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首页> 外文期刊>Crystal growth & design >Structure-directing effect of organic cations in the assembly of anionic In(III)/diazinedicarboxylate architectures
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Structure-directing effect of organic cations in the assembly of anionic In(III)/diazinedicarboxylate architectures

机译：阴离子In（III）/二嗪二羧酸酯结构组装中有机阳离子的结构导向作用

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摘要

We report herein the synthesis and physicochemical characterization of seven new indium-pyrazine-2,5-dicarboxylato (pzdc) and pyridazine-3,6- dicarboxylato (pddc) compounds: (dma) _6[In _6(μ-pzdc) _(12)]?xH _2O (1), (dea) _6[In _6(μ-pzdc) _(12)]?xH _2O (2), {(tma)[In(μ-pzdc) _2]?2H _2O} _n (3), {(dea)[In(μ-pzdc) _2]?2H _2O} _n (4), {(dma)[In(μ-pddc) _2]?xH _2O} _n (5), {(dma)[In(μ-pddc) _2]} _n (6), and (dma) _4[In _8(μ-pddc) _(12)(H _2O) _8(OH) _4]?xH _2O (7) (where dma = dimethylammonium, dea = diethylammonium, tma = tetramethylammonium). Two types of In(III)/pzdc structures have been obtained. The first one (1 and 2) is comprised of discrete hexanuclear anionic assemblies held together by hydrogen bonding interactions through the organic cations generated by the thermal hydrolysis of the amide solvents. The second one (3 and 4) consists of an anionic three-dimensional (3D) framework with channels that are occupied by the counterions and solvent molecules. The first type of structure seems to be the kinetically preferred one since it is obtained when using relatively soft solvothermal conditions (120 °C) and counterions that are able to establish relatively strong hydrogen bonding interactions. The 3D frameworks crystallize when the organic counterion is unable to establish hydrogen bonding interactions or when employing a higher temperature (150 °C). The metal-organic assemblies obtained in the In(III)/pddc system range from two-dimensional (2D) sheets (5 and 6) to discrete octameric entities (7) depending on the amount of water in the reaction mixture. It is worth noting that the open lamellar crystal structure of compound 5 undergoes a solid state transformation accompanied by the release of water molecules, rendering the solvent free 2D architecture of 6 that exhibits a different connectivity. Surprisingly, a prolonged exposure of 6 to a water saturated atmosphere does not revert to 5 but promotes a partial and reversible transformation to give a new unidentified In-pddc compound.
机译：我们在这里报告了七个新的铟-吡嗪-2,5-二羧基（pzdc）和哒嗪-3,6-二羧基（pddc）化合物的合成和理化性质：（dma）_6 [In _6（μ-pzdc）_（ 12）]？xH _2O（1），（dea）_6 [In _6（μ-pzdc）_（12）]？xH _2O（2），{（tma）[In（μ-pzdc）_2]？2H _2O } _n（3），{（dea）[In（μ-pzdc）_2]？2H _2O} _n（4），{（dma）[In（μ-pddc）_2]？xH _2O} _n（5）， {（dma）[In（μ-pddc）_2]} _n（6）和（dma）_4 [In _8（μ-pddc）_（12）（H _2O）_8（OH）_4]？xH _2O（ 7）（其中dma =二甲基铵，dea =二乙基铵，tma =四甲基铵）。已获得两种类型的In（III）/ pzdc结构。第一个（1和2）由离散的六核阴离子组件组成，这些组件通过酰胺溶剂热水解生成的有机阳离子通过氢键相互作用而保持在一起。第二个（3和4）由阴离子三维（3D）骨架组成，该骨架具有被反离子和溶剂分子占据的通道。第一种结构似乎是动力学上优选的结构，因为它是在使用相对较弱的溶剂热条件（120°C）和能够建立相对较强的氢键相互作用的抗衡离子时获得的。当有机抗衡离子无法建立氢键相互作用或使用较高温度（150°C）时，3D框架会结晶。在In（III）/ pddc系统中获得的金属有机组件的范围从二维（2D）薄片（5和6）到离散的八聚体（7），具体取决于反应混合物中的水量。值得注意的是，化合物5的开放层状晶体结构经历了固态转变，并伴随着水分子的释放，使6的无溶剂2D结构呈现出不同的连通性。出乎意料的是，长时间将6暴露在水饱和的气氛中不会恢复到5，而是促进了部分和可逆的转化，从而生成了一种新的未知In-pddc化合物。

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