Research progress in chemical preparation of polymer/inorganic nanoparticle composite microspheres
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摘要: 聚合物/无机纳米粒子复合微球，具有良好的可设计性、流动性、热稳定性、功能基表面特性等优良的综合性能。聚合物/无机纳米粒子复合微球的形貌、粒径及分布、表面结构等可根据制备方法发生显著变化，从而影响其理化性能。本文综述了乳液聚合法、悬浮聚合法、分散聚合法、两步复合法、自组装法、物理诱导和模板辅助法等化学方法在制备聚合物/无机纳米粒子复合微球方面的研究进展，对其中涉及的多层、核-壳、功能化复合微球的制备方法也做了一定总结。最后，提出了当前在化学制备聚合物/无机纳米粒子复合微球时仍面临的问题，并进行了展望。Abstract: Polymer/inorganic nanoparticle composite microspheres have excellent comprehensive properties such as good designability, fluidity, thermal stability and functional base surface characteristics. The morphology, particle size, distribution and surface structure of polymer/inorganic nanoparticle composite microspheres can be significantly changed according to the preparation method, which can affect their physical and chemical properties. This article reviews the research progress of emulsion polymerization, suspension polymerization, dispersion polymerization, two-step compounding, self-assembly, physical induction and template-assisted methods in preparing polymer/inorganic nanoparticle composite microspheres. The preparation methods of multi-layer, core-shell and functionalized composite microspheres have also been summarized. Finally, the current problems in the chemical preparation of polymer/inorganic nanoparticle composite microspheres are proposed and prospected.
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Key words:
- inorganic nanoparticle /
- polymer /
- composite microspheres /
- chemical preparation /
- research progress
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图 1 SiO2@聚苯乙烯(PS)复合微球形成过程示意图 (a)[26]、乳液聚合法制备SiO2@PS复合微球的示意图 (b)[27]、乳液聚合法制备核-壳型Fe3O4@聚乙炔(PA)复合微球的示意图 (c)[29]和乳液聚合法封装Fe3O4磁性纳米粒子的示意图 (d)[32]
Figure 1. Schematic diagram of the formation process of SiO2@Polystyrene (PS) microspheres (a)[26], schematic diagram of preparing SiO2@PS composite microspheres by emulsion polymerization (b)[27], schematic diagram of preparing core-shell Fe3O4@polyacetylene (PA) composite microspheres by emulsion polymerization (c)[29] and schematic diagram of Fe3O4 magnetic nanoparticles encapsulated by emulsion polymerization (d)[32]
Vi-D4—Tetramethyltetraethylene cyclotetrasiloxane; St—Styrene; NPs—Nanoparticles; OPNTU—O-(proparynyl)-N-(triethoxylsilyl) methyl carbamate
图 2 聚甲基丙烯酸甲酯(PMMA)/CaCO3复合微球的SEM图像 (a)[36]、PMMA/CaCO3复合微球的TEM图像 ((b)~(c))[36-37]和PMMA/CaCO3复合微球形成过程示意图 (d)[36]
Figure 2. SEM image of PMMA/CaCO3 composite microspheres (a)[36], TEM images of PMMA/CaCO3 composite microspheres ((b)-(c))[36-37] and scheme illustration of the formation process of PMMA/CaCO3 composite microspheres (d)[36]
图 3 聚(甲基丙烯酸硬脂酯-丙烯酸丁酯)共聚物(PSB)-SiO2复合微球的SEM和TEM图像 ((a)~(b))、PSB-SiO2复合微球的截面图 ((c)~(d)) 和PSB-SiO2复合微球的元素分布图 ((e)~(h))[52]
Figure 3. SEM and TEM images of poly(stearate methacrylate-butyl acrylate) copolymer (PSB)-SiO2 composite microspheres ((a)-(b)), cross section of PSB-SiO2 composite microspheres ((c)-(d)) and element mapping images of PSB-SiO2 composite microspheres ((e)-(h))[52]
图 4 PMMA/TiO2复合微球和纯TiO2悬浮液的稳定性曲线 (a)[59]、SiO2@ PMMA核-壳型复合微球的TEM图像 (b)[61]、石墨烯(GO)@甲基丙烯酸羟乙酯(PHEMA)复合微球的6次循环效率 (c)[62]和核-壳型聚丙烯酸(PAA)/PS/SiO2多层杂化微球的TEM图像 (d)[67]
Figure 4. Sedimentation stability measurement of both PMMA/TiO2 and pristine TiO2 suspensions as a function of time (a)[59], TEM image of PMMA/SiO2 core-shell composite microspheres (b)[61], Efficiency of the graphene (GO)@hydroxyethyl methacrylate (PHEMA) composite after six cycles (c)[62] and TEM image of core-shell SiO2@polyacrylic acid (PAA)@PS multilayer hybrid microspheres (d)[67]
图 5 聚苯胺(PANI)-还原氧化石墨烯(RGO)复合空心微球的制备过程示意图 (a)[79]、PANI-RGO复合空心微球的SEM图像 (b) [79]、PANI-RGO复合空心微球和PANI-RGO复合膜在电流密度为0.5 A/g下的循环性能 (c)[79]和PS@RGO核-壳微球的TEM图像 (d)[81]
Figure 5. Illustration of the fabrication procedure of the polyaniline (PANI)-reduced graphene oxide (RGO) hollow spheres (a)[79], SEM micrograph of PANI-RGO hollow spheres (b)[79], cycling stability of PANI-RGO hollow spheres and PANI-RGO film at a current density of 0.5 A/g (c)[79] and TEM image of the PS@RGO core-shell microspheres (d)[81]
THF—Tetrahydrofuran; HS—Hollow sphere; LBL—Layer-by-layer
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