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J Med Chem . Structure-Based Optimization of Pyridone α-Ketoamides as Inhibitors of the SARS-CoV-2 Main Protease

tetano

Editor, Senior Moderator
J Med Chem


. 2025 Jan 16.
doi: 10.1021/acs.jmedchem.4c02172. Online ahead of print. Structure-Based Optimization of Pyridone α-Ketoamides as Inhibitors of the SARS-CoV-2 Main Protease

Ravi Kumar Akula[SUP] 1 2 [/SUP], Haifa El Kilani[SUP] 2 [/SUP], Alina Metzen[SUP] 1 3 [/SUP], Judith Röske[SUP] 2 [/SUP], Kaixuan Zhang[SUP] 2 [/SUP], Matthias Göhl[SUP] 1 [/SUP], Nanaji Arisetti[SUP] 1 [/SUP], Graham P Marsh[SUP] 4 [/SUP], Hannah J Maple[SUP] 4 [/SUP], Mark S Cooper[SUP] 4 [/SUP], Burhan Karadogan[SUP] 4 [/SUP], Dirk Jochmans[SUP] 5 [/SUP], Johan Neyts[SUP] 5 [/SUP], Katharina Rox[SUP] 1 3 [/SUP], Rolf Hilgenfeld[SUP] 2 6 [/SUP], Mark Brönstrup[SUP] 1 3 7 [/SUP]



Affiliations
Abstract

The main protease M[SUP]pro[/SUP] is a clinically validated target to treat infections by the coronavirus SARS-CoV-2. Among the first reported M[SUP]pro[/SUP] inhibitors was the peptidomimetic α-ketoamide 13b, whose cocrystal structure with M[SUP]pro[/SUP] paved the way for multiple lead-finding studies. We established structure-activity relationships for the 13b series by modifying residues at the P1', P3, and P4 sites. Guided by cocrystal structures, we reduced the P1' substituent size to better fill the pocket and added a fluorine substituent to the pyridone ring, enabling a new hydrogen bond with Gln189 in P3. Among 22 novel analogues, 6d and 12d inhibited M[SUP]pro[/SUP] with IC[SUB]50[/SUB]s of 110 nM and 40 nM, improving the potency of 13b by up to 9.5-fold. Compound 6d had pronounced antiviral activity with an EC[SUB]50[/SUB] of 1.6 μM and was stable in plasma and microsomes. The study illustrates the potential of structure-based design to systematically improve peptidomimetic α-ketoamides.


 
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