土基沸石材料合成及修复重金属污染水体的性能与机制

  随着城市化与工业化发展进程加快，重金属已成为水污染的重要来源，对自然环境和人类健康构成严重威胁。为了解决这个问题，开发具有优异重金属吸附性能的新型吸附材料至关重要。沸石由于其独特的孔隙结构和较大的比表面积，在重金属污染水体修复中备受关注。然而，沸石的高合成成本阻碍了其在水处理工业中的大规模应用。本文提出了一种“以土治水”策略，即利用储量丰富、价格低廉，富含硅铝元素的黄土和红壤作为沸石合成的原料，以降低沸石生产成本。通过简单的水热法成功合成了八种低硅铝比（硅铝比为1~2）的土基沸石，包括黄土基ANA型沸石（Loess-ANA)、黄土基CAN型沸石（Loess-CAN）、红壤基ANA型沸石（RE-ANA）、红壤基CAN型沸石（RE-CAN）、红壤基FAU型沸石（RE-FAU）、红壤基JBW沸石（RE-JBW）、红壤基LTA型沸石（RE-LTA）和红壤基SOD型沸石（RE-SOD），并对八种土基沸石进行了形貌、物相、结构等表征。吸附实验结果表明，土基沸石对多种典型重金属具有良好的吸附性能，吸附机理包括离子交换、静电吸引和共沉淀。密度泛函理论（DFT）计算表明，从热力学的角度来看，大部分有效果的重金属离子的吸附过程可以自发进行。

  此外，本文进一步研究了八种土基沸石在多种复杂成分水体中，对重金属离子的选择性吸附性能。实验结果表明，八种土基沸石对Pb²⁺污染的去离子水、自来水、河水和海水，均有较好的去除效果，而对Cr₂O₇^2-离子的去除，几乎没有效果。在海水修复实验中，我们还探讨了pH值对典型重金属选择性吸附效果的影响。在两种重金属阴离子(AsO₂^-, Cr₂O₇^2-)共污染的海水中，当pH=5时，所有类型的土基沸石对Cr₂O₇^2-均无去除效果; 当pH=8时，除了RE-LTA，其它七种沸石材料对Cr₂O₇^2-有轻微去除效果。此外，海水中AsO₂^-的去除效果几乎不受pH条件的影响。

  总体而言，本文基于“以土治水”策略，开发了系列土基沸石材料，为典型沸石材料在重金属污染水体修复的工程应用，提出了系统的吸附效果评估数据；为未来基于“以土治水”策略的土基沸石材料合成，及其实际工程应用，提供了科学参考依据。

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