Nanocomposites hierarchically assembled with spatially-defined polymeric and inorganic building blocks provide a versatile platform for the precise design of materials with collective or enhanced properties of both components. However, the inability to scalably and efficiently synthesize hierarchical structures as well as the lack of orthogonally recognized interactions between diverse components greatly limited the scope of building blocks. In this presentation, a two-step approach was developed to tackle these challenges. In the first step, the polymer matrix with hierarchical nanostructures was constructed via a programmable molecular self-assembly strategy. Multicomponent mixed-graft block copolymers with intramolecularly defined block interfaces were designed and synthesized. These hierarchically-structured macromolecules exhibited broadly-tunable phase-<i>in</i>-phase morphologies. In the second step, inorganic components spanning from atomic scale luminescent metal ions, subnanoscale metal clusters, to nanoscale metal particles were introduced to the aforementioned matrix. With judiciously engineered intermolecular interactions, the inorganic components reside in select domains of the hierarchically-structured polymer matrix, leading to diverse and well-defined morphologies. We envision that this novel hierarchal co-assembly strategy will open a way for the discovery of next-generation materials for advanced applications in optoelectronics and catalysis.

Constructing hierarchically-structured nanocomposites from multicomponent mixed-graft block copolymers and functional inorganic fillers

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