Large-pore silica spheres as support for samarium-coordinated undecamolybdophosphate: Oxidative desulfurization of diesels

A novel composite has been prepared through the immobilization of the Keggin sandwich-type [Sm (PMo11O39)(2)](11-) anion (SmPOM) on large-pore silica spheres previously functionalized with trimethylammonium groups (TMA). The resulting SmPOM@TMA-LPMS material has been evaluated as heterogeneous catal...

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Detalhes bibliográficos
Autor principal: Mirante, Fátima (author)
Outros Autores: Alves, Ana C. (author), Julião, Diana (author), Almeida, Pedro L. (author), Gago, S. (author), Valença, Rita (author), Ribeiro, Jorge (author), De Castro, Baltazar (author), Granadeiro, Carlos (author), Balula, Salete (author)
Formato: article
Idioma:eng
Publicado em: 2020
Assuntos:
Texto completo:http://hdl.handle.net/10400.21/11015
País:Portugal
Oai:oai:repositorio.ipl.pt:10400.21/11015
Descrição
Resumo:A novel composite has been prepared through the immobilization of the Keggin sandwich-type [Sm (PMo11O39)(2)](11-) anion (SmPOM) on large-pore silica spheres previously functionalized with trimethylammonium groups (TMA). The resulting SmPOM@TMA-LPMS material has been evaluated as heterogeneous catalyst in a biphasic desulfurization 1:1 diesel/extraction solvent system using H2O2 as oxidant. Preliminary experiments were conducted with different extraction solvents, acetonitrile and [BMIM]PF6 ionic liquid. The optimized extractive and catalytic oxidative desulfurization system (ECODS) with [BMIM]PF6 was able to reach complete sulfur removal from a model diesel containing 2100 ppm S in just 60 min (10 min of initial extraction + 50 min of catalytic step). The reutilization of catalyst and extraction phase has been successfully performed without loss of desulfurization efficiency in consecutive cycles, turning the process more sustainable and cog-effective. The remarkable results with simulated diesel have motivated the application of the catalyst in the desulfurization of untreated real diesel and 74% of efficiency was achieved after only 2 h for three consecutive cycles.