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首页> 外文期刊>Chemistry: A European journal >Rational synthesis of supramolecular assemblies based on tetraplatinum units: Synthesis, characterization, and selective substitution reactions of four different Pt4 clusters
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Rational synthesis of supramolecular assemblies based on tetraplatinum units: Synthesis, characterization, and selective substitution reactions of four different Pt4 clusters

机译：基于四铂单元的超分子组装的合理合成：四种不同Pt4簇的合成，表征和选择性取代反应

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摘要

Four different types of square-planar Pt4 clusters, trans-[Pt_4(μ-OCOCH_3)_6(μ-ArNCHNAr) _2] (2: ArNCHNAr=N,N′-diarylformamidinate), [Pt _4(μ-OCOCH_3)_7(μ-ArNCHNAr)] (8), cis-[Pt_4(μ-OCOCH_3)_6(κ~4- N4-DArBp)] (9: DArBp=1,3-bis(arylbenzamidinate)propane), and [Pt _4Cl2(μ-OCOCH_3)_5(κ ~4-N_2,P_2-dpfam)] (13: dpfam=N,N′-bis[(2- diphenylphosphino)phenyl]formamidinate), were successfully prepared by using selective substitution reactions of in-plane acetate ligands of [Pt _4(μ-OCOCH_3)_8] (1), which has four in-plane and four out-plane acetate ligands, with appropriate capping ligands. Fundamental substitution reactions of the remaining in-plane acetates with benzoic acid derivatives were also investigated. All newly prepared complexes were characterized from spectral and physical data and combustion analysis. X-ray crystallographic studies of some of the clusters were also performed. Electrochemical measurements of amidinate-modified Pt4 clusters revealed stepwise oxidation processes of the Pt4 core due to Pt _4~(9+)/Pt_4~(8+) and Pt_4~(10)+/Pt_4(9+). Based on the lability of the in-plane acetate ligands of the modified Pt4 clusters, reactions of cis-[Pt4(μ-OCOCH_3)_6(κ~4- N4-DArBp)] (9 c: Ar=C_6H_4tBu-4) with ferrocenedicarboxylic acid and p-phenylenedipropionic acid resulted in the selective formation of cyclic dimers 17 and 18 and the reaction of 13 with 4,4′-biphenyldicarboxylic acid afforded a linear dimer 20. The dimers were characterized by spectral data, as well as X-ray analyses for 17 and 18. The finding of two Fe~(3+)/Fe~(2+) redox couples in the electrochemical measurement of dimer 17 indicated that two ferrocenyl units in dimer 17 communicated electronically.
机译：四种不同类型的方形Pt4簇，反-[Pt_4（μ-OCOCH_3）_6（μ-ArNCHNAr）_2]（2：ArNCHNAr = N，N'-二芳基甲酰胺基酸盐），[Pt _4（μ-OCOCH_3）_7（ μ-ArNCHNAr）]（8），顺式-[Pt_4（μ-OCOCH_3）_6（κ〜4- N4-DArBp）]（9：DArBp = 1,3-双（芳基苯甲酰胺基）丙烷）和[Pt _4Cl2（ μ-OCOCH_3）_5（κ〜4-N_2，P_2-dpfam）]（13：dpfam = N，N'-双[（2-二苯基膦基）苯基]甲酰胺基）成功制备出来， [Pt _4（μ-OCOCH_3）_8]（1）的平面乙酸盐配体，具有四个面内和四个面外乙酸盐配体，并带有适当的封端配体。还研究了剩余的平面内乙酸酯与苯甲酸衍生物的基本取代反应。所有新制备的配合物均通过光谱和物理数据以及燃烧分析进行表征。还对某些团簇进行了X射线晶体学研究。 mid胺修饰的Pt4团簇的电化学测量显示，由于Pt _4〜（9 +）/ Pt_4〜（8+）和Pt_4〜（10）+ / Pt_4（9 +），Pt4核的逐步氧化过程。根据修饰的Pt4簇的面内乙酸酯配体的不稳定性，顺式[Pt4（μ-OCOCH_3）_6（κ〜4- N4-DArBp）]（9 c：Ar = C_6H_4tBu-4）与二茂铁羧酸和对苯二丙酸导致选择性形成环状二聚体17和18，13与4,4'-联苯二甲酸的反应得到线性二聚体20。二聚体的特征在于光谱数据以及X-射线分析17和18。在二聚体17的电化学测量中发现两个Fe〜（3 +）/ Fe〜（2+）氧化还原对表明二聚体17中的两个二茂铁单元电子连通。

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