Laboratoire Réactions et Génie des Procédés (LRGP), UMR CNRS 7274, Université de Lorraine, 1 rue Grandville, 54001, Nancy, France.
Laboratory of Materials, Catalysis, Environment and Analytical Methods, Faculty of Sciences I, Lebanese University, Campus Rafic Hariri, Beirut, Lebanon.
Environ Sci Pollut Res Int. 2018 Dec;25(35):34950-34967. doi: 10.1007/s11356-018-1214-0. Epub 2018 Jan 11.
In this paper, for the first time, faujasite Y zeolite impregnated with iron (III) was employed as a catalyst to remove a real cocktail of micropollutants inside real water samples from the Meurthe river by the means of the heterogeneous photo-Fenton process. The catalyst was prepared by the wet impregnation method using iron (III) nitrate nonahydrate as iron precursor. First, an optimization of the process parameters was conducted using phenol as model macro-pollutant. The hydrogen peroxide concentration, the light wavelength (UV and visible) and intensity, the iron loading immobilized, as well as the pH of the solution were investigated. Complete photo-Fenton degradation of the contaminant was achieved using faujasite containing 20 wt.% of iron, under UV light, and in the presence of 0.007 mol/L of HO at pH 5.5. In a second step, the optimized process was used with real water samples from the Meurthe river. Twenty-one micropollutants (endocrine disruptors, pharmaceuticals, personal care products, and perfluorinated compounds) including 17 pharmaceutical compounds were specifically targeted, detected, and quantified. All the initial concentrations remained in the range of nanogram per liter (0.8-88 ng/L). The majority of the micropollutants had a large affinity for the surface of the iron-impregnated faujasite. Our results emphasized the very good efficiency of the photo-Fenton process with a cocktail of a minimum of 21 micropollutants. Except for sulfamethoxazole and PFOA, the concentrations of all the other microcontaminants (bisphenol A, carbamazepine, carbamazepine-10,11-epoxide, clarithromycin, diclofenac, estrone, ibuprofen, ketoprofen, lidocaine, naproxen, PFOS, triclosan, etc.) became lower than the limit of quantification of the LC-MS/MS after 30 min or 6 h of photo-Fenton treatment depending on their initial concentrations. The photo-Fenton degradation of PFOA can be neglected. The photo-Fenton degradation of sulfamethoxazole obeys first-order kinetics in the presence of the cocktail of the other micropollutants.
本文首次采用负载铁(III)的丝光沸石作为催化剂，通过非均相光芬顿法去除来自默尔特河的实际水样中的真实污染物混合物。催化剂采用硝酸铁九水合物作为铁前驱体制备。首先，通过使用苯酚作为模型大分子污染物对工艺参数进行了优化。考察了过氧化氢浓度、光波长（UV 和可见光）和强度、固定化铁负载量以及溶液 pH 值。在 pH 值为 5.5 的条件下，使用含有 20wt.%铁的丝光沸石，在紫外光下，完全实现了污染物的光芬顿降解。在第二步中，使用优化后的工艺处理来自默尔特河的实际水样。特别针对 21 种微污染物（内分泌干扰物、药物、个人护理产品和全氟化合物）进行了检测和定量分析，其中包括 17 种药物化合物。所有初始浓度均在纳克/升范围内（0.8-88ng/L）。大多数微污染物对负载铁的丝光沸石表面具有很强的亲和力。我们的结果强调了光芬顿工艺对至少 21 种微污染物混合物的非常高的效率。除了磺胺甲恶唑和 PFOA 外，所有其他微量污染物（双酚 A、卡马西平、卡马西平-10,11-环氧化物、克拉霉素、双氯芬酸、雌酮、布洛芬、酮洛芬、利多卡因、萘普生、PFOS、三氯生等）的浓度在光芬顿处理 30 分钟或 6 小时后均低于 LC-MS/MS 的检测限，具体取决于其初始浓度。PFOA 的光芬顿降解可以忽略不计。磺胺甲恶唑的光芬顿降解在其他微污染物混合物的存在下遵循一级动力学。
