The Influence of CeO2-Cube Supported Gold Nanoparticle on the Catalytic Performance of 1,3-Propanediol Oxidative Esterification
1. School of Environmental and Chemical Engineering, Shenyang Ligong University, Shenyang 110159, China;
2. CAS Key Laboratory of Biobased Materials, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China;
3. Laboratory of Chemical Engineering and Technology for Low-carbon energy, College of Chemical and Environmental Engineering, Shandong University of Science and Technology, Qingdao 266590, China
Abstract:Au nanoparticles supported on CeO2 nanocubes were successfully prepared by a deposition-precipitation method and tested for the oxidative esterification of 1,3-propanediol. The catalyst was characterized by inductively coupled plasma atomic emission spectrometry, transmission electron microscope (TEM), X-ray diffraction, and X-ray photoelectron spectroscopy. The different parameters which may affect catalytic performance, such as dosage of urea, the calcination temperature of CeO2 nanocubes, the calcination temperature of Au/CeO2-cube, Au loading and the loading temperature were investigated. The optimized preparation conditions of Au/CeO2-cube were obtained as follows: the mass ratio of urea/ceria 6, the calcination temperature of CeO2 nanocubes 400 ℃,the calcination temperature of Au/CeO2-cube 200 ℃,Au loading 1.5% and the loading temperature 80 ℃. Under the condition of 100 ℃, pressure of O2 2 MPa, the mole ratio of 1,3-propanediol to Au 75.5 and the reaction time 4 hours, the conversion of 1,3-propanediol was 97.5% and the selectivities to methyl 3-hydroxypropionate and dimethyl malonate were 90.1% and 6.1%, respectively. It was found that the catalytic performance decreased slightly when used catalyst was calcined at 200 ℃ for 2 h to burn the surface poisoning substance and recycled four times. This was mainly caused by the fact that Au particle size grew larger in the process of catalytic reaction. It was found that nano Au elemental catalyst particles with the size of 2.0-4.0 nm supported on CeO2 favors for the 1,3-propanediol oxidative esterification.
Zhao Guangzhen 1,2,Zhao Guoming 2 et al. The Influence of CeO2-Cube Supported Gold Nanoparticle on the Catalytic Performance of 1,3-Propanediol Oxidative Esterification[J]. 化学反应工程与工艺, 2016, 32(1): 39-48.