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Lysine-Targeting Reversible Covalent Inhibitors with Long Residence Time

Rahi M. Reja, Wenjian Wang, Yuhan Lyu, Fredrik Hæffner, Jianmin Gao

2022Journal of the American Chemical Society100 citationsDOIOpen Access PDF

Abstract

We report a new reversible lysine conjugation that features a novel diazaborine product and much slowed dissociation kinetics in comparison to the previously known iminoboronate chemistry. Incorporating the diazaborine-forming warhead RMR1 to a peptide ligand gives potent and long-acting reversible covalent inhibitors of the staphylococcal sortase. The efficacy of sortase inhibition is demonstrated via biochemical and cell-based assays. A comparative study of RMR1 and an iminoboronate-forming warhead highlights the significance and potential of modulating bond dissociation kinetics in achieving long-acting reversible covalent inhibitors.

Topics & Concepts

ChemistryCovalent bondSortase ASortaseKineticsLysineDissociation (chemistry)CysteinePeptideStereochemistryCombinatorial chemistryBiochemistryBiophysicsAmino acidEnzymeOrganic chemistryBacterial proteinQuantum mechanicsBiologyPhysicsGeneBiochemical and Structural CharacterizationPeptidase Inhibition and AnalysisSignaling Pathways in Disease
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