Tuning the porosity of {Co12IICo8III（μ3-OH）24（X）}11+ supramolecular frameworks by reaction time for D2/H2 separation
作者机构：State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of Sciences State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University
出 版 物：《Science China Chemistry》 (中国科学:化学(英文版))
年 卷 期：2025年
核心收录：
学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 081701[工学-化学工程] 0703[理学-化学]
基 金：supported by the National Natural Science Foundation of China (22101047, 92261109, 22371280) the Natural Science Foundation of Fujian Province (2023J01219) the Self-deployment Project Research Program of Haixi Institutes, Chinese Academy of Sciences (CXZX-2023-JQ06, CXZX-2022-JQ11) the XMIREM Autonomously Deployment Project (2023GG02, 2023CX04) the FJIRSM Autonomously Deployment Project (CXZX-2022-GH02) the Project Funded by China Postdoctoral Science Foundation (2023M733496) the Recruitment Program of Global Youth Experts the Youth Innovation Promotion Association CAS (2021302)
摘 要：Systematicly tuning the porosities of porous materials is crucial for targeted gas mixture separation,yet it remains a longstanding *** a common strategy,altering the phenylene ring count in the organic building units has been exploited to adjust pore apertures in metal organic frameworks （MOFs） and covalent organic frameworks （COFs）,resulting in only a stepwise pore size variation of approximately 2.8?.Unlike MOFs and COFs,the porosities for supramolecular assembly frameworks are highly dependent on the packings of the molecular building units in the *** above strategy cannot be applied to supramolecular assembly frameworks and other strategies are required to adjust pore apertures in supramolecular frameworks,especially to achieve porous materials with the optimal pore size for D2/H2separation （～3?）.Here,we successfully modulate the porosity of supramolecular frameworks of[CoII1+12CoIII8L12（μ3-OH）24（X）]1clusters （L=mono-deprotonated 1-iminoisoindole-3-amine,X=ClO?4or Cl?） by controlling the duration of self-assembly *** simply adjusting the reaction time,we obtain three[CoII12CoIII8L12（μ3-OH）24（X）]11+supramolecular frameworks:[CoII12CoIII8（μ3-OH）24（ClO4）L12)]·（Cl）4·（HCO2）7（1）,[CoII12CoIII8L12（μ3-OH）24（Cl）]·（ClOI4）4·（Cl）6·（HCO2）·（H2O）10（2）,and[CoI12CoIII8L12（μ3-OH）24（Cl）]·（Cl）11·（H2O）12（3）.The different stacking patterns of the[CoII12CoIII8L12（μ3-OH）24（X）]11+clusters in these frameworks lead to significantly varied stabilities and *** 1 exhibits permanent porosity with interconnected channels and maintains stability under harsh *** contrast,compound 2 is nearly nonporous,and compound 3 becomes unstable upon *** pores of compound 1 show higher affinity to D2than H2,and the pore aperture diameter of compound 1 （～3.06?） meets the optimal porosity for D2/***,compound 1 demonstrates moderate D2/H2separation at 77 K (retention time:～7 min/g for D2/H2/Ne （10/10/80 vol%） in a flow of 5 mL
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