Factors affecting the concentration of bisphenol A in leachates from solid waste disposal sites and its fate in treatment processes

 The concentrations of bisphenol A (BPA) contained in landfill leachates from solid waste disposal sites were measured. The concentrations of BPA contained in leachates from industrial waste sites were in the range below the detection limit to 2800 μg/l, while those from municipal sites were in the range 26–8400 μg/l. The leachates from ash-rich sites contained relatively lower concentrations of BPA compared with organic-rich leachates. It is suggested that BPA concentration increases with time after the completion of reclamation in the case of ash-rich sites, whereas the concentration of BPA decreases with time in the case of organic-rich sites. A 7-year survey on a site in Japan showed neither a decrease nor an increase in the concentration of BPA during on-going reclamation. A leachate from a site in the Philippines contained high concentrations of BPA. A slight positive correlation was found between BPA concentrations and total organic carbon (TOC). A major portion of the BPA in leachates was found in dissolved and organic unassociated fractions, which cannot be precipitated by coagulation. More than 99.9% of the BPA contained in raw leachates was removed by a conventional series of treatment processes consisting of biological treatment, coagulation, sedimentation, sand filtration, and activated carbon adsorption. Received: May 29, 2002 / Accepted: October 17, 2002     

Distribution of organophosphoric acid triesters between water and sediment at a sea-based solid waste disposal site

Organophosphoric acid triester (OPE) concentration levels in water and bottom sediment at the Osaka North Port Sea-Based Solid Waste Disposal Site were investigated, and the behavior of OPEs in the water environment of the waste disposal site was examined. The more highly water-soluble OPEs were frequently detected in raw water. Of the OPEs detected, TCEP and TCPP showed very high concentrations (1.0–90 μg/l), followed by TEP (0.3–10 μg/l) > TBXP (0.8–6.3 μg/l) > TDCPP (0.6–6.2 μg/l) > TBP (0.2–1.5 μg/l) > TPP (<0.1 μg/l). Most OPEs detected in water were eluted from the disposal waste to the water phase immediately and behaved as dissolved forms with no distribution in suspended solids (SS). On the other hand, the less water-soluble OPEs, such as TCP or TEHP, were detected in bottom sediment but hardly at all in water samples. All OPEs were detected at the waste disposal site, within which their concentration levels were uniform. It appeared that the less water-soluble OPEs were present as SS-associated forms and behaved in line with the floating surface sludge at the bottom. Received: July 6, 1998 / Accepted: February 25, 1999     

Comparative study on leachate in closed landfill sites: focusing on seasonal variations

This article is intended to provide background information on leachate management in closed landfill sites based on a comparison of two landfill sites and the identification of leachate characteristics depending on the final cover and the season. Site S is older and has no final cover, while site J is younger and has final capping. The results of leachate analysis from the two landfills show that the biological oxygen demand to chemical oxygen demand ratio decreases below 0.1 to the range 0.05–0.07 for site S, whereas the ratio at site J was in the range 0.08–0.55. The inorganic nitrogen concentration was in the range 169.9–386.1 mg/l with an average of 265.2 mg/l at site S. Ammonia nitrogen accounted for 98.9% of the total nitrogen. The absence of a final cover on closed landfill sites may contribute to the stabilization of such landfills due to flushing. The nitrogen content at landfill S dropped in the summer, whereas it decreased in the fall at site J. A higher fluctuation in the pollutant levels of organic matters and nitrogen at the younger landfill site was observed, compared to the older site, even though the younger site had final capping. Therefore, intensive leachate management should be arranged at the early stages after closing for proper treatment. Specifically, nitrogen management of leachate is a critical factor in treatment operations.     

Substance flow analysis of coplanar PCBs released from waste incineration processes

Previous reports have focused on the emission of coplanar polychlorinated biphenyls (Co-PCBs) which have a toxic mechanism similar to that of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDDs/DFs) released from municipal solid waste (MSW) incineration. Such emissions accounted for a small percentage of all the dioxins (PCDDs/DFs and Co-PCBs) recorded at the toxicity equivalent (TEQ) level. There is, however, very little information about Co-PCBs, such as the quantities being released and their effect on overall environmental pollution. The aim of this research has been to clarify the substance flow of Co-PCBs from MSW incineration processes. The results reveal that whereas the input of Co-PCBs into the MSW incineration facilities in Kyoto City was 0.13–0.29 μg-TEQ per ton waste, the total output of Co-PCBs (the sum of Co-PCBs released from emission gas, fly ash, and bottom ash) was 4.9 μg-TEQ per ton waste. The total output was therefore found to be higher than the total input. Over 90% of the total PCBs were decomposed in the incineration process. In comparing the profiles of congeners and homologues, those in the MSW were found to be similar to those detected in the atmosphere and products containing PCBs, but different from those in the MSW incineration gas. Received: August 26, 1998 / Accepted: March 2, 1999     

Size fractionation of organic matter and heavy metals in raw and treated leachate

This study characterized the organic matter and heavy metals in the leachate from two typical municipal solid waste (MSW) sanitary landfills in China, the recently established (3-year-old) Liulitun landfill and the mature (11-year-old) Beishenshu landfill, using a size fractionation procedure. The organic matter of all raw and treated leachate samples primarily existed in a truly-dissolved fraction with an apparent molecular weight (AMW) of <1 kDa, and its percentage decreased with an increase in overall AMW. The leachate from the newer landfill had a higher percentage of truly-dissolved organic matter. After anaerobic treatment, this leachate had a similar size fraction of organic matter to that seen for the raw leachate of the mature landfill. Biochemical processes had different removal efficiencies for various types of AMW organic matter, and the concentration of moderate AMW organic matter appeared to increase throughout these processes. Most of the heavy metals existed in a colloidal fraction (AMW >1 kDa and particle size <0.45 μm). The behaviors of different species of heavy metals had large variations. The size fractions of heavy metal species were significantly affected by treatment processes and landfill age, except for Zn. The concentration ratio of heavy metals to organic matter was maximal in the colloidal fraction and showed an inverse change to that seen for organic matter concentration changes caused by biochemical processes. Consequently, the pollution levels of heavy metals were substantially increased by treatment processes, although their concentrations decreased.     

Future landfill emissions and the effect of final cover installation--a case study

Municipal solid waste (MSW) landfills are potential long-term sources of emissions. Hence, they need to be managed after closure until they do not pose a threat to humans or the environment. The case study on the Breitenau MSW landfill was performed to evaluate future emission levels for this site and to illustrate the effect of final cover installation with respect to long-term environmental risks. The methodology was based on a comprehensive assessment of the state of the landfill and included analysis of monitoring data, investigations of landfilled waste, and an evaluation of containment systems. A model to estimate future emission levels was established and site-specific predictions of leachate emissions were presented based on scenario analysis. The results are used to evaluate the future pollution potential of the landfill and to compare different aftercare concepts in view of long-term emissions. As some leachable substances became available for water flow during cover construction due to a change in the water flow pattern of the waste, a substantial increase in leachate concentrations could be observed at the site (e.g. concentrations of chloride increased from 200 to 800 mg/l and of ammonia-nitrogen from 140 to about 500 mg/l). A period of intensive flushing before the final cover installation could have reduced the amount of leachable substances within the landfill body and rapidly decreased the leachate concentrations to 11 mg Cl/l and 79 mg NH₄-N/l within 50 years. Contrarily, the minimization of water infiltration is associated with leachate concentrations in a high range for centuries (above 400 mg Cl/l and 200 mg NH₄-N/l) with low concomitant annual emission loads (below 12 kg/year of Cl or 9 kg/year of NH₄-N, respectively). However, an expected gradual decrease of barrier efficiency over time would be associated with higher emission loads of 50 kg of chloride and 30 kg of ammonia-nitrogen at the maximum, but a faster decrease of leachate concentration levels.     

Comparing field investigations with laboratory models to predict landfill leachate emissions

Investigations into laboratory reactors and landfills are used for simulating and predicting emissions from municipal solid waste landfills. We examined water flow and solute transport through the same waste body for different volumetric scales (laboratory experiment: 0.08 m³, landfill: 80,000 m³), and assessed the differences in water flow and leachate emissions of chloride, total organic carbon and Kjeldahl nitrogen. The results indicate that, due to preferential pathways, the flow of water in field-scale landfills is less uniform than in laboratory reactors. Based on tracer experiments, it can be discerned that in laboratory-scale experiments around 40% of pore water participates in advective solute transport, whereas this fraction amounts to less than 0.2% in the investigated full-scale landfill. Consequences of the difference in water flow and moisture distribution are: (1) leachate emissions from full-scale landfills decrease faster than predicted by laboratory experiments, and (2) the stock of materials remaining in the landfill body, and thus the long-term emission potential, is likely to be underestimated by laboratory landfill simulations.     

Leachate formation and characteristics from gasification and grate incineration bottom ash under landfill conditions

Characteristics and formation of leachates from waste gasification and grate firing bottom ash were studied using continuous field measurements from 112 m³ lysimeters embedded into landfill body for three years. In addition, the total element concentrations of the fresh ash were analysed and laboratory batch tests were performed to study leachate composition. The three-year continuous flow measurement showed that about one fifth of the leachates were formed, when the flow rate was >200 l/d, covering <3.5% of the study time. After three years, the liquid/solid-ratio for the quenched grate ash was 1 (l/kg (d.m.)) and for the initially dry gasification ash 0.4 (l/kg (d.m.)). The low initial water and residual carbon content of the gasification ash kept the leachate pH at a high level (>13) major part of the study. In the grate ash leachate pH was lower (<8) due to the presence of organic carbon and biodegradation indicated by biological oxygen demand and redox potential measurements. In the gasification ash the high pH probably delayed leaching of major elements such as Ca, therefore, raising the need for a longer after-care period. The high pH also explains the higher leaching of As from the gasification ash compared to the grate ash both in the batch test and under landfill conditions.     

Pollution profiles and physicochemical parameters in old uncontrolled landfills

The long-term effectiveness of the geological barrier beneath municipal-waste landfills is a critical issue for soil and groundwater protection. This study examines natural clayey soils directly in contact with the waste deposited in three landfills over 12 years old in Spain. Several physicochemical and geological parameters were measured as a function of depth. Electrical conductivity (EC), water-soluble organic carbon (WSOC), Cl⁻, NH₄⁺, Na⁺ and exchangeable NH₄⁺ and Na⁺ were used as parameters to measure the penetration of landfill leachate pollution. Mineralogy, specific surface area and cationic-exchange capacities were analyzed to characterize the materials under the landfills. A principal component analysis, combined with a Varimax rotation, was applied to the data to determine patterns of association between samples and variables not evident upon initial inspection. The main factors explaining the variation in the data are related to waste composition and local geology. Although leachates have been in contact with clays for long time periods (13-24 years), WSOC and EC fronts are attenuated at depths of 0.2-1.5 m within the clay layer. Taking into account this depth of the clayey materials, these natural substrata (>45% illite-smectite-type sheet silicates) are suitable for confining leachate pollution and for complying with European legislation. This paper outlines the relevant differences in the clayey materials of the three landfills in which a diffusive flux attenuation capacity (A_c) is defined as a function (1) of the rate of decrease of the parameters per meter of material, (2) of the age and area of the landfill and (3) of the quantity and quality of the wastes.     

Application of a contaminant mass balance method at an old landfill to assess the impact on water resources

Old and unlined landfill sites pose a risk to groundwater and surface water resources. While landfill leachate plumes in sandy aquifers have been studied, landfills in clay till settings and their impact on receiving water bodies are not well understood. In addition, methods for quantitatively linking soil and groundwater contamination to surface water pollution are required. This paper presents a method which provides an estimate of the contaminant mass discharge, using a combination of a historical investigation and contaminant mass balance approach. The method works at the screening level and could be part of a risk assessment. The study site was Risby Landfill, an old unlined landfill located in a clay till setting on central Zealand, Denmark. The contaminant mass discharge was determined for three common leachate indicators: chloride, dissolved organic carbon and ammonium. For instance, the mass discharge of chloride from the landfill was 9.4 ton/year and the mass discharge of chloride to the deep limestone aquifer was 1.4 ton/year. This resulted in elevated concentrations of leachate indicators (chloride, dissolved organic carbon and ammonium) in the groundwater. The mass discharge of chloride to the small Risby Stream down gradient of the landfill was approximately 31 kg/year. The contaminant mass balance method worked well for chloride and dissolved organic carbon, but the uncertainties were elevated for ammonium due to substantial spatial variability in the source composition and attenuation processes in the underlying clay till.     

Bioreactor landfills: experimental and field results

Bioreactor landfills allow a more active landfill management that recognizes the biological, chemical and physical processes involved in a landfill environment. This paper presents the results of an experimental study carried out to determine the effect of solid waste size, leachate recirculation and nutrient balance on the rate of municipal solid waste (MSW) biodegradation. Higher rates of MSW biodegradation eventually cause a reduction of the contaminant life span of the landfill and decrease in the cost of long term monitoring. The study indicated that the smaller the size of the MSW the faster the biodegradation rate of the waste. In addition, the paper presents the results of leachate recirculation on solid waste biodegradation in a full-scale landfill site, which is located in Nepean, Ontario, Canada. The leachate was recirculated into the landfilled solid waste for 8 years through infiltration lagoons. Similar results to those obtained in the laboratory scale experiments were noted. The average pH of the leachate in the early stages of recirculation was on the acidic range of the pH scale, however, the pH value was in the range of 7-8 after 2 years of leachate recirculation. The concentration of chloride remained fairly constant at about 1000 mg/l during the leachate recirculation period. A decreasing trend of the organic load, measured as biological oxygen demand and chemical oxygen demand, was observed. Recovery of landfill air space was also noted because of the enhanced subsidence and decomposition of the solid waste.     

Removal of dissolved organic matter and phthalic acid esters from landfill leachate through a complexation-flocculation process

Dissolved organic macromolecules (DOM) and micropollutants, such as phthalic acid esters (PAEs), are often enriched in landfill leachate. PAEs were detected in 10 leachate samples from three landfills in Hubei province, central China. In particular, di-(2-ethyhexyl) phthalate (DEHP) concentration was higher than 70microgL(-1) in most samples, and the highest DEHP concentration was in the colloid fraction (1000Da-0.45microm). Use of flocculants may result in flocculation and precipitation of colloids and associated contaminants, such as DEHP. Biodegradation is not effective for long chain PAEs or the landfill leachate, given the low ratio of BOD5/COD (less than 0.2) and deficient phosphorus content. Complexation-flocculation is therefore proposed as an alternative process for removing DOM and PAEs. Jar-test experiments were employed to investigate the mechanism and feasibility of the process. Among tested coagulants (ferric chloride, aluminum sulfate and poly aluminum chloride (PAC)), PAC was the most efficient. Hydrophobic contaminants with log KOC greater than 4 and DOM in wastewater can be removed simultaneously through the complexation-flocculation process.     

Behavior of endocrine-disrupting chemicals in leachate from MSW landfill sites in Japan

Endocrine-disrupting chemicals (EDCs) in landfill leachates and the effluent from leachate treatment facilities have been analyzed by many researchers. However, seasonal and yearly variations and the influence of landfill age are still not clear. In this study, leachate was sampled on four occasions each, at different seasons, from two MSW landfills which receive different waste material. Then, the quantities of alkylphenols (APs), bisphenol A (BPA), phthalic acid esters (PAEs) and organotin compounds (OTs) in leachate were determined. By sampling leachate from landfill cells of different age, the long-term behavior of EDCs was studied. Furthermore, leachate was also sampled at different points in the process of a leachate treatment system, and then the behavior of EDCs in the facility was studied. The concentrations of APs were as low as in surface waters, and OTs were not detected (detection limit was 0.01 microg/l), while BPA and DEHP, which were the most abundant of the four substances measured as PAEs, were found in all the leachates that were measured. Concentrations of BPA and DEHP were almost constant regardless of season, except for a couple of low concentrations observed for BPA. The varying composition of landfilled waste did not influence BPA and DEHP in leachate. Concentration of BPA in raw leachate tends to decrease as the years go by, but the concentration of DEHP was observed to remain at a constant level. BPA was considerably degraded by aeration for leachates from the two landfills, except when the leachate temperature was low. Aeration, coagulation/sedimentation, and biological treatment could not remove DEHP.     

Removal of mixed contaminants by Fe0-based biobarrier in flow-through columns using recycled waste materials

The present study investigated the reactivity and ability of permeable reactive barriers [zero-valent iron (ZVI)-barrier plus biobarrier) to remove various contaminants (Cd, As, Zn, Cu, Mn, Cr, NO₃ ⁻, NH₄ ⁺, and COD_cr) from synthetic leachate. Two different reactive materials were used in this study, namely ZVI and autoclaved lightweight concrete (ALC). After 90 days of column operation, the contaminant profiles were determined along the length of the columns. The heavy metals were extensively removed in the bio-ALC and sequential barriers (ZVI plus bio-ALC), however the removal efficiencies for the heavy metals Zn and Cr in the ALC and bio-ALC barriers were comparatively low. Nitrate was completely removed (>99.9%) in the ALC, bio-ALC, and sequential barriers. More than 50% of the produced ammonium and organic materials were removed in the biologically reactive zone of the sequential barriers. The results of the present study suggest that sequential barriers are one of the best solutions for in situ remediation and that they can be applied to clean up the leachate released from landfills.     

Fundamental processes and implications during in situ aeration of old landfills

Results of investigations from many old landfills in Germany and Europe indicate that significant emissions occur under conventional landfill operating conditions (i.e., anaerobic conditions). Significant emissions via the gas phase are predicted to last at least three decades after landfill closure, while leachate emissions are predicted to continue for many decades, potentially even lasting for centuries. When considering the specific type and quality, and quite often lack of, protection barriers associated with old landfills, these leachate and gas emissions may result in a significant negative impact on the environment. However, complete sealing of the landfill only temporarily reduces emissions because dry-conservation of the biodegradable waste fraction results, thus not allowing any severe reduction in the emission and hazardous potential of the landfill to occur. If noticeable damage of the surface capping system occurred in these landfills, infiltrating water would restart the interrupted emission formation. In contrast, aerobic in situ stabilization by means of low pressure aeration attempts to stabilize and modify the inventory of organic matter inside the landfill, acting to reduce the emission potential in a more sustainable manner. By enabling faster and more extensive aerobic degradation processes in the landfill (compared with anaerobic processes), the organics (e.g., hydrocarbons) are degraded significantly faster, resulting in an increased carbon discharge via the gas phase, as well as reduced leachate concentrations. Because carbon dioxide (CO(2)) is the main compound in the extracted off-gas (instead of methane (CH(4)), which dominated under anaerobic landfill conditions), the negative impact of diffuse LFG emissions towards an increased global warming effect may be significantly lowered. With respect to leachate quality, a reduction of organic compounds as well as ammonia-nitrogen can be expected. In addition to these positive ecological effects, aerobic in situ stabilization is associated with significant cost savings potential due to both quantitative and qualitative reductions in the aftercare period. This paper describes the fundamental processes and implications of in situ landfill aeration. Additionally, possible criteria for defining an endpoint of the active aeration process are presented and discussed.     

Fungal and enzymatic treatment of mature municipal landfill leachate

The aim of our study was to evaluate biotreatability of mature municipal landfill leachate by using white rot fungus and its extracellular enzymes. Leachates were collected in one active and one closed regional municipal landfill. Both chosen landfills were operating for many years and the leachates generated there were polluted by organic and inorganic compounds. The white rot fungus Dichomitus squalens was able to grow in the mature leachate from the closed landfill and as it utilizes present organic matter as a source of carbon, the results were showing 60% of DOC and COD removal and decreased toxicity to the bacterium Aliivibrio fischeri. On the other hand, growth of the fungus was inhibited in the presence of the leachate from the active landfill. However, when the leachate was introduced to a crude enzyme filtrate containing extracellular ligninolytic enzymes, removal levels of COD and DOC reached 61% and 44%, respectively. Furthermore, the treatment led to detoxification of the leachate to the bacterium Aliivibrio fischeri and to reduction of toxicity (42%) to the plant Sinapis alba. Fungal and enzymatic treatment seems to be a promising biological approach for treatment of mature landfill leachates and their application should be further investigated.     

Influence of oxygen flow rate on reaction rate of organic matter in leachate from aerated waste layer containing mainly incineration ash

It is known that aeration reduces rapidly the concentration of organic matter in leachate. However, the oxygen flow rate required to attain a certain reaction rate of organic matter should be carefully estimated. In this study, using the oxygen ratio (the ratio of oxygen flow rate by aeration to oxygen consumption rate of waste layer) as a parameter, the reaction rate of organic matter in leachate from landfilled incineration ash and incombustible waste upon aeration was evaluated. Total organic carbon (TOC) in the leachate was reduced rapidly when the oxygen ratio was high. The decomposition rate exceeded the elution rate of TOC in the leachate from the waste layer for several days when the oxygen ratio was above 10². The results indicate that the oxygen ratio can be used as a parameter for the aeration operation in actual landfill sites, to rapidly stabilize organic matter in leachate.     

Size-fractionation and characterization of landfill leachate and the improvement of Cu2+ adsorption capacity in soil and aged refuse

Leachate was collected from an anaerobic lagoon at Shanghai Laogang refuse landfill, the largest landfill in China, and the sample was separated into six fractions using micro-filtration membranes, followed by ultra-filtration membranes. Several parameters of the samples were measured, including chemical oxygen demand (COD), total organic carbon (TOC), total solids (TS), pH, total phosphate (TP), total nitrogen (TN), fixed solids (FS), NH4+, orthophosphate, color, turbidity, and conductivity. These parameters were then quantitatively correlated with the molecular weight cutoff of the membrane used. Organic matter in the dissolved fraction (MW<1kDa) predominated in the leachate, accounting for 65% of TOC. Thermal infrared spectroscopy was used to characterize the filter residues. Asymmetric and symmetric stretching of methyl and methylene groups, and of functional groups containing nitrogen and oxygen atoms, were observed. In addition, the ability of two different samples to adsorb heavy metals was tested. Cu2+ was chosen as the representative heavy metal in this study, and the samples were soil; aged refuse, which had spent 8 years in a conventional sanitary landfill; and samples of soil and aged refuse treated for 48h with leachate in the ratio of 5g of sample per 50ml of leachate. Cu2+ uptake by the raw soil was approximately 4.60microg/g, while uptake by the leachate-contacted soil and leachate-contacted aged refuse were 5.66 and 5.11microg/g, respectively. These results show that the organic matter in the leachate enhanced the capacity of aqueous solutions to adsorb Cu2+.     

Risk assessment of an old landfill regarding the potential of gaseous emissions – A case study based on bioindication,FT-IR spectroscopy and thermal analysis

Risk assessment of two sections (I and II) of an old landfill (ALH) in Styria (Austria) in terms of reactivity of waste organic matter and the related potential of gaseous emissions was performed using conventional parameters and innovative tools to verify their effectiveness in practice. The ecological survey of the established vegetation at the landfill surface (plant sociological relevés) indicated no relevant emissions over a longer period of time. Statistical evaluation of conventional parameters reveals that dissolved organic carbon (DOC), respiration activity (RA₄), loss of ignition (LOI) and total inorganic carbon (TIC) mostly influence the variability of the gas generation sum (GS₂₁). According to Fourier Transform Infrared (FT-IR) spectral data and the results of the classification model the reactivity potential of the investigated sections is very low which is in accordance with the results of plant sociological relevés and biological tests. The interpretation of specific regions in the FT-IR spectra was changed and adapted to material characteristics. Contrary to mechanically–biologically treated (MBT) materials, where strong aliphatic methylene bands indicate reactivity, they are rather assigned to the CH vibrations of plastics in old landfill materials. This assumption was confirmed by thermal analysis and the characteristic heat flow profile of plastics containing landfill samples. Therefore organic carbon contents are relatively high compared to other stable landfills as shown by a prediction model for TOC contents based on heat flow profiles and partial least squares regression (PLS-R). The stability of the landfill samples, expressed by the relation of CO₂ release and enthalpies, was compared to unreactive landfills, archeological samples, earthlike materials and hardly degradable organic matter. Due to the material composition and the aging process the landfill samples are located between hardly degradable, but easily combustible materials and thermally resistant materials with acquired stability.