Thiadiazole Derivatives: Highly Potent and Specific HIV-1 Reverse Transcriptase Inhibitors

Journal of Medicinal Chemistry
1995.0

Abstract

Reverse transcriptase (RT) is an essential enzyme for the replication of HIV and thus is regarded as one of the most important targets for anti-HIV agents. So far, only nucleoside RT inhibitors such as 3'-azido-3'-deoxythymidine (AZT), 2',3'-dideoxyinosine (ddI), 2',3'-dideoxycytidine (ddC), and 2',3'-didehydro-3'-deoxythymidine (d4T) have been approved for the treatment of HIV-infected patients, but their long-term use leads to toxic side effects like bone marrow suppression. Non-nucleoside inhibitors such as 1-[(2-hydroxyethoxy)methyl]-6-(phenylthio)thymine, dipyridodiazepinone (Nevirapine), and α-anilinophenylacetamide (R-89439, Loviride) have been developed as specific and potent inhibitors of HIV-1 RT. From a random screening program of compounds with herbicidal activities, we identified a series of 1,2,5-thiadiazoles (TDA) as inhibitors of HIV-1. In this communication, we describe the efficient synthesis, anti-HIV-1 activity, and structure-activity relationship of novel non-nucleoside inhibitors with the thiadiazole skeleton. The 3-hydroxyl-4-substituted-1,2,5-thiadiazole nucleus was constructed in good yield by condensing α-amino acid amides with sulfur monochloride in dimethylformamide. The carbamoyl moiety was site-selectively introduced at the 3-hydroxy position of the thiadiazole skeleton using two methods: treatment with carbamoyl chlorides or reaction with triphosgene followed by secondary amines. Antiviral activity was assessed based on inhibition of HIV-1-induced cytopathic effect (CPE) in MT-4 cells or reduction of HIV-1 p24 antigen in peripheral blood lymphocytes (PBLs). The 4-(2,6-dichlorophenyl)-1,2,5-thiadiazol-3-yl N-methyl-N-propylcarbamate (19) exhibited the most potent activity, with an EC50 of 0.013 μM and a CC50 of 131 μM in MT-4 cells (selectivity index = 10 077) and an EC50 of 0.004 μM in PBLs, while it had no effect on HIV-2 replication at concentrations up to 131 μM. Structure-activity relationship studies indicated that the presence of both an aromatic ring at the C-4 position and a carbamate moiety at the C-3 position of the thiadiazole ring was essential for activity. In conclusion, TDA derivatives are highly potent and specific inhibitors of HIV-1. Considering their ease of synthesis, they have potential as candidate drugs for HIV-1 chemotherapy. Mechanistic studies revealed they belong to the family of nonnucleoside HIV-1 RT inhibitors, and further investigations on structure-activity relationships and drug resistance emergence are in progress.

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