Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing, 400045, PR China.
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing, 400045, PR China.
Chemosphere. 2019 Jan;214:361-370. doi: 10.1016/j.chemosphere.2018.09.115. Epub 2018 Sep 21.
To achieve an enhanced and selective adsorption of steroid estrogens, the n-propyl functionalization was applied to the mesoporous silica material (MCM-41) according to the physico-chemical property analysis of steroid estrogens. Adsorption behaviour and water chemistry effects were evaluated with the most concerned steroid estrogens: estrone (E1), 17β-estradiol (E2) and 17α-ethinyl estradiol (EE2) based on the materials characterization. The results showed the uptakes of E1, E2, and EE2 onto the modified MCM-41 were enhanced and accelerated by the n-propyl functionalization, which was positively correlated with the hydrophobicity of the synthesized materials. Kinetic data fitted the pseudo-second-order model well. Based on the Langmuir model, the maximum adsorption capacities of the n-propyl modified MCM-41 were up to 119.87, 88.38, and 86.91 mg g for EE2, E1, and E2, respectively. Importantly, both acid and neutral solutions were beneficial to estrogen removal, but ionic strength and humic acid did not affect the estrogen adsorption. The above results suggested that the n-propyl functionalized MCM-41 would be a promising adsorbent for the rapid and efficient removal of estrogens with the selectivity from natural organic matter like humic acid. Mechanism analysis showed the key role of hydrophobic interaction, and it also confirmed the contribution of the carbonylic lone pair electrons of E1, which helped the formation of stronger hydrogen bonds with silicon hydroxyls and enhanced the dipole-dipole interaction between E1 and the synthesized materials.
为了实现对甾体雌激素的增强和选择性吸附，根据对甾体雌激素的物理化学性质分析，将正丙基功能化应用于介孔硅材料（MCM-41）。基于材料特性，以最受关注的甾体雌激素：雌酮（E1）、17β-雌二醇（E2）和 17α-乙炔基雌二醇（EE2）为基础，评估了吸附行为和水化学效应。结果表明，通过正丙基功能化，E1、E2 和 EE2 对改性 MCM-41 的摄取得到增强和加速，这与合成材料的疏水性呈正相关。动力学数据很好地符合伪二阶模型。基于 Langmuir 模型，正丙基改性 MCM-41 的最大吸附容量分别达到 119.87、88.38 和 86.91 mg/g 用于 EE2、E1 和 E2。重要的是，酸性和中性溶液都有利于去除雌激素，但离子强度和腐殖酸对雌激素吸附没有影响。上述结果表明，正丙基功能化的 MCM-41 可能是一种很有前途的吸附剂，可用于从腐殖酸等天然有机物中快速高效地去除雌激素，并具有选择性。机理分析表明，疏水性相互作用起着关键作用，它还证实了 E1 的羰基孤对电子的贡献，这有助于与硅羟基形成更强的氢键，并增强 E1 和合成材料之间的偶极-偶极相互作用。
