The 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.

中文翻译：

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纳米颗粒填充的刷嵌段共聚物复合材料中的液体到固体的转变

密集接枝的嵌段共聚物（BBCP）的自然自组装可将功能性纳米颗粒（NP）引导到晶格间距大且NP含量高的有序结构中。要优化此类材料的加工窗口，必须了解NP对相行为和粘弹性的影响。在二嵌段瓶刷（dbBB）聚（组成的纳米复合材料模型系统的热结构和热流变性质进行了研究叔丁基丙烯酸酯） -嵌段-聚（环氧乙烷）（PtBA- b -PEO），络合表面功能化氧化锆（ZrO ₂）NP。NP通过协调的氢键选择性地螯合到微相分离的PEO域中。根据温度控制的小角度X射线散射（SAXS），可以达到高达φ = 30 wt％NP的加载量，并且层状形态在熔融状态下稳定。由小振幅振荡剪切（SAOS）确定的线性粘弹性的系统性跃迁表明，在较慢的时间尺度上，NP超结构抑制了dbBB体系结构固有的高度可移动的松弛过程。弛豫时间谱H（τ）的进一步分析用于描述这种弛豫机制的约束条件。 SAOS和SAXS实现的结构-属性关系使将来的机械性能操纵和BBCP / NP复合材料的加工既可用于已建立的应用，也可用于紧急应用。