4.
Eudy, J.D. Yao, S.; Weston, M. D.; Ma-Edmonds, M.; Talmadge,
C. B.; Cheng, J. J.; Kimberling, W. J.; Sumegi, J. Genomics 1998,
50, 382.
and β-sheet regions indicating ancillary hydrogen bond interactions
that likely contributes to its increased binding potency.
5.
6.
Jagannath M.; Kim, D. -K.; Choi, H.-S., Trends Endocrin. Met.
2017, 28, 261.
Narkar, V. A.; Fan, W.; Downes, M.; Yu, R. t.; Jonker, J. W.;
Alaynick, W. A.; Banayo, E.; Karunasiri, M. S.; Lorca, S.; Evans,
R. M. Cell Metab. 2011, 13, 283.
Figure 3. HDX analysis of selected ERR agonists
7.
8.
9.
Yang, X.; Downes, M.; Yu, R. T.; Bookout, A. L.; He, W.;
Straume, M.; Mangelsdorf, D. J.; Evans, R. M. Cell 2006, 126,
801.
Tremblay, G. B.; Kunath, T.; Bergeron, D.; Lapointe, L.;
Champigny, C.; Bader, J-A.; Rossant, J.; Giguère, V. Genes. Dev.
2001, 15, 833.
Coward, P.; Lee, D.; Hull, M. V.; Lehmann, J. M. PNAS. 2001,
98, 8880.
10. Tremblay, G. B.; Bergeron, D.; Giguere, V. Endocrinology 2001,
142, 4572.
SR-19797
SR-19881
11. Chao, E. Y. H.; Collins, J. L.; Gaillard, S.; Miller, A. B.; Wang, L.
P.; Orband-Miller, L. A.; Nolte, R. T.; McDonnell, D. P.;
Willson, T. M.; Zuercher, W. J. Bioorg. Med. Chem. Lett. 2006,
16, 821.
Selected compounds were tested for stability in human, rat and
mouse liver microsomes (Table 8). All analogs inlcuding GSK4716
had short half-lives. Nonetheless, we have successfully replaced the
acylhydrazone linkage with a saturated amide and maintained
potency and comparable metabolic stability to the lead GSK4716.
The phenethyl linkage is likely a metabolic soft spot in the saturated
analogs. We will continue to explore substitutions here to improve
stability. While not necessarily important to microsomal stability, the
phenol group will likely be subject to phase 2 metabolism. Future
SAR efforts will continue to search for suitable replacements for the
phenol group to reduce this liability.
12. Kim, J.; Chin, J.; Im, C. Y.; Yoo, E. K.; Woo, S.; Hwang, H. J.;
Cho, J-H.; Seo, K.; Song, J.; Hwang, H.; Kim, K-H.; Kim, N. D.;
Yoon, S. K.; Jeon, J-H.; Yoon, S-Y.; Jeon, Y. H.; Choi, H-S.; Lee,
I-K.; Kim, S. H.; Cho, S. J. Eur. J. Med. Chem. 2016, 120, 338.
13. Busch, B. B.; Stevens, W. C. Jr.; Martin, R.; Zhou, S.; Sapp, D.
W.; Horlick, R. A.; Mohan, R. J. Med. Chem. 2004, 47, 5593.
14. Zuercher, W. J.; Gaillard, S.; Orband-Miller, L. A.; Chao, E. Y.
H.; Shearer, B. G.; Jones, D. G.; Miller, A. B.; Collins, J. L.;
McDonnell, D. P.; Willson, T. M. J. Med. Chem. 2005, 48, 3107.
15. Bhat, V. T.; Caniard, A. M.; Luksch, T.; Brenk, R.; Campopiano,
D. J.; Greaney, M. F. nat. chem. 2010, 2, 490.
16. Ji, K.; Lee, C.; Janesko, B. G.; Simanek, E. E. Mol. Pharmaceutics
2015, 12, 2924.
17. Wang, L.; Zuercher, W. J.; Consler, T. G.; Lambert, M. H.; Miller,
A. B.; Orband-Miller, L. A.; McKee, D. D.; Willson, T. M.; Nolte,
R. T. J. Bio. Chem. 2006, 281, 37773.
Table 8: Metabolic stability
Half life in 1 mg/ml heptatic microsomes
Species (T1/2 in minutes)
Compound ID
GSK4716
SR20041
SR20012
SR20011
SR19881
SR19797
Human
6.4
3.0
2.9
3.6
Mouse
2.3
1.6
1.2
1.5
Rat
2.2
1.5
1.1
1.5
3.9
1.6
3.1
6.8
2.2
3.3
In summary, we have identified a series of amides as ERRγ
agonists with suitable potency for further development. Our
SAR studies of this chemotype identified SR19881 as the most
potent full agonist of ERRγ with an EC50=0.39 μM in a binding
assay and an EC50=4.7
also equipotent on ERR
equipotent dual agonist of ERR/
M in a cell-based assay. SR19881 was
with an EC50=0.63 μM making it an
. HDX studies help explain
how subtle changes to the molecule translate into improved
potency by increased stabilization of the receptor. These studies
provided valuable information and an opportunity to expand the
series in search of more potent, selective, and druglike
molecules. Further investigations of new chemotypes and
pharmacokinetic properties continue in an effort to explore the
role of ERRγ in vitro and in vivo. These results will be reported
in due course.
Acknowledgments
This work was supported by the Eunice Kennedy Shriver National
Institute of Child Health & Human Development (HD087046 to
P.R.G and T.M.K.).
References and notes
1.
2.
3.
Giguère, V. Endocr. Rev. 2008, 29, 677.
Audet-Walsh, E; Giguère, V. Acta. Pharmacol. Sin. 2015, 36, 51.
Huss, J. M.; Garbacz, W. G.; Xie, W. Biochim. Biophys. Acta.
2015, 1852, 1912.