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首页> 外文期刊>Chemistry: A European journal >Three-dimensional open-frameworks based on Ln~(III) ions and open-/closed-Shell PTM ligands: Synthesis, structure, luminescence, and magnetic properties
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Three-dimensional open-frameworks based on Ln~(III) ions and open-/closed-Shell PTM ligands: Synthesis, structure, luminescence, and magnetic properties

机译：基于Ln〜（III）离子和开/闭壳PTM配体的三维开放框架：合成，结构，发光和磁性

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A series of isostructural open-framework coordination polymers formulated as [Ln(dmf)3(ptmtc)] (Ln=Sm (1), Eu (2), Gd (3), Tb (4), Dy (5); PTMTC=polychlorotriphenylmethyl tricarboxylate) and [Ln(dmf)2H 2O(αH-ptmtc)] (Ln=Sm (1′), Eu (2′), Gd (3′), Tb (4′), Dy (5′)) have been obtained by treating LnIII ions with PTMTC ligands with a radical (PTMTC~(3-)) or a closed-shell character (αH-PTMTC~(3-)). X-ray diffraction analyses reveal that these coordination polymers possess 3D architectures that combine large channels and fairly rare lattice complex T connectivity. In addition, these compounds show selective framework dynamic sorption properties. For both classes of ligands, the ability to act as an antenna in Ln sensitization processes has been investigated. No luminescence was observed for compounds 1-5, and 3′ because of the PTMTC~(3-) ligand and/or Gd~(III) ion characteristics. Conversely, photoluminescence measurements show that 1′, 2′, 4′, and 5′ emit dark orange, red, green, and dark cyan metal-centered luminescence. The magnetic properties of all of these compounds have been investigated. The nature of the {Ln-radical} exchange interaction in these compounds has been assessed by comparing the behavior of the radical-based coordination polymers 1-5 with those of the compounds with the diamagnetic ligand set. While antiferromagnetic {Sm-radical} interactions are found in 1, ferromagnetic {Ln-radical} interactions propagate in the 3D architectures of 3, 4, and 5 (Ln=Gd, Tb, and Dy, respectively). This procedure also provided access to information on the {Ln-Ln} exchange existing in these magnetic systems.
机译：一系列等构的开放框架配位聚合物，配制成[Ln（dmf）3（ptmtc）]（Ln = Sm（1），Eu（2），Gd（3），Tb（4），Dy（5）; PTTMC =聚三氯三氯甲基苯甲酸）和[Ln（dmf）2H 2O（αH-ptmtc）]（Ln = Sm（1'），Eu（2'），Gd（3'），Tb（4'），Dy（5'） ）是通过使用具有自由基（PTMTC〜（3-））或闭壳特征（αH-PTMTC〜（3-））的PTMTC配体处理LnIII离子而获得的。 X射线衍射分析表明，这些配位聚合物拥有3D结构，这些结构结合了大通道和相当罕见的晶格复杂的T连接性。另外，这些化合物显示选择性的骨架动态吸附性能。对于两种配体，已经研究了在Ln敏化过程中充当天线的能力。由于PTMTC_（3-）配体和/或Gd〜（III）离子的特性，化合物1-5和3'未观察到发光。相反，光致发光测量结果表明1'，2'，4'和5'发出以橙色，红色，绿色和深青色为中心的深金属发光。已经研究了所有这些化合物的磁性。通过比较基于自由基的配位聚合物1-5与具有抗磁性配体组的化合物的行为，已经评估了这些化合物中的{Ln-自由基}交换相互作用的性质。虽然在1中发现了反铁磁{Sm-自由基}相互作用，但铁磁{Ln-自由基}相互作用在3、4和5的3D架构中传播（分别为Ln = Gd，Tb和Dy）。该过程还提供了对这些磁性系统中现有的{Ln-Ln}交换信息的访问。

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