Chung-Kai Chang , Hyun Jung Yu , Huiwon Jang , Ting-Hsiang Hung , Chung-Kai Chang , Jihan Kim , Jong Suk Lee , Dun-Yen Kang
{"title":"构象变化诱导的cu -10- pdc膜对H2/CH4和CO2/CH4分离选择性增强","authors":"Chung-Kai Chang , Hyun Jung Yu , Huiwon Jang , Ting-Hsiang Hung , Chung-Kai Chang , Jihan Kim , Jong Suk Lee , Dun-Yen Kang","doi":"10.1016/j.memlet.2021.100005","DOIUrl":null,"url":null,"abstract":"<div><p>The separation of H<sub>2</sub>/CH<sub>4</sub> or CO<sub>2</sub>/CH<sub>4</sub> is critical to the purification of natural gas. Herein, we report on novel membranes with a metal-organic framework of CAU-10-PDC for the separation of these two mixtures. The dense CAU-10-PDC membranes are fabricated on a porous alumina support using the seeded growth method. An unexpected increase in selectivity was observed while testing mixed gas permeation with either H<sub>2</sub>/CH<sub>4</sub> or CO<sub>2</sub>/CH<sub>4</sub> at a molar ratio of 50:50. Steady-state selectivity reached 101 for H<sub>2</sub>/CH<sub>4</sub> and 62 for CO<sub>2</sub>/CH<sub>4</sub>. Ideal selectivity measured from single gas permeation reached 475 for H<sub>2</sub>/CH<sub>4</sub> and 288 for CO<sub>2</sub>/CH<sub>4</sub>. Molecular dynamics simulations and time-resolved X-ray diffraction with a synchrotron radiation source were used to probe conformational changes in CAU-10-PDC induced by exposure to CH<sub>4</sub>. When exposed to an atmosphere containing CH<sub>4</sub>, CAU-10-PDC presented a change in the space group (from <em>I</em>4<sub>1</sub>/<em>amd</em> to <em>I</em>4<sub>1</sub>), which drastically reduced the pore limiting diameter from 4.15 to 2.95 Å, rendering the channel nearly impermeable to CH<sub>4</sub>.</p></div>","PeriodicalId":100805,"journal":{"name":"Journal of Membrane Science Letters","volume":null,"pages":null},"PeriodicalIF":4.9000,"publicationDate":"2021-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772421221000052/pdfft?md5=bc88058c566daef3e0c02c1d2c0cc52a&pid=1-s2.0-S2772421221000052-main.pdf","citationCount":"10","resultStr":"{\"title\":\"Conformational-change-induced selectivity enhancement of CAU-10-PDC membrane for H2/CH4 and CO2/CH4 separation\",\"authors\":\"Chung-Kai Chang , Hyun Jung Yu , Huiwon Jang , Ting-Hsiang Hung , Chung-Kai Chang , Jihan Kim , Jong Suk Lee , Dun-Yen Kang\",\"doi\":\"10.1016/j.memlet.2021.100005\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The separation of H<sub>2</sub>/CH<sub>4</sub> or CO<sub>2</sub>/CH<sub>4</sub> is critical to the purification of natural gas. Herein, we report on novel membranes with a metal-organic framework of CAU-10-PDC for the separation of these two mixtures. The dense CAU-10-PDC membranes are fabricated on a porous alumina support using the seeded growth method. An unexpected increase in selectivity was observed while testing mixed gas permeation with either H<sub>2</sub>/CH<sub>4</sub> or CO<sub>2</sub>/CH<sub>4</sub> at a molar ratio of 50:50. Steady-state selectivity reached 101 for H<sub>2</sub>/CH<sub>4</sub> and 62 for CO<sub>2</sub>/CH<sub>4</sub>. Ideal selectivity measured from single gas permeation reached 475 for H<sub>2</sub>/CH<sub>4</sub> and 288 for CO<sub>2</sub>/CH<sub>4</sub>. Molecular dynamics simulations and time-resolved X-ray diffraction with a synchrotron radiation source were used to probe conformational changes in CAU-10-PDC induced by exposure to CH<sub>4</sub>. When exposed to an atmosphere containing CH<sub>4</sub>, CAU-10-PDC presented a change in the space group (from <em>I</em>4<sub>1</sub>/<em>amd</em> to <em>I</em>4<sub>1</sub>), which drastically reduced the pore limiting diameter from 4.15 to 2.95 Å, rendering the channel nearly impermeable to CH<sub>4</sub>.</p></div>\",\"PeriodicalId\":100805,\"journal\":{\"name\":\"Journal of Membrane Science Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.9000,\"publicationDate\":\"2021-12-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2772421221000052/pdfft?md5=bc88058c566daef3e0c02c1d2c0cc52a&pid=1-s2.0-S2772421221000052-main.pdf\",\"citationCount\":\"10\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Membrane Science Letters\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2772421221000052\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Membrane Science Letters","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772421221000052","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Conformational-change-induced selectivity enhancement of CAU-10-PDC membrane for H2/CH4 and CO2/CH4 separation
The separation of H2/CH4 or CO2/CH4 is critical to the purification of natural gas. Herein, we report on novel membranes with a metal-organic framework of CAU-10-PDC for the separation of these two mixtures. The dense CAU-10-PDC membranes are fabricated on a porous alumina support using the seeded growth method. An unexpected increase in selectivity was observed while testing mixed gas permeation with either H2/CH4 or CO2/CH4 at a molar ratio of 50:50. Steady-state selectivity reached 101 for H2/CH4 and 62 for CO2/CH4. Ideal selectivity measured from single gas permeation reached 475 for H2/CH4 and 288 for CO2/CH4. Molecular dynamics simulations and time-resolved X-ray diffraction with a synchrotron radiation source were used to probe conformational changes in CAU-10-PDC induced by exposure to CH4. When exposed to an atmosphere containing CH4, CAU-10-PDC presented a change in the space group (from I41/amd to I41), which drastically reduced the pore limiting diameter from 4.15 to 2.95 Å, rendering the channel nearly impermeable to CH4.