Laboratory of Wastewater Treatment and Recycling, Research and Technology Center of Water, University of Carthage, BP 273, 8020 Soliman, Tunisia; National School of Engineers of Sfax, University of Sfax, Soukra road, Km 4, 3038 Sfax, Tunisia.
Solar Energy Research Centre (CIESOL), Ctra de Sacramento s/n, Almería ES04120, Spain; Chemical Engineering Department, University of Almería, Ctra de Sacramento s/n, Almería ES04120, Spain.
Sci Total Environ. 2020 Sep 20;736:139617. doi: 10.1016/j.scitotenv.2020.139617. Epub 2020 May 23.
This work presents, for the first time, a kinetic study of the solar photo-Fenton process at neutral pH mediated by the Fe-NTA complex (molar ratio 1: 1) applied to remove contaminants of emerging concern (CECs). To this end, wastewater treatment plant (WWTP) secondary effluents were treated in a raceway pond reactor (RPR) at pilot plant scale with 0.1 mM Fe-NTA and 0.88 mM HO under average solar UVA irradiance of 35 W/m. Sulfamethoxazole and imidacloprid, at 50 μg/L of initial concentration each, were selected as model CECs. Up to 40% of the sum of both model CECs was removed from simulated WWTP effluent by the Fe-NTA Fenton-like process, and >80% was removed by solar photo-Fenton. The effect of liquid depth in the reactor was evaluated, showing an increase of the treatment capacity from 12 mg CEC/m·h to 18 mg CEC/m·h when liquid depth increased from 5 to 15 cm. Afterwards, these results were validated with real WWTP effluents and compared with the results obtained with the Fe-EDDS complex under the same operating conditions. The same CEC removal rates were obtained with Fe-NTA and Fe-EDDS at 5 cm of liquid depth (kinetic constants of 0.110 min and 0.046 min for sulfamethoxazole and imidacloprid, respectively). Conversely, at 15 cm of liquid depth, the degradation rates were lower with Fe-NTA (kinetic constants of 0.034 min for sulfamethoxazole and 0.017 min for imidacloprid), whereas with Fe-EDDS the values were 0.076 min and 0.047 min for sulfamethoxazole and imidacloprid, respectively. Regarding process cost estimation, the use of NTA as iron chelate for solar photo-Fenton at neutral pH at pilot plant scale resulted very cost-effective (0.13-0.14 €/m) in comparison with the use of EDDS (0.46-0.48 €/m) at the two liquid depths tested.
本工作首次提出了在中性 pH 条件下,应用 Fe-NTA 配合物(摩尔比为 1:1)介导的太阳能光芬顿工艺对新兴污染物(CECs)进行动力学研究。为此,在中试规模的水道池反应器(RPR)中用 0.1 mM Fe-NTA 和 0.88 mM HO 处理了污水处理厂(WWTP)二级出水,平均太阳 UVA 辐照度为 35 W/m。选择磺胺甲恶唑和吡虫啉作为模型 CEC,初始浓度均为 50μg/L。通过 Fe-NTA 类芬顿工艺,模拟 WWTP 出水中的两种模型 CEC 之和的 40%被去除,而通过太阳能光芬顿则去除了>80%。评估了反应器中液体深度的影响,当液体深度从 5 cm 增加到 15 cm 时,处理能力从 12 mg CEC/m·h 增加到 18 mg CEC/m·h。然后,使用真实的 WWTP 废水对这些结果进行了验证,并与在相同操作条件下使用 Fe-EDDS 配合物获得的结果进行了比较。在 5 cm 液体深度下,使用 Fe-NTA 和 Fe-EDDS 获得了相同的 CEC 去除率(磺胺甲恶唑和吡虫啉的动力学常数分别为 0.110 min 和 0.046 min)。相反,在 15 cm 液体深度下,Fe-NTA 的降解速率较低(磺胺甲恶唑的动力学常数为 0.034 min,吡虫啉的动力学常数为 0.017 min),而 Fe-EDDS 的磺胺甲恶唑和吡虫啉的动力学常数分别为 0.076 min 和 0.047 min。关于工艺成本估算,在中试规模下,在中性 pH 条件下使用 NTA 作为铁螯合物进行太阳能光芬顿处理,与在测试的两种液体深度下使用 EDDS(0.46-0.48 欧元/m)相比,非常具有成本效益(0.13-0.14 欧元/m)。