Physico-chemical treatments for removal of recalcitrant contaminants from landfill leachate

In this paper, the technical applicability and treatment performance of physico-chemical techniques (individual and/or combined) for landfill leachate are reviewed. A particular focus is given to coagulation-flocculation, chemical precipitation, ammonium stripping, membrane filtration and adsorption. The advantages and limitations of various techniques are evaluated. Their operating conditions such as pH, dose required, characteristics of leachate in terms of chemical oxygen demand (COD) and NH3-N concentration and treatment efficiency are compared. It is evident from the survey of 118 papers (1983-2005) that none of the individual physico-chemical techniques is universally applicable or highly effective for the removal of recalcitrant compounds from stabilized leachate. Among the treatments reviewed in this article, adsorption, membrane filtration and chemical precipitation are the most frequently applied and studied worldwide. Both activated carbon adsorption and nanofiltration are effective for over 95% COD removal with COD concentrations ranging from 5690 to 17,000 mg/L. About 98% removal of NH3-N with an initial concentration ranging from 3260 to 5618 mg/L has been achieved using struvite precipitation. A combination of physico-chemical and biological treatments has demonstrated its effectiveness for the treatment of stabilized leachate. Almost complete removal of COD and NH3-N has been accomplished by a combination of reverse osmosis (RO) and an upflow anaerobic sludge blanket (UASB) with an initial COD concentration of 35,000 mg/L and NH3-N concentration of 1600 mg/L and/or RO and activated sludge with an initial COD concentration of 6440 mg/L and NH3-N concentration of 1153 mg/L. It is important to note that the selection of the most suitable treatment method for landfill leachate depends on the characteristics of landfill leachate, technical applicability and constraints, effluent discharge alternatives, cost-effectiveness, regulatory requirements and environmental impact.     

Granular activated carbon promoted ozonation of a food-processing secondary effluent

This paper reports on the application of a simultaneous combination of ozone and a granular activated carbon (O(3)/GAC) as a tertiary treatment of a wastewater generated from the activity of various food-processing industries. Prior to the O(3)/GAC treatment, the wastewater was subjected to conventional primary and secondary treatments in a full-scale wastewater treatment plant (WWTP). The effluent from the WWTP presented high organic load (COD>500 mg/l and TOC>150 mg/l), which could be much reduced by the O(3)/GAC treatment. Results from the O(3)/GAC experiments were compared with those obtained in single ozonation, single adsorption onto GAC and sequential O(3)-GAC adsorption experiments. While single processes and the sequential one showed limited capacity to remove organic matter for the food-processing effluent (COD removal <40%), the simultaneous O(3)/GAC process led to decreases of COD up to 82% at the conditions here applied. The combined process also improved the ozone consumption, which decreased from about 19 g O(3)/g TOC (single ozonation process) to 8.2-10.7 g O(3)/g TOC (O(3)/GAC process). The reusability of the GAC throughout a series of consecutive O(3)/GAC experiments was studied with no apparent loss of activity for a neutral GAC (PZC = 6.7) but for a basic GAC (PZC = 9.1).     

Degradation characteristics of secondary effluent of domestic wastewater by combined process of ozonation and biofiltration

The performance of the combined process of ozonation and biofiltration was studied for treating the secondary effluent from sewage treatment plant. It was found that COD, NH(3)-N, and TOC were removed from 40-52, 10-19, and 9-13 mg/L in the raw water to 18-23, 0.5-1.5, and 7-8.5 mg/L in the effluent water (removal efficiency were 58, 89, and 25%, respectively), respectively, with an ozone dose of 10 mg/L (0.7-1.1 mg O(3)/(mg TOC) and 0.2-0.25 mg O(3)/(mg COD)), and contacting time of 4 min. Under the operation conditions, ozonation enhanced the biodegradability of the organics in the secondary effluent, as illustrated by increasing biodegradable dissolved organic carbon (BDOC) value from 0.8-1.1 mg/L in the raw water to the 2.0-2.7 mg/L in the effluent water. Meanwhile, the percentage of the organics with molecular size less than 1k Da in the secondary effluent increased from 52.9 to 72.6%. The experimental results supported the expectation that the combined process of O(3)/Biofiltration might enhance the overall treatment efficiency of secondary effluent treatment.     

Ozonation of a landfill leachate: evaluation of toxicity removal and biodegradability improvement

This work shows an evaluation of treatments for the leachate produced at the Gramacho Municipal Landfill in Rio de Janeiro state, Brazil. This leachate has very peculiar characteristics, with a high salinity level and very low biodegradability (BOD(5)/COD of 0.05). A sequence of processes was employed in the treatment of this leachate. Initially, a physicochemical treatment was used, while the second stage consisted of application of ozone to improve the biodegradability of the leachate. The final stage comprised a biological treatment. The physical-chemical treatment led to COD and DOC removal levels of 40 and 25%, respectively, with the use of Al(2)(SO(4))(3). The sequence of treatments proposed brought good results, with an increase in the BOD(5)/COD ratio from 0.05 to 0.3 after ozonation. The toxicity tests performed using Brachydanio rerio and Poecilia vivipara showed that the toxicity of the leachate had hardly been reduced by ozonation. These results are in agreement with the fact that, despite the higher BOD(5)/COD ratio, the biological process did not present a good performance. The total average removal levels of COD and DOC achieved using the combined treatment were 73 and 63%, respectively, for an ozone dose of 3.0 gL(-1) by the leachate.     

Decomposition of toxic pollutants in landfill leachate by ozone after coagulation treatment

This study deals with evaluation of organic matter from Mexico City waste sanitary landfill leachate of Bordo Poniente (including domestic and industrial) by ozonation after a coagulation treatment with Fe2(SO4)(3) (2.5 g/L at pH 4-5). The content of humic substances after the coagulation treatment decreases up to 70%. Then leachate obtained from a solid with initial COD=1511 mg/L and the pH 8.5 was treated by ozone. The aqueous samples by a UV-vis and HPLC technique were analyzed. The partial identification of the initial composition of the organic matter as well as of intermediates and final products was carried out after the extraction of the initial and ozonated leachate with benzene, chloroform:methanol (2:1) and hexane. Then the extracts with a gas chromatograph with mass detector and FID were analyzed. In the HPLC results we identify malonic and oxalic acids. The initial concentrations of these acids were 19 mg/L and 214 mg/L, respectively. The oxalic acid is formatted and accumulated in ozonation. The obtained results show that the color disappears (visually) at 100% during 5 min of ozonation. The organic substances, extracted with chloroform-methanol, may be destructed during 15 min of ozonation; the organic matter, extracted with benzene, destructs completely by ozone during 5 min, and the organic compounds extracted with hexane have a low ozonation rate. The toxic compounds presented in leachate decompose completely during 15 min of ozonation. The ozonation rate constants for each group of organics (as observed constants) were calculated applying simplified mathematical model and the recurrent least square method using the program MATLAB 6.5.     

Tertiary treatment of textile wastewater with combined media biological aerated filter (CMBAF) at different hydraulic loadings and dissolved oxygen concentrations

An up-flow biological aerated filter packed with two layers media was employed for tertiary treatment of textile wastewater secondary effluent. Under steady state conditions, good performance of the reactor was achieved and the average COD, NH(4)(+)-N and total nitrogen (TN) in the effluent were 31, 2 and 8mg/L, respectively. For a fixed dissolved oxygen (DO) concentration, an increase of hydraulic loading resulted in a decrease in substrate removal. With the increase of hydraulic loadings from 0.13 to 0.78m(3)/(m(2)h), the removal efficiencies of COD, NH(4)(+)-N and TN all decreased, which dropped from 52 to 38%, from 90 to 68% and from 45 to 33%, respectively. In addition, the results also confirmed that the increase of COD and NH(4)(+)-N removal efficiencies resulted from the increase of DO concentrations, but this variation trend was not observed for TN removal. With the increase of DO concentrations from 2.4 to 6.1mg/L, the removal efficiencies of COD and NH(4)(+)-N were 39-53% and 64-88%, whenas TN removal efficiencies increased from 39 to 42% and then dropped to 35%.     

Biological treatability of raw and ozonated penicillin formulation effluent

In the present study, oxidative pre-treatment of pharmaceutical wastewater originating from the formulation of the penicillin Sultamycillin Tosylate Diydrate via ozonation at varying pH and ozone feed rates was investigated. Biological treatability studies were performed with a synthetic wastewater alone and supplemented with raw and ozonated penicillin formulation effluents. The highest COD (34%) and TOC (24%) removal efficiencies were obtained at pH 11.0, whereas the BOD5 value increased from 16 mg l(-1) to 128 mg l(-1) after 40 min of ozonation, corresponding to an applied ozone dose of 1670 mg l(-1) and 33% relative ozone absorption. The studies showed that no degradation of raw penicillin fraction (30% of total COD) occurred, and degradation of the synthetic wastewater being completely treatable without penicillin addition, was inhibited by 7%. Upon 40 min ozonation, the synthetic wastewater could be completely oxidized and at the same time 35% of ozonated penicillin wastewater removal was obtained. Respirometric studies were conducted in parallel and produced results indicating a 22% decrease in the total oxygen consumption rate established for raw penicillin formulation effluent compared to the results obtained from the aerobic batch reactor. No inhibition of the synthetic fraction was observed for the 40 min-ozonated penicillin formulation effluent, biodegradability of the 60 min-ozonated penicillin effluent decreased possibly due to recalcitrant oxidation product accumulation. The modeling study provided experimental support and information on inhibition kinetics in activated sludge model no. 3 (ASM3) by means of respirometric tests for the first time.     

Ammonia removal from leachate solution using natural Chinese clinoptilolite

This paper assesses the potential of natural Chinese clinoptilolite for ammonia removal from the leachate solution of sewage sludge. In batch study the effects of relevant parameters, such as contact time, initial ammonia concentration and particle size of clinoptilolite, were examined respectively. The results show that the data obtained from batch studies were fit to Langmuir and Freundlich isotherms and the Langmuir isotherms reflect more reasonable for ammonium ion uptake onto clinoptilolite; the clinoptilolite adsorption process has been proved effective, at laboratory scale, the maximum adsorption capacity of the clinoptilolite, for ammonium concentration ranging from 11.12 to 115.16 mg NH(4)-N L(-1) in leachate solution, was about 1.74 mg NH(4)-Ng(-1); the time to adsorption equilibrium was 2.5 h in leachate solution and 1.5 h more than for in NH(4)Cl synthetic solution; ammonium adsorption increased with decreasing clinoptilolite particle size; the ammonia removal capacity of clinoptilolite increased with increasing initial ammonia concentration. It is believed that as adsorption agent for NH(4)-N removal from sludge leachate, natural Chinese clinoptilolite can be feasible.     

Industrial wastewater treatment in a new gas-induced ozone reactor

The present work was to investigate industrial wastewater treatment by ozonation in a new gas-induced reactor in conjunction with chemical coagulation pretreatment. The reactor was specifically designed in a fashion that gas induction was created on the liquid surface by the high-speed action of an impeller turbine inside a draft tube to maximize the ozone gas utilization. A new design feature of the present reactor system was a fixed granular activated carbon (GAC) bed packed in a circular compartment between the reactor wall and the shaft tube. The fixed GAC bed provided additional adsorption and catalytic degradation of organic pollutants. Combination of the fixed GAC bed and ozonation results in enhanced oxidation of organic pollutants. In addition to enhanced pollutant oxidation, ozonation was found to provide in situ GAC regeneration that was considered crucial in the present reaction system. Kinetic investigations were also made using a proposed complex kinetic model to elucidate the possible oxidation reaction mechanisms of the present gas-induced ozonation system. As a complementary measure, chemical coagulation pretreatment was found able to achieve up to 50% COD and 85% ADMI removal. Experimental tests were conducted to identify its optimum operating conditions.     

新型生态膜＋活性炭深度处理深圳某小区生活污水的研究

通过对新型生态膜反应器处理生活污水的试验研究,考察了不同水力停留时间（HRT）对反应器中去除CODer、NH,-N、TP污染物效果的影响。通过实验表明,在实际工况下,控制HRT为最佳工况状态,CODcr、NH3-N、TP的去除率分别达到80％、78％、65％以上,出水浓度可达到30mg／L、5mg／L、1mg／以下。出水水质达到国家标准《城镇污水处理厂污染物排放标准》（GB18918—2002）一级A标准要求。     

Landfill leachate treatment with a novel process: anaerobic ammonium oxidation (Anammox) combined with soil infiltration system

A novel combined process was proposed to treat municipal landfill leachate with high concentrations of ammonium and organics. This process consisted of a partial nitritation reactor (PNR), an anaerobic ammonium oxidation (Anammox) reactor (AR) and two underground soil infiltration systems (USIS-1 and USIS-2). Based on the optimum operating conditions obtained from batch tests of individual unit, the combined process was continuously operated on a bench scale for 166 days. Partial nitritation was performed in a fixed bio-film reactor (PNR, working volume=12 L). Ammonium nitrogen-loading rate (Nv) and DO were combined to monitor partial nitritation, and at T=30+/-1 degrees C, Nv=0.27-1.2 kg/(m3.d), DO=0.8-2.3 mg/L, the ratios of nitrite nitrogen (NO2--N) to ammonium nitrogen (NH4+-N) were successfully kept close to 1.0-1.3 in the effluent. Nitrate nitrogen (NO3--N) less than 43 mg/L was observed. The effluent of PNR was ideally suited as influent of AR. Sixty-nine percent CODcr from the raw leachate was degraded in the PNR. Anammox was carried out in a fixed bio-film reactor (AR, working volume=36 L). At T=30+/-1 degrees C, Nv=0.06-0.11 kg/(m3.d), about 60% NH4+-N and 64% NO2--N in the influent of AR were simultaneously removed. Inhibition of high-strength NO2--N (up to 1011 mg/L) should be responsible for the low removal rate of nitrogen. About 35% aquatic humic substance (AHS) was degraded in the AR. With the same working volume (200 L), USIS-1 and USIS-2 were alternately performed to treat the effluent from AR at one cycle of about 30 days. At hydraulic loading rate (HLR)=0.02-0.04 m3/m3.d, pollutant loading rates (PLR)=NH4+-N相似文献   

New sequential treatment for mature landfill leachate by cationic/anionic and anionic/cationic processes: optimization and comparative study

Two new applications for sequence treatment of mature (stabilized) landfill leachate, that is, cationic resin followed by anionic resin (cationic/anionic) and anionic resin followed by cationic resin (anionic/cationic), are employed and documented for the first time in the literature. Response surface methodology (RSM) concerning central composite design (CCD) is used to optimize each treatment process, as well as evaluate the individual and interactive effects of operational cationic resin dosage and anionic resin dosage on the effectiveness of each application in terms of color, chemical oxygen demand (COD), and NH(3)-N removal efficiency. A statistically significant model for color, COD, and NH(3)-N removal was obtained with high coefficient of determination values (R(2)>0.8). Under optimum operational conditions, the removal efficiency levels for color, COD, and NH(3)-N are 96.8%, 87.9%, and 93.8% via cationic/anionic sequence, and 91.6%, 72.3%, and 92.5% via anionic/cationic sequence, respectively. The experimental results and the model predictions agree well with each other.     

Pre-treatment of penicillin formulation effluent by advanced oxidation processes

A variety of advanced oxidation processes (AOPs; O3/OH-, H2O2/UV, Fe2+/H2O2, Fe3+/H2O2, Fe2+/H2O2/UV and Fe3+/H2O2/UV) have been applied for the oxidative pre-treatment of real penicillin formulation effluent (average COD0 = 1395 mg/L; TOC0 = 920 mg/L; BOD(5,0) approximately 0 mg/L). For the ozonation process the primary involvement of free radical species such as OH* in the oxidative reaction could be demonstrated via inspection of ozone absorption rates. Alkaline ozonation and the photo-Fenton's reagents both appeared to be the most promising AOPs in terms of COD (49-66%) and TOC (42-52%) abatement rates, whereas the BOD5 of the originally non-biodegradable effluent could only be improved to a value of 100 mg/L with O3/pH = 3] treatment (BOD5/COD, f = 0.08). Evaluation on COD and TOC removal rates per applied active oxidant (AOx) and oxidant (Ox) on a molar basis revealed that alkaline ozonation and particularly the UV-light assisted Fenton processes enabling good oxidation yields (1-2 mol COD and TOC removal per AOx and Ox) by far outweighed the other studied AOPs. Separate experimental studies conducted with the penicillin active substance amoxicillin trihydrate indicated that the aqueous antibiotic substance can be completely eliminated after 40 min advanced oxidation applying photo-Fenton's reagent (pH = 3; Fe(2+):H2O2 molar ratio = 1:20) and alkaline ozonation (at pH = 11.5), respectively.     

Treatment of wastewater containing azo dye reactive brilliant red X-3B using sequential ozonation and upflow biological aerated filter process

In this work, the treatment of wastewater containing azo dye reactive brilliant red X-3B using sequential ozonation and upflow biological aerated filter process has been studied. Decolorization was almost complete after 120min with an ozone concentration of 34.08mg/L, the biological oxygen demand for 5 days (BOD5)/chemical oxygen demand (COD) ratio increased from 0.102 to 0.406, which was more effective for the subsequent upflow biological aerated filter (UBAF) to reduce COD concentration. Under the conditions of gas/liquid=3, hydraulic load=4.8m3/m3.d, T=20-25 degrees C, the mass ratio of ozone to dye=4.5, pH 11, the COD and color of the effluent were less than 40mg/L and 20 Pt-Co units, respectively, and the average decolorization and COD removal efficiency were 97% and 90%, respectively. The experimental results showed that the combination of ozone oxidation and upflow biological aerated filter was a promising technique to treat wastewater containing azo dye.     

Hydrophobic organic chemicals (HOCs) removal from biologically treated landfill leachate by powder-activated carbon (PAC), granular-activated carbon (GAC) and biomimetic fat cell (BFC)

Biological pretreatment efficiently remove organic matter from landfill leachate, but further removal of refractory hydrophobic organic chemicals (HOCs) is hard even with advanced treatment. In this work, three-stage-aged refuse bioreactor (ARB) efficiently removed chemical oxygen demand (COD) and biochemical oxygen demand (BOD) of fresh leachate produced in Shanghai laogang landfill, from 8603 to 451 mg L(-1) and 1368 to 30 mg L(-1), respectively. In downstream treatment, 3 g L(-1) powder-activated carbon (PAC), granular-activated carbon (GAC) and biomimetic fat cell (BFC) removed 89.2, 73.4 and 81.1% HOCs, but only 24.6, 19.1 and 8.9% COD, respectively. Through the specific HOCs accumulation characteristics of BFC, about 11.2% HOCs with low molecular weight (<1000 Da) in the biologically treated leachate were concluded. Since HOCs are competitively trapped by dissolved organic matters (DOM), the ultimate removal of HOCs from leachate is unreachable by activated carbon or BFC. It was also found that the biologically treated leachate effluent exhibited a wide molecular weight distribution (34-514,646 Da). These constitutes are derived from both autochthonous and allochthonous matters as well as biological activities.     

Effects of ozonation process on lignin-derived compounds in pulp and paper mill effluents

The effect of ozonation process on pulp and paper mill effluents was investigated. The objectives were to: (1) identify various compounds in wastewater from a pulp and paper mill, (2) evaluate decolorization and organic removal efficiency by conventional bubble reactor and (3) evaluate the biodegradability at various progressive stages of ozonation. The qualitative GC/MS analyses were performed before and after the biological treatment and ozonation process. Two groups of compounds were observed in this wastewater: lignin-derived compounds and aliphatic compounds used in the pulp and paper production process (i.e. n-alkanes, fatty alcohols, fatty acid and ester). Treatment efficiency was measured by decolorization and TOC removal rates. Additionally, the utilization coefficient (k) and BOD/COD ratio were determined to observe the biodegradability of ozonized effluents. The results indicated that after 45 min, the ozonation of effluents yielded almost colorless effluent with over 90% decolorization efficiency and with corresponding ozone capacity rate of 20.0 mg O(3)L(-1). This decolorization was not always accompanied by the mineralization of the organic matters therefore ozonation was not related to TOC removal rates. The BOD/COD ratio increased from 0.10 to a maximum value of 0.32 with ozone flow rate (O/F) of 4.0 L min(-1). It was confirmed by the utilization coefficient as first order BOD equation, the magnitude k value increased from 0.21 day(-1) to maximum value of 0.47 day(-1) as the ozonation time was raised to 60 min with O/F 4.0 L min(-1).     

Treatment of landfill leachate by using electro-Fenton method

In this study, the effects of various operating conditions such as treatment time, DC current, initial pH, initial H(2)O(2) concentration and distance between the electrodes on treatability of landfill leachate by using electro-Fenton (EF) method were examined. The settling characteristics of waste sludge produced from the treatment were also determined. According to the results, EF method can be used efficiently for the treatment of landfill leachate by using the proper operating conditions. The best removal efficiencies were obtained when: treatment duration is 20 min, constant DC current value is 3A, H(2)O(2) concentration is 2000 mg L(-1) and the initial pH value is 3. For these conditions, 72% COD, 90% color, 87% PO(4)-P and 28% NH(4)-N removals were obtained. It was also observed that using electrode distance between 1.8 cm and 2.8 cm increases efficiency of the COD removal, significantly. Sedimentation characteristics of the waste sludge produced from the EF method is fairly good.     

Landfill leachate treatment using powdered activated carbon augmented sequencing batch reactor (SBR) process: optimization by response surface methodology

In this study, landfill leachate was treated by using the sequencing batch reactor (SBR) process. Two types of the SBR, namely non-powdered activated carbon and powdered activated carbon (PAC-SBR) were used. The influence of aeration rate and contact time on SBR and PAC-SBR performances was investigated. Removal efficiencies of chemical oxygen demand (COD), colour, ammoniacal nitrogen (NH(3)-N), total dissolved salts (TDS), and sludge volume index (SVI) were monitored throughout the experiments. Response surface methodology (RSM) was applied for experimental design, analysis and optimization. Based on the results, the PAC-SBR displayed superior performance in term of removal efficiencies when compared to SBR. At the optimum conditions of aeration rate of 1L/min and contact time of 5.5h the PAC-SBR achieved 64.1%, 71.2%, 81.4%, and 1.33% removal of COD, colour, NH(3)-N, and TDS, respectively. The SVI value of PAC-SBR was 122.2 mL/g at optimum conditions.     

Treatment of leachate by electrocoagulation using aluminum and iron electrodes

In this paper, treatment of leachate by electrocoagulation (EC) has been investigated in a batch process. The sample of leachate was supplied from Odayeri Landfill Site in Istanbul. Firstly, EC was compared with classical chemical coagulation (CC) process via COD removal. The first comparison results with 348 A/m2 current density showed that EC process has higher treatment performance than CC process. Secondly, effects of process variables such as electrode material, current density (from 348 to 631 A/m2), pH, treatment cost, and operating time for EC process are investigated on COD and NH4-N removal efficiencies. The appropriate electrode type search for EC provided that aluminum supplies more COD removal (56%) than iron electrode (35%) at the end of the 30 min operating time. Finally, EC experiments were also continued to determine the efficiency of ammonia removal, and the effects of current density, mixing, and aeration. All the findings of the study revealed that treatment of leachate by EC can be used as a step of a joint treatment.     

Decomposition of dimethyl phthalate in an aqueous solution by ozonation with high silica zeolites and UV radiation

This study investigates the enhanced ozonation of dimethyl phthalate (DMP), which is a pollutant of concern in water environments, with high silica zeolites and ultraviolet (UV) radiation. Semibatch ozonation experiments are performed under various reaction conditions to examine the effects of inlet gas ozone concentration, high silica zeolite dosage, and UV radiation intensity on the decomposition of DMP. The complete removal of DMP can be efficiently achieved via both O(3) and O(3)/UV treatments. Note that the presence of high silica zeolites accelerates the decomposition rate of DMP in the O(3) process. On the other hand, the removal efficiencies of both chemical oxygen demand (COD) and total organic carbons (TOC) are significantly enhanced by employing the ozonation combined with UV radiation. The O(3)/UV process is also advantageous for the utilization efficiency of fed ozone especially in the late ozonation period. Furthermore, the correlation between the COD removal percentage (%) and the mole ratio of ozone consumed to the DMP treated (mol mol(-1)) is obtained. The clear-cut removal relationship of the TOC with COD during the ozonation of DMP has also been presented. Consequently, the results evaluate the flexibility of ozonation system associated with high silica zeolites and UV radiation for the removal of DMP and provide the useful information in engineering application.