Evans Sian E, Goult Benjamin T, Fairall Louise, Jamieson Andrew G, Ko Ferrigno Paul, Ford Robert, Schwabe John W R, Wagner Simon D
Department of Biochemistry, University of Leicester, Leicester, United Kingdom; Department of Cancer Studies and Molecular Medicine and MRC Toxicology Unit, University of Leicester, Leicester, United Kingdom.
Department of Biochemistry, University of Leicester, Leicester, United Kingdom.
PLoS One. 2014 Mar 4;9(3):e90889. doi: 10.1371/journal.pone.0090889. eCollection 2014.
BCL6 is a transcriptional repressor that is over-expressed due to chromosomal translocations, or other abnormalities, in ∼40% of diffuse large B-cell lymphoma. BCL6 interacts with co-repressor, SMRT, and this is essential for its role in lymphomas. Peptide or small molecule inhibitors, which prevent the association of SMRT with BCL6, inhibit transcriptional repression and cause apoptosis of lymphoma cells in vitro and in vivo. In order to discover compounds, which have the potential to be developed into BCL6 inhibitors, we screened a natural product library. The ansamycin antibiotic, rifamycin SV, inhibited BCL6 transcriptional repression and NMR spectroscopy confirmed a direct interaction between rifamycin SV and BCL6. To further determine the characteristics of compounds binding to BCL6-POZ we analyzed four other members of this family and showed that rifabutin, bound most strongly. An X-ray crystal structure of the rifabutin-BCL6 complex revealed that rifabutin occupies a partly non-polar pocket making interactions with tyrosine58, asparagine21 and arginine24 of the BCL6-POZ domain. Importantly these residues are also important for the interaction of BLC6 with SMRT. This work demonstrates a unique approach to developing a structure activity relationship for a compound that will form the basis of a therapeutically useful BCL6 inhibitor.
BCL6是一种转录抑制因子,在约40%的弥漫性大B细胞淋巴瘤中,由于染色体易位或其他异常而过度表达。BCL6与共抑制因子SMRT相互作用,这对其在淋巴瘤中的作用至关重要。肽或小分子抑制剂可阻止SMRT与BCL6结合,在体外和体内均可抑制转录抑制并导致淋巴瘤细胞凋亡。为了发现有潜力开发成BCL6抑制剂的化合物,我们筛选了一个天然产物文库。安莎霉素类抗生素利福霉素SV可抑制BCL6转录抑制,核磁共振光谱证实利福霉素SV与BCL6之间存在直接相互作用。为了进一步确定与BCL6-POZ结合的化合物的特性,我们分析了该家族的其他四个成员,结果表明利福布汀结合力最强。利福布汀-BCL6复合物的X射线晶体结构显示,利福布汀占据了一个部分非极性口袋,与BCL6-POZ结构域的酪氨酸58、天冬酰胺21和精氨酸24相互作用。重要的是,这些残基对于BLC6与SMRT的相互作用也很重要。这项工作展示了一种独特的方法来建立一种化合物的构效关系,这将成为一种治疗有用的BCL6抑制剂的基础。