杂原子Ga[Al]Y分子筛吸附脱氮的模拟计算研究  

Theoretical Calculation of Nitrogen Removal by Adsorption of Heteroatom Ga[Al]Y Molecular Sieve

作　　者：房欣 孙潇镝 唐克[1] 王涵 FANG Xin;SUN Xiao-di;TANG Ke;WANG Han(School of chemistry and environmental engineering,Liaoning university of technology,Jinzhou 121001,China)

机构地区：[1]辽宁工业大学化学与环境工程学院,辽宁锦州121001

出　　处：《唐山师范学院学报》2024年第3期23-26,38,共5页Journal of Tangshan Normal University

基　　金：2023年度辽宁省教育厅高等学校基本科研项目(面上项目)(JYTMS20230852);2023年国家级大学生创新创业训练计划项目(202310154014)。

摘　　要：利用Materials Studio软件,采用巨正则蒙特卡洛和密度泛函理论对Ga[Al]Y分子筛吸附氮化物机理进行了模拟计算研究。通过Mulliken和Hirshfeld布居分析方法,判断金属原子转移电荷数的顺序大小,得出Ga[Al]Y分子筛吸附吡啶时相对亲电性最强,吸附喹啉时的相对亲电性最弱;通过比较两种吸附构型的吸附能和吸附距离,得知Ga[Al]Y分子筛吸附脱氮主要以水平吸附构型为主,吸附能的绝对值大小顺序为:吡啶>苯胺>喹啉,分子间距离大小为:喹啉>苯胺>吡啶;由吸附等温线的模拟结果可知,Ga[Al]Y分子筛在三个温度下(288 K、293 K、298 K)对吡啶的最大吸附量均高于苯胺和喹啉。The mechanism of adsorption of nitride by heteratom Ga[Al]Y molecular sieve was simulated by means of Giant Canonical Monte Carlo(GCMC)and density functional theory(DFT)using Materials Studio software.According to Mulliken and Hirshfeld population analysis,the order of charge transfer number of metal atoms was determined.The relative electrophilicity of Ga[Al]Y molecular sieve was the strongest when adsorbing pyridine,and was the weakest when adsorbing quinoline.By comparing the adsorption energy and adsorption distance of the two adsorption configurations,it was found that Ga[Al]Y molecular sieve was mainly horizontal adsorption configurations.The absolute order of adsorption energy was pyridine>aniline>quinoline,and the order of intermolecular distance was quinoline>aniline>pyridine.According to the simulation results of adsorption isotherm,the maximum adsorption capacity of Ga[Al]Y molecular sieve at three temperatures(288 K,293 K,298 K)for pyridine was higher than that of aniline and quinoline.

关 键 词：杂原子Ga[Al]Y 分子筛 吸附脱氮 模拟计算 

分 类 号：TE624[石油与天然气工程—油气加工工程] O647.3[理学—物理化学]