LAUSR

Abstract Industrially viable processes enabling effective control of nanoparticle (NP) spatial organization in polymers are vitally important for achieving potential of nano-composites as building blocks of dynamic composites. Here, we report on the small and large strain mechanical properties of glassy polymers with spatial organization of spherical NPs controlled by the balance of the (polymer-NP)/(NP-solvent) interfacial attraction and mixing conditions. While strong polymer-NP attraction yielded good NP dispersion regardless of the mixing rate, weak polymer-NP attraction and low shear rate mixing resulted in chain bound NP clusters. Polymers with individually dispersed NPs exhibited the largest elastic moduli and strength while polymers filled with deformable chain bridged NP clusters possessed the largest ductility, at the same NP content. Hybrid systems, consisting of chain bridged NP clusters embedded in a polymer with individually dispersed NPs, exhibited simultaneous enhancement of stiffness, strength and ductility with its extent tunable by the cluster content. Our results confirm the pivotal role of NP spatial organization in translating the nano- and micro-scale phenomena to macro-scale mechanical response of polymer nano-composites. The obtained knowledge enables the design of additive fabrication technologies capable of employing polymer nano-composites in manufacturing of lightweight, functional engineering structures.