噻吩、吡咯、呋喃在H-FAU分子筛中吸附和扩散行为的分子模拟  

Molecular Simulation of Adsorption and Diffusion of Thiophene, Pyrrole and Furan in H-FAU Zeolite

作　　者：党宇 杨晓东 刘熠斌[1] 冯翔 杨朝合[1] DANG Yu;YANG Xiaodong;LIU Yibin;FENG Xiang;YANG Chaohe(State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Qingdao 266580,China)

机构地区：[1]中国石油大学重质油国家重点实验室

出　　处：《石油学报（石油加工）》2019年第5期911-919,共9页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(21476263,21776312);中央高校基本科研业务费专项资金(18CX02130A)资助

摘　　要：采用蒙特卡洛方法(GCMC)和分子动力学方法(MD),研究了在823 K、100~1000 kPa条件下噻吩、吡咯和呋喃3种典型的杂原子分子在H-FAU分子筛中吸附和扩散性能,分析了3种分子在H-FAU分子筛中的概率密度分布、分子扩散动力学和径向分布函数(RDF)。单组分吸附模拟的结果表明,噻吩的饱和吸附量和吸附热最大,吡咯居中,呋喃最小。三元混合组分的吸附模拟表明:噻吩的吸附强度明显大于吡咯和呋喃;3种分子在分子筛的超笼和SOD笼中均有分布,且噻吩在超笼中更加集中;3种分子在孔道中扩散阻力的大小依次为噻吩、吡咯、呋喃;噻吩、吡咯和呋喃主要通过分子环区的离域电子及杂原子与孔道表面H质子进行作用。In this paper,Monte Carlo(GCMC)and molecular dynamics(MD)methods were used to study the adsorption and diffusion properties of three typical heteroatom molecules i.e.thiophene,pyrrole and furan in H-FAU zeolite,at 823 K,100-1000 kPa.The probability density distribution,molecule diffusion dynamics and radial distribution function(RDF)were analyzed.The results of single-component adsorption simulation showed that the saturated adsorption amount and adsorption heat of thiophene were the largest,pyrrole was in the middle,and furan was the smallest.The adsorption of three molecules mixtures onto the zeolite was further conducted,and the results indicated that the adsorption strength of thiophene is significantly greater than that of pyrrole and furan.The probability density distribution results confirmed that the three molecules were distributed in the supercages and SOD cages of zeolite,and the thiophenes were more concentrated in the supercages.The kinetic study found that the order of diffusion resistance of the three molecules in the pores was thiophene,pyrrole and furan.The radial distribution function(RDF)analysis revealed that the interactions between three molecules and zeolite are dominated by the delocalized electrons in the molecular ring region as well as the heteroatoms on the molecules and the H protons on the pore surface.

关 键 词：杂原子分子 八面沸石(FAU)分子筛 吸附 扩散 分子模拟 

分 类 号：TE624[石油与天然气工程—油气加工工程]