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分子水平上理解环糊精聚合物对可电离抗生素土霉素的 pH 依赖吸附和去除作用。

Molecular insights into the pH-dependent adsorption and removal of ionizable antibiotic oxytetracycline by adsorbent cyclodextrin polymers.

机构信息

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian, China.

出版信息

PLoS One. 2014 Jan 21;9(1):e86228. doi: 10.1371/journal.pone.0086228. eCollection 2014.

Abstract

Effects of pH on adsorption and removal efficiency of ionizable organic compounds (IOCs) by environmental adsorbents are an area of debate, because of its dual mediation towards adsorbents and adsorbate. Here, we probe the pH-dependent adsorption of ionizable antibiotic oxytetracycline (comprising OTCH2 (+), OTCH(±), OTC(-), and OTC(2-)) onto cyclodextrin polymers (CDPs) with the nature of molecular recognition and pH inertness. OTCH(±) commonly has high adsorption affinity, OTC(-) exhibits moderate affinity, and the other two species have negligible affinity. These species are evidenced to selectively interact with structural units (e.g., CD cavity, pore channel, and network) of the polymers and thus immobilized onto the adsorbents to different extents. The differences in adsorption affinity and mechanisms of the species account for the pH-dependent adsorption of OTC. The mathematical equations are derived from the multiple linear regression (MLR) analysis of quantitatively relating adsorption affinity of OTC at varying pH to adsorbent properties. A combination of the MLR analysis for OTC and molecular recognition of adsorption of the species illustrates the nature of the pH-dependent adsorption of OTC. Based on this finding, γ-HP-CDP is chosen to adsorb and remove OTC at pH 5.0 and 7.0, showing high removal efficiency and strong resistance to the interference of coexisting components.

摘要

pH 值对环境吸附剂中可离子化有机化合物(IOCs)的吸附和去除效率的影响是一个有争议的领域,因为它对吸附剂和吸附物都具有双重调节作用。在这里,我们研究了可离子化抗生素土霉素(包括 OTCH2(+)、OTCH(±)、OTC(-)和 OTC(2-))在具有分子识别和 pH 值惰性的环糊精聚合物(CDPs)上随 pH 值变化的吸附作用。OTCH(±)通常具有高吸附亲和力,OTC(-)具有中等亲和力,而另外两种物质则几乎没有亲和力。这些物质被证明可以选择性地与聚合物的结构单元(例如 CD 空腔、孔道和网络)相互作用,从而以不同程度固定在吸附剂上。这些物质的吸附亲和力和机制的差异解释了 OTC 的 pH 值依赖性吸附。通过对 OTC 在不同 pH 值下的吸附亲和力与吸附剂特性的定量关系进行多元线性回归(MLR)分析,推导出了数学方程。OTC 的 MLR 分析与吸附物的分子识别相结合,说明了 OTC 的 pH 值依赖性吸附的本质。基于这一发现,选择 γ-HP-CDP 在 pH 值为 5.0 和 7.0 时吸附和去除 OTC,表现出高去除效率和对共存成分干扰的强抵抗力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1635/3897700/8b7c3a153b36/pone.0086228.g001.jpg

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