Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.

A bioassay-guided investigation of Melicope ptelefolia Champ ex Benth (Rutaceae) resulted in the identification of an acyphloroglucinol, 2,4,6-trihydroxy-3-geranylacetophenone or tHGA, as the active principle inhibiting soybean 15-LOX. The anti-inflammatory action was also demonstrated on human leuk...

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Main Authors: Shaari, Khozirah, Suppaiah, Velan, Lam, Kok Wai, Stanslas, Johnson, Tejo, Bimo Ario, Israf Ali, Daud Ahmad, Abas, Faridah, Ismail, Intan Safinar, Shuaib, Nor Hasifi, Zareen, Seema, Lajis, Md. Nordin
Format: Article
Language:English
English
Published: Elsevier 2011
Online Access:http://psasir.upm.edu.my/id/eprint/25047/
http://psasir.upm.edu.my/id/eprint/25047/1/Bioassay-guided%20identification%20of%20an%20anti-inflammatory%20prenylated%20acylphloroglucinol%20from%20Melicope%20ptelefolia%20and%20molecular%20insights%20into%20its%20interaction%20with%205-lipoxygenase..pdf
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author Shaari, Khozirah
Suppaiah, Velan
Lam, Kok Wai
Stanslas, Johnson
Tejo, Bimo Ario
Israf Ali, Daud Ahmad
Abas, Faridah
Ismail, Intan Safinar
Shuaib, Nor Hasifi
Zareen, Seema
Lajis, Md. Nordin
author_facet Shaari, Khozirah
Suppaiah, Velan
Lam, Kok Wai
Stanslas, Johnson
Tejo, Bimo Ario
Israf Ali, Daud Ahmad
Abas, Faridah
Ismail, Intan Safinar
Shuaib, Nor Hasifi
Zareen, Seema
Lajis, Md. Nordin
author_sort Shaari, Khozirah
building UPM Institutional Repository
collection Online Access
description A bioassay-guided investigation of Melicope ptelefolia Champ ex Benth (Rutaceae) resulted in the identification of an acyphloroglucinol, 2,4,6-trihydroxy-3-geranylacetophenone or tHGA, as the active principle inhibiting soybean 15-LOX. The anti-inflammatory action was also demonstrated on human leukocytes, where the compound showed prominent inhibitory activity against human PBML 5-LOX, with an IC 50 value of 0.42 μM, very close to the effect produced by the commonly used standard, NDGA. The compound concentration-dependently inhibited 5-LOX product synthesis, specifically inhibiting cysteinyl leukotriene LTC4 with an IC 50 value of 1.80 μM, and showed no cell toxicity effects. The anti-inflammatory action does not seem to proceed via redox or metal chelating mechanism since the compound tested negative for these bioactivities. Further tests on cyclooxygenases indicated that the compound acts via a dual LOX/COX inhibitory mechanism, with greater selectivity for 5-LOX and COX-2 (IC 50 value of 0.40 μM). The molecular features that govern the 5-LOX inhibitory activity was thus explored using in silico docking experiments. The residues Ile 553 and Hie 252 were the most important residues in the interaction, each contributing significant energy values of 13.45 (electrostatic) and 5.40 kcal/mol (electrostatic and Van der Waals), respectively. The hydroxyl group of the phloroglucinol core of the compound forms a 2.56 Å hydrogen bond with the side chain of the carboxylate group of Ile 553. Both Ile 553 and Hie 252 are crucial amino acid residues which chelate with the metal ion in the active site. Distorting the geometry of these ligands could be the reason for the inhibition activity shown by tHGA. The molecular simulation studies supported the bioassay results and served as a good model for understanding the way tHGA binds in the active site of human 5-LOX enzyme.
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spelling upm-250472016-02-18T01:57:30Z http://psasir.upm.edu.my/id/eprint/25047/ Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase. Shaari, Khozirah Suppaiah, Velan Lam, Kok Wai Stanslas, Johnson Tejo, Bimo Ario Israf Ali, Daud Ahmad Abas, Faridah Ismail, Intan Safinar Shuaib, Nor Hasifi Zareen, Seema Lajis, Md. Nordin A bioassay-guided investigation of Melicope ptelefolia Champ ex Benth (Rutaceae) resulted in the identification of an acyphloroglucinol, 2,4,6-trihydroxy-3-geranylacetophenone or tHGA, as the active principle inhibiting soybean 15-LOX. The anti-inflammatory action was also demonstrated on human leukocytes, where the compound showed prominent inhibitory activity against human PBML 5-LOX, with an IC 50 value of 0.42 μM, very close to the effect produced by the commonly used standard, NDGA. The compound concentration-dependently inhibited 5-LOX product synthesis, specifically inhibiting cysteinyl leukotriene LTC4 with an IC 50 value of 1.80 μM, and showed no cell toxicity effects. The anti-inflammatory action does not seem to proceed via redox or metal chelating mechanism since the compound tested negative for these bioactivities. Further tests on cyclooxygenases indicated that the compound acts via a dual LOX/COX inhibitory mechanism, with greater selectivity for 5-LOX and COX-2 (IC 50 value of 0.40 μM). The molecular features that govern the 5-LOX inhibitory activity was thus explored using in silico docking experiments. The residues Ile 553 and Hie 252 were the most important residues in the interaction, each contributing significant energy values of 13.45 (electrostatic) and 5.40 kcal/mol (electrostatic and Van der Waals), respectively. The hydroxyl group of the phloroglucinol core of the compound forms a 2.56 Å hydrogen bond with the side chain of the carboxylate group of Ile 553. Both Ile 553 and Hie 252 are crucial amino acid residues which chelate with the metal ion in the active site. Distorting the geometry of these ligands could be the reason for the inhibition activity shown by tHGA. The molecular simulation studies supported the bioassay results and served as a good model for understanding the way tHGA binds in the active site of human 5-LOX enzyme. Elsevier 2011-11 Article PeerReviewed application/pdf en http://psasir.upm.edu.my/id/eprint/25047/1/Bioassay-guided%20identification%20of%20an%20anti-inflammatory%20prenylated%20acylphloroglucinol%20from%20Melicope%20ptelefolia%20and%20molecular%20insights%20into%20its%20interaction%20with%205-lipoxygenase..pdf Shaari, Khozirah and Suppaiah, Velan and Lam, Kok Wai and Stanslas, Johnson and Tejo, Bimo Ario and Israf Ali, Daud Ahmad and Abas, Faridah and Ismail, Intan Safinar and Shuaib, Nor Hasifi and Zareen, Seema and Lajis, Md. Nordin (2011) Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase. Bioorganic & Medicinal Chemistry, 19 (21). pp. 6340-6347. ISSN 0968-0896; ESSN:1464-3391 http://www.elsevier.com/ 10.1016/j.bmc.2011.09.001 English
spellingShingle Shaari, Khozirah
Suppaiah, Velan
Lam, Kok Wai
Stanslas, Johnson
Tejo, Bimo Ario
Israf Ali, Daud Ahmad
Abas, Faridah
Ismail, Intan Safinar
Shuaib, Nor Hasifi
Zareen, Seema
Lajis, Md. Nordin
Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title_full Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title_fullStr Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title_full_unstemmed Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title_short Bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from Melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
title_sort bioassay-guided identification of an anti-inflammatory prenylated acylphloroglucinol from melicope ptelefolia and molecular insights into its interaction with 5-lipoxygenase.
url http://psasir.upm.edu.my/id/eprint/25047/
http://psasir.upm.edu.my/id/eprint/25047/
http://psasir.upm.edu.my/id/eprint/25047/
http://psasir.upm.edu.my/id/eprint/25047/1/Bioassay-guided%20identification%20of%20an%20anti-inflammatory%20prenylated%20acylphloroglucinol%20from%20Melicope%20ptelefolia%20and%20molecular%20insights%20into%20its%20interaction%20with%205-lipoxygenase..pdf