Identification of diaminoquinazoline histone lysine methyltransferase structure activity relationships that allow for segregation of human G9a inhibition and anti-Plasmodium activity
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Published version
Author(s)
Type
Journal Article
Abstract
Plasmodium falciparum HKMTs (PfHKMTs) play a key role in controlling Plasmodium gene expression and represent exciting new anti-malarial epigenetic targets. Using an inhibitor series derived from the diaminoquinazoline HKMT inhibitory chemotype, we have previously identified compounds with highly promising antimalarial activity, including irreversible asexual cycle blood stage-independent cytotoxic activity at nM concentrations, oral efficacy in in vivo models of disease, and the unprecedented ability to reactivate dormant liver stage parasites (hypnozoites). However, future development of this series will need to address host versus parasite selectivity, where inhibitory activity against human G9a is removed from the lead compounds, while maintaining potent anti-Plasmodium activity. Herein, we report an extensive study of the SAR of this series against both G9a and P. falciparum. We have identified key SAR features which demonstrate that high parasite vs. G9a selectivity can be achieved by selecting appropriate substituents at position 2, 4 and 7 of the quinazoline ring. We have also, in turn, discovered that potent G9a inhibitors can be identified by employing a 6-carbon ‘Nle mimic’ at position 7. Together, this data suggests that while broadly similar, the G9a and potential PfHKMT target(s) binding pockets and/or binding modes of the diaminoquinazoline analogues exhibit clear and exploitable differences. Based on this, we believe this scaffold to have clear potential for development into a novel anti-malarial therapeutic.
Date Issued
2017-03-15
Date Acceptance
2017-03-10
Citation
MedChemComm, 2017, 8, pp.1069-1092
ISSN
2040-2511
Publisher
Royal Society of Chemistry
Start Page
1069
End Page
1092
Journal / Book Title
MedChemComm
Volume
8
Copyright Statement
© The Royal Society of Chemistry 2017. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (https://creativecommons.org/licenses/by/3.0/)
Sponsor
Commission of the European Communities
Cancer Research UK
Grant Number
PIIF-GA-2011-299857
C33325/A19435
Subjects
Science & Technology
Life Sciences & Biomedicine
Biochemistry & Molecular Biology
Chemistry, Medicinal
Pharmacology & Pharmacy
PROTEIN METHYLTRANSFERASES
2,4-DIAMINO-6,7-DIMETHOXYQUINOLINE DERIVATIVES
ALPHA-1-ADRENOCEPTOR ANTAGONISTS
DIALKYLBIARYL PHOSPHINES
ANTIMALARIAL ACTIVITY
CATALYZED AMINATION
RESISTANT MALARIA
DRUG DISCOVERY
CHEMICAL PROBE
FALCIPARUM
0304 Medicinal And Biomolecular Chemistry
0305 Organic Chemistry
1115 Pharmacology And Pharmaceutical Sciences
Publication Status
Published