College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 300014, PR China.
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 300014, PR China.
Ultrason Sonochem. 2021 May;73:105484. doi: 10.1016/j.ultsonch.2021.105484. Epub 2021 Feb 3.
Although the traditional Stoˇber process-based methods are widely used for encapsulation of metal nanoparticles in SiO, these time-consuming methods are not effective for coating metal microparticles with a uniform SiO layer of desired thickness. Herein, an ultrasound-assisted, interface-confined sol-gel method is proposed for fast encapsulation of metal microparticles in SiO, and the encapsulation of Sn microparticles is chosen as an example to illustrate its feasibility. The proposed method involves covering metal microparticles with liquid films that contain water, alcohol, surfactant (Span-80) and catalyst (NHF) and then ultrasonically dispersing these particles into cyclohexane, where tetraethylorthosilicate (TEOS) is added. To ensure the hydrolysis-condensation reactions of TEOS occurring at the particle-cyclohexane interface so that the formed SiO is coated on the particles, the microparticles should be well dispersed into cyclohexane with the liquid films being not broken away from their surfaces. It is found that the assistance of probe sonication and the addition of surfactant are crucial to achievement of a good dispersion of metal microparticles in cyclohexane. And using high-viscosity alcohol (namely glycerol), controlling the volume ratio of water to alcohol and the amount of water, and choosing a suitable ultrasonic power are essential for preventing the formation of free SiO (namely SiO that is not coated on the particles), which is a result that the liquid films escape from the particle surfaces under ultrasonic cavitation. Our results have also revealed that the thickness of SiO layer can be adjusted by changing the reaction time or the total amount of water. In particular, the thickness of SiO layer can be easily raised by simply repeating the encapsulation procedure. Compared with the traditional Stoˇber process-based methods, the proposed method is time-saving (reaction time: about 30 min vs. more than 12 h) and extremely effective for coating microparticles with a continuous, uniform SiO layer of desired thickness.
虽然基于传统的 Stoˇber 过程的方法被广泛用于将金属纳米粒子封装在 SiO 中,但这些耗时的方法对于用所需厚度的均匀 SiO 层涂覆金属微粒子并不有效。在此,提出了一种超声辅助、界面受限的溶胶-凝胶方法,用于快速将金属微粒子封装在 SiO 中,并选择 Sn 微粒子作为示例来说明其可行性。该方法涉及用包含水、醇、表面活性剂(Span-80)和催化剂(NHF)的液体膜覆盖金属微粒子,然后将这些粒子超声分散到环己烷中,同时加入正硅酸乙酯(TEOS)。为了确保 TEOS 的水解-缩合反应发生在粒子-环己烷界面上,从而使形成的 SiO 涂覆在粒子上,微粒子应该很好地分散在环己烷中,液体膜不会从其表面脱离。结果发现,探针超声的辅助和表面活性剂的添加对于实现金属微粒子在环己烷中的良好分散至关重要。此外,使用高粘度醇(即甘油)、控制水与醇的体积比和水量,以及选择合适的超声功率对于防止游离 SiO(即未涂覆在粒子上的 SiO)的形成也是必不可少的,这是由于在超声空化作用下液体膜从粒子表面逸出所致。我们的结果还表明,通过改变反应时间或水的总量可以调整 SiO 层的厚度。特别是,通过简单地重复封装程序,可以很容易地提高 SiO 层的厚度。与传统的基于 Stoˇber 过程的方法相比,该方法节省时间(反应时间:约 30 分钟 vs. 超过 12 小时),并且对于涂覆具有所需厚度的连续、均匀 SiO 层的微粒子非常有效。