改性Y型分子筛吸附脱除喹啉和吲哚过程的模拟计算

石油炼制与化工 ›› 2019, Vol. 50 ›› Issue (7): 19-24.

改性Y型分子筛吸附脱除喹啉和吲哚过程的模拟计算

高畅,唐克,唐天涯,任茂

辽宁工业大学化学与环境工程学院

收稿日期:2018-11-20 修回日期:2019-02-27 出版日期:2019-07-12 发布日期:2019-07-25
通讯作者: 唐克 E-mail:tangke0001@163.com
基金资助:
辽宁省自然科学基金

SIMULATION CALCULATION OF ADSORPTION OF QUINOLINE AND INDOLE ON MODIFIED Y ZEOLITE

Received:2018-11-20 Revised:2019-02-27 Online:2019-07-12 Published:2019-07-25
Contact: Tang Ke E-mail:tangke0001@163.com
Supported by:
The project was supported by the Liaoning Provincial Natural Science Foundation of China

摘要/Abstract

摘要： 运用密度泛函理论（DFT）研究4种阳离子改性Y型分子筛(CeY,NiY,CuY,AgY)的吸附脱氮性能。采用GGA近似下BLYP交换的相关泛函和DNP基组，基于Fukui函数描述和布居分析法计算各个改性Y型分子筛的Lewis酸强度，结果显示Mulikun和Hirshfeld两种布居分析方法得到的4种改性Y型分子筛酸性强度由大到小的顺序均为：CeY>NiY>CuY>AgY；通过计算η1N和η5构型的吸附能，发现喹啉和吲哚在4种改性Y型分子筛的η5构型的吸附能要比η1N构型大，表明喹啉和吲哚的吸附构型以η5为主；计算了不同温度下CeY分子筛对喹啉和吲哚的吸附等温线，结果表明，吸附温度对吸附喹啉和吲哚影响不大，温度为298 K时CeY对吲哚的平衡吸附量大于喹啉。

关键词: 密度泛函理论, Y分子筛, 改性, Lewis酸强度, 吸附脱氮

Abstract: Adsorptive and denitrogenation performances of CuY, AgY, NiY, CeY zeolites prepared by cation exchange were studied by using Dense Function Theory (DFT). In the theoretical calculation, the relevant functional and DNP basis sets of BLYP exchange under GGA approximation were used; The strength of Lewis acid in Y zeolites was studied quantitatively using Fukui functional response description and layout analysis. The results showed that the relationship between the acidity of different cation exchanged Y zeolites studied by Mulikun and Hirshfeld was: CeY>NiY>CuY>AgY; by calculating the adsorption energy of the two adsorption configurations, η5 and η1N, it could be concluded that the adsorption energy of quinoline and indole at the substituted η5 configurations of the four modified Y zeolites was higher than that of the substituted η1N, which indicates that the main adsorption configuration of quinoline and indole is η5. and the adsorption configuration was mainly in η5 .The adsorption isotherm of quinoline and indole at different temperature over CeY molecular sieve showed that the adsorption temperature had less impact on the adsorption of quinoline and indole, the balance adsorption amount of indole at 298 K over CeY was greater than that of quinoline.

Key words: DFT, Y zeolite, modification, Lewis acid strength, adsorptive denitrogenation

中图分类号:

高畅唐克唐天涯任茂. 改性Y型分子筛吸附脱除喹啉和吲哚过程的模拟计算[J]. 石油炼制与化工, 2019, 50(7): 19-24.

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