Polyoxomolybdate based ionic-liquids as active catalysts for oxidative desulfurization of simulated diesel

Fatima Mirante; Neide Gomes; Marta C. Corvo; Sandra Gago; Salete S. Balula

doi:10.1016/j.poly.2019.06.019

Polyoxomolybdate based ionic-liquids as active catalysts for oxidative desulfurization of simulated diesel

Fatima Mirante, Neide Gomes, Marta C. Corvo, Sandra Gago, Salete S. Balula

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Abstract

This work compares the stability and the catalytic efficiency of different ionic liquid phosphomolybdates ([BPy]₃[PMo₁₂O₄₀] and [BMIM]₃[PMo₁₂O₄₀]) with a cationic (propylpyridinium) functionalized mesoporous silica nanoparticle composite (PMo₁₂O₄₀@PPy-MSN). These were used as solid catalysts for the oxidative desulfurization of a multicomponent model diesel using hydrogen peroxide as oxidant and a polar immiscible extraction solvent. Ionic liquid ([BMIM][PF₆] was successfully used as solvent to extract sulfur compounds from model diesel. The ionic liquid phosphomolybdates showed partial solubility in the ionic liquid phase, occurring some decomposition of their Keggin structure in the soluble reaction media, probably caused by their interaction with oxidant. On the other hand, the phosphomolybdate composite PMo₁₂O₄₀@PPy-MSN presented high structural stability and only negligible leaching occurrence after various consecutive reaction cycles. The model diesel was near complete desulfurized after 3 h and consecutive desulfurization cycles were performed without loss of activity. Therefore, the immobilization of Keggin phosphomolybdate structure [PMo₁₂O₄₀]³⁻ using cationic propylpyridinium silica nanoparticle is an assertive strategy to produce stable and active heterogeneous catalysts.

Original language	English
Pages (from-to)	762-770
Number of pages	9
Journal	Polyhedron
Volume	170
DOIs	https://doi.org/10.1016/j.poly.2019.06.019
Publication status	Published - 15 Sept 2019

Keywords

Fuels
Heterogeneous catalysis
Mesoporous silica nanoparticles
Oxidative desulfurization
Polyoxomolybdate

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10.1016/j.poly.2019.06.019Licence: CC BY-NC-ND

Polyoxomolybdate based Ionic-Liquids as Active Catalysts for OxidativeAccepted author manuscript, 2.24 MBLicence: CC BY-NC-ND

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@article{b6688f9963d94a219c1acdce19a759d8,

title = "Polyoxomolybdate based ionic-liquids as active catalysts for oxidative desulfurization of simulated diesel",

abstract = "This work compares the stability and the catalytic efficiency of different ionic liquid phosphomolybdates ([BPy]3[PMo12O40] and [BMIM]3[PMo12O40]) with a cationic (propylpyridinium) functionalized mesoporous silica nanoparticle composite (PMo12O40@PPy-MSN). These were used as solid catalysts for the oxidative desulfurization of a multicomponent model diesel using hydrogen peroxide as oxidant and a polar immiscible extraction solvent. Ionic liquid ([BMIM][PF6] was successfully used as solvent to extract sulfur compounds from model diesel. The ionic liquid phosphomolybdates showed partial solubility in the ionic liquid phase, occurring some decomposition of their Keggin structure in the soluble reaction media, probably caused by their interaction with oxidant. On the other hand, the phosphomolybdate composite PMo12O40@PPy-MSN presented high structural stability and only negligible leaching occurrence after various consecutive reaction cycles. The model diesel was near complete desulfurized after 3 h and consecutive desulfurization cycles were performed without loss of activity. Therefore, the immobilization of Keggin phosphomolybdate structure [PMo12O40]3− using cationic propylpyridinium silica nanoparticle is an assertive strategy to produce stable and active heterogeneous catalysts.",

keywords = "Fuels, Heterogeneous catalysis, Mesoporous silica nanoparticles, Oxidative desulfurization, Polyoxomolybdate",

author = "Fatima Mirante and Neide Gomes and Corvo, {Marta C.} and Sandra Gago and Balula, {Salete S.}",

note = "info:eu-repo/grantAgreement/FCT/5876/147333/PT# This work was partly funded through the Associate Laboratory for Green Chemistry- LAQV which is financed by national funds from FCT/MCTES (POCI-01-0145-FEDER-007265, UID/QUI/50006/2019) and CENIMAT, I3N (POCI-01-0145-FEDER-007688, UID/CTM/50025/2013), also financed by national funds through the FCT/MCTES, and when appropriate co-financed by the Fundo Europeu de Desenvolvimento Regional (FEDER) under the PT2020 Partnership Agreement. This work is funded by national funds (OE), through FCT – Funda{\c c}{\~a}o para a Ci{\^e}ncia e a Tecnologia. European Social Fund through the program POPH of QREN. The authors also acknowledge the Portuguese Nuclear Magnetic Resonance Network (PTNMR).",

year = "2019",

month = sep,

day = "15",

doi = "10.1016/j.poly.2019.06.019",

language = "English",

volume = "170",

pages = "762--770",

journal = "Polyhedron",

issn = "0277-5387",

publisher = "Elsevier",

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TY - JOUR

T1 - Polyoxomolybdate based ionic-liquids as active catalysts for oxidative desulfurization of simulated diesel

AU - Mirante, Fatima

AU - Gomes, Neide

AU - Corvo, Marta C.

AU - Gago, Sandra

AU - Balula, Salete S.

N1 - info:eu-repo/grantAgreement/FCT/5876/147333/PT# This work was partly funded through the Associate Laboratory for Green Chemistry- LAQV which is financed by national funds from FCT/MCTES (POCI-01-0145-FEDER-007265, UID/QUI/50006/2019) and CENIMAT, I3N (POCI-01-0145-FEDER-007688, UID/CTM/50025/2013), also financed by national funds through the FCT/MCTES, and when appropriate co-financed by the Fundo Europeu de Desenvolvimento Regional (FEDER) under the PT2020 Partnership Agreement. This work is funded by national funds (OE), through FCT – Fundação para a Ciência e a Tecnologia. European Social Fund through the program POPH of QREN. The authors also acknowledge the Portuguese Nuclear Magnetic Resonance Network (PTNMR).

PY - 2019/9/15

Y1 - 2019/9/15

N2 - This work compares the stability and the catalytic efficiency of different ionic liquid phosphomolybdates ([BPy]3[PMo12O40] and [BMIM]3[PMo12O40]) with a cationic (propylpyridinium) functionalized mesoporous silica nanoparticle composite (PMo12O40@PPy-MSN). These were used as solid catalysts for the oxidative desulfurization of a multicomponent model diesel using hydrogen peroxide as oxidant and a polar immiscible extraction solvent. Ionic liquid ([BMIM][PF6] was successfully used as solvent to extract sulfur compounds from model diesel. The ionic liquid phosphomolybdates showed partial solubility in the ionic liquid phase, occurring some decomposition of their Keggin structure in the soluble reaction media, probably caused by their interaction with oxidant. On the other hand, the phosphomolybdate composite PMo12O40@PPy-MSN presented high structural stability and only negligible leaching occurrence after various consecutive reaction cycles. The model diesel was near complete desulfurized after 3 h and consecutive desulfurization cycles were performed without loss of activity. Therefore, the immobilization of Keggin phosphomolybdate structure [PMo12O40]3− using cationic propylpyridinium silica nanoparticle is an assertive strategy to produce stable and active heterogeneous catalysts.

AB - This work compares the stability and the catalytic efficiency of different ionic liquid phosphomolybdates ([BPy]3[PMo12O40] and [BMIM]3[PMo12O40]) with a cationic (propylpyridinium) functionalized mesoporous silica nanoparticle composite (PMo12O40@PPy-MSN). These were used as solid catalysts for the oxidative desulfurization of a multicomponent model diesel using hydrogen peroxide as oxidant and a polar immiscible extraction solvent. Ionic liquid ([BMIM][PF6] was successfully used as solvent to extract sulfur compounds from model diesel. The ionic liquid phosphomolybdates showed partial solubility in the ionic liquid phase, occurring some decomposition of their Keggin structure in the soluble reaction media, probably caused by their interaction with oxidant. On the other hand, the phosphomolybdate composite PMo12O40@PPy-MSN presented high structural stability and only negligible leaching occurrence after various consecutive reaction cycles. The model diesel was near complete desulfurized after 3 h and consecutive desulfurization cycles were performed without loss of activity. Therefore, the immobilization of Keggin phosphomolybdate structure [PMo12O40]3− using cationic propylpyridinium silica nanoparticle is an assertive strategy to produce stable and active heterogeneous catalysts.

KW - Fuels

KW - Heterogeneous catalysis

KW - Mesoporous silica nanoparticles

KW - Oxidative desulfurization

KW - Polyoxomolybdate

UR - http://www.scopus.com/inward/record.url?scp=85068838044&partnerID=8YFLogxK

U2 - 10.1016/j.poly.2019.06.019

DO - 10.1016/j.poly.2019.06.019

M3 - Article

AN - SCOPUS:85068838044

SN - 0277-5387

VL - 170

SP - 762

EP - 770

JO - Polyhedron

JF - Polyhedron

ER -

Polyoxomolybdate based ionic-liquids as active catalysts for oxidative desulfurization of simulated diesel

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Keywords

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