β-D-2'-C-Methyl-2,6-diaminopurine Ribonucleoside Phosphoramidates are Potent and Selective Inhibitors of Hepatitis C Virus (HCV) and Are Bioconverted Intracellularly to Bioactive 2,6-Diaminopurine and Guanosine 5'-Triphosphate Forms

  • J Med Chem. 2015 Apr 23;58(8):3445-58. doi: 10.1021/jm501874e.
Longhu Zhou  1 Hong-wang Zhang  1 Sijia Tao  1 Leda Bassit  1  2 Tony Whitaker  3 Tamara R McBrayer  2  3 Maryam Ehteshami  1 Sheida Amiralaei  1 Ugo Pradere  1 Jong Hyun Cho  1 Franck Amblard  1  2 Drew Bobeck  3 Mervi Detorio  1  2 Steven J Coats  3 Raymond F Schinazi  1  2
Affiliations
  • 1. †Center for AIDS Research, Laboratory of Biochemical Pharmacology, Department of Pediatrics, Emory University School of Medicine, Atlanta, Georgia 30322, United States.
  • 2. ‡Veterans Affairs Medical Center, Decatur, Georgia 30033, United States.
  • 3. §CoCrystal Pharma, Inc., Tucker, Georgia 30084, United States.
Abstract

The conversion of selected β-D-2,6-diaminopurine nucleosides (DAPNs) to their phosphoramidate prodrug (PD) substantially blocks the conversion to the G-analog allowing for the generation of two bioactive nucleoside triphosphates (NTPs) in human hepatocytes. A variety of 2'-C-methyl DAPN-PDs were prepared and evaluated for inhibition of HCV viral replication in Huh-7 cells, cytotoxicity in various cell lines, and cellular pharmacology in both Huh-7 and primary human liver cells. The DAPN-PDs were pan-genotypic, effective against various HCV resistant mutants, and resistant variants could not be selected. 2'-C-Me-DAPN-TP and 2'-C-Me-GTP were chain terminators for genotype 1b HCV-pol, and single nucleotide incorporation assays revealed that 2'-C-Me-DAPN-TP was incorporated opposite U. No cytotoxicity was observed with our DAPN-PD when tested up to 50 μM. A novel, DAPN-PD, 15c, has been selected for further evaluation because of its good virologic and toxicologic profile and its ability to deliver two active metabolites, potentially simplifying HCV treatment.