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Chemical Denitrification of Nitrate from Groundwater Via Sulfamic Acid and Zinc Metal

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Chemical Denitrification of Nitrate from Groundwater Via Sulfamic Acid and Zinc Metal Iran. J. Environ. Health. Sci. Eng., 2006, Vol. 3, No. 3, pp. 141-146 CHEMICAL DENITRIFICATION OF NITRATE FROM GROUNDWATER VIA SULFAMIC ACID AND ZINC METAL *A. Sabzali, M. Gholami, A. R. Yazdanbakhsh, A. Khodadadi, B. Musavi, R. Mirzaee Department of Environmental Health, School of Public Health, Isfahan University of Medical Science, Isfahan, Iran Received 19 Jaunuary 2006; revised 5 March 2006; accepted 20 May 2006 ABSTRACT Nitrate contamination in drinking water can cause methemoglobinemia, which is especially detrimental to infants and nursing mothers. Batch experiments in two units for catalytic reduction of nitrate from groundwater with Zn catalyst and sulfamic acid were conducted. The system includes chemical denitriphication (ChemDen reactor) and electrolytic recovery reactoers. A batch study was conducted to optimize parameters like pH, sulfamic acid concentration, Zn concentration, temperature and reaction time governing the ChemDen process. The concentrations of remained nitrate and Zn were measured at the end of the reactions. Results showed that near to 100% of nitrate decreased and the quantity of remained nitrate was <1 mg/L. pH and agitation had great effect on denitrification, and the nitrate removal rate changed rapidly when pH value ranged between 3-4. Two water quality parameters which limit this process were sulfate and chloride ions concentrations in nitrate contaminated water. Key words: Chemical denitrification, groundwater, zinc, sulfamic acid, electrolytic reactor INTRODUCTION - Nitrate (NO3 ) concentrations in groundwater organic carbon is present. Water treatment have increased globally (Kapoor and Viraragh- processes stimulate denitrification by injection of avan 1997). Wastewater, fertilizers, and livestock nutrients. Such organic compounds as methanol, farming are major sources of nitrate in groundwater methane, glucose, and starch or mixtures of these supplies. Groundwater in many locations is used (e.g. a sugary brewery waste) can be used as as a supply for drinking water, and high nitrate carbon sources (Soresen and Jorgensen, concentrations present a potential risk to public 1993). The feasibility of biologically removing health, particular to infants (Gangolli et al., 1994). nitrate from groundwater had tested by using In the United States, the Environmental Protection cyanobacterial cultures. Results demonstrated Agency has set a maximum contaminant level that nitrate contaminated groundwater, when (MCL) for nitrate in drinking water of 0.71 mM supplemented with phosphate and some trace (10 mg of NO3-N L) (Pontius, 1993). There are elements, can be used as growth medium many methods for nitrate removal from water. supporting vigorous growth of several strains of Biological denitrification reduces nitrate to a cyanobacteria. As cyanobacteria grew, nitrate was gaseous nitrogen species. The gaseous product is removedfrom the water (Qiang et al., 2001). primarily nitrogen gas, but it may also be nitrous Nitrate removal by hydrogen coupled denitrification oxide or nitric oxide. A broad range of bacteria, was examined using flow through, packed-bed including many in the genera Pseudomonas, bioreactors for treating nitrate contaminated Micrococus, Archromobacter, Thiobacillus, and drinking-water supplies. Nitrate removal was Bacillus can reduce nitrate. Natural biological accomplished using a Rhodocyclus sp., strain denitrification occurs, although not extensively, in HOD 5, isolated from a sole-source drinking-water aquifiers in which a sufficient source of reducing aquifer (Smith et al., 2005). Chemical methods for decomposing nitrate can *Corresponding author-Email: [email protected] be divided into two groups: nonspecific methods Tel: +98 21 5506 9284, Fax: +98 21 5531 8695 and methods designed for nitrate decomposition. 141 Iran.A. J.Sabzali, Environ. et Health. al., CHEMICAL Sci. Eng., DENITRIFICATION 2006, Vol. 3, No. 3,OF... pp. 141-146 There is no simple chemical method that would The process can be configured in two ways. The reduce nitrate to nitrogen gas at low temperature electrolytic cell is installed as a separate unit, or it and pressure. It is relatively easy to reduce nitrate is built into the denitrifying reactor. In the second to ammonia, but it is much more challenging to case, the reactor first performs the denitrification stop the reduction at molecular nitrogen. Many and then is switched to the Zn recovery mode. A metals, such as magnesium, manganese, Zn, power supply provides a low-voltage DC current chromium, iron, cadmium, tin, aluminum, and lead for Zn recovery in the reactor (Dziewinski and will reduce nitrate. The final reduction products Barber, 1999). are governed by the temperature, the pH, and the metal used. MATERIALS AND METHODS Zhang and coworkers (2003) had conducted a Sulfamic Acid 99% (Merck), Zn Metal Powder batch experiment on catalytic reduction of nitrate (Merck), KNO3 (Merck), NaCl (Merck), CaCO3 from groundwater with Pd and/Cu catalysts. It (Merck). Nitrate concentrations were measured was founded that Pd-Cu combined catalysts at a by PU 8700 UV/Visible spectrophotometer in ratio of 4 can maximize the nitrate reduction into wavelengths of 220nm and 275nm. All samples nitrogen; above 80% total nitrogen removal were measured as dilutions series and directly efficiency was achieved (Zhang et al., 2003). At injected into the cell of spectrophotometer. Los Alamos National Laboratory (LANL), Dr. Zn concentrations were measured by Varian Dziewinski had invented a simple and robust Techtron AA-5 atomic absorption unit. The unit chemical process that converts nitrate in water was operated at a wavelength o f 2146 Aº, a s lit into environmentally benign gaseous nitrogen. In width o f 150 µm, and a constant current of 5 this process, nitrate-contaminated water is added milliamps. An air-acetylene fuel mixture was used to a simple chemical reactor, where it is contacted and was adjusted t o produce an oxidizing flame. with two inexpensive chemical reagents: sulfamic A spike and recovery analysis was performed on acid and Zn. These two reagents reduce the nitrate samples collected from effluent to check for to gaseous nitrogen according to the following interferences. This was accomplished by taking overall reaction (Dziewinski and Barber, 1999): 300 m l samples o f known concentrations and NO3- + Zn + H+ + H NSO H adding a 20% spike (Zn concentration) prior to 2 3 reanalysis. These results typically showed 2- 2+ N2 + SO4 + Zn + 2H2O excellent agreement between expected and (1) measured values (less than 5% deviation), The generated Zn cations were subsequently suggesting no significant interferences were electrolytically reduced back to the metallic state. present. Water samples were collected from each Thus Zn was not a consumed reagent; it of the two separate compartments. A schematic considered as a mediator or catalyst. The system drawing of the pilot plant includes chemical consisted of a simple reaction vessel, an agitator, denitriphication (ChemDen reactor) and and an electrolytic cell. Sulfamic acid was a electrolytic recovery reactoers which was consumable reagent, and Zn was a reusable developed for testing is shown in Fig. 1. The pilot reagent. Based on the nitrate concentration in the consisted of a two plexiglas rectangular container waste, appropriate quantities of sulfamic acid were with effective volume of 4.5 liters. ChemDen added while Zn remains in excess in the reactor contained one stainless steel mixer and reactor. Zn is oxidized to form Zn++ ion and then one outlet valve. In electrolytic recovery reactor reduced back to Zn metal by electrolysis. stainless steel plate as anode and graphite as The process begins immediately after nitrate is cathode were utilized as electrodes because it was introduced to the reactor and bubbles of nitrogen believed that this type of material would be readily gas are released to the atmosphere. When the available to the typical plates, increasing the ease reaction is complete, the treated water can be at which this configuration could be set up by the safely released to the environment. platter in their own facility. The electrodes plates 142 Iran. J. Environ. Health. Sci. Eng., 2006, Vol. 3, No. 3, pp. 141-146 were hung from an electrically insulated rack medium). Manual line was obtained by collecting above the reactor and extended vertically 500 mL samples at 30 min intervals for 2 hours. downward into the water. Alternate plates were Three 300 mL aliquots of the composite were taken connected in parallel to a 2 amps direct current for analysis. In optimum ratio of reactants, the rectifier and voltage had changed from 0-5 v. concentration of sulfate and chloride were measured in various nitrate concentrations. All Chem Den reactor samples in first experiments had prepared via distilled water. In second experiment prepared sample from Firouzkooh wells was used in order Mixer Electrolytic unit to evaluate the effects of other anions and cations in groundwater. The water quality parameters in prepared sample have been shown in Table 1. The Electrodes Valve Zn powder and sulfamic acid were added into water as obtained optimum ratio of reactants. Table 1: Water quality parameters in groundwater sample from Firouzkooh Parameter Unit Concentration (mg/L) Nitrate mg/L 130 Sulfate mg/L 75 Chloride mg/L 45 Alkalinity mg/L as CaCO3 315 pH - 7.6 Fig. 1: The schematic drawing of the pilot plant T.H mg/L as CaCO3 420 ChemDen reaction was carried out in duplicate and in a batch mode. This experiment had done in RESULTS
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