| 在平面构型[PdnClm]2-阴离子驱动下三种瓜环基超分子框架化合物的构筑 |
| Three Cucurbit[n]uril-Based Supramolecular Frameworks Assembled by Planar Configuration[PdnClm]2- Anions |
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| 摘要: 采用无机阴离子诱导方法，以具有平面构型的[PdnClm]2-阴离子为结构导向试剂，成功制备了3种具有框架结构特征的瓜环基超分子化合物：{Na2（H2O）6TMeQ[6]}[Pd2Cl6]·3H2O（1）、（H3O）2{CyH5Q[5]}[Pd2Cl6]·3H2O（2）及（H3O）2{Q[5]}[PdCl4]·23H2O（3）。X射线单晶衍射的结果表明：在1中，Na+离子与TMeQ[6]端口羰基氧直接配位形成一维结构的超分子链，在[Pd2Cl6]2-阴离子与TMeQ[6]的外壁作用下，进一步构筑形成三维的框架结构；在2中，在[Pd2Cl6]2-阴离子与CyH5Q[5]的外壁作用下，CyH5Q[5]以一维链有序排列，且4条CyH5Q[5]分子链可堆砌成一孔道，孔道中填充了[Pd2Cl6]2-阴离子，最终形成三维框架结构；在3中，8个[PdCl4]2-阴离子与4个Q[5]分子通过瓜环外壁相互作用，形成二维层状框架结构，层与层之间再通过非共价键作用力，最终形成三维层状框架结构。在这3种瓜环基超分子框架化合物中，[PdnClm]2-阴离子促进了瓜环分子有序化排列，形成了具有框架结构特征的自组装体。这种主要驱动力来源于瓜环的外壁作用，即瓜环"正电性外壁"与[PdnClm]2-阴离子间的离子偶极作用。 |
| 关键词: [PdnClm]2- 结构导向剂 瓜环 超分子框架 外壁作用 |
| 基金项目: 国家自然科学基金（No.51463004，51663005）资助项目。 |
| Abstract: Three novel cucurbit[n]uril-based (Q[n]-based) supramolecular frameworks(QSFs) have been successfully prepared by using the planar configuration[PdnClm]2- anion as the structure-directing agent, namely {Na2(H2O)6TMeQ[6]}[Pd2Cl6]·3H2O (1), (H3O)2{CyH5Q[5]}[Pd2Cl6]·3H2O (2) and (H3O)2{Q[5]}[PdCl4]·23H2O (3), respectively. Structural analysis reveals that using the[PdnClm]2- anion as the structure-directing agent in different Q[n] systems that can promote the orderly arrangement of Q[n]s, and contribute to the formation of QSFs with different frame structures. For 1, the carbonyl groups of TMeQ[6] bind directly to the Na（Ⅰ） ions to form 1D coordination chains, which can be further built into 3D supramolecular architecture by outer surface interactions between TMeQ[6] and the[Pd2Cl6]2- anions. For 2, under the guidance of[Pd2Cl6]2- anions, CyH5Q[5] molecules can be orderly arranged to construct a 3D structure with pores which are filled with[Pd2Cl6]2- anions, while it can be found in 3 that Q[5] molecules can also be orderly arranged by[PdCl4]2- anions to form a 3D frameworks with a 1D channel. The driving force to result in the formation of such frameworks is attributed to the outer surface interaction of Q[n]s, which is ion-dipole between the electrostatic potential positive outer surface of Q[n]s and the[PdnClm]2- anions. |
| Keywords: [PdnClm]2- structure-directing agent cucurbit[n]uril supramolecular framework outer surface interaction of Q[n]s |
| 投稿时间：2019-10-08 修订日期：2020-04-17 |
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| 程瑞雪,田飞扬,张云黔,陶朱.在平面构型[PdnClm]2-阴离子驱动下三种瓜环基超分子框架化合物的构筑[J].无机化学学报,2020,36(7):1241-1248. |
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