杂原子[Ga]AlY分子筛吸附脱除模拟柴油中的氮化物  

Heteroatom[Ga]AlY molecular sieve adsorbs and removes nitride from model fuel

作　　者：孙潇镝 唐克[1] 富添 王聚财 洪新[1] 王鹏 SUN Xiao-di;TANG Ke;FU Tian;WANG Ju-cai;HONG Xin;WANG Peng(School of chemical 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：《化学研究与应用》2024年第8期1740-1750,共11页Chemical Research and Application

基　　金：辽宁省教育厅高等学校基本科研项目(面上项目)(JYTMS20230852)资助。

摘　　要：采用液-固相同晶取代法制备了杂原子[Ga] AlY分子筛,并利用X射线衍射(XRD)和红外光谱(FT-IR)等手段对其进行了表征。将[Ga] AlY分子筛用于模拟柴油中碱性氮化物苯胺、吡啶或喹啉的静态吸附脱氮实验,采用Materials Studio软件对[Ga] AlY分子筛吸附脱氮机理进行了分子模拟计算研究。结果表明,在模拟柴油用量15 mL时,[Ga] AlY分子筛较适宜的吸附脱氮条件为:室温,分子筛用量0.2 g、吸附时间20 min。模拟计算的吸附能、d距离及吸附等温线结果表明,[Ga] AlY分子筛吸附三种碱性氮化物的强弱顺序均为:吡啶>苯胺>喹啉,较符合Freundlich模型,这也与实验结果一致。吸附热力学和吸附动力学研究结果表明,苯胺的吸附反应是自发进行的吸附熵增过程,吡啶和喹啉为吸附熵减过程,三者的吸附均为放热过程。在303 K条件下,喹啉的吸附过程较符合准一级动力学模型,吡啶和苯胺的程较符合准二级动力学模型。Heteroatom [Ga] AlY molecular sieve was prepared by the isomorphous substitution method and characterized by X-ray diffraction(XRD) and infrared spectroscopy(FT-IR).Static adsorption denitrification experiment of basic nitrogen compounds aniline,pyridine or quinoline in model fuel was carried out by using the[Ga] AlY molecular sieve as adsorbent,and the mechanism of adsorption denitrification of[Ga] AlY molecular sieve was studied by using Materials Studio software.when the model fuel dosage is15 mL,the results show that the most suitable adsorption denitrification conditions for[Ga] AlY molecular sieve are the molecular sieve dosage 0.2 g and the adsorption time 20 min at room temperature.The results of simulated calculation of adsorption energy,d(T-N) distance and adsorption isotherm showed that the strength order of[Ga] AlY molecular sieve adsorption of three basic nitrides was as follows:pyridine>aniline>quinoline,which were more in line with the Freundlich model and consistent with the experimental results.The results of adsorption thermodynamics and adsorption kinetics show that the adsorption of aniline is a spontaneous adsorption entropy increase process,the adsorption pyridine and quinoline are entropy reduction processes,and the adsorption of the three nitrides are exothermic processes.At 303 K,the adsorption process of quinoline conformed to the quasi-primary kinetic model,the adsorption process of pyridine and aniline and conformed to the quasi-secondary kinetic model.

关 键 词：杂原子 [Ga]AlY分子筛 吸附脱氮 模拟计算 热力学 动力学 

分 类 号：O614.4[理学—无机化学]