Xiao Duoduo, Zhang Dengqing, Chen Beihua, Xie Dahai, Xiang Yunjie, Li Xianying, Jin Wusong
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University , 2999 North Renmin Road, Songjiang, Shanghai 201620, People's Republic of China.
School of Environmental Science and Engineering, Donghua University , 2999 North Renmin Road, Songjiang, Shanghai 201620, People's Republic of China.
Langmuir. 2015 Oct 6;31(39):10649-55. doi: 10.1021/acs.langmuir.5b02273.
Study of artificial tubular assemblies as a useful host scaffold for size-selective recognition and release of guest molecules is an important subject in host-guest chemistry. We describe well-defined self-assembled nanotubes (NT6mer) formed from π-conjugated m-phenylene-pyrimidinylene alternated macrocycle 16mer that exhibit size-selective recognition toward a specific aromatic acid. In a series of guest molecules, a size-matched trimesic acid (G3) gives inclusion complexes (NT6mer⊃G3) in dichloromethane resulting in an enhanced and red-shifted fluorescence. (1)H nuclear magnetic resonance (NMR) titration experiments indicated that the complex was formed in a 1:1 molar ratio. Density functional theory (DFT) calculations and the binding constant value (K = 1.499 × 10(5) M(-1)) of NT6mer with G3 suggested that the complex involved triple hydrogen-bonding interactions. The encapsulated guest G3 molecules can be readily released from the tubular channel through the dissociation of hydrogen bonding by the addition of a polar solvent such as dimethylsulfoxide (DMSO). In contrast, 16mer could not form self-assembled nanotubes in CHCl3 or tetrahydrofuran (THF) solution, leading to weak or no size-selective recognizability, respectively.
将人工管状组装体作为用于客体分子的尺寸选择性识别和释放的有用主体支架进行研究是主客体化学中的一个重要课题。我们描述了由π共轭间亚苯基 - 嘧啶撑交替大环16聚体形成的定义明确的自组装纳米管(NT6聚体),其对特定芳香酸表现出尺寸选择性识别。在一系列客体分子中,尺寸匹配的均苯三甲酸(G3)在二氯甲烷中形成包合物(NT6聚体⊃G3),导致荧光增强和红移。氢核磁共振(NMR)滴定实验表明该配合物以1:1的摩尔比形成。密度泛函理论(DFT)计算以及NT6聚体与G3的结合常数(K = 1.499 × 10⁵ M⁻¹)表明该配合物涉及三重氢键相互作用。通过加入极性溶剂如二甲基亚砜(DMSO)使氢键解离,封装的客体G3分子可以很容易地从管状通道中释放出来。相比之下,16聚体在CHCl₃或四氢呋喃(THF)溶液中不能形成自组装纳米管,分别导致尺寸选择性识别能力较弱或没有。