Hierarchical Self-Organization of AB (n) Dendron-like Molecules into a Supramolecular Lattice Sequence.
Hierarchical Self-Organization of AB (n) Dendron-like Molecules into a Supramolecular Lattice Sequence.
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AB(n) 树突状分子的分层自组织成超分子晶格序列
DOI：
10.1021/acscentsci.7b00188
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发表时间：
2017-08-23
影响因子：
18.2
通讯作者：
Cheng SZD
中科院分区：
文献类型：
--
作者：
Feng X;Zhang R;Li Y;Hong YL;Guo D;Lang K;Wu KY;Huang M;Mao J;Wesdemiotis C;Nishiyama Y;Zhang W;Zhang W;Miyoshi T;Li T;Cheng SZD
为了理解软材料的分级自组织行为及其对分子几何结构的依赖性，设计并合成了一系列基于多面体低聚倍半硅氧烷（POSS）纳米粒子的ABn树枝状分子.这些分子的顶点是具有14个羟基的亲水性POSS笼（表示为DPOSS）。在其外围，存在不同数量（n = 1-8）的具有七个异丁基基团的疏水POSS笼（表示为BPOSS），其经由柔性树枝化基元型接头连接至顶端DPOSS。通过改变BPOSS数从1到7，超分子晶格形成序列从片层（DPOSS-BPOSS），双回转体（空间群Ia 3 → d，DPOSS-BPOSS 2），六方柱（P6 mm平面组，DPOSS-BPOSS 3），Frank-Kasper A15（空间群Pm 3/mnm，DPOSS-BPOSS 4，DPOSS-BPOSS 5，和DPOSS-BPOSS 6），到Frank-Kasper sigma（空间群P42/mnm，DPOSS-BPOSS 7）相。在这一系列的ABn树枝状分子的纳米结构的形成主要是由分子的几何形状。此外，在每个球形图案内，球形核心由具有柔性连接的亲水性DPOSS笼组成，而疏水性BPOSS笼形成相对刚性的壳，并与邻居接触以提供减少的球形图案之间的界面，用于在这些Frank-Kasper晶格中构建最终的多面体图案。该研究提供了具有特定几何形状和官能团的分子的设计原理，以实现预期的结构和宏观性质。合成了一系列ABn树枝状分子，并研究了其主要由大分子几何形状指导的自组装纳米结构。
To understand the hierarchical self-organization behaviors of soft materials as well as their dependence on molecular geometry, a series of ABn dendron-like molecules based on polyhedral oligomeric silsesquioxane (POSS) nanoparticles were designed and synthesized. The apex of these molecules is a hydrophilic POSS cage with 14 hydroxyl groups (denoted DPOSS). At its periphery, there are different numbers (n = 1–8) of hydrophobic POSS cages with seven isobutyl groups (denoted BPOSS), connected to the apical DPOSS via flexible dendron type linker(s). By varying the BPOSS number from one to seven, a supramolecular lattice formation sequence ranging from lamella (DPOSS-BPOSS), double gyroid (space group of Ia3̅d, DPOSS-BPOSS2), hexagonal cylinder (plane group of P6mm, DPOSS-BPOSS3), Frank–Kasper A15 (space group of Pm3̅n, DPOSS-BPOSS4, DPOSS-BPOSS5, and DPOSS-BPOSS6), to Frank–Kasper sigma (space group of P42/mnm, DPOSS-BPOSS7) phases can be observed. The nanostructure formations in this series of ABn dendron-like molecules are mainly directed by the molecular geometric shapes. Furthermore, within each spherical motif, the spherical core consists hydrophilic DPOSS cages with flexible linkages, while the hydrophobic BPOSS cages form the relative rigid shell, and contact with neighbors to provide decreased interfaces among the spherical motifs for constructing final polyhedral motifs in these Frank–Kasper lattices. This study provides the design principle of molecules with specific geometric shapes and functional groups to achieve anticipated structures and macroscopic properties. A series of ABn dendron-like molecules were synthesized, and their self-assembled nanostructures were studied which are mainly directed by the macromolecular geometric shapes.
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