{"title":"通过孔隙芳香化实现高效天然气净化的高稳定性金属有机框架,具有创纪录的 C3H8 和 C2H6 吸收能力","authors":"","doi":"10.1016/j.seppur.2024.129824","DOIUrl":null,"url":null,"abstract":"<div><div>Selective capture of C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> from CH<sub>4</sub> is extremely key in natural gas purification, but there is a trade-off between uptake and selectivity. Herein, we proposed a method for pore aromatization to build an ultramicroporous metal–organic framework Ni(ndc)(dabco)<sub>0.5</sub> with a robust structure and examine its separation performance for C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> mixtures. The pore walls of the material are composed of opposite and parallel naphthalene rings with a pore size of 6.0 Å and rich electronegative binding sites, and the overlapping areas between naphthalene rings form extremely strong potential energy overlaps. This MOF owns a record C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> uptake (91.4 and 46.5 cm<sup>3</sup>(STP) g<sup>−1</sup>) in actual natural gas components at 298 K and 0.05 and 0.1 bar respectively with excellent C<sub>3</sub>H<sub>8</sub> (<em>119.0</em> cm<sup>3</sup>(STP) g<sup>−1</sup>) and C<sub>2</sub>H<sub>6</sub> (<em>116.6</em> cm<sup>3</sup>(STP) g<sup>−1</sup>) and 1.0 bar, presenting a strong binding ability toward C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub>. Meanwhile, the IAST-predicted C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> (1947.4) and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> (42.6) selectivity is also superior to all adsorbents so far, only inferior to BSF-2, thus overcoming the aforementioned trade-off and setting a novel benchmark. The theoretical studies imply that the enhanced C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> adsorption performance is attributed to the aromatized ultramicropores modified by dense low-polarity naphthalene rings, causing a strong affinity for the two gases. Additionally, the breakthrough test proved that the C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> accompanied by C<sub>3</sub>H<sub>8</sub>/C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> mixtures were fully separated at ambient temperature with superb recyclability. Accordingly, these results confirm the great potentiality of Ni(ndc)(dabco)<sub>0.5</sub> for natural gas purification.</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":"{\"title\":\"A highly stable metal–organic framework via pore aromatization for efficient natural gas purification with record C3H8 and C2H6 uptake\",\"authors\":\"\",\"doi\":\"10.1016/j.seppur.2024.129824\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Selective capture of C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> from CH<sub>4</sub> is extremely key in natural gas purification, but there is a trade-off between uptake and selectivity. Herein, we proposed a method for pore aromatization to build an ultramicroporous metal–organic framework Ni(ndc)(dabco)<sub>0.5</sub> with a robust structure and examine its separation performance for C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> mixtures. The pore walls of the material are composed of opposite and parallel naphthalene rings with a pore size of 6.0 Å and rich electronegative binding sites, and the overlapping areas between naphthalene rings form extremely strong potential energy overlaps. This MOF owns a record C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> uptake (91.4 and 46.5 cm<sup>3</sup>(STP) g<sup>−1</sup>) in actual natural gas components at 298 K and 0.05 and 0.1 bar respectively with excellent C<sub>3</sub>H<sub>8</sub> (<em>119.0</em> cm<sup>3</sup>(STP) g<sup>−1</sup>) and C<sub>2</sub>H<sub>6</sub> (<em>116.6</em> cm<sup>3</sup>(STP) g<sup>−1</sup>) and 1.0 bar, presenting a strong binding ability toward C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub>. Meanwhile, the IAST-predicted C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> (1947.4) and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> (42.6) selectivity is also superior to all adsorbents so far, only inferior to BSF-2, thus overcoming the aforementioned trade-off and setting a novel benchmark. The theoretical studies imply that the enhanced C<sub>3</sub>H<sub>8</sub> and C<sub>2</sub>H<sub>6</sub> adsorption performance is attributed to the aromatized ultramicropores modified by dense low-polarity naphthalene rings, causing a strong affinity for the two gases. Additionally, the breakthrough test proved that the C<sub>3</sub>H<sub>8</sub>/CH<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> accompanied by C<sub>3</sub>H<sub>8</sub>/C<sub>2</sub>H<sub>6</sub>/CH<sub>4</sub> mixtures were fully separated at ambient temperature with superb recyclability. Accordingly, these results confirm the great potentiality of Ni(ndc)(dabco)<sub>0.5</sub> for natural gas purification.</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/S1383586624035639\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624035639","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}
A highly stable metal–organic framework via pore aromatization for efficient natural gas purification with record C3H8 and C2H6 uptake
Selective capture of C3H8 and C2H6 from CH4 is extremely key in natural gas purification, but there is a trade-off between uptake and selectivity. Herein, we proposed a method for pore aromatization to build an ultramicroporous metal–organic framework Ni(ndc)(dabco)0.5 with a robust structure and examine its separation performance for C3H8/CH4 and C2H6/CH4 mixtures. The pore walls of the material are composed of opposite and parallel naphthalene rings with a pore size of 6.0 Å and rich electronegative binding sites, and the overlapping areas between naphthalene rings form extremely strong potential energy overlaps. This MOF owns a record C3H8 and C2H6 uptake (91.4 and 46.5 cm3(STP) g−1) in actual natural gas components at 298 K and 0.05 and 0.1 bar respectively with excellent C3H8 (119.0 cm3(STP) g−1) and C2H6 (116.6 cm3(STP) g−1) and 1.0 bar, presenting a strong binding ability toward C3H8 and C2H6. Meanwhile, the IAST-predicted C3H8/CH4 (1947.4) and C2H6/CH4 (42.6) selectivity is also superior to all adsorbents so far, only inferior to BSF-2, thus overcoming the aforementioned trade-off and setting a novel benchmark. The theoretical studies imply that the enhanced C3H8 and C2H6 adsorption performance is attributed to the aromatized ultramicropores modified by dense low-polarity naphthalene rings, causing a strong affinity for the two gases. Additionally, the breakthrough test proved that the C3H8/CH4 and C2H6/CH4 accompanied by C3H8/C2H6/CH4 mixtures were fully separated at ambient temperature with superb recyclability. Accordingly, these results confirm the great potentiality of Ni(ndc)(dabco)0.5 for natural gas purification.
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.