UCL School of Pharmacy, University College London, 29/39 Brunswick Square, London, WC1N 1AX, UK.
UCL School of Pharmacy, University College London, 29/39 Brunswick Square, London, WC1N 1AX, UK.
Eur J Med Chem. 2022 Oct 5;240:114571. doi: 10.1016/j.ejmech.2022.114571. Epub 2022 Jun 28.
Inhibition of β-lactamases is a promising strategy to overcome antimicrobial resistance to commonly used β-lactam antibiotics. Boronic acid derivatives have proven to be effective inhibitors of β-lactamases due to their direct interaction with the catalytic site of these enzymes. We synthesized a series of phenylboronic acid derivatives and evaluated their structure-activity relationships as Klebsiella pneumoniae carbapenemase (KPC-2) inhibitors. We identified potent KPC-2 inhibitors 2e & 6c (Ki = 0.032 μM and 0.038 μM, respectively) that enhance the activity of cefotaxime in KPC-2 expressing Escherichia coli. The measured acid dissociation constants (pKa) of selected triazole-containing phenylboronic acids was broad (5.98-10.0), suggesting that this is an additional property of the compounds that could be tuned to optimize the target interaction and/or the physicochemical properties of the compounds. These findings will help to guide the future development of boronic acid compounds as inhibitors of KPC-2 and other target proteins.
抑制β-内酰胺酶是克服常用β-内酰胺类抗生素抗药性的一种有前途的策略。硼酸衍生物因其与这些酶的催化位点的直接相互作用而被证明是β-内酰胺酶的有效抑制剂。我们合成了一系列苯硼酸衍生物,并评估了它们作为肺炎克雷伯菌碳青霉烯酶(KPC-2)抑制剂的结构-活性关系。我们确定了两种有效的 KPC-2 抑制剂 2e 和 6c(Ki 值分别为 0.032 μM 和 0.038 μM),它们可增强 KPC-2 表达的大肠埃希菌中头孢噻肟的活性。所选含三唑的苯硼酸的实测酸离解常数(pKa)较宽(5.98-10.0),表明这是化合物的另一个特性,可通过调整来优化目标相互作用和/或化合物的物理化学性质。这些发现将有助于指导硼酸化合物作为 KPC-2 和其他靶蛋白抑制剂的未来发展。