Institute of Organic Contaminant Control and Soil Remediation, College of Resources and Environmental Sciences, Nanjing Agricultural University, Nanjing 210095, China.
Department of Chemistry, University of Torino, Via Pietro Giuria 5, 10125 Torino, Italy.
Water Res. 2021 Mar 15;192:116834. doi: 10.1016/j.watres.2021.116834. Epub 2021 Jan 13.
The rapid and efficient degradation of polycyclic aromatic hydrocarbon (PAH) derivatives with toxicological properties remains a substantial challenge. In this study, a cost-effective and eco-friendly catalyst, nano-MoO (0.05 g L), exhibited excellent performance in activating 4.0 mmol L peroxymonosulfate (PMS) for the degradation of naphthalene derivatives with 1 mg L in aqueous systems; these derivatives include 1-methylnaphthalene, 1-nitronaphthalene, 1-chloronaphthalene, 1-naphthylamine and 1-naphthol, with high degradation rates of 87.52%, 86.23%, 97.87%, 99.74%, and 77.16%. Nano-MoO acts as an electron donor by transferring an electron causing O-O bond of PMS to cleave producing SO, and later OH. Electron paramagnetic resonance (EPR) analysis combined with free radical quenching research indicated that SO and OH dominated the degradation of naphthalene derivatives, and O and O participated in the processes. X-ray photoelectron spectroscopy (XPS) revealed the transformation of Mo(IV) to Mo(V) and Mo(VI), which suggested that the activation process proceeded via electron transfer from nano-MoO to PMS. The applicability of the nano-MoO/PMS system in influencing parameters and stability was explored. The degradation pathways were primarily elucidated for each naphthalene derivative based on the intermediates identified in the systems. The -CH, -NO, -Cl, -OH substituents increased the positive electrostatic potential (ESP) on the molecular surface of 1-methylnaphthalene, 1-nitronaphthalene, 1-chloronaphthalene, and 1-naphthol, which reduced the electrophilic reaction and electron transfer between the reactive species and pollutants, leading to a lower degradation rate of naphthalene derivatives than the parent compound. However, the effect of -NH substituents is the opposite. These findings suggest that nano-MoO may aid as a novel catalyst in the future remediation of environments polluted with PAH derivatives.
具有毒理学性质的多环芳烃(PAH)衍生物的快速高效降解仍然是一个重大挑战。在这项研究中,一种具有成本效益和环保效益的催化剂,纳米-MoO(0.05 g L),在激活 4.0 mmol L 过一硫酸盐(PMS)方面表现出优异的性能,用于在水系统中降解萘衍生物,浓度为 1 mg L;这些衍生物包括 1-甲基萘、1-硝基萘、1-氯萘、1-萘胺和 1-萘酚,降解率高达 87.52%、86.23%、97.87%、99.74%和 77.16%。纳米-MoO 作为电子供体,通过转移电子导致 PMS 的 O-O 键断裂,产生 SO 和 OH。电子顺磁共振(EPR)分析结合自由基猝灭研究表明,SO 和 OH 主导了萘衍生物的降解,而 O 和 O 也参与了降解过程。X 射线光电子能谱(XPS)显示 Mo(IV)向 Mo(V)和 Mo(VI)的转化,这表明活化过程是通过纳米-MoO 向 PMS 的电子转移进行的。还探讨了纳米-MoO/PMS 体系在影响参数和稳定性方面的适用性。根据系统中鉴定的中间产物,主要阐明了每种萘衍生物的降解途径。-CH、-NO、-Cl、-OH 取代基增加了 1-甲基萘、1-硝基萘、1-氯萘和 1-萘酚分子表面的正静电势(ESP),降低了活性物质与污染物之间的亲电反应和电子转移,导致萘衍生物的降解率低于母体化合物。然而,-NH 取代基的影响则相反。这些发现表明,纳米-MoO 可能有助于成为未来修复受 PAH 衍生物污染环境的新型催化剂。