Effect of the Support Material on Structure and Reactivity of Copper Catalysts for the Hydrogenation of Dimethyl Malonate to 1,3-Propanediol
1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China;
2. Pujing Chemical Industry (SHA) Limited Company, Shanghai 201102, China
Abstract The influence of the type of support (Al2O3, MgO, HMS, and SiO2) on the structure and catalytic performance of copper catalysts for the heterogeneous synthesis of 1,3-propanediol (1,3-PDO) from the hydrogenation of dimethyl malonate (DMM) was investigated. The supported copper catalysts prepared via a urea-assisted homogeneous depiction-precipitation method have been characterized by multiple characterizations including Fourier-transform infrared spectroscopy, X-ray diffraction, temperature-programmed reduction, temperature-programmed desorption of hydrogen, X-ray photoelectron spectroscopy, and in-situ infrared spectroscopy study of CO adsorption. These results revealed that a synergistic effect linked to the copper-support interactions of the catalysts play crucial roles in the surface Cu0 area and surface Cu+ concentration, thereby determining the catalytic activity of Cu catalysts for DMM hydrogenation. The following activity order was obtained: Cu/SiO2 > Cu/HMS > Cu/MgO > Cu/Al2O3. Cu/SiO2 exhibited a highest reactivity of DMM conversion of 92.7% with 39.5% selectivity to 1,3-PDO, which is attributed the catalyst having a favorable Cu0 surface (26.2 m2/g-cat) and surface ratio of Cu+/(Cu0 + Cu+) (~0.32). The Cu/SiO2 catalyst showed a good stability and a promising industrial application in DMM hydrogenation.
Zheng Sainan 1,Sun Jianlei 1,Li Wei 1 et al. Effect of the Support Material on Structure and Reactivity of Copper Catalysts for the Hydrogenation of Dimethyl Malonate to 1,3-Propanediol[J]. 化学反应工程与工艺, 2018, 34(2): 104-112.
Zheng Sainan 1,Sun Jianlei 1,Li Wei 1 et al. Effect of the Support Material on Structure and Reactivity of Copper Catalysts for the Hydrogenation of Dimethyl Malonate to 1,3-Propanediol[J]. 化学反应工程与工艺, 2018, 34(2): 104-112.
