Synthesis and Optimization of Nitroxide-Based Inhibitors of Ferroptotic Cell Death in Cancer Cells and Macrophages

DOI

10.1021/acsmedchemlett.1c00561

Document Type

Journal Article

Publication Date

3-10-2022

Publication Title

ACS Medicinal Chemistry Letters

Volume

13

Issue

3

First Page

403

Last Page

408

Keywords

alkene isomerization, Ferroptosis, imine addition, macrophages, vinylogous Mannich reaction

Abstract

JP4-039 is an alkene peptide isostere that acts as a low-micromolar inhibitor of erastin- and RSL-3-induced ferroptotic cell death in the HT-1080 cell line. In this work, we have developed new synthetic strategies that allow access to analogues of this lead structure. Enantioselective vinylogous Mannich or cross-metathesis reactions were key to the preparation of a series of analogues that culminated in the preparation of the ca. 30-fold more potent analogue (S)-6c. Structure-activity relationship analyses used both HT-1080 cells and a luminescence-based ferroptosis assay in RAW 264.7 macrophages. In particular, α,α-disubstituted alkene peptide isosteres (Rα ≠ H) were found to exceed the potency of the corresponding glycine (Rα = H) derivatives.

Open Access

Green Final

Share

COinS