抗生素在非均质多孔介质中的迁移机制研究

作为四大新型污染物之一的抗生素已在全球范围内严格控制使用，但由于其持续性排入以及去除率低的特性，其在环境中的检出频率和浓度依旧逐年增加。环境中的抗生素能诱导产生抗性基因，导致人类生活环境充满抗生素和抗性基因，承受巨大安全风险。抗生素在地表水环境中的形态、分布和降解等性质目前研究较多，但在沉积物中的迁移转化机制的研究相对较少，在沉积物中的吸附动力学机制及与水动力等过程的耦合机制尚不清楚，对预测抗生素在环境中的浓度和分布，评估其环境风险带来极大挑战。为此，本文以我国高密度人口的深圳市茅洲河流域为例，研究了抗生素在河流潜流带沉积物中的分布规律，和常见抗生素在典型沉积物矿物上的吸附动力学机制和与水动力的耦合过程中抗生素的迁移机制。研究取得了如下结论：
探明了深圳市茅洲河流域潜流带中抗生素的种类、浓度水平以及分布规律。建立了快速同时检出 24 种抗生素的方法，并对茅洲河流域 26 个采样点的河水和沉积物样品中抗生素进行了检测。发现河流中抗生素浓度范围为 0.14~1.75 μg/L，沉积物中为 0~50.44 μg/kg；河流和潜流带沉积物中抗生素检出浓度最高的采样组均为养殖场和医院组，说明流域抗生素浓度受潜在污染源影响显著；河水中 β-内酰胺类和氟喹诺酮类抗生素检出总浓度占比最高，但在沉积物中四环素类抗生素检出总浓度占比最高，说明不同的抗生素迁移分配规律并不相同；大部分沉积物的上中下层并未有显著差异，说明潜流带沉积物长期受到抗生素的污染影响。揭示了沿矿物内部微裂隙扩散和吸附过程是导致抗生素呈现宏观吸附动力学行为和不可逆吸附行为的主要原因。以流域潜流带中常见的抗生素四环素（TC）和左氧氟沙星（LEV），以及常见的石英和蒙脱石矿物为例，采用批实验方法和显微光谱分析技术研究了抗生素的吸附和脱附过程及机制。研究结果表明，具有不同理化性质的 TC 和 LEV 均可沿矿物微裂隙扩散到颗粒内部，并吸附在颗粒内部微裂隙表面，呈非均质分布，与微裂隙的非均质分布相关。抗生素的扩散和吸附速率和程度受到颗粒内域表面积及性质、微裂隙体积和连通性以及抗生素离子性质的影响。吸附脱附研究发现扩散和吸附过程导致颗粒内部吸附的 TC 和 LEV明显表现出不可逆的吸附行为（脱附率约为 1.86%~20.51%），表明颗粒内部区域可能是抗生素在沉积物中的长期储存场所，并可能成为次生污染源。
抗生素在非均质多孔介质中的迁移机制复杂，受到多种过程的影响，为预测抗生素在非均质多孔介质中的迁移转化带来极大挑战。采用流动柱、微流体实验和溶质迁移模拟等方法，研究了抗生素在不同粒径/矿物填充组成的多种非均质多孔介质中的迁移过程，研究结果发现抗生素受到抗生素沿水流通道的迁移、抗生素在不同矿物表面的吸附、吸附有抗生素的细小颗粒随水流的迁移、细小颗粒沉降并在其他矿物颗粒表面形成盖层、以及颗粒盖层对后续抗生素吸附脱附等过程的影响，这些过程相互耦合，影响抗生素的迁移速率和分布。
本研究通过野外观察和采样分析、实验室吸附脱附和迁移实验、微观实验和观察、及数值模拟分析等方法，发现抗生素在城市河流的潜流带沉积物中有广泛分布，会受到矿物颗粒表面吸附和内部区域扩散和吸附过程的影响，在非均质介质中的迁移过程将进一步受到细小颗粒迁移和沉降并形成颗粒盖层的复杂耦合影响。研究结果对认识抗生素在城市流域潜流带中的分布，抗生素在多孔介质中的迁移过程和影响因素具有重要意义，对建立研究抗生素的迁移预测模型也有重要的指导意义。

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