Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases

Class IIa histone deacetylases (HDACs) have been linked to tumorigenesis in various cancers. Previously, we designed phenylhydroxamic acid LH4f as a potent class IIa HDAC inhibitor. However, it also unselectively inhibited class I and class IIb HDACs. To enhance the compound’s selectivity towards cl...

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Main Authors: Kai-Cheng Hsu, Yun-Yi Huang, Jung-Chun Chu, Yu-Wen Huang, Jing-Lan Hu, Tony Eight Lin, Shih-Chung Yen, Jing-Ru Weng, Wei-Jan Huang
Format: Article
Language:English
Published: Taylor & Francis Group 2024-12-01
Series:Journal of Enzyme Inhibition and Medicinal Chemistry
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Online Access:https://www.tandfonline.com/doi/10.1080/14756366.2024.2406025
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author Kai-Cheng Hsu
Yun-Yi Huang
Jung-Chun Chu
Yu-Wen Huang
Jing-Lan Hu
Tony Eight Lin
Shih-Chung Yen
Jing-Ru Weng
Wei-Jan Huang
author_facet Kai-Cheng Hsu
Yun-Yi Huang
Jung-Chun Chu
Yu-Wen Huang
Jing-Lan Hu
Tony Eight Lin
Shih-Chung Yen
Jing-Ru Weng
Wei-Jan Huang
author_sort Kai-Cheng Hsu
collection DOAJ
description Class IIa histone deacetylases (HDACs) have been linked to tumorigenesis in various cancers. Previously, we designed phenylhydroxamic acid LH4f as a potent class IIa HDAC inhibitor. However, it also unselectively inhibited class I and class IIb HDACs. To enhance the compound’s selectivity towards class IIa HDACs, the ortho-phenyl group from the selective HDAC7 inhibitor 1 is incorporated into ortho position of the phenylhydroxamic acid in LH4f. Compared to LH4f, most resulting compounds displayed substantially improved selectivity towards the class IIa HDACs. Notably, compound 7 g exhibited the strongest HDAC9 inhibition with an IC50 value of 40 nM. Molecular modelling further identified the key interactions of compound 7 g bound to HDAC9. Compound 7 g significantly inhibited several human cancer cells, induced apoptosis, modulated caspase-related proteins as well as p38, and caused DNA damage. These findings suggest the potential of class IIa HDAC inhibitors as lead compounds for the development of cancer therapeutics.
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institution OA Journals
issn 1475-6366
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language English
publishDate 2024-12-01
publisher Taylor & Francis Group
record_format Article
series Journal of Enzyme Inhibition and Medicinal Chemistry
spelling doaj-art-2d0d3d594369440e9a61c2c583b064c22025-08-20T02:35:33ZengTaylor & Francis GroupJournal of Enzyme Inhibition and Medicinal Chemistry1475-63661475-63742024-12-0139110.1080/14756366.2024.2406025Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylasesKai-Cheng Hsu0Yun-Yi Huang1Jung-Chun Chu2Yu-Wen Huang3Jing-Lan Hu4Tony Eight Lin5Shih-Chung Yen6Jing-Ru Weng7Wei-Jan Huang8Ph.D. Program in Drug Discovery and Development Industry, College of Pharmacy, Taipei Medical University, Taipei, TaiwanPh.D. Program in Drug Discovery and Development Industry, College of Pharmacy, Taipei Medical University, Taipei, TaiwanPh.D. Program in Drug Discovery and Development Industry, College of Pharmacy, Taipei Medical University, Taipei, TaiwanGraduate Institute of Pharmacognosy, College of Pharmacy, Taipei Medical University, Taipei, TaiwanDepartment of Marine Biotechnology and Resources, National Sun Yat-sen University, Kaohsiung, TaiwanGraduate Institute of Cancer Biology and Drug Discovery, College of Medical Science and Technology, Taipei Medical University, Taipei, TaiwanWarshel Institute for Computational Biology, The Chinese University of Hong Kong (Shenzhen), Shenzhen, Guangdong, ChinaDepartment of Marine Biotechnology and Resources, National Sun Yat-sen University, Kaohsiung, TaiwanPh.D. Program in Drug Discovery and Development Industry, College of Pharmacy, Taipei Medical University, Taipei, TaiwanClass IIa histone deacetylases (HDACs) have been linked to tumorigenesis in various cancers. Previously, we designed phenylhydroxamic acid LH4f as a potent class IIa HDAC inhibitor. However, it also unselectively inhibited class I and class IIb HDACs. To enhance the compound’s selectivity towards class IIa HDACs, the ortho-phenyl group from the selective HDAC7 inhibitor 1 is incorporated into ortho position of the phenylhydroxamic acid in LH4f. Compared to LH4f, most resulting compounds displayed substantially improved selectivity towards the class IIa HDACs. Notably, compound 7 g exhibited the strongest HDAC9 inhibition with an IC50 value of 40 nM. Molecular modelling further identified the key interactions of compound 7 g bound to HDAC9. Compound 7 g significantly inhibited several human cancer cells, induced apoptosis, modulated caspase-related proteins as well as p38, and caused DNA damage. These findings suggest the potential of class IIa HDAC inhibitors as lead compounds for the development of cancer therapeutics.https://www.tandfonline.com/doi/10.1080/14756366.2024.2406025Class IIa histone deacetylases (HDACs)structure-activity relationship (SAR)molecular modellingcancer cells
spellingShingle Kai-Cheng Hsu
Yun-Yi Huang
Jung-Chun Chu
Yu-Wen Huang
Jing-Lan Hu
Tony Eight Lin
Shih-Chung Yen
Jing-Ru Weng
Wei-Jan Huang
Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
Journal of Enzyme Inhibition and Medicinal Chemistry
Class IIa histone deacetylases (HDACs)
structure-activity relationship (SAR)
molecular modelling
cancer cells
title Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
title_full Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
title_fullStr Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
title_full_unstemmed Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
title_short Synthesis and biological evaluation of ortho-phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class IIa histone deacetylases
title_sort synthesis and biological evaluation of ortho phenyl phenylhydroxamic acids containing phenothiazine with improved selectivity for class iia histone deacetylases
topic Class IIa histone deacetylases (HDACs)
structure-activity relationship (SAR)
molecular modelling
cancer cells
url https://www.tandfonline.com/doi/10.1080/14756366.2024.2406025
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