resumo
An ionic lamellar coordination polymer based on a flexible triphosphonic acid linker, [Gd(H(4)nmp)(H2O)(2)]Cl2H2O (1) (H(6)nmp stands for nitrilo(trimethylphosphonic) acid), presents high efficiency to remove sulfur and nitrogen pollutant compounds from model diesel. Its oxidative catalytic performance was investigated using single sulfur (1-BT, DBT, 4-MDBT and 4,6-DMDBT, 2350 ppm of S) and nitrogen (indole and quinolone, 400 ppm of N) model diesels and further, using multicomponent S/N model diesel. Different methodologies of preparation followed (microwave, one-pot, hydrothermal) originated small morphological differences that did not influenced the catalytic performance of catalyst. Complete desulfurization and denitrogenation were achieved after 2 h using single model diesels, an ionic liquid as extraction solvent ([BMIM]PF6) and H(2)O(2)as oxidant. Simultaneous desulfurization and denitrogenation processes revealed that the nitrogen compounds are more easily removed from the diesel phase to the [BMIM]PF(6)phase and consequently, faster oxidized than the sulfur compounds. The lamellar catalyst showed a high recycle capacity for desulfurization. The reusability of the diesel/H2O2/[BMIM]PF(6)system catalyzed by lamellar catalyst was more efficient for denitrogenation than for desulfurization process using a multicomponent model diesel. This behavior is not associated with the catalyst performance but it is mainly due to the saturation of S/N compounds in the extraction phase.
palavras-chave
METAL-ORGANIC FRAMEWORKS; OXIDATIVE DESULFURIZATION; DIESEL; EXTRACTION; POLYOXOMETALATE; DENITROGENATION; PERFORMANCE; EMISSIONS; VEHICLES; SOLVENT
categoria
Chemistry
autores
Mirante, F; Mendes, RF; Paz, FAA; Balula, SS
nossos autores
Filipe Alexandre Almeida Paz
Investigador Principal
Ricardo Faria Mendes
Investigador Júnioragradecimentos
This work was partly funded through the project REQUIMTE-LAQV (Ref. UID/QUI/50006/2019) and the project GlyGold, PTDC/CTM-CTM/31983/2017, and partially developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020& UIDP/50011/2020, LAQV-REQUIMTE (UIDB/50006/2020) and CQE (UIDB/00100/2020) research units, financed by national funds through the FCT/MCTES (Fundacao para a Ciencia e a Tecnologia/Ministerio da Ciencia, Tecnologia e Ensino Superior) and when appropriate co-financed by FEDER (Fundo Europeu de Desenvolvimento Regional) under the PT2020 Partnership Agreement. FCT is also gratefully acknowledged for the Junior Research Position CEECIND/00553/2017 (to RFM).