State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China; State Environmental Protection Engineering Center for Organic Chemical Wastewater Treatment and Resource Reuse, Nanjing 210023, China.
Sci Total Environ. 2022 Feb 25;809:152201. doi: 10.1016/j.scitotenv.2021.152201. Epub 2021 Dec 7.
In this study, a new catalyst was fabricated by pyrolysis under nitrogen atmosphere with MIL-53(Fe) as the precursor, and was applied to catalyze Fenton-like process. Effects of calcination temperature and pH on decontamination performance, and stability of materials were investigated. Under optimal conditions (calcination temperature of 500 °C and pH of 5.0), the new Fenton-like system remained low iron leaching, and achieved high pseudo-first-order rate constant of 0.0251 min for bisphenol S (BPS) removal, which is much higher than those in MIL-53(Fe), and nano-FeO catalyzed Fenton-like systems. The superiority of the new catalyst for Fenton-like catalysis was attributed to high specific surface area, as well as formed Fe(II), coordinatively unsaturated iron center and the Fe-O/Fe-C compounds based on the analyses of characterizations. Furthermore, main active species for BPS degradation was identified as hydroxyl radicals, and total hydroxyl radical generation was determined by trapping experiments. The degradation pathways of BPS were also proposed by intermediates monitoring. Moreover, this catalyst showed good potential for practical application, according to the evaluation of reuse, different pollutants degradation, and BPS removal in real wastewater. We believe this study developed a new catalyst with high catalytic activity, high stability and wide application scope, and also sheds light on further development of metal-organic frameworks for Fenton-like catalysis.
在这项研究中，通过在氮气气氛下进行热解制备了一种新型催化剂，以 MIL-53(Fe) 为前驱体，并将其应用于类芬顿催化过程。考察了煅烧温度和 pH 值对材料去除性能和稳定性的影响。在最佳条件下（煅烧温度为 500°C，pH 值为 5.0），新型类芬顿体系保持了低铁浸出，并且双酚 S (BPS) 的去除率具有较高的拟一级速率常数为 0.0251 min，远高于 MIL-53(Fe) 和纳米 FeO 催化的类芬顿体系。新型催化剂在类芬顿催化中具有优越性，归因于其具有较高的比表面积，以及形成的 Fe(II)、配位不饱和铁中心和基于表征分析的 Fe-O/Fe-C 化合物。此外，通过捕获实验确定了 BPS 降解的主要活性物质为羟基自由基，并测定了总羟基自由基的生成量。通过中间产物监测还提出了 BPS 的降解途径。此外，根据重复使用、不同污染物降解和实际废水中 BPS 去除的评估，该催化剂显示出良好的实际应用潜力。我们相信这项研究开发了一种具有高催化活性、高稳定性和广泛应用范围的新型催化剂，并为金属有机骨架在类芬顿催化中的进一步发展提供了思路。
