A Hydrogen‐Bonded yet Hydrophobic Porous Molecular Crystal for Molecular‐Sieving‐like Separation of Butane and Isobutane
Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen‐bo...
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| Published in | Angewandte Chemie International Edition Vol. 59; no. 51; pp. 23322 - 23328 |
|---|---|
| Main Authors | , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Weinheim
Wiley Subscription Services, Inc
14.12.2020
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| Edition | International ed. in English |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen‐bonded cyclic dinuclear AgI complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2–13. The seemingly rigid adsorbent shows a pore‐opening or nonporous‐to‐porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co‐adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single‐crystal X‐ray diffraction and computational simulations reveal that a trivial guest‐induced structural transformation plays a critical role.
A rigid hydrogen‐bonded porous molecular crystal shows not only exceptionally high hydrophobicity and chemical stability, but also molecular‐sieving‐like separation of butane/isobutane associated with a trivial guest‐induced structural transformation revealed by powder/single‐crystal X‐ray diffraction and computational simulations. |
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| AbstractList | Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen-bonded cyclic dinuclear AgI complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2-13. The seemingly rigid adsorbent shows a pore-opening or nonporous-to-porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co-adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single-crystal X-ray diffraction and computational simulations reveal that a trivial guest-induced structural transformation plays a critical role.Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen-bonded cyclic dinuclear AgI complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2-13. The seemingly rigid adsorbent shows a pore-opening or nonporous-to-porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co-adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single-crystal X-ray diffraction and computational simulations reveal that a trivial guest-induced structural transformation plays a critical role. Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen‐bonded cyclic dinuclear AgI complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2–13. The seemingly rigid adsorbent shows a pore‐opening or nonporous‐to‐porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co‐adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single‐crystal X‐ray diffraction and computational simulations reveal that a trivial guest‐induced structural transformation plays a critical role. Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen‐bonded cyclic dinuclear AgI complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2–13. The seemingly rigid adsorbent shows a pore‐opening or nonporous‐to‐porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co‐adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single‐crystal X‐ray diffraction and computational simulations reveal that a trivial guest‐induced structural transformation plays a critical role. A rigid hydrogen‐bonded porous molecular crystal shows not only exceptionally high hydrophobicity and chemical stability, but also molecular‐sieving‐like separation of butane/isobutane associated with a trivial guest‐induced structural transformation revealed by powder/single‐crystal X‐ray diffraction and computational simulations. Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient adsorptive separation because of poor structural robustness and tailorability. Herein, we report a porous molecular crystal based on hydrogen‐bonded cyclic dinuclear Ag I complex, which exhibits exceptional hydrophobicity with a water contact angle of 134°, and high chemical stability in water at pH 2–13. The seemingly rigid adsorbent shows a pore‐opening or nonporous‐to‐porous type butane adsorption isotherm and complete exclusion of isobutane, indicating potential molecular sieving. Quantitative column breakthrough experiments show slight co‐adsorption of isobutane with an experimental butane/isobutane selectivity of 23, and isobutane can be purified more efficiently than for butane. In situ powder/single‐crystal X‐ray diffraction and computational simulations reveal that a trivial guest‐induced structural transformation plays a critical role. |
| Author | Huang, Ning‐Yu Zhou, Dong‐Dong Zhang, Jie‐Peng Liao, Pei‐Qin Xie, Yi Liu, De‐Xuan Ye, Zi‐Ming Zhang, Xue‐Wen Wang, Chao Zhang, Xue‐Feng Qiu, Ze‐Hao Xu, Yan‐Tong He, Chun‐Ting |
| Author_xml | – sequence: 1 givenname: Zi‐Ming surname: Ye fullname: Ye, Zi‐Ming organization: Sun Yat-Sen University – sequence: 2 givenname: Xue‐Wen surname: Zhang fullname: Zhang, Xue‐Wen organization: Sun Yat-Sen University – sequence: 3 givenname: Pei‐Qin surname: Liao fullname: Liao, Pei‐Qin organization: Sun Yat-Sen University – sequence: 4 givenname: Yi surname: Xie fullname: Xie, Yi organization: Sun Yat-Sen University – sequence: 5 givenname: Yan‐Tong surname: Xu fullname: Xu, Yan‐Tong organization: Sun Yat-Sen University – sequence: 6 givenname: Xue‐Feng surname: Zhang fullname: Zhang, Xue‐Feng organization: Sun Yat-Sen University – sequence: 7 givenname: Chao surname: Wang fullname: Wang, Chao organization: Sun Yat-Sen University – sequence: 8 givenname: De‐Xuan surname: Liu fullname: Liu, De‐Xuan organization: Sun Yat-Sen University – sequence: 9 givenname: Ning‐Yu surname: Huang fullname: Huang, Ning‐Yu organization: Sun Yat-Sen University – sequence: 10 givenname: Ze‐Hao surname: Qiu fullname: Qiu, Ze‐Hao organization: Sun Yat-Sen University – sequence: 11 givenname: Dong‐Dong surname: Zhou fullname: Zhou, Dong‐Dong organization: Sun Yat-Sen University – sequence: 12 givenname: Chun‐Ting surname: He fullname: He, Chun‐Ting email: hct@jxnu.edu.cn organization: Ministry of Education – sequence: 13 givenname: Jie‐Peng orcidid: 0000-0002-2614-2774 surname: Zhang fullname: Zhang, Jie‐Peng email: zhangjp7@mail.sysu.edu.cn organization: Sun Yat-Sen University |
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| Snippet | Porous molecular crystals sustained by hydrogen bonds and/or weaker connections are an intriguing type of adsorbents, but they rarely demonstrate efficient... |
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| SubjectTerms | Adsorbents Adsorption adsorptive separation Adsorptivity Bonding strength Butane Computer applications Contact angle Crystal structure Crystals Hydrogen Hydrogen bonding Hydrogen bonds hydrogen-bonded organic frameworks (HOFs) Hydrophobicity molecular sieve Selectivity Separation single-crystal-to-single-crystal |
| Title | A Hydrogen‐Bonded yet Hydrophobic Porous Molecular Crystal for Molecular‐Sieving‐like Separation of Butane and Isobutane |
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