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Light‐Controlled Tyrosine Nitration of Proteins

Tengfang Long, Lei Liu, Youqi Tao, Wanli Zhang, Jiale Quan, Jie Zheng, Julian D. Hegemann, Motonari Uesugi, Wenbing Yao, Hong Tian, Huan Wang

2021Angewandte Chemie International Edition69 citationsDOI

Abstract

Tyrosine nitration of proteins is one of the most important oxidative post-translational modifications in vivo. A major obstacle for its biochemical and physiological studies is the lack of efficient and chemoselective protein tyrosine nitration reagents. Herein, we report a generalizable strategy for light-controlled protein tyrosine nitration by employing biocompatible dinitroimidazole reagents. Upon 390 nm irradiation, dinitroimidazoles efficiently convert tyrosine residues into 3-nitrotyrosine residues in peptides and proteins with fast kinetics and high chemoselectivity under neutral aqueous buffer conditions. The incorporation of 3-nitrotyrosine residues enhances the thermostability of lasso peptide natural products and endows murine tumor necrosis factor-α with strong immunogenicity to break self-tolerance. The light-controlled time resolution of this method allows the investigation of the impact of tyrosine nitration on the self-assembly behavior of α-synuclein.

Topics & Concepts

TyrosineChemistryNitrationNitrotyrosineBiochemistryBiophysicsCombinatorial chemistryOrganic chemistryBiologyEnzymeNitric oxide synthaseRedox biology and oxidative stressReceptor Mechanisms and SignalingNeutrophil, Myeloperoxidase and Oxidative Mechanisms
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