Recently, researchers Tao Tao and Wang Aiqin, researchers of Dalian Institute of Chemical Physics, Chinese Academy of Sciences, have made new progress in the reduction and amination of biomass-based aldehydes and ketones. They have successfully achieved a series of biomass-based aldehydes and ketones as substrates in aqueous solutions. The primary amine was prepared, and on the basis of which cellulose was directly used as raw material, ethanolamine was obtained by a two-step process. The relevant research results were published in "Angew. Chem. Int. Ed. (DOI:10.1002/anie.201610964)) and were selected as the current Hot Paper of the magazine.
Nitrogen-containing compounds are important chemicals and are widely used in the fields of polymers, surfactants, dyes, pharmaceuticals, and pesticides. At present, most of the nitrogen-containing compounds are still obtained through fossil resources. Since biomass raw materials such as lignocellulose are mainly composed of three elements: C, H, and O, the chemicals obtained through catalytic conversion of biomass are mainly concentrated on oxygenated chemicals such as alcohols, aldehydes, ketones, acids, esters, etc. This limits the diversity and applicability of biomass-based chemicals. The selective conversion of oxygen-containing functional groups to amino functional groups in biomass feedstocks and their derivatives is achieved by a reductive amination method, which provides a simple, efficient, and renewable new pathway for the synthesis of amine compounds and extends biomass The application of resources also has important significance.
The research team first used glycolaldehyde as the reaction substrate, ammonia as the ammonia source, and Ru/ZrO2 as the catalyst to obtain ethanolamine with high selectivity under the mild reaction conditions (the yield reached 94%); then, the raw material was cellulose. The ethanolamine is obtained through a two-step reaction route of "cellulose-glycolaldehyde-ethanolamine". A variety of in-situ characterization techniques have been used to show that Ru nanoparticles on the mixed valence state can be obtained by controlling the Ru reduction depth. This microstructure has both Lewis acid sites and hydrogenation active sites, making the catalyst highly selective. The catalytic system has a good universality, and it can efficiently convert a series of aldehydes and ketones with different structures into the corresponding primary amines, providing an effective way for the production of nitrogenous chemicals from biomass.
The above research work was supported by the National Natural Science Foundation of China's major projects, the national key research and development program of the Ministry of Science and Technology, the "Nanotechnology" key project, the Chinese Academy of Sciences' strategic pilot technology project, and the Ministry of Education's Energy Materials Chemistry Collaborative Innovation Center (iChem). Postdoctoral incentive fund support.
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