Kinetics and mechanism for oxidative desulfurization of fuels catalyzed by peroxo-molybdenum amino acid complexes in water-immiscible ionic liquids
Kinetics and mechanism for oxidative desulfurization of fuels catalyzed by peroxo-molybdenum amino acid complexes in water-immiscible ionic liquids
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DOI：
10.1016/j.molcata.2010.12.003
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发表时间：
2011-02
影响因子：
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通讯作者：
Wenshuai Zhu;Hua-ming Li;Qingqing Gu;Peiwen Wu;G. Zhu;Yongsheng Yan;Guangying Chen
中科院分区：
文献类型：
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作者：
Wenshuai Zhu;Hua-ming Li;Qingqing Gu;Peiwen Wu;G. Zhu;Yongsheng Yan;Guangying Chen
合成了三种过氧钼氨基酸配合物(PMAAC)，并对其进行了表征。用不同的离子液体评价了它们在萃取和催化氧化脱硫(ECODS)体系中对二苯并噻吩氧化(DBT)的催化活性。与单一催化剂Na2MoO4·2H2O相比，在ECODS中，PMAAC是一种有效的广谱催化剂，不仅在水相态的IL[bmim]BF4中表现出较高的脱硫效率，而且在水不相容的[bmim]PF6、[Omim]BF4和[OMIM]PF6中也表现出较高的脱硫效率。尤其是4，6-二甲基二苯并噻吩(4，6-DMDBT)是加氢脱硫中最难降解的化合物，在最佳条件下可以完全脱除。用UV-Vis研究和解释了Na2MoO4·2H2O催化剂与PMAAc在水互溶和水不互溶离子液体中的反应机理和脱硫差异。研究了DBT、BT和4，6-DMDBT的氧化动力学参数。
Three peroxo-molybdenum amino acid complexes (PMAACs) were synthesized and characterized. Their catalytic activities for oxidation of dibenzothiophene (DBT) in extraction and catalytic oxidative desulfurization system (ECODS) were evaluated using different ionic liquids. Comparing with simple catalyst Na2MoO4·2H2O in ECODS, PMAACs were effective wide-ranging catalysts and exhibited high desulfurization efficiency not only in water-miscible IL [bmim]BF4but also in water-immiscible [bmim]PF6, [omim]BF4and [omim]PF6. Especially 4,6-dimethyldibenzothiophene (4,6-DMDBT), the most difficult refractory compound in HDS, could be completely removed under optimal conditions. The reaction mechanism and desulfurization differences between using Na2MoO4·2H2O catalyst and PMAACs in water-miscible and water-immiscible ionic liquids have been investigated and explained by UV–vis. Kinetic parameters of the oxidation of DBT, BT and 4,6-DMDBT were studied.