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International Journal of Scientific Research in Environmental Sciences (IJSRES), 1(2), pp. 16-25, 2013 Available online at http://www.ijsrpub.

com/ijsres 2013 IJSRPUB

Trends in Physical-Chemical Methods for Landfill Leachate Treatment


Amin Mojiri1, Hamidi Abdul Aziz1*, Shuokr Qarani Aziz2
1

School of Civil Engineering, Engineering Campus, University Sains Malaysia, 14300 Nibong Tebal, Penang, Malaysia 2 Department of Civil Engineering, College of Engineering, University of SalahaddinErbil, Iraq *Corresponding Author: cehamidi@eng.usm.my
Received 25 December 2012; Accepted 19 January 2013

Abstract. Leachate is created while water penetrates through the waste in a landfill, carrying some forms of pollutants. The aims of this study were the review on physical-chemical methods for landfill leachate treatment. The physical-chemical ways for landfill leachate treatment like Chemical precipitation, Chemical Oxidation, CoagulationFlocculation, Membrane filtration, Ion exchange, Adsorption and Electrochemical treatment are studied. Chemical precipitation is generally used as pretreatment in order to remove high strength of ammonium nitrogen; fenton oxidation is one of these advanced oxidation processes with high efficiency and low capital costs; coagulationflocculation has been used for the removal of nonbiodegradable organic compounds and heavy metals from landfill leachate; nanofiltration (NF) is one of membrane filter and it has found a place in the removal of recalcitrant organic compounds and heavy metals from landfill leachate; adsorption is the most widely used technique for the removal of recalcitrant organic compounds from landfill leachate; the ion-exchange method offers a number of benefits containing the ability to handle shock loadings and operate over a wider range of temperatures. The landfill leachate properties, technical applicability and constraints, effluent discharge alternatives, cost-effectiveness, regulatory requirements and environmental impact are important factors to selection of the most suitable treatment technique for landfill leachate treatment. Key word: Adsorption method, Chemical Oxidation, Ion exchange, Leachate, Membrane filtration,

1. INTRODUCTION Which passes through the solid waste fill and facilitates transfer of pollutants from solid phase to liquid phase, landfill leachate is generated by the penetrating water. Because of the inhomogeneous nature of the waste and due to the different compaction densities that will be encountered, water will be able to percolate through and appear as leachate at the base of the site (Cotman and Gotvajn, 2010). Landfill leachate could be a main foundation of water contamination, if not treated and disposed safely, because it could enter through soil and subsoil. Therefore, before release, the treatment of hazardous leachate components has been made a legitimate obligation to prevent pollution of water resources and to elude both acute and chronic toxicities (Aziz et al., 2011a). Landfill leachate includes organic and inorganic contaminants in high rates. Leachate is created while water penetrates through the waste in a landfill, carrying some forms of pollutants like ammonianitrogen (NH3-N), chemical oxygen demand (COD), biological oxygen demand (BOD5), colour, suspended solids and heavy metals. It may become a potential contamination source which threats soil, surface water and groundwater, if they are not collected carefully and not discharged safely. Therefore, landfill leachate is recognized as a vital environmental problem by modern societies (Deng, 2007). Because of the increase in the world population and changes in the consumption habits, solid waste

removal has become a serious environmental problem. In the solid waste management, landfill is one of the most prevalent methods used by many countries in the world (Veli et al., 2008). The any single way is no obtainable for environmentally friendly and economically. There will be many other studies concerning the top available technology providing both maximum treatment efficiency and optimum cost. The landfill leachate treatment ways are physical, chemical and biological ones which are used in combinations (Kl et al., 2007). Removals by direct biological treatment of urban landfill leachates are generally low because of high COD (600015,000 mg.l-1) and ammonium ion (500 3000 mg.l-1) contents, high COD/BOD ratio and also due to the presence of toxic compounds such as metal ions and COD. The treatment strategy generally depends on the characteristics of the leachate. Young landfill leachates are generally treated more easily as compared to the old ones. Ways advanced for treatment of landfill leachates can be classified as physical, chemical and biological which are usually used in combinations in order to improve the treatment efficiency. The sedimentation, air-stripping, adsorption, membrane filtration are the physical methods for leachate treatment. Among the chemical ways used for leachate treatment coagulation flocculation, chemical precipitation, chemical electrochemical oxidations are the major ones (Karg and Pamukoglu, 2004).

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2. PHYSICAL AND CHEMICAL METHODS The reduction of suspended solids, colloidal particles, floating material, color, and toxic compounds by flotation, coagulation/flocculation, adsorption, chemical oxidation and air stripping are physical and chemical processes. Physical/chemical treatments for the landfill leachate are used in addition at the treatment line (pre-treatment or last purification) or to treat a specific pollutant (stripping for ammonia) (Renou et al., 2008). 3. CHEMICAL PRECIPITATION The chemical precipitation is generally used as pretreatment in order to remove high strength of ammonium nitrogen (NH4+-N), in the case of leachate treatment (Renou et al., 2008). Chemical precipitation has been used for the removal of non-biodegradable organic compounds, NH3N and heavy metals from landfill leachate because of its capability, the simplicity of the process and inexpensive equipment employed. During chemical precipitation, dissolved ions in the solution are converted to the insoluble solid phase via chemical reactions. The removal of ammoniacalnitrogen from anaerobically pre-treated leachate was studied using struvite (magnesium ammonium phosphate (MAP) precipitation in the Odayeri landfill (Turkey). Using this method, ammonia was converted into a nitrogen fertilizer such as urea. About 50% COD and 90% NH3N, with an initial COD concentration of 4024 mg/L and NH3N concentration of 2240 mg/L, were removed (Kurniawan et al., 2006). Ozturk et al. (2003) used Struvite as precipitant for the removal of NH3-N from anaerobically pre-treated leachate. The removal efficiency of NH3-N and COD were 90% and 50%, respectively. It is confirmed that the ammonium concentration in leachate could be considerably reduced by struvite precipitation. However, this process requires relatively expensive chemicals (Kochany and Lipczynska-Kochany, 2009). 4. CHEMICAL OXIDATION Chemical oxidation processes were developed at different sites in during the last years. A combination of oxidation agents as ozone or hydrogen peroxide and ultraviolet light (UV) is employed in opposite to earlier experiments. This combination shows high oxidation rates for leachate COD and AOX. The process contains of a mixing chamber to mix influent leachate and the oxidation agent and thereafter a chamber with UV-lamps. Flows are recirculated to increase elimination rates manifold of leachate. In

opposite to mixing hydrogen peroxide and water the mixing of gaseous ozone and water is more difficult. It has to be encountered that also anorganic compounds may be oxidised during the chemical oxidation step. To prevent the expensive oxidation of easy biodegradable components a biological pretreatment including nitrification / denitrification should be considered. During chemical oxidation not all organics are oxidized to carbon dioxide and water. Some organics are only partly oxidized often to biological degradable inter medial products. These new biodegradable organics shall be reduced by biological treatment. A fixed film reactor may be an option for the reduction of these relatively low concentrations of organics. It can also be considered to feed the effluent of the chemical oxidation plant back to the influent of the biological reactor (Stegmann et al., 2005). Amokrane et al. (1997) used oxidants like chlorine, potassium permanganate, ozone, and calcium hydrochloride, for landfill leachate treatment and found COD removal of 2050%. Researchers reported that the efficiency of COD reduction for mature and biologically pretreated landfill leachates were 60 to 75 %, respectively by using Fenton reagent (Lopez et al., 2004; Kang and Hwang, 2000). 4.1. Fenton Treatment The Fenton process has been widely studied in recent years, and analyses indicate Fenton process to be one of the most cost-effective alternatives among potential physicochemical technologies for leachate treatment (Deng, 2007). Fenton's oxidation is one of these advanced oxidation processes (AOPs) with high efficiency and low capital costs. It is a mixture of H2O2 and ferrous salts, capable to generate aggressive hydroxyl radicals at ambient temperature. The shaped radicals are able to oxidise a wide range of chemicals in aquatic medium, theoretically all organic compounds containing hydrogen (RH). The Fenton's procedure could be effective to achieve not only good oxidation of organics, but also their removal due to the coagulation run in the presence of ferrous salts (Gotvajn et al., 2011). Fenton process can achieve two alternative goals exploiting the strong oxidation potential of hydroxyl radicals (OH) as one of advanced oxidation processes (AOPs): first is the reduction of the chemical oxygen demand (COD) content of wastewater up to the chosen maximum allowable concentration value through the mineralization of recalcitrant contaminants; the second is the development of the biodegradability of treated effluents with the aim of making their subsequent biological treatment possible. Commonly, Fenton process is composed of following

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International Journal of Scientific Research in Environmental Sciences (IJSRES), 1(2), pp. 16-25, 2013

steps: pH adjustment, oxidation reaction, neutralization, coagulation and solidliquid separation. Under acidic situation, the organic substances are degraded by reactive free radicals OH produced in the H2O2/Fe2+ mixture, and removed by means of coagulation with formation of ferric hydroxy complexes after neutralization. Both oxidation and coagulation play vital roles in the removal of organics. It is vital to understand the mutual relationships between reaction parameters in terms of hydroxyl radical production and consumption, in order to understand better and improve Fenton reaction (Wu et al., 2010). Fenton oxidation was used by Mohajeri et al. (2010) for the removal of colour and COD from Pulau Burung stabilized landfill leachate whereby colour and COD removal were 78% and 58%, respectively (Mohajeri et al., 2010). Additionally, Gotvajn et al. (2009) mentioned that the removal efficiency of NH3N by Fenton oxidation was 40%. Several authors have been reported, that Fenton's process can achieve 6090% of COD removal of organics from landfill leachate (Gotvajn et al., 2011). Kang and Hwang (2000) mentioned that COD removal efficiency by oxidation was greatly affected by the pH value and the most effective oxidation reaction was observed below pH 4.0 (Wu et al., 2010). 5. COAGULATION-FLOCCULATION FLOCCULATION-PRECIPITATION OR

an increase on the concentration of aluminium or iron, in the liquid phase, may be observed. After the biological treatment, Flocculation/Precipitation e.g. with FeCl3, is mostly practised to reduce the organic load of the leachate. This method is not used frequently also due to the fact of the increase of chloride and/or sulfate in the leachate effluent. The flocculation / precipitation step will be necessary for the removal of the loaded activated carbon if powered activated carbon is used (Stegmann et al., 2005). The coagulationflocculation processes are widely used in drinking and wastewater treatment plants because of implementation and operation simplicity (Rivas et al., 2004). 6. MEMBRANE FILTRATION A membrane could be defined as a material that creates a thin barrier capable of selectively resisting the move of different constituents of a fluid and therefore affecting separation of the constituents (Visvanathan et al., 2000). Usually, a thin layer of material with a high surface porosity and a narrow domain of pore size affect the physical structure of the membrane. Different membrane filtration techniques: microfiltration, ultrafiltration, nanofiltration, and reverse osmosis are used in landfill leachate treatment. 6.1. Microfiltration Microfiltration with pore sizes of 0.05 to 10 microns is employed to capture microbial cells, small particles, and large colloidal. According to landfill leachate treatment, this method is not suitable to be used alone. It is recommended to be used as pretreatment process with other membrane processes (i.e. ultrafiltration, nanofiltration or reverse osmosis) or in combination with chemical treatment 10 processes so as to remove suspended matters and colloids. Piatkiewicz et al. (2001) used this method as pre-filtration stage and obtained COD removal of 25% to 35 %. 6.2. Ultrafiltration Ultrafiltration is a selective process utilizing pressures up to 10 bar. This technique is efficient to remove suspended matters either by direct filtration or with biological treatment to replace sedimentation unit. It is strongly dependant on the kind of material constituting the membrane. Syzdek and Ahlert (1984) proposed that this process might prove to be useful as a pre-treatment method for reverse osmosis. It could be employed to eliminate the larger molecular weight components of leachate that tend to foul reverse osmosis membranes (Bohdziewicz et al., 2001; Rautenbach et al., 1997). COD removal of 50% was

As shown in Table 1, coagulationflocculation has been used for the removal of non-biodegradable organic compounds and heavy metals from landfill leachate. The coagulation process destabilizes colloidal particles by the addition of a coagulant. To increase the particle size, coagulation is typically followed by flocculation of the unstable particles into bulky floccules so that they can settle more easily. This method facilitates the removal of suspended solids and colloid particles from a solution. The general approach for this method contains pH adjustment and involves the addition of ferric/alum salts as the coagulant to overcome the repulsive forces between the particles. The coagulation with FeCl3 was studied for removal of heavy metals from stabilized leachate containing high concentrations of organic and inorganic matter (Kurniawan et al., 2006). Silva et al. (2004) was expressed the coagulation and flocculation is a relatively simple method that may be used successfully in treating old landfill leachates. However, this treatment only leads to moderate removals of COD and TOC, and it has its drawbacks: sludge is produced, and in some cases, when traditional chemical coagulants are employed,

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obtained by using ultrafiltration alone (Bohdziewicz et al., 2001). Lastly, Tabet et al. (2002) reported that ultrafiltration membranes have been successfully employed in full scale membrane bioreactor plants by combination of bioreactors and membrane technology. High levels for landfill leachate treatment have been obtained by using this method. 6.3. Nanofiltration (NF) Nanofiltration (NF) has found a place in the removal of recalcitrant organic compounds and heavy metals from landfill leachate because of its unique properties between ultrafiltration (UF) and reverse osmosis (RO) membranes. It has the ability to remove particles with a molecular weight of higher than 300 Da also to inorganic substances through electrostatic interactions between the ions and membranes. Which allow charged solutes smaller than the membrane pores to be rejected, along with bigger neutral solutes and salts the significance of this membrane lies in its surface charges. As shown in Table 2, NF is also effective for the removal of heavy metals because of the negatively charged groups on the membrane. The application of NF allows material dissolved in water to be separated into monovalent and divalent ions (Kurniawan et al., 2006). 6.4. Reverse Osmosis (RO) Reverse osmosis (RO) is one of the developments in the last decade for leachate treatment is the. But in contrast to the biological treatment it is a separation process into two streams - one low contaminated permeate stream and one highly contaminated concentrate stream. If leachate from the acetic phase has to be treated a biological pre-treatment may be necessary for several reasons as increased precipitation has to be expected, low molecules may pass the membrane and fowling on the membrane surface may be enhanced. The separation of ammonium is often not sufficient during reverse osmosis. The reduction of ammonia concentrations in permeate may be increased by means of a two or multiple step reverse osmosis. In some cases ammonium is removed by means of a prestripping process or a biological nitrification and denitrification step. A disadvantage of RO is the production of the liquid concentrate (about 20 % of the leachate). The technique of back passing the concentrate into the landfill is in the opinion of the authors not the best option (Stegmann et al., 2005). Unlike RO, NF has a looser membrane structure, enabling higher fluxes and lower operating pressure for the treatment of leachate (Kurniawan et al., 2006).

Ahn et al. (2002) stated that a landfill leachate treatment plant in Korea was retrofitted to improve treatment efficiency by employing integrated membrane technique that was composed of membrane bioreactor and reverse osmosis method. The removal efficiencies of COD and NH3-N from young landfill leachate were 96% and 97 %, respectively. Other researchers stated that the removal of COD and NH3N from landfill leachate was 98% (Linde et al., 1995). 7. ION EXCHANGE Ion exchange is a reversible interchange of ions between the solid and liquid phases where there is no permanent change in the structure of the solid. This treatment is capable of effectively removing the traces of metal impurities to meet the increasingly strict discharge standards in developed countries. Prior to ion exchange, the leachate should first be subjected to a biological treatment (Kurniawan et al., 2006). The solid ion exchange particles can be classified as natural-inorganic particles (zeolites) and syntheticorganic resins, which were developed from highmolecular-weight polyelectrolytes (Bashir et al., 2010). Development of ion exchange resins and characterization of naturally occurring ion exchange materials has demonstrated a wide range of possible applications of the technology in water and wastewater treatment (Wang and Peng, 2010). The ion-exchange technique offers a number of benefits containing the ability to handle shock loadings and operate over a wider range of temperatures. Ion-exchange/adsorption processes can be advanced as post treatment to a membrane bioreactor (MBR) due to the very high degree of clarification possible. Further, sorption processes by selective ion-exchangers are ideal candidates for reduction of dissolved ammonia and phosphate to near-zero levels provided that the sorbent is ammonia and/or phosphate selective, cost effective and amenable to efficient regeneration and reuse. Some of the most popular and widely available natural ion exchangers are zeolites, which consist of an aluminosilicate molecular structure with weak cationic bonding sites. Natural zeolites have been avoided in high purity processes or where consistency is vital because of irregularities and impurities of the material. Zeolites are hydrated alumino silicates comprising silica and aluminium tetrahedra which are mutually bound by chemical covalent bonds with common oxygen atoms (Mojiri, 2011). 8. ADSORPTION Adsorption is the most widely used technique for the removal of recalcitrant organic compounds from

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International Journal of Scientific Research in Environmental Sciences (IJSRES), 1(2), pp. 16-25, 2013

landfill leachate. Fundamentally, adsorption is a mass transfer process by which a substance is transferred from the liquid phase to the surface of a solid, and becomes bound by physical and/or chemical interactions (Kurniawan et al., 2006). The adsorption of contaminants onto Activated Carbon in columns or in powder form provides better reduction in COD levels than the chemicals ways, whatever the initial organic matter concentration (Table 3). The main drawback is the need for frequent regeneration of columns or an equivalently high consumption of powdered activated carbon (PAC). Adsorption by activated carbon has been used along with biological treatment for effective treatment of landfill leachate. Nonbiodegradable organics, inert COD and the color may be reduced to acceptable levels for biologically treated landfill leachate (Renou et al., 2008). Adsorption technique is recognized as the efficient and promising elementary approach in wastewater treatment processes (Foo and Hameed, 2009). It is used as a stage of integrated chemical-physicalbiological method for leachate treatment, or simultaneously with a biological process. The most commonly used adsorbent is granular activated carbon or PAC (Mojiri, 2011). The adsorption using granular activated carbon (GAC) or powder activated carbon (PAC) has been receiving a considerable attention newly for the removal of organic and inorganic contaminants from polluted wastewater because of its inherent physical properties, large surface area, micro-porous structure, high adsorption capacity and surface reactivity (Kurniawan et al., 2006). Rodriguez et al. (2004) studied PAC and different resins efficiency in the reduction of nonbiodegradable organic matter from landfill leachate. Activated carbon presented the highest adsorption capacities with 85% COD decrease and a residual COD of 200 mg L1 (Renou et al., 2008). 9. ELECTROCHEMICAL TREATMENT In recent years, electro-chemical ways were used for treatment of organic materials having high toxicity

and low biological degradability. Electro-chemical ways like electrocoagulation (EC), electro-oxidation and electro-photo-oxidation were frequently applied for treatment of wastewaters from textile, tannery and oil industries. Treatment of landfill leachate via electro-chemical ways is also another important interest area. In most of the studies in this field, especially the electro-oxidation method was examined (Deng, 2007). 9.1. Electro oxidation In recent years, the electrochemical oxidation process has been shown to be promising for wastewater treatment, mainly because of its effectiveness and ease in operation, The process has a great efficacy for the destruction of refractory pollutants like cyanide, EDTA, aniline, and also for color removal (Chiang et al., 1995). 10. CONLUSION The landfill leachate treatment ways are physical, chemical and biological ones which are used in combinations. Physical/chemical treatments for the landfill leachate are used in addition at the treatment line (pre-treatment or last purification) or to treat a specific pollutant. Physical/chemical treatments such as Chemical precipitation, Chemical Oxidation, CoagulationFlocculation, Membrane filtration, Ion exchange, Adsorption, and Electrochemical treatment were studied in this manuscript. The landfill leachate properties, technical applicability and constraints, effluent discharge alternatives, cost-effectiveness, regulatory requirements and environmental impact are important factors to selection of the most suitable treatment technique for landfill leachate treatment.

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International Journal of Scientific Research in Environmental Sciences (IJSRES), 1(2), pp. 16-25, 2013

Table 2: Removal of organic and inorganic compounds using NF or RO ( Kurniawan et al., 2006)
Location of Landfill Kind of Process NF Type of Membrane NTR-7250 Species Pressure (bar) 3 Initial concentration (mg/L) COD NA NH3-N NA Metal 0.69 0.23 0.03 NA NA 0.61 0.50 0.03 NA 4.77 0.50 BOD NA NA NA BOD/COD pH Rejection rates (%) COD NA NH3-N NA Metal 100 99 93 NA NA 97 88 94 NA 100 100 97 99 NA NA NA 98 NA NA

NA (Not Available)

Odayeri (Turkey) Mustankorkea (Finland) Spillepeng (Sweden)

NF NF NF

SW Desal 5-DL AFC-30

Chung Nam (South Korea) Yachiyo (Japan) Pietramelina (Italy)

RO RO RO

SW-4040 DT SW30-2521

Cr(III) Cu(II) Pb(II) NA NA Pb(II) Zn(II) Cd(II) NA Mn(II) Cd(II) Zn(II) Cu(II) Cr(III) NA NA NA NA

25 6-8 20

3000 920 2000

950 220 NA

NA 84 NA

NA 0.40 NA

NA 7.6 NA

89 66 NA

72 50 NA

NA 9-11 52

1500 97.4 3840

1400 33.7 NA

450 5 1200

0.30 0.05 0.31

NA 6 6

97 100 98

96 98 NA

Hedeskoga (Sweden) Spillepeng (Sweden) Wijster (Holland) Ihlenberg (Germany) Lipowka (Poland)

RO RO RO NF RO

AFC99 NA NA NA SS

40 30 40 36-60 NA 27.6

1254 925 335 1797 170000 1780

541 280 140 336 3350 743

0.02 NA NA 0.25 NA NA

125 NA NA 54 510 331

0.10 NA NA 0.03 0.03 0.28

7 6.5 6.5 7.7 6.4 7-8

95 98 98 99 96 97

82 98 98 100 58 NA

Table 3: Treatment effectiveness of landfill leachate with the use of adsorption (Renou et al., 2008)
COD (mg.L-1) 879-940 640 108 800-2000 625 9500 1533-2580 10,750-18,420 7000 716-1765 BOD/COD 0.03 0.06 0.04-0.07 0.3 0.03-0.04 0.55 pH 7.5 8 7.9 7 7.5-9.4 7.7-8.2 7 7.58-7.60 From Landfill Landfill Landfill Landfill Landfill Landfill Landfill Landfill Landfill leachate + Municipal sewage Synthetic wastewater Pilot plant Adsorbent Granular activated carbon (columns) Granular activated carbon (columns) Powdered activated carbon Activated carbon (concentration range 210 g L1) Powdered activated carbon (2 g L1) Peat Powdered activated carbon (2 g L1) CaCO3 (particle size range 24 mm) Powdered activated carbon (concentration range 0.13.5 g L1) Powdered activated carbon (02 g L1) Granular activated carbon and resins Removal (%) 91 COD 96 TOC 55-77 color 69 COD 38 COD 90 COD 90 COD 85 non-biodegradable COD (GAC) 59 non-biodegradable COD (resin)

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Amin Mojiri is a PhD candidate in environmental engineering, School of Civil Engineering, Universiti Sains Malaysia (USM), Pulau Pinang. He is fellowship holder and research assistant at the School of Civil Engineering (USM). He is a member of Young Researchers Club, Islamic Azad University, Iran. He is editor and reviewer of some international journals. His area of specialization is waste management, waste recycling, wastewater treatment, wastewater recycling, and soil pollutions.

Dr Aziz is a Professor in environmental engineering at the School of Civil Engineering, Universiti Sains Malaysia. Dr. Aziz received his Ph.D in civil engineering (environmental engineering) from University of Strathclyde, Scotland in 1992. He has published over 200 refereed articles in professional journals/proceedings and currently sits as the Editorial Board Member for 8 International journals. Dr Aziz's research has focused on alleviating problems associated with water pollution issues from industrial wastewater discharge and solid waste management via landfilling, especially on leachate pollution. He also interests in biodegradation and bioremediation of oil spills.

Dr. Shuokr Qarani Aziz is a lecturer in the Civil Engineering Department, College of Engineering, University of Salahaddin-Erbil, Iraq. He received B.Sc. degree in Civil Engineering and M.Sc. in Sanitary Engineering from University of Salahaddin-Erbil, Iraq; Ph.D. in Environmental Engineering from Universiti Sains Malaysia (USM), Malaysia. He is editor and reviewer of some international journals. His area of specialization is Water Supply Engineering, Wastewater Engineering, Solid Waste Management, and Noise Pollution.

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