Improvement of Asparagine Ethylenediamines as Anti-malarial

Authors

Wenhu Zhan, Department of Microbiology & Immunology , Weill Cornell MedicineFollow
Joseph Visone, Department of Microbiology & Immunology , Weill Cornell MedicineFollow
Tierra Ouellette, Department of Microbiology & Immunology , Weill Cornell Medicine
Jacob C. Harris, Department of Microbiology & Immunology , Weill Cornell Medicine
Rong Wang, NMR Analytical Core Facility , Memorial Sloan Kettering Cancer CenterFollow
Hao Zhang, Department of Microbiology & Immunology , Weill Cornell MedicineFollow
Pradeep K. Singh, Chemical Core Facility, Department of Biochemistry , Weill Cornell MedicineFollow
John Ginn, Tri-Institutional Therapeutics Discovery Institute
George Sukenick, NMR Analytical Core Facility , Memorial Sloan Kettering Cancer CenterFollow
Tzu-Tshin Wong, Takeda Pharmaceutical Company Ltd.Follow
Judith I. Okoro, Infectious Diseases Research Collaboration
Ryan M. Scales, Department of Public Health , University of North Carolina
Patrick K. Tumwebaze, Infectious Diseases Research CollaborationFollow
Philip J. Rosenthal, Department of Medicine, University of California, San FranciscoFollow
Björn F. C. Kafsack, Department of Microbiology & Immunology , Weill Cornell Medicine
Roland A. Cooper, Department of Natural Sciences and Mathematics, Dominican University of CaliforniaFollow
Peter T. Meinke, Tri-Institutional Therapeutics Discovery Institute
Laura A. Kirkman, Department of Microbiology & Immunology , Weill Cornell MedicineFollow
Gang Lin, Department of Microbiology & Immunology , Weill Cornell MedicineFollow

Department

Natural Sciences and Mathematics

Document Type

Article

Source

Journal of Medicinal Chemistry

Publication Date

7-11-2019

ISSN

1520-4804

Volume

62

Issue

13

First Page

6137

Last Page

6145

Abstract

The Plasmodium proteasome (Pf20S) emerged as a target for antimalarials. Pf20S inhibitors are active at multiple stages of the parasite life cycle and synergize with artemisinins, suggesting that Pf20S inhibitors have potential to be prophylactic, therapeutic, and transmission blocking as well as are useful for combination therapy. We recently reported asparagine ethylenediamines (AsnEDAs) as immunoproteasome inhibitors and modified AsnEDAs as selective Pf20S inhibitors. Here, we report further a structure–activity relationship study of AsnEDAs for selective inhibition of Pf20S over human proteasomes. Additionally, we show new mutation that conferred resistance to AsnEDAs and collateral sensitivity to an inhibitor of the Pf20S β2 subunit, the same as previously identified resistant mutation. This resistance could be overcome through the use of the structure-guided inhibitor design. Collateral sensitivity to inhibitors among respective proteasome subunits underscores the potential value of treating malaria with combinations of inhibitors of different proteasome subunits to minimize the emergence of drug resistance.

PubMed ID

31177777

Rights

Copyright © 2019 American Chemical Society

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