5306

ISSN: 1089-5639

Publisher: American Chemical Society

Indexing

ISI Web of Knowledge - 19 Citations

Scopus - 16 Citations

Other information

Authenticus ID: 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.

Language: English

Type (Professor's evaluation): Scientific

No. of pages: 7