Characterization of L,D-transpeptidase YnhG in Carbapenem Resistant Enterobacteriaceae

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2022-05

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The Ohio State University

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Abstract

This project is focused on analyzing and characterizing an enzyme hypothesized to contribute to the antibiotic resistance of the pathogen Klebsiella pneumoniae. The enzymes of interest are L,D-transpeptidases (Ldts). These proteins perform a similar task to D,Dtranspeptidases (Penicillin-Binding Proteins (PBPs)) but are sufficiently different both structurally and in molecule-specific function that they are not recognized by standard β-lactam antibiotics. Both Ldts and PBPs operate in the cell wall of bacteria. They work to catalyze the cross-links between peptide stems in peptidoglycan, a network of amino acids and carbohydrates that comprises the cell wall. Where they differ is in the specifics of the cross-link itself. PBPs recognize a donor stem of five amino acids ending in two consecutive D-alanine's, whereas Ldts recognize a donor stem of four amino acids ending in only one D-alanine. Generally, PBPs are the main driving force of cell wall synthesis. However, it is hypothesized that, when under pressure from βlactam antibiotics, Ldts can take over and continue the cell wall synthesis process without hindrance from the antibiotic. This project aimed to characterize a selected Ldt, YnhG, found in Klebsiella pneumoniae in both its structure and function. 3D modelling via crystallography of both apo- and holoenzyme will be utilized to study the structure of the full enzyme as well as the nature of its active-site interactions. Kinetics assays were utilized to study the activity of YnhG. Activity assays were performed using a chromogenic substrate nitrocefin in both solo and competition assays. Assays using just YnhG and nitrocefin gave light to the baseline activity of the enzyme, whereas competition assays between nitrocefin and various other select β-lactam antibiotics gave light to the efficacy of said β-lactams against the enzyme. Both the crystallography and kinetics assays provided critical information regarding the nature of YnhG and set the stage for novel drug development in future research.

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Antibiotic resistance, β-lactam, protein, column chromatography, X-ray crystallography, nitrocefin

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