Hydrogel-Assisted Robust Supraparticles Evolved from Droplet Evaporation

Supraparticles, formed through the self-assembly of nanoparticles, are promising contenders in catalysis, sensing, and drug delivery due to their exceptional specific surface area and porosity. However, their mechanical resilience, especially in dimensions spanning micrometers and beyond, is challenged by the inherently weak interactions among their constituent building blocks, significantly constraining their broad applicability. Here, we have exploited a robust supraparticle fabrication strategy by integrating hydrogel components into the assembly system and evaporating on the superamphiphobic surface. The resultant SiO₂/SA (sodium alginate) supraparticles, achieved by evaporating a 15% volume fraction dispersion of SiO₂ nanoparticles containing 18.46 mg/mL of sodium alginate and subsequently cross-linking with Ca²⁺, demonstrate mechanical robustness with a fracture force of 6.04 N, representing a mechanical strength enhancement of 60 times higher than that prior to the incorporation of the hydrogel component. The supraparticles maintain their original morphology after 30 min of ultrasonic treatment (200 W), demonstrating mechanical stability. This method exhibits generalizability, enabling the customization of supraparticles with various building blocks and hydrogel backbone materials. Based on such a methodology, we have synthesized enzyme-carrying supraparticles, further expanding the potential applications in intricate cascade reactions. The encapsulated glucose oxidase and horseradish peroxidase maintained their inherent reactivity, and such hydrogel-assisted robust supraparticles exhibited exceptional performance in accurate glucose assays, indicating great practical application in biocatalysis.