Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2013, Vol. 34 ›› Issue (5): 1020-1026.DOI: 10.1016/S1872-2067(12)60543-9

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Physically mixed ZnO and skeletal NiMo for one-pot reforming-hydrogenolysis of glycerol to 1,2-propanediol

HU Jiyea, LIU Xiaoyua, FAN Yiqiua, XIE Songhaia, PEI Yana, QIAO Minghuaa, FAN Kangniana, ZHANG Xiaoxinb, ZONG Baoningb   

  1. a Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China;
    b State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, Beijing 100083, China
  • Received:2012-12-20 Revised:2013-05-20 Online:2013-05-06 Published:2013-05-06
  • Supported by:

    This work was supported by the Program for New Century Excellent Talents in Universities (NCET-08-0126), the National Basic Research Program of China (973 Program, 2012CB224804), the National Natural Science Foundation of China (21073043), Shanghai Science and Technology Committee (10JC1401800, 08DZ2270500), and Shanghai Key Laboratory of Rare Earth Functional Materials, Shanghai Normal University.

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Abstract:

The one-pot aqueous phase reforming (APR) and hydrogenolysis of glycerol to 1,2-propanediol (PDO) was catalyzed by physically mixed skeletal NiMo and zinc oxide catalysts in a continuous flow fixed-bed reactor without the aid of added H2. The skeletal NiMo catalyst alone is highly active towards glycerol but the selectivity for 1,2-PDO is only moderate. Physically mixing of MgO, SiO2, Al2O3, HZSM-5, TiO2, ZrO2, or CeO2 as a cocatalyst with skeletal NiMo was detrimental to the conversion of glycerol and yield of 1,2-PDO. However, physically mixing with ZnO gave an advantageous promoting effect on both the catalytic activity and selectivity for 1,2-PDO, and gave a 1,2-PDO yield of 52.0%, which is higher than that obtained with noble metal catalysts for the APR-hydrogenolysis of glycerol. The synergistic effect between physically mixed ZnO and skeletal NiMo was attributed to in situ enhancement of the Lewis acidity of ZnO by chemisorbed CO2 from the APR of glycerol on skeletal NiMo, which benefited both the dehydration of glycerol to acetol on ZnO and the hydrogenation of acetol to 1,2-PDO on skeletal NiMo.

Key words: Glycerol, Hydrogenolysis, Zinc oxide, Nickel, Molybdenum, Synergistic effect