scholarly journals Influence of UiO-66(Zr) Preparation Strategies in Its Catalytic Efficiency for Desulfurization Process

Materials ◽  
2019 ◽  
Vol 12 (18) ◽  
pp. 3009 ◽  
Author(s):  
Alexandre M. Viana ◽  
Susana O. Ribeiro ◽  
Baltazar de Castro ◽  
Salete S. Balula ◽  
Luís Cunha-Silva

Porous metal-organic framework (MOF) materials UiO-66(Zr) obtained by solvothermal and microwave advanced synthesis (MWAS) procedures were characterized, and their catalytic efficiency was investigated for oxidative desulfurization (ODS) processes using a multicomponent model diesel containing benzothiophene and dibenzothiophene derivatives. The preparation parameters as the cooling time after oven use in the solvothermal procedure, and also the reaction time in the MWAS method seemed to play an important role in the catalytic performance of the UiO-66(Zr) material, as well as in its recycle capacity. The material prepared by the solvothermal procedure with a fast cooling time showed the best catalytic performance (desulfurization efficiency of 99.5% after 3 h). However, the application of the UiO-66(Zr) material prepared by the MWAS method (desulfurization efficiency of 96% after 3 h) conciliated a higher number of advantages, such as shorter reaction time preparation (15 min) and high catalytic activity for a higher number of reaction cycles. The UiO-66(Zr) prepared by the MWAS method was used for the first time in an oxidative desulfurization process, and according to the catalytic results obtained (high recycle capacity and stability) and shorter reaction time preparation, seems to be a promising material for industrial application.

Molecules ◽  
2020 ◽  
Vol 25 (23) ◽  
pp. 5494
Author(s):  
Yan Gao ◽  
Fátima Mirante ◽  
Baltazar de Castro ◽  
Jianshe Zhao ◽  
Luís Cunha-Silva ◽  
...  

A peroxotungstate composite comprising the chromium terephthalate metal–organic framework MIL-101(Cr) and the Venturello peroxotungstate [PO4{WO(O2)2}4]3− (PW4) has been prepared by the impregnation method. The PW4@MIL-101(Cr) composite presents high catalytic efficiency for oxidative desulfurization of a multicomponent model diesel containing the most refractory sulfur compounds present in real fuels (2000 ppm of total S). The catalytic performance of this heterogeneous catalyst is similar to the corresponding homogeneous PW4 active center. Desulfurization efficiency of 99.7% was achieved after only 40 min at 70 °C using H2O2 as an oxidant and an ionic liquid as an extraction solvent ([BMIM]PF6, 2:1 model diesel/[BMIM]PF6). High recycling and reusing capacity was also found for PW4@MIL-101(Cr), maintaining its activity for consecutive oxidative desulfurization cycles. A comparison of the catalytic performance of this peroxotungstate composite with others previously reported tungstate@MIL-101(Cr) catalysts indicates that the presence of active oxygen atoms from the peroxo groups promotes a higher oxidative catalytic efficiency in a shorter reaction time.


RSC Advances ◽  
2016 ◽  
Vol 6 (99) ◽  
pp. 97399-97403 ◽  
Author(s):  
Rui Kuang ◽  
Luyi Zheng ◽  
Ethan Cottrill ◽  
Ning Pan ◽  
Yanhui Chi ◽  
...  

A hierarchical porous MOF nanocrystal, hpCuL (L = 2,4,6-tris(3,5-dicarboxylatephenylamino)-1,3,5-triazine) was prepared via a facile gel-aging process. This nanocomposite exhibits high catalytic activity and stability for the reduction of 4-nitrophenol.


Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 731
Author(s):  
Fátima Mirante ◽  
Ricardo F. Mendes ◽  
Filipe A. Almeida Paz ◽  
Salete S. Balula

An ionic lamellar coordination polymer based on a flexible triphosphonic acid linker, [Gd(H4nmp)(H2O)2]Cl2 H2O (1) (H6nmp 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 H2O2 as oxidant. Simultaneous desulfurization and denitrogenation processes revealed that the nitrogen compounds are more easily removed from the diesel phase to the [BMIM]PF6 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]PF6 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.


2021 ◽  
Author(s):  
Na Li ◽  
Zongwen Zhang ◽  
Jia-Ni Zhang ◽  
Yue Ma ◽  
Xiao-Yu Chen ◽  
...  

The Ti-based metal-organic framework (Ti-MOF) MIL-125 with tunable crystalline size in the range of ca. 50 nm to 1500 nm was synthesized by coordination modulation method using trans-cinnamic acid (CA)...


Molecules ◽  
2020 ◽  
Vol 25 (21) ◽  
pp. 4961
Author(s):  
Fátima Mirante ◽  
Baltazar de Castro ◽  
Carlos M. Granadeiro ◽  
Salete S. Balula

Two quaternary ammonium catalysts based on the monovacant polyoxotungstate ([PW11O39]7−, abbreviated as PW11) were prepared and characterized. The desulfurization performances of the PW11-based hybrids (of tetrabutylammonium and trimethyloctadecylammonium, abbreviated as TBA[PW11] and ODA[PW11], respectively), the corresponding potassium salt (K7PW11O39, abbreviated as KPW11) and the peroxo-compound (TBA-PO4[WO(O2)2], abbreviated as TBA[PW4]) were compared as catalysts for the oxidative desulfurization of a multicomponent model diesel (2000 ppm S). The oxidative desulfurization studies (ODS) were performed using solvent-free systems and aqueous H2O2 as oxidant. The nature of the cation in the PW11 catalyst showed to have an important influence on the catalytic performance. In fact, the PW11-hybrid catalysts showed higher catalytic efficiency than the peroxo-compound TBA[PW4], known as Venturello compound. TBA[PW11] revealed a remarkable desulfurization performance with 96.5% of sulfur compounds removed in the first 130 min. The reusability and stability of the catalyst were also investigated for ten consecutive ODS cycles without loss of activity. A treated clean diesel could be recovered without sulfur compounds by performing a final liquid/liquid extraction diesel/EtOH:H2O mixture (1:1) after the catalytic oxidative step.


CrystEngComm ◽  
2017 ◽  
Vol 19 (29) ◽  
pp. 4219-4226 ◽  
Author(s):  
Diana Julião ◽  
André D. S. Barbosa ◽  
Andreia F. Peixoto ◽  
Cristina Freire ◽  
Baltazar de Castro ◽  
...  

An emerging strategy to improve the performance of porous metal–organic framework (MOF) materials as heterogeneous catalysts is reported.


2012 ◽  
Vol 518-523 ◽  
pp. 878-883 ◽  
Author(s):  
Feng Xing Niu ◽  
Feng Fu ◽  
Xiao Ming Gao ◽  
Xue Mei Zhang ◽  
Yu Fei Wu

A type of visible light photocatalyst kaolin/Cu2O was prepared from kaolin, CuCO3·Cu(OH)2·XH2O, NaOH and C6H12O6 by means of hydrothermal method and was characterized by XRD, SEM and UV-vis. The desulfurization process for model fuel was studied based on a combination of photochemical reaction and liquid-liquid extraction. The effects of the doping of kaolin, volume of air, reaction time, and dosage of photocatalyst kaolin/Cu2O on the desulfurization efficiency were also investigated. When the load kaolin ratio of 20%, reaction time is 2 h, the volume of O2 is 150 mL·min-1, the amount of kaolin/Cu2O is 2 g·L-1 and solvent/oil ratio of 0.5, the desulfurization rate of model compound reached over 97 %.


2013 ◽  
Vol 30 (2) ◽  
pp. 314-320 ◽  
Author(s):  
Ling Tang ◽  
Guangqing Luo ◽  
Lihua Kang ◽  
Mingyuan Zhu ◽  
Bin Dai

2022 ◽  
Vol 9 ◽  
Author(s):  
Yutong Zhu ◽  
Xiaofei Xu ◽  
Jian He ◽  
Jie Guo ◽  
Ke Song

High-effective synthesis of 5-hydroxymethylfurfural (HMF) from carbohydrates is an interesting reaction among biomass valorization. The as-synthesized Ti-SBA-15 catalysts with mesoporous structures showed high catalytic efficiency for the conversion of fructose to HMF. Ti-SBA-15 catalysts with different Si/Ti ratios were characterized by characterization techniques such as elemental analysis, XRD, TEM, N2 adsorption–desorption, NH3-TPD, and pyridine-FTIR. The acidity of Ti-SBA-15 catalysts could be tuned by altering addition amount of titanium. The effects of reaction conditions, including reaction time, temperature, and amount of catalyst, on the conversions of fructose and the yields of HMF were also investigated. It is found that Ti-SBA-15 catalysts whose Si/Ti ratio is 120 gave the best yields of HMF, which demonstrated 100% conversion of fructose with a maximum HMF yield of 82% at 140°C after 1 h. In addition, its catalytic performance was retained after 5 recycles in fructose conversion reaction, proving its good catalytic stability.


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