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首页> 外文期刊>Chemistry: A European journal >Construction of Open Metal-Organic Frameworks Based on Predesigned Carboxylate Isomers:From Achiral to Chiral Nets
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Construction of Open Metal-Organic Frameworks Based on Predesigned Carboxylate Isomers:From Achiral to Chiral Nets

机译：基于预先设计的羧酸盐异构体的开放金属有机骨架的构建：从手性网络到手性网络

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摘要

The four-connected carboxylate ligand N,N,N',N'-tetrakis(4-carboxyphenyl)-1,4-phenylenediamine(TCPPDA)exists as three stereoisomers:a pair of enantiomers(~(delta)D_2-and ~(gamma)D_2-TCPPDA)and a diastereomer(C_(2h)-TCPPDA).TCPPDA was predesigned for the construction of isomeric coordination networks.Reactions of M(NO_3)_2(M=Cu,Zn,Co)or Nd(NO)_3 with TCPPDA under solvo-thermal conditions gave rise to five novel porous metal-organic frame works: [Cu_2(D_2-tcppda)-(H_2O)_2] centre dot 2DMSO centre dot 6H_2O(1),[Cu_2(C_(2h)-tcppda)(H_2O)_2] centre dot 2DMS06H_2O(2),[Co_3(D_2-Htcppda)_2] centre dot 4DEF centre dot 5H_2O(3),[Nd_2(D_2-tcppda)(C_(2h)-tcppda)_(0.5)-(DMSO)_3] centre dot 3DMSO centre dot 5H_2O(4),and [Zn_4O(D_2-tcppda)_(1.5)] centre dot DMF centre dot H_2O(5)(DMSO=dimethyl sulfoxide,DEF=diethylformamide,DMF=dimethyl-formamide).Complexes 1 and 2 are su-pramolecular isomers,in which all the ligands adopt pseudotetrahedral(both ~(delta)D_2-and ~(gamma)D_2-TCPPDA)and rectangular(C_(2h)-TCPPDA)geometries,respectively.Both compounds connect pad-dlewheel secondary building units(SBUs)to form three-dimensional porous networks possessing PtS and NbO nets,respectively.In 3,all ligands possess pseudotetrahedral(both ~(delta)D_2-and ~(gamma)D_2-TCPPDA)geometry and link hourglass SBUs to form a three-dimensional porous framework.Compound 4 contains all three stereoisomers(C_(2~-),~(delta)D_2-and ~(gamma)D_2-TCPPDA),thus,has both pseudotetrahedral and rectangular geometries.D_2-TCPPDA connects the bi-nuclear neodymium units to generate a two-dimensional layer,further linked by C_(2h)TCPPDA to create a three-dimensional open framework.In 5,all the ligands possess pseudotetrahedral geometry(D_2-TCPPDA),as found in 1 and 3.However,all the TCPPDA ligands in 5 appear as either the ~(delta)D_2-or the ~(gamma)D_2 form,thus,the whole structure is homochiral.Complex 5 crystallizes in the I4_132 space group and the octahedral SBU in 5 is connected by the enantiopure TCPPDA to generate a three-dimensional porous network possessing the corundum Al_2O_3 net.Complexes 1,2,and 5 possess permanent porosity,and 4 and 5 exhibit strong luminescence at lambda_(max)=423 and 424 nm,respectively,upon excitation at 268.5 nm.
机译：四连接的羧酸酯配体N，N，N'，N'-四（4-羧苯基）-1,4-苯二胺（TCPPDA）存在三种立体异构体：一对对映异构体（〜δD_2-和〜（ γ）D_2-TCPPDA）和非对映异构体（C_（2h）-TCPPDA）.TCPPDA已预先设计用于异构异构配位网络的构建.M（NO_3）_2（M = Cu，Zn，Co）或Nd（NO）的反应溶剂热条件下用TCPPDA _3产生了五种新颖的多孔金属有机框架：[Cu_2（D_2-tcppda）-（H_2O）_2]中心点2DMSO中心点6H_2O（1），[Cu_2（C_（2h） -tcppda）（H_2O）_2]中心点2DMS06H_2O（2），[Co_3（D_2-Htcppda）_2]中心点4DEF中心点5H_2O（3），[Nd_2（D_2-tcppda）（C_（2h）-tcppda）_ （0.5）-（DMSO）_3]中心点3DMSO中心点5H_2O（4）和[Zn_4O（D_2-tcppda）_（1.5）]中心点DMF中心点H_2O（5）（DMSO =二甲基亚砜，DEF =二乙基甲酰胺，配合物1和2是超分子异构体，其中所有配体均采用伪四面体（〜δD_2-和〜γD_2-TCPPDA）和矩形（C_（2 h）-TCPPDA）的几何形状。这两种化合物都连接桨叶轮辅助建筑单元（SBU），分别形成具有PtS和NbO网的三维多孔网络。3，所有配体均具有伪四面体（〜δDD_2） -和〜（γ_D_2-TCPPDA）几何形状并链接沙漏SBU以形成三维多孔框架。化合物4包含所有三个立体异构体（C_（2〜-），〜δD_2-和〜γD_2 -TCPPDA），因此具有伪四面体和矩形几何形状。D_2-TCPPDA连接双核钕单元以生成二维层，并通过C_（2h）TCPPDA进一步链接以创建三维开放框架。5 ，所有配体都具有伪四面体几何形状（D_2-TCPPDA），如在1和3中所见。但是，5中的所有TCPPDA配体都以〜δD_2-或〜γD_2形式出现，因此，复杂的5在I4_132空间群中结晶，而5中的八面体SBU通过对映纯TCPPDA连接到这是一个具有刚玉Al_2O_3网的三维多孔网络。复合物1,2和5具有永久孔隙，并且4和5在268.5 nm激发时分别在lambda_（max）= 423和424 nm处显示强发光。

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