含柔性雙醯胺雙吡啶與四芽羧酸基的配位高分子晶體工程

巴凱達

doi:10.6840/cycu201700029

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含柔性双醯胺双吡啶与四芽羧酸基的配位高分子晶体工程

Crystal Engineering of Coordination Polymers based on Flexible Bis-pyridyl-bis-amide and Tetracarboxylate Ligands.

巴凯达 , 博士　　导师：陈志德　　

英文 DOI： 10.6840/cycu201700029

双醯胺双吡啶基； Bis-pyridyl-bis-amide Ligands

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摘要 │ 参考文献 (215) │ 国际计量

摘要〈TOP〉

本论文分五部份探讨含柔性双醯胺双吡啶与四芽羧酸基配位高分子的合成，结构与特性。
第一部分：此部份回顾了本实验室在过去几年在柔性双醯胺双吡啶的研究工作。这种配位基具有柔软的-CH2-骨架与多样性的键结模式，可经由氮原子或氧原子键结到金属原子上，在合成配位高分子上具有重大的效益。我们将回顾以此配位基或加入羧酸配位基所合成的配位高分子的结构并探讨此类配位基在配位高分子中的构型。
第二部分: 此部分报导了两对的超分子异构物:[HgBr2(GAG-L1)]∞ [L1 =  N,N-di(3-pyridyl)adipoamide] ， 1 ，[HgBr2(AAA-L1)]∞， 2 ， [HgI2(GAG-L1)]∞， 3 ，与 [HgI2(AAA-L1)]∞， 4。这四化合物以不同的方法制备，并以单晶绕射仪监定其结构。化合物1形成一个meso-helical的链状化合物，化合物2与4为一维的螺旋状化合物，而化合物3为sinusoidal链状化合物。化合物1与3的L1配位机具有GAG trans syn-syn的构型，而在化合物2与4中具有AAA trans syn-syn的构型。化合物1与3在加热或水热的条件下可可逆地转换为2与4。除此之外化合物1在固态中呈现较强的蓝紫色的萤光，化合物2与3的蓝绿萤光较弱，而化合物4侦测不到萤光。
第三部分:利用柔性配位基bis(3,5-dicarboxyphenyl)adipoamide， H4L6， bis(N-pyrid-3-ylmethyl)adipoamide， L4 与  bis(N-pyrid-3-ylmethyl) suberoamide， L5， 在水热条件下可制备四个配位高分子{[M(L6)0.5(L4)(H2O)2]H2O}n (M = Co, 5; Ni, 6) 与{[M2(L6)(L5)2(H2O)4]3H2O}n (M = Co, 7; Ni, 8)。这些化合物的结构皆以单晶绕射仪监定。化合物5 - 8具有相同的拓谱学结构，皆属2-fold交互穿透的三维结构，拓谱学名称为moganite。除此之外，两个Co(II)化合物在加热去除溶剂後具变色的特性，且可进行可逆的转换，但Ni(II)化合物不具此特性。此四化合物皆具良好的光降解能力，且Co(II)化合物效率较Ni(II)化合物为佳。
第四部分:利用柔软的四芽羧酸bis(3,5-dicarboxyphenyl) adipoamide， H4L6 与其异构物，bis(2,5-dicarboxyphenyl)adipoamide ，H4L7，以水热法制备了三个Mg(II)配位高分子[Mg2(L6)(H2O)2]2EtOH3H2O， 9 ，[Mg2(L6)(H2O)8] ， 10与 [Mg2(L7)(H2O)6]H2O， 11。其结构以单晶绕射仪监定。化合物9与10的形成与溶剂比例有关且皆为稳定的产物。化合物9的配位基形成独特的8-nonadentate构型，为三维的结构，其拓谱学为(44.66)-pcu-5-Pmna，而化合物10与11的配位基分别形成4-tetradentate 与 6-hexadentate构型，其结构分别为一维链状与具{4.62}2{42.610.83}-rtl拓谱学的三维结构。化合物9与10可进行一系列的可逆结构转换，但化合物11的结构转换则为不可逆。所有的化合物皆发生蓝色的萤光，其中化合物11的强度较佳。
      第五部分:利用三个柔软的配位基bis(3,5-dicarboxyphenyl) adipoamide ，H4L6，N,N’-bis(3-pyridyl)sebacoamide，L2 与N,N’-bis(3-pyridyl)dodecanedipoamide， L3，以水热法制备了四个配位高分子[Co(L6)0.5(H2O)3]H2O， 12， [Co(L6)0.5(L2)(H2O)]4H2O， 13， [Cd(L6)(H2O)2]2EtOH3H2O ，14 与 [HgI2(L3)]∞, 15。这些化合物的结构皆以单晶绕射仪监定。化合物12形成二维的环状结构，其拓谱学为(4.62)2(42.62.82)，化合物13为二维结构，其拓谱学为{42.82.102}{42.84}2{4}2，化合物14为三维之结构，其拓谱学为(44.66)-pcu，而化合物15为一维的链状结构。化合物12与13的热分析亦将加以探讨。

并列摘要〈TOP〉

In this dissertation, the syntheses, structures and properties of coordination polymers based on the flexible bis-pyridyl-bis-amide and/or tetracarboxylate ligands, have been extensively discussed and summarized basically in five parts. 
      Part I: The contribution of flexible bis-pyridyl-bis-amide (bpba) ligands, which are also known as versatile ligands possessing various active coordination atoms (N and O) and different flexible –CH2– skeletons, is significant in the construction of coordination polymers. In this Highlight, structures of the different dimensional networks based on the flexible bpba ligands with or without participation of auxiliary polycarboxylate ligands are discussed, along with an overview of the preparations and conformations of the ligands.
    Part II: Two pairs of Hg(II) supramolecular isomers, [HgBr2(GAG-L1)]∞ [L1 =  N,N-di(3-pyridyl)adipoamide], 1, and [HgBr2(AAA-L1)]∞, 2, and [HgI2(GAG-L1)]∞, 3, and [HgI2(AAA-L1)]∞, 4, have been successfully synthesized by various methods, and structurally characterized by single crystal X-ray crystallography. Complex 1 forms a one-dimensional (1D) meso-helical chain, 2 and 4 exhibit normal 1D helical chains, while 3 displays a 1D sinusoidal chain. The L1 ligands in 1 and 3 display GAG trans syn-syn conformation, while those in 2 and 4 adopt the AAA trans syn-syn conformation. In addition, complexes 1 and 3 can be irreversibly transformed to 2 and 4, respectively, under simple heating or hydrothermal condition. Moreover, complex 1 exhibits intense violet-blue photoluminescence in the solid state, whereas 2 and 3 display weak broad emissions in the blue-green region and 4 shows undetectable emission intensity. 
     Part III: By utilizing the flexible ligands, bis(3,5-dicarboxyphenyl)adipoamide, H4L6; bis(N-pyrid-3-ylmethyl)adipoamide, L4; and  bis(N-pyrid-3-ylmethyl) suberoamide, L5, four coordination polymers of the types {[M(L6)0.5(L4)(H2O)2]H2O}n (M = Co, 5; Ni, 6) and {[M2(L6)(L5)2(H2O)4]3H2O}n (M = Co, 7; Ni, 8) have been hydrothermally synthesized and structurally characterized by the single crystal X-ray diffraction. Complexes 5 - 8 are topologically identical coordination polymers having the moganite type 2-fold interpenetrating 4,4-connected 3D net. Additionally, both Co(II) complexes are thermochromic and exhibit the reversible structural transformation on dehydration/rehydration followed by the color change but Ni(II) complexes are unable to show such behavior. All four complexes display good photo-degradation performance and the Co(II) complexes show slightly higher efficiencies than the Ni(II) ones.
      Part IV: By using a new flexible tetracarboxylic acid, bis(3,5-dicarboxyphenyl) adipoamide, H4L6, and its isomer, bis(2,5-dicarboxyphenyl)adipoamide, H4L7, three Mg(II) coordination polymers, [Mg2(L6)(H2O)2]2EtOH3H2O, 9, [Mg2(L6)(H2O)8], 10, and [Mg2(L7)(H2O)6].H2O, 11, have been hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction. Complexes 9 and 10 are the solvent ratio dependent hydrothermally stable products. The tetracarboxylate ligand of complex 9 adopts a unique 8-nonadentate bonding mode, resulting in a three-dimensional (3D) 5-connected uninodal (44.66)-pcu-5-Pmna net, whereas those of 10 and 11 display the 4-tetradentate and 6-hexadentate bonding modes, forming a 1D linear chain and a 3,6-connected 2-nodal 3D net having {4.62}2{42.610.83}-rtl topology, respectively. Complex 9 shows a series of structural transformations on heating up to 200 oC and almost reversible structural transformation when the activated products were immersed in the mixture of ethanol and water or on hydrothermal. Likewise, complex 10 exhibits reversible structural transformation on heating/hydrothermal while 11 exhibits the irreversible structural transformations. All three complexes exhibit blue light emissions and that of complex 11 is much more intense. 
     Part V: By applying three flexible ligands, bis(3,5-dicarboxyphenyl) adipoamide, H4L6; N,N’-bis(3-pyridyl)sebacoamide, L2 and N,N’-bis(3-pyridyl)dodecanedipoamide, L3; four new coordination polymers: [Co(L6)0.5(H2O)3]H2O, 12; [Co(L6)0.5(L2)(H2O)]4H2O, 13; [Cd(L6)(H2O)2]2EtOH3H2O, 14 and [HgI2(L3)]∞, 15; have been hydrothermally synthesized and structurally characterized by the single crystal X-ray diffraction. Complex 12 forms the 2D looped like structure with (4.62)2(42.62.82) topology, while 13 possesses a 2,4,4-connected-3-nodal 2D net with the new topology {42.82.102}{42.84}2{4}2. Further, complex 14 possesses a three-dimensional (3D) 5-connected uninodal (44.66)-pcu net, whereas 15 displays a 1D linear chain. Moreover, the thermal properties of complexes 12-13 were investigated.

参考文献 ( 215 ) 〈TOP〉

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连结：
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连结：

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