Exploration of Charge-Transfer Solids Utilizing Nucleobases: Nanoarchitectures by Hydrogen-Bonds in the Ionic Assemblies of Guanine and TCNQ Derivatives
Exploration of Charge-Transfer Solids Utilizing Nucleobases: Nanoarchitectures by Hydrogen-Bonds in the Ionic Assemblies of Guanine and TCNQ Derivatives
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DOI：
10.1021/cg400059h
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发表时间：
2013-06
影响因子：
3.8
通讯作者：
T. Murata;G. Saito;Kenji Nakamura;M. Maesato;T. Hiramatsu;Y. Yoshida
中科院分区：
文献类型：
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作者：
T. Murata;G. Saito;Kenji Nakamura;M. Maesato;T. Hiramatsu;Y. Yoshida
研究了9-正丁基鸟嘌呤（BuG）与氟代四氰基醌二甲烷衍生物（FnTCNQ，n = 4，2和1）的电荷转移固体的形成和结构特征。在含甲醇（MeOH）的溶剂中形成复合物生成两种类型的盐组成的甲氧基取代的阴离子或完全离子阴离子自由基的FnTCNQ。在所有的阴离子自由基盐中，BuG分别以质子化或半质子化的形式存在，BuGH+或（BuG）（BuGH+），并形成氢键（H-键合）组装体。在这些BuGH+组装体中，FnTCNQ·-分子被固定并周期性排列，提供H-键合的聚阳离子模板。在（BuGH+）（F4 TCNQ·-）中，BuGH+二聚体通过互补氢键形成二维聚阳离子片层。F4 TCNQ·-面对面的二聚体通过与BuGH+形成氢键而形成一维（1D）分离柱。在（BuGH+）（F2 TCNQ·-）（MeOH）溶液中，BuGH+通过互补的氢键形成了一维聚阳离子带。
We studied formation and structural characteristics of charge-transfer solids of 9-n-butylguanine (BuG) with fluorinated tetracyanoquinodimethane derivatives (FnTCNQ, n = 4, 2, and 1). Complex formation in a methanol (MeOH)-containing solvent generated two types of salts composed of either a methoxy-substituted anion or a fully ionic anion radical of FnTCNQ. In all anion radical salts, BuG existed as a protonated or a hemiprotonated species, BuGH+ or (BuG)(BuGH+), respectively, and formed hydrogen-bonded (H-bonded) assemblies. In these BuGH+ assemblies, FnTCNQ•– molecules were fixed and aligned periodically, providing H-bonded polycationic templates. In (BuGH+)(F4TCNQ•–), BuGH+ dimers by complementary H-bonds formed a two-dimensional (2D) polycationic sheet. The F4TCNQ•– face-to-face dimers formed a one-dimensional (1D) segregated column aided by formation of H-bonds with BuGH+. In (BuGH+)(F2TCNQ•–)(MeOH), BuGH+ dimers by complementary double H-bonds formed a 1D polycationic ribbon supported by MeOH-media...