Periotrap Pharmaceuticals GmbH, Halle (Saale), Germany.
Department of Molecular Drug Design and Target Validation, Fraunhofer Institute for Cell Therapy and Immunology, Halle (Saale), Germany.
J Biol Chem. 2021 Jan-Jun;296:100263. doi: 10.1016/j.jbc.2021.100263. Epub 2021 Jan 8.
The development of a targeted therapy would significantly improve the treatment of periodontitis and its associated diseases including Alzheimer's disease, rheumatoid arthritis, and cardiovascular diseases. Glutaminyl cyclases (QCs) from the oral pathogens Porphyromonas gingivalis, Tannerella forsythia, and Prevotella intermedia represent attractive target enzymes for small-molecule inhibitor development, as their action is likely to stabilize essential periplasmic and outer membrane proteins by N-terminal pyroglutamination. In contrast to other microbial QCs that utilize the so-called type I enzymes, these oral pathogens possess sequences corresponding to type II QCs, observed hitherto only in animals. However, whether differences between these bacteroidal QCs and animal QCs are sufficient to enable development of selective inhibitors is not clear. To learn more, we recombinantly expressed all three QCs. They exhibit comparable catalytic efficiencies and are inhibited by metal chelators. Crystal structures of the enzymes from P. gingivalis (PgQC) and T. forsythia (TfQC) reveal a tertiary structure composed of an eight-stranded β-sheet surrounded by seven α-helices, typical of animal type II QCs. In each case, an active site Zn ion is tetrahedrally coordinated by conserved residues. Nevertheless, significant differences to mammalian enzymes are found around the active site of the bacteroidal enzymes. Application of a PgQC-selective inhibitor described here for the first time results in growth inhibition of two P. gingivalis clinical isolates in a dose-dependent manner. The insights gained by these studies will assist in the development of highly specific small-molecule bacteroidal QC inhibitors, paving the way for alternative therapies against periodontitis and associated diseases.
靶向治疗的发展将显著改善牙周炎及其相关疾病(包括阿尔茨海默病、类风湿性关节炎和心血管疾病)的治疗效果。口腔病原体牙龈卟啉单胞菌、福赛斯坦纳菌和中间普氏菌的谷氨酰胺环化酶(QC)代表了小分子抑制剂开发的有吸引力的靶酶,因为它们的作用可能通过 N 端焦谷氨酸化稳定必需的周质和外膜蛋白。与其他利用所谓的 I 型酶的微生物 QC 不同,这些口腔病原体具有与迄今仅在动物中观察到的 II 型 QC 相对应的序列。然而,这些细菌 QC 和动物 QC 之间的差异是否足以使选择性抑制剂的开发成为可能尚不清楚。为了了解更多信息,我们重组表达了所有三种 QC。它们表现出可比的催化效率,并被金属螯合剂抑制。来自牙龈卟啉单胞菌(PgQC)和福赛斯坦纳菌(TfQC)的酶的晶体结构揭示了一种由八链β-折叠包围的七螺旋结构,这是动物 II 型 QC 的典型结构。在每种情况下,一个活性位点 Zn 离子被保守残基四面配位。然而,在细菌酶的活性位点周围发现了与哺乳动物酶的显著差异。本文首次应用一种对 PgQC 具有选择性的抑制剂,结果表明该抑制剂以剂量依赖的方式抑制了两种牙龈卟啉单胞菌临床分离株的生长。这些研究的结果将有助于开发高度特异性的细菌 QC 小分子抑制剂,为牙周炎和相关疾病的替代疗法铺平道路。