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Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide

Abstract

Highlights: • Concerned with the question why ODS catalyst is not effective for real gasoline. • Reported the strong inhibiting effect of gasoline composition on ODS for the 1st time. • ODS reactivity is suggested to be determined by partial charge on S atom of thiophene. • Proposed approaches to improve ODS selectivity for real gasoline desulfurization. - Abstract: This work is concerned with the question of why oxidative desulfurization (ODS) catalyst that show good catalytic performance for ODS of model gasoline thiophenic compounds is not effective for real gasoline. For the first time, the effects of gasoline composition on ODS using a phosphotungstic acid/activated carbon (HPW/AC) catalyst with H{sub 2}O{sub 2} were investigated. ODS of thiophene, one of the most difficult thiophenic compounds to be oxidized, was studied in a model fuel system, where a high thiophene conversion rate of 90% could be reached in 2 h at 90 °C. However, when applying the ODS to a real gasoline, the ODS conversion rate decreased to only 32%, suggesting a strong inhibiting effect of gasoline composition on ODS. The ODS studies in different model fuels suggested that the inhibiting effect can be ascribed to the competitive adsorption and oxidation with  More>>
Publication Date:
Jan 15, 2014
Product Type:
Journal Article
Resource Relation:
Journal Name: Applied Energy; Journal Volume: 113; Other Information: Copyright (c) 2013 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ACTIVATED CARBON; ADSORPTION; ALKENES; AROMATICS; CATALYSTS; DESULFURIZATION; ELECTRONS; FUEL SYSTEMS; GASOLINE; HYDROGEN PEROXIDE; OPTIMIZATION; OXIDATION; OXIDIZERS; POLYCYCLIC SULFUR HETEROCYCLES; SULFUR; THIONAPHTHENES; THIOPHENE; TUNGSTOPHOSPHORIC ACID
OSTI ID:
22296433
Country of Origin:
United Kingdom
Language:
English
Other Identifying Numbers:
Journal ID: ISSN 0306-2619; CODEN: APENDX; Other: PII: S0306-2619(13)00554-0; TRN: GB14R1315002604
Availability:
Available from http://dx.doi.org/10.1016/j.apenergy.2013.06.047
Submitting Site:
INIS
Size:
page(s) 78-85
Announcement Date:
Jan 19, 2015

Citation Formats

Xiao, Jing, Wu, Luoming, Wu, Ying, Liu, Bing, Dai, Lu, Li, Zhong, Xia, Qibin, and Xi, Hongxia. Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide. United Kingdom: N. p., 2014. Web. doi:10.1016/J.APENERGY.2013.06.047.
Xiao, Jing, Wu, Luoming, Wu, Ying, Liu, Bing, Dai, Lu, Li, Zhong, Xia, Qibin, & Xi, Hongxia. Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide. United Kingdom. https://doi.org/10.1016/J.APENERGY.2013.06.047
Xiao, Jing, Wu, Luoming, Wu, Ying, Liu, Bing, Dai, Lu, Li, Zhong, Xia, Qibin, and Xi, Hongxia. 2014. "Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide." United Kingdom. https://doi.org/10.1016/J.APENERGY.2013.06.047.
@misc{etde_22296433,
title = {Effect of gasoline composition on oxidative desulfurization using a phosphotungstic acid/activated carbon catalyst with hydrogen peroxide}
author = {Xiao, Jing, Wu, Luoming, Wu, Ying, Liu, Bing, Dai, Lu, Li, Zhong, Xia, Qibin, and Xi, Hongxia}
abstractNote = {Highlights: • Concerned with the question why ODS catalyst is not effective for real gasoline. • Reported the strong inhibiting effect of gasoline composition on ODS for the 1st time. • ODS reactivity is suggested to be determined by partial charge on S atom of thiophene. • Proposed approaches to improve ODS selectivity for real gasoline desulfurization. - Abstract: This work is concerned with the question of why oxidative desulfurization (ODS) catalyst that show good catalytic performance for ODS of model gasoline thiophenic compounds is not effective for real gasoline. For the first time, the effects of gasoline composition on ODS using a phosphotungstic acid/activated carbon (HPW/AC) catalyst with H{sub 2}O{sub 2} were investigated. ODS of thiophene, one of the most difficult thiophenic compounds to be oxidized, was studied in a model fuel system, where a high thiophene conversion rate of 90% could be reached in 2 h at 90 °C. However, when applying the ODS to a real gasoline, the ODS conversion rate decreased to only 32%, suggesting a strong inhibiting effect of gasoline composition on ODS. The ODS studies in different model fuels suggested that the inhibiting effect can be ascribed to the competitive adsorption and oxidation with the presence of the alkenes and alkylated aromatic hydrocarbons in real gasoline. The active pi-electrons in alkenes and alkyl groups in alkylated aromatic hydrocarbons may react with polyoxoperoxo species or peroxo-metallate complexes formed by phosphotungstic acid–H{sub 2}O{sub 2} interaction. Additionally, it was indicated that the ODS selectivity followed the order of benzothiophene > trimethylthiophene > dimethylthiophene ∼ methylthiophene > thiophene, suggesting the partial charge on the electron-rich sulfur atom may play a decisive role for its oxidation reactivity. To mitigate the inhibiting effect of gasoline composition on ODS, we propose (a) implementation of selective separation–oxidation processes; (b) choice of suitable selective oxidants; (c) optimization of selective ODS reaction temperature, etc. to improve ODS selectivity for real gasoline desulfurization applications.}
doi = {10.1016/J.APENERGY.2013.06.047}
journal = []
volume = {113}
journal type = {AC}
place = {United Kingdom}
year = {2014}
month = {Jan}
}