Simultaneous sulfur and nitrogen removal from fuel combining activated porous MIL-100(Fe) catalyst and sustainable solvents

resumo

The high costs associated with commercially available desulfurization technologies in the refinery industry urge for the development of novel, highly efficient and sustainable alternative processes. On the other hand, the presence of nitrogen compounds significantly decreases the efficiency of the process. Therefore, effective alternative methodologies capable of removing simultaneously sulfur and nitrogen compounds from fuels under economic and sustainable procedures are desirable and needed for the petroleum industry. This work reports a sustainable catalytic process that conciliates oxidation and liquid-liquid extraction to efficiently remove sulfur and nitrogen from fuels. The effective catalytic oxidation was achieved by using a MIL-100(Fe)-based composite encapsulating the phosphomolybdic acid (PMo12) active center. Complete desulfurization of a multicomponent model fuel containing the most refractory sulfur and nitrogen compounds was achieved after only 30 min. Also, the nitrogen compounds were able to be removed after this short period, mainly by extraction using strategic solvents. The S/N removal process was faster when the expensive ionic liquid [BMIM]PF6 was replaced by the cost-effective ethanol. Furthermore, the catalyst could be reused in several consecutive desulfurization and denitrogenation cycles, as well as the ethanol extraction solvent was reused for at least four cycles without loss of efficiency.

palavras-chave

METAL-ORGANIC FRAMEWORK; OXIDATIVE DESULFURIZATION; LIQUID; POLYOXOMETALATE; ANION

categoria

Chemistry; Engineering

autores

Silva, DF; Faria, RG; Santos-Vieira, I; Cunha-Silva, L; Granadeiro, CM; Balula, SS

Grupos

G1 - Materiais Porosos e Nanossistemas

Projectos

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

agradecimentos

This research work received financial support from Portuguese national funds (FCT/MCTES, Fundacao para a Ciencia e Tecnologia and Ministerio da Ciencia, Tecnologia e Ensino Superior) through the strategic project UIDB/50006/2020 (for LAQV-REQUIMTE), and also from the European Union (FEDER funds through COMPETE POCI-01-0145-FEDER-031983). This work was partially developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020, UIDP/50011/2020 & amp; LA/P/0006/2020, financed by national funds through the FCT/MCTES (PIDDAC). The position held by ISV (Ref. 197_97_ARH-2018) was funded by national funds (OE), through FCT, I. P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of article 23 of the Decree-Law 57/2016 of 29 August, changed by Law 57/2017 of 19 July. LCS, CMG and SSB thank FCT/MCTES for funding through the Individual Call to Scientific Employment Stimulus (Ref. CEECIND/00793/2018, Ref. 2022.02651.CEECIND, and Ref. CEECIND/03877/2018, respectively). DFS and RF thanks FCT/MCTES and ESF (European Social Fund) through POCH (Programa Operacional Capital Humano) for their PhD grants (Refs. 2022.14787. BD and UI/BD/151277/2021, respectively).