- Centre for Environmental and Marine Sciences,
University of Hull,
Scarborough
YO11 3AZ
UK
- Water Pollution, Environmental Remediation, Water, Hydrology, Wetlands, Water quality, and 14 moreAcid Mine Drainage, Heavy Metal Pollution, Mine Water, Vanadium, Environmental Science, Water resources, Disaster Studies, Red Mud, Diffuse pollution, Biology, Ecology, Ajka Spill 2010 Hungary Vanadium, Weathering of Steel Slag, and Groundwater Qualityedit
- I joined the Centre for Environmental and Marine Sciences at the University of Hull in September 2009 from Newcastle ... moreI joined the Centre for Environmental and Marine Sciences at the University of Hull in September 2009 from Newcastle University where I obtained his PhD and spent six years as a post-doctoral researcher. My research to date has traversed a range of disciplines and scales, from catchment-scale hydrological processes to aquatic geochemistry through to laboratory-based development of novel remedial tools for inorganic pollutants. My main current research interests are:
- Characterization and remediation of hyperalkaine industrial drainage (e.g. steel slag, lime works and red mud leachate)
- Monitoring and remediation of pollutants from abandoned minesedit
<p>The production of iron and steel has generated substantial volumes of slag as waste, with estimates of up to 384 million tonnes (Mt) of iron slag and 280 Mt of steel slag produced globally, to date. Whilst the... more
<p>The production of iron and steel has generated substantial volumes of slag as waste, with estimates of up to 384 million tonnes (Mt) of iron slag and 280 Mt of steel slag produced globally, to date. Whilst the majority of these by-products (approximately 70 %) have seen bulk re-use in a number of applications (e.g. as ballast in construction applications), a significant volume of slag has been disposed of in environmental settings, where the release of metal-rich alkaline leachates can cause enduring pollution. However, the mineralogical and physical properties of slags also offer opportunity for environmental benefits, namely; through sequestration of atmospheric carbon dioxide, by acting as stockpiles of critical raw materials, and in certain situations performing as incidental coastal defences.</p><p>Findings are presented from national-scale field investigations, laboratory experiments, and spatial data analyses, which aim to explore the resource potential of iron and steel slags in the United Kingdom (UK). Within the 236 Mt of slags disposed of in the UK environment, projected carbonation rates revealed a potential for uptake of 138 Mt CO<sub>2 </sub>under enhanced weathering conditions. Notable masses of technologically-critical elements were also estimated within UK slags, with reserves in the region of 1.55 Mt of V<sub>2</sub>O<sub>5</sub>, 1.58 Mt of TiO<sub>2</sub>, and 1.26 Mt of Cr<sub>2</sub>O<sub>3</sub> estimated. Further to acting as a resource, in areas of coastal deposition, slag banks were observed to offer tidal protection. At a number of sites this allowed the development of nationally-significant ecological communities, whilst laboratory leaching experiments reveal a very low risk of chemical leaching in saline conditions. The integration of spatial analyses with chemical composition and leaching data can help to inform decisions on maximising resource potential whilst minimising the potential environmental risks associated with slag reworking.</p>
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ABSTRACT The flux of metals at the tidal limits of major rivers are an important metric of freshwater contaminant transfer to marine habitats, reported in Northeast Atlantic bordering countries under the 1992 Oslo-Paris (OSPAR)... more
ABSTRACT The flux of metals at the tidal limits of major rivers are an important metric of freshwater contaminant transfer to marine habitats, reported in Northeast Atlantic bordering countries under the 1992 Oslo-Paris (OSPAR) Convention. This paper presents an assessment of long-term OSPAR data for four trace metals (Cd, Cu, Pb, and Zn) using a range of spatial datasets to assess the broad distribution of metal flux and yield across England and Wales. Mine site records and geological and land use data are used to classify river basins into six classes. The bulk of metal flux to seas around England and Wales occurs from catchments containing extensive mineralization and a legacy of metal mining (52 % of the total Zn flux, 47 % of Pb, 39 % of Cu, and 48 % of Cd were associated with mined catchments). Catchment area, metal flux from point mine discharges at source, and extent of mineralization typically accounted most for variation in catchment outlet metal flux in stepwise multiple linear regression (SMLR). There are a number of small mining-impacted rural catchments contributing significant fluxes of metals to coastal waters. Of particular prominence are Restronguet Creek (drainage area 87 km2) in southwest England that discharges 176 t Zn/year and 18 t Cu/year and the Afon Goch Dulas (27 km2) in north Wales, which releases 20 t Zn/year and 9 t Cu/year. Although such exercises cannot directly determine the provenance of metals, comparison with metal release data and a review of catchment-scale studies suggest a critical role of mining-related contaminants in contributing to catchment metal export.
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Priorities for the exploration of Mars involve the identification and observation of biosignatures that indicate the existence of life on the planet. The atmosphere and composition of the sediments on Mars suggest suitability for... more
Priorities for the exploration of Mars involve the identification and observation of biosignatures that indicate the existence of life on the planet. The atmosphere and composition of the sediments on Mars suggest suitability for anaerobic chemolithotrophic metabolism. Carbonates are often considered as morphological biosignatures, such as stromatolites, but have not been considered as potential electron acceptors. Within the present study, hydrogenotrophic methanogen enrichments were generated from sediments that had received significant quantities of lime from industrial processes (lime kiln/steel production). These enrichments were then supplemented with calcium carbonate powder or marble chips as a sole source of carbon. These microcosms saw a release of inorganic carbon into the liquid phase, which was subsequently removed, resulting in the generation of methane, with 0.37 ± 0.09 mmoles of methane observed in the steel sediment enrichments supplemented with calcium carbonate po...
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A cement-based geological disposal facility (GDF) is one potential option for the disposal of intermediate level radioactive wastes. The presence of both organic and metallic materials within a GDF provides the opportunity for both... more
A cement-based geological disposal facility (GDF) is one potential option for the disposal of intermediate level radioactive wastes. The presence of both organic and metallic materials within a GDF provides the opportunity for both acetoclastic and hydrogenotrophic methanogenesis. However, for these processes to proceed, they need to adapt to the alkaline environment generated by the cementitious materials employed in backfilling and construction. Within the present study, a range of alkaline and neutral pH sediments were investigated to determine the upper pH limit and the preferred route of methane generation. In all cases, the acetoclastic route did not proceed above pH 9.0, and the hydrogenotrophic route dominated methane generation under alkaline conditions. In some alkaline sediments, acetate metabolism was coupled to hydrogenotrophic methanogenesis via syntrophic acetate oxidation, which was confirmed through inhibition studies employing fluoromethane. The absence of acetocla...
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Steel slag is a major by-product of the steel industry and a potential resource of technology critical elements. For this study, a basic oxygen furnace (BOF) steel slag was tested for bacterial leaching and recovery of aluminium (Al),... more
Steel slag is a major by-product of the steel industry and a potential resource of technology critical elements. For this study, a basic oxygen furnace (BOF) steel slag was tested for bacterial leaching and recovery of aluminium (Al), chromium (Cr), and vanadium (V). Mixed acidophilic bacteria were adapted to the steel slag up to 5% (w/v). In the batch tests, Al, Cr, and V were bioleached significantly more from steel slag than in control treatments. No statistical difference was observed arising from the duration of the leaching (3 vs 6 d) in the batch tests. Al and Cr concentrations in the leachate were higher for the smaller particle size of the steel slag (<75 μm), but no difference was observed for V. In the column tests, no statistical difference was found for pH, Al, Cr and V between the live culture (one-step bioleaching) and the supernatant (two-step bioleaching). The results show that the culture supernatant can be effectively used in an upscaled industrial application ...
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Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined... more
Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined atmospheric carbon dioxide sequestration in a >20 million ton legacy slag deposit in northern England, United Kingdom. Carbonates formed from the drainage water of the heap had stable carbon and oxygen isotope values between -12 and -25 ‰ and -5 and -18 ‰ for δC and δO, respectively, suggesting atmospheric carbon dioxide sequestration in high-pH solutions. From the analyses of solution saturation states, we estimate that between 280 and 2900 tons of CO have precipitated from the drainage waters. However, by combining a 37 year long data set of the drainage water chemistry with geospatial analysis, we estimate that <1% of the maximum carbon-capture potential of the deposit may have been realized. This implies that uncontrolled deposition of slag i...
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Alkalinity generation and toxic trace metal (such as vanadium) leaching from basic oxygen furnace (BOF) steel slag particles must be properly understood and managed by pre-conditioning if beneficial reuse of slag is to be maximised. Water... more
Alkalinity generation and toxic trace metal (such as vanadium) leaching from basic oxygen furnace (BOF) steel slag particles must be properly understood and managed by pre-conditioning if beneficial reuse of slag is to be maximised. Water leaching under aerated conditions was investigated using fresh BOF slag at three different particle sizes (0.5-1.0, 2-5 and 10 × 10 × 20 mm blocks) and a 6-month pre-weathered block. There were several distinct leaching stages observed over time associated with different phases controlling the solution chemistry: (1) free-lime (CaO) dissolution (days 0-2); (2) dicalcium silicate (Ca2SiO4) dissolution (days 2-14) and (3) Ca-Si-H and CaCO3 formation and subsequent dissolution (days 14-73). Experiments with the smallest size fraction resulted in the highest Ca, Si and V concentrations, highlighting the role of surface area in controlling initial leaching. After ~2 weeks, the solution Ca/Si ratio (0.7-0.9) evolved to equal those found within a Ca-Si-H ...
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Bauxite residue is a high volume byproduct of alumina manufacture which is commonly disposed of in purpose-built bauxite residue disposal areas (BRDAs). Natural waters interacting with bauxite residue are characteristically highly... more
Bauxite residue is a high volume byproduct of alumina manufacture which is commonly disposed of in purpose-built bauxite residue disposal areas (BRDAs). Natural waters interacting with bauxite residue are characteristically highly alkaline, and have elevated concentrations of Na, Al, and other trace metals. Rehabilitation of BRDAs is therefore often costly and resource/infrastructure intensive. Data is presented from three neighboring plots of bauxite residue that was deposited 20 years ago. One plot was amended 16 years ago with process sand, organic matter, gypsum, and seeded (fully treated), another plot was amended 16 years ago with process sand, organic matter, and seeded (partially treated), and a third plot was left untreated. These surface treatments lower alkalinity and salinity, and thus produce a substrate more suitable for biological colonisation from seeding. The reduction of pH leads to much lower Al, V, and As mobility in the actively treated residue and the beneficia...
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Basic oxygen furnace (BOF) steelmaking slag is enriched in potentially toxic V which may become mobilized in high pH leachate during weathering. BOF slag was weathered under aerated and air-excluded conditions for 6 months prior to... more
Basic oxygen furnace (BOF) steelmaking slag is enriched in potentially toxic V which may become mobilized in high pH leachate during weathering. BOF slag was weathered under aerated and air-excluded conditions for 6 months prior to SEM/EDS and μXANES analysis to determine V host phases and speciation in both primary and secondary phases. Leached blocks show development of an altered region in which free lime and dicalcium silicate phases were absent and Ca-Si-H was precipitated (CaCO3 was also present under aerated conditions). μXANES analyses show that V was released to solution as V(V) during dicalcium silicate dissolution and some V was incorporated into neo-formed Ca-Si-H. Higher V concentrations were observed in leachate under aerated conditions than in the air-excluded leaching experiment. Aqueous V concentrations were controlled by Ca3(VO4)2 solubility, which demonstrate an inverse relationship between Ca and V concentrations. Under air-excluded conditions Ca concentrations w...
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The management of alkaline (pH11-12.5) leachate is an important issue associated with the conditioning, afteruse or disposal of steel slags. Passive in-gassing of atmospheric CO2 is a low cost option for reducing Ca(OH)2 alkalinity, as... more
The management of alkaline (pH11-12.5) leachate is an important issue associated with the conditioning, afteruse or disposal of steel slags. Passive in-gassing of atmospheric CO2 is a low cost option for reducing Ca(OH)2 alkalinity, as Ca(OH)2 is neutralised by carbonic acid to produce CaCO3. The relative effectiveness of such treatment can be affected by both the system geometry (i.e. stepped cascades versus settlement ponds) and biological colonization. Sterilized mesocosm experiments run over periods of 20days showed that, due to more water mixing and enhanced CO2 dissolution at the weirs, the cascade systems (pH11.2→9.6) are more effective than settlement ponds (pH11.2→11.0) for lowering leachate alkalinity in all the tested conditions. The presence of an active microbial biofilm resulted in significantly more pH reduction in ponds (pH11.2→9.5), but had a small impact on the cascade systems (pH11.2→9.4). The pH variation in biofilm colonized systems shows a diurnal cycle of 1 to...
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Leachable vanadium (V) from steel production residues poses a potential environmental hazard due to its mobility and toxicity under the highly alkaline pH conditions that characterise these leachates. This work aims to test the efficiency... more
Leachable vanadium (V) from steel production residues poses a potential environmental hazard due to its mobility and toxicity under the highly alkaline pH conditions that characterise these leachates. This work aims to test the efficiency of anion exchange resins for vanadium removal and recovery from steel slag leachates at a representative average pH of 11.5. Kinetic studies were performed to understand the vanadium sorption process. The sorption kinetics were consistent with a pseudo-first order kinetic model. The isotherm data cannot differentiate between the Langmuir and Freundlich models. The maximum adsorption capacity (Langmuir value qmax) was 27 mg V g(-1) resin. In column anion exchange, breakthrough was only 14% of the influent concentration after passing 90 L of steel slag leachate with 2 mg L(-1) V through the column. When eluting the column 57-72% of vanadium was recovered from the resin with 2 M NaOH. Trials on the reuse of the anion exchange resin showed it could be ...
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Bauxite residue is an important by-product of the alumina industry, and current management practices do not allow their full valorisation, especially with regard to the recovery of critical metals. This work aims to test the efficiency of... more
Bauxite residue is an important by-product of the alumina industry, and current management practices do not allow their full valorisation, especially with regard to the recovery of critical metals. This work aims to test the efficiency of ion exchange resins for vanadium (V) removal and recovery from bauxite residue leachates at alkaline pH (11.5 and 13). As an environmental pollutant, removal of V from leachates may be an obligation of bauxite residue disposal areas (BRDA) long-term management requirements. Vanadium removal from the leachate can be coupled with the recovery, and potentially can be used to offset long-term legacy treatment costs in legacy sites. Kinetics studies were performed to understand the adsorption process. The rate kinetics for the V adsorption was consistent with the pseudo-first-order kinetic model, with a higher adsorption rate for pH 11.5 (1.2 min(-1)). Adsorption isotherm data fitted better to Freundlich equations than to the Langmuir model. The maximum...
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The disposal of slag generated by the steel industry can have negative consequences upon the surrounding aquatic environment by the generation of high pH waters, leaching of potentially problematic trace metals, and rapid rates of calcite... more
The disposal of slag generated by the steel industry can have negative consequences upon the surrounding aquatic environment by the generation of high pH waters, leaching of potentially problematic trace metals, and rapid rates of calcite precipitation which smother benthic habitats. A 36-year dataset was collated from the long-term ambient monitoring of physicochemical parameters and elemental concentrations of samples from two steel slag leachate-affected watercourses in northern England. Waters were typified by elevated pH (>10), high alkalinity, and were rich in dissolved metals (e.g. calcium (Ca), aluminium (Al), and zinc (Zn)). Long-term trend analysis was performed upon pH, alkalinity, and Ca concentration which, in addition to Ca flux calculations, were used to highlight the longevity of pollution arising as a result of the dumping and subsequent leaching of steel slags. Declines in calcium and alkalinity have been modest over the monitoring period and not accompanied by ...
Research Interests: Environmental Science, Aquatic Chemistry, Environmental Monitoring, Waste Management, Water Pollution, and 13 moreMultidisciplinary, Time series analysis, England, Steel, Metals, Vanadium, Environmental monitoring and assessment, Alkaline Water, Time Factors, Industrial Waste, Calcium Carbonate, Environment, and Steel Slag
Research Interests: Environmental Science, Soil, Wetlands, Groundwater, Environmental Chemistry, and 14 moreWater Pollution, Soil Pollution, Biological Sciences, Environmental Sciences, Disasters, Copper, Hungary, Floods, Nickel, CHEMICAL SCIENCES, Red Mud, Aluminum oxide, Hydrogen-Ion Concentration, and Soil Pollutants
Rapid recovery of rivers contaminated by largest recorded release of red mud to the environment is apparent due to fine-grained nature of spill material and remedial efforts.
Research Interests: Environmental Science, Geology, Water quality, Environmental Monitoring, Rivers, and 14 moreEnvironmental Chemistry, Water Pollution, Environmental Pollution, Medicine, Earth and Environmental Sciences, Environmental Sciences, Hungary, Bauxite, Metals, CHEMICAL SCIENCES, Red Mud, Water Quality, Geologic Sediments, and Medical and Health Sciences
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Research Interests: Environmental Science, Geology, Geochemistry, Chemistry, Environmental Studies, and 10 moreArsenic, Environmental Chemistry, Water Pollution, Environmental Soil Science, Environmental Pollution, Environmental Aqueous Geochemistry, Applied Geochemistry, Bauxite, Red Mud, and ENVIRONMENTAL SCIENCE AND MANAGEMENT
ABSTRACT This study assesses the physical and chemical characteristics of hyperalkaline steel slag leachate from a former steelworks on two streams in England and their impacts on benthic invertebrate communities. Using multivariate... more
ABSTRACT This study assesses the physical and chemical characteristics of hyperalkaline steel slag leachate from a former steelworks on two streams in England and their impacts on benthic invertebrate communities. Using multivariate methods (CCA), we related invertebrate richness and diversity with chemical parameters along the environmental gradient from point sources to less impacted sites downstream. Point discharges are characterised by high pH (10.6–11.5), high ionic strength (dominated by Ca–CO3–OH waters), elevated trace elements (notably Li, Sr and V) and high rates of calcium carbonate precipitation. This combination of stressors gives rise to an impoverished benthic invertebrate community in source areas. The total abundance, taxonomic richness and densities of most observed organisms were strongly negatively correlated with water pH. Analysis using biological pollution monitoring indices (e.g. BMWP and Functional Feeding Groups) shows the system to be highly impacted at source, but when pH approaches values close to aquatic life standards, some 500 m downstream, complex biological communities become established. In addition to showing the rapid recovery of invertebrate communities downstream of the discharges, this study also provides a baseline characterisation of invertebrate communities at the extreme alkaline range of the pH spectrum.
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A number of emergency pollution management measures were enacted after the accidental release of caustic bauxite processing residue that occurred in Ajka, western Hungary in October, 2010. These centred on acid and gypsum dosing to reduce... more
A number of emergency pollution management measures were enacted after the accidental release of caustic bauxite processing residue that occurred in Ajka, western Hungary in October, 2010. These centred on acid and gypsum dosing to reduce pH and minimise mobility of oxyanion contaminants mobile at high pH. This study assessed the effectiveness of gypsum dosing on contaminant mobility and carbon sequestration through assessment of red mud and gypsum-affected fluvial sediments via elemental analysis and stable isotope analysis. There was a modest uptake of contaminants (notably As, Cr, and Mn) on secondary carbonate-dominated deposits in reaches subjected to gypsum dosing. C and O stable isotope ratios of carbonate precipitates formed as a result of gypsum dosing were used to quantify the importance of the neutralisation process in sequestering atmospheric carbon dioxide. This process was particularly pronounced at sites most affected by gypsum addition, where up to 36% of carbonate-C...
Research Interests: Environmental Engineering, Environmental Science, Geology, Hydrogeology, Chemistry, and 15 moreCarbon Sequestration, Disaster Management, Environmental Chemistry, Hazardous Waste, Disasters, Carbon dioxide removal, Hungary, Groundwater Quality, Bauxite, Chemical Industry, Industrial Waste, Elsevier, Carbonate Precipitation, Geologic Sediments, and Calcium Sulfate
An integrated assessment of biological activity and ecotoxicity of fluvial sediments in the Marcal river catchment (3078 km(2)), western Hungary, is presented following the accidental spill of bauxite processing residue (red mud) in Ajka.... more
An integrated assessment of biological activity and ecotoxicity of fluvial sediments in the Marcal river catchment (3078 km(2)), western Hungary, is presented following the accidental spill of bauxite processing residue (red mud) in Ajka. Red mud contaminated sediments are characterised by elevated pH, elevated trace element concentrations (e.g. As, Co, Cr, V), high exchangeable Na, and induce an adverse effect on test species across a range of trophic levels. While background contamination of the river system is highlighted by adverse effects on some test species at sites unaffected by red mud, the most pronounced toxic effects apparent in Vibrio fischeri bioluminescence inhibition, Lemna minor bioassay and Sinapis alba root and shoot growth occur at red mud depositional hotspots in the lower Torna Creek and upper Marcal. Heterocypris incongruens bioassays show no clear patterns, although the most red mud-rich sites do exert an adverse effect. Red mud does however appear to induce an increase in the density of aerobic and facultative anaerobic bacterial communities when compared with unaffected sediments and reference sites. Given the volume of material released in the spill, it is encouraging that the signal of the red mud on aquatic biota is visible at a relatively small number of sites. Gypsum-affected samples appear to induce an adverse effect in some bioassays (Sinapis alba and Heterocypris incongruens), which may be a feature of fine grain size, limited nutrient supply and greater availability of trace contaminants in the channel reaches that are subject to intense gypsum dosing. Implications for monitoring and management of the spill are discussed.
Research Interests: Environmental Science, Environmental Toxicology, Crustacea, Environmental Monitoring, Rivers, and 15 moreWater Pollution, Medicine, Environmental Sciences, Hungary, Animals, Plants, Groundwater Quality, Sediment, CHEMICAL SCIENCES, Industrial Waste, Aluminum oxide, Biological Assay, Geologic Sediments, Aliivibrio fischeri, and Medical and Health Sciences
Research Interests: Biochemistry, Environmental Science, Biophysics, Chemistry, Environmental Geology, and 15 moreDisaster Studies, Arsenic, Arsenic Contamination in Ground Water, Acid Mine Drainage, Ecology, Environmental Monitoring, Cell Biology, Disaster Response, Environmental Chemistry, Environmental science and technology, Analysis, Chromium, Cr, Aluminum oxide, and Arsenate
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Management of steel slag (a major by-product of the steel industry) includes the treatment of highly alkaline leachate (pH > 11.5) from rainwater infiltration of slag deposits to prevent adverse impact upon surface or ground waters. This... more
Management of steel slag (a major by-product of the steel industry) includes the treatment of highly alkaline leachate (pH > 11.5) from rainwater infiltration of slag deposits to prevent adverse impact upon surface or ground waters. This study aims to compare different treatment options for steel slag leachate through a life cycle assessment (LCA). Five options were compared: active treatment by acid dosing (A-H 2 SO 4), active treatment by carbon dioxide dosing (A-CO 2), active treatment by calcium chloride dosing (A-CaCl 2), passive treatment by cascade and reedbeds with pumping (P-P), and passive treatment by cascade and reedbeds in a gravity-driven configuration (P-G). The functional unit was 1 m 3 of treated leachate with pH < 9, considering 24 h and 365 days of operating, maintenance operations every year, and service life of 20 years. Inventory data were obtained from project designers, commercial suppliers, laboratory data and field tests. The environmental impacts were calculated in OpenLCA using the ELCD database and ILCD 2011 method, covering twelve impact categories. The A-CaCl 2 option scored worse than all other treatments for all considered environmental impact categories. Regarding human toxicity, A-CaCl 2 impact was 1260 times higher than the lowest impact option (A-CO 2) for carcinogenics and 53 times higher for non-carcinogenics (A-H 2 SO 4). For climate change, the lowest impact was calculated for P-G < P-P < A-H 2 SO 4 < A-CO 2 < A-CaCl 2 , while for particulate matter/respiratory inorganics, the options ranked as follows P-G < P-P < A-CO 2 < A-H 2 SO 4 < A-CaCl 2. The major contributor to these impact categories was the Solvay process to produce CaCl 2. Higher uncertainty was associated with the categories particulate matter formation, climate change and human toxicity, as they are driven by indirect emissions from electricity and chemicals production. Both passive treatment options had better environmental performance than the active treatment options. Potential design measures to enhance environmental performance of the treatments regarding metal removal and recovery are discussed and could inform operational management at active and legacy steel slag disposal sites.
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Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined... more
Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined atmospheric carbon dioxide sequestration in a >20 million ton legacy slag deposit in northern England, United Kingdom. Carbonates formed from the drainage water of the heap had stable carbon and oxygen isotope values between −12 and −25 ‰ and −5 and −18 ‰ for δ 13 C and δ 18 O, respectively, suggesting atmospheric carbon dioxide sequestration in high-pH solutions. From the analyses of solution saturation states, we estimate that between 280 and 2900 tons of CO 2 have precipitated from the drainage waters. However, by combining a 37 year long data set of the drainage water chemistry with geospatial analysis, we estimate that <1% of the maximum carbon-capture potential of the deposit may have been realized. This implies that uncontrolled deposition of slag is insufficient to maximize carbon sequestration, and there may be considerable quantities of unreacted legacy deposits available for atmospheric carbon sequestration.
Alkalinity generation and toxic trace metal (such as vanadium) leaching from basic oxygen furnace (BOF) steel slag particles must be properly understood and managed by pre-conditioning if beneficial reuse of slag is to be maximised. Water... more
Alkalinity generation and toxic trace metal (such as vanadium) leaching from basic oxygen furnace (BOF) steel slag particles must be properly understood and managed by pre-conditioning if beneficial reuse of slag is to be maximised. Water leaching under aerated conditions was investigated using fresh BOF slag at three different particle sizes (0.5–1.0, 2–5 and 10 × 10 × 20 mm blocks) and a 6-month pre-weathered block. There were several distinct leaching stages observed over time associated with different phases controlling the solution chemistry: (1) free-lime (CaO) dissolution (days 0–2); (2) dicalcium silicate (Ca 2 SiO 4) dissolution (days 2–14) and (3) Ca– Si–H and CaCO 3 formation and subsequent dissolution (days 14–73). Experiments with the smallest size fraction resulted in the highest Ca, Si and V concentrations, highlighting the role of surface area in controlling initial leaching. After ~2 weeks, the solution Ca/ Si ratio (0.7–0.9) evolved to equal those found within a Ca–Si–H phase that replaced dicalcium silicate and free-lime phases in a 30-to 150-μm altered surface region. V release was a two-stage process; initially, V was released by dicalcium silicate dissolution, but Valso isomorphically substituted for Si into the neo-formed Ca–Si–H in the alteration zone. Therefore, on longer timescales, the release of V to solution was primarily controlled by considerably slower Ca–Si–H dissolution rates, which decreased the rate of V release by an order of magnitude. Overall, the results indicate that the BOF slag leaching mechanism evolves from a situation initially dominated by rapid hydration and dissolution of primary dicalcium silicate/free-lime phases, to a slow diffusion limited process controlled by the solubility of secondary Ca–Si–H and CaCO 3 phases that replace and cover more reactive primary slag phases at particle surfaces.
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Bauxite residue is a high volume byproduct of alumina manufacture which is commonly disposed of in purpose-built bauxite residue disposal areas (BRDAs). Natural waters interacting with bauxite residue are characteristically highly... more
Bauxite residue is a high volume byproduct of alumina manufacture which is commonly disposed of in purpose-built bauxite residue disposal areas (BRDAs). Natural waters interacting with bauxite residue are characteristically highly alkaline, and have elevated concentrations of Na, Al, and other trace metals. Rehabilitation of BRDAs is therefore often costly and resource/infrastructure intensive. Data is presented from three neighboring plots of bauxite residue that was deposited 20 years ago. One plot was amended 16 years ago with process sand, organic matter, gypsum, and seeded (fully treated), another plot was amended 16 years ago with process sand, organic matter, and seeded (partially treated), and a third plot was left untreated. These surface treatments lower alkalinity and salinity, and thus produce a substrate more suitable for biological colonisation from seeding. The reduction of pH leads to much lower Al, V, and As mobility in the actively treated residue and the beneficial effects of treatment extend passively 20−30 cm below the depth of the original amendment. These positive rehabilitation effects are maintained after 2 decades due to the presence of an active and resilient biological community. This treatment may provide a lower cost solution to BRDA end of use closure plans and orphaned BRDA rehabilitation.
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Basic oxygen furnace (BOF) steelmaking slag is enriched in potentially toxic V which may become mobilized in high pH leachate during weathering. BOF slag was weathered under aerated and air-excluded conditions for 6 months prior to... more
Basic oxygen furnace (BOF) steelmaking slag is enriched in potentially toxic V which may become mobilized in high pH leachate during weathering. BOF slag was weathered under aerated and air-excluded conditions for 6 months prior to SEM/EDS and μXANES analysis to determine V host phases and speciation in both primary and secondary phases. Leached blocks show development of an altered region in which free lime and dicalcium silicate phases were absent and Ca−Si−H was precipitated (CaCO 3 was also present under aerated conditions). μXANES analyses show that V was released to solution as V(V) during dicalcium silicate dissolution and some V was incorporated into neo-formed Ca−Si−H. Higher V concentrations were observed in leachate under aerated conditions than in the air-excluded leaching experiment. Aqueous V concentrations were controlled by Ca 3 (VO 4) 2 solubility, which demonstrate an inverse relationship between Ca and V concentrations. Under air-excluded conditions Ca concentrations were controlled by dicalcium silicate dissolution and Ca−Si−H precipitation, leading to relatively high Ca and correspondingly low V concentrations. Formation of CaCO 3 under aerated conditions provided a sink for aqueous Ca, allowing higher V concentrations limited by kinetic dissolution rates of dicalcium silicate. Thus, V release may be slowed by the precipitation of secondary phases in the altered region, improving the prospects for slag reuse.
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Road mitigation tunnels are increasingly deployed for amphibians but very little is known about chemical pollution in such schemes. We assessed pollution pressures associated with road runoff at a major great crested newt mitigation... more
Road mitigation tunnels are increasingly deployed for amphibians but very little is known about chemical pollution in such schemes. We assessed pollution pressures associated with road runoff at a major great crested newt mitigation scheme in England. Sediments and waters in the mitigation system were analysed for major physico-chemical parameters, trace metals and total petroleum hydrocarbons and compared to a nearby reference site. Seven out of eight tested metals including copper, zinc, lead and iron were in significantly greater concentrations in the tunnels than at a reference site and at environmentally significant concentrations. Water samples also exhibited elevated concentrations of aluminium and chromium and occasionally extreme alkaline pH associated with leaching of portlandite in tunnel cements. High conductivity values in waters and sediments corresponding with seasonal de-icing salt application were also apparent. The study highlights the potential pollutant pressures for amphibians associated with large-scale urban development and road mitigation schemes.