Enhanced adsorption of steroid estrogens by one-pot synthesized phenyl-modified mesoporous silica: Dependence on phenyl-organosilane precursors and pH condition

被引：22

作者：

Gao, Pei ^{[1
]}

Liang, Zhijie ^{[1
]}

Zhao, Zhiwei ^{[1
]}

Wang, Wenhao ^{[1
]}

Yang, Chun ^{[1
]}

Hu, Bibo ^{[1
]}

Cui, Fuyi ^{[1
]}

机构：

[1] Chongqing Univ, Minist Educ, Key Lab Three Gorges Reservoir Reg Ecoenvironm, Chongqing 400045, Peoples R China

来源：

CHEMOSPHERE | 2019年 / 234卷

基金：

中国国家自然科学基金;

关键词：

Mesoporous silica; Phenyl-organosilane precursors; Organic functionalization; Adsorption; Steroid estrogens; Solution chemistry; PARTICLE-SIZE CONTROL; EMERGING CONCERN; HEAVY-METALS; REMOVAL; WATER; CONTAMINANTS; 17-BETA-ESTRADIOL; PERFORMANCE; CARBON; NANOPARTICLES;

D O I：

10.1016/j.chemosphere.2019.06.089

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

In this study, the phenyl-modified mesoporous materials were successfully synthesized using phenyl-organosilanes (trimethoxyphenylsilane and triethoxyphenylsilanea) by one-pot co-condensation method for the removal of estrone (El), 178-estradiol (E2), and 17 alpha-ethinyl estradiol (EE2). Both the triethoxyphenylsilane-modified material (20%EtPh-MCM-41) and trimethoxyphenylsilane-modified material (20%MePh-MCM-41) could rapidly achieve equilibrium in 30 min at low adsorbent dosage of 0.025 g L-1. But the different hydrolysable groups of trimethoxyphenylsilane and triethoxyphenylsilane led to the discrepancies in physicochemical properties of the 20%EtPh-MCM-41 and 20%MePh-MCM-41, and thus affected adsorption performance. The 20%EtPh-MCM-41 exhibited the faster estrogen adsorption rates expressed in pseudo-second-order kinetic constant than the 20%MePh-MCM-41 due to the more hydrophobicity. Conversely, the 20%MePh-MCM-41 had much more estrogen adsorption capacities than the 20%EtPh-MCM-41 because of the more available adsorption sites. The addition of the phenyl-organosilane improved estrogen adsorption by pi-pi and hydrophobic interactions, and the Langmuir-model-based maximum adsorption amounts could reach 99.02, 83.47, and 53.60 mg g(-1) for EE2, E2, and El, respectively. But excessive concentration of phenyl-organosilane decreased adsorption capacities due to poor pore structure. Alkaline solution, which induced estrogen deprotonation and negative surface charge of absorbents, inhibited estrogen adsorption by electrostatic repulsion and the decreased hydrophobic interaction, but acidic and neutral solutions, ionic strength, and humic acid didnot significantly affect estrogen removal. This work not only showed the high potential of trimethoxyphenylsilane-modified MCM-41 used in water purification for steroid estrogens, but also demonstrated the suitable selection of organosilane precursors was key in producing favorable materials with designed functionality. (C) 2019 Elsevier Ltd. All rights reserved.

引用

页码：438 / 449

页数：12