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Hierarchical Self-Organization of ABn Dendron-like Molecules into a Supramolecular Lattice Sequence
ACS Central Science ( IF 12.7 ) Pub Date : 2017-08-07 00:00:00 , DOI: 10.1021/acscentsci.7b00188 Xueyan Feng 1 , Ruimeng Zhang 1 , Yiwen Li 2 , You-Lee Hong 3, 4 , Dong Guo 1 , Kening Lang 1 , Kuan-Yi Wu 1 , Mingjun Huang 1 , Jialin Mao 1 , Chrys Wesdemiotis 1 , Yusuke Nishiyama 3, 4 , Wei Zhang 1 , Wei Zhang 5 , Toshikazu Miyoshi 1 , Tao Li 6 , Stephen Z D Cheng 1
ACS Central Science ( IF 12.7 ) Pub Date : 2017-08-07 00:00:00 , DOI: 10.1021/acscentsci.7b00188 Xueyan Feng 1 , Ruimeng Zhang 1 , Yiwen Li 2 , You-Lee Hong 3, 4 , Dong Guo 1 , Kening Lang 1 , Kuan-Yi Wu 1 , Mingjun Huang 1 , Jialin Mao 1 , Chrys Wesdemiotis 1 , Yusuke Nishiyama 3, 4 , Wei Zhang 1 , Wei Zhang 5 , Toshikazu Miyoshi 1 , Tao Li 6 , Stephen Z D Cheng 1
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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.
中文翻译：
ABn 树枝状分子的分层自组织成超分子晶格序列
为了了解软材料的分层自组织行为及其对分子几何形状的依赖性，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AB n树枝状分子。这些分子的顶端是具有 14 个羟基的亲水性 POSS 笼（表示为 DPOSS）。在其外围，有不同数量（ n = 1–8）的疏水性 POSS 笼，具有七个异丁基（表示为 BPOSS），通过柔性树枝状连接体连接到顶端 DPOSS。通过改变 BPOSS 数从 1 到 7，超分子晶格形成序列范围从片层 (DPOSS-BPOSS)、双螺旋体 ( Ia 3̅ d空间群、DPOSS-BPOSS 2 )、六角柱体 ( P 6 mm平面群， DPOSS-BPOSS 3 )、Frank–Kasper A15 ( Pm 3̅ n空间群、DPOSS-BPOSS 4 、DPOSS-BPOSS 5和 DPOSS-BPOSS 6 )、Frank–Kasper sigma ( P 4 2 /mnm空间群、可以观察到 DPOSS-BPOSS 7 ) 阶段。这一系列 AB n树枝状分子中的纳米结构形成主要由分子几何形状决定。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 笼形成相对刚性的外壳，并与邻居接触以减少球形图案之间的界面，从而在这些弗兰克-卡斯帕晶格。 这项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。
更新日期：2017-08-07
中文翻译：
ABn 树枝状分子的分层自组织成超分子晶格序列
为了了解软材料的分层自组织行为及其对分子几何形状的依赖性，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AB n树枝状分子。这些分子的顶端是具有 14 个羟基的亲水性 POSS 笼（表示为 DPOSS）。在其外围，有不同数量（ n = 1–8）的疏水性 POSS 笼，具有七个异丁基（表示为 BPOSS），通过柔性树枝状连接体连接到顶端 DPOSS。通过改变 BPOSS 数从 1 到 7，超分子晶格形成序列范围从片层 (DPOSS-BPOSS)、双螺旋体 ( Ia 3̅ d空间群、DPOSS-BPOSS 2 )、六角柱体 ( P 6 mm平面群， DPOSS-BPOSS 3 )、Frank–Kasper A15 ( Pm 3̅ n空间群、DPOSS-BPOSS 4 、DPOSS-BPOSS 5和 DPOSS-BPOSS 6 )、Frank–Kasper sigma ( P 4 2 /mnm空间群、可以观察到 DPOSS-BPOSS 7 ) 阶段。这一系列 AB n树枝状分子中的纳米结构形成主要由分子几何形状决定。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 笼形成相对刚性的外壳，并与邻居接触以减少球形图案之间的界面，从而在这些弗兰克-卡斯帕晶格。 这项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。
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