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SiO2 纳米颗粒的溶解速率与颗粒尺寸的关系。

The dissolution rates of SiO2 nanoparticles as a function of particle size.

机构信息

GET-Université de Toulouse-CNRS-IRD-OMP, 14 Avenue Edouard Belin, 31400 Toulouse, France.

出版信息

Environ Sci Technol. 2012 May 1;46(9):4909-15. doi: 10.1021/es2045053. Epub 2012 Apr 16.

Abstract

There is a critical need to better define the relationship among particle size, surface area, and dissolution rate for nanoscale materials to determine their role in the environment, their toxicity, and their technological utility. Although some previous studies concluded that nanoparticles dissolve faster than their bulk analogs, contradictory evidence suggests that nanoparticles dissolve more slowly. Furthermore, insufficient characterization of the nanoparticulate samples and the solution chemistry in past studies obscures the relationship between particle size, surface area, and dissolution rate. Here we report amorphous SiO(2) dissolution rates in aqueous solutions determined from complementary mixed-flow and closed reactor experiments at 6.9 ≥ pH ≥ 11.2 and 25 °C as a function of particle diameter from 25 to 177 nm. Experiments were performed at far-from-equilibrium conditions to isolate kinetic effects from those of changing the reaction driving force on overall dissolution rates. Measured far-from-equilibrium mass normalized dissolution rates are nearly independent of particle size, but corresponding BET surface area normalized rates decrease substantially with decreasing particle size. Combining these observations with existing established kinetic rate equations allows the prediction of nanoparticle dissolution rates as a function of both particle size and aqueous fluid saturation state.

摘要

目前迫切需要更好地定义纳米材料的粒径、表面积和溶解速率之间的关系,以确定它们在环境中的作用、毒性及其技术实用性。尽管一些先前的研究得出结论,纳米颗粒的溶解速度比其大块类似物快,但矛盾的证据表明,纳米颗粒的溶解速度较慢。此外,过去研究中对纳米颗粒样品和溶液化学的描述不足,使得粒径、表面积和溶解速率之间的关系变得模糊。在这里,我们报告了在 6.9≥pH≥11.2 和 25°C 的水溶液中无定形 SiO2 的溶解速率,作为粒径从 25nm 到 177nm 的函数。实验在远离平衡条件下进行,以将动力学效应与整体溶解速率变化的反应驱动力分离开来。测量得到的远离平衡的质量归一化溶解速率几乎与粒径无关,但相应的 BET 表面积归一化速率随粒径的减小而显著降低。将这些观察结果与现有的既定动力学速率方程相结合,可以预测纳米颗粒的溶解速率作为粒径和水相流体饱和状态的函数。

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