Rocha Brunno C, Vashisth Harish
Department of Chemical Engineering, University of New Hampshire, Durham, New Hampshire 03824, United States.
J Chem Theory Comput. 2024 Feb 27;20(4):1590-1599. doi: 10.1021/acs.jctc.3c00406. Epub 2023 Aug 31.
Self-assembly of colloidal particles is emerging as a promising approach for producing novel materials. These colloidal particles can be synthesized with protrusions (lobes) on their surfaces that allow the formation of porous structures with a wide range of applications. Using Langevin dynamics simulations, we studied self-assembly in the binary mixtures of lobed colloidal particles with variations in their lobe sizes to investigate the feasibility of using dumbbell particles (with two lobes) as cross-linkers to increase the porosity in self-assembled morphologies. Each binary system was formed by mixing the dumbbell particles with one of the following types of particles: trigonal planar (three lobes), tetrahedral (four lobes), trigonal bipyramidal (five lobes), and octahedral (six lobes). We observed that the lobe size on each particle can be tuned to favor the formation of random aggregates and spherical aggregates when the lobes are larger and well-ordered crystalline structures when the lobes are smaller. We also observed that these polydisperse systems form self-assembled structures characterized by porosities higher than those of the structures formed by the monodisperse systems. These results indicate that the lobe size is an important design feature that can be optimized to achieve desired structures with distinct morphologies and porosities, and the dumbbell particles are effective cross-linking agents to enhance the porosity in self-assembled structures.
胶体粒子的自组装正成为一种生产新型材料的有前途的方法。这些胶体粒子可以在其表面合成有凸起（叶瓣），从而形成具有广泛应用的多孔结构。通过朗之万动力学模拟，我们研究了叶瓣尺寸不同的带叶瓣胶体粒子二元混合物中的自组装，以研究使用哑铃形粒子（有两个叶瓣）作为交联剂来增加自组装形态中孔隙率的可行性。每个二元体系是通过将哑铃形粒子与以下类型的粒子之一混合形成的：三角平面形（三个叶瓣）、四面体（四个叶瓣）、三角双锥形（五个叶瓣）和八面体（六个叶瓣）。我们观察到，当叶瓣较大时，每个粒子上的叶瓣尺寸可以调整以有利于形成随机聚集体和球形聚集体；当叶瓣较小时，则有利于形成有序的晶体结构。我们还观察到，这些多分散体系形成的自组装结构的特征是孔隙率高于单分散体系形成的结构。这些结果表明，叶瓣尺寸是一个重要的设计特征，可以进行优化以实现具有不同形态和孔隙率的所需结构，并且哑铃形粒子是增强自组装结构中孔隙率的有效交联剂。
