Citation: Jinling Song, Guiyang Yu, Xi Li, Xuwei Yang, Wenxiang Zhang, Wenfu Yan, Gang Liu. Oxidative coupling of alcohols and amines to an imine over Mg-Al acid-base bifunctional oxide catalysts[J]. Chinese Journal of Catalysis, ;2018, 39(2): 309-318. doi: 10.1016/S1872-2067(17)63006-7 shu

Oxidative coupling of alcohols and amines to an imine over Mg-Al acid-base bifunctional oxide catalysts

Jinling Song ^a, ,
Guiyang Yu ^a ,
Xi Li ^a ,
Xuwei Yang ^a ,
Wenxiang Zhang ^a ,
Wenfu Yan ^b ,
Gang Liu ^a

a Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, Jilin, China;
b State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, Jilin, China

Received Date: 13 November 2017
Revised Date: 25 December 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21473073, 21473074), the Development Project of Science and Technology of Jilin Province (20170101171JC), "13th Five-Year" science and technology research of the Education Department of Jilin Province (2016403) and the Open Project of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry (201703).

A series of Mg-Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine. The structure and surface properties of Mg-Al oxides are modulated by changing the Mg/Al ratios, calcination temperature and treatment with probe molecules. Detailed characterization, including X-ray diffraction, ²⁷Al magic angle spinning nuclear magnetic resonance spectroscopy, N₂-adsorption, NH₃-temperature-programmed desorption, CO₂-temperature-programmed desorption and X-ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts. The Mg-Al oxides with Mg/Al=3 exhibit the highest activity in the reaction, which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites. The role of the acidic and basic sites in the reaction process is systematically investigated, and are shown to serve as adsorption and activation sites for amines and alcohols, respectively. Under the synergistic effect of these acid-base centers, the oxidative coupling process successfully occurs on the surface of Mg-Al mixed oxides. Compared with the acidic sites, the weak basic sites play a more important role in the catalytic process. The acidic sites are the catalytic centers for the benzyl alcohol activation, which control the reaction rate of the oxidative coupling reaction.
- Oxidative coupling,
- Imine synthesis,
- Alcohol oxidation,
- Mg-Al mixed oxides,
- Acid-base catalysis
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