N-alkyl amines are important chemical intermediates, and they are mainly produced by N-alkylation of amines. In the last decades, researchers in this field have concentrated on the development of new methods and novel catalytic materials for N-alkylation reactions.  

Since 2009, extensive studies about heterogeneous catalyst preparation for N-alkyl amine synthesis have been performed by the research group headed by Professor Shi Feng at the Lanzhou Institute of Chemical Physics (LICP) of the Chinese Academy of Sciences (CAS). Heterogeneous catalysts including supported nano-Pd, Ag and Au were successfully prepared, and good results were obtained (Chem. Commun., 2014, 50, 13521-13523; ChemSusChem., 2014, 7, 720-722; ACS Catal., 2013, 3, 808-811; Chem. Eur. J., 2013, 19, 3665-3675; Chem. Commun., 2012, 48, 7586-7588; 2012, 48, 9391-9393; 2011, 47, 6476-6478; Chem. Eur. J. 2011, 17, 1021-1028; 2011, 17, 2587-2591). 

Recently, new progress was made by Professor Shi Feng’s group in new catalytic material and new method studies for N-alkyl amine synthesis. 

An efficient nickel-copper hybrid catalytic material was designed and prepared for the synthesis of N-alkyl amine via alcohol amination without the addition of noble-metal and organic ligand. This novel catalyst is stable to air and moisture, and can be re-covered from the reaction mixture and reused easily. This new method has obtained the patent authorization of the United States Patent and Trademark Office (US8901354 B2, by Shi Feng, Cui Xinjiang, Yuan Hangkong and Deng Youquan).  

In order to promote the recycling of CO2 in fine chemical synthesis, CuAlOx and supported nano-Pd catalysts were prepared for the one-pot synthesis of N-methyl, N,N-dimethyl, and N-formamide amines with CO2/H2 as the methyl and carbonyl source. The starting materials can be extended to nitrobenzene derivatives and aromatic nitriles (Chem. Sci., 2014, 5, 649-656; Chem. Commun., 2012, 50, 189-191; 13521-13523). Chinese and US patent applications have been submitted. 

In previous reports about N-alkyl amine synthesis, the catalysts are mainly composed of transition-metals, and less report concerns regarding application of heterogeneous non-transition-metal catalytic material. Here, a simple and efficient nano-carbon catalyst was prepared for the N-alkyl amine synthesis via alcohol amination reaction. This catalytic material exhibits excellent performance in the borrowing-hydrogen reactions including alcohol amination and catalytic reduction of nitro- and carbonyl groups. This relevant achievement was published online at Nature Communications (2015, 6, 6478, doi: 10.1038/ncomms7478). 

For more information, please contact: Ms. Jing Se at jingse@licp.cas.cn