炭载纳米尖晶石锰铁氧体复合材料同步去除水体中PPCPs/重金属的效能与机理

In the past decade, great attentions have been focused on the issue of combined pollution of pharmaceuticals and personal care products (PPCPs) and heavy metal ions in surface/groundwater because of its evidence-based risks to aquatic life and human health and the lack of cost-effective and appropriate remediation techniques for removing such combined pollutants. To this end, a worthwhile study aimed at exploring and implementing an integrative technique centered on coremoval and subsequent recycle of PPCPs and heavy metals from waters using carbon supported nano-spinel manganese ferrite (CNSMF) hybrids is featured and conducted in this research program. The primary goal of this research is to develop a simple and straightforward strategy to synthesize less-aggregated and well-dispersed CNSMF while simultaneously improving its coremoval efficacy. Herein, active carbon, graphene, active carbon fibers, and carbon nanotubes are selected as models of carbon supporters to electrostatically, sterically, or electrosterically stabilize and disperse NSMF during the solvo(hydro)thermal or co-precipitation processes. Coremoval practices of PPCPs and heavy metals by CNSMF and NSMF are first presented, along with the influences of varying synthetic conditions on the dispersity and stability of NSMF and the removal of target combined pollutants, which are to be taken into account for optimizing synthesis procedures of CNSMF hybrids. Impacts of single environmental factor and its multiple ones on performance of CNSMF toward PPCPs and heavy metals are also systematically examined. Subsequently, the mechanisms for coremoval of PPCPs and heavy metals by CNSMF under differing conditions and its corresponding kinetic models are probed. Lastly, regenerating practices of used CNSMF hybrids are performed to assess the cost effectivity, manipuility and safety of integrative technique exhibited in this proposal. Research findings from this project are expected to open an avenue to exploring NSMF-related nano-remediation techniques to address the challenges associated with the combined pollution of PPCPs and heavy metals.

针对水体PPCPs和重金属复合污染问题，开展炭载纳米尖晶石锰铁氧体（CNSMF）复合材料同步去除水中PPCPs和重金属的研究，采用溶剂/水热法或共沉淀法合成CNSMF复合材料，利用复合材料的高吸附性同步去除水中PPCPs和重金属。将从微观层面上深入探究合成CNSMF复合材料的最佳工艺条件和机理，实现CNSMF的可控制备；研究影响CNSMF同步去除水中PPCPs和重金属效能的主要环境条件和工艺条件；揭示能充分反映各影响因素作用下的同步去除动力学规律与机理；探索实现CNSMF再生利用与PPCPs和重金属回收的有效方法；构建出一种高效、经济、安全且资源化程度高的CNSMF同步去除水中PPCPs和重金属的技术工艺与原理，为锰铁氧体基纳米功能材料同时去除水中PPCPs和重金属的理论发展和实际工程应用提供科学依据与技术支撑。

针对水中 PPCPs与重金属离子所形成复合污染及其潜在生态风险，开发炭载纳米尖晶石锰铁氧体（CNSMF）复合材料同步去除水中 PPCPs 和重金属的研究具有十分重要的意义。通过项目的施行，本项目实现CNSMF复合材料的可控制备及结构形貌表征，考察了并明确了各种复合材料结构形貌特征的去除PPCPs和重金属的效能，阐明了CNSMF去除PPCPs和重金属的机理和过程，并考察重收利用CNSMF和回收资源的可能性。主要完成了以下研究内容： 1. 采用共沉淀法和溶剂热法耦合高温煅烧过程制备了不同的形貌的炭载纳米尖晶石锰铁氧体复合材料Fe3O4@-MnO2、MnFexOy、磁性Mn-Fe（MFOs），对比分析了合成条件（水与异丙醇体积比、铁锰摩尔比、煅烧温度和时间）对MnFexOy晶型的影响，同时也对MnFexOy表面形貌、颗粒尺寸、表面电位、光谱吸收特征和元素价态等进行了表征分析，实现复合材料的可控制备，同时研究了不同合成条件下合成各种CNSMF对抗生素羟基苯甲酸丁酯（BuP）PPCPs和重金属（As）的去除效能，筛选出具备备高吸附位点、易于回收和可再生利用、以及能同步去除水中PPCPs和重金属的MnFexOy高效复合材料。2. 研究了溶液温度、MnFexOy剂量、PMS剂量、共存无机离子和常温下不同溶液初始pH等不同水环境化学条件下MnFexOy对BuP和As的去除影响及机制。3. 研究了不同形貌的MFOs材料去除水中典型PPCPs尼泊金丁酯（BPB）和As的效能、机理及反应动力学。4. 研究了Fe3O4@-MnO2、MnFexOy、MFOs材料的磁性及其可再生性，并比较了材料在循环实验中的效能，同时研究分析了PPCPs 和重金属回收的可能性。所取得的结果对去除水体中的PPCPs和重金属复合污染具有理论指导和实际应用参考价值。.通过项目的实施，制备出3种明显具有选择去除重金属、吸附容量高、易于回收的CNSMF复合材料，项目已发表论文8 篇（其中 SCI 论文 7 篇），待发表论文 2 篇，申请发明专利 3 项（授权 1 项），举办和参加国内外学术会议 5 次（应邀作报告 3 次），参加学术交流 1 次，培养博士后 1 名，博士生 1 名，硕士生 3 名。