Michailidis E, Singh K, Ryan E M, Hachiya A, Ong Y T, Kirby K A, Marchand B, Kodama E N, Mitsuya H, Parniak M A, Sarafianos S G
Christopher S. Bond Life Sciences Center and Department of Molecular Microbiology & Immunology, School of Medicine, University of Missouri, Columbia, MO 65211, USA.
Cell Mol Biol (Noisy-le-grand). 2012 Dec 22;58(1):187-95.
4'-ethynyl-2-fluoro-2'-deoxyadenosine (EFdA) is a highly potent inhibitor of HIV-1 reverse transcriptase (RT). We have previously shown that its exceptional antiviral activity stems from a unique mechanism of action that is based primarily on blocking translocation of RT; therefore we named EFdA a Translocation Defective RT Inhibitor (TDRTI). The N348I mutation at the connection subdomain (CS) of HIV-1 RT confers clinically significant resistance to both nucleoside (NRTIs) and non-nucleoside RT inhibitors (NNRTIs). In this study we tested EFdA-triphosphate (TP) together with a related compound, ENdA-TP (4'-ethynyl-2-amino-2'-deoxdyadenosine triphosphate) against HIV-1 RTs that carry clinically relevant drug resistance mutations: N348I, D67N/K70R/L210Q/T215F, D67N/K70R/L210Q/T215F/N348I, and A62V/V5I/F77L/F116Y/Q151M. We demonstrate that these enzymes remain susceptible to TDRTIs. Similar to WT RT, the N348I RT is inhibited by EFdA mainly at the point of incorporation through decreased translocation. In addition, the N348I substitution decreases the RNase H cleavage of DNA terminated with EFdA-MP (T/P(EFdA-MP)). Moreover, N348I RT unblocks EFdA-terminated primers with similar efficiency as the WT enzyme, and further enhances EFdA unblocking in the background of AZT-resistance mutations. This study provides biochemical insights into the mechanism of inhibition of N348I RT by TDRTIs and highlights the excellent efficacy of this class of inhibitors against WT and drug-resistant HIV-1 RTs.
4'-乙炔基-2-氟-2'-脱氧腺苷(EFdA)是一种高效的HIV-1逆转录酶(RT)抑制剂。我们之前已经表明,其卓越的抗病毒活性源于一种独特的作用机制,该机制主要基于阻断RT的易位;因此我们将EFdA命名为易位缺陷型RT抑制剂(TDRTI)。HIV-1 RT连接亚结构域(CS)的N348I突变赋予了对核苷类(NRTIs)和非核苷类RT抑制剂(NNRTIs)临床上显著的耐药性。在本研究中,我们将EFdA-三磷酸(TP)与一种相关化合物ENdA-TP(4'-乙炔基-2-氨基-2'-脱氧腺苷三磷酸)一起针对携带临床相关耐药突变的HIV-1 RTs进行了测试:N348I、D67N/K70R/L210Q/T215F、D67N/K70R/L210Q/T215F/N348I以及A62V/V5I/F77L/F116Y/Q151M。我们证明这些酶对TDRTIs仍然敏感。与野生型RT相似,N348I RT主要在掺入点被EFdA抑制,通过减少易位实现。此外,N348I替代降低了以EFdA-MP(T/P(EFdA-MP))终止的DNA的核糖核酸酶H切割。而且,N348I RT以与野生型酶相似的效率解封以EFdA终止的引物,并在AZT耐药突变背景下进一步增强EFdA的解封。本研究为TDRTIs抑制N348I RT的机制提供了生化见解,并突出了这类抑制剂对野生型和耐药HIV-1 RTs的优异疗效。