Insight into the effect of Si/Al ratio on the adsorption and diffusion behavior of butane isomers in HZSM-5 zeolites

IF 3.5 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Journal of Materials Science Pub Date : 2024-09-12 DOI:10.1007/s10853-024-10195-5

Shengyu Se, Huan Wang, Jian Zhou, Qiang Li, Yucai Qin, Lijuan Song

{"title":"Insight into the effect of Si/Al ratio on the adsorption and diffusion behavior of butane isomers in HZSM-5 zeolites","authors":"Shengyu Se, Huan Wang, Jian Zhou, Qiang Li, Yucai Qin, Lijuan Song","doi":"10.1007/s10853-024-10195-5","DOIUrl":null,"url":null,"abstract":"<div><p>The adsorption and diffusion properties of zeolite materials for molecules depend on their pore structure and acidic properties, which have a profound impact on their catalytic performance. In this work, the influence mechanism of the Si/Al ratio on the adsorption and diffusion behaviors of n-butane and isobutane in HZSM-5 zeolites was investigated via Grand Canonical Monte Carlo (GCMC) and Molecular Dynamics (MD) methods. It is found that the difference in adsorption amount of <i>n</i>-butane and isobutane is not significant in MFI zeolites with varying the Si/Al ratio from 12 to ∞. However, an increase in Brønsted acidity of HZSM-5 can significantly influence the adsorption modes of butane, as analyzed through a parameter of the probability distribution of nearest distance (PDND) techniques. The diffusion of <i>n</i>-butane was impeded by the Brønsted acid site, particularly at low loading, due to increased collisions with H atoms at the active site. Furthermore, the relationship between the diffusion and the adsorption probability of <i>n</i>-butane in the straight channel was built. These findings contribute to a deeper understanding of adsorption and diffusion behaviors and their influencing factors, including pore structure and modifications, which are of great significance to the rational design of zeolite catalytic materials.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":645,"journal":{"name":"Journal of Materials Science","volume":null,"pages":null},"PeriodicalIF":3.5000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Science","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10853-024-10195-5","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

The adsorption and diffusion properties of zeolite materials for molecules depend on their pore structure and acidic properties, which have a profound impact on their catalytic performance. In this work, the influence mechanism of the Si/Al ratio on the adsorption and diffusion behaviors of n-butane and isobutane in HZSM-5 zeolites was investigated via Grand Canonical Monte Carlo (GCMC) and Molecular Dynamics (MD) methods. It is found that the difference in adsorption amount of n-butane and isobutane is not significant in MFI zeolites with varying the Si/Al ratio from 12 to ∞. However, an increase in Brønsted acidity of HZSM-5 can significantly influence the adsorption modes of butane, as analyzed through a parameter of the probability distribution of nearest distance (PDND) techniques. The diffusion of n-butane was impeded by the Brønsted acid site, particularly at low loading, due to increased collisions with H atoms at the active site. Furthermore, the relationship between the diffusion and the adsorption probability of n-butane in the straight channel was built. These findings contribute to a deeper understanding of adsorption and diffusion behaviors and their influencing factors, including pore structure and modifications, which are of great significance to the rational design of zeolite catalytic materials.

Graphical abstract

Abstract Image

查看原文本刊更多论文

透视硅/铝比例对 HZSM-5 沸石中丁烷异构体吸附和扩散行为的影响

沸石材料对分子的吸附和扩散特性取决于其孔隙结构和酸性，这对其催化性能有着深远的影响。本研究通过大卡农蒙特卡洛（GCMC）和分子动力学（MD）方法研究了 Si/Al 比对正丁烷和异丁烷在 HZSM-5 沸石中的吸附和扩散行为的影响机理。研究发现，随着硅/铝比例从 12 到 ∞ 的变化，正丁烷和异丁烷在 MFI 沸石中的吸附量差异不大。然而，通过最近距离概率分布（PDND）技术参数分析，HZSM-5 的布氏硬度增加会显著影响丁烷的吸附模式。正丁烷的扩散受到布氏酸性位点的阻碍，特别是在低负载时，这是由于与活性位点上的 H 原子的碰撞增加所致。此外，还建立了正丁烷在直道中的扩散与吸附概率之间的关系。这些发现有助于加深对吸附和扩散行为及其影响因素（包括孔结构和改性）的理解，对合理设计沸石催化材料具有重要意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Materials Science 工程技术-材料科学：综合

CiteScore

7.90

自引率

4.40%

发文量

1297

审稿时长

2.4 months

期刊介绍： The Journal of Materials Science publishes reviews, full-length papers, and short Communications recording original research results on, or techniques for studying the relationship between structure, properties, and uses of materials. The subjects are seen from international and interdisciplinary perspectives covering areas including metals, ceramics, glasses, polymers, electrical materials, composite materials, fibers, nanostructured materials, nanocomposites, and biological and biomedical materials. The Journal of Materials Science is now firmly established as the leading source of primary communication for scientists investigating the structure and properties of all engineering materials.