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首页> 外文期刊>ACS applied materials & interfaces >Synthesis of Spherical Carbon Nitride-Based Polymer Composites by Continuous Aerosol-Photopolymerization with Efficient Light Harvesting
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Synthesis of Spherical Carbon Nitride-Based Polymer Composites by Continuous Aerosol-Photopolymerization with Efficient Light Harvesting

机译：连续气溶胶-光聚合高效捕光合成球形氮化碳基聚合物复合材料

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摘要

Here we report a novel, facile, and sustainable approach for the preparation of spherical submicrometer carbon nitride-based polymer composites by a continuous aerosol-photopolymerization process. In this regard, spherical mesoporous carbon nitride (SMCN) nanoparticles were initially prepared-via a nanocasting approach using spray-drying synthesized spherical mesoporous silica (SMS) nano particles as hard templates. In addition to experimental characterization, the effect of porosity on the light absorption enhancement and consequently the generation rate of electron-hole pairs inside the SMCN was simulated using a three-dimensional finite difference time domain (FDTD) method. To produce the carbon nitride-based polymer composite, SMCN nanoparticles exhibit excellent performance in photopolymerization of butyl acrylate (PBuA) monomer in the presence of n-methyldiethanolamine (MDEA) as a co-initiator in a continuous aerosol-based process. In this one-pot synthesis, SMCN nanoparticles act not only as photoinitiators but at the same time as fillers and templates. The average aerosol residence time in the photoreactor is about 90 s. The presented aerosol-photopolymerization process avoids the need for solvent and surfactant, operates at room temperature, and, more importantly, is suitable to produce the spherical composite with hydrophobic polymers. Furthermore, we simulated the condition of SMCN nanoparticles during illumination in the gas phase process, which can freely rotate. The results demonstrated that the hole (h(+)) density is almost equally distributed in the whole part of the SMCN nanoparticles due to their rotation, leading to efficient light harvesting and more homogeneous photoreaction. The combination of the outstanding features of environmentally friendly SMCN, photopolymerization, and aerosol processing might open new avenues, especially in green chemistry, to produce novel polymer composites with multifunctional properties.
机译：在这里，我们报告了一种新颖，简便且可持续的方法，该方法通过连续的气溶胶光聚合工艺制备球形亚微米氮化碳基聚合物复合材料。在这方面，首先通过纳米浇铸方法制备球形中孔氮化碳（SMCN）纳米颗粒，该方法使用喷雾干燥合成的球形中孔二氧化硅（SMS）纳米颗粒作为硬模板。除实验表征外，还使用三维时域有限差分（FDTD）方法模拟了孔隙率对光吸收增强的影响，并因此模拟了SMCN内部电子-空穴对的生成速率。为了生产基于氮化碳的聚合物复合材料，SMCN纳米颗粒在基于连续气溶胶的工艺中，在作为辅助引发剂的正甲基二乙醇胺（MDEA）的存在下，丙烯酸丁酯（PBuA）单体的光聚合表现出卓越的性能。在这种一锅法合成中，SMCN纳米颗粒不仅充当光引发剂，而且同时充当填充剂和模板。气溶胶在光反应器中的平均停留时间约为90 s。提出的气溶胶-光聚合方法避免了对溶剂和表面活性剂的需求，在室温下操作，并且更重要的是，适合于生产具有疏水性聚合物的球形复合材料。此外，我们模拟了气相过程中SMCN纳米粒子在光照过程中的状态，该条件可以自由旋转。结果表明，由于其旋转，空穴（h（+））密度几乎均匀分布在SMCN纳米颗粒的整个部分中，从而导致有效的光收集和更均匀的光反应。环保型SMCN，光聚合和气溶胶处理等突出特征的结合可能会开辟新途径，特别是在绿色化学领域，以生产具有多功能特性的新型聚合物复合材料。

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