Identification and Optimization of Novel Inhibitors of the Polyketide Synthase 13 Thioesterase Domain with Antitubercular Activity

Simon R. Green, Caroline Wilson, Thomas C. Eadsforth, Avinash S. Punekar, Fabio K. Tamaki, Gavin Wood, Nicola Caldwell, Barbara Forte, Neil R. Norcross, Michael Kiczun, John M. Post, Eva Maria Lopez-Román, Curtis A. Engelhart, Iva Lukac, Fabio Zuccotto, Ola Epemolu, Helena I. M. Boshoff, Dirk Schnappinger, Chris Walpole, Ian H. Gilbert, Kevin D. Read, Paul G. Wyatt, and Beatriz Baragaña.

J. Med. Chem. 2023, XXXX, XXX, XXX-XXX
Publication Date:November 10, 2023
https://doi.org/10.1021/acs.jmedchem.3c01514

Abstract

There is an urgent need for new tuberculosis (TB) treatments, with novel modes of action, to reduce the incidence/mortality of TB and to combat resistance to current treatments. Through both chemical and genetic methodologies, polyketide synthase 13 (Pks13) has been validated as essential for mycobacterial survival and as an attractive target for Mycobacterium tuberculosis growth inhibitors. A benzofuran series of inhibitors that targeted the Pks13 thioesterase domain, failed to progress to preclinical development due to concerns over cardiotoxicity. Herein, we report the identification of a novel oxadiazole series of Pks13 inhibitors, derived from a high-throughput screening hit and structure-guided optimization. This new series binds in the Pks13 thioesterase domain, with a distinct binding mode compared to the benzofuran series. Through iterative rounds of design, assisted by structural information, lead compounds were identified with improved antitubercular potencies (MIC < 1 μM) and in vitro ADMET profiles.