PUBLICATION

(+)/(-)-Gerbeloid A, a pair of unprecedented coumarin-based polycyclic meroterpenoid enantiomers from Gerbera piloselloides: Structural elucidation, semi-synthesis, and lipid-lowering activity

Authors
Zhao, C., Li, J., Hu, Y., Li, L., Yu, M., Huang, Y., Zhang, T., Shang, H., Zou, Z.
ID
ZDB-PUB-240603-9
Date
2024
Source
Acta pharmaceutica Sinica. B   14: 265726682657-2668 (Journal)
Registered Authors
Keywords
3T3-L1 adipocytes, Biomimetic synthesis, Coumarin meroterpenoid, Gerbera piloselloides, High-fat diet zebrafish model, Lipid-lowering activity, Natural products, Structural elucidation
MeSH Terms
none
PubMed
38828137 Full text @ Acta Pharm Sin B
Abstract
A pair of coumarin-based polycyclic meroterpenoid enantiomers (+)/(-)-gerbeloid A [(+)-1a and (-)-1b] were isolated from the medicinal plant Gerbera piloselloides, which have a unique caged oxatricyclo [4.2.2.03,8] decene scaffold. Their planar and three-dimensional structures were exhaustively characterized by comprehensive spectroscopic data and X-ray diffraction analysis. Guided by the hypothetical biosynthetic pathway, the biomimetic synthesis of racemic 1 was achieved using 4-hydroxy-5-methylcoumarin and citral as the starting material via oxa-6π electrocyclization and intramolecular [2 + 2] photocycloaddition. Subsequently, the results of the biological activity assay demonstrated that both (+)-1a and (-)-1b exhibited potent lipid-lowering effects in 3T3-L1 adipocytes and the high-fat diet zebrafish model. Notably, the lipid-lowering activity of (+)-1a is better than that of (-)-1b at the same concentration, and molecular mechanism study has shown that (+)-1a and (-)-1b impairs adipocyte differentiation and stimulate lipolysis by regulating C/EBPα/PPARγ signaling and Perilipin signaling in vitro and in vivo. Our findings provide a promising drug model molecule for the treatment of obesity.
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