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首页> 外文期刊>Crystal growth & design >Intermolecular hydrogen-bond networks and physical properties of BF _4 ~- and TCNQ ~(?-) salts of three-fold symmetric tris(alkylamino) phenalenyliums
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Intermolecular hydrogen-bond networks and physical properties of BF _4 ~- and TCNQ ~(?-) salts of three-fold symmetric tris(alkylamino) phenalenyliums

机译：三倍对称三（烷基氨基）苯并鎓盐的BF _4〜-和TCNQ〜（α-）盐的分子间氢键网络和物理性质

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摘要

Synthesis, redox properties, and crystal structures of tris(alkylamino) phenalenyliums (TAP) having alkyl groups (n-Pr, i-Pr, t-Bu) and their charge-transfer salts with tetracyanoquinodimethane radical anion (TCNQ ~(?-)) were investigated. The electrochemical measurements revealed that TAP exhibits two irreversible reduction processes to neutral radical and anion species. The introduction of an alkylamino group caused a large negative shift of the first reduction potential and a significant decrease of the on-site Coulomb repulsion because of the electron-donating nature of amino groups and the extension of the p-electronic system. In the crystal structures of the BF _4 ~- salts, the TAP skeleton possesses a nearly 3-fold symmetric molecular plane indicating the delocalization of positive charge. The face-to-face stack of TAP formed p-dimer or columnar structures, which were connected through intermolecular N-H···F hydrogen bonds with BF _4 ~- to construct multidimensional network structures. The TCNQ ~(?-) salts prepared by the metathesis method were characterized as fully ionic salts with a 1:1 component ratio. In the crystal structures, both TAP and TCNQ ~(?-) molecules formed p-dimers, and the intermolecular hydrogen bonds between TAP and TCNQ ~(?-) constructed a two-dimensional sheet.
机译：具有烷基（n-Pr，i-Pr，t-Bu）的三（烷基氨基）苯撑鎓（TAP）及其与四氰基喹二甲烷自由基阴离子（TCNQ〜（β-）的电荷转移盐）的合成，氧化还原性质和晶体结构）进行了调查。电化学测量表明，TAP对中性自由基和阴离子具有两种不可逆的还原过程。烷基氨基的引入由于氨基的供电子特性和p电子系统的扩展，引起第一还原电位的较大负移，并导致现场库仑排斥的显着降低。在BF_4〜-盐的晶体结构中，TAP骨架具有接近3倍的对称分子平面，表明正电荷的离域。 TAP的面对面堆叠形成p-二聚体或柱状结构，它们通过分子间N-H···F氢键与BF _4〜-连接在一起，以构建多维网络结构。通过复分解方法制备的TCNQ〜（α-）盐被表征为组分比例为1：1的全离子盐。在晶体结构中，TAP和TCNQ〜（α-）分子均形成p-二聚体，而TAP和TCNQ〜（α-）之间的分子间氢键构成了二维薄片。

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