Oxidative denitrogenation of a simulated fuel under a biphasic green system
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abstract
Este trabalho trata da desnitrificação catalítica de um combustível simulado (quinolina (QN) em
2,2,4-trimetilpentano) por oxidação com peróxido de hidrogénio em meio bifásico. Como catalisadores, foram
utilizados três materiais: (i) ferro suportado em alumina (Fe/Al2O3) obtido por sol-gel, (ii) nanotubos de
carbono (CNT) produzidos através da deposição química em fase de vapor de propileno (PP) sobre o
catalisador anterior (Fe/Al2O3), e (iii) os CNT fornecidos pela Sigma Aldrich. A contribuição da adsorção e da
extração foi avaliada, sendo ambas consideradas desprezáveis ou pouco efetivas para a remoção da QN. O
desempenho de cada material foi analisado em testes de reação de 4 h, a 80 °C, através da monitorização da
degradação de H2O2 e da concentração de QN em meio oleoso e aquoso. Como resultados, todos os materiais
utilizados atenderam ao objetivo proposto, sendo 100% da QN removida da fase oleosa nos ensaios de
oxidação bifásica. Em resumo, todos os catalisadores produzidos foram eficientes no processo proposto e são
comparáveis ao desempenho obtido pelo CNT comercial
This work deals with the catalytic denitrogenation of a simulated fuel (quinoline (QN) in
2,2,4-trimethylpentane) by oxidation with hydrogen peroxide in a biphasic medium. As catalysts, three
materials were used (i) iron supported on alumina (Fe/Al2O3) obtained by sol-gel, carbon nanotubes (CNT)
produced by chemical vapor deposition of propylene (PP) growth on the previous catalyst (Fe/Al2O3) and (iii)
a commercial sample of CNT supplied by Sigma Aldrich. The contribution of adsorption and extraction was
also assessed, both being considered negligible or ineffective for the removal of QN. The performance of each
catalyst was analysed in 4 h reaction tests, at 80 °C, by monitoring the degradation of H2O2 and the
concentration of QN in the oily and aqueous media. As a result, all catalysts used met the proposed objective,
with 100% of QN being removed from the oily phase in the biphasic oxidation tests. In summary, all the
catalysts produced were efficient in the proposed process and are comparable to the performance obtained by
the commercial CNT sample.
This work was financially supported by project
“PLASTIC_TO_FUEL&MAT – Upcycling Waste
Plastics into Fuel and Carbon Nanomaterials”
(PTDC/EQU-EQU/31439/2017), LA/P/0045/2020
(ALiCE), UIDB/50020/2020 and
UIDP/50020/2020 (LSRE-LCM), funded by
national funds through FCT/MCTES (PIDDAC)
and CIMO (UIDB/00690/2020) through FEDER
under Program PT2020. Fernanda F. Roman
acknowledges the national funding by FCT,
Foundation for Science and Technology, and FSE,
European Social Fund, through the individual
research grant SFRH/BD/143224/2019. Jose L.
Diaz de Tuesta acknowledges the financial support
through the program of “Atracción al Talento” of
“Comunidad de Madrid” (Spain) for the individual
research grant 2020-T2/AMB-19836.