{"title":"Defective MOF incorporating CF3 functionality via fragmented linker co-assembly for high C2H6/C2H4 selectivity and C2H6 uptake","authors":"","doi":"10.1016/j.seppur.2024.129821","DOIUrl":null,"url":null,"abstract":"<div><div>The production of high-purity ethylene requires an adsorbent with high C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity, outstanding C<sub>2</sub>H<sub>6</sub> adsorption, and facile C<sub>2</sub>H<sub>6</sub> regeneration. Towards this goal, a series of novel defective CF<sub>3</sub>-functionalized metal–organic framework (MOF) materials (UiO-66-<em>n</em>CF<sub>3</sub>, <em>n</em> = 25, 50, 60, and 75) were synthesized by co-assembling the framework with terephthalic acid as the linker and various percentages (<em>n</em>) of CF<sub>3</sub>-functionalized ligands. The C<sub>2</sub>H<sub>6</sub> adsorption strength increased as the density of CF<sub>3</sub> groups increased. In particular, UiO-66-50CF<sub>3</sub> exhibited high C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (2.04), excellent C<sub>2</sub>H<sub>6</sub> adsorption (2.5 mmol/g), and modest C<sub>2</sub>H<sub>6</sub> isosteric heat of adsorption (Q<sub>st</sub>) (∼28.9 kJ/mol). Additionally, the material exhibited high C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> breakthrough selectivity (1.64) and large high-purity (>99.9 %) C<sub>2</sub>H<sub>4</sub> productivity (7.32 L<sub>STP</sub> kg<sup>−1</sup>) under dynamic flow conditions (C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> = 1:15 (v/v)). UiO-66-50CF<sub>3</sub> could readily be regenerated at room temperature, and demonstrated good hydrothermal stability in boiling water for 1 h and high thermal stability up to 500 °C. The incorporation of a high density of CF<sub>3</sub> groups within a MOF via fragmented linker co-assembly is a promising strategy for developing adsorbents for C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> separation.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624035603","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The production of high-purity ethylene requires an adsorbent with high C2H6/C2H4 selectivity, outstanding C2H6 adsorption, and facile C2H6 regeneration. Towards this goal, a series of novel defective CF3-functionalized metal–organic framework (MOF) materials (UiO-66-nCF3, n = 25, 50, 60, and 75) were synthesized by co-assembling the framework with terephthalic acid as the linker and various percentages (n) of CF3-functionalized ligands. The C2H6 adsorption strength increased as the density of CF3 groups increased. In particular, UiO-66-50CF3 exhibited high C2H6/C2H4 selectivity (2.04), excellent C2H6 adsorption (2.5 mmol/g), and modest C2H6 isosteric heat of adsorption (Qst) (∼28.9 kJ/mol). Additionally, the material exhibited high C2H6/C2H4 breakthrough selectivity (1.64) and large high-purity (>99.9 %) C2H4 productivity (7.32 LSTP kg−1) under dynamic flow conditions (C2H6/C2H4 = 1:15 (v/v)). UiO-66-50CF3 could readily be regenerated at room temperature, and demonstrated good hydrothermal stability in boiling water for 1 h and high thermal stability up to 500 °C. The incorporation of a high density of CF3 groups within a MOF via fragmented linker co-assembly is a promising strategy for developing adsorbents for C2H6/C2H4 separation.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.