Synthesis of Monodispersed Hollow Mesoporous Organosilica and Silica Nanoparticles with Controllable Shell Thickness Using Soft and Hard Templates
Synthesis of Monodispersed Hollow Mesoporous Organosilica and Silica Nanoparticles with Controllable Shell Thickness Using Soft and Hard Templates
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DOI：
10.1021/acs.langmuir.2c03121
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发表时间：
2023-03-21
期刊：
影响因子：
3.9
通讯作者：
Kubo，Masaru
中科院分区：
文献类型：
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作者：
Fujii，Yuji;Zhou，Shujun;Kubo，Masaru
具有可控尺寸（小于100 nm）的中空介孔纳米颗粒被期望作为药物递送载体。在此，我们报告了单分散的中空介孔有机硅（HMOS）和中空介孔二氧化硅（HMS）纳米粒子的合成使用软和硬模板方法。以1，2-二（三乙氧基硅基）乙烷（BTEE）为前体，十六烷基三甲基溴化铵和十二烷基硫酸钠（SDS）为软模板，在单分散SiO2纳米粒子（SNPs）上制备了HMOS壳层，并将其作为硬模板。通过在三轮氨透析后去除SNP获得HMOS和HMS纳米颗粒。HMOS的中空尺寸可以通过改变SNP的尺寸来调节。通过使用尺寸为36.5nm的SNP，约20 nm的中空空间通过窄孔（<5 nm）连接表面。表面活性剂胶束形成约12 nm的介孔。此外，在HMOS和HMS中的颗粒间空间约为12 nm。HMOS和HMS的壳层厚度可以通过改变BTEE的量在5-9 nm范围内进行调节。此外，表面活性剂的用量改变了多孔结构。厚度为5 nm的HMOS表现出268 m2/g的Brunauer-Emmett-Teller（BET）表面积和1.14cm3/g的总孔体积。同时，HMS表现出553 m2/g的BET表面积和1.82cm3/g的总孔体积，同时保持中空结构。HMOS对布洛芬具有较高的载药量（3009 mg/g），其释药系统具有一定的缓释性能。因此，本文提出的使用硬模板和软模板的HMOS制备可以控制药物递送应用的中空尺寸和壳厚度。
Hollow mesoporous nanoparticles with controllable size (less than 100 nm) are desired as drug-delivery carriers. Herein, we report the synthesis of monodispersed hollow mesoporous organosilica (HMOS) and hollow mesoporous silica (HMS) nanoparticles using soft and hard templating methods. HMOS shells, with 1,2-bis(triethoxysilyl)ethane (BTEE) as the precursor and hexadecyltrimethylammonium bromide and sodium dodecyl sulfate (SDS) as the soft templates, were formed on monodispersed silica nanoparticles (SNPs), which were used as the hard templates. HMOS and HMS nanoparticles were obtained by removing the SNPs after three rounds of ammonia dialysis. The hollow size of HMOS can be tuned by changing the size of the SNPs. By using SNPs with a size of 36.5 nm, hollow spaces of approximately 20 nm connected the surface through narrow pores (<5 nm). Mesopores of approximately 12 nm were formed by the surfactant micelles. Additionally, the interparticle space in HMOS and HMS was approximately 12 nm. The shell thicknesses of HMOS and HMS could be tuned in the range of 5–9 nm by changing the BTEE amount. Moreover, the amount of surfactant used varied the porous structure. The HMOS with a thickness of 5 nm exhibited a Brunauer–Emmett–Teller (BET) surface area of 268 m2/g and a total pore volume of 1.14 cm3/g. Meanwhile, HMS demonstrated a BET surface area of 553 m2/g and a total pore volume of 1.82 cm3/g while maintaining a hollow structure. HMOS displayed a high loading capacity for ibuprofen (3009 mg/g), and its drug release system showed a sustained-release property. Therefore, the HMOS preparation using hard and soft templates proposed herein can control the hollow size and shell thickness for drug-delivery applications.