SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 50 ›› Issue (10): 379-388.DOI: 10.1016/j.cjche.2022.06.022

• Materials and Product Engineering • 上一篇    下一篇

Establishment of nucleation and growth model of silica nanostructured particles and comparison with experimental data

Yubai Liu1, Zhiyuan Yu1, Thomas Pelster2, Ting-Tai Lee3, Yujun Wang1, Guangsheng Luo1   

  1. 1 State Key Lab of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China;
    2 Evonik Operations GmbH, Brühler Straße 2, Wesseling 50389, Germany;
    3 Evonik Specialty Chemicals (Shanghai) Co., Ltd., Shanghai 201108, China
  • 收稿日期:2022-03-10 修回日期:2022-06-19 出版日期:2022-10-28 发布日期:2023-01-04
  • 通讯作者: Yujun Wang,E-mail:wangyujun@mail.tsinghua.edu.cn
  • 基金资助:
    This work was financially supported by the National Natural Science Foundation of China (21878169, 21991102), the National Key Research and Development Program of China (2019YFA0905100), and the Tsinghua University Initiative Scientific Research Program (2018Z05JZY010).

Establishment of nucleation and growth model of silica nanostructured particles and comparison with experimental data

Yubai Liu1, Zhiyuan Yu1, Thomas Pelster2, Ting-Tai Lee3, Yujun Wang1, Guangsheng Luo1   

  1. 1 State Key Lab of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China;
    2 Evonik Operations GmbH, Brühler Straße 2, Wesseling 50389, Germany;
    3 Evonik Specialty Chemicals (Shanghai) Co., Ltd., Shanghai 201108, China
  • Received:2022-03-10 Revised:2022-06-19 Online:2022-10-28 Published:2023-01-04
  • Contact: Yujun Wang,E-mail:wangyujun@mail.tsinghua.edu.cn
  • Supported by:
    This work was financially supported by the National Natural Science Foundation of China (21878169, 21991102), the National Key Research and Development Program of China (2019YFA0905100), and the Tsinghua University Initiative Scientific Research Program (2018Z05JZY010).

摘要: A mathematical model is developed for the calculation of the nucleation and growth process of silica nanostructured particles prepared by using the drop-by-drop method, and the calculation results of the proposed model is compared with the experimental value obtained from SAXS data. The model provides a non-ideal improvement in the supersaturation calculation and considers the impact of both mass transfer and surface reaction on the particle growth rate. The nucleation and growth rates are coupled depending on the change in monomer concentration over time, based on which the particle size and distribution are calculated. The growth curve of the silica particles from 3 nm to 20 nm and the change in particle number from 0 to over 1020 are calculated, which are consistent with the experimental values, establishing the reliability of the model. The calculations of the growth rate reveal that mass transfer controls the growth of silica particles before 10 min and the surface reaction is the rate-determining step after 10 min. The changes in the model parameters obtained by fitting with the SAXS data under different reaction conditions indicate the sensitivity of the corresponding process to different conditions. Moreover, the relationship between the particle growth rate and monomer concentration change is analyzed using the proposed model.

关键词: Silica, Nucleation, Growth, Mathematical modeling, Mass transfer, Surface reaction

Abstract: A mathematical model is developed for the calculation of the nucleation and growth process of silica nanostructured particles prepared by using the drop-by-drop method, and the calculation results of the proposed model is compared with the experimental value obtained from SAXS data. The model provides a non-ideal improvement in the supersaturation calculation and considers the impact of both mass transfer and surface reaction on the particle growth rate. The nucleation and growth rates are coupled depending on the change in monomer concentration over time, based on which the particle size and distribution are calculated. The growth curve of the silica particles from 3 nm to 20 nm and the change in particle number from 0 to over 1020 are calculated, which are consistent with the experimental values, establishing the reliability of the model. The calculations of the growth rate reveal that mass transfer controls the growth of silica particles before 10 min and the surface reaction is the rate-determining step after 10 min. The changes in the model parameters obtained by fitting with the SAXS data under different reaction conditions indicate the sensitivity of the corresponding process to different conditions. Moreover, the relationship between the particle growth rate and monomer concentration change is analyzed using the proposed model.

Key words: Silica, Nucleation, Growth, Mathematical modeling, Mass transfer, Surface reaction