The leaching characteristics of Cl−, SO42−, Na, K, Al, Si, Ca, Mg, Ba, Cd, Co, Cr, Cu, Mn, Mo, Ni, Pb, Sb, Se, Sr, Tl, V, Zn from fly ash and metakaolin geopolymer mortars were characterized in a ...broad pH range (1–14) in this work. Apart from revealing the partitioning of chemical species between the solid and aqueous phase, the acid neutralization property of both geopolymers were studied. In contrast with the virtually pH independent characteristic of chloride and sulfate, the leaching of the other elements showed pH dependent features, which can be further divided into amphoteric, cationic and oxyanionic patterns. Formation of montmorillonite and amorphous silica were detected by X-ray diffraction after the leaching. The leaching results and mineralogical measurement were coupled with geochemical modelling to identify the solubility controlling phases of Al, Si, Ca and Mg.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
•First LEAF leaching study on US sources of concrete materials containing fly ash.•pH-dependent leaching from concrete/microconcrete with and without fly ash.•Cement chemistry controls pH-dependent ...Sb, As, B, Cr, and Se concentrations.•Microconcretes (no coarse aggregate) can be conservative concrete surrogates.•Screening indicates insignificant impact for up to 45% fly ash replacement.
Current concerns about the environmental safety of coal combustion fly ash have motivated this evaluation of the impact of fly ash use as a cement replacement in concrete materials on the leaching of constituents of potential concern. The chemical effects of fly ash on leaching were determined through characterization of liquid–solid partitioning using EPA Method 1313 for four fly ash materials as well as concrete and microconcrete materials containing 0% (control materials), 25% and 45% replacement of portland cement with the fly ash source. All source materials, concrete formulations and replacement levels are representative of US concrete industry practices. Eluate concentrations as a function of pH were compared to a broader range of available testing results for international concretes and mortars for which the leaching characteristics of the component fly ashes were unknown. The chemistry of the hydrated cement fraction was found to dominate the liquid–solid partitioning resulting in reduced leaching concentrations of most trace metals compared to concentrations from fly ash materials alone. Compared to controls, eluate concentrations of Sb, As, B, Cr, Mo, Se, Tl and V from concrete products containing fly ash were essentially the same as the eluate concentrations from control materials produced without fly ash replacement indicating little to no significant impact on aqueous partitioning.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Leaching assessment procedures have been used to determine the leachability of heavy metals as input for evaluating the risk from sewage sludge compost land application. However, relatively little ...attention has been paid to understanding leaching from soils with repeated application of sewage sludge compost with elevated levels of heavy metals. In this paper, leaching assessment is extended to evaluate the potential leaching of heavy metals during repetitive application of composted sewage sludge to soils. Four cycling of compost additions and percolation leaching were conducted to investigate how leaching behavior of heavy metals changed with repeated additions of compost. Results showed that repetitive additions of compost to soil significantly increased the content of organic matter, which favored the formation of reducing condition due to improved microbial activities and oxygen consumption. Establishment of reducing conditions can enhance the leaching concentrations of As by approximately 1 order of magnitude, especially for the soil rich in organic matter. For Cd, Cr, Cu, and Pb, repeated additions of compost will cause accumulation in total contents but not enhancement in leaching concentrations. The infiltration following compost additions will leach out the mobile fraction and the residual fraction might not release in the next cycling of compost addition and infiltration. The cumulative release of Cd, Cr, Cu, and Pb accounted for less than 5% of the total contents during four times of compost applications.
•Leaching of heavy metals during repetitive land application of SSC was evaluated.•Percolation and pH-dependent leaching test were used to understand the leaching behavior.•Repeated additions of SSC favored the formation of reducing condition.•Establishment of reducing conditions can enhance the release of accumulated As.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
In the present study, the metal leaching from recycled concrete aggregates (RCA) used in road sub-base is presented after >10years of exposure. The released levels of inorganic constituents, the ...effect of small variation of pH and the use of de-icing salt during winter season were studied. In addition, speciation modelling for the major elements has been provided. The pH varied from 7.5 to 8.5 for the sub-base constructed with RCA whereas the pH of around 8 was obtained for the test section not affected by the traffic and de-icing salts. Despite a small variation in pH, the leachability of Al, Ca and Mg was found to be strongly dependent on pH and fair agreement between the measured and predicted concentrations was obtained. The speciation modelling indicated that gibbsite, calcite and magnesite controlled the solubility of Al, Ca and Mg, respectively, which was in agreement with the expected carbonation products. Due to the larger pH fluctuations in the test sections exposed to the road traffic, increased concentrations were observed for the oxyanions. The same effect was not seen for the trace metal cations Cd, Cu, Ni, Pb and Zn. The distinct pH dependent leaching profile (solubility maximum in the mildly basic pH region) for vanadium could be seen after 10years of exposure. The simplified risk assessment showed that the released quantities did not exceed the chosen acceptance criteria for groundwater and fresh water. The results obtained for the test section not influenced by road dust and de-icing salts, complied with these criteria even without considering any dilution effects caused by the mixing of pore water with groundwater.
•Leaching from crushed concrete applied as road sub-base has been assessed after >10years exposure.•Calcite, gibbsite and magnesite were identified as solubility controlling phases by geochemical modelling.•These simulated mineral phases were in agreement with the expected degradation products from the carbonation process.•When field pH changed from 7.4–8.5, leaching of V increased more than one order of magnitude.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
In this paper, the leaching behaviour of major components (Al, Ca, SO
4, Mg, Si, Fe, Na and DOC) and trace elements (Ni, Zn, Cd, Cu, Pb, Mo and Sb) from MSWI bottom ash is studied as a function of ...time over a wide range of pH, under pH-controlled conditions. Equilibrium geochemical modelling using the modelling framework ORCHESTRA is used to enable a process-based interpretation of the results and to investigate whether ‘equilibrium’ is attained during the time scale of the experiments. Depending on the element and setpoint-pH value, net concentration increases or decreases of up to one order of magnitude were observed. Different concentration–time trends (increase or decrease) are observed in different pH ranges. The direction of the concentration–time trends depends on: (1) the shape of the ‘equilibrium’ solubility curve, and (2) the position of the setpoint-pH in the leaching test relative to the natural pH of the sample. Although the majority of the elements do not reach steady state, leached concentrations over a wide pH range have been shown to closely approach ‘equilibrium’ model curves within an equilibration time of 168
h. The different effects that leaching kinetics may have on the pH dependent leaching patterns have been identified for a wide range of elements, and can generally be explained in a mechanistic way. The results are in support of the currently prescribed equilibration time of 48
h in the European standard for the pH-static leaching test (TS14997). Finally, this study demonstrates that pH-static leaching experiments such as described in the European standards (TS14497 and TS14429), in combination with selective chemical extractions and a mechanistically based modelling approach, constitute a powerful set of tools for the characterization of leaching processes in waste materials over a wide range of conditions.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
This paper provides an improved understanding of the leaching behavior of waste incineration air-pollution-control (APC) residues in a long-term perspective. Leaching was investigated by a series of ...batch experiments reflecting leaching conditions after initial washout of highly soluble salts from residues. Leaching experiments were performed at a range of pH-values using carbonated and noncarbonated versions of two APC residues. The leaching data were evaluated by geochemical speciation modeling and discussed with respect to possible solubility control. The leaching of major elements as well as trace elements was generally found to be strongly dependent on pH. As leaching characterization was performed in the absence of high salt levels, the presented results represent long-term leaching after initial washout from a disposal site, that is, liquid-to-solid ratios above 1−2 L/kg. The leaching of Al, Ba, Ca, Cr, Pb, S, Si, V, and Zn was found influenced by solubility control from Al2O3, Al(OH)3, Ba(S,Cr)O4 solid solutions, BaSO4, Ca6Al2(SO4)3(OH)12·26H2O, CaAl2Si4O12·2H2O, Ca(OH)2, CaSiO3, CaSO4·2H2O, CaZn2(OH)6·2H2O, KAlSi2O6, PbCO3, PbCrO4, Pb2O3, Pb2V2O7, Pb3(VO4)2, ZnO, Zn2SiO4, and ZnSiO3. The presented dataset and modeling results form a thorough contribution to the assessment of long-term leaching behavior of APC residues under a wide range of conditions.
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IJS, KILJ, NUK, PNG, UL, UM
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•Low liquid-to-solid test (0.3–1 L/kg) described As, B, Mo, and V release to porewater.•Field leaching mechanisms are inferred using geochemical speciation modeling.•Carbonates and ...ettringite in weathered impoundment ash immobilized B, Mo, and V.•Ca-bearing minerals controlled concentrations of As and V in porewater (0.01–1 mg/L)•Field suboxic (pe 0–4) and alkaline conditions (pH 9–11) inhibited Cr and Se leaching.
Field monitoring combined with laboratory leaching characterization and geochemical speciation modeling were used to identify important geochemical parameters and controlling mechanisms for leaching of oxyanions from coal ash in a disposal site. The site consisted of dry stacked ash on top of a former surface impoundment. Constituents leached from the dry stacked ash served as sources for the soluble fractions of constituents in underlying impoundment ash. Weathering of field ash was evidenced by the identification of calcite and ettringite. Porewater concentrations of As, B, and V in the field pH range (9–11) and liquid-to-solid ratio (L/S) condition (∼0.6 L/kg-dry) were primarily controlled by Ca-bearing precipitates (Ca-arsenate, B-substituted carbonate solid solution, Ca-vanadate, and V-substituted ettringite solid solution). The leachable fraction of Mo as a function of pH was limited by the available content in the solid, with aqueous concentrations of Mo being a function of L/S. Leaching behavior of Cr and Se was sensitive to the redox changes (from suboxic to oxic conditions) during field ash collection and laboratory leaching tests, including oxidative dissolution of insoluble Cr(III)-oxides and conversion of Se(0) in the solid to dissolved Se(IV)/Se(VI). Oxidation resulted in increased Cr concentrations from < 0.00005 (in porewater) to 0.001–0.1 mg/L (in laboratory eluates). The identified geochemical parameters and leaching-controlling mechanisms provide the bases for understanding and estimating the partitioning of oxyanions in other disposal sites with alkaline and suboxic conditions. This case study also provides a typical example of laboratory test results interpretation and field leaching behavior estimation for other studies.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The release of major and trace elements from recycled concrete aggregates used in an asphalt covered road sub-base has been monitored for more than 4years. A similar test field without an asphalt ...cover, directly exposed to air and rain, and an asphalt covered reference field with natural aggregates in the sub-base were also included in the study. It was found that the pH of the infiltration water from the road sub-base with asphalt covered concrete aggregates decreased from 12.6 to below pH 10 after 2.5years of exposure, whereas this pH was reached within only one year for the uncovered field. Vertical temperature profiles established for the sub-base, could explain the measured infiltration during parts of the winter season. When the release of major and trace elements as function of field pH was compared with pH dependent release data measured in the laboratory, some similar pH trends were found. The field concentrations of Cd, Ni, Pb and Zn were found to be low throughout the monitoring period. During two of the winter seasons, a concentration increase of Cr and Mo was observed, possibly due to the use of de-icing salt. The concentrations of the trace constituents did not exceed Norwegian acceptance criteria for ground water and surface water Class II.
► An extensive field work was carried out to study the potential leaching from a road sub-base constructed with crushed concrete. ► Field pH development as a function of time was established. ► Leaching as function of field pH was compared to laboratory data and for some elements a correlation was found. ► The presence of de-icing salt may influence constituents that readily form oxyanions (e.g. CrO42−). ► Risk assessment was carried out and the released concentrations were found to be acceptable.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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•Variations in chemical composition have an effect on the slag mineralogy.•The leaching of ladle slag is governed by surface phenomena.•Variations in cooling treatment and steel type ...have a small effect on leachability.•The solubility-controlling minerals were predicted by geochemical modelling.•Mineralogical identification of the solubility-controlling minerals (Ca(OH)2, CSH).
In this study, the leachability of freshly produced ladle slag derived from both austenitic and ferritic stainless steel production, and from electrical and structural steel production, was investigated, in order to determine whether variations in the chemical and mineralogical composition of these slags affect their leaching behaviour. The effect of the method used for slag cooling was also studied. The results obtained by using the single batch test were combined with those obtained by means of more sophisticated characterisation leaching tests, which, in combination with geochemical speciation modelling, helped to better identify the release mechanisms and phases that control the release of individual elements. It was found that, although variations in the chemical composition of the slag can affect the slag's minerology, neither such variations, nor the choice of the slag cooling treatment, have a significant effect on the leachability of individual elements, since the leaching is governed by surface phenomena. In fact, the mineral transformations on the slag surface, rather than the bulk mineral composition, dictate the release of these elements from the ladle slag. The solubility-controlling phases were predicted by multi-element modelling, and verified to the extent made possible by the performed mineralogical investigations.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Cast Stone is a cementitious waste form being considered for the solidification of low activity waste at the DOE Hanford Site. Under near-surface disposal conditions in an arid environment, Cast ...Stone is subject to drying and carbonation which may impact retention of waste constituents. This study investigates the effects of environmental CO2 concentration and relative humidity (RH) on the carbonation of Cast Stone. The rate of carbonation front ingress and the extent of carbonation reaction were characterized for samples aged up to 48 weeks at three RH levels and two CO2 concentrations. While the 68% RH environment allowed the greatest reaction extent, the 15% RH environment yielded the deepest carbonation front ingress. At 68% RH, there was a linear relationship between the ingress rate and CO2 concentration. Carbonation reactions increased the drying rate of Cast Stone. Redistribution of sodium toward the wetting front was observed under drying and carbonation conditions.
•In disposal scenarios, Cast Stone waste forms may age by drying and carbonation.•Carbonation ingress rate is linear with CO2 and increased in drying environments.•The extent of carbonation reaction is greatest under intermediate relative humidity.•Drying is increased in carbonated matrices due porosity and moisture changes.•Capillary water movement leads to redistribution of sodium salts.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
