Wang Yan-Ning, Huo Qi-Sheng, Zhang Ping, Yu Jie-Hui, Xu Ji-Qing
College of Chemistry, Jilin University, Changchun, Jilin 130012, China; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun, Jilin 130012, China.
College of Chemistry, Jilin University, Changchun, Jilin 130012, China.
Spectrochim Acta A Mol Biomol Spectrosc. 2016 Oct 5;167:33-40. doi: 10.1016/j.saa.2016.05.021. Epub 2016 May 20.
By utilizing the hydrothermal in situ acylation of organic acids with N2H4, three acylhydrazidate-coordinated compounds [Mn(L1)2(H2O)2] (L1=2,3-quinolinedicarboxylhydrazidate; HL1=2,3-dihydropyridazino[4,5-b] quinoline-1,4-dione) 1, [Mn2(ox)(L2)2(H2O)6]·2H2O (L2=benzimidazolate-5,6-dicarboxylhydrazide; HL2=6,7-dihydro-1H-imidazo[4,5-g]phthalazine-5,8-dione; ox=oxalate) 2, and [Cd(HL3)(bpy)] (L3=4,5-di(3'-carboxylphenyl)phthalhydrazidate; H3L3=6,7-dihydro-1H-imidazo[4,5-g]phthalazine-5,8-dione; bpy=2,2'-bipyridine) 3, as well as two acylhydrazide molecules L4 (L4=oxepino[2,3,4-de:7,6,5-d'e']diphthalazine-4,10(5H,9H)-dione) 4 and L5 (L5=4,5-dibromophthalhydrazide; L5=6,7-dibromo-2,3-dihydrophthalazine-1,4-dione) 5 were obtained. X-ray single-crystal diffraction analysis reveals that (i) 1 only possesses a mononuclear structure, but it self-assembles into a 2-D supramolecular network via the NhydrazineH⋯Nhydrazine and OwH⋯Ohydroxylimino interactions; (ii) 2 exhibits a dinuclear structure. Ox acts as the linker, while L2 just serves as a terminal ligand; (iii) In 3, L3 acts as a 3-connected node to propagate the 7-coordinated Cd(2+) centers into a 1-D double-chain structure; (iv) 4 is a special acylhydrazide molecule. Two OH groups for the intermediates 3,3'-biphthalhydrazide further lose one water molecule to form 4; (v) 5 is a common monoacylhydrazide molecule. Via the NhydrazineH⋯Ohydrazine, OhydroxyliminoH⋯Oacylamino and the π⋯π interactions, it self-assembles into a 2-D supramolecular network. The photoluminescence analysis reveals that 4 emits light with the maxima at 510nm.
通过利用有机酸与肼的水热原位酰化反应，得到了三种酰肼配位化合物[Mn(L1)2(H2O)2]（L1 = 2,3 - 喹啉二甲酰肼；HL1 = 2,3 - 二氢哒嗪并[4,5 - b]喹啉 - 1,4 - 二酮）1、[Mn2(ox)(L2)2(H2O)6]·2H2O（L2 = 苯并咪唑 - 5,6 - 二甲酰肼；HL2 = 6,7 - 二氢 - 1H - 咪唑并[4,5 - g]酞嗪 - 5,8 - 二酮；ox = 草酸根）2和[Cd(HL3)(bpy)]（L3 = 4,5 - 二(3'-羧基苯基)邻苯二甲酰肼；H3L3 = 6,7 - 二氢 - 1H - 咪唑并[4,5 - g]酞嗪 - 5,8 - 二酮；bpy = 2,2'-联吡啶）3，以及两个酰肼分子L4（L4 = 氧杂环庚并[2,3,4 - de:7,6,5 - d'e']二酞嗪 - 4,10(5H,9H) - 二酮）4和L5（L5 = 4,5 - 二溴邻苯二甲酰肼；L5 = 6,7 - 二溴 - 2,3 - 二氢酞嗪 - 1,4 - 二酮）5。X射线单晶衍射分析表明：（i）1仅具有单核结构，但通过N - 肼基H⋯N - 肼基和O - wH⋯O - 羟基亚氨基相互作用自组装成二维超分子网络；（ii）2呈现双核结构。草酸根作为连接体，而L2仅作为末端配体；（iii）在3中，L3作为三连接节点将七配位的Cd(2+)中心扩展成一维双链结构；（iv）4是一种特殊的酰肼分子。中间体3,3'-联邻苯二甲酰肼的两个OH基团进一步失去一个水分子形成4；（v）5是一种常见的单酰肼分子。通过N - 肼基H⋯O - 肼基、O - 羟基亚氨基H⋯O - 酰氨基和π⋯π相互作用，它自组装成二维超分子网络。光致发光分析表明4在510nm处发射出最大强度的光。
