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DOI | 10.1038/s41467-017-01959-6 |
N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks | |
Li, Hu1,2,3; Guo, Haixin2; Su, Yaqiong4; Hiraga, Yuya3; Fang, Zhen1; Hensen, Emiel J. M.4; Watanabe, Masaru2,3; Smith, Richard Lee, Jr.2,3 | |
2019-02-11 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2019 |
卷号 | 10 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China; Japan; Netherlands |
英文摘要 | Nitrogen-containing compounds, especially primary amines, are vital building blocks in nature and industry. Herein, a protocol is developed that shows in situ formed N-formyl quasicatalytic species afford highly selective synthesis of formamides or amines with controllable levels from a variety of aldehyde-and ketone-derived platform chemical substrates under solvent-free conditions. Up to 99% yields of mono-substituted formamides are obtained in 3 min. The C-N bond formation and N-formyl species are prevalent in the cascade reaction sequence. Kinetic and isotope labeling experiments explicitly demonstrate that the C-N bond is activated for subsequent hydrogenation, in which formic acid acts as acid catalyst, hydrogen donor and as N-formyl species source that stabilize amine intermediates elucidated with density functional theory. The protocol provides access to imides from aldehydes, ketones, carboxylic acids, and mixed-substrates, requires no special catalysts, solvents or techniques and provides new avenues for amination chemistry. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000458297200003 |
WOS关键词 | MICROWAVE-ASSISTED PYROLYSIS ; DIRECT REDUCTIVE AMINATION ; PRIMARY AMINES ; RUTHENIUM NANOPARTICLES ; ACID ; HYDROGEN ; CONVERSION ; FORMAMIDE ; KETONES ; WATER |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203583 |
专题 | 资源环境科学 |
作者单位 | 1.Nanjing Agr Univ, Coll Engn, Biomass Grp, 40 Dianjiangtai Rd, Nanjing 210031, Jiangsu, Peoples R China; 2.Tohoku Univ, Grad Sch Environm Studies, Aoba Ku, 6-6-11 Aoba, Sendai, Miyagi 9808579, Japan; 3.Tohoku Univ, Res Ctr Supercrit Fluid Technol, Grad Sch Engn, Aoba Ku, 6-6-11 Aoba, Sendai, Miyagi 9808579, Japan; 4.Eindhoven Univ Technol, Dept Chem Engn & Chem, Lab Inorgan Mat Chem, Schuit Inst Catalysis, POB 513, NL-5600 MB Eindhoven, Netherlands |
推荐引用方式 GB/T 7714 | Li, Hu,Guo, Haixin,Su, Yaqiong,et al. N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks[J]. NATURE COMMUNICATIONS,2019,10. |
APA | Li, Hu.,Guo, Haixin.,Su, Yaqiong.,Hiraga, Yuya.,Fang, Zhen.,...&Smith, Richard Lee, Jr..(2019).N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks.NATURE COMMUNICATIONS,10. |
MLA | Li, Hu,et al."N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks".NATURE COMMUNICATIONS 10(2019). |
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