Denitration of Nitroarenes Under Ambient Physiological Conditions Catalyzed by Graphdiyne-Supported Palladium  

作　　者：Endong Zhang Yanyan Chen Fengting Lv Zicheng Zuo Feng He Yongjun Li Yiming Huang Yuliang Li Shu Wang 

机构地区：[1]Beijing National Laboratory for Molecular Sciences,Key Laboratory of Organic Solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190 [2]College of Chemistry,University of Chinese Academy of Sciences,Beijing 100049

出　　处：《CCS Chemistry》2024年第3期641-651,共11页中国化学会会刊（英文）

基　　金：support from the National Natural Science Foundation of China(grant nos.22021002,22020102005,and 22022705);the CAS-Croucher Funding Scheme for Joint Laboratories.

摘　　要：The direct cleavage of C–NO_(2)bonds for reductive denitration of nitroarenes remains a challenging transformation in synthetic organic chemistry.Herein,we report a biocompatible palladium-deposited graphdiyne nanocatalyst(Pd@GDY/DSPE-PEG)that can catalyze reductive denitration of nitroarenes under ambient physiological conditions.Mechanistic studies support this transformation via the oxidative addition of nitroarenes with Pd(0)and subsequent ligand exchange to form arylpalladium hydride.This one-step reductive denitration via Pd@GDY/DSPE-PEG successfully facilitates the repair of the nitrated proteins arising from endogenic ONOO−and restores their physiological function,including blocking the apoptosis pathway in living cells.Moreover,Pd@GDY/DSPE-PEG was further successfully applied for catalytic denitration to reduce the level of 3-nitrotyrosine residues of proteins located in the mouse brain hippocampus in vivo.This study provides an ideal strategy for designing highly active enzymatic mimicking synthetic catalysts for the regulation of the nitrated protein level and the detoxification of nitrative damage of living cells and tissues.

关 键 词：3-NITROTYROSINE artificial nanaocatalysts reductive denitration palladium-deposited graphdiyne repairing nitrated protein 

分 类 号：O64[理学—物理化学]