Department of Chemical Engineering, Graduate School of Engineering, Tohoku University 6-6-07 Aoba, Aramaki-aza Aoba-ku, Sendai, 980-8579, Japan.
Langmuir. 2010 May 18;26(10):7512-5. doi: 10.1021/la904316f.
A facile one-pot synthesis to produce micrometer-sized silica particles with low polydispersity was examined in a semibatch process where an ethanol solution of tetraethyl orthosilicate (TEOS) was continuously supplied to another ethanol solution of water and ammonia containing an electrolyte of LiCl, NaCl, or KCl. Supply rates of the TEOS solution was ranged with the water and electrolyte concentrations, which indicated that the addition of KCl at a low water concentration was effective to increase size of silica particles in a micrometer range. Highly monodisperse silica particles with an average size of 6.6 microm were successfully produced at 3 mol/m(3) KCl and 5 kmol/m(3) water. The efficiency of KCl addition for producing the large particles is interpreted by the previously proposed nucleation and growth mechanism that expects rapid particle coagulation in early reaction stage for particles which have reduced surface potential by the adsorption of cations with a large ionic radius. It is confirmed from competitive growth reactions that the silica particle growth follows the reaction-limited mechanism even in the semibatch process.
一种简便的一锅法合成具有低多分散性的微米级硅溶胶的方法,在半分批过程中进行了研究,其中四乙氧基硅烷(TEOS)的乙醇溶液连续供给到含有电解质 LiCl、NaCl 或 KCl 的水和氨的另一种乙醇溶液中。TEOS 溶液的供给速率与水和电解质浓度有关,这表明在低水浓度下添加 KCl 有利于增加粒径在微米范围内的硅溶胶颗粒的大小。在 3 mol/m(3) KCl 和 5 kmol/m(3) 水的条件下,成功制备出平均粒径为 6.6 微米的高度单分散硅溶胶颗粒。通过先前提出的成核和生长机制来解释添加 KCl 以制备大颗粒的效率,该机制预计在阳离子具有较大离子半径时,通过吸附来降低表面电势,从而使颗粒在早期反应阶段快速发生团聚。通过竞争生长反应证实,即使在半分批过程中,硅溶胶颗粒的生长也遵循反应控制的机制。