Abstract
AbstractThe natural self‐assembly of densely grafted brush block copolymers (BBCP) is used to direct functional nanoparticles (NP) into well‐ordered structures with large lattice spacings and high NP content. Understanding the NP's impact on the phase behavior and viscoelastic properties is necessary for optimizing the processing windows for such materials. Thermo‐structural and thermo‐rheological properties are investigated in a model nanocomposite system composed of a di‐block bottlebrush (dbBB) poly(tert‐butyl acrylate)‐block‐poly(ethylene oxide) (PtBA‐b‐PEO), complexed with surface functionalized zirconium oxide (ZrO2) NPs. The NPs selectively sequester into the microphase separated PEO domains through coordinated hydrogen bonding. Loading up to φ = 30 wt% NP is achieved, and the lamellar morphologies are stable in the melt state according to temperature controlled small angle X‐ray scattering (SAXS). Systematic transitions in the linear viscoelasticity, determined by small amplitude oscillatory shear (SAOS) suggest that at slow timescales, the NP superstructure inhibits the highly mobile relaxation processes inherent to the dbBB architecture. Further analysis of the relaxation time spectrum H(τ) is used to describe the constraint of such relaxation mechanisms. The structure–property relationships realized by SAOS and SAXS enable future manipulation of mechanical properties and processing of BBCP/NP composites for both established and emergent applications.
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