乙苯和对二甲苯在ZSM-5分子筛上吸附的蒙特卡罗模拟
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摘要
采用巨正则统计系综蒙特卡罗模拟方法(GCMC)研究了高温条件下乙苯和对二甲苯在不同硅铝比ZSM-5分子筛上的吸附行为,并结合工业样品的催化反应进行验证。GCMC模拟结果表明:在不同硅铝比ZSM-5上乙苯的吸附能均高于对二甲苯,乙苯和对二甲苯的吸附位在两种孔道的交叉处,随Al含量的增加,吸附状态多样化;在温度623K下,压力为200kPa左右时吸附量已达到平稳。催化反应评价结果表明,乙苯生成苯的反应比对二甲苯生成甲苯的反应更容易进行,与吸附扩散的规律一致。
The adsorption behavior of ethylbenzene and p-xylene on ZSM-5 zeolites with different SiAl ratio was studied by using the macro-canonical statistics ensemble Monte Carlo simulation method and verified by the catalytic reaction of industrial samples.GCMC simulation showed that the adsorption energy of EB is higher than that of PX on different ZSM-5 zeolites.EB and PX were adsorped mainly at the intersection of the two channels of the zeolites.With increasing Al content,the adsorption states are diverse.The adsorption quantity reaches a platform at 200 kPa and 623 K.It was shown by the catalytic experiments that the reaction of ethylbenzene to benzene is much easier than that of PX to toluene,which is consistent with the adsorption trend simulated by GCMC.
The adsorption behavior of ethylbenzene and p-xylene on ZSM-5 zeolites with different SiAl ratio was studied by using the macro-canonical statistics ensemble Monte Carlo simulation method and verified by the catalytic reaction of industrial samples.GCMC simulation showed that the adsorption energy of EB is higher than that of PX on different ZSM-5 zeolites.EB and PX were adsorped mainly at the intersection of the two channels of the zeolites.With increasing Al content,the adsorption states are diverse.The adsorption quantity reaches a platform at 200 kPa and 623 K.It was shown by the catalytic experiments that the reaction of ethylbenzene to benzene is much easier than that of PX to toluene,which is consistent with the adsorption trend simulated by GCMC.
引文
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[2] Guisnet M,Gnep N S,Morin S.Mechanisms of xylene isomerization over acidic solid catalysts[J].Microporous and Mesoporous Materials,2000,35/36:47-59
[3]康承琳,周震寰,吴巍,等.乙基环己烷在择形分子筛上的异构化反应[J].石油炼制与化工,2012,43(5):1-5
[4]阮迟,冯小兵,胡满生,等.低铂脱乙基型C8芳烃异构化催化剂的工业应用[J].石油炼制与化工,2013,45(2):64-68
[5]周震寰,贾树岩,张培贵,等.ZSM-5分子筛酸性修饰及探针分子表征[J].石油炼制与化工,2016,47(3):5-9
[6]周震寰,张爱军,胡维军,等.碳八芳烃异构化分子筛的酸性与反应分析[J].石油炼制与化工,2017,48(11):76-81
[7]戴厚良.芳烃生产技术展望[J].石油炼制与化工,2013,44(1):1-10
[8]康承琳,周震寰,冯小兵,等.ZSM-5分子筛酸性质对二甲苯异构化反应的影响[J].石油炼制与化工,2013,44(12):35-41
[9]胡家芬,蔡健健,黄月芳,等.二甲苯异构化催化剂的表面酸性及其催化活性[J].催化学报,1985,6(4):325-331
[10]孙晓岩,宋泓阳,项曙光.ZSM-5分子筛上氯乙酸和二氯乙酸吸附行为的蒙特卡罗研究[J].计算机与应用化学,2017,34(2):109-113
[11]丁雪,刘熠斌,杨朝合,等.FCC干气在ZSM-5分子筛中吸附的分子模拟及热力学分析[J].石油炼制与化工,2015,46(9):58-64
[12]Bauer F,Bilz E,Freyer A.C-14studies in xylene isomerization on modified HZSM-5[J].Applied Catalysis A:General,2005,289:2-9
[13]赵仁殿,金彰礼,陶志华,等.芳烃工学[M].北京:化学工业出版社,2001:158