Glycosylated neurotensin analogues exhibit sub-picomolar anticonvulsant potency in a pharmacoresistant model of epilepsy - PubMed (original) (raw)
Glycosylated neurotensin analogues exhibit sub-picomolar anticonvulsant potency in a pharmacoresistant model of epilepsy
Hee-Kyoung Lee et al. ChemMedChem. 2009 Mar.
Abstract
Neurotensin (NT) is an endogenous neuropeptide involved in a variety of central and peripheral neuromodulatory effects. Herein we show the effects of site-specific glycosylation on the in vitro and in vivo pharmacological properties of this neuropeptide. NT analogues containing O-linked disaccharides (beta-melibiose and alpha-TF antigen) or beta-lactose units linked by a PEG(3) spacer were designed and chemically synthesized using Fmoc chemistry. For the latter analogue, Fmoc-Glu-(beta-Lac-PEG(3)-amide) was prepared. Our results indicate that the addition of the disaccharides does not negatively affect the sub-nanomolar affinity or the low-nanomolar agonist potency for the neurotensin receptor subtype 1 (NTS1). Interestingly, three glycosylated analogues exhibited sub-picomolar potency in the 6 Hz limbic seizure mouse model of pharmacoresistant epilepsy following intracerebroventricular administration. Our results suggest for the first time that chemically modified NT analogues may lead to novel antiepileptic therapies.
Figures
Figure 1. The structure of glycoamino acids introduced to NT and the C-terminal hexapeptide, NT(8–13)
Figure 2. Synthesis of Fmoc-Glu-(β-Lac-PEG3-amide), 4, the intermediate compound for the preparation of NT(8–13)-PEG3-Lac
a) Pentafluorophenol (PFP), DCC, CH2Cl2, rt, 72%; b) DIPEA, CH2Cl2, 57%; c) H2, 10% Pd/C, EtOAc, 70%.
Figure 3. HPLC profile of NT-TF before deacetylation (A) and after deacetylation (B)
The retention time changed from 19.5 min to 16.3 min during deacetylation reaction. The analogs were purified by RP-HPLC using a semi-preparative C18 column in a linear gradient (5–65%) of Buffer B (90% acetonitrile, 0.1% TFA). The molecular weight of the analogs was confirmed by MALDI-TOF mass spectrometry.
Figure 4. Receptor binding curve for NT analogs (top) and the agonist activity from functional assay (bottom)
The binding affinity of NT and NT-TF for NTS1 remains same, 0.5 nM. EC50 values in intracellular calcium mobilization assay for NT and NT-TF are 1.1 nM and 0.9 nM, respectively.
Figure 5. Dose response curves of NT and a representative glycosylated NT analog, NT-TF, in the 6 Hz (32 mA) anticonvulsant assay in mice following the icv administration
The log values of dose were plotted against the percentage of mice protected from seizures. The ED50 values for NT and NT-TF were 1.0 pmol and 0.4 pmol, respectively.
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