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Active Core in a Triazole Peptide Dual Site Antagonist of HIV-1 gp120
Journal article   Open access   Peer reviewed

Active Core in a Triazole Peptide Dual Site Antagonist of HIV-1 gp120

Muddegowda Umashankara, Karyn McFadden, Isaac Zentner, Arne Schön, Srivats Rajagopal, Ferit Tuzer, Syna A Kuriakose, Mark Contarino, Judith LaLonde, Ernesto Freire, …
ChemMedChem, v 5(11), pp 1871-1879
08 Nov 2010
PMID: 20677318
url
https://doi.org/10.1002/cmdc.201000222View
Published, Version of Record (VoR) Open

Abstract

HIV-1 click chemistry surface plasmon resonance entry inhibitors peptide triazole
In an effort to identify broadly active inhibitors of HIV-1 entry into host cells, we had previously reported a family of dodecamer triazole-peptide conjugates with nanomolar affinity for viral surface protein gp120. This class of peptides exhibits potent antiviral activity and the capacity to simultaneously inhibit interaction of viral envelope protein with both CD4 and co-receptor. In the current investigation, we used minimization of structural complexity of the lead triazole inhibitor HNG-156 (peptide 1 ) in order to explore the limits of the pharmacophore that enables dual antagonism and to improve opportunities for peptidomimetic design. Truncations of both carboxyl- and amino-terminal residues of the initial 12 amino acid residues of peptide 1 were found to have minimal effect on both affinity and antiviral activity. In contrast, the central triazole Pro-Trp cluster at residues 6 and 7 with ferrocenyl-triazole-Pro (Ftp) was found to be critical for bioactivity. Amino terminal residues distal to the central triazole Pro-Trp sequence tolerated decreasing degrees of side chain variation upon approaching the central cluster. A peptide fragment containing residues 3-7 (Asn-Asn-Ile-Ftp-Trp) exhibited substantial direct binding affinity, antiviral potency, dual receptor site antagonism and induction of gp120 structuring, all properties defining the functional signature of the parent compound 1 . This active core contains a stereochemically specific hydrophobic triazole-Pro-Trp cluster, with a short N-terminal peptide extension providing groups for potential main chain and side chain hydrogen binding. The results of this work argue that the pharmacophore for dual antagonism is structurally limited, enhancing the potential to develop minimized peptidomimetic HIV-1 entry inhibitors that simultaneously suppress binding of envelope protein to both of its host cell receptors. The results also argue that the target epitope on gp120 is relatively small, pointing to a localized allosteric inhibition site in the HIV-1 envelope that could be targeted for small-molecule inhibitor discovery.

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Collaboration types
Domestic collaboration
Web of Science research areas
Chemistry, Medicinal
Pharmacology & Pharmacy
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