Photocatalytic ozonation was employed for the first time in continuous mode with TiO2-coated glass Raschig rings and light emitting diodes (LEDs) to treat urban wastewater as well as surface water collected from the supply area of a drinking water treatment plant (DWTP). Different levels of contamination and types of contaminants were considered in this work, including chemical priority substances (PSs) and contaminants of emerging concern (CECs), as well as potential human opportunistic antibiotic resistant bacteria and their genes (ARB&ARG). Photocatalytic ozonation was more effective than single ozonation (or even than TiO2 catalytic ozonation) in the degradation of typical reaction by-products (such as oxalic acid), and more effective than photocatalysis to remove the parent micropollutants determined in urban wastewater. In fact, only fluoxetine, clarithromycin, erythromycin and 17-alpha-ethinylestradiol (EE2) were detected after photocatalytic ozonation, by using solid-phase extraction (SPE) pre-concentration and LC-MS/MS analysis. In surface water, this treatment allowed the removal of all determined micropollutants to levels below the limit of detection (0.01-0.20 ng L(-1)). The efficiency of this process was then assessed based on the capacity to remove different groups of cultivable microorganisms and housekeeping (16S rRNA) and antibiotic resistance or related genes (intI1, blaTEM, qnrS, sul1). Photocatalytic ozonation was observed to efficiently remove microorganisms and ARGs. Although after storage total heterotrophic and ARB (to ciprofloxacin, gentamicin, meropenem), fungi, and the genes 16S rRNA and intI1, increased to values close to the pre-treatment levels, the ARGs (blaTEM, qnrS and sul1) were reduced to levels below/close to the quantification limit even after 3-days storage of treated surface water or wastewater. Yeast estrogen screen (YES), thiazolyl blue tetrazolium reduction (MTT) and lactate dehydrogenase (LDH) assays were also performed before and after photocatalytic ozonation to evaluate the potential estrogenic activity, the cellular metabolic activity and the cell viability. Compounds with estrogenic effects and significant differences concerning cell viability were not observed in any case. A slight cytotoxicity was only detected for Caco-2 and hCMEC/D3 cell lines after treatment of the urban wastewater, but not for L929 fibroblasts.
The use of the Fenton's process for the depuration of a post-biological treated milk whey wastewater was studied, aiming to achieve adequate operational conditions for a cost effective treatment to generate a suitable effluent to be directly discharged into the natural water courses. A design of experiments was implemented in order to understand the role of the independent parameters and their combinations over the treatment process. From our results the hydrogen peroxide concentration and the ratio between [H 2 O 2 ]:[Fe 2+ ] as well as their interaction were statistically important concerning both TOC and COD removal. The experiments performed at the highest value of [H 2 O 2 ] and at the lowest level of [H 2 O 2 ]:[Fe 2+] lead to effluents accomplishing the environmental legislation. Moreover, toxicological tests revealed that the treated effluent was harmless to the ecosystems. A cost estimation analysis was performed and the catalytic activity of the remaining sludge from the homogeneous process was checked. This activity decreases with the number of reuses which reduces the possibility of the direct utilization of the sludge.
A complete industrial treatment system (involving the integration of coagulation/flocculation and Fenton processes) to depurate real wastewaters coming from two-phase olive oil production mills has been studied. The experimental results indicated that at the end of this combined strategy, involving a primary physical separation stage followed by Fenton's chemical oxidation, chemical oxygen demand (COD) is reduced up to 90% and total polyphenols' concentration is decreased up to 92%. The treated stream biodegradability (BOD5/COD) reached 0.52 and the Total Suspended Solids (TSSs) and Total Dissolved Solids (TDSs) decreased up to 95% and 69%, respectively. Fenton's procedure was optimized bearing in mind the pH adjustment step, different procedures for hydrogen peroxide addition and the use of coagulants instead of the chemical precipitation (by raising pH) to promote iron sludge settling. Our results demonstrated that pH (3.0 ± 0.1) control during the oxidation reaction improves the oxidation efficiency. Moreover, the final NaOH addition is essential to a better sludge formation and consequent precipitation of the residual iron removing also some organic matter.
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