Physical containment of municipal solid waste incineration bottom ash by accelerated carbonation

Accelerated carbonation of municipal solid waste incineration residues is effective for immobilizing heavy metals. In this study, the contribution of the physical containment by carbonation to immobilization of some heavy metals was examined by some leaching tests and SEM–EDS analysis of untreated, carbonated, and milled bottom ash after carbonation that was crushed with a mortar to a mean particle size of approximately 1 μm. The surface of carbonated bottom ash particles on SEM images seemed mostly coated, while there were uneven micro-spaces on the surface of the untreated bottom ash. Results of Japan Leaching Test No. 18 (JLT18) for soil pollution showed that milling carbonated bottom ash increased the pH and EC. The leaching concentration of each element tended to be high for untreated samples, and was decreased by carbonation. However, after the milling of carbonated samples, the leaching concentration became high again. The immobilization effect of each element was weakened by milling. The ratio of physical containment effect to immobilization effects by accelerated carbonation was calculated using the results of JLT18. The ratio for each element was as follows: Pb: 13.9–69.0 %, Cu: 12.0–49.1 %, Cr: 24.1–99.7 %, Zn: 20.0–33.3 %, and Ca: 28.9–63.4 %.     

Stabilization/solidification of MSW incineration residues from facilities with different air pollution control systems. Durability of matrices versus carbonation

This paper discusses the stabilisation/solidification process with Portland cement applied to municipal solid waste incineration residues. Two types of residues were considered: fly ash (FA) produced in an electrostatic precipitator, and air pollution control (APC) residues from a semi-dry scrubber process. Cement pastes with different percentages of FA and APC residues were characterised according to their physical properties, the effect of the hydration products and their leaching behaviour. Portland pastes prepared with APC residues showed a rapid setting velocity in comparison with setting time for those pastes substituted with FA residues. Portland cement hydration was retarded in FA pastes. Leaching test results showed that heavy metals (such as Zn, Pb and Cd) and sulphates are immobilised within the paste, whereas chlorides are only partially retained. The carbonation process increases the leachability of S04(2-) and heavy metals such as Zn and Cr.     

Assessment of long-term pH developments in leachate from waste incineration residues.

Environmental assessment of residue disposal needs to account for long-term changes in leaching conditions. Leaching of heavy metals from incineration residues are highly affected by the leachate pH; the overall environmental consequences of disposing of these residues are therefore greatly influenced by changes in pH over time. The paper presents an approach for assessing pH changes in leachate from municipal solid waste incineration (MSWI) air-pollution-control (APC) residues. Residue samples were subjected to a stepwise batch extraction method in order to obtain residue samples at a range of pH values (similar to common pH-dependence tests), and then on these samples to determine leaching of alkalinity as well as remaining solid phase alkalinity. On a range of APC residues covering various pretreatment and disposal options, this procedure was used to determine leachable and residual alkalinity as a function of pH. Mass balance calculations for typical disposal scenarios were used to provide data on pH as a function of the liquid-to-solid (L/S) ratio in the leaching system. Regardless of residue type and pretreatment, pH was found to stay above 7 for L/S ratios up to about 2000 L kg(-1) corresponding to about 100,000 years in typical landfill scenarios. It was found that pH changes were mainly governed by alkalinity decreases from leaching processes rather than neutralization reactions. The results suggest that leaching testing for assessment purposes should be carried out in the alkaline range, for example, at pH 9. The paper offers a thorough basis for further modelling of incineration residue leaching and for modelling the environmental consequences of landfilling and utilization of these residues.     

Mobility of organic carbon from incineration residues

Dissolved organic carbon (DOC) may affect the transport of pollutants from incineration residues when landfilled or used in geotechnical construction. The leaching of dissolved organic carbon (DOC) from municipal solid waste incineration (MSWI) bottom ash and air pollution control residue (APC) from the incineration of waste wood was investigated. Factors affecting the mobility of DOC were studied in a reduced 2(6-1) experimental design. Controlled factors were treatment with ultrasonic radiation, full carbonation (addition of CO2 until the pH was stable for 2.5h), liquid-to-solid (L/S) ratio, pH, leaching temperature and time. Full carbonation, pH and the L/S ratio were the main factors controlling the mobility of DOC in the bottom ash. Approximately 60 weight-% of the total organic carbon (TOC) in the bottom ash was available for leaching in aqueous solutions. The L/S ratio and pH mainly controlled the mobilization of DOC from the APC residue. About 93 weight-% of TOC in the APC residue was, however, not mobilized at all, which might be due to a high content of elemental carbon. Using the European standard EN 13 137 for determination of total organic carbon (TOC) in MSWI residues is inappropriate. The results might be biased due to elemental carbon. It is recommended to develop a TOC method distinguishing between organic and elemental carbon.     

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.     

Air pollution control residues from waste incineration: current UK situation and assessment of alternative technologies

Current disposal options for APC residues in the UK and alternative treatment technologies developed world-wide have been reviewed. APC residues are currently landfilled in the UK where they undergo in situ solidification, although the future acceptability of this option is uncertain because the EU waste acceptance criteria (WAC) introduce strict limits on leaching that are difficult to achieve. Other APC residue treatment processes have been developed which are reported to reduce leaching to below relevant regulatory limits. The Ferrox process, the VKI process, the WES-PHix process, stabilisation/solidification using cementitious binders and a range of thermal treatment processes are reviewed. Thermal treatment technologies convert APC residues combined with other wastes into inert glass or glass-ceramics that encapsulate heavy metals. The waste management industry will inevitably use the cheapest available option for treating APC residues and strict interpretation and enforcement of waste legislation is required if new, potentially more sustainable technologies are to become commercially viable.     

The influence of pH on the leaching behaviour of inorganic components from municipal solid waste APC residues

The influence of pH on the leaching behaviour of air pollution control (APC) residues produced in municipal solid waste incineration (MSWI) is addressed in this study. The residue is considered hazardous waste, and in accordance with their chemical properties, the leaching of contaminants into the environment is the main concern. Several leaching tests can be used for research studies or regulatory purposes, where a wide variety of conditions may be tested. Our work deals mainly with the leaching behaviour of toxic heavy metals (Pb, Cd, Zn, Cr, Ni, Cu) and inorganics associated with soluble salts (Na, K, Ca, Cl). The main goal is to obtain an overview of the leachability of APC residues produced in a Portuguese MSWI process. Among the different variables that may have influence on the leaching behaviour, pH of the leachant solution is the most important one, and was evaluated through pH static tests. The acid neutralization capacity (ANC) of the residue was also determined, which is in the range of 6.2–6.8 meq g^?1 (for pH = 7) and 10.1–11.6 meq g^?1 (for pH = 4). The analysis of the leaching behaviour is particularly important when the leaching is solubility controlled. The amphoteric behaviour of some elements was observed, namely for Pb and Zn, which is characterized through high solubilization at low and high pH and moderate or low solubility at neutral or moderate high pH. The solubility curves for Pb, Cd, Zn, Cr, Ni and Cu as a function of pH were obtained, which are very useful for predicting the leaching behaviour in different scenarios. The solubility of K and Na reveals to be nearly independent of the solution pH and the released amount is mainly availability-controlled. Moreover, the pH static test showed that Cl^? is the most pH-independent species. The APC residue turns out to be a hazardous waste because of the high leaching of lead and chloride. On the other hand, leaching of elements like cadmium, nickel and copper is limited by the high pH of the residue, and as long as the waste keeps its ANC, the risk of mobilization of these elements is low.     

脱硫用电石渣的重金属浸出特性及其对环境的影响

针对电厂用脱硫剂电石渣,分析了其基本组成及重金属浸出特性,为电厂脱硫设施的参数设计和环境影响评价提供依据和参考。研究结果表明,脱硫用电石渣主要成分为Ca（OH）2,含量在40%～50%之间;在8种重金属的含量中,只有Cd的含量超出土壤质量三级标准的要求,基本不会对土壤造成污染。浸出毒性试验表明,电石渣及其脱硫产物属于非危险废物,其各种重金属的浸出浓度主要受其本身重金属含量和最终pH的影响,这种影响在Pb、Cu和Cd上表现得较为突出,酸性环境下更有利于他们的浸出;碱性环境下有利于Pb和Ni的浸出。     

Leaching behavior of heavy metals from municipal solid waste incineration bottom ash and its geochemical modeling

With the increase in the number of municipal solid waste incineration (MSWI) plants constructed in China recently, great attention has been paid to the heavy metal leaching toxicity of MSWI residues. In this study, the effects of various parameters, including extractant, leaching time, liquid-to-solid ratio, leachate pH, and heavy metal content, on the release properties of Cd, Cr, Cu, Ni, Pb, and Zn from MSWI bottom ash were investigated. Partial least-squares analysis was employed to highlight the interrelationships between the factors and response variables. Both experimental research and geochemical modeling using Visual MINTEQ software were conducted to study the pH-dependent leaching behavior of these metals in fresh and weathered bottom ash, considering precipitation/dissolution and surface complexation reactions (adsorption by hydrous ferric oxide and amorphous aluminum oxide/hydroxide). The results showed that leachate pH was the predominant factor influencing heavy metal leachability. The leaching of Cu, Pb, and Zn was mainly controlled by precipitation/dissolution reactions, whereas surface complexation had some effect on the leaching of Cr, Cd, and Ni for certain pH ranges. The modeling results aggreed well with the experimental results. Part of this work was presented at the Fourth International Conference on Combustion, Incineration/Pyrolysis and Emission Control (i-CIPEC)     

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.     

Belgian MSWI fly ashes and APC residues: a characterisation study

Municipal Solid Waste Incineration (MSWI) produces different sorts of residues, bottom ash, fly ashes and Air Pollution Control (APC) residues. Generally, fly ashes and APC residues are mixed at the MSWI plant and manage as a sole residue. In this study, fly ashes and APC residues have been sampled separately at different Belgian MSWI plant and analysed by X-ray fluorescence in order to highlight the composition differences that may appear between the solids. Ca and Cl are found to be the major elements in most of the samples. Lithophilic elements, such as Al and Si, are richer in furnace and boiler ashes, as can be expected. Leaching tests also show differences between the residues; leachates from furnace and boiler ashes are alkaline while those from bag filter residues present a pH value of 6, which impacts the leaching of heavy metals (Pb and Zn). The results suggest that it could be advantageous to manage fly ashes and APC residues separately by adjusting the treatment to their specificities.     

Effects of carbonation and leaching on porosity in cement-bound waste

Porosity is possibly an important parameter with respect to leaching of constituents from cement monoliths. During its lifetime, the pore structure of cementitious matrices changes due to carbonation and leaching. This paper discusses the effects of both accelerated carbonation and continuous leaching on the porosity, and, conversely, how porosity affects leaching properties. Two sample types are investigated: a mortar with MSWI-bottom ash substituting the sand fraction and a cement paste with 30 wt% of the cement substituted by a flue gas cleaning residue. The samples have been intensively carbonated in a 20% CO(2) atmosphere for up to 60 days and were subsequently leached. The porosity was investigated by mercury intrusion porosimetry. Accelerated carbonation decreases total porosity by 12% in the case of 60 days of treatment of bottom ash mortars, whereas continuous leaching during 225 days increases it by 16%. Both carbonation and leaching decrease the amount of smaller capillary pores. Carbonation decreases both porosity and pH. Decreasing porosity diminishes leaching of sodium and potassium, while the decrease in pH increases leaching. However, the former process dominates the latter, resulting in a net decreasing effect of carbonation on the release of sodium and potassium from these cement matrices.     

Comparison of leaching characteristics of heavy metals in APC residue from an MSW incinerator using various extraction methods

This study investigates four extraction methods (water extraction, toxicity characteristics leaching procedure (TCLP), modified TCLP with pH control, and sequential chemical extraction (SCE)), each representing different liquid-to-solid (L/S) ratios, pH controls, and types of leachant, and their effects on the leaching concentration of heavy metals in municipal solid waste (MSW) incinerator air pollution control (APC) residue. The results indicated that for extraction with distilled water, the heavy metal leaching concentration (mg/l) decreased with L/S ratio, but the amount of heavy metal released (AHMR), defined as the leached amount of heavy metals to the weight of the tested sample (mg/kg), increased with an increase in L/S ratio, in the range of 2-100. The results also showed that both the leaching concentration and the amount of released metals were strongly pH-dependent in the TCLP and modified TCLP tests. In the case of pHs lower than 6.5, the leaching concentrations of Cd, Pb, Cu, Zn, and Cr decreased with an increase in pH. As pH increased higher than 6.5, Cr and Zn were almost insoluble. Meanwhile, Cd and Cu also showed a similar trend but at pHs of 8.5 and 7.5, respectively. Due to the nature of amphoteric elements, in the case of pHs higher than 7, the Pb leaching concentration increased with increasing pH. In modified TCLP tests with the pH value controlled at the same level as in the SCE test, the heavy metal speciation approached the extractable carbonate bound fraction by the SCE. Both amounts of targeted metals leached from the SCE and modified TCLP tests were much higher than those for the regular TCLP and water extraction tests.     

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.     

The influence of mix parameters and binder choice on the carbonation of cement solidified wastes

This paper explores the kinetics of carbonation of cement-based solidified hazardous waste. This study is part of a wide investigation into the effects of carbonation on solidified waste forms. Two commercially produced heavy metal wastes were solidified with three different types of Portland cement and two mineral admixtures and carbonated under controlled conditions. Measurements of the uptake of carbon dioxide were made for the different mixes and areas showing the degree of carbonation for each cement system were defined. The effects of water/binder ratio, waste and binder type on both total uptake of carbon dioxide and rate of carbonation were investigated and are discussed.     

Changes in mineralogical and leaching properties of converter steel slag resulting from accelerated carbonation at low CO2 pressure

Steel slag can be applied as substitute for natural aggregates in construction applications. The material imposes a high pH (typically 12.5) and low redox potential (Eh), which may lead to environmental problems in specific application scenarios. The aim of this study is to investigate the potential of accelerated steel slag carbonation, at relatively low pCO₂ pressure (0.2 bar), to improve the environmental pH and the leaching properties of steel slag, with specific focus on the leaching of vanadium. Carbonation experiments are performed in laboratory columns with steel slag under water-saturated and -unsaturated conditions and temperatures between 5 and 90 °C. Two types of steel slag are tested; free lime containing (K3) slag and K1 slag with a very low free lime content. The fresh and carbonated slag samples are investigated using a combination of leaching experiments, geochemical modelling of leaching mechanisms and microscopic/mineralogical analysis, in order to identify the major processes that control the slag pH and resulting V leaching. The major changes in the amount of sequestered CO₂ and the resulting pH reduction occurred within 24 h, the free lime containing slag (K3-slag) being more prone to carbonation than the slag with lower free lime content (K1-slag). While carbonation at these conditions was found to occur predominantly at the surface of the slag grains, the formation of cracks was observed in carbonated K3 slag, suggesting that free lime in the interior of slag grains had also reacted. The pH of the K3 slag (originally pH ± 12.5) was reduced by about 1.5 units, while the K1 slag showed a smaller decrease in pH from about 11.7 to 11.1. However, the pH reduction after carbonation of the K3 slag was observed to lead to an increased V-leaching. Vanadium leaching from the K1 slag resulted in levels above the limit values of the Dutch Soil Quality Decree, for both the untreated and carbonated slag. V-leaching from the carbonated K3 slag remained below these limit values at the relatively high pH that remained after carbonation. The V-bearing di-Ca silicate (C2S) phase has been identified as the major source of the V-leaching. It is shown that the dissolution of this mineral is limited in fresh steel slag, but strongly enhanced by carbonation, which causes the observed enhanced release of V from the K3 slag. The obtained insights in the mineral transformation reactions and their effect on pH and V-leaching provide guidance for further improvement of an accelerated carbonation technology.     

Changes in constituent equilibrium leaching and pore water characteristics of a Portland cement mortar as a result of carbonation

Two equilibrium-based characterization protocols were applied to ground samples of a cement-based material containing metal oxide powders in both noncarbonated and carbonated states. The effects of carbonation were shown through comparison of (i) material buffering capacity, (ii) constituent equilibrium as a function of leachate pH, and (iii) constituent solubility and release as a function of liquid-to-solid (LS) ratio. As expected, the material alkalinity was significantly neutralized during carbonation. In addition, carbonation of the cement material led to the formation of calcium carbonate and a corresponding increase in arsenic release across the entire pH range. The solubility as a function of pH for lead and copper was lower in the alkaline pH range (pH>9) for carbonated samples compared with the parent material. When solubility and release as a function of LS ratio was compared, carbonation was observed to decrease calcium solubility, sodium and potassium release, and ionic strength. In response to carbonate solid formation, chloride and sulfate release as a function of LS ratio was observed to increase. Trends in constituent concentration as a function of LS ratio were extrapolated to estimate pore water composition at a 0.06 mL/g LS ratio. Significant differences were observed upon comparison of estimated pore water composition to leachate concentrations extracted at LS ratio of 5 mL/g. These differences show that practical laboratory extractions cannot be assumed directly representative of pore water concentrations.     

Life cycle assessment of biogas upgrading technologies

This article evaluates the life cycle assessment (LCA) of three biogas upgrading technologies. An in-depth study and evaluation was conducted on high pressure water scrubbing (HPWS), as well as alkaline with regeneration (AwR) and bottom ash upgrading (BABIU), which additionally offer carbon storage. AwR and BABIU are two novel technologies that utilize waste from municipal solid waste incinerators - namely bottom ash (BA) and air pollution control residues (APC) - and are able to store CO(2) from biogas through accelerated carbonation processes. These are compared to high pressure water scrubbing (HPWS) which is a widely used technology in Europe. The AwR uses an alkaline solution to remove the CO(2) and then the solution - rich in carbonate and bicarbonate ions - is regenerated through carbonation of APC. The BABIU process directly exposes the gas to the BA to remove and immediately store the CO(2), again by carbonation. It was determined that the AwR process had an 84% higher impact in all LCA categories largely due to the energy intensive production of the alkaline reactants. The BABIU process had the lowest impact in most categories even when compared to five other CO(2) capture technologies on the market. AwR and BABIU have a particularly low impact in the global warming potential category as a result of the immediate storage of the CO(2). For AwR, it was determined that using NaOH instead of KOH improves its environmental performance by 34%. For the BABIU process the use of renewable energies would improve its impact since accounts for 55% of the impact.     

Characterization of a mineral waste resulting from the melting treatment of air pollution control residues

Air pollution control (APC) residues which are generated by municipal solid waste (MSW) incineration show a high-level of pollution potential. In order to stabilize such APC residues, the French power supply company (EDF) is developing a thermal treatment process which leads to the production of a vitrified material. A structural characterization of the vitrified product was carried out by applying complementary investigation methods: XRD, SEM, Raman spectroscopy, EPMA, and data interpretation methods such as mineralogical analysis and principal component analysis (PCA). The major phase of the material was a solid solution of melilite type composed of five end-members: gehlenite (44%), åkermanite (25%), ferri-gehlenite (5%), sodamelilite (14%) and hardystonite (11%). The minor phases identified were spinels and pyroxenes.An ANC leaching test was performed in order to observe the treatment effect on pollutant release. The natural pH was close to 10, and the major element release was less than in the case of untreated APC. This was a consequence of melilite formation. The effect of pH was fundamental for heavy metals release: lower solubilization occurs at pH 10 than at APC’s natural pH (11–12).     

Solidification/stabilisation of air pollution control residues using Portland cement: Physical properties and chloride leaching

Portland cement (CEMI) was used to solidify air pollution control (APC) residues from an energy-from-waste plant burning municipal solid waste. APC residue/CEMI mixes were prepared with CEMI additions ranging from 0 to 50 weight% (wt%) of total dry mass and water/solids ratios between 0.40 and 0.80. Isothermal conduction calorimetry was used to assess the effect of APC residues on the hydration of CEMI. Although up to 30wt% additions of APC residues accelerated CEMI hydration, the total heat of hydration during the initial 98h was significantly reduced. Higher levels of APC residues severely inhibited CEMI hydration. The consistence, setting time, compressive strength, porosity and chloride leaching characteristics of the solidified products were determined. As might be expected, increasing the CEMI addition and reducing the water content resulted in increased compressive strengths. All mixes achieved compressive strengths greater than 1MPa at 7 and 28days but only 50wt% samples did not show significant strength reduction when tested after immersion in water. Monolithic leaching tests indicated low physical immobilisation of chloride in the CEMI solidified APC residues, with chloride leaching in excess of relevant UK landfill waste acceptance criteria (WAC). The results of this study show that greater than 50% CEMI additions would be required to effectively treat APC residues to meet current WAC limits.