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Frontiers of Chemical Science and Engineering

Front. Chem. Sci. Eng.    2020, Vol. 14 Issue (6) : 929-936     https://doi.org/10.1007/s11705-019-1912-2
RESEARCH ARTICLE
Selective hydrogenation of acetylene over Pd/CeO2
Kai Li, Tengteng Lyu, Junyi He, Ben W. L. Jang()
Department of Chemistry, Texas A&M University Commerce, PO Box 3011, Commerce, TX 75429, USA
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Abstract

Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction. Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction. Excellent ethylene selectivity of ~100% was obtained in the whole reaction temperature range of 50°C–200°C for samples calcined at temperatures of 600°C and 800°C. This could be ascribed to the formation of PdxCe1xO2−y or Pd-O-Ce surface species based on the X-ray diffraction and X-ray photoelectron spectroscopy results, indicating the strong interaction between palladium and ceria.

Keywords selective hydrogenation      acetylene      Pd/CeO2      strong interaction     
Corresponding Author(s): Ben W. L. Jang   
Just Accepted Date: 13 February 2020   Online First Date: 20 March 2020    Issue Date: 11 September 2020
 Cite this article:   
Kai Li,Tengteng Lyu,Junyi He, et al. Selective hydrogenation of acetylene over Pd/CeO2[J]. Front. Chem. Sci. Eng., 2020, 14(6): 929-936.
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http://journal.hep.com.cn/fcse/EN/10.1007/s11705-019-1912-2
http://journal.hep.com.cn/fcse/EN/Y2020/V14/I6/929
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Kai Li
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Fig.1  Schematic diagram of the experimental setup.
Fig.2  H2-TPR profiles of 500 ppm Pd/CeO2.
Fig.3  XRD patterns for 500 ppm Pd/CeO2 and commercial ceria.
Fig.4  (a) Pd 3d and (b) O 1s XPS spectra for 500 ppm Pd/CeO2.
Fig.5  FTIR spectra after 5-min desorption on 500 ppm Pd/CeO2 (a) without reduction and (b) reduced at 250°C.
Fig.6  FTIR adsorption spectra versus time on 500 ppm Pd/CeO2 C450 without reduction.
Sample Lattice parameter/nm Pdd+ (2<d≤4) percentage/% BET surface area/(m2?g1) Adsorbed H2
/(mmol?g-Pd1)
Commercial CeO2 0.5414 ? 53.8 0
Pd/CeO2 C300 0.5414 28.5 ? 52.0
Pd/CeO2 C450 0.5405 31.8 51.9 46.7
Pd/CeO2 C600 0.5410 62.8 ? 35.9
Pd/CeO2 C800 0.5410 60.5 28.0 34.3
Tab.1  Lattice parameter, Pdd+ percentage, BET surface area and adsorbed hydrogen of Pd/CeO2 catalysts
Fig.7  (a) Acetylene conversion and (b) ethylene selectivity over 500 ppm Pd/CeO2 C450 without reduction, and reduced at 100°C and 250°C.
Fig.8  Effect of calcination temperature on (a) acetylene conversion and (b) ethylene selectivity over 500 ppm Pd/CeO2 catalyst.
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