Department of Applied Chemistry, National Yang Ming Chiao Tung University, 1001 Ta Hsueh Road, Hsinchu 30010, Taiwan.
Institute of Chemistry, Academia Sinica, Taipei 11529, Taiwan.
J Am Chem Soc. 2022 Jun 1;144(21):9390-9398. doi: 10.1021/jacs.2c01715. Epub 2022 May 19.
The shapeshifting behavior for synthetic matters was found at either the molecular or supramolecular level, but the connection between shapeshifting at the two hierarchical levels remains missing. In this study, an 8-arm star giant molecule, , was synthesized to connect the molecular and supramolecular shapeshifting. Controlling the conditions of bulk self-assembly allowed us to bring into three different Ostwald's stages of nucleation. The high conformational flexibility of facilitates molecular shapeshifting and allows to take the discotic, rod-like and star-like geometries in different Ostwald's stages. Simultaneous changes in the supramolecular scaffolds were observed as the discotic, rod-like and star-like molecules self-assembled into the supramolecular scaffolds of 1D columns, 2D lamellae, and 3D networks, respectively. These changes in the hierarchical structures also affect the CO affinity of . Therefore, the connection between the molecular/supramolecular shapeshifting and the structure-driven property changes of were established by taking advantage of the high conformational freedom of the 8-arm star giant molecule and its diverse self-assembly pathways leading to the different Ostwald's stages.
在分子或超分子水平上发现了形状变化行为，但在这两个层次之间的形状变化之间的联系仍然缺失。在这项研究中，合成了一种 8 臂星型大分子 ，将分子和超分子形状变化连接起来。控制体相自组装的条件使我们能够将 带入奥斯特瓦尔德成核的三个不同阶段。 的高构象灵活性促进了分子形状变化，并允许 在不同奥斯特瓦尔德阶段呈现盘状、棒状和星状几何形状。当盘状、棒状和星状 分子自组装成 1D 柱、2D 层和 3D 网络的超分子支架时，观察到超分子支架的同时变化。这些层次结构的变化也会影响 的 CO 亲和力。因此，通过利用 8 臂星型大分子的高构象自由度及其导致不同奥斯特瓦尔德阶段的多种自组装途径，建立了分子/超分子形状变化与 的结构驱动性质变化之间的联系。
