Encapsulation of particle ensembles in graphene nanosacks as a new route to multifunctional materials.

ABSTRACT

Hybrid nanoparticles with multiple functions are of great interest in biomedical diagnostics, therapies, and theranostics but typically require complex multistep chemical synthesis. Here we demonstrate a general physical method to create multifunctional hybrid materials through aerosol-phase graphene encapsulation of ensembles of simple unifunctional nanoparticles. We first develop a general theory of the aerosol encapsulation process based on colloidal interactions within drying microdroplets. We demonstrate that a wide range of cargo particle types can be encapsulated, and that high pH is a favorable operating regime that promotes colloidal stability and limits nanoparticle dissolution. The cargo-filled graphene nanosacks are then shown to be open structures that rapidly release soluble salt cargoes when reintroduced into water, but can be partially sealed by addition of a polymeric filler to achieve slow release profiles of interest in controlled release or theranostic applications. Finally, we demonstrate an example of multifunctional material by fabricating graphene/Au/Fe3O4 hybrids that are magnetically responsive and show excellent contrast enhancement as multimodal bioimaging probes in both magnetic resonance imaging and X-ray computed tomography in full-scale clinical instruments.