Nijampatnam Bhavitavya, Casals Luke, Zheng Ruowen, Wu Hui, Velu Sadanandan E
Department of Chemistry, University of Alabama at Birmingham, 901, 14th Street S, Birmingham, AL 35294, USA.
Department of Pediatric Dentistry, UAB School of Dentistry, Birmingham, AL 35294, USA.
Bioorg Med Chem Lett. 2016 Aug 1;26(15):3508-13. doi: 10.1016/j.bmcl.2016.06.033. Epub 2016 Jun 14.
Streptococcus mutans has been implicated as the major etiological agent in the initiation and the development of dental caries due to its robust capacity to form tenacious biofilms. Ideal therapeutics for this disease will aim to selectively inhibit the biofilm formation process while preserving the natural bacterial flora of the mouth. Several studies have demonstrated the efficacies of flavonols on S. mutans biofilms and have suggested the mechanism of action through their effect on S. mutans glucosyltransferases (Gtfs). These enzymes metabolize sucrose into water insoluble and soluble glucans, which are an integral measure of the dental caries pathogenesis. Numerous studies have shown that flavonols and polyphenols can inhibit Gtf and biofilm formation at millimolar concentrations. We have screened a group of 14 hydroxychalcones, synthetic precursors of flavonols, in an S. mutans biofilm assay. Several of these compounds emerged to be biofilm inhibitors at low micro-molar concentrations. Chalcones that contained a 3-OH group on ring A exhibited selectivity for biofilm inhibition. Moreover, we synthesized 6 additional analogs of the lead compound and evaluated their potential activity and selectivity against S. mutans biofilms. The most active compound identified from these studies had an IC50 value of 44μM against biofilm and MIC50 value of 468μM against growth displaying >10-fold selectivity inhibition towards biofilm. The lead compound displayed a dose dependent inhibition of S. mutans Gtfs. The lead compound also did not affect the growth of two commensal species (Streptococcus sanguinis and Streptococcus gordonii) at least up to 200μM, indicating that it can selectively inhibit cariogenic biofilms, while leaving commensal and/or beneficial microbes intact. Thus non-toxic compounds have the potential utility in public oral health regimes.
变形链球菌因其形成坚韧生物膜的强大能力,被认为是龋齿发生和发展的主要病原体。针对这种疾病的理想治疗方法旨在选择性抑制生物膜形成过程,同时保留口腔中的天然细菌菌群。多项研究已证明黄酮醇对变形链球菌生物膜的疗效,并提出了其通过对变形链球菌葡糖基转移酶(Gtfs)的作用机制。这些酶将蔗糖代谢为水不溶性和可溶性葡聚糖,这是龋齿发病机制的一个重要指标。大量研究表明,黄酮醇和多酚在毫摩尔浓度下可抑制Gtf和生物膜形成。我们在变形链球菌生物膜试验中筛选了一组14种羟基查耳酮,它们是黄酮醇的合成前体。其中几种化合物在低微摩尔浓度下表现出生物膜抑制作用。在A环上含有3-OH基团的查耳酮对生物膜抑制具有选择性。此外,我们合成了先导化合物的6种额外类似物,并评估了它们对变形链球菌生物膜的潜在活性和选择性。从这些研究中鉴定出的最具活性的化合物对生物膜的IC50值为44μM,对生长的MIC50值为468μM,对生物膜表现出>10倍的选择性抑制。先导化合物对变形链球菌Gtfs表现出剂量依赖性抑制。先导化合物在至少200μM浓度下也不影响两种共生菌(血链球菌和戈登链球菌)的生长,这表明它可以选择性抑制致龋生物膜,同时保持共生和/或有益微生物的完整。因此,无毒化合物在公共口腔卫生领域具有潜在用途。