Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization

Fátima Mirante; Neide Gomes; Luís C. Branco; Luís Cunha-Silva; Pedro L. Almeida; Martyn Pillinger; Sandra Gago; Carlos M. Granadeiro; Salete S. Balula

doi:10.1016/j.micromeso.2018.07.036

Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization

Fátima Mirante, Neide Gomes, Luís C. Branco, Luís Cunha-Silva, Pedro L. Almeida, Martyn Pillinger, Sandra Gago, Carlos M. Granadeiro, Salete S. Balula

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Abstract

Mesoporous silica nanoparticles (MSNs) strategically functionalized were used to immobilize a homogeneous polyoxomolybdate catalyst [PMo ₁₂ O ₄₀ ] ^3- (PMo ₁₂ ), active but unstable. The PMo ₁₂ @TBA-MSN composite (where TBA refers to surface-tethered tributylammonium groups) conferred high stability to the polyoxomolybdate catalytic center and displayed an increase in efficiency for the oxidative desulfurization (ECODS) of a diesel simulant under sustainable conditions (using H ₂ O ₂ as oxidant and an ionic liquid, [BMIM]PF ₆ , as solvent). Continuous reuse of the catalyst and ionic liquid solvent in consecutive ECODS cycles was successfully performed, avoiding the production of residual wastes. The performance of the PMo ₁₂ @TBA-MSN catalyst improved upon its reuse, leading to complete desulfurization of a multicomponent model diesel containing benzothiophene derivatives after just 1 h of the catalytic stage of the process. The robust nature of the supported catalyst was indicated by characterization of the recovered solid which showed retention of the structural and chemical integrities.

Original language	English
Pages (from-to)	163-171
Number of pages	9
Journal	Microporous and Mesoporous Materials
Volume	275
DOIs	https://doi.org/10.1016/j.micromeso.2018.07.036
Publication status	Published - 1 Feb 2019

Keywords

Fuels
Heterogeneous catalysis
Mesoporous silica nanoparticles
Oxidative desulfurization
Polyoxomolybdate

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10.1016/j.micromeso.2018.07.036Licence: CC BY-NC-ND

Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurizationAccepted author manuscript, 1.39 MBLicence: CC BY-NC-ND

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@article{a7ddf1cace2b46a4b2abebd4f370e673,

title = "Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization",

abstract = " Mesoporous silica nanoparticles (MSNs) strategically functionalized were used to immobilize a homogeneous polyoxomolybdate catalyst [PMo 12 O 40 ] 3- (PMo 12 ), active but unstable. The PMo 12 @TBA-MSN composite (where TBA refers to surface-tethered tributylammonium groups) conferred high stability to the polyoxomolybdate catalytic center and displayed an increase in efficiency for the oxidative desulfurization (ECODS) of a diesel simulant under sustainable conditions (using H 2 O 2 as oxidant and an ionic liquid, [BMIM]PF 6 , as solvent). Continuous reuse of the catalyst and ionic liquid solvent in consecutive ECODS cycles was successfully performed, avoiding the production of residual wastes. The performance of the PMo 12 @TBA-MSN catalyst improved upon its reuse, leading to complete desulfurization of a multicomponent model diesel containing benzothiophene derivatives after just 1 h of the catalytic stage of the process. The robust nature of the supported catalyst was indicated by characterization of the recovered solid which showed retention of the structural and chemical integrities. ",

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

author = "F{\'a}tima Mirante and Neide Gomes and Branco, {Lu{\'i}s C.} and Lu{\'i}s Cunha-Silva and Almeida, {Pedro L.} and Martyn Pillinger and Sandra Gago and Granadeiro, {Carlos M.} and Balula, {Salete S.}",

note = "info:eu-repo/grantAgreement/FCT/5876/136099/PT# info:eu-repo/grantAgreement/FCT/5876/147332/PT# This work was partly funded through the projects REQUIMTE-LAQV, POCI-01-0145-FEDER-007265 [FCT (Fundacao para a Ciencia e a Tecnologia) Ref. UID/QUI/50006/2013] and CICECO -Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT Ref. UID/CTM/50011/2013), financed by national funds through the FCT/MEC and when appropriate co-financed by FEDER under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for post-doctoral grants to C.M.G. (SFRH/BPD/109253/2015) and L.C.S. (SFRH/BPD/111899/2015) co-funded by MCTES and the European Social Fund through the program POPH of QREN. ",

year = "2019",

month = feb,

day = "1",

doi = "10.1016/j.micromeso.2018.07.036",

language = "English",

volume = "275",

pages = "163--171",

journal = "Microporous and Mesoporous Materials",

issn = "1387-1811",

publisher = "Elsevier Science B.V., Inc",

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TY - JOUR

T1 - Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization

AU - Mirante, Fátima

AU - Gomes, Neide

AU - Branco, Luís C.

AU - Cunha-Silva, Luís

AU - Almeida, Pedro L.

AU - Pillinger, Martyn

AU - Gago, Sandra

AU - Granadeiro, Carlos M.

AU - Balula, Salete S.

N1 - info:eu-repo/grantAgreement/FCT/5876/136099/PT# info:eu-repo/grantAgreement/FCT/5876/147332/PT# This work was partly funded through the projects REQUIMTE-LAQV, POCI-01-0145-FEDER-007265 [FCT (Fundacao para a Ciencia e a Tecnologia) Ref. UID/QUI/50006/2013] and CICECO -Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT Ref. UID/CTM/50011/2013), financed by national funds through the FCT/MEC and when appropriate co-financed by FEDER under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for post-doctoral grants to C.M.G. (SFRH/BPD/109253/2015) and L.C.S. (SFRH/BPD/111899/2015) co-funded by MCTES and the European Social Fund through the program POPH of QREN.

PY - 2019/2/1

Y1 - 2019/2/1

N2 - Mesoporous silica nanoparticles (MSNs) strategically functionalized were used to immobilize a homogeneous polyoxomolybdate catalyst [PMo 12 O 40 ] 3- (PMo 12 ), active but unstable. The PMo 12 @TBA-MSN composite (where TBA refers to surface-tethered tributylammonium groups) conferred high stability to the polyoxomolybdate catalytic center and displayed an increase in efficiency for the oxidative desulfurization (ECODS) of a diesel simulant under sustainable conditions (using H 2 O 2 as oxidant and an ionic liquid, [BMIM]PF 6 , as solvent). Continuous reuse of the catalyst and ionic liquid solvent in consecutive ECODS cycles was successfully performed, avoiding the production of residual wastes. The performance of the PMo 12 @TBA-MSN catalyst improved upon its reuse, leading to complete desulfurization of a multicomponent model diesel containing benzothiophene derivatives after just 1 h of the catalytic stage of the process. The robust nature of the supported catalyst was indicated by characterization of the recovered solid which showed retention of the structural and chemical integrities.

AB - Mesoporous silica nanoparticles (MSNs) strategically functionalized were used to immobilize a homogeneous polyoxomolybdate catalyst [PMo 12 O 40 ] 3- (PMo 12 ), active but unstable. The PMo 12 @TBA-MSN composite (where TBA refers to surface-tethered tributylammonium groups) conferred high stability to the polyoxomolybdate catalytic center and displayed an increase in efficiency for the oxidative desulfurization (ECODS) of a diesel simulant under sustainable conditions (using H 2 O 2 as oxidant and an ionic liquid, [BMIM]PF 6 , as solvent). Continuous reuse of the catalyst and ionic liquid solvent in consecutive ECODS cycles was successfully performed, avoiding the production of residual wastes. The performance of the PMo 12 @TBA-MSN catalyst improved upon its reuse, leading to complete desulfurization of a multicomponent model diesel containing benzothiophene derivatives after just 1 h of the catalytic stage of the process. The robust nature of the supported catalyst was indicated by characterization of the recovered solid which showed retention of the structural and chemical integrities.

KW - Fuels

KW - Heterogeneous catalysis

KW - Mesoporous silica nanoparticles

KW - Oxidative desulfurization

KW - Polyoxomolybdate

UR - http://www.scopus.com/inward/record.url?scp=85052642414&partnerID=8YFLogxK

U2 - 10.1016/j.micromeso.2018.07.036

DO - 10.1016/j.micromeso.2018.07.036

M3 - Article

AN - SCOPUS:85052642414

SN - 1387-1811

VL - 275

SP - 163

EP - 171

JO - Microporous and Mesoporous Materials

JF - Microporous and Mesoporous Materials

ER -

Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization

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Keywords

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