resumo
Highly efficient, deep desulfurization of a multi-component model diesel containing benzothiophene (BT), dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) has been achieved by using the peroxophosphomolybdate [(n-C4H9)(4)N](3)(PO4[MoO(O-2)(2)](4)} (Q(3)PMo(4)) directly as catalyst, and aqueous H2O2 as oxidant. Q(3)PMo(4) behaves as a heterogeneous catalyst in the complete oxidation of the various sulfur compounds to the corresponding sulfones within 3 h at 70 degrees C, using a relatively low H2O2/S molar ratio of 3.7, and could be recycled for ten times with only a minimal decrease in activity. A study was performed to adapt the catalyst Q(3)PMo(4) for the removal of sulfur from a real untreated diesel while maintaining a low, economically desirable, H2O2/S molar ratio of 3.7. The highest desulfurization performance was achieved in the presence of an extraction solvent during the catalytic oxidative stage, reinforced by two extraction steps before and after sulfur oxidation. Under these conditions, the sulfur content of the real diesel was reduced from 2300 to 500 ppm (78% desulfurization efficiency) after 3 h.
palavras-chave
CAMBRIDGE STRUCTURAL DATABASE; ULTRA-DEEP DESULFURIZATION; GAS OIL; FUELS; COMPLEXES; MODEL; MOLYBDENUM; EXTRACTION; REACTIVITY; KINETICS
categoria
Chemistry; Environmental Sciences & Ecology
autores
Juliao, D; Gomes, AC; Cunha-Silva, L; Valenca, R; Ribeiro, JC; Pillinger, M; de Castro, B; Goncalves, IS; Balula, SS
nossos autores
Ana Catarina Costa Gomes Alves
Investigador Auxiliar
Diana Julião
Estudante de doutoramento
Isabel Maria de Sousa Gonçalves
Professor associado
Martyn Pillinger
Investigador Principalagradecimentos
This work was partly funded through the projects REQUIMTE-LAQV within the scope of the projects UID/QUI/50006/2019 (REQUIMTE/LAQV) and CICECO -Aveiro Institute of Materials (FCT Ref. UID/CTM/50011/2019), both institutions were financed by national funds through the FCT/MCTES and when appropriate co-financed by FEDER (Fundo Europeu de Desenvolvimento Regional) under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for personal grants to D.J. (SFRH/BD/102783/2014) and L.C.-S. (SFRH/BPD/111899/2015) co-funded by MCTES and the European Social Fund through the program POPH of QREN.