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Observation of intensity dependent phase-separation in photoreactive monomer-nanoparticle formulations under non-uniform visible light irradiation.
Soft Matter ( IF 2.9 ) Pub Date : 2020-07-02 , DOI: 10.1039/d0sm00922a Shreyas Pathreeker 1 , Fu-Hao Chen , Saeid Biria , Ian D Hosein
Soft Matter ( IF 2.9 ) Pub Date : 2020-07-02 , DOI: 10.1039/d0sm00922a Shreyas Pathreeker 1 , Fu-Hao Chen , Saeid Biria , Ian D Hosein
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We report observations of photopolymerization driven phase-separation in a mixture of a photo-reactive monomer and inorganic nanoparticles. The mixture is irradiated with visible light possessing a periodic intensity profile that elicits photopolymerization along the depth of the mixture, establishing a competition between photo-crosslinking and thermodynamically favorable phase-separating behavior inherent to the system. In situ Raman spectroscopy was used to monitor the polymerization reaction and morphology evolution, and reveals a key correlation between irradiation intensity and composite morphology extending the entire depth of the mixture, i.e. unhindered phase-separation at low irradiation intensity and arrested phase-separation at high irradiation intensity. 3D Raman volume mapping and energy dispersive X-ray mapping confirm that the intensity-dependent irradiation process dictates the extent of phase separation, enabling single-parameter control over phase evolution and subsequent composite morphology. These observations can potentially enable a single-step route to develop polymer–inorganic composite materials with tunable morphologies.
中文翻译：
在不均匀可见光照射下观察光反应性单体-纳米颗粒配方中强度依赖的相分离。
我们报告在光反应性单体和无机纳米粒子的混合物中进行光聚合驱动相分离的观察。用具有周期性强度分布的可见光照射该混合物，该周期性强度分布沿混合物的深度引发光聚合，从而在光交联和系统固有的热力学上有利的相分离行为之间形成竞争。原位拉曼光谱法用于监测聚合反应和形态演变，并揭示了辐射强度与延伸混合物整个深度的复合形态之间的关键相关性，即在低辐照强度下无阻碍的相分离，在高辐照强度下有阻滞的相分离。3D拉曼体积映射和能量色散X射线映射证实，取决于强度的辐照过程决定了相分离的程度，从而可以对相演化和随后的复合形态进行单参数控制。这些观察结果可能使单步开发具有可调整形态的聚合物-无机复合材料成为可能。
更新日期：2020-08-12
中文翻译：
在不均匀可见光照射下观察光反应性单体-纳米颗粒配方中强度依赖的相分离。
我们报告在光反应性单体和无机纳米粒子的混合物中进行光聚合驱动相分离的观察。用具有周期性强度分布的可见光照射该混合物，该周期性强度分布沿混合物的深度引发光聚合，从而在光交联和系统固有的热力学上有利的相分离行为之间形成竞争。原位拉曼光谱法用于监测聚合反应和形态演变，并揭示了辐射强度与延伸混合物整个深度的复合形态之间的关键相关性，即在低辐照强度下无阻碍的相分离，在高辐照强度下有阻滞的相分离。3D拉曼体积映射和能量色散X射线映射证实，取决于强度的辐照过程决定了相分离的程度，从而可以对相演化和随后的复合形态进行单参数控制。这些观察结果可能使单步开发具有可调整形态的聚合物-无机复合材料成为可能。
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