´
A. S. Hernandez et al. / Bioorg. Med. Chem. Lett. 17 (2007) 5928–5933
5932
Table 3. In vitro and in vivo activity in the acute anesthetized IV rat
model of 1H-tetrazoles
2. DeVita, R. J.; Schoen, W. R.; Fischer, M. H.; Fontier, A.
J.; Pisano, J. M.; Wyvratt, M. J.; Cheng, K.; Chan, W.-S.;
Butler, B. S.; Hickey, G. J.; Jacks, T. M.; Smith, R. G.
Bioorg. Med. Chem. Lett. 1994, 4, 2229.
Compounds Structure
EC50 ED50
(nM)a (lmol/kg)b
CLogP
3. Patchett, A. A.; Nargund, R. P.; Tata, J. R.; Chen, M.-H.;
Barakat, K. J.; Johnston, D. B. R.; Cheng, K.; Chan, W.
W.-S.; Butler, B.; Hickey, G.; Jacks, T.; Schleim, K.; Pong,
S.-S.; Chaung, L.-Y. P.; Chen, H. Y.; Frazier, E.; Leung,
K. H.; Chiu, S.-H. L.; Smith, R. G. Proc. Natl. Acad. Sci.
U.S.A. 1995, 92, 7001.
4. Ghrelin is a 28-amino acid peptide that displays a unique
octanoyl-serine residue and is secreted in the stomach.
5. Kojima, M.; Hosoda, H.; Date, Y. Nature 1999, 402,
656.
NH2
O
NH
BnO
9j
4
>17.4
1.8
O O
S
N
N
N
N
N
NH2
O
6. (a) Svensson, J. Exp. Opin. Ther. Patents 2000, 10, 1071;
(b) Carpino, P. A. Exp. Opin. Ther. Patents 2002, 12, 1599.
7. Dodge, J. A.; Heiman, M. L. Annu. Rep. Med. Chem.
2003, 38, 81.
NH
N
BnO
9h
12
26.4
2.5
N
N
N
8. (a) Thornber, C. W. Chem. Soc. Revs. 1979, 8, 563; (b)
Singh, H.; Chawla, A. S.; Kapoor, V. K.; Paul, D.;
Malhotra, R. K. Prog. Med. Chem. 1980, 17, 151.
9. De Lombaert, S.; Blanchard, L.; Tan, J.; Sakane, Y.;
Berry, C. Bioorg. Med. Chem. Lett. 1995, 5, 145.
10. Duncia, J. V.; Pierce, M. E.; Santella, J. B., III J. Org.
Chem. 1991, 56, 2395.
NH2
O
NH
N
9q
30
8.5
À0.3
BnO
N
N
11. Isomer separation was usually achieved at this step by
column chromatography on silica gel. For a few analogs,
1H/2H isomeric mixtures were more easily separated by
CN
N
a See Ref. 12 for detailed description.
b See Ref. 17 for detailed description.
1
preparative HPLC. HNMR easily distinguished between
the 1H and 2H isomers by comparison of the Dd between
the methyls of the 2-aminoisobutyric fragment. The Dd is
significantly larger in the 1H isomer than in the 2H isomer.
12. H4 glioma cells in which expression of the endogenous
human GHS receptor was enhanced by RAGE-activation
were utilized for both the functional and binding assays.
For details about random Activation for GENE EXPRE-
SION (RAGE)TM technology (Athersys, Inc.), see: Harr-
inton, J. J.; Sherf, B.; Rundlett, S.; Jackson, P. D.; Perry,
R.; Cain, S.; Leventhal, C.; Thorton, M.; Ramachandran,
R.; Whittington, J.; Lerner, L.; Costanzo, D.; McElligott,
K.; Boozer, S.; Mays, R.; Smith, E.; Veloso, N.; Klika, A.;
Hess, J.; Cothren, K.; Lo, K.; Offenbacher, J.; Danzig, J.;
Ducar, M. Nat. Biotechnol. 2001, 19, 440, The EC50 was
measured by determining intracellular calcium concentra-
tion in a FLIPR assay with Ghrelin as having 100%
intrinsic functional activity. All EC50 values are averages
of at least three measurements.
13. Binding affinities were determined by 12-point dose–
response curve analysis using membranes from RAGE-
based GHSR1a expressing cells. Typically, 0.5 ug mem-
brane was incubated in the presence of 0.02 nM [125I]
Ghrelin in 25 mM Hepes (pH 7.2) with 10 mM MgCl2,
2 mM EGTA, and 0.1% BSA in a total volume of 0.2 ml
for 1 h in the presence of increasing concentrations of test
compound. Reactions were terminated by rapid vacuum
filtration over GFB filterplates coated with 0.1% poly-
ethylenimine, and plates were then washed with 0.8 ml of
binding buffer and radioactivity subsequently measured by
scintillation spectroscopy on a TopCount (Perkin-Elmer)
scintillation counter. Curves were fit by nonlinear regres-
sion analysis using a four parameter logistic equation, and
Ki values were determined using the Cheng-Prusoff equa-
tion. Compounds were routinely tested on three separate
occasions.
other two more liphophilic classes of tetrazoles. This re-
sult may be attributed to a potentially better ADME
profile of the polar smaller agonist 9q. The oral bioavail-
ability of 9q was 56% and 76% in rats and dogs, respec-
tively. When administered orally to beagle dogs at a
10 mg/kg dose, 9q increased GH mean peak levels to
30 ng/mL compared to 0 ng/mL for vehicle control.
Although maximum GH levels occurred between 40
and 45 min post-dose, elevated plasma concentrations
of GH persisted for up to 120 min after dosing.
In summary, several novel series of GHS-receptor ago-
nists based on a novel tetrazole template have been de-
scribed. Reliable solution and solid phase protocols
have been developed for the synthesis of the three re-
lated sets of analogs 9, 10, and 19. The SAR of the linker
and H-bond acceptor were explored. The lead analog 9q
exhibited good oral bioavailability in rats and dogs;
moreover, it was orally efficacious in dogs at the
10 mg/kg dose. Further efforts to improve the in vitro
and in vivo potency of this 1H-tetrazole chemotype will
be reported elsewhere.
Acknowledgments
We thank Dr. William Washburn, Dr. Scott Priestley,
and Dr. Robert Zahler for their suggestions on the
manuscript.
14. Full experimental details will be disclosed in a manuscript
which is in preparation.
References and notes
´
15. (a) Hernandez, A. S.; Hodges, J. C. J. Org. Chem. 1997,
62, 3153; (b) Wilson, M. W.; Hernandez, A. S.; Calvet, A.
´
1. Bowers, C. Y.; Momany, F. A.; Reynolds, G. A.; Hong,
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P.; Hodges, J. C. Mol. Diversity 1998, 3, 95.