Single-Atom Fe-Catalyzed Acceptorless Dehydrogenative Coupling to Quinolines

被引：19

作者：

Lu, Yanze ^{[1
]}

Zhu, Meiling ^{[1
,2
]}

Chen, Sanxia ^{[1
]}

Yao, Jiewen ^{[1
]}

Li, Ting ^{[2
]}

Wang, Xu ^{[3
]}

Tang, Conghui ^{[1
]}

机构：

[1] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Mat Chem & Serv Failure, Key Lab Mat Chem Energy Convers & Storage, 1037 Luoyu Rd, Wuhan 430074, Peoples R China

[2] Nanyang Normal Univ, Coll Chem & Pharmaceut Engn, Nanyang 473061, Peoples R China

[3] Shenzhen IASF, Inst Adv Sci Facil, 268 Zhenyuan Rd, Shenzhen 518107, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2024年 / 146卷 / 33期

基金：

中国国家自然科学基金;

关键词：

N-C CATALYST; BORROWING HYDROGEN; PINCER COMPLEXES; ALPHA-ALKYLATION; CARBOXYLIC-ACIDS; ALCOHOLS; KETONES; SITES; OXIDATION; DESIGN;

D O I：

10.1021/jacs.4c06145

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

A single-atom iron catalyst was found to exhibit exceptional reactivity in acceptorless dehydrogenative coupling for quinoline synthesis, outperforming known homogeneous and nanocatalyst systems. Detailed characterizations, including aberration-corrected HAADF-STEM, XANES, and EXAFS, jointly confirmed the presence of atomically dispersed iron centers. Various functionalized quinolines were efficiently synthesized from different amino alcohols and a range of ketones or alcohols. The iron single-atom catalyst achieved a turnover number (TON) of up to 105, far exceeding the results of current homogeneous and nanocatalyst systems. Detailed mechanistic studies verified the significance of single-atom Fe sites in the dehydrogenation process.

引用

页码：23338 / 23347

页数：10

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