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首页> 外文期刊>Crystal growth & design >Driving the assembling of zirconium tetraoxalate metallotectons and benzimidazolium cations: From three dimensional hydrogen-bonded compact architectures to open-frameworks
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Driving the assembling of zirconium tetraoxalate metallotectons and benzimidazolium cations: From three dimensional hydrogen-bonded compact architectures to open-frameworks

机译：推动四草酸锆金属弹体和苯并咪唑鎓阳离子的组装：从三维氢键致密结构到开放框架

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Charge-assisted H-bond associations between [Zr(C_2O _4)_4]~(4-) preformed anionic complexes and several ditopic monocations based on the benzimidazolium motif ([H_(2-)Bim] ~+ cations) have been envisioned for the tentative elaboration of 3D H-bonded and open-framework architectures. Reactions involving [Zr(C _2O_4)_4]~(4-) units and [H _(2-)Bim]~+ cations in (a) a charge stoichiometric amount, (b) a defect, and (c) an excess of cation afforded three different compounds of formula {(H_2-Bim)_4[Zr(C_2O_4) _4]}·H_2O (1), {K(H_2O)(H _(2-)Bim)_3[Zr(C_2O_4)_4]} ·2H_2O (2), and {(H_(2-)Bim)_4[Zr(C _2O_4)_4]} (3), respectively. Structural analyses revealed marked differences in their formulations and in their supramolecular connectivities. These results traduce the importance of cation concentration on the association schemes. Among them, compound 3 exhibits a chiral structure analyzed as resulting from the interpenetration of two 3D H-bonded homochiral and independent networks. To avoid this interpenetration and to study the influence of the cation substitution for fixed experimental parameters, 2-amino and 2-methyl substituted [H_2-Bim]~+ cations ([H _2-2-NH_2Bim]~+ and [H_2-2-MeBim] ~+, respectively) have been envisioned as cationic building-blocks. Structure analysis for the corresponding materials ({(H_2-2-NH _2Bim)_4[Zr(C_2O_4)_4]} (4) and {(H_2-2-MeBim)_4[Zr(C_2O_4) _4]}·7H_2O (5), respectively) revealed that the amino group contributes in the H-bonded framework, whereas the methyl impairs the formation of H-bonds between the cations and the anions. These observations contribute to explain the marked structural differences between 3 and these two networks. With 5-methyl-and 5-chlorobenzimidazolium cations ([H _2-5-MeBim]~+ and [H_2-5-ClBim]~+, respectively), [Zr(C_2O_4)_4]_4- is converted into its binuclear version, [Zr_2(C_2O _4)_7]~(6-), yielding {(H_2-5-MeBim) _6[Zr_2(C_2O_4)_7]} ·3H_2O (6) with a close-packed 3D-network and {(H _2-5-ClBim)_6[Zr_2(C_2O _4)_7]}·13.5H_2O (7) with an open-framework architecture (potential solvent accessible void volume of 23%). For 7, Cl?π interactions contribute to the cohesion of the 3D supramolecular architecture.
机译：[Zr（C_2O _4）_4]〜（4-）形成的阴离子络合物与基于苯并咪唑鎓基序的几个二位单阳离子（[H_（2-）Bim]〜+阳离子）之间的电荷辅助氢键缔合3D H键合和开放框架架构的初步阐述。 （a）电荷化学计量的量，（b）缺陷和（c）过量的涉及[Zr（C _2O_4）_4]〜（4-）单元和[H _（2-）Bim]〜+阳离子的反应阳离子得到三种不同的式{（H_2-Bim）_4 [Zr（C_2O_4）_4]}·H_2O（1），{K（H_2O）（H _（2-）Bim）_3 [Zr（C_2O_4）_4 ]}·2H_2O（2）和{（H_（2-）Bim）_4 [Zr（C _2O_4）_4]}（3）。结构分析表明，它们的配方和超分子连接性存在明显差异。这些结果证明了阳离子浓度对缔合方案的重要性。其中，化合物3表现出由两个3D H键合的手性和独立网络的互穿所导致的手性结构。为避免这种相互渗透并研究阳离子取代对固定实验参数的影响，使用2-氨基和2-甲基取代的[H_2-Bim]〜+阳离子（[H _2-2-NH_2Bim]〜+和[H_2-2 -MeBim]〜+）分别被设想为阳离子结构单元。相应材料（{（H_2-2-NH _2Bim）_4 [Zr（C_2O_4）_4]}（4）和{（H_2-2-MeBim）_4 [Zr（C_2O_4）_4]}·7H_2O（5的结构分析））分别表明，氨基在氢键构架中起重要作用，而甲基则损害了阳离子和阴离子之间的氢键形成。这些观察有助于解释3和这两个网络之间明显的结构差异。使用5-甲基和5-氯苯并咪唑鎓阳离子（分别为[H _2-5-MeBim]〜+和[H_2-5-ClBim]〜+），将[Zr（C_2O_4）_4] _4-转换为双核形式，[Zr_2（C_2O _4）_7]〜（6-），得到{（H_2-5-MeBim）_6 [Zr_2（C_2O_4）_7]}·3H_2O（6），它带有紧凑的3D网络和{（H _2-5-ClBim）_6 [Zr_2（C_2O _4）_7]}·13.5H_2O（7）具有开放式框架结构（潜在的溶剂可及空隙体积为23％）。对于7，Clαπ相互作用有助于3D超分子体系结构的内聚。

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