>Magister Scientiae - MSc / In South Africa, water pollution problems have continued to increase due to increasing anthropogenic activities. The increasing number of organic contaminants in various water sources can be attributed to industrial development, population growth and agricultural run- off. These activities have impacted negatively on the availability and accessibility to sustainable clean water resources, exposing citizens to water borne diseases such as cholera, diarrhoea and typhoid fever; commonly reported among children. Advanced oxidation technologies such as dielectric barrier electrohydraulic discharge (EHD), also referred to as dielectric barrier discharge (DBD), have the ability to decompose persistent organics and eliminate microbes. DBD offers advantages such as efficiency, energy saving, rapid processing, use of few or no chemicals, and non-destructive impact on the ecosystem. The system is also capable of generating ozone, hydrogen peroxide, singlet oxygen, superoxide radicals, hydroxyl radicals and other active species. The combination of these reactive species has been reported to degrade biological and chemical pollutants rapidly and efficiently. In this study, the DBD system was optimized by investigating the effect of physico-chemical, electrical parameters and reactor configurations on Methylene Blue (MB) decolouration efficiency. The physico-chemical parameters included MB concentration, solution pH and conductivity, solution volume, NaCl electrolyte concentration in the electrode compartment and air flow rate. As for electrical parameters, the effects of voltage, electrode type and size on MB decolouration efficiency were studied. The effect of the aforementioned parameters on MB decolouration efficiency was assessed by varying one parameter at a time. The following physico-chemical parameters: time (from 0 - 60 minutes), pH (2.5 - 10.5), solution conductivity (5 - 20 mS/cm), MB concentration (0.5 – 10 mg/L), solution volume (500 – 2000 mL), NaCl electrode electrolyte concentration (10 – 50 g/L) and air flow rate (2– 4 L/min) were varied in their respective ranges under the applied experimental conditions: reactor air gap 2 mm, solution volume 1500 mL, NaCl electrolyte concentration of 50 g/L in the electrode compartment, voltage 25 V (7.8 kV), airflow rate 3 L/min, 0.5 mm silver electrode and a running time of 60 minutes. As for electrical parameters, voltage (from 20 - 25 V), electrode type (copper, silver and stainless steel) and electrode diameter (0.5 – 1.5 mm) were also altered individually at the applied experimental conditions. The reactor air gap was varied from 2 to 6 mm. At the same experimental conditions, the free reactive species generated mainly H2O2 and O3, were detected and quantified using the Eisenberg and indigo methods, respectively. The optimum physico-chemical parameters were found to be MB concentration 5 mg/L, concentration of NaCl electrolyte used in the central compartment of the DBD reactor 50 g/L, solution pH 2.5, solution conductivity 10 mS/cm, air flow rate 3 L/min, solution volume 1500 mL and an optimum contact time of 30 minutes. The optimum electrical parameters were found to be: applied voltage 25 and 1.5 mm silver electrode. The following parameters MB concentration, solution conductivity and pH, applied voltage and reactor configuration significantly affected MB decolouration efficiency compared to parameters such as solution volume, the inlet air flow rate, electrode type and size and NaCl electrolyte concentration in the electrode compartment, which were less effective in enhancing MB decolouration. Moreover, for all DBD experiments performed at the applied experimental conditions, complete decolouration of MB was achieved in the first 30 minutes. However, trends between the optimized parameters and MB decolouration efficiency were mostly observed after 10 minutes. The optimized DBD system reduced the treatment time from 30 to 20 minutes without any chemical additives. Moreover, at 5 mg/L MB under the applied optimum conditions, it was proved that besides 99% of MB decolouration reached after 60 minutes, 53% of total organic carbon (TOC) removal was also achieved. The chemical oxygen demand (COD) characterizing MB toxicity was less than 5 mg/L before as well as after the DBD experiment. After 10 minutes of experiment under the following conditions: Applied voltage 25 V, MB concentration 5 mg/L, solution pH (in between 6.04 and 6.64), solution volume 1500 mL, air flow rate 3 L/min, 0.5 mm silver electrode and a contact time of 60 minutes, about 3.73 x 10-5 mol/L H2O2 was produced which decreased to 2.93 x 10-5 mol/L 10 minutes later, while O3 concentration was initially very low and could not be detected. However, 0.5 mol/L of O3 was detected after 20 minutes of operating time, thereafter, H2O2 concentration decreased continuously with time while that of O3 fluctuated as the treatment time increased. Likewise, the energy density for the production of free reactive species reached 0.87 g/ kWh in the first 10 minutes due to the presence of chromophoric functional groups such as =N+(CH3)2 in MB structure that had to be destroyed. Thereafter, the energy consumption decreased progressively to zero with an increase in treatment time due to the destruction of =N+(CH3)2 groups in MB structure with time. The correlation between the rise in the of H2O2 concentration and energy density after 10 minutes was probably due to dissociation of OH- OH bonds in H2O2 by UV light to yield OH radicals which unselectively may have attacked MB dye. Thus, MB decomposition in the current DBD reactor was mostly initiated by H2O2 and O3. The irradiation of H2O2 by UV light generated in the
DBD system was found to accelerate dye decomposition in the first 30 minutes of the experiment. The UV-vis analysis of treated MB samples confirmed that the complete decolouration of MB achieved in the first 30 minutes was due to the destruction of the chromophoric [=N+(CH3)2] group in Methylene blue structure, while the FT-IR confirmed the presence of traces of various functional groups such as C=C, C=O, C=N, NH, NH3, NO2, etc. characteristics of carboxylic acids, amines, amides, nitrogen based compounds (salts), aliphatic and unsaturated by-products remaining in the bulk solution after treatment. The salts analysis after treatment showed that 16 mg/L of nitrates and nitrites and 1.1mg/L of sulphates mainly originating from air and MB decomposition were present in the treated samples. The EHD/DBD system used in this study offers an approach to partially treat water/wastewaters and its optimization was able to significantly enhance the decomposition of the target MB dye as indicated by the reduction of total organic carbon (TOC) from 8.3 mg/L to 3.9 mg/L. Compared to previous research, this study successfully optimised a complete double cylindrical dielectric barrier discharge (DBD) reactor at ambient condition without any chemical additives.
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:uwc/oai:etd.uwc.ac.za:11394/4330 |
| Date | January 2014 |
| Creators | Mouele, Emile Salomon Massima |
| Contributors | Fatoba, O., Petrik, Leslie |
| Publisher | University of the Western Cape |
| Source Sets | South African National ETD Portal |
| Language | English |
| Detected Language | English |
| Rights | University of the Western Cape |
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