Exploring the Role of 2-Chloro-6-fluoro Substitution in 2-Alkylthio-6-benzyl-5-alkylpyrimidin-4(3H)-ones: Effects in HIV-1-Infected Cells and in HIV-1 Reverse Transcriptase Enzymes


Por: Rotili, D, Tarantino, D, Nawrozkij, MB, Babushkin, AS, Botta, G, Marrocco, B, Cirilli, R, Menta, S, Badia, R, Crespan, E, Ballante, F, Ragno, R, Este, JA, Maga, G and Mai, A

Publicada: 26 jun 2014
Resumen:
A comparison of the effects of the 6-(2-chloro-6-fluorobenzyl)-2-(alkylthio)pyrimidin-4(3H)-ones (2-Cl-6-F-S-DABOs) 7-12 and the related 6-(2,6-difluorobenzyl) counterparts 13-15 in HIV-1 infected cells and in the HIV-1 reverse transcriptase (RT) assays is here described. The new 2-Cl-6-F-S-DABOs showed up to picomolar activity against wt HIV-1. Against clinically relevant HIV-1 mutants and in enzyme assays, the simultaneous C5(methyl)/C6(methyl/ethyl) substitution in the 2-Cl-6-F- and 2,6-F-2-benzyl series furnished compounds with the highest, wide-spectrum inhibitory activity against HIV-1. Three representative 2-Cl-6-F-S-DABOs carrying two (9c, 10c) or one (10a) stereogenic centers were resolved into their individual stereoisomers and showed a significant diastereo- and enantioselectivity in HIV-1 inhibition, the highest antiviral activity well correlating with the R absolute configuration to the stereogenic center of the C6-benzylic position in both cellular and enzymatic tests. Application of previously reported COMBINEr protocol on 9c and 10c confirmed the influence of the stereogenic centers on their binding modes in the HIV-1 RT.

Filiaciones:
Rotili, D:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

Tarantino, D:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

Nawrozkij, MB:
 Volgograd State Tech Univ, Volgograd 400131, Russia

Babushkin, AS:
 Volgograd State Tech Univ, Volgograd 400131, Russia

Botta, G:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

Marrocco, B:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

Cirilli, R:
 Ist Super Sanita, Dipartimento Farmaco, I-00161 Rome, Italy

Menta, S:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

:
 Univ Autonoma Barcelona, Hosp Univ Germans Trias & Pujol, IrsiCaixa, Badalona 08916, Spain

Crespan, E:
 CNR, IGM, I-27100 Pavia, Italy

Ballante, F:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, Rome Ctr Mol Design, I-00185 Rome, Italy

 Washington Univ, Sch Med, Dept Biochem & Mol Biophys, St Louis, MO 63130 USA

Ragno, R:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, Rome Ctr Mol Design, I-00185 Rome, Italy

:
 Univ Autonoma Barcelona, Hosp Univ Germans Trias & Pujol, IrsiCaixa, Badalona 08916, Spain

Maga, G:
 CNR, IGM, I-27100 Pavia, Italy

Mai, A:
 Univ Roma La Sapienza, Dipartimento Chim & Tecnol Farmaco, I-00185 Rome, Italy

 Univ Roma La Sapienza, Ist Pasteur Fdn Cenci Bolognetti, I-00185 Rome, Italy
ISSN: 15204804





Journal of Medicinal Chemistry
Editorial
American Chemical Society, 1155 16TH ST, NW, WASHINGTON, DC 20036 USA, Estados Unidos America
Tipo de documento: Article
Volumen: 57 Número: 12
Páginas: 5212-5225
WOS Id: 000338184100018
ID de PubMed: 24933420
imagen Green Published

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