Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, School of Environment and Energy, South China University of Technology, Guangzhou, 510006, Guangdong, China.
Key Laboratory of Ministry of Education on Pollution Control and Ecosystem Restoration in Industry Clusters, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, School of Environment and Energy, South China University of Technology, Guangzhou, 510006, Guangdong, China.
Chemosphere. 2022 Mar;291(Pt 3):133072. doi: 10.1016/j.chemosphere.2021.133072. Epub 2021 Nov 25.
Organophosphorus flame retardants (OPFRs) have been regarded as one of the most rebarbative classes of emerging contaminants due to their persistence and toxicity. In the current study, Fe-based metal organic framework (MIL-88A) was synthesized and employed as photo-Fenton catalyst for the degradation of tris-(2-chloroisopropyl) phosphate (TCPP), a typical representative of OPFRs. The observations indicated that visible light could boost the reduction of ≡Fe to ≡Fe in Fe-O clusters of MIL-88A during the photo-Fenton system and consequently induce the transformation of HO to OH, which realized efficient degradation of TCPP. Due to the excellent function of MIL-88A, the effective pH application range of photo-Fenton system was extended in comparison with traditional Fenton system. The degradation efficiency of TCPP was visibly influenced in presence of humic acid (HA). MIL-88A exhibited a commendable reusability and stability after 3 times cycle. As the photo-Fenton reaction proceeded, TCPP was disintegrated to several kinds of carboxylated, dechlorinated and hydroxylated products. The observations of metabolomics endorsed that the interference of intermediate products mixture on E. coli weakened to a certain extent. In conclusion, carboxylation, dechlorination, hydroxylation and oxidation of TCPP were likewise effective for its detoxification, revealing that heterogeneous photo-Fenton system driven by Fe-based metal organic framework will be an attractive and safe treatment technique for OPFRs control.
有机磷阻燃剂 (OPFRs) 因其持久性和毒性而被认为是最令人讨厌的新兴污染物之一。在本研究中，合成了基于铁的金属有机骨架 (MIL-88A)，并将其用作光芬顿催化剂，用于降解典型的 OPFR 代表物三-(2-氯异丙基)磷酸酯 (TCPP)。研究表明，可见光可以在光芬顿体系中促进 MIL-88A 中 Fe-O 簇中≡Fe 向≡Fe 的还原，从而诱导 HO 向 OH 的转化，实现了 TCPP 的有效降解。由于 MIL-88A 的卓越功能，与传统芬顿体系相比，光芬顿体系的有效 pH 应用范围得到了扩展。在腐殖酸 (HA) 的存在下，TCPP 的降解效率明显受到影响。MIL-88A 在经过 3 次循环后表现出良好的可重复使用性和稳定性。随着光芬顿反应的进行，TCPP 分解为几种羧化、脱氯和羟基化产物。代谢组学的观察结果证实，中间产物混合物对大肠杆菌的干扰在一定程度上减弱。总之，TCPP 的羧化、脱氯、羟基化和氧化对于其解毒同样有效，表明由基于铁的金属有机骨架驱动的非均相光芬顿体系将成为 OPFRs 控制的一种有吸引力和安全的处理技术。
