Sun Qiang, Zheng Huaili, Hu Xuebin, Li Jun, Zhao Rui, Zhao Chun, Ding Wei
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, State Ministry of Education, Chongqing University, Chongqing 400045, China.
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China.
Polymers (Basel). 2020 Jan 2;12(1):72. doi: 10.3390/polym12010072.
In this study, a novel system was set up by preparing a magnetic flocculant combining with ultraviolet/HO to realize the rapid enrichment and degradation of diclofenac sodium (DCFS). For the magnetic flocculant, template anion polyacrylamide (TAPAM) with anion micro-block structure was prepared. Thereafter, polydopamine was used to modify TAPAM, FeO nanoparticles was grafted to the modified TAPAM by chelation, named template anion polyacrylamide-polydopamine-FeO (TAPAM-PDA-FeO). Furthermore, the TAPAM-PDA-FeO preparation protocol was optimized by the response surface method (RSM). In the DCFS enrichment section, the rapid separation of flocs from water was realized by an external magnetic field and it indicated that the π-π stacking effect was dominant in neutral/alkaline condition, whereas charge neutralization was favored in acidic conditions. Meanwhile, a DCFS enrichment kinetic curve was much fitted by the pseudo-second-order kinetic model and DCFS enrichment isothermal curve was close to the Freundlich isothermal model, indicating the dependence of DCFS quantity enriched by TAPAM-PDA-FeO and a multilayer heterogeneous enrichment process. The degradation experiment confirmed that DCFS was effectively degraded by ultraviolet/HO/TAPAM-PDA-FeO and the maximum value of DCFS degradation efficiency reached 98.1%. Furthermore, the regeneration experiment showed that the enrichment and degradation efficiency of DCFS could maintain a relatively high level in the initial three recycles.
在本研究中,通过制备一种与紫外光/羟基自由基相结合的磁性絮凝剂,建立了一个新型系统,以实现双氯芬酸钠(DCFS)的快速富集和降解。对于磁性絮凝剂,制备了具有阴离子微嵌段结构的模板阴离子聚丙烯酰胺(TAPAM)。此后,使用聚多巴胺对TAPAM进行改性,通过螯合将Fe₃O₄纳米颗粒接枝到改性后的TAPAM上,命名为模板阴离子聚丙烯酰胺-聚多巴胺-Fe₃O₄(TAPAM-PDA-Fe₃O₄)。此外,采用响应面法(RSM)对TAPAM-PDA-Fe₃O₄的制备工艺进行了优化。在DCFS富集部分,通过外部磁场实现了絮凝物与水的快速分离,结果表明,在中性/碱性条件下,π-π堆积效应起主导作用,而在酸性条件下,电荷中和作用更有利。同时,DCFS富集动力学曲线与准二级动力学模型拟合良好,DCFS富集等温线接近Freundlich等温模型,表明TAPAM-PDA-Fe₃O₄对DCFS的富集量具有依赖性,且为多层非均相富集过程。降解实验证实,紫外光/羟基自由基/TAPAM-PDA-Fe₃O₄能有效降解DCFS,DCFS降解效率的最大值达到98.1%。此外,再生实验表明,在最初的三次循环中,DCFS的富集和降解效率能够保持在较高水平。