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首页> 外文期刊>Crystal growth & design >Single-crystal-to-single-crystal structural transformation in a three-dimensional bimetallic (4f-3d) supramolecular porous framework
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Single-crystal-to-single-crystal structural transformation in a three-dimensional bimetallic (4f-3d) supramolecular porous framework

机译：三维双金属（4f-3d）超分子多孔框架中的单晶到单晶结构转变

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摘要

A three-dimensional (3D) bimetallic (4f-3d) supramolecular framework, {[Nd(pyno)_2(H_2O)_4][Fe(CN)_6]?H _2O}_n (1) (pyno = pyridine-N-oxide), has been synthesized and structurally characterized. Structure determination reveals that one-dimensional (1D) cyano-bridged chains of Nd~(III) and Fe ~(III) form an alternative basket-like arrangement and are connected by (O-HN) H-bonding interactions through coordinated water molecules and pendent CN groups forming a two-dimensional (2D) sheet-like structure. 2D sheets are further connected by another set of similar (O-HN) interactions resulting in a 3D supramolecular framework with 1D water-filled channels. Controlled heating of the as-synthesized crystal at 85 °C causes a color change from yellow to a light brown compound {[Nd(pyno)_2(H_2O)_4][Fe(CN) 6]}n (1′) and structure determination shows significant contraction of the overall framework with selective removal of the guest water molecules. 1′ exhibits a similar framework topology as 1. The dehydrated crystal (1′) regenerates the virgin as-synthesized framework (1a) with structural expansion upon exposure to the water vapor. Adsorption studies reveal that 1′ can selectively uptake H~2O but not MeOH, EtOH, and CO~2 consistent with the channel size. Removal of the guest as well as coordinated water molecules gives another phase {[Nd(pyno) _2][Fe(CN)_6]}_n (2), which shows sorption of H_2O and MeOH vapors but not CO_2. Temperature-dependent magnetic measurement (300-2 K) suggests the as-synthesized framework is antiferromagnetically coupled at low temperature.
机译：三维（3D）双金属（4f-3d）超分子框架，{[Nd（pyno）_2（H_2O）_4] [Fe（CN）_6] HH _2O} _n（1）（pyno =吡啶-N-已经合成并在结构上进行了表征。结构确定表明，Nd〜（III）和Fe〜（III）的一维（1D）氰基桥链形成了另一种篮子状排列，并通过（O-HN）H键相互作用通过协调的水分子连接悬垂的CN基团形成二维（2D）片状结构。 2D薄片通过另一组相似的（O-HN）相互作用进一步连接，从而形成具有1D充水通道的3D超分子框架。合成晶体在85°C的受控加热会导致颜色从黄色变为浅棕色化合物{[Nd（pyno）_2（H_2O）_4] [Fe（CN）6]} n（1'）和结构测定表明，选择性除去了客体水分子后，整个构架显着收缩。 1'具有与1相似的骨架拓扑。脱水晶体（1'）再生原始的合成骨架（1a），并在暴露于水蒸气时具有结构膨胀。吸附研究表明1'可以选择性地吸收H〜2O，但不能吸收与通道大小一致的MeOH，EtOH和CO〜2。除去客体以及配位的水分子得到另一相{[Nd（pyno）_2] [Fe（CN）_6]} _ n（2），该相显示了H_2O和MeOH蒸气的吸附，但没有CO_2的吸附。与温度有关的磁测量（300-2 K）表明，合成后的骨架在低温下反铁磁耦合。

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