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机构地区:[1]东北石油大学化学化工学院,黑龙江大庆163318 [2]东北石油大学石油与天然气化工省重点实验室,黑龙江大庆163318
出 处:《燃料化学学报》2016年第12期1509-1517,共9页Journal of Fuel Chemistry and Technology
基 金:国家自然科学基金(21276048);黑龙江省自然科学基金(ZD201201);黑龙江省教育厅面上项目(12541060)资助~~
摘 要:以硅铝比为5.3的NaY分子筛为母体,分别采用微波辅助离子交换法(AgCeY-1)、水热离子交换法(AgCeY-2)和液相离子交换法(AgCeY-3)制备了AgCeY-n吸附剂,并利用XRD、BET、XPS和Py-FTIR对吸附剂进行了表征。以噻吩和苯并噻吩为模型硫化物,甲苯和环己烯为竞争吸附组分,考察了制备方法对制备得到的吸附剂脱硫性能的影响。结果表明,AgCeY-n吸附剂上Ag、Ce元素分别以Ag^+、Ce^(4+)形式存在。经微波辅助离子交换法制备得到的AgCeY-1吸附剂表面Ag^+、Ce^(4+)含量均最高,且具有最高的L酸和B酸量。AgCeY-n吸附剂对硫化物的吸附选择大小顺序为:BT>TP,竞争吸附组分对AgCeY-n吸附脱硫性能的影响顺序为:环己烯>甲苯。在所研究的制备方法中,微波辅助离子交换法所需时间最短(20 min),合成的AgCeY-1对所研究的模拟油的吸附效果均最好,且具有较好的重复使用性能。各吸附剂对TP和BT的脱除能力大小顺序为:AgCeY-1>AgCeY-2>AgCeY-3。The AgCeY-n adsorbents were successfully synthesized by microwave-assisted liquid ion exchange (AgCeY -1),hydrothermal ion exchange (AgCeY -2) and liquid phase ion exchange (A g C e Y -3) methods with NaY (S^Al ration = 5. 3) molecular sieve parent and characterized by XRD , B E T ,X P S and Py-FTIR analysis. With thiophene (TP ) and benzothiophene (BT ) as the model sulfides,and toluene and cyclohexene as the competition components,the effects of the preparation method on the adsorptive desulfurization properties of the as-prepared adsorbents were evaluated. The results show that the A g and C e species in A g C e Y -n zeolites exist as Ag + and Ce4+. The AgCeY -1 prepared via microwave-assisted liquid ion exchange method possesses the highest Ag + and Ce4+ contents. In addition,it possesses the highest amounts of L and B acid. The adsorption selectivity to sulfur compounds follows the order: BT 〉TP . The effects of competition components on the sulfur removal with AgCeY-n zeolites follow the order: cyclohexene 〉 toluene. A m o n g the preparation methods tested,the microwave-assisted liquid ion exchange method takes the shortest time (20 m i n ). The as-prepared A g C e Y -1 adsorbent exhibits most satisfied performance of adsorption for all the model oils and a wonderful regeneration property. The removal ability for TP and BT of various adsorbents follows the order: AgCeY -1 〉 AgCeY -2〉 AgCeY -3.
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