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Self-Assembly and Properties of a Discrete Water-Soluble Prussian Blue Analogue FeII/CoIII Cube: Confinement of a Water Molecule in Aqueous Solution.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-01-13 , DOI: 10.1021/acs.inorgchem.9b03274 Miguel A Gonzálvez 1 , Albert Gallen 1 , Montserrat Ferrer 1 , Manuel Martínez 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-01-13 , DOI: 10.1021/acs.inorgchem.9b03274 Miguel A Gonzálvez 1 , Albert Gallen 1 , Montserrat Ferrer 1 , Manuel Martínez 1
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Novel types of water-soluble anionic cubic cages, K4[{CoIII(Me3-Tacn)}4{FeII(CN)6}4] and Na4[{CoIII(Me3-Tacn)}4{FeII(CN)6}4] (Me3-Tacn = 1,4,7-trimethyl-1,4,7-triazacyclononane), were prepared by means of a mechanistically designed self-assembly process between [Co(Me3-Tacn)Cl3] and A4[FeII(CN)6] (M = Na or K), consisting of a rate-limiting outer-sphere redox step, followed by a fast substitution/inner-sphere redox reaction sequence. These compounds show remarkable stability in aqueous solution at different pH ranges, displaying neat protonation processes and reversible oxidation with peroxodisulfate to its neutral {FeIII4CoIII4} form. Furthermore, the cages behave as a robust and water-soluble molecular Prussian Blue analogue capable of encapsulating {Na-OH2}+ pairs and K+ cations in aqueous solution, with the cubic structure of the complex being preserved. Substitution of the {Na-OH2}+ pairs by K+ is easily accomplished, and the electrochemical properties of the sodium and potassium salts of the new cages have been found to be dramatically dependent on the encapsulated units.
中文翻译：
离散水溶性普鲁士蓝类似物FeII / CoIII立方体的自组装和性质：水溶液中水分子的限制。
新型的水溶性阴离子立方笼，K4 [{CoIII（Me3-Tacn）} 4 {FeII（CN）6} 4]和Na4 [{CoIII（Me3-Tacn）} 4 {FeII（CN）6} 4 ]] [Me3-Tacn = 1,4,7-三甲基-1,4,7-三氮杂环壬烷）是通过机械设计的[Co（Me3-Tacn）Cl3]与A4 [FeII（ CN）6]（M = Na或K），由限速外球氧化还原步骤组成，然后进行快速取代/内球氧化还原反应。这些化合物在不同pH范围内在水溶液中显示出显着的稳定性，显示出纯净的质子化过程，并与过二硫酸盐可逆氧化为中性{FeIII4CoIII4}形式。此外，笼子的作用类似于坚固的水溶性分子普鲁士蓝类似物，能够将{Na-OH2} +对和K +阳离子包封在水溶液中，保留了复杂的立方结构。{Na-OH2} +对被K +取代很容易实现，并且发现新笼的钠盐和钾盐的电化学性质极大地取决于所包封的单元。
更新日期：2020-01-13
中文翻译：
离散水溶性普鲁士蓝类似物FeII / CoIII立方体的自组装和性质：水溶液中水分子的限制。
新型的水溶性阴离子立方笼，K4 [{CoIII（Me3-Tacn）} 4 {FeII（CN）6} 4]和Na4 [{CoIII（Me3-Tacn）} 4 {FeII（CN）6} 4 ]] [Me3-Tacn = 1,4,7-三甲基-1,4,7-三氮杂环壬烷）是通过机械设计的[Co（Me3-Tacn）Cl3]与A4 [FeII（ CN）6]（M = Na或K），由限速外球氧化还原步骤组成，然后进行快速取代/内球氧化还原反应。这些化合物在不同pH范围内在水溶液中显示出显着的稳定性，显示出纯净的质子化过程，并与过二硫酸盐可逆氧化为中性{FeIII4CoIII4}形式。此外，笼子的作用类似于坚固的水溶性分子普鲁士蓝类似物，能够将{Na-OH2} +对和K +阳离子包封在水溶液中，保留了复杂的立方结构。{Na-OH2} +对被K +取代很容易实现，并且发现新笼的钠盐和钾盐的电化学性质极大地取决于所包封的单元。
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