An improvement of MCM-41 supported phosphoric acid catalyst for alkylation desulfurization of fluid catalytic cracking gasoline

An improvement of MCM-41 supported phosphoric acid catalyst for alkylation desulfurization of fluid catalytic cracking gasoline
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MCM-41负载型磷酸流化催化裂化汽油烷基化脱硫催化剂的改进

DOI:
10.1016/j.fuel.2014.11.093
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发表时间:
2015-03
期刊:
影响因子:
7.4
通讯作者:
Hongwei Sun
Hongwei Sun
中科院分区:
工程技术1区
文献类型:
--
作者:
Rong Wang;Jinbao Wan;Yonghong Li;Hongwei Sun

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对MCM-41负载磷酸(SPAM)在流化催化裂化(FCC)汽油烷基化脱硫中的催化机理的理论计算表明,适当降低表面有效酸的量有利于进一步提高催化剂性能。本工作在之前优化的SPAM制备方法(总酸/MCM-41重量比6:1、焙烧温度773 K、H3PO4/H4P2O71:2.5重量比)的基础上,通过稀释浸渍液中混合磷酸的浓度进行了改进。分别通过结构表征和实验验证研究了改进SPAM的表面结构和催化行为。结果表明,降低SPAM制备过程中浸渍液中混合磷酸的浓度,可以通过提高催化剂结晶度,有效降低催化剂表面存在的酸量,使SPAM的表面酸强度和总酸量均降低。此外,改进的SPAM在烷基化脱硫中对噻吩硫烷基化的催化活性和选择性得到增强,并且烯烃聚合反应被抑制到较低程度。此外,本研究验证了理论计算,为SPAM在汽油工业烷基化脱硫中的应用提供了特别有吸引力的机会。
The theoretical calculation about the catalytic mechanism of MCM-41 supported phosphoric acid (SPAM) in the alkylation desulfurization of fluid catalytic cracking (FCC) gasoline demonstrated that properly reducing the amount of effective acid on the surface was beneficial to further enhancing the catalyst performance. Based on the previously optimized preparation of SPAM (weight ratio of total acid/MCM-41 6:1, calcination temperature 773 K and weigh ratio of H3PO4/H4P2O71:2.5), an improvement by diluting the concentration of mixed phosphoric acids in the impregnating solution was carried out in this work. The surface structure and catalytic behavior of improved SPAM were investigated by structural characterization and experimental verification, respectively. The results proved that decreasing the concentration of mixed phosphoric acids in the impregnating solution in the preparation of SPAM could effectively reduce the existing acid amount on the catalyst surface by increasing the catalyst crystallinity, and both the surface acid strength and the total acids amount of SPAM were reduced. Moreover, the catalytic activity and selectivity of improved SPAM for thiophenic sulfurs alkylation in the alkylation desulfurization were enhanced and the olefins polymerization reactions were suppressed to a lower extent. Besides, the theoretical calculation was verified by this study, which opened a particularly appealing opportunity for the application of SPAM in the industrial alkylation desulfurization of gasoline.
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