State Key Laboratory of Chirosciences and Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China.
Shenzhen Key Laboratory for Food Biological Safety Control, Food Safety and Technology Research Centre, The Hong Kong PolyU Shenzhen Research Institute, Shenzhen, China.
Eur J Med Chem. 2018 Jul 15;155:285-302. doi: 10.1016/j.ejmech.2018.06.007. Epub 2018 Jun 6.
The worldwide prevalence of NDM-1-producing bacteria has drastically undermined the clinical efficacy of the last line antibiotic of carbapenems, prompting a need to devise effective strategy to preserve their clinical value. Our previous studies have shown that ebselen can restore the efficacy of meropenem against a laboratory strain that produces NDM-1. Here we report the construction of a focused compound library of 1,2-benzisoselenazol-3(2H)-one derivatives which comprise a total of forty-six candidate compounds. The structure-activity relationship of these compounds and their potential to serve as an adjuvant to enhance the antimicrobial efficacy of meropenem against a collection of clinical NDM-1-producing carbapenem-resistant Enterobacteriaceae isolates was examined. Drug combination assays indicated that these derivatives exhibited synergistic antimicrobial activity when used along with meropenem, effectively restoring the activity of carbapenems against the resistant strains tested in a Galleria mellonella larvae in vivo infection model. The mode of inhibition of one compound, namely 11_a38, which was depicted when tested on the purified NDM-1 enzyme, indicated that it could covalently bind to the enzyme and displaced one zinc ion from the active site. Overall, this study provides a novel 1,2-benzisoselenazol-3(2H)-one scaffold that exhibits strong synergistic antimicrobial activity with carbapenems, and low cytotoxicity. The prospect of application of such compounds as carbapenem adjuvants warrants further evaluation.
全球范围内产生 NDM-1 的细菌的流行率急剧降低了碳青霉烯类抗生素的最后一线治疗效果,因此需要制定有效的策略来保持其临床价值。我们之前的研究表明,依布硒啉可以恢复美罗培南对产生 NDM-1 的实验室菌株的疗效。在这里,我们报告了 1,2-苯并异硒唑-3(2H)-酮衍生物的聚焦化合物文库的构建,该文库共包含 46 种候选化合物。这些化合物的结构-活性关系及其作为佐剂增强美罗培南对临床产 NDM-1 碳青霉烯类耐药肠杆菌科分离株抗菌功效的潜力进行了研究。药物联合试验表明,这些衍生物与美罗培南联合使用时表现出协同抗菌活性,有效恢复了在大蜡螟幼虫体内感染模型中对耐药菌株的碳青霉烯类药物的活性。在对纯化的 NDM-1 酶进行测试时,一种化合物,即 11_a38 的抑制模式表明,它可以与酶发生共价结合,并从活性部位置换出一个锌离子。总的来说,这项研究提供了一个新的 1,2-苯并异硒唑-3(2H)-酮支架,与碳青霉烯类药物表现出很强的协同抗菌活性,且细胞毒性低。将这些化合物作为碳青霉烯类抗生素佐剂应用的前景值得进一步评估。