Identification and Validation of PKG as the Primary Target of MMV030084
(A) MMV030084-exposure of schizonts affected the phosphorylation status of several peptides in various pathways and provided evidence indicating that MMV030084 likely targets a kinase that is central to Pf parasite metabolism.
(B) PKG, CDPK1, and AAT emerged as candidate targets in competitive chemoproteomic studies using bead-bound compounds on treated and untreated (control) parasite lysates (Table S1 (E1-3)).
(C) Exposing MMV030084-treated parasite lysates to a panel of bead-immobilized kinase inhibitors (Kinobeads) or bead-immobilized MMV030084 (‘084-beads) identified the lowest Kdapp values for PKG, CDPK1, and AAT. Results shown are the mean of two repeated experiments, except for AAT, which was detected in only one of the experiments (Table S1 (E1-3)).
(D) cKD of PKG resulted in the largest growth defect compared with control conditions, with cKDs of CDPK1 and AAT affecting parasite growth to a lesser extent. Error bars indicate the SEM based on two independently repeated experiments with technical duplicates. p values are based on unpaired t tests (Table S1 (F)).
(E) cKD of PKG increased parasite susceptibility to MMV030084, while cKD of CDPK1 or AAT caused no or minor differences in MMV030084 susceptibility versus control conditions. Results shown are based on four independently repeated experiments with technical duplicates (Table S1 (G)).
(F) MMV030084 and its analogs dock well into the crystal structure of PKG (Table S1 (H)). H-bonding residues are highlighted in the docking graphs.
(G) MMV030084 potently inhibited the kinase activity of recombinant PfPKG in vitro. IC50 data are based on three independently repeated experiments with technical duplicates. MMV’084, MMV030084; TCMDC‘154, TCMDC-141154; ctrl, control; PKG, cGMP-dependent protein kinase (PF3D7_1436600); CDPK1, calcium-dependent protein kinase 1 (PF3D7_0217500); AAT, putative amino acid transporter (PF3D7_1231400); Kdapp, apparent dissociation constant; cKD, conditional knockdown; SEM, standard error of the mean. ∗p < 0.05, ∗∗p < 0.01, ∗∗∗p < 0.001, ∗∗∗∗p < 0.0001.