Ultralight hybrid silica aerogels derived from supramolecular hydrogels self-assembled from insoluble nano building blocks

Abstract

Supramolecular hydrogels are a type of hydrogel cross-linked by non-chemical bonds and they have been widely applied in the field of smart systems, sensors, tissue engineering, and controlled drug delivery. Most supramolecular hydrogels are formed by soluble molecules, polymers, and metal ions. In this work, supramolecular hydrogels self-assembled between two insoluble nano building blocks (ISNBBs), graphene oxide (GO) and amino-functionalized silica nanoparticles (SiO₂–NH₂), have been discovered and synthesized. The gelation conditions of the two ISNBBs have been investigated. A step further, ultralight hybrid silica aerogels are obtained by supercritical drying of the physical hydrogels. No visible volume shrinkage is observed, due to the fact that the hydrogel networks are formed by rigid ISNBBs. Thus the hybrid aerogels possess ultralow density (down to 7.5 mg cm⁻³), high specific surface areas (178.6 m² g⁻¹), and extremely high porosity (99.6%). The present work shows an alternative strategy to design and synthesize supramolecular hydrogels and aerogels using predetermined building blocks, together with designable morphology and physical properties for the target aerogels.