School of Engineering, University of Edinburgh, Edinburgh EH9 3JL, United Kingdom.
Environ Sci Technol. 2012 Oct 2;46(19):10597-604. doi: 10.1021/es301843s. Epub 2012 Sep 13.
The influence of solute-solute interactions on hormone retention during nanofiltration (NF) was quantified and mechanisms underlying retention identified. A new approach to predict both the mass of hormone sorbed to organic matter and the retention of hormone influenced by solute-solute interactions was applied. Laboratory-scale experiments were carried out in a cross-flow filtration system examining organic matter concentration, solution pH, and hormone type. Solute-solute interactions between HA and estrone improved estrone retention while decreasing estrone adsorption to membranes. HA concentration determined the amount of estrone bound to HA and hence affected estrone retention based on the mechanism of size exclusion. The solution pH influenced both solute-solute as well as solute-membrane interactions. Solute-solute interactions were most important below the pK(a) of estrone, whereas charge repulsion between estrone and negative functional groups of the membrane dominated estrone retention above the pK(a). Of the four hormones studied, progesterone had the greatest affinity for both HA and NF membrane, which was attributed to hydrogen bonding ability. Using partition coefficients K(OM) from solid-phase microextraction (SPME) resulted in very good agreement between predicted and experimental retention.
研究了溶质-溶质相互作用对纳滤(NF)过程中激素保留的影响,并确定了保留的机制。应用了一种新方法来预测被有机物吸附的激素质量和受溶质-溶质相互作用影响的激素保留。在跨流过滤系统中进行了实验室规模的实验,考察了有机物浓度、溶液 pH 值和激素类型。腐殖酸(HA)与雌酮之间的溶质-溶质相互作用提高了雌酮的保留率,同时降低了雌酮对膜的吸附。HA 浓度决定了与 HA 结合的雌酮的量,因此根据尺寸排阻的机制影响了雌酮的保留。溶液 pH 值影响溶质-溶质相互作用以及溶质-膜相互作用。在雌酮的 pK(a) 以下,溶质-溶质相互作用最为重要,而在 pK(a) 以上,雌酮与膜的负官能团之间的电荷排斥主导了雌酮的保留。在所研究的四种激素中,孕酮对 HA 和 NF 膜都具有最大的亲和力,这归因于氢键能力。使用固相微萃取(SPME)的分配系数 K(OM),预测和实验保留之间具有非常好的一致性。