Removal of Paracetamol Using Effective Advanced Oxidation Processes (original) (raw)
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Water Research, 2012
The photo-Fenton degradation of paracetamol (PCT) was evaluated using FeSO 4 and the iron complex potassium ferrioxalate (FeOx) as iron source under simulated solar light. The efficiency of the degradation process was evaluated considering the decay of PCT and total organic carbon concentration and the generation of carboxylic acids, ammonium and nitrate, expressed as total nitrogen. The results showed that the degradation was favored in the presence of FeSO 4 in relation to FeOx. The higher concentration of hydroxylated intermediates generated in the presence of FeSO 4 in relation to FeOx probably enhanced the reduction of Fe(III) to Fe(II) improving the degradation efficiency. The degradation products were determined using liquid chromatography electrospray time-of-flight mass spectrometry. Although at different concentrations, the same intermediates were generated using either FeSO 4 or FeOx, which were mainly products of hydroxylation reactions and acetamide. The toxicity of the sample for Vibrio fischeri and Daphnia magna decreased from 100% to less than 40% during photo-Fenton treatment in the presence of both iron species, except for D. magna in the presence of FeOx due to the toxicity of oxalate to this organism. The considerable decrease of the sample toxicity during photo-Fenton treatment using FeSO 4 indicates a safe application of the process for the removal of this pharmaceutical.
Photonic efficiency of the photodegradation of paracetamol in water by the photo-Fenton process
Environmental Science and Pollution Research, 2014
An experimental study of the homogeneous Fenton and photo-Fenton degradation of 4-amidophenol (Paracetamol, PCT) is presented. For all the operation conditions evaluated, PCT degradation is efficiently attained by both Fenton and photo-Fenton processes. Also, photonic efficiencies of PCT degradation and mineralization are determined under different experimental conditions, characterizing the influence of hydrogen peroxide (H 2 O 2) and Fe(II) on both contaminant degradation and sample mineralization. The maximum photonic degradation efficiencies for 5 and 10 mg L-1 Fe(II) were 3.9 (H 2 O 2 = 189 mg L-1) and 5 (H 2 O 2 = 378 mg L-1), respectively. For higher concentrations of oxidant, H 2 O 2 acts as a "scavenger" radical, competing in pollutant degradation and reducing the reaction rate. Moreover, in order to quantify the consumption of the oxidizing agent, the Specific Consumption of the Hydrogen Peroxide was also evaluated. For all operating conditions of both hydrogen peroxide and Fe(II) concentration, the consumption values obtained for Fenton process were always higher than the corresponding values observed for photo-Fenton. This implies a less efficient use of the oxidizing agent for dark conditions.
Latin American Applied Research - An international journal, 2016
Environmental hazards are a consequence of the massive use of synthetic chemicals that are prevalent in nearly every aspect of modern life. The outburst of the so-called “emerging pollutants” (pharmaceuticals and pesticides among others) generates an additional problem due to the scarce available information on their impact on the environment or their interferences with the biological processes. Among them, paracetamol is one of the drugs the most widely found in hospital effluents, in the effluents of wastewater treatment plants, as well as in rivers. In this work, the feasibility of paracetamol degradation by different processes based on ultraviolet radiation is discussed: photolysis, photo-oxidation with hydrogen peroxide, photo-Fenton reaction, and heterogeneous photocatalysis with TiO2 are evaluated. The best results are obtained with the photoFenton process, for which more than 99% of the pharmaceutical is degraded within 5 minutes. At best experimental conditions the minerali...
Treatment of real paracetamol wastewater by fenton process
Chemical Industry and Chemical Engineering Quarterly, 2017
The study investigated the pretreatment of real paracetamol (PCT) wastewater of a pharmaceutical industry by Fenton process. At the best experimental conditions (COD/H2O2 = 1/1, Fe+2/H2O2 = 1/70, settling method:centrifuging, pH 6 at settling step), 92.7, 92.7, 95.5, 99.1, 99.9 and 99.4% of chemical oxygen demand (COD), total organic carbon (TOC), 5-day biological oxygen demand (BOD5), PCT, para-amino phenol (PAP) and aniline were removed, respectively. Changes in the concentrations of these parameters were also investigated for both oxidation and settling steps of Fenton process. It was found that COD and TOC were removed at the settling step (precipitation) whereas PCT, PAP and aniline were removed at the oxidation step. Mass balance calculations were also studied to show the mass distributions of COD in different phases (gas + foam, effluent and sludge). Fenton process was found as an effective method for the pretreatment of real PCT wastewater for discharging in a determined col...
Pharmaceuticals are one of the most reported categories of anthropogenic micropollutants, which often require a specific remediation type to be eliminated from the environment. This study aimed to address the potential of degrading the pharmaceutical pollutant paracetamol (PCT) in the aqueous environment under ultrasound (US) assisted electro-Fenton by Fe 2 O 3 (hematite) nanoparticles (HNPs) as a catalyst. The synthesized sample was characterized by various techniques including XRD, FESEM, EDS, X-ray dot-mapping, and FTIR. The performance of the electro-Fenton (EF) and US processes was evaluated separately and in combination under optimum conditions. The results showed that the sonoelectro-Fenton (SEF) process under optimum conditions, including pH of 5, HNPs dosage 0.15 g/L, applied current 230 mA, initial PCT concentration 20 mg/L, resulted in a PCT degradation of 98.9% within 60 min of electrolysis time. PCT degradation was well-fitted to the pseudo-firstorder kinetic model. Meanwhile, scavenging experiments indicated the vital role of • OH in the decomposition of PCT compared to the negligible role of O •− 2. The nitrate ions had a strong inhibitory effect, whereas chloride anions affected PCT elimination slightly. The reusability test of HNPs revealed that almost a 14% drop occurred at the end of the fourth cycle. The HNPs showed high catalytic activity for degradation of PCT compared to other conventional homogeneous transition metals. Besides, SEF-HNPs can successfully detoxify the PCT solution based on the bioassay test. The by-products of PCT degradation by SEF-HNPs were determined and degradation pathway was also proposed. Conclusively, the SEF-HNPs process could be an appropriate system for the removal of various contaminants from aqueous solutions.
AIChE Journal, 2016
Paracetamol is commonly found in wastewaters, as a consequence of its high consumption and incomplete elimination by conventional treatments. Homogenous (photo-)Fenton oxidation has proved efficient for its remediation, but it suffers from uneasy dissolved iron recovery. Therefore this work examines the performance and stability of an iron containing zeolite (Fe/MFI) as catalyst for this reaction. Effects of reaction parameters (pH, temperature, catalyst and H 2 O 2 concentrations, UV/vis irradiation) are investigated in batch conditions, by comparing the pollutant and Total Organic Carbon disappearance rates in solution, as well as the overall mineralization yield (including solid phase) and oxidant consumption. At near neutral pH paracetamol can be fully converted after 5 h, while TOC removal reaches up to 60%. Finally, thanks to good catalyst stability (low leaching), a continuous process coupling oxidation and membrane filtration is proposed, showing constant TOC conversion over 40 h and iron loss in the permeate <0.3 ppm.
Applied Catalysis B: Environmental, 2011
The degradation of 10 L of 157 mg L −1 paracetamol solutions in 0.05 M Na 2 SO 4 has been studied by the solar photoelectro-Fenton (SPEF) method. A solar flow plant with a Pt/air-diffusion electrochemical cell and a compound parabolic collector (CPC) photoreactor was used operating under recirculation mode at a liquid flow of 180 L h −1 with an average UV irradiation intensity of about 32 W m −2. A central composite rotatable design coupled with response surface methodology was applied to optimize the experimental variables. Optimum SPEF treatment was achieved by applying a current of 5 A, 0.40 mM Fe 2+ and pH 3.0 at 120 min of electrolysis, being reduced total organic carbon (TOC) by 75%, with an energy cost of 93 kWh kg −1 TOC (7.0 kWh m −3) and a mineralization current efficiency of 71%. Initial N was partially converted into NH 4 + ion. Under these optimized conditions, paracetamol decays followed a pseudo first-order kinetics. HPLC analysis of the electrolyzed solution allowed the detection of hydroquinone, p-benzoquinone, 1,2,4-trihydroxybenzene, 2,5-dihydroxy-p-benzoquinone and tetrahydroxy-p-benzoquinone. All aromatics were destroyed by the attack of • OH. Maleic, fumaric, succinic, lactic, oxalic, formic and oxamic acids were identified as generated carboxylic acids, which form Fe(III) complexes that are quickly photodecarboxylated under UV irradiation of sunlight. A reaction sequence involving all the detected byproducts was proposed for the SPEF degradation of paracetamol.
Current Organic Chemistry, 2018
Background: In recent years, there has been a growing interest in the environmental relevance of the presence of several pharmaceutical compounds and their metabolites in water. To avoid further accumulation of these compounds and their metabolites in the aquatic environment, several research groups are investigating chemical and photochemical methods that could be applied in their destruction and subsequent removal from natural and wastewater. Objective & Method: Different chemical advanced oxidation processes are being developed to destroy organic pollutants in water. Most of these methods are based on the production of HO• radicals that are known to be highly reactive and strong oxidizing agents. In aqueous chemical processes, these radicals can be generated using a variety of reagents and under different reaction conditions such as O3, H2O2/UV, TiO2/UV, O3/UV, H2O2/Fe 2+ , H2O2/Fe 2+ /UV and O3/Fe 2+ /Cu 2+ /UV. This review is a survey on recent advances in the application of different chemical advanced oxidation processes to mineralize pharmaceuticals. Paracetamol was selected as a model compound since its structure is the main component or metabolite of several anesthetic and analgesic compounds. The degradation of paracetamol by different advanced oxidation methods has been investigated by a combination of techniques (TOC, UV-Vis, IR, HPLC and GC-MS) in order to determine the optimal reaction conditions, kinetics, intermediate and product compounds generated. Conclusion: Understanding the basic concepts about reaction conditions, intermediates and mechanistic details on mineralization of paracetamol will be quite useful for future applications of several techniques in the removal of this and other structurally related pharmaceutical and aromatic compounds from water.
Enhancement of Paracetamol Degradation by Sono-Fenton Process
The study of the advanced oxidation processes involving enough quantities of "in situ" free radicals formation to produce water purification, has become a research topic of special interest in the last years. The paracetamol is one of the pharma-ceuticals frequently detected in wastewaters, surface waters, groundwaters, drinking water, soils and sediments. In this work, the intensification of paracetamol degradation in aqueous solution by ultrasound/H2O2 and ultrasound/Fenton processes was studied. The paracetamol degradation was strongly affected by the ultrasonic power and frequency, pH and the initial concentrations of Fe2+/H2O2. The degradation of paracetamol increases with increasing ultrasonic power. The total degradation of pharmaceutical is obtained at 60 min for all studied concentrations of hydrogen peroxide and ferrum salt. The optimal conditions of sono-Fenton process guarantee a mineralization higher than 60 % are 4.7 mmol L-1 of Fe2+ and 14.4 mmol L-1 H2O2.