ABP validation. (A) In-gel
fluorescence showing active rhKLK6 labeled
by fABP 21 after 1 h incubation. A KLK6 western blot
of the gel shows total KLK6. WT = wild-type, S195A = mutated inactive
KLK6. (B) KLK6 blot of a pulldown experiment with bABP 17 (IMP-2352) on conditioned media from a panel of PDAC cell lines.
Pulldown lanes show enriched proteins after streptavidin binding.
Before pulldown shows total KLK6 in each cell line. (C) KLK6 blot
of a pulldown experiment with bABP 17 (IMP-2352) at different
concentrations on Capan-2 conditioned media. The inactive control 18 shows no labeling. 2 h preincubation with FP-alkyne reduces
the labeling of bABP 17 (IMP-2352). (D) NeutrAvidin-HRP
blot of Capan-2 media after incubation of compounds 17 (IMP-2352) and 18 for 1 h. (E) NeutrAvidin-HRP blot
of Capan-2 media after incubation of the KLK6-selective alkyne probe
(YnABP) 19 for 2 h, followed by bABP 17 (IMP-2352)
for 1 h. This competition experiment shows that YnABP 19 selectively inhibits KLK6 over tPA and uPA. (F) KLK6 ABP selectivity
and on-target validation using LC–MS/MS. Capan-2 conditioned
media was treated with bABP 17 (IMP-2352) or DMSO for
1 h, followed by a chemical proteomics workflow to enrich for labeled
proteins. The volcano plot compares the changes of protein quantification
between DMSO and ABP-treated media, showing the targets of bABP 17 (IMP-2352). (G) Recombinant tPA, uPA, or KLK6 were treated
with bABP 17 (IMP-2352) for 2 h, followed by fABP 21 for 1 h. In-gel fluorescence shows selective inhibition
of KLK6 over tPA and uPA by bABP 17.