Warecki Brenda A, Tomatis Pablo E, Mojica María F, Bethel Christopher R, Rodríguez Saravia Magdalena, Drusin Salvador I, Ono Daisuke, Bahr Guillermo, Papp-Wallace Krisztina, Tamma Pranita D, Moreno Diego M, Mahler Graciela, Bonomo Robert A, Vila Alejandro J
Instituto de Biología Molecular y Celular de Rosario (IBR), CONICET, Universidad Nacional de Rosario Rosario Argentina
Facultad de Ciencias Bioquímicas y Farmacéuticas, Universidad Nacional de Rosario Rosario Argentina.
Chem Sci. 2025 Jun 3. doi: 10.1039/d5sc02122g.
The global spread of antimicrobial resistance (AMR) underscores the critical need for the rapid development of new drugs. Particularly alarming is the surge in metallo-β-lactamases (MBLs) - broad spectrum enzymes able to inactivate penicillins, cephalosporins, and carbapenems. Cefiderocol (FDC), a siderophore-containing cephalosporin, was initially reported as resistant to MBL hydrolysis. Indeed, FDC has been designated as the preferred treatment for Gram-negative pathogens producing MBLs - with the most common MBLs of clinical concern belonging to the NDM, VIM, or IMP families. Regrettably, increasing reports of FDC resistance are emerging. Many of these events are linked to overexpression of NDM, sometimes coupled to alterations in iron transporters, challenging the notion of FDC being invulnerable to MBL hydrolysis. Herein, we demonstrate that NDM-1 and -5 are able to inactivate FDC efficiently, while VIM-2 and IMP-1 show impaired catalytic efficiency against this substrate. All these MBL enzymes form a reversible enzyme-product adduct with FDC, whose lifetime varies considerably among MBLs. In IMP-1 and VIM-2, this results in efficient enzyme inhibition. In contrast, NDM variants are poorly inhibited, eliciting efficient turnover rates. We propose a mechanistic explanation for FDC action that aligns with clinical findings suggesting NDMs contributing to FDC resistance. Based on these conclusions, we suggest caution when using this potent cephalosporin against NDM-producers. FDC paired with an NDM-inhibitor may be a strategy to preserve this important antibiotic.
抗菌药物耐药性(AMR)在全球范围内的传播凸显了快速开发新药的迫切需求。尤其令人担忧的是金属β-内酰胺酶(MBL)的激增,这是一类能够使青霉素、头孢菌素和碳青霉烯类药物失活的广谱酶。头孢地尔(FDC)是一种含铁载体的头孢菌素,最初报道其对MBL水解具有抗性。事实上,FDC已被指定为治疗产生MBL的革兰氏阴性病原体的首选药物,临床上最常见的引起关注的MBL属于NDM、VIM或IMP家族。遗憾的是,越来越多关于FDC耐药性的报道不断出现。其中许多事件与NDM的过度表达有关,有时还伴有铁转运蛋白的改变,这对FDC不易被MBL水解的观点提出了挑战。在此,我们证明NDM-1和-5能够有效使FDC失活,而VIM-2和IMP-1对该底物的催化效率受损。所有这些MBL酶都与FDC形成可逆的酶-产物加合物,其寿命在不同的MBL之间有很大差异。在IMP-1和VIM-2中,这导致有效的酶抑制。相比之下,NDM变体的抑制作用较弱,周转率较高。我们提出了一种与临床研究结果相符的FDC作用机制解释,提示NDMs与FDC耐药性有关。基于这些结论,我们建议在使用这种强效头孢菌素治疗产生NDM的病原体时要谨慎。FDC与NDM抑制剂联合使用可能是保留这种重要抗生素的一种策略。