Environmental behaviour of a construction made of a mixture of hydraulic binders and air pollution control residues from municipal solid waste incineration Part 1. Physico-chemical characterisation and modelling of the source term

The reuse of waste materials requires the development of assessment methods for the long-term release of pollutants (source term) from wastes (or materials containing wastes) in contact with water. These methods depend on the scenario conditions: characteristics of the materials (especially physical structure and composition), contact with water. The scenario studied here is a water storage reservoir for fire fighting. The reservoir construction is made of a mixture of hydraulic binders and air pollution control (APC) residues from a municipal solid waste incinerator (MSWI). The modelling of the source term is performed in 5 steps ranging from the physico-chemical characterisation of the material to the validation of the proposed model by means of field simulation devices. This article presents the first steps of the methodology: physico-chemical characterisation of the source term, identification of the main transfer mechanisms and laboratory scale modelling of the source term. During the physico-chemical characterisation, it has been shown that the solidified waste shows a high basic capacity and that a relative decrease in pH during leaching favours retention of the main pollutants. During the first leaching sequences, the dynamic leaching tests show that the release of pollutants such as cadmium, arsenic, zinc and lead is extremely low but that the release of alkaline species (sodium and potassium) and chloride is very high from the beginning, whereas the release of calcium remains very high even after 3600 h of leaching. Identification of the main transfer mechanisms concludes that the release of soluble pollutants is the combined result of diffusional transfer of pollutants in the solution and the physico-chemical specificity of the species. The modelling based on these features enables a good simulation of the release but reveals a deviation from the experimental results after 500 h for alkaline species and 1000 h for Ca and Cl leaching. However, this deviation only appears after release of the major part of these elements.     

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.     

Temporary stabilization of air pollution control residues using carbonation

Carbonation presents a good prospect for stabilizing alkaline waste materials. The risk of metal leaching from carbonated waste was investigated in the present study; in particular, the effect of the carbonation process and leachate pH on the leaching toxicity of the alkaline air pollution control (APC) residues from municipal solid waste incinerator was evaluated. The pH varying test was conducted to characterize the leaching characteristics of the raw and carbonated residue over a broad range of pH. Partial least square modeling and thermodynamic modeling using Visual MINTEQ were applied to highlight the significant process parameters that controlled metal leaching from the carbonated residue. By lowering the pH to 8-11, the carbonation process reduced markedly the leaching toxicity of the alkaline APC residue; however, the treated APC residue showed similar potential risk of heavy metal release as the raw ash when subjected to an acid shock. The carbonated waste could, thereby, not be disposed of safely. Nonetheless, carbonation could be applied as a temporary stabilization process for heavy metals in APC residues in order to reduce the leaching risk during its transportation and storage before final disposal.     

Washing of waste prior to landfilling

The main impact produced by landfills is represented by the release of leachate emissions. Waste washing treatment has been investigated to evaluate its efficiency in reducing the waste leaching fraction prior to landfilling. The results of laboratory-scale washing tests applied to several significant residues from integrated management of solid waste are presented in this study, specifically: non-recyclable plastics from source separation, mechanical-biological treated municipal solid waste and a special waste, automotive shredded residues. Results obtained demonstrate that washing treatment contributes towards combating the environmental impacts of raw wastes. Accordingly, a leachate production model was applied, leading to the consideration that the concentrations of chemical oxygen demand (COD) and total Kjeldahl nitrogen (TKN), parameters of fundamental importance in the characterization of landfill leachate, from a landfill containing washed wastes, are comparable to those that would only be reached between 90 and 220years later in the presence of raw wastes. The findings obtained demonstrated that washing of waste may represent an effective means of reducing the leachable fraction resulting in a consequent decrease in landfill emissions. Further studies on pilot scale are needed to assess the potential for full-scale application of this treatment.     

Leaching of inorganic contaminants from cement-based waste materials as a result of carbonation during intermittent wetting

Characterization of the leaching behavior of wastes is a crucial step in the environmental assessment for reuse or disposal scenarios. The release of inorganic contaminants from waste materials is typically evaluated by tank leaching of continuously water-saturated material. However, materials, in many field or management scenarios, experience cyclic wetting and drying under varied environmental conditions (i.e. variable relative humidity, atmospheric CO2 or CO2 from biologic activities). During periods of storage in an unsaturated environment, many processes may occur that can influence the release potential and release rate of inorganic constituents. The research presented here was carried out to examine how the phenomena of carbonation during drying influence the release of inorganic contaminants from Portland cement-based materials during cyclic wetting and storage. Batch equilibrium leaching tests were used to determine constituent solubility as a function of pH. Dynamic leaching tests on monolithic material were carried out to determine the rate of constituent release as a function of leaching time and intermittent storage conditions. This paper presents the results observed for three typical waste constituents, arsenic, cadmium and lead.     

Leaching behaviour of elements and evaluation of pre-treatment methods for municipal solid waste incinerator residues in column leaching tests.

Two new pre-treatment methods (water-washing/carbonation and carbonation/phosphate stabilization) of municipal solid waste (MSW) incinerator residues were evaluated by column leaching tests under aerobic conditions and anaerobic conditions (which were changed to aerobic conditions after 10 months). A mixture of bottom ash and fly ash (5:1 ratio) was pre-treated using each method. Shredded incombustible residues (SIR) were added to each ash preparation in proportions similar to the ratios present in landfills. For comparison, landfill wastes typical of Japan, namely, a mixture of bottom ash, chelating-pre-treated fly ash, and SIR, were also examined. Leachate samples were collected periodically and analysed over a 15-month period. When compared with chelating pretreatment, both water-washing/carbonation and carbonation/ phosphate stabilization reduced the leaching of Pb, Al, and Cu by about one to two orders of magnitude. Moreover, the initial concentrations of Ca and Pb in leachates from column of water-washing/carbonation were 56-57% and 84-96% less than those from the column of carbonation/phosphate stabilization. Therefore, water-washing/carbonation was considered to be a promising approach to obtain early waste stabilization and to reduce the release of heavy metals to near-negligible levels. The leaching behaviour of elements was also discussed.     

Multiple-scale dynamic leaching of a municipal solid waste incineration ash

Predicting the impact on the subsurface and groundwater of a pollutant source, such as municipal solid waste (MSW) incineration ash, requires a knowledge of the so-called "source term". The source term describes the manner in which concentrations in dissolved elements in water percolating through waste evolve over time, for a given percolation scenario (infiltration rate, waste source dimensions, etc.). If the source term is known, it can be coupled with a model that simulates the fate and transport of dissolved constituents in the environment of the waste (in particular in groundwater), in order to calculate potential exposures or impacts. The standardized laboratory upward-flow percolation test is generally considered a relevant test for helping to define the source term for granular waste. The LIMULE project (Multiple-Scale Leaching) examined to what extent this test, performed in very specific conditions, could help predict the behaviour of waste at other scales and for other conditions of percolation. Three distinct scales of percolation were tested: a laboratory upward-flow percolation column (30cm), lysimeter cells (1-2m) and a large column (5m) instrumented at different depths. Comparison of concentration data collected from the different experiments suggests that for some non-reactive constituents (Cl, Na, K, etc.), the liquid versus solid ratio (L/S) provides a reasonable means of extrapolating from one scale to another; if concentration data are plotted versus this ratio, the curves coincide quite well. On the other hand, for reactive elements such as chromium and aluminium, which are linked by redox reactions, the L/S ratio does not provide a means of extrapolation, due in particular to kinetic control on reactions. Hence extrapolation with the help of coupled chemistry-transport modelling is proposed.     

Real time alteration of a nuclear waste glass and remobilization of lanthanide into an interphase

The development of predictive models for the long term evolution of nuclear waste glass requires the complete knowledge of the glass dissolution at the laboratory scale. A new approach was developed to determine the initial reaction during the first steps of experience, a new concept was developed, based on the combination of dynamic leaching test and the characterization of the altered materials. With this experimental set-up it is possible to follow in real time the glass alteration process at a fine temporal scale. The results put in evidence a singular behaviour of the lanthanide, shown by a concentration peak of La, Nd and Ce after 2 h and a quick decrease of their concentration measured on line in the solution during the leaching test. This fact is directly linked to the development of an interphase (altered layer which differs from the initial solid by its texture, structure and chemical composition) at the interface of the glass surface and the leaching solution. This work is an attempt to integrate the formation of the alteration products (here the interphase) during leaching into the dissolution mechanisms of a nuclear waste glass. A model is proposed and discussed.     

The effects of accelerated carbonation on CO2 uptake and metal release from incineration APC residues

This work presents the results of a study on accelerated carbonation of incinerator air pollution control residues, with a particular focus on the modifications in the leaching behaviour of the ash. Aqueous carbonation experiments were carried out using 100% CO₂ at different temperatures, pressures and liquid-to-solid ratios, in order to assess their influence on process kinetics, CO₂ uptake and the leaching behaviour of major and trace elements. The ash showed a particularly high reactivity towards CO₂, owing to the abundance of calcium hydroxides phases, with a maximum CO₂ uptake of ～250 g/kg. The main effects of carbonation on trace metal leaching involved a significant decrease in mobility for Pb, Zn and Cu at high pH values, a slight change or mobilization for Cr and Sb, and no major effects on the release of As and soluble salts. Geochemical modelling of leachates indicated solubility control by different minerals after carbonation. In particular, in the stability pH range of carbonates, solubility control by a number of metal carbonates was clearly suggested by modelling results. These findings indicate that accelerated carbonation of incinerator ashes has the potential to convert trace contaminants into sparingly soluble carbonate forms, with an overall positive effect on their leaching behaviour.     

Leaching assessment of road materials containing primary lead and zinc slags

Characterisation of the leaching behaviour of waste-containing materials is a crucial step in the environmental assessment for reuse scenarios. In our research we applied the multi-step European methodology ENV 12-920 to the leaching assessment of road materials containing metallurgical slag. A Zn slag from an imperial smelting furnace (ISF) and a Pb slag from a lead blast furnace (LBF) are investigated. The two slags contain up to 11.2 wt% of lead and 3.5 wt% of zinc and were introduced as a partial substitute for sand in two road materials, namely sand-cement and sand-bitumen. At the laboratory scale, a leaching assessment was performed first through batch equilibrium leaching tests. Second, the release rate of the contaminants was evaluated using saturated leaching tests on monolithic material. Third, laboratory tests were conducted on monolithic samples under intermittent wetting conditions. Pilot-scale tests were conducted for field testing of intermittent wetting conditions. The results show that the release of Pb and Zn from the materials in a saturated scenario was controlled by the pH of the leachates. For the intermittent wetting conditions, an additional factor, blocking of the pores by precipitation during the drying phase is proposed. Pilot-scale leaching behaviour only partially matched with the laboratory-scale test results: new mass transfer mechanisms and adapted laboratory leaching tests are discussed.     

Metal releases from a municipal solid waste incineration air pollution control residue mixed with compost

The influence of 10 wt.% mature compost was tested on the heavy metal leachate emissions from a calcium-rich municipal solid waste incineration air pollution control residue (MSWI APC). Apart from elongated columns (500 and 1250 mm), an otherwise norm compliant European percolation test setup was used. More than 99% of the metals Al, As, Cd, Cr, Cu, Fe and Ni were left in the APC residue after leaching to a liquid-to-solid ratio (L/S) of 10. Apparent short-term effects of elevated leachate DOC concentrations on heavy metal releases were not detected. Zn and Pb leachate concentrations were one order of magnitude lower for L/S 5 and 10 from the pure APC residue column, which suggests a possible long-term effect of compost on the release of these elements. Prolonging the contact time between the pore water and the material resulted in elevated leachate concentrations at L/S 0.1 to L/S 1 by a factor of 2. Only Cr and Pb concentrations were at their maxima in the first leachates at L/S 0.1. Equilibrium speciation modelling with the PHREEQC code suggested portlandite (Ca(OH)2) to control Ca solubility and pH.     

Hazardous chemical site remediation through capping: Problems with long-term protection

The capping of waste management units and contaminated soils is receiving increasing attention as a low-cost method for hazardous chemical site remediation. Capping is used to prevent further groundwater pollution by existing waste management units and contaminated soils through limiting the moisture that enters the wastes. In principle, for wastes located above the water table, the construction of an impermeable cap can prevent leaching of the wastes (leachate generation) and groundwater pollution. In practice, appropriately designed and constructed RCRA caps can provide for only short-term prevention of groundwater pollution. Alternative approaches are available for capping of wastes that can be effective in preventing moisture from entering the wastes and concomitant groundwater pollution. These approaches recognize the inability of the typical RCRA cap to keep wastes dry for as long as waste constituents will be a threat and, most importantly, provide the necessary funds to effectively address all plausible worst-case scenario failures that could occur at a capped waste management unit or contaminated soil area.     

Contribution of 3-D time-lapse ERT to the study of leachate recirculation in a landfill

Leachate recirculation is a key process in the operation of municipal waste landfills as bioreactors. It aims at increasing the moisture content to optimise the biodegradation. Because waste is a very heterogeneous and anisotropic porous media, the geometry of the leachate plume recirculation is difficult to delineate from the surface at the scale of the bioreactor site. In this study, 3-D time-lapse electrical resistivity tomography (ERT) was used to obtain useful information for understanding leachate recirculation hydrodynamics. The ERT inversion methodology and the electrode arrays were optimised using numerical modelling simulating a 3-D leachate injection scenario. Time-lapse ERT was subsequently applied at the field scale during an experimental injection. We compared ERT images with injected volumes to evaluate the sensitivity of time-lapse ERT to delineate the plume migration. The results show that time-lapse ERT can accomplish the following: (i) accurately locate the injection plume, delineating its depth and lateral extension; (ii) be used to estimate some hydraulic properties of waste.     

Accelerated carbonation treatment of industrial wastes

The disposal of industrial waste presents major logistical, financial and environmental issues. Technologies that can reduce the hazardous properties of wastes are urgently required. In the present work, a number of industrial wastes arising from the cement, metallurgical, paper, waste disposal and energy industries were treated with accelerated carbonation. In this process carbonation was effected by exposing the waste to pure carbon dioxide gas. The paper and cement wastes chemically combined with up to 25% by weight of gas. The reactivity of the wastes to carbon dioxide was controlled by their constituent minerals, and not by their elemental composition, as previously postulated. Similarly, microstructural alteration upon carbonation was primarily influenced by mineralogy. Many of the thermal wastes tested were classified as hazardous, based upon regulated metal content and pH. Treatment by accelerated carbonation reduced the leaching of certain metals, aiding the disposal of many as stable non-reactive wastes. Significant volumes of carbon dioxide were sequestrated into the accelerated carbonated treated wastes.     

Comparison of leaching tests to determine and quantify the release of inorganic contaminants in demolition waste

The changes in waste management policy caused by the massive generation of waste materials (e.g. construction and demolition waste material, municipal waste incineration products) has led to an increase in the reuse and recycling of waste materials. For environmental risk assessment, test procedures are necessary to examine waste materials before they can be reused. In this article, results of column and lysimeter leaching tests having been applied to inorganic compounds in a reference demolition waste material are presented. The results show a good agreement between the leaching behaviour determined with the lysimeter unit and the column units used in the laboratory. In view of less time and system requirements compared to lysimeter systems, laboratory column units can be considered as a practicable instrument to assess the time-dependent release of inorganic compounds under conditions similar to those encountered in a natural environment. The high concentrations of elements in the seepage water at the initial stage of elution are reflected by the laboratory column leaching tests. In particular, authorities or laboratories might benefit and have an easy-to-use, but nevertheless reliable, method to serve as a basis for decision-making.     

Investigations into the landfill behaviour of pretreated wastes

Mechanical-biological treatment of municipal solid waste has become popular throughout the UK and other parts of Europe to enable compliance with the Landfill Directive. Pretreatment will have a major influence on the degradation and settlement characteristics of the waste in landfills owing to the changes in the composition and properties of the wastes. This paper presents and compares the results of long term landfill behaviour of the UK and German MBT wastes pretreated to different standards. The gas generating potential, leachate quality and settlement characteristics are highlighted. The results reveal that it is possible to achieve stabilisation of MBT waste within a year and the biogas yield and leachate strength of German MBT waste was significantly reduced compared with the UK MBT waste. The settlement resulting from mechanical creep is more significant than the biodegradation induced settlement in both cases.     

Assessment of mobility and bioavailability of contaminants in MSW incineration ash with aquatic and terrestrial bioassays

Incineration of municipal solid waste (MSW) is a waste treatment method which can be sustainable in terms of waste volume reduction as well as a source of renewable energy. In the process fly and bottom ash is generated as a waste material. The ash residue may vary greatly in composition depending on the type of waste incinerated and it can contain elevated levels of harmful contaminants such as heavy metals. In this study, the ecotoxicity of a weathered, untreated incineration bottom ash was characterized as defined by the H14 criterion of the EU Waste Framework Directive by means of an elemental analysis, leaching tests followed by a chemical analysis and a combination of aquatic and solid-phase bioassays. The experiments were conducted to assess the mobility and bioavailability of ash contaminants. A combination of aquatic and terrestrial bioassays was used to determine potentially adverse acute effects of exposure to the solid ash and aqueous ash leachates. The results from the study showed that the bottom ash from a municipal waste incineration plant in mid-Sweden contained levels of metals such as Cu, Pb and Zn, which exceeded the Swedish EPA limit values for inert wastes. The chemical analysis of the ash leachates showed high concentrations of particularly Cr. The leachate concentration of Cr exceeded the limit value for L/S 10 leaching for inert wastes. Filtration of leachates prior to analysis may have underestimated the leachability of complex-forming metals such as Cu and Pb. The germination test of solid ash and ash leachates using T. repens showed a higher inhibition of seedling emergence of seeds exposed to the solid ash than the seeds exposed to ash leachates. This indicated a relatively low mobility of toxicants from the solid ash into the leachates, although some metals exceeded the L/S 10 leaching limit values for inert wastes. The Microtox® toxicity test showed only a very low toxic response to the ash leachate exposure, while the D. magna immobility test showed a moderately high toxic effect of the ash leachates. Overall, the results from this study showed an ecotoxic effect of the solid MSW bottom ash and the corresponding ash leachates. The material may therefore pose an environmental risk if used in construction applications. However, as the testing of the solid ash was rather limited and the ash leachate showed an unusually high leaching of Cr, further assessments are required in order to conclusively characterize the bottom ash studied herein as hazardous according to the H14 criterion.     

Evaluation of leaching and extraction procedures for soil and waste

Laboratory leaching tests may be used for source term determination as a basis for risk assessment for soil-groundwater pathways on contaminated sites. In order to evaluate different leaching procedures, batch extraction tests and percolation tests were performed using three reference materials produced from contaminated soil, demolition waste and municipal solid waste incinerator bottom ash. Emphasis was placed on the investigation of the leachability of the heavy metals copper and chromium, polycyclic aromatic hydrocarbons (PAHs) and the anions chloride and sulfate. Significant discrepancies between column experiments and batch/extraction tests were found for the release of PAHs and to a lesser extent for the heavy metals Cu and Cr. Additionally interlaboratory comparisons were conducted based on different leaching tests with the reference materials and evaluated using the criteria of comparability and reproducibility. The best reproducibility was achieved for all investigated substances in column tests. The reproducibility of batch tests was acceptable except for PAHs. The results from the experimental work will help establish standardized and feasible laboratory procedures as fundamental for substance specific risk assessment of contaminated sites.     

Comparison of percolation to batch and sequential leaching tests: Theory and data

Leaching tests are becoming more relevant in assessing solid waste material, particularly with respect to groundwater risks. In the field, water infiltration is the dominant leaching mechanism, which is simulated in the lab with batch and column tests. In this study, we compared percolation, through analytical solutions of the advection–dispersion equation, to laboratory batch and sequential leaching tests. The analytical solutions are supported with comprehensive data from various field and laboratory leaching of different solutes from waste materials and soils collected in long-term joint research projects funded by the German Federal Ministry for Education and Research and the Federal Environment Agency. The comparison of theory and data is facilitated if concentrations and cumulative release are plotted versus the liquid–solid ratios (LS). Both theory and data indicate that leaching behaviour is independent of duration and physical dimensions of the leaching tests. This holds even if field lysimeters are compared to laboratory columns of different size, different flow velocities as well as different contact times. In general, laboratory batch tests over predict effluent concentrations (for LS < K_d). Leaching of solutes from solid samples of certain materials (e.g. chloride from incineration ashes or sulphate from demolition waste) in column and lysimeter tests compares very well and agrees with the analytical solutions. Overall, reproducibility and agreement with theory of column tests are better than batch tests, presumably because the latter are prone to artefacts (e.g. in liquid–solid separation steps). Theory and data fit surprisingly well, despite the fact that the theory is based on the local equilibrium assumption; non-linear sorption and chemical reactions in the solid waste materials are not considered.     

Demobilisation of critical contaminants in four typical waste-to-energy ashes by carbonation

Two bottom ashes, one air pollution control (APC) residue and one fly ash from three different Swedish municipal solid waste incineration (MSWI) plants were characterised regarding the leaching of environmentally relevant components. Characterisation was performed using a diffusion tank leaching test. The impact of carbonation on the release of eight critical components, i.e., Cl(-), Cr, Cu, Mo, Pb, Sb, Se, SO(4)(2-) and Zn, was assessed at a lab-scale and showed carbonation to have a more pronounced demobilising effect on critical components in bottom ashes than in APC residue and fly ash. From grate type incinerator bottom ash, the release of Cr decreased by 97%, by 63% for Cu and by 45% for Sb. In the investigated APC residue, the releases of Cr, Se and Pb were defined as critical, although they either remained unaffected or increased after carbonation. Cl(-) and SO(4)(2-) remained mobile after carbonation in all investigated residues.