Arico-Muendel Christopher, Zhu Zhengrong, Dickson Hamilton, Parks Derek, Keicher Jesse, Deng Jianghe, Aquilani Leah, Coppo Frank, Graybill Todd, Lind Kenneth, Peat Andrew, Thomson Michael
GlaxoSmithKline, Boston, Massachusetts, USA.
GlaxoSmithKline, Research Triangle Park, North Carolina, USA.
Antimicrob Agents Chemother. 2015;59(6):3450-9. doi: 10.1128/AAC.00070-15. Epub 2015 Mar 30.
To identify novel antivirals to the hepatitis C virus (HCV) NS4B protein, we utilized encoded library technology (ELT), which enables purified proteins not amenable to standard biochemical screening methods to be tested against large combinatorial libraries in a short period of time. We tested NS4B against several DNA-encoded combinatorial libraries (DEL) and identified a single DEL feature that was subsequently progressed to off-DNA synthesis. The most active of the initial synthesized compounds had 50% inhibitory concentrations (IC50s) of 50 to 130 nM in a NS4B radioligand binding assay and 300 to 500 nM in an HCV replicon assay. Chemical optimization yielded compounds with potencies as low as 20 nM in an HCV genotype 1b replicon assay, 500 nM against genotype 1a, and 5 μM against genotype 2a. Through testing against other genotypes and genotype 2a-1b chimeric replicons and from resistance passage using the genotype 1b replicon, we confirmed that these compounds were acting on the proposed first transmembrane region of NS4B. A single sequence change (F98L) was identified as responsible for resistance, and it was thought to largely explain the relative lack of potency of this series against genotype 2a. Unlike other published series that appear to interact with this region, we did not observe sensitivity to amino acid substitutions at positions 94 and 105. The discovery of this novel compound series highlights ELT as a valuable approach for identifying direct-acting antivirals to nonenzymatic targets.
为了鉴定针对丙型肝炎病毒(HCV)NS4B蛋白的新型抗病毒药物,我们采用了编码文库技术(ELT),该技术能够在短时间内针对大型组合文库测试那些不适用于标准生化筛选方法的纯化蛋白。我们用NS4B对几个DNA编码组合文库(DEL)进行了测试,并鉴定出一个单一的DEL特征,随后将其推进到非DNA合成阶段。最初合成的化合物中活性最高的在NS4B放射性配体结合试验中的50%抑制浓度(IC50)为50至130 nM,在HCV复制子试验中为300至500 nM。化学优化产生的化合物在HCV 1b基因型复制子试验中的效力低至20 nM,对1a基因型的效力为500 nM,对2a基因型的效力为5 μM。通过对其他基因型和2a-1b基因型嵌合复制子的测试以及使用1b基因型复制子进行抗性传代,我们证实这些化合物作用于NS4B提议的第一个跨膜区域。鉴定出一个单一的序列变化(F98L)是导致抗性的原因,并且认为这在很大程度上解释了该系列对2a基因型相对缺乏效力的原因。与其他已发表的似乎与该区域相互作用的系列不同,我们没有观察到对94和105位氨基酸取代的敏感性。这个新型化合物系列的发现突出了ELT作为鉴定针对非酶靶点的直接作用抗病毒药物的一种有价值方法。