Acta Phys. -Chim. Sin. ›› 2016, Vol. 32 ›› Issue (7): 1765-1774.doi: 10.3866/PKU.WHXB201604085

• ARTICLE • Previous Articles     Next Articles

Effect of the Support on Partial Hydrogenation of Toluene over Ru/Oxide Catalysts

Hui-Zi BI1,Rong-Fei DOU1,Hao WANG1,Yan PEI1,Ming-Hua QIAO1,*(),Bin SUN2,Bao-Ning ZONG2,*()   

  1. 1 Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, P. R. China
    2 State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, P. R. China
  • Received:2016-02-11 Published:2016-07-08
  • Contact: Ming-Hua QIAO,Bao-Ning ZONG E-mail:mhqiao@fudan.edu.cn;zongbn.ripp@sinopec.com
  • Supported by:
    the National Key Basic Research Program of China (973)(2012CB224804);National Natural Science Foundation of China(21373055);Science and Technology Commission of Shanghai Municipality, China(08DZ2270500);Technology Development Programof SINOPEC, China(S411043)

Abstract:

The supported Ru catalysts were prepared by the impregnation-chemical reduction method to investigate the effect of some conventional oxide supports (SiO2, m-ZrO2, t-ZrO2, γ-Al2O3, and P25) on the partial hydrogenation of toluene to methylcyclohexenes. The catalysts were characterized by N2 physisorption, powder X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). It was found that the supports influenced the size of the Ru nanoparticles (NPs) and consequently the catalytic performance. With the increase in the size of the Ru NPs from 2.6 to 17.3 nm, the turnover frequency (TOF) of toluene and the initial selectivity (S0) to methylcyclohexenes increased first, reached the maximum, and then decreased, following a volcano-like curve. At the Ru particle size of 3.0 nm, both TOF and S0 reached the highest values. Reaction conditions, such as the type and concentration of the modifiers, the temperature, and the pressure, were optimized over the best Ru/P25 catalyst among the supported Ru catalysts investigated herein. Under the reaction conditions of 423 K, H2 pressure of 5.0 MPa, and using 0.25 g zinc sulfate heptahydrate as the modifier, the initial hydrogenation activity (r0) of 26 mmol·g-1·min-1, the S0 of 57%, and the methylcyclohexenes yield of 36% were obtained.

Key words: Support, Ruthenium, Toluene, Partial hydrogenation, Methylcyclohexene

MSC2000: 

  • O643