College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
Soft Matter. 2021 Jan 7;17(1):153-159. doi: 10.1039/d0sm01405b. Epub 2020 Nov 9.
Contrary to the popular belief that multicomponent assembly systems will theoretically co-assemble under the same type of driving forces, two distinct assembly modes from a system composed of two chemically similar supramolecules were demonstrated in this work. Although with exactly the same driving forces, molecule-level self-sorting unexpectedly occurred in this two-component system made of polyhedral oligomeric silsesquioxane (POSS) core-based supramolecules with one and eight lysine derivative arms. From the experiments, it was concluded that instead of driving force types, driving force counterpoise plays a vital role here, which we called "identity card hypothesis". The hypothesis suggests that two highly similar components show high affinity for the same molecules through the differentiated "identity card"-like balance of driving forces induced by the difference in the molecular spatial shape, which has never been reported before.
与普遍认为的多组分组装体系在相同类型驱动力作用下将理论上共组装的观点相反,本工作中展示了由两个化学相似的超分子组成的体系存在两种截然不同的组装模式。尽管驱动力完全相同,但令人惊讶的是,在由基于多面体低聚倍半硅氧烷(POSS)核的超分子组成的这个两组分体系中出现了分子级自分类。从实验中得出结论,起作用的不是驱动力类型,而是驱动力平衡,我们称之为“身份证假说”。该假说表明,两个高度相似的组分通过由分子空间形状差异引起的差异化“身份证样”驱动力平衡对相同分子表现出高亲和力,这在此之前从未有过报道。