南方科技大学知识苑(SUSTech KC): Iron Corrole-Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [Fe<SUP>V</SUP>(Cor)(NAd)]

题名	Iron Corrole-Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [Fe^V(Cor)(NAd)]
作者	You, Tingjie 1; Shing, Ka-Pan 1; Wu, Liangliang 1; Wu, Kai 1; Wang, Hua-Hua2 ; Liu, Yungen2 ; Du, Lili 1; Liang, Runhui 1; Phillips, David Lee 1; Chang, Xiao-Yong2 ; Huang, Jie-Sheng 1; Che, Chi-Ming 1,2,3,4
通讯作者	Che, Chi-Ming
发表日期	2024-08-01
DOI	10.1002/advs.202401420
发表期刊	ADVANCED SCIENCE 影响因子和分区
EISSN	2198-3844
摘要	As nitrogen analogues of iron-oxo species, high-valent iron-imido species have attracted great interest in the past decades. Fe-V-alkylimido species are generally considered to be key reaction intermediates in Fe(III)-catalyzed C(sp(3))& horbar;H bond aminations of alkyl azides but remain underexplored. Here, it is reported that iron-corrole (Cor) complexes can catalyze a wide range of intramolecular C & horbar;H amination reactions of alkyl azides to afford a variety of 5-, 6- and 7-membered N-heterocycles, including alkaloids and natural product derivatives, with up to 3880 turnover numbers (TONs) and excellent diastereoselectivity (>99:1 d.r.). Mechanistic studies including density functional theory (DFT) calculations and intermolecular hydrogen atom abstraction (HAA) reactions reveal key reactive Fe-V-alkylimido intermediates. The [Fe-V(Cor)(NAd)] (Ad = adamantyl) complex is independently prepared and characterized through electron paramagnetic resonance (EPR), resonance Raman (rR) measurement, and X-ray photoelectron spectroscopy (XPS). This complex is reactive toward HAA reactions with kinetic isotope effects (KIEs) similar to [Fe(Cor)]-catalyzed intramolecular C & horbar;H amination of alkyl azides.
关键词	C & horbar H activation corrole imido complexes iron N-heterocycles
相关链接	[来源记录]
收录类别	SCI ; EI
语种	英语
学校署名	通讯
资助项目	Hong Kong Research Grants Council General Research Fund[17315122]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:001294118300001
出版者	WILEY
来源库	Web of Science
引用统计
成果类型	期刊论文
条目标识符	http://sustech.caswiz.com/handle/2SGJ60CL/804655
专题	理学院_化学系
作者单位	1.Univ Hong Kong, Dept Chem, State Key Lab Synthet Chem, Pokfulam Rd, Hong Kong 000000, Peoples R China 2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China 3.HKU Shenzhen Inst Res & Innovat, Shenzhen 518057, Guangdong, Peoples R China 4.Hong Kong Sci & Technol Pk, Lab Synthet Chem & Chem Biol Ltd, Units 1503 1511, 15-F,Bldg 17W, Hong Kong 000000, Peoples R China
通讯作者单位	化学系
推荐引用方式 GB/T 7714	You, Tingjie,Shing, Ka-Pan,Wu, Liangliang,et al. Iron Corrole-Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [Fe^V(Cor)(NAd)][J]. ADVANCED SCIENCE,2024.
APA	You, Tingjie.,Shing, Ka-Pan.,Wu, Liangliang.,Wu, Kai.,Wang, Hua-Hua.,...&Che, Chi-Ming.(2024).Iron Corrole-Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [Fe^V(Cor)(NAd)].ADVANCED SCIENCE.
MLA	You, Tingjie,et al."Iron Corrole-Catalyzed Intramolecular Amination Reactions of Alkyl Azides. Spectroscopic Characterization and Reactivity of [Fe^V(Cor)(NAd)]".ADVANCED SCIENCE (2024).