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Ligand‐Enabled Pd‐Catalyzed sp<sup>3</sup> C−H Macrocyclization: Synthesis and Evaluation of Macrocyclic Sulfonamide for the Treatment of Parkinson's Disease

Tongyu Bi, Yunxia Cui, Shuai Liu, Hou–Yong Yu, Weirong Qiu, Ke‐Qiang Hou, Jiaqi Zou, Zhipeng Yu, Feili Zhang, Zhongliang Xu, Jian Zhang, Xiaojun Xu, Weibo Yang

2024Angewandte Chemie International Edition15 citationsDOIOpen Access PDF

Abstract

Abstract The development of simplified synthetic strategy to create structurally and functionally diverse pseudo‐natural macrocyclic molecules is highly appealing but poses a marked challenge. Inspired by natural scaffolds, herein, we describe a practical and concise ligand‐enabled Pd(II)‐catalyzed sp 3 C−H alkylation, olefination and arylation macrocyclization, which could offer a novel set of pseudo‐natural macrocyclic sulfonamides. Interestingly, the potential of ligand acceleration in C−H activation is also demonstrated by an unprecedented enantioselective sp 3 C−H alkylation macrocyclization. Moreover, a combination of in silico screening and biological evaluation led to the identification of a novel spiro‐grafted macrocyclic sulfonamide 2 a , which showed a promising efficacy for the treatment of Parkinson's disease (PD) in a mouse model through the activation of silent information regulator sirtuin 3 (SIRT3).

Topics & Concepts

SulfonamideLigand (biochemistry)ChemistryCombinatorial chemistryIn silicoEnantioselective synthesisAlkylationStereochemistrySIRT3SirtuinCatalysisReceptorBiochemistryAcetylationGeneCatalytic C–H Functionalization MethodsSynthesis and Catalytic ReactionsCatalytic Cross-Coupling Reactions
Ligand‐Enabled Pd‐Catalyzed sp<sup>3</sup> C−H Macrocyclization: Synthesis and Evaluation of Macrocyclic Sulfonamide for the Treatment of Parkinson's Disease | Litcius