Key Laboratory of Jiangsu Province for Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
Key Laboratory of Jiangsu Province for Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
Chemosphere. 2022 Dec;308(Pt 2):136255. doi: 10.1016/j.chemosphere.2022.136255. Epub 2022 Sep 2.
Developing new catalysts for efficient degradation of micropollutants in water is of significant importance in advanced oxidation processes (AOPs). Herein, TiO/C coated CoO nanocages (CoO@TiO/C) were synthesized and their performance on micropollutants degradation was evaluated. Specifically, cobalt-based Zeolitic imidazolate framework (ZIF-67) coated by a thin layer of titanium species and polydopamine (PDA) was used as a precursor for the preparation of CoO@TiO/C by two-step calcination. The catalytic performance of peroxymonosulfate (PMS) activation towards the degradation of organic pollutants was investigated by using atrazine (ATZ) and Bisphenol A (BPA) as typical micropollutants. The efficiency and the effect of TiO/C shell on the as-synthesized catalyst were analyzed by comparing CoO derived from ZIF-67 and CoO/C derived from ZIF-67/PDA. ATZ degradation results showed that the CoO@TiO/C catalyst was the most efficient for catalytic oxidation when 99.5% of ATZ was removed within 4 min, which is 57.5% and 74.6% faster than that of CoO@C and CoO, respectively. The enhanced performance of CoO@TiO/C is attributed to their unique nanocages structure and improved specific surface area. The catalysis mechanisms and ATZ degradation pathways were presented based on the results of electron paramagnetic resonance (EPR), XPS, and LC-MS analysis. Our results might have added to the design of heterogeneous catalysts of large surface area for efficient PMS activation in AOPs.
开发用于水中微污染物有效降解的新型催化剂在高级氧化工艺(AOPs)中具有重要意义。在此,合成了 TiO/C 包覆的 CoO 纳米笼(CoO@TiO/C),并评估了其对微污染物降解的性能。具体而言,以钴基金属沸石咪唑酯骨架(ZIF-67)为前驱体,通过两步煅烧法制备 CoO@TiO/C,其中 ZIF-67 表面包覆有一层钛物种和聚多巴胺(PDA)。以莠去津(ATZ)和双酚 A(BPA)为典型微污染物,考察了过一硫酸盐(PMS)活化对有机污染物降解的催化性能。通过比较 ZIF-67 衍生的 CoO 和 ZIF-67/PDA 衍生的 CoO/C,分析了 TiO/C 壳对合成催化剂的效率和影响。ATZ 降解结果表明,CoO@TiO/C 催化剂在 4 分钟内去除了 99.5%的 ATZ,是 CoO@C 和 CoO 的 57.5%和 74.6%,是最有效的催化氧化催化剂。CoO@TiO/C 的优异性能归因于其独特的纳米笼结构和提高的比表面积。根据电子顺磁共振(EPR)、X 射线光电子能谱(XPS)和液质联用(LC-MS)分析的结果,提出了催化机制和 ATZ 降解途径。我们的研究结果可能为 AOPs 中高效 PMS 活化的大表面积异相催化剂的设计提供了参考。