Mao Yi, Shan Wang, Shenfang Li, Shuo Zhang, Yilian Liu, Laiyu Zhang, Zifeng You, Xiongli Liu, Lin Li, Junhua Wang, Hao Wang, Qiao Zhao, Baiyan Li, Xian-He Bu
{"title":"干湿条件下乙烷与乙烯高效分离的超疏水分子选择器","authors":"Mao Yi, Shan Wang, Shenfang Li, Shuo Zhang, Yilian Liu, Laiyu Zhang, Zifeng You, Xiongli Liu, Lin Li, Junhua Wang, Hao Wang, Qiao Zhao, Baiyan Li, Xian-He Bu","doi":"10.1021/jacs.5c00658","DOIUrl":null,"url":null,"abstract":"Exploring humidity-resistant, ethane-selective adsorbents for the one-step purification of polymer-grade (>99.95%) ethylene from ethane-ethylene mixtures is of great importance, yet remains a significant challenge. To address this challenge, we present a novel strategy for constructing a “superhydrophobic molecular selector” (SMS) based on a porous organic cage (POC), which features a superhydrophobic outer surface and an inner cavity with multiple ethane-selective functional sites. The resulting SMS-POC-1 demonstrates excellent C<sub>2</sub>H<sub>6</sub> adsorption capacity (97 cm<sup>3</sup> g<sup>–1</sup> at 298 K) and C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (<i>S</i><sub>ads</sub> = 2.40 at 298 K), offering a superior trade-off between ethane adsorption capacity and C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> adsorption selectivity among all C<sub>2</sub>H<sub>6</sub>-selective adsorbents. Especially, breakthrough experiments demonstrate that SMS-POC-1 efficiently produces polymer-grade C<sub>2</sub>H<sub>4</sub> from C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> mixtures at 60% relative humidity (RH), making it the highest-selectivity adsorbent reported to date that can stably operate in a humid environment. The combination of experimental results and theoretical calculations reveals that the coexistence of a superhydrophobic outer surface and synergistic C–H···π interactions and hydrogen-bonding sites accounts for the high C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> separation performance under humid conditions for SMS-POC-1. Our work thus not only demonstrates a general strategy for guiding the design of humidity-resistant adsorption-separation materials but also presents a promising candidate for potential applications in hydrocarbon separation.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"91 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Superhydrophobic Molecular Selector for Efficient Separation of Ethane over Ethylene under Dry and Humid Conditions\",\"authors\":\"Mao Yi, Shan Wang, Shenfang Li, Shuo Zhang, Yilian Liu, Laiyu Zhang, Zifeng You, Xiongli Liu, Lin Li, Junhua Wang, Hao Wang, Qiao Zhao, Baiyan Li, Xian-He Bu\",\"doi\":\"10.1021/jacs.5c00658\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Exploring humidity-resistant, ethane-selective adsorbents for the one-step purification of polymer-grade (>99.95%) ethylene from ethane-ethylene mixtures is of great importance, yet remains a significant challenge. To address this challenge, we present a novel strategy for constructing a “superhydrophobic molecular selector” (SMS) based on a porous organic cage (POC), which features a superhydrophobic outer surface and an inner cavity with multiple ethane-selective functional sites. The resulting SMS-POC-1 demonstrates excellent C<sub>2</sub>H<sub>6</sub> adsorption capacity (97 cm<sup>3</sup> g<sup>–1</sup> at 298 K) and C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (<i>S</i><sub>ads</sub> = 2.40 at 298 K), offering a superior trade-off between ethane adsorption capacity and C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> adsorption selectivity among all C<sub>2</sub>H<sub>6</sub>-selective adsorbents. Especially, breakthrough experiments demonstrate that SMS-POC-1 efficiently produces polymer-grade C<sub>2</sub>H<sub>4</sub> from C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> mixtures at 60% relative humidity (RH), making it the highest-selectivity adsorbent reported to date that can stably operate in a humid environment. The combination of experimental results and theoretical calculations reveals that the coexistence of a superhydrophobic outer surface and synergistic C–H···π interactions and hydrogen-bonding sites accounts for the high C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> separation performance under humid conditions for SMS-POC-1. 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Superhydrophobic Molecular Selector for Efficient Separation of Ethane over Ethylene under Dry and Humid Conditions
Exploring humidity-resistant, ethane-selective adsorbents for the one-step purification of polymer-grade (>99.95%) ethylene from ethane-ethylene mixtures is of great importance, yet remains a significant challenge. To address this challenge, we present a novel strategy for constructing a “superhydrophobic molecular selector” (SMS) based on a porous organic cage (POC), which features a superhydrophobic outer surface and an inner cavity with multiple ethane-selective functional sites. The resulting SMS-POC-1 demonstrates excellent C2H6 adsorption capacity (97 cm3 g–1 at 298 K) and C2H6/C2H4 selectivity (Sads = 2.40 at 298 K), offering a superior trade-off between ethane adsorption capacity and C2H6/C2H4 adsorption selectivity among all C2H6-selective adsorbents. Especially, breakthrough experiments demonstrate that SMS-POC-1 efficiently produces polymer-grade C2H4 from C2H6/C2H4 mixtures at 60% relative humidity (RH), making it the highest-selectivity adsorbent reported to date that can stably operate in a humid environment. The combination of experimental results and theoretical calculations reveals that the coexistence of a superhydrophobic outer surface and synergistic C–H···π interactions and hydrogen-bonding sites accounts for the high C2H6/C2H4 separation performance under humid conditions for SMS-POC-1. Our work thus not only demonstrates a general strategy for guiding the design of humidity-resistant adsorption-separation materials but also presents a promising candidate for potential applications in hydrocarbon separation.
期刊介绍:
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