The structure of supraparticles (SPs) is a key parameter for achieving advanced functionalities arising from the combination of different nanoparticle (NP) types in one hierarchical entity. However, whenever a droplet-assisted forced assembly approach is used, e.g., spray-drying, the achievable structure is limited by the inherent drying phenomena of the method. In particular, mixed NP dispersions of differently sized colloids are heavily affected by segregation during the assembly. Herein, the influence of the colloidal arrangement of Pt and SiO NPs within a single supraparticulate entity is investigated. A salt-based electrostatic manipulation approach of the utilized NPs is proposed to customize the structure of spray-dried Pt/SiO SPs. By this, size-dependent separation phenomena of NPs during solvent evaporation, that limit the catalytic performance in the reduction of 4-nitrophenol, are overcome by achieving even Pt NP distribution. Additionally, the textural properties (pore size and distribution) of the SiO pore framework are altered to improve the mass transfer within the material leading to increased catalytic activity. The suggested strategy demonstrates a powerful, material-independent, and universally applicable approach to deliberately customize the structure and functionality of multi-component SP systems. This opens up new ways of colloidal material combinations and structural designs in droplet-assisted forced assembly approaches like spray-drying.
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