Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309-0215, USA.
Biochemistry. 2012 Oct 9;51(40):7833-45. doi: 10.1021/bi300365k. Epub 2012 Sep 26.
Chromosome ends are complex structures, consisting of repetitive DNA sequence terminating in an ssDNA overhang with many associated proteins. Because alteration of the regulation of these ends is a hallmark of cancer, telomeres and telomere maintenance have been prime drug targets. The universally conserved ssDNA overhang is sequence-specifically bound and regulated by Pot1 (protection of telomeres 1), and perturbation of Pot1 function has deleterious effects for proliferating cells. The specificity of the Pot1/ssDNA interaction and the key involvement of this protein in telomere maintenance have suggested directed inhibition of Pot1/ssDNA binding as an efficient means of disrupting telomere function. To explore this idea, we developed a high-throughput time-resolved fluorescence resonance energy transfer (TR-FRET) screen for inhibitors of Pot1/ssDNA interaction. We conducted this screen with the DNA-binding subdomain of Schizosaccharomyces pombe Pot1 (Pot1pN), which confers the vast majority of Pot1 sequence-specificity and is highly similar to the first domain of human Pot1 (hPOT1). Screening a library of ∼20 000 compounds yielded a single inhibitor, which we found interacted tightly with sub-micromolar affinity. Furthermore, this compound, subsequently identified as the bis-azo dye Congo red (CR), was able to competitively inhibit hPOT1 binding to telomeric DNA. Isothermal titration calorimetry and NMR chemical shift analysis suggest that CR interacts specifically with the ssDNA-binding cleft of Pot1, and that alteration of this surface disrupts CR binding. The identification of a specific inhibitor of ssDNA interaction establishes a new pathway for targeted telomere disruption.
染色体末端是复杂的结构,由重复的 DNA 序列组成,末端有一个 ssDNA 突出,还有许多相关的蛋白质。由于这些末端的调控改变是癌症的一个标志,端粒和端粒维持已成为主要的药物靶点。普遍保守的 ssDNA 突出由 Pot1(端粒保护 1)特异性结合和调控,而 Pot1 功能的扰动对增殖细胞有有害影响。Pot1/ssDNA 相互作用的特异性和该蛋白在端粒维持中的关键作用表明,定向抑制 Pot1/ssDNA 结合是破坏端粒功能的有效方法。为了探索这个想法,我们开发了一种高通量时间分辨荧光共振能量转移(TR-FRET)筛选 Pot1/ssDNA 相互作用抑制剂的方法。我们用酿酒酵母 Pot1(Pot1pN)的 DNA 结合亚结构域进行了这种筛选,该亚结构域赋予了 Pot1 绝大部分的序列特异性,并且与人类 Pot1(hPOT1)的第一个结构域高度相似。筛选了大约 20000 种化合物的文库,得到了一种单一的抑制剂,我们发现它与亚微摩尔亲和力紧密相互作用。此外,这种化合物,随后被确定为双偶氮染料刚果红(CR),能够竞争性抑制 hPOT1 与端粒 DNA 的结合。等温滴定量热法和 NMR 化学位移分析表明,CR 特异性地与 Pot1 的 ssDNA 结合裂缝相互作用,并且这种表面的改变会破坏 CR 结合。ssDNA 相互作用的特异性抑制剂的鉴定为靶向端粒破坏建立了新的途径。