1,2-Dichloroethane Deep Oxidation over Bifunctional Ru/CexAly Catalysts
Author(s) -
Yufeng Gu,
Xingxing Jiang,
Wei Sun,
Shuxing Bai,
Qiguang Dai,
Xingyi Wang
Publication year - 2018
Publication title -
acs omega
Language(s) - Uncategorized
Resource type - Journals
SCImago Journal Rank - 0.779
H-Index - 40
ISSN - 2470-1343
DOI - 10.1021/acsomega.8b00592
Subject(s) - bifunctional , 1,2 dichloroethane , catalysis , dichloroethane , inorganic chemistry , chemistry , nuclear chemistry , materials science , organic chemistry
Ru/Ce x Al y catalysts were synthesized with impregnation of RuCl 3 aqueous solution on Ce x Al y (Al 2 O 3 -CeO 2 ) and used in 1,2-dichloroethane (1,2-DCE) oxidation. Characterization by X-ray diffraction, Raman, NH 3 -temperature-programmed desorption (TPD), CO 2 -TPD, X-ray photoelectron spectroscopy, and H 2 -temperature-programmed reduction indicates that CeO 2 exists as a form of face-centered cubic fluorite structure, whereas the chemical states and the structure of Ru species are dependent on the Ce content. The reducibility and acidity of catalysts increase with Ce/Ce + Al ratio. However, the latter is promoted only in a Ce/Ce + Al range of 0-0.25 and then decreases quickly. Ru/Ce x Al y catalysts have considerable activity for 1,2-DCE combustion. TOF Ru of 1,2-DCE oxidation increases with strong acid, which is ascribed to a synergy of reducibility and acidity. Ru greatly inhibits the chlorination through the decreases in both Cl deposition and CH 2 =CHCl formation. High stability of Ru/Ce 10 Al 90 maintains at 280 °C for at least 25 h with CO 2 selectivity of 99% or higher. In situ Fourier transform infrared spectroscopy indicates that 1,2-DCE dissociates to form ClCH 2 -CH 2 O- species, which is an intermediate species for the production of CH 3 CHO and CH 2 =CHCl, the former responsible for deep oxidation.
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