Ag^(+)、Zn^(2+)、Cr^(3+)改性Y型分子筛吸附脱除喹啉的模拟计算研究  

Study on the simulation of quinoline adsorption from model fuel on Y zeolites modified by Ag^(+),Zn^(2+)and Cr^(3+)

作　　者：孙潇镝 唐克[1] 高畅 富添 王聚财 洪新[1] SUN Xiao-Di;TANG Ke;GAO Chang;FU Tian;WANG Ju-Cai;HONG Xin(School of Chemistry and Environmental Engineering,Liaoning University of Technology,Jinzhou 121001,China;Huludao Emergency Management Bureau,Huludao 125000,China)

机构地区：[1]辽宁工业大学化学与环境工程学院,锦州121001 [2]葫芦岛市应急管理局,葫芦岛125000

出　　处：《原子与分子物理学报》2025年第1期61-68,共8页Journal of Atomic and Molecular Physics

基　　金：辽宁省自然科学基金(2019-ZD-0699)。

摘　　要：首先考察了吸附时间对三种改性Y型分子筛AgY、ZnY、CrY吸附脱除模拟燃料中喹啉的影响,结果发现三种分子筛对喹啉的吸附容量和去除率大小顺序均为:AgY>CrY>ZnY.运用Materials Studio软件,采用巨正则蒙特卡洛(GCMC)和密度泛函理论(DFT)对改性Y型分子筛吸附喹啉机理进行了模拟计算研究,得出以下结论:模拟计算AgY、ZnY、CrY的比表面积和孔体积与其低温N2吸附-脱附表征结果基本一致,并且发现改性Y型分子筛的吸附脱氮能力与比表面积和孔体积关系不大;以Fukui函数为基础,采用Mulliken和Hirshfeld两种布局数分析方法模拟计算了三种改性Y型分子筛的相对亲电性并分析Lewis酸强弱,其Lewis酸大小顺序为:AgY>CrY>ZnY;对三种改性分子筛进行了前线轨道分析,其化学吸附活性大小为AgYCrY>ZnY,模拟计算所得各种结果与实验结果顺序完全一致.The adsorption capacity and removal rate of quinoline by AgY,ZnY and CrY zeolites from model fuel at different adsorption times were investigated by experiments.The order of adsorption capacity and removal rate of quinoline was AgY>CrY>ZnY.Theoretical study on the mechanism of adsorption of quinoline on AgY,CrY and ZnY was made by using the theory of Grand Canon Monte Carlo(GCMC)and Density Functional Theory(DFT)in Materials Studio software.The experiment results indicated that modified Y zeolites for N 2 adsorption-desorption and simulated calculation of specific surface area and pore volume of AgY,ZnY and CrY are consistent.It is found that the adsorption capacity of modified Y zeolites has little relationship with specific surface area and pore volume;based on Fukui function,Mulliken and Hirshfeld are used to analyze the relative electrophilicity and Lewis acid of three modified Y zeolites and the order of Lewis acidity is as follows:AgY>CrY>ZnY.The adsorption mode is theπ-complexed adsorption.The simulation and calculation of the adsorption energy of three modified Y zeolites suggest that the order of adsorption energy is:AgY>CrY>ZnY.All results of simulation are in good agreement with the experimental results.

关 键 词：Y型分子筛 改性 吸附 喹啉 模拟 

分 类 号：O561.2[理学—原子与分子物理]