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Deep Oxidative Desulfurization of Fuels in the Presence of Brönsted Acidic Polyoxometalate-Based Ionic Liquids
Molecules ( IF 4.2 ) Pub Date : 2020-01-26 , DOI: 10.3390/molecules25030536
Argam Akopyan 1 , Ekaterina Eseva 1 , Polina Polikarpova 1 , Anastasia Kedalo 1 , Anna Vutolkina 1, 2 , Aleksandr Glotov 1, 2
Affiliation  

Polyoxometalate-based ionic liquid hybrid materials with a pyridinium cation, containing Brönsted acid sites, were synthesized and used as catalysts for the oxidation of model and real diesel fuels. Keggin-type polyoxometalates with the formulae [PMo12O40]3−, [PVMo11O40]4−, [PV2Mo10O40]4−, [PW12O40]3− were used as anions. It was shown that increasing the acid site strength leads to an increase of dibenzothiophene conversion to the corresponding sulfone. The best results were obtained in the presence of a catalyst, containing a nicotinic acid derivative as cation and phosphomolybdate as anion. The main factors affecting the process consisting of catalyst dosage, temperature, reaction time, oxidant dosage were investigated in detail. Under optimal conditions full oxidation of dibenzothiophene and more than a 90% desulfurization degree of real diesel fuel (initial sulfur content of 2050 ppm) were obtained (the oxidation conditions: NK-1 catalyst, molar ratio H2O2:S 10:1, molar ratio S:Mo 8:1, 1 mL MeCN, 70 °C, 1 h). The synthesized catalysts could be used five times with a slight decrease in activity.

中文翻译:


布朗斯台德酸性多金属氧酸盐基离子液体存在下的燃料深度氧化脱硫



合成了具有吡啶鎓阳离子且含有布朗斯台德酸位点的多金属氧酸盐基离子液体杂化材料,并将其用作模型柴油和真实柴油氧化的催化剂。使用化学式为 [PMo12O40]3−、[PVMo11O40]4−、[PV2Mo10O40]4−、[PW12O40]3− 的 Keggin 型多金属氧酸盐作为阴离子。结果表明,增加酸性位点强度会导致二苯并噻吩转化为相应的砜的转化率增加。最好的结果是在含有烟酸衍生物作为阳离子和磷钼酸盐作为阴离子的催化剂存在下获得的。详细考察了催化剂用量、温度、反应时间、氧化剂用量等影响该过程的主要因素。在最佳条件下,二苯并噻吩完全氧化,真实柴油脱硫率达到90%以上(初始硫含量2050 ppm)(氧化条件:NK-1催化剂,H2O2:S摩尔比10:1,摩尔比S:Mo 8:1,1 mL MeCN,70 °C,1 小时)。合成的催化剂可使用5次,活性略有下降。
更新日期:2020-01-26
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