具有杂原子功能化纳米通道的铝基金属有机框架吸附剂用于分离己烷异构体

IF 3.8 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Jingxian Hua, Yawei Gu, Zemin Li, Luogang Wu, Haiqian Lian, Lixiong Zhang, Rujing Hou, Yichang Pan, Weihong Xing
{"title":"具有杂原子功能化纳米通道的铝基金属有机框架吸附剂用于分离己烷异构体","authors":"Jingxian Hua, Yawei Gu, Zemin Li, Luogang Wu, Haiqian Lian, Lixiong Zhang, Rujing Hou, Yichang Pan, Weihong Xing","doi":"10.1021/acs.iecr.4c02953","DOIUrl":null,"url":null,"abstract":"Metal–organic frameworks (MOFs) have emerged as attractive options for the nonthermal separation of hexane isomers due to their variable channel environments and structural diversity. Here, we report three robust Al-MOFs, KMF-1, MIL-160, and CAU-23, which have nanochannels functionalized with heteroatoms (N, O, and S) for the adsorptive separation of hexane isomers. The adsorption isotherms reveal that these three Al-MOFs can simultaneously adsorb linear, mono-, and dibranched isomers due to their relatively large pore sizes, while showing distinct thermodynamic adsorption behaviors. Significantly, CAU-23, constructed with “S”-atom-functionalized ligands, boasts a notable <i>n</i>-hexane uptake of 3.4 mmol·g<sup>–1</sup>, coupled with <i>n</i>-hexane/3-methylpentane and <i>n</i>-hexane/2,2-dimethylbutane uptake ratios of 1.2 and 1.7 at 298 K and a pressure of 19 kPa, respectively, surpassing those of most reported thermodynamically separated MOF materials. Breakthrough measurements demonstrate that CAU-23 effectively separates an <i>n</i>-hexane/3-methylpentane/2,2-dimethylbutane mixture system into linear, mono-, and dibranched components, achieving <i>n</i>-hexane purity levels of up to 99.9%, while providing sufficient retention time between <i>n</i>-hexane, 3-methylpentane, and 2,2-dimethylbutane. The configurational bias Monte Carlo and density functional theory calculations confirmed atomic-scale interactions between heteroatom sites within Al-MOF nanochannels and various isomers, leading to distinct distributions and adsorption characteristics. Moreover, CAU-23 offers a benchmark balance among separation performance, regeneration ability, cost of production, and scalability, highlighting its potential for further research in industrial adsorptive separation of hexane isomers.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"14 1","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Robust Aluminum-Based Metal–Organic Framework Adsorbents with Heteroatom-Functionalized Nanochannels for Hexane Isomer Separation\",\"authors\":\"Jingxian Hua, Yawei Gu, Zemin Li, Luogang Wu, Haiqian Lian, Lixiong Zhang, Rujing Hou, Yichang Pan, Weihong Xing\",\"doi\":\"10.1021/acs.iecr.4c02953\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Metal–organic frameworks (MOFs) have emerged as attractive options for the nonthermal separation of hexane isomers due to their variable channel environments and structural diversity. Here, we report three robust Al-MOFs, KMF-1, MIL-160, and CAU-23, which have nanochannels functionalized with heteroatoms (N, O, and S) for the adsorptive separation of hexane isomers. The adsorption isotherms reveal that these three Al-MOFs can simultaneously adsorb linear, mono-, and dibranched isomers due to their relatively large pore sizes, while showing distinct thermodynamic adsorption behaviors. Significantly, CAU-23, constructed with “S”-atom-functionalized ligands, boasts a notable <i>n</i>-hexane uptake of 3.4 mmol·g<sup>–1</sup>, coupled with <i>n</i>-hexane/3-methylpentane and <i>n</i>-hexane/2,2-dimethylbutane uptake ratios of 1.2 and 1.7 at 298 K and a pressure of 19 kPa, respectively, surpassing those of most reported thermodynamically separated MOF materials. Breakthrough measurements demonstrate that CAU-23 effectively separates an <i>n</i>-hexane/3-methylpentane/2,2-dimethylbutane mixture system into linear, mono-, and dibranched components, achieving <i>n</i>-hexane purity levels of up to 99.9%, while providing sufficient retention time between <i>n</i>-hexane, 3-methylpentane, and 2,2-dimethylbutane. The configurational bias Monte Carlo and density functional theory calculations confirmed atomic-scale interactions between heteroatom sites within Al-MOF nanochannels and various isomers, leading to distinct distributions and adsorption characteristics. Moreover, CAU-23 offers a benchmark balance among separation performance, regeneration ability, cost of production, and scalability, highlighting its potential for further research in industrial adsorptive separation of hexane isomers.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"14 1\",\"pages\":\"\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2025-01-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.iecr.4c02953\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1021/acs.iecr.4c02953","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0

摘要

金属有机骨架(mof)由于其多变的通道环境和结构多样性,已成为非热分离己烷异构体的有吸引力的选择。在这里,我们报道了三种强大的al - mof, KMF-1, MIL-160和CAU-23,它们具有被杂原子(N, O和S)功能化的纳米通道,用于吸附分离己烷异构体。吸附等温线表明,这三种Al-MOFs由于孔径较大,可以同时吸附线性、单支和双支异构体,并表现出不同的热力学吸附行为。值得注意的是,以“S”原子功能化配体构建的CAU-23在298 K和19 kPa压力下,正己烷/3-甲基戊烷和正己烷/2,2-二甲基丁烷的摄取比分别为1.2和1.7,达到了3.4 mmol·g-1的正己烷摄取率,超过了目前报道的大多数热分离MOF材料。突破性的测量结果表明,CAU-23可以有效地将正己烷/3-甲基戊烷/2,2-二甲基丁烷混合物体系分离成线性、单支和双支组分,使正己烷纯度达到99.9%,同时在正己烷、3-甲基戊烷和2,2-二甲基丁烷之间提供足够的保留时间。构型偏差蒙特卡罗和密度泛函理论计算证实了Al-MOF纳米通道内杂原子位点与各种异构体之间的原子尺度相互作用,导致不同的分布和吸附特征。此外,CAU-23在分离性能、再生能力、生产成本和可扩展性方面提供了一个基准平衡,突出了其在己烷异构体工业吸附分离方面的进一步研究潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Robust Aluminum-Based Metal–Organic Framework Adsorbents with Heteroatom-Functionalized Nanochannels for Hexane Isomer Separation

Robust Aluminum-Based Metal–Organic Framework Adsorbents with Heteroatom-Functionalized Nanochannels for Hexane Isomer Separation
Metal–organic frameworks (MOFs) have emerged as attractive options for the nonthermal separation of hexane isomers due to their variable channel environments and structural diversity. Here, we report three robust Al-MOFs, KMF-1, MIL-160, and CAU-23, which have nanochannels functionalized with heteroatoms (N, O, and S) for the adsorptive separation of hexane isomers. The adsorption isotherms reveal that these three Al-MOFs can simultaneously adsorb linear, mono-, and dibranched isomers due to their relatively large pore sizes, while showing distinct thermodynamic adsorption behaviors. Significantly, CAU-23, constructed with “S”-atom-functionalized ligands, boasts a notable n-hexane uptake of 3.4 mmol·g–1, coupled with n-hexane/3-methylpentane and n-hexane/2,2-dimethylbutane uptake ratios of 1.2 and 1.7 at 298 K and a pressure of 19 kPa, respectively, surpassing those of most reported thermodynamically separated MOF materials. Breakthrough measurements demonstrate that CAU-23 effectively separates an n-hexane/3-methylpentane/2,2-dimethylbutane mixture system into linear, mono-, and dibranched components, achieving n-hexane purity levels of up to 99.9%, while providing sufficient retention time between n-hexane, 3-methylpentane, and 2,2-dimethylbutane. The configurational bias Monte Carlo and density functional theory calculations confirmed atomic-scale interactions between heteroatom sites within Al-MOF nanochannels and various isomers, leading to distinct distributions and adsorption characteristics. Moreover, CAU-23 offers a benchmark balance among separation performance, regeneration ability, cost of production, and scalability, highlighting its potential for further research in industrial adsorptive separation of hexane isomers.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信