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Mesoporous nanosilica-supported polyoxomolybdate as catalysts for sustainable desulfurization

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Resumo: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.
Autores principais:Mirante, Fátima
Outros Autores:Gomes, Neide; Branco, Luís C.; Cunha-Silva, Luís; Almeida, Pedro L.; Pillinger, Martyn; Gago, Sandra; Granadeiro, Carlos M.; Balula, Salete S.
Assunto:Fuels Heterogeneous catalysis Mesoporous silica nanoparticles Oxidative desulfurization Polyoxomolybdate General Chemistry General Materials Science Condensed Matter Physics Mechanics of Materials
Ano:2019
País:Portugal
Tipo de documento:artigo
Tipo de acesso:acesso aberto
Instituição associada:Universidade Nova de Lisboa
Idioma:inglês
Origem:Repositório Institucional da UNL
Descrição
Resumo: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.