In this study, a method for quantifying the 3D multiscale dispersion structure of nanofillers including nano-sized primary filler nanoparticles, nano-to sub-micron-sized agglomerates, and micron-sized filler networks in rubber nanocomposites was established for the first time by combining 3D-Scanning Transmission Electron Microscopy (3D-STEM) in a High-angle Annular Dark Field mode and Synchrotron Radiation X-ray CT. By using this method, a model of multiscale dispersion structure of silica (SiO₂) in hydrogenated nitrile butadiene rubber (HNBR) nanocomposites with different SiO₂-HNBR interactions (I_f-r) was established. Interestingly, when the content of SiO₂ is near the percolation threshold, as the I_f-r increases, the homogeneity of SiO₂ increases, the compactness of SiO₂ agglomerates decreases, and the branching degree of SiO₂ agglomerates increases, resulting in higher branching degree and connectivity of filler networks. Furthermore, it was firstly revealed that the stronger Payne effect directly correlate with the higher connectivity of filler networks, rather than the higher homogeneity of nanofillers.

在这项研究中，首次建立了一种方法，用于量化纳米填料的3D多尺度分散结构，该结构包括纳米级主要填料纳米粒子，纳米级至亚微米级团聚物和微米级填料网络在橡胶纳米复合材料中的结合高角度环形暗场模式和同步辐射X射线CT的3D扫描透射电子显微镜（3D-STEM）。通过这种方法，建立了二氧化硅（SiO ₂）在具有不同SiO ₂ -HNBR相互作用（I _f-r）的氢化丁腈橡胶（HNBR）纳米复合材料中的多尺度分散结构模型。有趣的是，当二氧化硅的含量₂是接近渗透阈值，作为余_FR增大，由SiO均匀性_2度增加时，二氧化硅的紧凑_2个团块减小，并且支化度的的SiO ₂聚集体的增加，从而导致更高的支化度和填料网络的连通性。此外，首先揭示了较强的佩恩效应与填料网络的较高连通性直接相关，而不是与纳米填料的较高同质性直接相关。