Hou Jin, Wan Jinquan, Yan Zhicheng, Wang Yan, Ma Yongwen, Xie Yongchang, Chen Huajian, Xue Yangyang
College of Environment and Energy, South China University of Technology, Guangzhou, 510006, China.
College of Environment and Energy, South China University of Technology, Guangzhou, 510006, China; Guangdong Plant Fiber High-Valued Cleaning Utilization Engineering Technology Research Center, Guangzhou, 510006, China.
Chemosphere. 2022 Jun;297:134100. doi: 10.1016/j.chemosphere.2022.134100. Epub 2022 Feb 24.
In this study, a novel polydopamine (PDA)-modified metal organic frameworks (MOFs) catalyst (MIL/PDA) was successfully fabricated to activate persulfate (PS) for the degradation of sulfamethoxazole (SMX) in wastewater. The experimental results indicated that PDA-modified catalyst exhibited superior catalytic performance and enhanced the degradation of SMX (91.5%) compared to pure MOFs. The physical-chemical properties of the MIL/PDA catalyst were comprehensively characterized, and the applications in the catalytic degradation of SMX were evaluated. It was found that the modification of PDA enhanced the electron transfer, while promoting the redox cycle of Fe(III)/Fe(II), which in turn boosted the production of active oxygen species. Furthermore, MIL/PDA showed high stability and reusable performance over multiple cycles. Both radical and non-radical pathways were jointly involved in the activation process of PS were confirmed by quenching experiments combined with electron paramagnetic resonance (EPR). Based on this, the possible mechanism of the catalytic reaction was investigated. Finally, five degradation pathways of SMX degradation were proposed according to the results of liquid chromatography-mass spectrometry (LC-MS). This work provided a new insight into the design of novel and efficient heterogeneous catalysts for advanced wastewater treatment.
在本研究中,成功制备了一种新型的聚多巴胺(PDA)修饰的金属有机框架(MOF)催化剂(MIL/PDA),用于活化过硫酸盐(PS)以降解废水中的磺胺甲恶唑(SMX)。实验结果表明,与纯MOF相比,PDA修饰的催化剂表现出优异的催化性能,提高了SMX的降解率(91.5%)。对MIL/PDA催化剂的物理化学性质进行了全面表征,并评估了其在SMX催化降解中的应用。发现PDA的修饰增强了电子转移,同时促进了Fe(III)/Fe(II)的氧化还原循环,进而促进了活性氧物种的产生。此外,MIL/PDA在多个循环中表现出高稳定性和可重复使用性能。通过猝灭实验结合电子顺磁共振(EPR)证实,自由基和非自由基途径共同参与了PS的活化过程。基于此,研究了催化反应的可能机理。最后,根据液相色谱-质谱(LC-MS)结果提出了SMX降解的五条途径。这项工作为设计用于深度废水处理的新型高效非均相催化剂提供了新的见解。