Asymmetric synthesis of tetrahydroquinoline-type ecdysone agonists and QSAR for their binding affinity against Aedes albopictus ecdysone receptors.


Journal

Pest management science
ISSN: 1526-4998
Titre abrégé: Pest Manag Sci
Pays: England
ID NLM: 100898744

Informations de publication

Date de publication:
Jan 2019
Historique:
received: 11 06 2018
revised: 27 07 2018
accepted: 30 07 2018
pubmed: 3 8 2018
medline: 3 1 2019
entrez: 3 8 2018
Statut: ppublish

Résumé

Tetrahydroquinolines (THQs) are a class of non-steroidal ecdysone agonists that specifically bind to mosquito ecdysone receptors (EcR). The THQ scaffold contains two chiral centers at the C-2 and C-4 positions, resulting in four stereoisomers. We have previously shown that the (2R,4S)-isomers are the most biologically active; however, the lack of a practical synthetic method for these isomers has hampered further structure-activity studies. In this study, a chiral phosphoric acid-catalyzed Povarov reaction was employed to develop a facile asymmetric synthesis of THQs with a (2R,4S)-configuration, which allowed the preparation of a 40-compound library of enantiopure THQs. Evaluation of their binding affinity against Aedes albopictus EcR, followed by quantitative structure-activity relationship (QSAR) analyses, uncovered the physicochemical properties of THQs that are important for the ligand-receptor interaction. The most potent THQ derivative was twofold more active than the molting hormone, 20-hydroxyecdysone. The QSAR results provide valuable information for the rational design of novel mosquito-specific ecdysone agonists. © 2018 Society of Chemical Industry.

Sections du résumé

BACKGROUND BACKGROUND
Tetrahydroquinolines (THQs) are a class of non-steroidal ecdysone agonists that specifically bind to mosquito ecdysone receptors (EcR). The THQ scaffold contains two chiral centers at the C-2 and C-4 positions, resulting in four stereoisomers. We have previously shown that the (2R,4S)-isomers are the most biologically active; however, the lack of a practical synthetic method for these isomers has hampered further structure-activity studies.
RESULTS RESULTS
In this study, a chiral phosphoric acid-catalyzed Povarov reaction was employed to develop a facile asymmetric synthesis of THQs with a (2R,4S)-configuration, which allowed the preparation of a 40-compound library of enantiopure THQs. Evaluation of their binding affinity against Aedes albopictus EcR, followed by quantitative structure-activity relationship (QSAR) analyses, uncovered the physicochemical properties of THQs that are important for the ligand-receptor interaction. The most potent THQ derivative was twofold more active than the molting hormone, 20-hydroxyecdysone.
CONCLUSION CONCLUSIONS
The QSAR results provide valuable information for the rational design of novel mosquito-specific ecdysone agonists. © 2018 Society of Chemical Industry.

Identifiants

pubmed: 30070016
doi: 10.1002/ps.5160
doi:

Substances chimiques

Insect Proteins 0
Quinolines 0
Receptors, Steroid 0
ecdysone receptor 0
Ecdysone 3604-87-3

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

115-124

Subventions

Organisme : JSPS KAKENHI
ID : JP17J01486
Organisme : JSPS KAKENHI
ID : JP16K07625

Informations de copyright

© 2018 Society of Chemical Industry.

Auteurs

Taiyo Yokoi (T)

Division of Applied Life Sciences, Graduate School of Agriculture, Kyoto University, Kyoto, Japan.

Yoshiaki Nakagawa (Y)

Division of Applied Life Sciences, Graduate School of Agriculture, Kyoto University, Kyoto, Japan.

Hisashi Miyagawa (H)

Division of Applied Life Sciences, Graduate School of Agriculture, Kyoto University, Kyoto, Japan.

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Classifications MeSH