CIESC Journal ›› 2019, Vol. 70 ›› Issue (3): 937-943.doi: 10.11949/j.issn.0438-1157.20181083

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

Preparation of palladium-based catalysts by complexing-solvothermal method and catalytic oxidation of m-xylene

Shuai HE1,2(),Feng GUO2(),Guojun KANG1(),Jian YU2,Xuefeng REN1,Guangwen XU3   

  1. 1. Key Laboratory of Coal-based CO2 Capture and Geological Storage, School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 221116, Jiangsu, China
    2. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
    3. Shenyang University of Chemical Technology, Shenyang 110142, Liaoning, China
  • Received:2018-09-26 Revised:2018-12-07 Online:2019-03-05 Published:2018-12-07
  • Contact: Feng GUO,Guojun KANG E-mail:shuaih@cumt.edu.cn;guofeng@ipe.ac.cn;gjkang@cumt.edu.cn

Abstract:

The Pd/Al2O3 catalysts with a loading of 0.6% (mass fraction) were prepared by complexation-solvent thermal method, hydrothermal method and impregnation method. The effect of different preparation methods on the performance of the catalyst was evaluated by using m-xylene as the representative of volatile organic compounds (VOCs). The results showed that the most effective catalyst Pd/Al2O3-com was prepared by complexing-solvothermal. The m-xylene with volume fraction of 0.002% can completely converted to CO2 and H2O (T100) at 130℃ over Pd/Al2O3-com catalyst from the complexing-solvothermal method, which was lower about 30℃ than the catalyst (Pd/Al2O3-imp) from the impregnation method. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET) and scanning electron microscopy (SEM) techniques were performed to characterize the physico-chemical properties of synthesized Pd/Al2O3 catalysts. The results indicated that the Pd element of Pd/Al2O3-com was mainly dispersed on the surface of the support at the reduction state Pd0, while the Pd element of Pd/Al2O3-imp and Pd/Al2O3-hyd catalyst was at the form of Pd2+ with poor dispersion. Combined with the catalytic activity performance and evaluation results, a highly dispersed and reduction state form of Pd active component on the surface of the carrier resulted in a remarkable catalytic activity on m-xylene conversion. The Pd/Al2O3-com catalyst with these features exhibit good activity for removing VOCs under high concentration (0.02%-0.07%, vol) and wide space velocity (5×104-10×104 h-1) conditions, and thus meet well the requirements of industrial application.

Key words: palladium-based catalyst, catalytic oxidation, volatile organic compounds, complexing-solvothermal method, reduction

CLC Number: 

  • O 643.36

Fig.1

Experimental set-up for catalytic tests"

Table1

XRF analysis results for Pd/Al2O3 catalyst/%(mass)"

样品PdAlOOthers
Pd/Al2O3-com0.4551.9846.680.89
Pd/Al2O3-hyd0.4851.8246.790.91
Pd/Al2O3-imp0.3951.6847.130.8

Fig.2

XRD patterns of Pd/Al2O3 catalyst from different preparation methods"

Fig.3

Adsorption isotherms and desorption isotherms of carrier and Pd/Al2O3 catalyst from different preparation methods"

Fig.4

Pore size distribution of carrier and Pd/Al2O3 catalyst from different preparation methods"

Table2

BET surface area, pore volume and pore diameter of carrier and catalysts"

样品比表面积/(m2/g)孔容/(cm3/g)孔径/nm
Al2O31870.429.09
Pd/Al2O3-com1490.318.27
Pd/Al2O3-hyd1740.296.71
Pd/Al2O3-imp1620.358.73

Fig.5

XPS spectra of Pd/Al2O3 catalysts from different preparation methods"

Fig.6

SEM and EDS images of Pd/Al2O3catalysts from different preparation methods"

Fig.7

Catalytic performance of synthesized Pd/Al2O3 from different preparation methods"

Fig.8

Catalytic performance of Pd/Al2O3-com catalyst varied with concentrations and space velocities of m-xylene"

Fig.9

Stability performance of Pd/Al2O3-com(260℃,0.07%(vol.), GHSV:5×104 h-1)"

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