Dibenzothiophene oxidation in a model diesel fuel using CuO/GC catalysts and H <inf>2</inf> O <inf>2</inf> in the presence of acetic acid under acidic condition

U. Arellano, J. M. Shen, J. A. Wang, M. T. Timko, L. F. Chen, J. T. Vázquez Rodríguez, M. Asomoza, A. Estrella, O. A. González Vargas, M. E. Llanos

Research output: Contribution to journalArticleResearchpeer-review

21 Citations (Scopus)

Abstract

©2014 Elsevier Ltd. All rights reserved. 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 N 2 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-NH 3 ). Surface Cu 2+ ions, H 2 O 2 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 Cu 2+ and Cu + coexisted on the carbon surface and the Cu 2+ /(Cu 2+ + Cu + ) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu 2+ ions are the active catalytic sites. Acetic acid reacted with H 2 O 2 to form surface peroxyacetic species that coordinated with Cu 2+ 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 H 2 O 2 -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.
Original languageAmerican English
Pages (from-to)15-25
Number of pages12
JournalFuel
DOIs
StatePublished - 1 Jun 2015

Fingerprint

Gasoline
Diesel fuels
Acetic acid
Acetic Acid
Copper
Photoelectron Spectroscopy
X-Ray Diffraction
Oxidation
Desulfurization
Catalysts
Catalytic Domain
Carbon
Ions
Temperature programmed desorption
Temperature
Graphite
Raman Spectrum Analysis
Fourier Transform Infrared Spectroscopy
Transmission Electron Microscopy
Ammonia

Cite this

@article{c2310df6c24e45d8b3adda1c46a14d69,
title = "Dibenzothiophene oxidation in a model diesel fuel using CuO/GC catalysts and H 2 O 2 in the presence of acetic acid under acidic condition",
abstract = "{\circledC}2014 Elsevier Ltd. All rights reserved. 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 N 2 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-NH 3 ). Surface Cu 2+ ions, H 2 O 2 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 Cu 2+ and Cu + coexisted on the carbon surface and the Cu 2+ /(Cu 2+ + Cu + ) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu 2+ ions are the active catalytic sites. Acetic acid reacted with H 2 O 2 to form surface peroxyacetic species that coordinated with Cu 2+ 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 H 2 O 2 -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.",
author = "U. Arellano and Shen, {J. M.} and Wang, {J. A.} and Timko, {M. T.} and Chen, {L. F.} and {V{\'a}zquez Rodr{\'i}guez}, {J. T.} and M. Asomoza and A. Estrella and {Gonz{\'a}lez Vargas}, {O. A.} and Llanos, {M. E.}",
year = "2015",
month = "6",
day = "1",
doi = "10.1016/j.fuel.2014.11.001",
language = "American English",
pages = "15--25",
journal = "Fuel",
issn = "0016-2361",
publisher = "Elsevier BV",

}

Dibenzothiophene oxidation in a model diesel fuel using CuO/GC catalysts and H <inf>2</inf> O <inf>2</inf> in the presence of acetic acid under acidic condition. / Arellano, U.; Shen, J. M.; Wang, J. A.; Timko, M. T.; Chen, L. F.; Vázquez Rodríguez, J. T.; Asomoza, M.; Estrella, A.; González Vargas, O. A.; Llanos, M. E.

In: Fuel, 01.06.2015, p. 15-25.

Research output: Contribution to journalArticleResearchpeer-review

TY - JOUR

T1 - Dibenzothiophene oxidation in a model diesel fuel using CuO/GC catalysts and H 2 O 2 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.

PY - 2015/6/1

Y1 - 2015/6/1

N2 - ©2014 Elsevier Ltd. All rights reserved. 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 N 2 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-NH 3 ). Surface Cu 2+ ions, H 2 O 2 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 Cu 2+ and Cu + coexisted on the carbon surface and the Cu 2+ /(Cu 2+ + Cu + ) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu 2+ ions are the active catalytic sites. Acetic acid reacted with H 2 O 2 to form surface peroxyacetic species that coordinated with Cu 2+ 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 H 2 O 2 -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 - ©2014 Elsevier Ltd. All rights reserved. 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 N 2 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-NH 3 ). Surface Cu 2+ ions, H 2 O 2 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 Cu 2+ and Cu + coexisted on the carbon surface and the Cu 2+ /(Cu 2+ + Cu + ) ratio increased with increasing of copper oxide loading. The copper speciation result is in good correlation with the catalytic activity, indicating that surface Cu 2+ ions are the active catalytic sites. Acetic acid reacted with H 2 O 2 to form surface peroxyacetic species that coordinated with Cu 2+ 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 H 2 O 2 -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.

UR - https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=84923825332&origin=inward

UR - https://www.scopus.com/inward/citedby.uri?partnerID=HzOxMe3b&scp=84923825332&origin=inward

U2 - 10.1016/j.fuel.2014.11.001

DO - 10.1016/j.fuel.2014.11.001

M3 - Article

SP - 15

EP - 25

JO - Fuel

JF - Fuel

SN - 0016-2361

ER -