{"title":"通过孔几何拟合金属有机框架从裂解气中直接提纯乙烯","authors":"","doi":"10.1016/j.eng.2024.01.024","DOIUrl":null,"url":null,"abstract":"<div><div>The direct one-step separation of polymer-grade C<sub>2</sub>H<sub>4</sub> from complex light hydrocarbon mixtures has high industrial significance but is very challenging. Herein, an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks (MOFs) with pillar-layered structures, dubbed TYUT-10/11/12/13. Based on its pore geometry design and functional group regulation, TYUT-12 exhibits exceptional selective adsorption selectivity toward C<sub>3</sub>H<sub>8</sub>, C<sub>3</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, and CO<sub>2</sub> over C<sub>2</sub>H<sub>4</sub>; its C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> adsorption selectivity reaches 4.56, surpassing the record value of 4.4 by Fe<sub>2</sub>(O<sub>2</sub>)(dobdc) (dobdc<sup>4−</sup> = 2,5-dioxido-1,4-benzenedicarboxylate). The weak π–π stacking binding affinity toward C<sub>2</sub>H<sub>4</sub> in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations. Breakthrough experiments demonstrate that C<sub>2</sub>H<sub>4</sub> can be directly obtained from binary, ternary, quaternary, and six-component light hydrocarbon mixtures with over 99.95% purity.</div></div>","PeriodicalId":11783,"journal":{"name":"Engineering","volume":null,"pages":null},"PeriodicalIF":10.1000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Direct Ethylene Purification from Cracking Gas via a Metal–Organic Framework Through Pore Geometry Fitting\",\"authors\":\"\",\"doi\":\"10.1016/j.eng.2024.01.024\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The direct one-step separation of polymer-grade C<sub>2</sub>H<sub>4</sub> from complex light hydrocarbon mixtures has high industrial significance but is very challenging. Herein, an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks (MOFs) with pillar-layered structures, dubbed TYUT-10/11/12/13. Based on its pore geometry design and functional group regulation, TYUT-12 exhibits exceptional selective adsorption selectivity toward C<sub>3</sub>H<sub>8</sub>, C<sub>3</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, and CO<sub>2</sub> over C<sub>2</sub>H<sub>4</sub>; its C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> adsorption selectivity reaches 4.56, surpassing the record value of 4.4 by Fe<sub>2</sub>(O<sub>2</sub>)(dobdc) (dobdc<sup>4−</sup> = 2,5-dioxido-1,4-benzenedicarboxylate). The weak π–π stacking binding affinity toward C<sub>2</sub>H<sub>4</sub> in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations. Breakthrough experiments demonstrate that C<sub>2</sub>H<sub>4</sub> can be directly obtained from binary, ternary, quaternary, and six-component light hydrocarbon mixtures with over 99.95% purity.</div></div>\",\"PeriodicalId\":11783,\"journal\":{\"name\":\"Engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.1000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2095809924001309\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2095809924001309","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, MULTIDISCIPLINARY","Score":null,"Total":0}
Direct Ethylene Purification from Cracking Gas via a Metal–Organic Framework Through Pore Geometry Fitting
The direct one-step separation of polymer-grade C2H4 from complex light hydrocarbon mixtures has high industrial significance but is very challenging. Herein, an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks (MOFs) with pillar-layered structures, dubbed TYUT-10/11/12/13. Based on its pore geometry design and functional group regulation, TYUT-12 exhibits exceptional selective adsorption selectivity toward C3H8, C3H6, C2H6, C2H2, and CO2 over C2H4; its C2H6/C2H4 adsorption selectivity reaches 4.56, surpassing the record value of 4.4 by Fe2(O2)(dobdc) (dobdc4− = 2,5-dioxido-1,4-benzenedicarboxylate). The weak π–π stacking binding affinity toward C2H4 in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations. Breakthrough experiments demonstrate that C2H4 can be directly obtained from binary, ternary, quaternary, and six-component light hydrocarbon mixtures with over 99.95% purity.
期刊介绍：
Engineering, an international open-access journal initiated by the Chinese Academy of Engineering (CAE) in 2015, serves as a distinguished platform for disseminating cutting-edge advancements in engineering R&D, sharing major research outputs, and highlighting key achievements worldwide. The journal's objectives encompass reporting progress in engineering science, fostering discussions on hot topics, addressing areas of interest, challenges, and prospects in engineering development, while considering human and environmental well-being and ethics in engineering. It aims to inspire breakthroughs and innovations with profound economic and social significance, propelling them to advanced international standards and transforming them into a new productive force. Ultimately, this endeavor seeks to bring about positive changes globally, benefit humanity, and shape a new future.
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