Zhou Eric, Seminara Anna B, Kim Soo-Kyoung, Hall Cherisse L, Wang Yan, Lee Vincent T
Department of Cell Biology and Molecular Genetics, University of Maryland , Bioscience Research Building, College Park, Maryland 20742, United States.
Maryland Pathogen Research Institute , Bioscience Research Building, College Park, Maryland 20742, United States.
ACS Chem Biol. 2017 Dec 15;12(12):3076-3085. doi: 10.1021/acschembio.7b00826. Epub 2017 Nov 22.
Pseudomonas aeruginosa is an opportunistic pathogen that affects a large proportion of cystic fibrosis (CF) patients. CF patients have dehydrated mucus within the airways that leads to the inability of the mucociliary escalator to expel inhaled microbes. Once inhaled, P. aeruginosa can persist in the lungs of the CF patients for the remainder of their lives. During this chronic infection, a phenomenon called mucoid conversion can occur in which P. aeruginosa can mutate and inactivate their mucA gene. As a consequence, transcription of the alg operon is highly expressed, leading to the copious secretion of the alginate exopolysaccharide, which is associated with decreased lung function and increased CF patient morbidity and mortality. Alginate biosynthesis by P. aeruginosa is post-translationally regulated by bis(3'-5')-cyclic dimeric guanosine monophosphate (c-di-GMP), which binds to the receptor protein Alg44 to activate alginate production. The identification of small molecules that disrupt the binding of c-di-GMP to Alg44 could inhibit the ability of P. aeruginosa to produce alginate. In this work, a class of thiol-benzo-triazolo-quinazolinone compounds that inhibited Alg44 binding to c-di-GMP in vitro was identified after screening chemical libraries consisting of ∼50 000 chemical compounds. Thiol-benzo-triazolo-quinazolinones were shown to specifically inhibit Alg44-c-di-GMP interactions by forming a disulfide bond with the cysteine residue in the PilZ domain of Alg44. The more potent thiol-benzo-triazolo-quinazolinone had the ability to reduce P. aeruginosa alginate secretion by up to 30%. These compounds serve as leads in the development of novel inhibitors of alginate production by P. aeruginosa after mucoid conversion.
铜绿假单胞菌是一种机会致病菌,会感染很大一部分囊性纤维化(CF)患者。CF患者气道内的黏液脱水,导致黏液纤毛清除系统无法排出吸入的微生物。一旦被吸入,铜绿假单胞菌可在CF患者的肺部持续存在直至其生命结束。在这种慢性感染过程中,会发生一种称为黏液样转化的现象,即铜绿假单胞菌可发生突变并使其mucA基因失活。结果,藻酸盐操纵子的转录高度表达,导致藻酸盐胞外多糖大量分泌,这与肺功能下降以及CF患者发病率和死亡率增加有关。铜绿假单胞菌的藻酸盐生物合成在翻译后由双(3'-5')-环二聚鸟苷单磷酸(c-di-GMP)调节,c-di-GMP与受体蛋白Alg44结合以激活藻酸盐的产生。鉴定出能破坏c-di-GMP与Alg44结合的小分子,可能会抑制铜绿假单胞菌产生藻酸盐的能力。在这项研究中,在筛选了由约50000种化合物组成的化学文库后,鉴定出了一类在体外抑制Alg44与c-di-GMP结合的硫醇-苯并三唑-喹唑啉酮化合物。硫醇-苯并三唑-喹唑啉酮通过与Alg44的PilZ结构域中的半胱氨酸残基形成二硫键,特异性抑制Alg44-c-di-GMP相互作用。更有效的硫醇-苯并三唑-喹唑啉酮能够将铜绿假单胞菌的藻酸盐分泌减少多达30%。这些化合物可作为开发新型抑制剂的先导物,用于抑制黏液样转化后铜绿假单胞菌的藻酸盐产生。