论文标题
线性肿胀行为的基于丙烯酰胺的核壳微凝胶中核心单体的空间分布
Spatial distribution of core monomers in acrylamide-based core-shell microgels with linear swelling behaviour
论文作者
论文摘要
核心壳微凝胶的特殊线性温度依赖性肿胀已被认为与结合了不同过渡温度的材料的核壳结构相关。在这里,使用与选择性脱位的小角度中子散射,研究了水中的PNIPMAM核心和PNNPAM-shell微凝胶作为温度的函数。光子相关光谱用于仔细检查胶体颗粒的肿胀行为,并揭示线性肿胀。此外,这些实验还被用于检查氘化对肿胀的影响。使用自由形式的多壳反向蒙特卡洛方法,将小角度散射数据转换为径向单体密度曲线。与完全氢化的核心壳微凝胶组成的“仅核心”颗粒的比较,最后与H核/D壳体结构的最终比较表明,核心和外壳单体显示出具有较强的插入性的梯度曲线,从而导致核心嵌入了比其隔离的“核心”核心“仅核心”的壳中嵌入的壳体。对于包括两个过渡的温度范围,这种令人惊讶的结果进一步推广到不同的核心交叉接头内容。我们的分析表明,PNIPMAM核心和PNNPAM-Shell微凝胶的内部结构是异质且强烈互穿的,可能只允许在温度中间的渐进式核心肿胀中间,从而促进了两种过渡温度,从而促进了线性溶胀行为。
The peculiar linear temperature-dependent swelling of core-shell microgels has been conjectured to be linked to the core-shell architecture combining materials of different transition temperatures. Here the structure of pNIPMAM-core and pNNPAM-shell microgels in water is studied as a function of temperature using small-angle neutron scattering with selective deuteration. Photon correlation spectroscopy is used to scrutinize the swelling behaviour of the colloidal particles and reveals linear swelling. Moreover, these experiments are also employed to check the influence of deuteration on swelling. Using a form free multi-shell reverse Monte Carlo approach, the small-angle scattering data are converted into radial monomer density profiles. The comparison of 'core-only' particles consisting of identical cores to fully hydrogenated core-shell microgels, and finally to H core/D shell architectures unambiguously shows that core and shell monomers display gradient profiles with strong interpenetration, leading to cores embedded in shells which are bigger than their isolated 'core only' precursor particles. This surprising result is further generalized to different core cross linker contents, for temperature ranges encompassing both transitions. Our analysis demonstrates that the internal structure of pNIPMAM-core and pNNPAM-shell microgels is heterogeneous and strongly interpenetrated, presumably allowing only progressive core swelling at temperatures intermediate to both transition temperatures, thus promoting linear swelling behaviour.