High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil

Thalgaspitiya, Wimalika R.K.; Kankanam Kapuge, Tharindu; He, Junkai; Rathnayake, Dinithi; Suib, Steven L.

doi:10.1016/j.apmt.2020.100616

Title: High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil

Abstract

Mesoporous, multi-valent tungsten oxide with high surface area (209 m²/g) is synthesized via a novel metal dissolution coupled with reverse micelle formation approach. Mesoporous tungsten oxide with highest surface area reported is obtained by this method. The material is used as an excellent heterogeneous catalyst for the oxidation of organosulfur compounds present in crude oil. The complete oxidation of dibenzothiophene was observed with excellent yield (>99%) within 15 min at room temperature (20 °C). The catalyst is reusable up to 5 reaction cycles without losing significant activity. A green oxidant, H₂O₂ is used and the reaction mechanism involves the activation of peroxo species by W⁶⁺. The oxidation activity decreases in the order of DBT > 4,6-DMDBT > 1-BT due to the changes in the electronic environment of sulfur and steric effects.

Authors:

Thalgaspitiya, Wimalika R.K. ^[1]; Kankanam Kapuge, Tharindu ^[1];

^[2]; Rathnayake, Dinithi ^[1];

^[2]

Univ. of Connecticut, Storrs, CT (United States)
Univ. of Connecticut, Storrs, CT (United States). Inst. of Materials Science

Publication Date:: Sun Mar 08 00:00:00 EST 2020

Research Org.:: Univ. of Connecticut, Storrs, CT (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE

OSTI Identifier:: 1775558

Alternate Identifier(s):: OSTI ID: 1603746

Grant/Contract Number:: FG02-86ER13622

Resource Type:: Accepted Manuscript

Journal Name:: Applied Materials Today

Additional Journal Information:: Journal Volume: 19; Journal ID: ISSN 2352-9407

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Thalgaspitiya, Wimalika R.K., Kankanam Kapuge, Tharindu, He, Junkai, Rathnayake, Dinithi, and Suib, Steven L. High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil.  United States: N. p., 2020. 
Web.  doi:10.1016/j.apmt.2020.100616.

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                    Thalgaspitiya, Wimalika R.K., Kankanam Kapuge, Tharindu, He, Junkai, Rathnayake, Dinithi, & Suib, Steven L. High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil.  United States.  https://doi.org/10.1016/j.apmt.2020.100616

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                    Thalgaspitiya, Wimalika R.K., Kankanam Kapuge, Tharindu, He, Junkai, Rathnayake, Dinithi, and Suib, Steven L. Sun .  
"High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil".  United States.  https://doi.org/10.1016/j.apmt.2020.100616.  https://www.osti.gov/servlets/purl/1775558.

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@article{osti_1775558,

  title        = {High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil},

  author       = {Thalgaspitiya, Wimalika R.K. and Kankanam Kapuge, Tharindu and He, Junkai and Rathnayake, Dinithi and Suib, Steven L.},

  abstractNote = {Mesoporous, multi-valent tungsten oxide with high surface area (209 m2/g) is synthesized via a novel metal dissolution coupled with reverse micelle formation approach. Mesoporous tungsten oxide with highest surface area reported is obtained by this method. The material is used as an excellent heterogeneous catalyst for the oxidation of organosulfur compounds present in crude oil. The complete oxidation of dibenzothiophene was observed with excellent yield (>99%) within 15 min at room temperature (20 °C). The catalyst is reusable up to 5 reaction cycles without losing significant activity. A green oxidant, H2O2 is used and the reaction mechanism involves the activation of peroxo species by W6+. The oxidation activity decreases in the order of DBT > 4,6-DMDBT > 1-BT due to the changes in the electronic environment of sulfur and steric effects.},

  doi          = {10.1016/j.apmt.2020.100616},

  journal      = {Applied Materials Today},

  number       = ,

  volume       = 19,

  place        = {United States},

  year         = {Sun Mar 08 00:00:00 EST 2020},

  month        = {Sun Mar 08 00:00:00 EST 2020}

}

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https://doi.org/10.1016/j.apmt.2020.100616

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Title: High surface area mesoporous tungsten oxide for fast, green oxidation of organosulfur compounds in crude oil

Abstract

Citation Formats

Highly Ordered Mesoporous Tungsten Oxides with a Large Pore Size and Crystalline Framework for H 2 S Sensing journal, July 2014

Synthesis and electrochromic properties of mesoporous tungsten oxide journal, January 2001

Electrochromic and optical properties of mesoporous tungsten oxide films journal, July 2002

Scalable synthesis of improved nanocrystalline, mesoporous tungsten oxide films with exceptional electrochromic performance journal, January 2015

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Structure and optical properties of mesoporous tungsten oxide journal, June 2005

Ordered Mesoporous Tungsten Suboxide Counter Electrode for Highly Efficient Iodine-Free Electrolyte-Based Dye-Sensitized Solar Cells journal, December 2012

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Catalytic oxidation of dibenzothiophene and thioanisole by a diiron(III) complex and hydrogen peroxide journal, January 2015

Desulfurization of model diesel by extraction/oxidation using a zinc-substituted polyoxometalate as catalyst under homogeneous and heterogeneous (MIL-101(Cr) encapsulated) conditions journal, March 2015

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Oxidative removal of dibenzothiophene and related sulfur compounds from fuel oils under pressurized oxygen at room temperature with hydrogen peroxide and a phosphorus-free catalyst: sodium decatungstate journal, October 2018

Desulfurization of fuel oil by oxidation and extraction. 2. Kinetic modeling of oxidation reaction journal, March 1990

Oxidative desulfurization of dibenzothiophene and diesel over [Bmim]3PMo12O40 journal, April 2011

Oxidative desulfurization of dibenzothiophene with molecular oxygen using emulsion catalysis journal, January 2007

V-, Mo- and W-containing layered double hydroxides as effective catalysts for mild oxidation of thioethers and thiophenes with H2O2 journal, October 2008

Mechanism and optimization for oxidative desulfurization of fuels catalyzed by Fenton-like catalysts in hydrophobic ionic liquid journal, February 2014

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journal, August 2018

Catalytic thiophene oxidation by groups 4 and 5 framework-substituted zeolites with hydrogen peroxide: Mechanistic and spectroscopic evidence for the effects of metal Lewis acidity and solvent Lewis basicity
journal, August 2018

Catalytic oxidation of dibenzothiophene and thioanisole by a diiron(III) complex and hydrogen peroxide
journal, January 2015

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journal, March 2015

Development of ultra-deep HDS catalyst for production of clean diesel fuels
journal, February 2006

An Overview of Hydrodesulfurization and Hydrodenitrogenation
journal, January 2004

Removal of Dibenzothiophene from Model Diesel by Adsorption on Carbon Aerogels for Fuel Cell Applications
journal, December 2003

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journal, October 2018

Desulfurization of fuel oil by oxidation and extraction. 2. Kinetic modeling of oxidation reaction
journal, March 1990

Oxidative desulfurization of dibenzothiophene and diesel over [Bmim]3PMo12O40
journal, April 2011

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journal, January 2007

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journal, October 2008

Mechanism and optimization for oxidative desulfurization of fuels catalyzed by Fenton-like catalysts in hydrophobic ionic liquid
journal, February 2014

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Catalytic kinetics of oxidative desulfurization with surfactant-type polyoxometalate-based ionic liquids
journal, February 2013

Extractive oxidative desulfurization of model oil/crude oil using KSF montmorillonite-supported 12-tungstophosphoric acid
journal, October 2016

Phosphotungestovanadate immobilized on PVA as an efficient and reusable nano catalyst for oxidative desulphurization of gasoline
journal, December 2015

Ultra-deep oxidative desulfurization of diesel fuel by the Mo/Al2O3-H2O2 system: The effect of system parameters on catalytic activity
journal, January 2008