Shi Yi, Zhang Tianren, Guo Rui, Zhang Zihan, McCahill Amanda L, Tang Yao, Liskey Sabrina E, Yang Dai-Bei, Kloxin Christopher J, Saven Jeffery G, Pochan Darrin J
Department of Materials Science and Engineering, University of Delaware, Newark, DE, USA.
Department of Chemistry, University of Pennsylvania, Philadelphia, PA, USA.
Nat Commun. 2024 Nov 20;15(1):10057. doi: 10.1038/s41467-024-54340-9.
Surface charge patchiness of different charge types can influence the solution behaviours of colloidal particles and globular proteins. Herein, coiled-coil 'bundlemer' nanoparticles that display only a single type of surface charge (SC) are computationally designed to compare their solution behaviours to mixed charge-type (MC) counterparts with both positively and negatively charged side chains. Nematic and columnar liquid crystal phases are discovered in low concentrations of SC particles, indicative of particle end-to-end stacking into columns combined with lateral electrostatic repulsion between columns, while MC particles with the same net charge and particle shape produced only amorphous, soluble aggregates. Similarly, porous lattices are formed in mixtures of SC/MC particles of opposite charges while MC/MC mixtures of opposite charges produce only amorphous aggregates. The lattice structure is inferred with a machine learning optimization approach. The differences between SC and MC particle behaviours directly show the importance of surface electrostatic patchiness.
不同电荷类型的表面电荷不均匀性会影响胶体颗粒和球状蛋白质的溶液行为。在此，通过计算设计出仅显示单一类型表面电荷（SC）的卷曲螺旋“束聚体”纳米颗粒，以将其溶液行为与具有带正电和带负电侧链的混合电荷类型（MC）对应物进行比较。在低浓度的SC颗粒中发现了向列相和柱状液晶相，这表明颗粒端对端堆叠成柱，并伴随着柱之间的横向静电排斥，而具有相同净电荷和颗粒形状的MC颗粒仅产生无定形的可溶性聚集体。同样，在带相反电荷的SC/MC颗粒混合物中形成了多孔晶格，而带相反电荷的MC/MC混合物仅产生无定形聚集体。通过机器学习优化方法推断出晶格结构。SC和MC颗粒行为之间的差异直接表明了表面静电不均匀性的重要性。
