Medium controlled aggregative growth as a key step in mesoporous silica nanoparticle formation

分散性 介孔材料 化学工程 介孔二氧化硅 成核 胶体 纳米颗粒 粒径 化学 离子强度 肺表面活性物质 多孔性 粒子(生态学) 多孔介质 材料科学 纳米技术 无机化学 催化作用 有机化学 水溶液 海洋学 地质学 工程类
作者
Viktoriya Semeykina,Ilya Zharov
出处
期刊:Journal of Colloid and Interface Science [Elsevier BV]
卷期号:615: 236-247 被引量:17
标识
DOI:10.1016/j.jcis.2022.01.166
摘要

Near monodisperse mesoporous silica nanoparticles (MSN) represent a promising and rapidly developing type of mesoporous silica materials; however, the vast data on their synthesis remains unorganized and ill-understood. We systematically studied the formation of MSN under basic and neutral conditions using various temperatures, CTAB concentrations, hydrolyzing agents (triethanolamine, ammonia, phosphate buffers), and media with different colloidal stabilization properties (with ethanol as a cosolvent and monovalent salts). In the typical conditions for the preparation of stable MSN colloids, the particle size was controlled by colloidal stabilization by the medium (solvent type, ionic strength, and surfactant concentration) in agreement with the "aggregative growth" mechanism, rather than by solely the hydrolysis and condensation rates conventionally used for data interpretation in the classical nucleation theory. Medium properties (pH, ion types and concentration, polarity) also defined the efficiency of silica-surfactant cooperative self-assembly, which directly affected the porosity, mesopore size and pore wall thickness. Interestingly, this traditional silica-surfactant route showed a limited effect on the particle size, emphasizing the dominating role of colloidal stabilization in the studied reaction conditions. In situ pH measurements showed that every reaction medium has unique pH evolution profiles depending on the buffer capacity, hydrolysis and condensation rates. Reaction systems that fail to maintain the working pH can lead to non-porous products or undesired particle morphology and size distribution. The established particle formation mechanism allowed us to formulate comprehensive guidelines for preparing relatively concentrated colloids of near monodisperse (PDI 5-15%) mesoporous 30-700 nm silica spheres with variable porosity and mesopore size. These findings will be particularly useful in designing new mesoporous silica-containing materials for biomedical applications.
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