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Scandium-Promoted Direct Conversion of Dinitrogen into Hydrazine Derivatives via N-C Bond Formation

文献类型：期刊论文

作者Lv, Ze-Jie; Huang, Zhe; Zhang, Wen-Xiong; Xi, Zhenfeng
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2019-06-05
卷号141期号:22页码:8773-8777
ISSN号0002-7863
DOI10.1021/jacs.9b04293
通讯作者Zhang, Wen-Xiong(wx_zhang@pku.edu.cn) ; Xi, Zhenfeng(zfxi@pku.edu.cn)
英文摘要Direct conversion of dinitrogen (N-2) into organic compounds, not through ammonia (NH3), is of great significance both fundamentally and practically. Here we report a highly efficient scandium-mediated synthetic cycle affording hydrazine derivatives (RMeN-NMeR') directly from N-2 and carbon-based electrophiles. The cycle includes three main steps: (i) reduction of a halogen-bridged discandium complex under N-2 leading to a (N-2)(3-)-bridged discandium complex via a (N-2)(2-) intermediate; (ii) treatment of the (N-2)(3-) complex with methyl triflate (MeOTf), affording a (N2Me2)(2-)-bridged discandium complex; and (iii) further reaction of the (N2Me2)(2-) complex with the carbon-based electrophile, producing the hydrazine derivative and regenerating the halide precursor. Furthermore, insertion of a CO molecule into one Sc-N bond in the (N2Me2)(2-)-scandium complex was observed. Most notably, this is the first example of rare-earth metal-promoted direct conversion of N-2 to organic compounds; the formation of C-N bonds by the reaction of these (N-2)(3-) and (N2Me2)(2-) complexes with electrophiles represents the first case among all N-2-metal complexes reported.
WOS关键词SIDE-ON ; COMPLEX ; REDUCTION ; CLEAVAGE ; N-2 ; HYDROGENATION ; FUNCTIONALIZATION ; CHEMISTRY ; AMMONIA ; COORDINATION
资助项目National Natural Science Foundation of China[21725201] ; National Natural Science Foundation of China[21890721] ; National Natural Science Foundation of China[21690061] ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; High-Performance Computing Platform of Peking University
WOS研究方向Chemistry
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000470939200023
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; High-Performance Computing Platform of Peking University ; High-Performance Computing Platform of Peking University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; High-Performance Computing Platform of Peking University ; High-Performance Computing Platform of Peking University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; High-Performance Computing Platform of Peking University ; High-Performance Computing Platform of Peking University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; Peking University, Beijing National Laboratory for Molecular Sciences (BNLMS) ; High-Performance Computing Platform of Peking University ; High-Performance Computing Platform of Peking University
源URL[http://cas-ir.dicp.ac.cn/handle/321008/172053]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Zhang, Wen-Xiong; Xi, Zhenfeng
作者单位Peking Univ, BNLMS, Key Lab Bioorgan Chem & Mol Engn, Minist Educ,Coll Chem, Beijing 100871, Peoples R China
推荐引用方式
GB/T 7714		 Lv, Ze-Jie,Huang, Zhe,Zhang, Wen-Xiong,et al. Scandium-Promoted Direct Conversion of Dinitrogen into Hydrazine Derivatives via N-C Bond Formation[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(22):8773-8777.
APA Lv, Ze-Jie,Huang, Zhe,Zhang, Wen-Xiong,&Xi, Zhenfeng.(2019).Scandium-Promoted Direct Conversion of Dinitrogen into Hydrazine Derivatives via N-C Bond Formation.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(22),8773-8777.
MLA Lv, Ze-Jie,et al."Scandium-Promoted Direct Conversion of Dinitrogen into Hydrazine Derivatives via N-C Bond Formation".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.22(2019):8773-8777.

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来源：大连化学物理研究所

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