TY - JOUR
T1 - Dibenzothiophene oxidation in a model diesel fuel using CuO/GC catalysts and H2O2 in the presence of acetic acid under acidic condition
AU - Arellano, U.
AU - Shen, J. M.
AU - Wang, J. A.
AU - Timko, M. T.
AU - Chen, L. F.
AU - Vázquez Rodríguez, J. T.
AU - Asomoza, M.
AU - Estrella, A.
AU - González Vargas, O. A.
AU - Llanos, M. E.
N1 - Publisher Copyright:
©2014 Elsevier Ltd. All rights reserved.
PY - 2015/6/1
Y1 - 2015/6/1
N2 - A series of CuO supported on graphite carbon catalysts (noted as Cu/GC) was prepared with impregnation method and CuO loading varied from 1 wt% to 5, 10 and 15 wt%. Textural properties, crystalline structure, phase composition, copper oxidation states, and morphology of the Cu/GC catalysts were characterized by N2 physisorption, X-ray diffraction (XRD), Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy. Surface acidity was measured by using temperature-programmed desorption of ammonia (TPD-NH3). Surface Cu2+ ions, H2O2 oxidant, acetic acid promoter, and acidic media were all crucial for oxidative desulfurization (ODS) of a model diesel fuel. Both XRD and XPS results confirmed that Cu2+ and Cu+ coexisted on the carbon surface and the Cu2+/(Cu2+ + Cu+) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu2+ ions are the active catalytic sites. Acetic acid reacted with H2O2 to form surface peroxyacetic species that coordinated with Cu2+ on the Cu/GC catalysts in acidic media and promoted the ODS activity. Low pH condition favored significantly dibenzothiophene (DBT) oxidation. Under the optimal operation condition (pH = 0, reaction temperature 70 °C, and catalyst loading 0.3 g with H2O2-glacial acetic acid), DBT concentration in oil was reduced from an initial value of 300 ppm to 78 ppm, 9 ppm, 3 ppm and 0 ppm after ODS treatment using Cu/GC catalysts loading with 1, 5, 10, and 15 wt% of CuO, respectively.
AB - A series of CuO supported on graphite carbon catalysts (noted as Cu/GC) was prepared with impregnation method and CuO loading varied from 1 wt% to 5, 10 and 15 wt%. Textural properties, crystalline structure, phase composition, copper oxidation states, and morphology of the Cu/GC catalysts were characterized by N2 physisorption, X-ray diffraction (XRD), Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy. Surface acidity was measured by using temperature-programmed desorption of ammonia (TPD-NH3). Surface Cu2+ ions, H2O2 oxidant, acetic acid promoter, and acidic media were all crucial for oxidative desulfurization (ODS) of a model diesel fuel. Both XRD and XPS results confirmed that Cu2+ and Cu+ coexisted on the carbon surface and the Cu2+/(Cu2+ + Cu+) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu2+ ions are the active catalytic sites. Acetic acid reacted with H2O2 to form surface peroxyacetic species that coordinated with Cu2+ on the Cu/GC catalysts in acidic media and promoted the ODS activity. Low pH condition favored significantly dibenzothiophene (DBT) oxidation. Under the optimal operation condition (pH = 0, reaction temperature 70 °C, and catalyst loading 0.3 g with H2O2-glacial acetic acid), DBT concentration in oil was reduced from an initial value of 300 ppm to 78 ppm, 9 ppm, 3 ppm and 0 ppm after ODS treatment using Cu/GC catalysts loading with 1, 5, 10, and 15 wt% of CuO, respectively.
KW - Acetic acid
KW - Dibenzothiophene
KW - Graphite carbon
KW - HO
KW - Oxidative desulfurization
UR - http://www.scopus.com/inward/record.url?scp=84923825332&partnerID=8YFLogxK
U2 - 10.1016/j.fuel.2014.11.001
DO - 10.1016/j.fuel.2014.11.001
M3 - Artículo
SN - 0016-2361
VL - 149
SP - 15
EP - 25
JO - Fuel
JF - Fuel
ER -