Effects of limestone addition and sintering on heavy metal leaching from hazardous waste incineration slag

Hazardous waste incineration (HWI) in rotary kilns and the disposal of the residual slag on landfills play an important role in German waste treatment. In order to save disposal costs the elution behaviour of HWI-slag should be further optimised. Quality-improved slag may be disposed off on cheaper landfill sites still applying to landfill regulations. In a new process-integrated approach hazardous waste is mixed with limestone, which initiates chemical reactions with heavy metals in the rotary kiln yielding new compounds of different solubility. In this work HWI-slag/limestone mixtures are thermally treated and then examined by elution tests. Experimental data indicate that the heavy metals pertinent to landfill class assignment of a HWI-slag share a solubility minimum at a CaO-content of about 15%. Such improved HWI-slags are allowed to be disposed off on cheaper landfill sites. Furthermore, a new combination of thermodynamic calculation methods is applied to predict heavy metal solubility for different process conditions. Used models hold the opportunity to explain the tendencies of heavy metal leaching and propose plausible chemical reactions. With it, a new tool to examine the impact of temperature treatment and slag composition on heavy metal elution from HWI-slag is presented.     

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.     

Assessment of internal condition of waste in a roofed landfill

Recently, roofed landfills have been gaining popularity in Japan. Roofed landfills have several advantages over non-roofed landfills such as eliminating the visibility of waste and reducing the spread of offensive odours. This study examined the moisture balance and aeration conditions, which promote waste stabilisation, in a roofed landfill that included organic waste such as food waste. Moisture balance was estimated using waste characterization and the total amount of landfilled waste. Internal conditions were estimated based on the composition, flux, and temperature of the landfill gas. Finally, in situ aeration was performed to determine the integrity of the semi-aerobic structure of the landfill.With the effects of rainfall excluded, only 15% of the moisture held by the waste was discharged as leachate. The majority of the moisture remained in the waste layer, but was less than the optimal moisture level for biodegradation, indicating that an appropriate water spray should be administered. To assess waste degradation in this semi-aerobic landfill, the concentration and flow rate of landfill gas were measured and an in situ aeration test was performed. The results revealed that aerobic biodegradation had not occurred because of the unsatisfactory design and operation of the landfill.     

Evaluation of heavy metal leaching from spent household batteries disposed in municipal solid waste

Batch leaching tests and simulated landfill lysimeter tests were performed to evaluate the contents of heavy metals leached from spent batteries in the municipal solid waste. The toxicity characteristic leaching procedure was utilized to perform the batch leaching tests of 36 spent batteries. Four lysimeters were prepared with battery contents ranging from 0% to 100% by weight for column tests, and the experiments were performed at ambient temperature. The age of all the batteries used in the study ranged from freshly disposed up to approximately 3 years old. The results from the batch tests showed that the type of battery influenced the heavy metal concentrations in the leached solutions. The lysimeter experiment results illustrated that at lower pH levels more metals are leached than at higher pH levels. The increasing amount of batteries disposed in landfills can contribute to the leaching of more metals, especially Mn and Zn, into the environment. These results indicate that the direct disposal of spent household batteries into a MSW landfill can increase the heavy metal contents in the landfill leachate.     

Changes in carbon and nitrogen pool during in-situ aeration of old landfills under varying conditions

Emissions from old landfills via leachate and the gas phase are influenced by state and stability of the organic matter in the solid waste and by environmental conditions within the landfill. Remediation of landfills by means of in-situ aeration is one possibility to reduce these emissions. By establishing aerobic conditions, biological processes in the landfill are accelerated. To investigate the effects of this remediation technology, lab-scale experiments with column tests have been carried out. The main goal of the present work is to characterize the changes of the carbon and nitrogen compounds in the aerated solid waste, the leachate and the gas phase under varying conditions. The results demonstrate a clear reduction of emissions and a stabilization of the organic matter. Furthermore, it is shown that both the intensity of aeration and the amount of water affect biological processes to a certain extent. Even when columns were operated under anaerobic conditions after a long running period of aeration, the emissions remained low.     

Ecotoxicological assessment and evaluation of a pine bark biosorbent treatment of five landfill leachates

When selecting a landfill leachate treatment method the contaminant composition of the leachate should be considered in order to obtain the most cost-effective treatment option. In this study the filter material pine bark was evaluated as a treatment for five landfill leachates originating from different cells of the same landfill in Sweden. The objective of the study was to determine the uptake, or release, of metals and dissolved organic carbon (DOC) during a leaching test using the pine bark filter material with the five different landfill leachates. Furthermore the change of toxicity after treatment was studied using a battery of aquatic bioassays assessing luminescent bacteria (Vibrio fischeri) acute toxicity (30-min Microtox®), immobility of the crustacean Daphnia magna, growth inhibition of the algae Pseudokirchneriella subcapitata and the aquatic plant Lemna minor; and genotoxicity with the bacterial Umu-C assay. The results from the toxicity tests and the chemical analysis were analyzed in a Principal Component Analysis and the toxicity of the samples before and after treatment was evaluated in a toxicity classification. The pine bark filter material reduced the concentrations of metal contaminants from the landfill leachates in the study, with some exceptions for Cu and Cd. The Zn uptake of the filter was high for heavily contaminated leachates (≥73%), although some desorption of zinc occurred in less contaminated waters. Some of the leachates may require further treatment due to discharge into a natural recipient in order to reduce the risk of possible biological effects. The difference in pH changes between the different leachates was probably due to variations in buffering capacity, affected by physicochemical properties of the leachate. The greatest desorption of phenol during filtration occurred in leachates with high conductivity or elevated levels of metals or salts. Generally, the toxicity classification of the leachates implies that although filter treatment with pine bark removes metal contaminants from the leachates effectively, it does not alter leachate toxicity noticeably. The leachates with the highest conductivity, pH and metal concentrations are most strongly correlated with an increased toxic response in the score plots of both untreated and treated leachates. This is in line with the toxicity classification of the leachate samples. The results from this study highlight the importance of evaluating treatment efficiency from the perspective of potential recipient effects, rather than in terms of residual concentrations of individual contaminants when treating waters with a complex contamination matrix, such as landfill leachates.     

Stable isotope signatures for characterising the biological stability of landfilled municipal solid waste

Stable isotopic signatures of landfill leachates are influenced by processes within municipal solid waste (MSW) landfills mainly depending on the aerobic/anaerobic phase of the landfill. We investigated the isotopic signatures of δ¹³C, δ²H and δ¹⁸O of different leachates from lab-scale experiments, lysimeter experiments and a landfill under in situ aeration. In the laboratory, columns filled with MSW of different age and reactivity were percolated under aerobic and anaerobic conditions. In landfill simulation reactors, waste of a 25 year old landfill was kept under aerobic and anaerobic conditions. The lysimeter facility was filled with mechanically shredded fresh waste. After starting of the methane production the waste in the lysimeter containments was aerated in situ. Leachate and gas composition were monitored continuously. In addition the seepage water of an old landfill was collected and analysed periodically before and during an in situ aeration.We found significant differences in the δ¹³C-value of the dissolved inorganic carbon (δ¹³C-DIC) of the leachate between aerobic and anaerobic waste material. During aerobic degradation, the signature of δ¹³C-DIC was mainly dependent on the isotopic composition of the organic matter in the waste, resulting in a δ¹³C-DIC of ?20‰ to ?25‰. The production of methane under anaerobic conditions caused an increase in δ¹³C-DIC up to values of +10‰ and higher depending on the actual reactivity of the MSW. During aeration of a landfill the aerobic degradation of the remaining organic matter caused a decrease to a δ¹³C-DIC of about ?20‰. Therefore carbon isotope analysis in leachates and groundwater can be used for tracing the oxidation–reduction status of MSW landfills.Our results indicate that monitoring of stable isotopic signatures of landfill leachates over a longer time period (e.g. during in situ aeration) is a powerful and cost-effective tool for characterising the biodegradability and stability of the organic matter in landfilled municipal solid waste and can be used for monitoring the progress of in situ aeration.     

Sustainable disposal of municipal solid waste: Post bioreactor landfill polishing

Sustainable disposal of municipal solid waste (MSW) requires assurance that contaminant release will be minimized or prevented within a reasonable time frame before the landfill is abandoned so that the risk of contamination release is not passed to future generations. This could be accomplished through waste acceptance criteria such as those established by the European Union (EU) that prohibit land disposal of untreated organic matter. In the EU, mechanical, biological and/or thermal pretreatment of MSW is therefore necessary prior to landfilling which is complicated and costly. In other parts of the world, treatment within highly engineered landfills is under development, known as bioreactor landfills. However, the completed bioreactor landfill still contains material, largely nonbiodegradable carbon and ammonia that may be released to the environment over the long-term. This paper provides a conceptual analysis of an approach to ensure landfill sustainability by the rapid removal of these remaining materials, leachate treatment and recirculation combined with aeration. The analysis in this paper includes a preliminary experimental evaluation using real mature leachate and waste samples, a modeling effort using a simplified mass balance approach and input parameters from real typical bioreactor cases, and a cost estimate for the suggested treatment method.     

Comparison between lab- and full-scale applications of in situ aeration of an old landfill and assessment of long-term emission development after completion

Sustainable landfilling has become a fundamental objective in many modern waste management concepts. In this context, the in situ aeration of landfills has been recognised for its potential to convert conventional anaerobic landfills into biological stabilised state, whereby both current and potential (long-term) emissions of the landfilled waste are mitigated. In recent years, different in situ aeration concepts have been successfully applied in Europe, North America and Asia, all pursuing different objectives and strategies.In Austria, the first full-scale application of in situ landfill aeration by means of low pressure air injection and simultaneous off-gas collection and treatment was implemented on an old, small municipal solid waste (MSW) landfill (2.6 ha) in autumn 2007. Complementary laboratory investigations were conducted with waste samples taken from the landfill site in order to provide more information on the transferability of the results from lab- to full-scale aeration measures. In addition, long-term emission development of the stabilised waste after aeration completion was assessed in an ongoing laboratory experiment. Although the initial waste material was described as mostly stable in terms of the biological parameters gas generation potential over 21 days (GP₂₁) and respiration activity over 4 days (RA₄), the lab-scale experiments indicated that aeration, which led to a significant improvement of leachate quality, was accompanied by further measurable changes in the solid waste material under optimised conditions. Even 75 weeks after aeration completion the leachate, as well as gaseous emissions from the stabilised waste material, remained low and stayed below the authorised Austrian discharge limits. However, the application of in situ aeration at the investigated landfill is a factor 10 behind the lab-based predictions after 3 years of operation, mainly due to technical limitations in the full-scale operation (e.g. high air flow resistivity due to high water content of waste and temporarily high water levels within the landfill; limited efficiency of the aeration wells). In addition, material preparation (e.g. sieving, sorting and homogenisation) prior to the emplacement in Landfill Simulation Reactors (LSRs) must be considered when transferring results from lab- to full-scale application.     

Aerobic in situ stabilization of Landfill Konstanz Dorfweiher: Leachate quality after 1 year of operation

Modern landfill understanding points out controlled operation of landfills. Emissions from landfills are caused mainly by anaerobic biodegradation processes which continue for very long time periods after landfill closure. In situ landfill stabilization aims controlled reduction of emissions towards reduced expenditures as well as aftercare measures. Since April 2010, a new in situ stabilization technique is being applied at a pilot scale landfill (BAIV) within Landfill Konstanz Dorfweiher. This new method utilizes intermittent aeration and leachate recirculation for waste stabilization. In this study, influence of this technique on leachate quality is investigated. Among many other parameters, leachate analyses were conducted for COD, BOD₅, NH₄–N, NO₂–N, NO₃–N, TKN and chloride besides continuously on site recorded pH, electrical conductivity and oxidation–reduction potential (ORP). Results from leachate quality analyses showed that biological activity in the landfill was accelerated resulting in initial higher leachate strength and reduced emission potential of landfill. During full scale in situ aeration, ambient conditions differ from optimized laboratory scale conditions which mainly concern temperature increase and deficient aeration of some landfill parts (Ritzkowski and Stegmann, 2005). Thus, as a field application results of this study have major importance on further process optimization and application.     

Metal speciation in landfill leachates with a focus on the influence of organic matter

This study characterises the heavy-metal content in leachates collected from eight landfills in France. In order to identify heavy metal occurrence in the different size fractions of leachates, a cascade filtration protocol was applied directly in the field, under a nitrogen gas atmosphere to avoid metal oxidation. The results of analyses performed on the leachates suggest that most of the metals are concentrated in the <30 kDa fraction, while lead, copper and cadmium show an association with larger particles. Initial speciation calculations, without considering metal association with organic matter, suggest that leachate concentrations in lead, copper, nickel and zinc are super-saturated with respect to sulphur phases. Speciation calculations that account for metal complexation with organic matter, considered as fulvic acids based on C1(s) NEXAFS spectroscopy, show that this mechanism is not sufficient to explain such deviation from equilibrium conditions. It is therefore hypothesized that the deviation results also from the influence of biological activity on the kinetics of mineral phase precipitation and dissolution, thus providing a dynamic system. The results of chemical analyses of sampled fluids are compared with speciation calculations and some implications for the assessment of metal mobility and natural attenuation in a context of landfill risk assessment are discussed.     

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.     

Impact of using high-density polyethylene geomembrane layer as landfill intermediate cover on landfill gas extraction

Clay is widely used as a traditional cover material for landfills. As clay becomes increasingly costly and scarce, and it also reduces the storage capacity of landfills, alternative materials with low hydraulic conductivity are employed. In developing countries such as China, landfill gas (LFG) is usually extracted for utilization during filling stage, therefore, the intermediate covering system is an important part in a landfill. In this study, a field test of LFG extraction was implemented under the condition of using high-density polyethylene (HDPE) geomembrane layer as the only intermediate cover on the landfill. Results showed that after welding the HDPE geomembranes together to form a whole airtight layer upon a larger area of landfill, the gas flow in the general pipe increased 25% comparing with the design that the HDPE geomembranes were not welded together, which means that the gas extraction ability improved. However as the heat isolation capacity of the HDPE geomembrane layer is low, the gas generation ability of a shallow landfill is likely to be weakened in cold weather. Although using HDPE geomembrane layer as intermediate cover is acceptable in practice, the management and maintenance of it needs to be investigated in order to guarantee its effective operation for a long term.     

Generating CO2-credits through landfill in situ aeration

Landfills are some of the major anthropogenic sources of methane emissions worldwide. The installation and operation of gas extraction systems for many landfills in Europe and the US, often including technical installations for energy recovery, significantly reduced these emissions during the last decades. Residual landfill gas, however, is still continuously produced after the energy recovery became economically unattractive, thus resulting in ongoing methane emissions for many years. By landfill in situ aeration these methane emissions can be widely avoided both, during the aeration process as well as in the subsequent aftercare period. Based on model calculations and online monitoring data the amount of avoided CO_2-eq. can be determined. For an in situ aerated landfill in northern Germany, acting as a case study, 83–95% (depending on the kind and quality of top cover) of the greenhouse gas emission potential could be reduced under strictly controlled conditions. Recently the United Nations Framework Convention on Climate Change (UNFCCC) has approved a new methodology on the “Avoidance of landfill gas emissions by in situ aeration of landfills” (UNFCCC, 2009). Based on this methodology landfill aeration projects might be considered for generation of Certified Emission Reductions (CERs) in the course of CDM projects. This paper contributes towards an evaluation of the potential of landfill aeration for methane emissions reduction.     

Landfill aeration within the scope of post-closure care and its completion

The time frame required for post-closure care of Municipal Solid Waste (MSW) landfills is often assessed over several decades or centuries. One possibility to significantly shorten this period and, at the same time, improve the emission behavior exists with in situ aeration. Positive effects in connection with this method for biological stabilization have been investigated and published elsewhere. However, until today neither generally accepted monitoring guidelines nor completion criteria have been defined. With the paper on hand the authors propose a methodology for the assessment of both, total and remaining stabilization periods for aerated landfills. The central component of this methodology is a carbon balance. The latter is based on a detailed waste characterization in combination with online monitoring of the emissions (gas and leachate). The methodology is exemplarily demonstrated by means of data derived from a full scale project in Northern Germany. Here it could be shown that the predicted aeration period of approximately 6.4 years was sufficient to bio-stabilize the landfill.Furthermore, proposals for the completion of landfill aeration are presented. In this connection, carbon balance is of particular importance since the amount of biodegradable organic carbon mainly determines the emission potential. Additional parameters, aiming at a validation of the state of biological stabilization achieved during aeration are proposed and described.     

A critique of risk modeling and risk assessment of municipal landfills based on U.S. Environmental Protection Agency techniques

Environmental risks are a growing public concern in America. The threat of contaminated drinking water from municipal solid waste (MSW) landfills is receiving increased attention from citizens and from the United States Environmental Protection Agency (USEPA). Examination of USEPA data collected from MSW landfills reveals approximate risks posed by these landfills. USEPA research suggests that 60% of MSW landfills present less than a 1 in 10 billion risk of cancer incidence. Another 6% pose risks less than 1 in a billion, while 17% present risks less than 1 in a million. This study addresses the USEPA risk assessment techniques and models for estimating MSW landfill risks. USEPA data for toxic constituents of landfill leachate are also analysed in order to better understand the difficulties encountered in estimating landfill risks. The study also presents a brief discussion of public perceptions of risk as they relate to communicating the USEPA landfill model results to those who might be affected.     

Probabilistic approach for estimating the release of contaminants under field management scenarios

A probabilistic approach is presented for estimating the release of contaminants by leaching, when wastes are being considered for disposal in a class of landfills but the specific landfill disposal site is uncertain. A simple percolation and equilibrium-based release model is used in conjunction with laboratory testing results and observations of field leachate characteristics for municipal solid waste landfills, hazardous waste landfills and industrial co-disposal landfills. The approach is applied for assessing the efficacy of potential treatment processes for mercury contaminated soils. For each landfill scenario, historical values of leachate pH and annual leachate generation quantities were used to derive the probability distribution functions of the field pH and LS ratio that may be expected to contact the disposed material over an estimated time period of 100 years. For each potential treatment process, laboratory testing was used to establish the treated material's leaching characteristics as a function of pH LS ratio. This approach allowed determination of distribution frequencies and limit values for release estimates instead of single point estimates. The probability of the mass of a constituent of interest released exceeding a hypothetical threshold was examined for each treatment process and landfill system. Results of the probabilistic analysis allowed for integration of a range of data and provided a good basis for assessing the efficacy of the examined treatment processes over the three assumed disposal scenarios.     

Modelling and experimental investigation of environmental influences on the acetate and methane formation in solid waste

An anaerobic reaction model is represented and used for simulation of the biodegradation of organic compounds and the generation of biogas. The model is based on fundamental relationships among physical, chemical, thermodynamic and microbial processes occurring in municipal landfills. Local microbially mediated degradation processes occurring in municipal landfills are simulated in terms of hydrolysis of readily and inherently degradable organic matter, the formation of acetate as surrogate for intermediary low-molecular carbon substrates, and the generation of the biogases CH4 and CO2. Thus, the overall decomposition of the organic matter has been assumed to follow three sequential anaerobic reactions steps: hydrolysis, acetogenesis and methanogenesis. In order to study the impact of environmental factors on the biological decomposition processes, experiments have been conducted to investigate the effect of temperature and water content. In the degradation model, the impact of temperature and water content was defined as reaction rate influencing factors. Further, waste samples have been taken from four drill holes on a municipal landfill near Wolfsburg (Germany) and used to analyze and to describe the waste composition and prevailing environmental conditions dependent on the depth of the drill hole. The data and waste samples obtained from the landfill have also been used for model development and validation.     

The use of volcanic soil as mineral landfill liner--III. Heavy metals retention capacity.

The volcanic soil of Southern Chile was tested for its heavy metal retention capacity. The maximum uptakes for CrO4(2-) (CrVI), Cu(2+), Zn(2+) and Pb(2+) were determined to be 2.74, 5.32, 5.86 and 7.44 mg g(-1), respectively. At a slightly alkaline pH value (7.5), it seems that a precipitation-adsorption process was responsible for the Cu(2+) and Zn(2+) uptake onto volcanic soil. All the determined values are of the same order of magnitude as natural zeolites heavy metals adsorption capacities. In addition, the heavy metals diffusion model through a 1 m volcanic soil mineral liner shows breakthrough times of 21.6, 10.2 and 8.9 years, for Pb(2+), Zn(2+) and Cu(2+), respectively, confirming the trend obtained in the adsorption isotherms. The natural volcanic soil of Southern Chile is an interesting material for possible use as landfill mineral basal sealing. It has an appropriate sealing potential (average Kf value of 5.85 x 10(-9) m s(-1)) and a heavy metals retention capacity comparable with natural zeolites. About two-thirds of the agricultural land in Chile (approximately 0.4 million km2) is derived from volcanic ash, suggesting an important soil volume for future landfill projects, that could be obtained in sufficient quantities from urban building activities.