3 Open Access. © 2020 Gostečnik M., Šinik P., Mladenovič A., Ščančar J., Milačič R., published by Sciendo. This work is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 License. Received: Mar 11, 2020 Accepted: Mar 13, 2020 DOI: 10.2478/rmzmag-2020-0002 Original scientific paper Abstract During carbon steel manufacturing, large amounts of electric arc furnace (EAF) slag are generated. EAF slag, if properly treated and processed into aggregate, is an alternative source of high-quality material, which can substitute the use of natural aggregates in most de- manding applications in the construction sector , mostly for wearing asphalt courses. In this screening process of high-quality aggregates, a side material with grain size 0/32 mm is also produced, which can be used as an aggregate for unbound layers in road construction. In this study, the environmental impacts of slag aggregate (fraction 0/32 mm) were evaluated in mixed natural/ slag aggregates. Different mixtures of natural/slag ag- gregates were prepared from aged (28 days) and fresh slag, and their environmental impacts were evaluated using leaching tests. It was shown that among the el- ements, chromium (Cr) was leached from some mixed aggregates in quantities that exceeded the criterion for inert waste. The data from the present investigation revealed that mixed aggregates, prepared from aged slag (fraction 0/32 mm) and natural stone in the ratio 10/90, are environmentally acceptable and can be safe- ly used in unbound materials for road construction. Keywords: electric arc furnace slag, natural aggrega- te, mixed aggregates, environmental impacts, unbound materials for road construction. Environmental Impacts of Mixed Aggregates for use in Unbound Layers in Road Construction Okoljski vplivi mešanih agregatov za uporabo v nevezanih materialih v cestogradnji Metka Gostečnik 1,2 , Predrag Šinik 1 , Ana Mladenovič 3 , Janez Ščančar 2,4 , Radmila Milačič 2,4,* 1 Ekomineral d.o.o., Savinjska cesta 25, 3310 Žalec, Slovenia 2 Jožef Stefan International Postgraduate School, Jamova 39, 1000 Ljubljana, Slovenia 3 Department of Materials, Slovenian National Building and Civil Engineering Institute, Dimičeva 12, 1000 Ljubljana, Slovenia 4 Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana, Slovenia * radmila.milacic@ijs.si Povzetek Med proizvodnjo ogljičnega jekla v elektroobločnih pe- čeh nastajajo velike količine žlindre. Pravilno obdelana in predelana žlindra je odličen material, ki lahko uspe- šno nadomesti naravne agregate. Pred uporabo se žlin- dra stara, drobi in separira v agregate različnih frakcij, ki se uporabljajo v gradbeništvu, predvsem kot visoko- kakovosten agregat v obrabnih asfaltnih plasteh. Med separiranjem nastaja tudi agregat zrnavosti 0/32 mm, ki ni primeren za uporabo v asfaltnih plasteh, temveč se uporablja za nevezane nosilne plasti v cestogradnji. V našem delu smo preučili okoljske vplive mešanega agregata (frakcija 0/32 mm) žlindre in naravnega agre- gata za njegovo uporabo v nevezanih materialih v ce- stogradnji. Pripravili smo različne mešanice iz naravne- ga agregata in agregata iz žlindre. Uporabili smo svežo in starano (28 dni) žlindro ter ocenili okoljske vplive pripravljenih mešanic z izlužitvenimi testi. Rezultati naše raziskave so pokazali, da se iz nekaterih pripra- vljenih mešanic lahko izlužuje element krom (Cr) v ko- ličinah, ki presegajo mejno vrednost za inertne odpad- ke. Kot nevezane materiale v cestogradnji varno lahko uporabimo agregate, ki smo jih pripravili iz agregata iz starane žlindre (frakcija 0–32 mm) in naravnega agre- gata v razmerju med 10/90. Ključne besede: žlindra iz elektroobločne peči, narav- ni agregat, mešani agregati, okoljski vplivi, nevezani materiali v cestogradnji. Gostečnik M., Šinik P ., Mladenovič A., Ščančar J., Milačič R. RMZ – M&G | 2020 | Vol. 67 | pp. 003–012 4 Introduction Industrial wastes or by-products are increas- ingly being used as alternative materials that successfully substitute natural raw materials. Recycling and use of these materials lead to the preservation of natural resources, signif- icant reduction of landfill load and protection of the environment [1]. Recycling of waste materials is in line with the main objectives of green building, i.e. application of processes that are environmentally responsible and re- source efficient. The latter goals are strongly supported by the Directive 2018/851/ES on waste [2] and Construction Products Regula- tion No. 305/2011 [3]. During steel manufac- ture, huge amounts of waste materials, such as electric arc furnace (EAF) slag, ladle slag and EAF filter dust, are produced. In the Štore Steel plant, Slovenia, the annual steel produc- tion is about 150,000 tonnes. Approximately 20,000 tons of EAF slag, 2,000 tons of ladle slag and 2,500 tons of EAF dust are generated as waste per year [4]. During the production of steel in an EAF, scrap metal or metallised ore, or both, are melted along with lime in refractory lined vessels. Throughout the melting process, oxygen is in- jected into the molten steel, which oxidises a part of metallic Fe and alloying components (e.g. Mn, Ni, Cr, Mo, V), as well as the impuri- ties in steel scrap (e.g. Al, Si, Mn, P and C). The EAF steel slag is poured from the furnace in a molten state at the end of the process. About 15–20% of EAF slag occurs per equivalent unit of steel. The principal components of EAF steel slag are calcium silicates and ferrites, together with oxides and compounds of iron, magne- sium, manganese and alumina, which together make up 95% of the slag [5]. The main minerals in slag are wustite, dicalcium silicate, tricalcium silicate and brownmillerite; and the accessory minerals can be spinel, barite, CaO and MgO. Both of the latter components are unstable. In the presence of moisture, they transform into Mg(OH) 2 and/or Ca(OH) 2 , which occupy a larg- er volume than the primary components. The result is swelling of the composite into which the slag has been placed. The slag must there- fore be “aged” long enough for the CaO and MgO to be transformed into stable forms. Slow, con- trolled cooling also enables this material to de- velop a microtexture, which ensures long-term toughness and roughness and is comparable with the porphyric texture of volcanic rocks. EAF slag is highly durable and is, in terms of its physico-mechanical characteristics, compa- rable to high-quality natural rocks. Due to its excellent physical and mechanical properties, it can be used as an alternative material that suc- cessfully replaces natural aggregates. Hence, the greatest potential for recycling and use of steel slag is in the construction sector [6–9]. EAF slag aggregate is used in different types of concrete [9–13], in sub-base layer constructions [14, 15], and especially in asphalt mixes [6, 7, 16–18]. Other EAF slag applications include water and wastewater treatment [9], as well as usage in synthesis of alkali-activated materials [19]. The use of materials that contain industrial waste and/or by-products is possible when such materials possess appropriate technical characteristics [15, 20–23] and are environ- mentally acceptable [20–24]. For evaluation of the environmental impacts of raw materi- als and final products, the extent of leaching of contaminants is estimated by applying different leaching tests, e.g. the European test method for leaching of aggregates (Slovenian Institute for Standardisation [SIST] EN 1744-3) [25] and the compliance test for the leaching of granular waste materials and sludges (SIST EN 12457-4) [26]. In these leaching tests, shaking of the solid material with water (a liquid-to-solid ratio of 10 L/kg) is performed over 24 h. The EAF slag, which is generated during the met- allurgical process of carbon steel production in Štore Steel (waste classification no.: 10 02 02), is first subjected to stabilisation by ageing. For this purpose, a process of slow cooling, wet- ting with water and temporary storage for a period of 28 days (ageing) is carried out. Be- fore final crushing and screening of the aggre- gate, iron is extracted by magnetic separation. The 32/300 mm fraction is mostly used for un- bound layers, the 32/63 mm fraction particles for railway ballast and the 2/4 mm, 4/8 mm and 8/11 mm fractions for asphalt mixes. During these screenings, an additional fraction (0/32 mm) is also formed, which is the mate- rial for unbound layers in road construction. Therefore, the aim of the present study was to Environmental Impacts of Mixed Aggregates for use in Unbound Layers in Road Construction 5 evaluate the potential use of the mixed aggre- gate (0/32 mm) from the EAF slag aggregate and natural aggregate as the unbound material for road construction from the environmental point of view. Different mixed aggregates were prepared and their environmental impacts were estimated by applying leaching tests. Materials and Methods Reagents Merck (Darmstadt, Germany) suprapur acids and Milli-Q water (Direct-Q 5 Ultrapure wa- ter system; Millipore, Watertown, MA, USA) were used for the preparation of samples and standard solutions. Certipur inductively cou- pled plasma spectroscopy (ICP) multi-ele- ment standard solution IV (1,000 ± 5 mg/L in 5% HNO 3 ) and single stock standard solution of Hg (1,000 ± 5 mg/L in 5% HCl), both pur- chased from Merck, were used for the prepa- ration of calibration curves in ICP–mass spec- troscopy (MS) determinations. To control the stability of ICP–MS, Merck Ge, Rh, Sc and In (1,000 ± 2 mg/L in 5% HNO 3 ) were used as in- ternal standards. The reagents for spectropho- tometry were obtained from Hach Lange GmbH (Düsseldorf, Germany). Cellulose nitrate mem- brane filters (0.45 mm; Sartorius, Gottingen, Germany) were used for filtration. The certified reference material CRM 320R (trace elements in river sediment; Community Bureau of Ref- erence, Geel, Belgium), the standard reference material SPS-SW1 (reference material for mea- surement of elements in surface waters; ob- tained from Spectrapure Standards, Oslo, Nor- way) and reference material Anions – Whole Volume (purchased from Merck) were used to check the accuracy of the analytical procedures. Apparatus The concentrations of elements in the leach- ates of natural aggregate, EAF slag aggregate and mixed aggregates were determined by ICP–MS on an Agilent 7700´ spectrometer (Ag- ilent Technologies, Tokyo, Japan). The ICP–MS operating parameters are presented in Table 1. Table 1. ICP–MS operating parameters for determination of element concentrations Parameter Type/value Helium mode No gas mode Sample introduction Nebuliser Mira Mist Spray chamber Scott Skimmer and sampler Ni Plasma conditions Forward power 1,550 W Plasma gas flow 15.0 L/min Carrier gas flow 1.05 L/min 0.75 L/min Dilution gas flow 0.10 L/min 0.45 L/min He gas flow 4.5 mL/min Quadrupole (QP) bias –15 V –3.6 V Octapole (Oct) bias –18 V –8.0 V Cell entrance –40 V –40 V Cell exit –60 V –50 V Deflect –2.2 V 13.4 V Plate bias –60 V –40 V Sample uptake rate 0.3 mL/min Data acquisition parameters Isotopes monitored 52 Cr, 60 Ni, 63 Cu, 66 Zn, 75 As, 78 Se, 95 Mo 111 Cd, 121 Sb, 137 Ba, 201 Hg, 208 Pb Isotopes of internal standards 45 Sc, 72 Ge, 103 Rh, 115 In 45 Sc, 72 Ge, 103 Rh, 115 In Gostečnik M., Šinik P ., Mladenovič A., Ščančar J., Milačič R. RMZ – M&G | 2020 | Vol. 67 | pp. 003–012 6 The contents of chlorides, sulphates and fluo- rides were determined on the DR 3900 portable spectrophotometer (Hach, Manchester, Great Britain). The MARS 6 Microwave System (CEM Corporation; Matthews, NC, USA) was used for digestion of the slag samples. The WTW 330 pH meter (WTW, Weilheim, Germany) was used to determine the pH. The Mettler AE 163 (Mettler Toledo, Zürich, Switzerland) analytical balance was used for weighing. Samples The EAF slag samples from different batches were obtained from Štore Steel Company, Štore, Slovenia. After ageing of the slag and produc- tion of aggregate fractions, the 0/32 mm frac- tions from fresh and aged slags (time of ageing: 28 days) were used in the present study. Nat- ural aggregate (dolomite) was obtained from Andraž Quarry, Slovenia. Mixed aggregates of different natural-to-slag ratios were prepared from fresh and aged slags. Sample preparation To determine the total content of elements in the slag and aggregate samples, about 0.25 g of sample was subjected to microwave-assisted digestion, using a mixture of nitric, hydrochlo- ric and hydrofluoric acids [27], and the concen- trations of the elements in the digested samples were determined by ICP-MS. The extent of leaching of selected elements and anions from bulk natural aggregates, bulk slag aggregates and bulk mixed aggregates of dif- ferent ratios was evaluated by the preparation of aqueous leachates (a liquid-to-solid ratio of 10 L/kg), following the SIST EN 1744-3 [25] test method for leaching of aggregates and the SIST EN 12457-4 [26] compliance test for the leaching of granular waste materials and slud- ges. The concentrations of elements and anions in the aqueous leachates were determined by ICP-MS and spectrophotometry, respectively. The results are presented on a dry mass basis. Results and Discussion Quality control of the analytical data The accuracy of determination of the total met- al concentrations in the EAF slag aggregate was checked by analysis of CRM 320R, the total met- al concentrations in the leachates were analysed by the SPS-SW1 quality control method and de- termination of anions was done by analysing the reference material Anions – Whole Volume. The results are presented in Tables 2–4. Table 2. Concentrations of elements in certified reference material CRM 320R (Trace Elements in River Sediment) determined by ICP-MS after microwave-assisted digestion Element Certified (mg/kg) Determined (mg/kg) Fe 25,700 ± 1,300 24,350 ± 700 Mn 910 ± 50 940 ± 30 Cr 59 ± 4 61 ± 2 Note: The results represent the mean concentration from two parallel samples. Table 3. Concentrations of elements in standard reference material SPS-SW1 (reference material for measurements of elements in surface waters) determined by ICP-MS Parameter Certified concentration (mg/L) Determined concentration (mg/L) As 10.0 ± 0.1 10.4 ± 0.3 Ba 50 ± 1 52 ± 1 Cd 0.50 ± 0.01 0.48 ± 0.01 Total Cr 2.00 ± 0.02 1.97 ± 0.02 Cu 20 ± 1 19.6 ± 0.3 Mo 10.0 ± 0.1 9.8 ± 0.2 Ni 10.0 ± 0.1 10.2 ± 0.3 Pb 5.0 ± 0.1 4.91 ± 0.01 Se 2.00 ± 0.02 2.03 ± 0.02 Zn 20 a 21.0 ± 0.2 a Informative value. Notes: The results represent the mean concentration from two parallel samples. Table 4. Concentrations of chlorides, fluorides and sulphates in reference material Anions – Whole Volume determined by spectrophotometry Parameter Certified concentration (mg/L) Determined concentration (mg/L) Chlorides 95.0 ± 9.50 92.5 ± 5.0 Fluorides 1.17 ± 0.117 1.14 ± 0.06 Sulphates 44.3 ± 4.43 42.5 ± 2.0 Note: The results represent the mean concentration from two parallel samples. Environmental Impacts of Mixed Aggregates for use in Unbound Layers in Road Construction 7 Data from Tables 2–4 show good agreement be- tween the determined and certified values (the agreement between the results is better than ±5%), which confirmed the accuracy of the ap- plied analytical procedures for the determina- tion of (a) elements in the EAF slag aggregate and (b) elements and anions in aqueous leach- ate samples. Chemical composition of the EAF slag The chemical composition of the EAF slag ag- gregate may differ according to the additives used in steel production. The concentration ranges of the main components in the EAF slag analysed are presented in Table 5. During EAF slag processing, elemental oxides are formed. Therefore, concentrations of the measured el- ements in Table 5 are expressed in the form of their corresponding oxides. Results showed that the content of P 2 O 5 and V 2 O 5 was <1%, while oxides of other elements (Mo, Ba, Ni and Zn) were found in trace amounts. As can be seen from the data of Table 5, the main components in the EAF slag are oxides of Fe, Ca, Si and Mg, whereas oxides of Al, Mn and Cr in general occur in concentrations <5%. Environmental impacts of mixed aggregates from natural and EAF slag aggregates In order to evaluate the environmental impacts of the mixed aggregates prepared from natural aggregate and EAF slag aggregate, leachates of bulk aggregates were prepared according to relevant test methods (a liquid-to-solid ra- tio of 10 L/kg) [25, 26]. First, natural aggre- gate from the Andraž Quarry, aged EAF slag aggregate (0/32 mm) and mixed aggregate containing aged slag aggregate (natural aggre- gate-to-EAF slag aggregate ratio 30/70) were examined. Concentrations of elements and an- ions in leachates were determined by ICP-MS and spectrophotometry, respectively. The mea- sured parameters were selected based on the legislative requirements for inert waste [28]. Aggregates used in the unbound materials for road construction and earthwork structures are generally compacted at optimum moisture content in order to ensure maximum density and bearing capacity of the final product. In order to evaluate the environmental impacts of such aggregates, the worst-case scenario was considered. Therefore, the leaching procedure was not performed on the compacted aggregate sample but rather on the bulk sample without any pre-treatment. The results of these exper- iments, along with the concentration limits for inert waste [28], are presented in Table 6. As evident, the leaching of elements and anions from natural aggregate is below the instrumen- tal limits of detection for all measured param- eters. Due to the presence of soluble Ca(OH) 2 , which is formed after reaction of CaO with water, the pH values of EAF slag aggregate and mixed natural/EAF slag aggregate are high (pH 12.5 and 12, respectively). As a consequence of the high pH, most of the elements in the aque- ous leachates are precipitated. Hence, their concentrations in the leachates are very low, in general, far below the concentration limits for inert waste (Table 6). Attention should be paid to Cr, the concentration of which exceeded the concentration limit of 0.5 mg/kg for inert waste in EAF slag aggregate and in mixed natural/ EAF slag aggregates. Cr in EAF slag aggregate is present in the highly insoluble chromite min- eral in its trivalent oxidation state. However, at high pH, traces of trivalent Cr are solubilised as the Cr(OH) 4 – complex. Although only a negligi- ble amount, about 0.01% of the total Cr content in the EAF slag aggregate is leached with water; the solubilised Cr(III) is, under the highly alka- line conditions, almost completely oxidised to hazardous Cr(VI) by the presence of dissolved oxygen. As an oxyanion, chromate (CrO 4 2– ), un- der alkaline pH values, is a highly mobile and Table 5. Concentration ranges of elemental oxides in EAF slag aggregate samples (0–32 mm) determined by ICP-MS after microwave-assisted digestion Parameter Concentration (%) FeO and Fe 2 O 3 33–46 CaO 20–35 SiO 2 10–20 MgO 3–13 Al 2 O 3 3–6 Mn 2 O 5 3–5 Cr 2 O 3 1–3 Notes: Measurement uncertainty is better than ±3%. Results represent concentration ranges obtained from five EAF slag samples. Gostečnik M., Šinik P ., Mladenovič A., Ščančar J., Milačič R. RMZ – M&G | 2020 | Vol. 67 | pp. 003–012 8 highly stable species [23]. Similarly to Cr, Mo also forms the oxyanion molybdate (MoO 4 2– ), and thus, its leaching from slag aggregates is favourable at high pH values. Leaching of chlo- rides, fluorides and sulphates from mixed ag- gregates does not represent any environmental burden. In the following experiments, mixed aggregates from stone and cured EAF slag of the same batch were prepared in different stone–to-EAF slag ratios. Based on the data from Table 6, only Cr and Mo were measured in the aqueous leach- ates (Figure 1). It can be seen that Cr and Mo concentrations in the leachates decrease with higher natural aggregate-to-slag aggregate ratio in the mixed aggregate. As expected, the pH also gradual- ly decreased from pH 12 to pH 10. At natural aggregate-to-slag aggregate ratio 30/70 and 90/10, about 0.25 and 0.05 mg/kg of Mo, re- spectively is leached from the mixed aggre- gate. These concentrations are lower than the legislative requirements for inert waste Table 6. Concentrations of As, Ba, Cd, Cr, Cu, Hg, Mo, Ni, Pb, Sb, Se and Zn in aqueous leachates (a liquid-to-solid ratio of 10 L/kg) of bulk natural aggregate, bulk aged EAF slag aggregate (0–32 mm) and bulk mixed aggregate from the aged EAF slag aggregate (natural aggregate-to-slag aggregate ratio 30/70) determined by ICP-MS and the content of chlorides, fluorides and sulphates determined by spectrophotometry Parameter Natural aggregate EAF slag aggregate (0–30 mm) Mixed aggregate (natural aggregate-to-slag aggregate ratio 30/70) Concentration limits for inert waste * As (mg/kg) <0.001 <0.001 <0.001 0.5 Ba (mg/kg) <0.02 14 2.2 20 Cd (mg/kg) <0.002 <0.002 <0.002 0.04 Total Cr (mg/kg) <0.002 1.4 0.95 0.5 Cu (mg/kg) <0.001 <0.001 <0.001 2 Hg (mg/kg) <0.001 <0.001 <0.001 0.01 Mo (mg/kg) <0.002 0.26 0.24 0.5 Ni (mg/kg) <0.002 <0.002 <0.002 0.4 Pb (mg/kg) <0.005 0.45 0.15 0.5 Sb (mg/kg) <0.001 0.08 0.02 0.06 Se (mg/kg) <0.003 <0.003 <0.003 0.1 Zn (mg/kg) <0.005 1.95 0.2 4 Chlorides (mg/kg) <7 <7 <7 800 Fluorides (mg/kg) <1 4.59 <1 10 Sulphates (mg/kg) <10 19.5 <10 1000 pH 8.7 12.5 12.0 / * Decree on waste (2015): Official Gazette of Republic Slovenia RS, No. 37/15 and No. 69/15. Notes: The results represent the mean concentration obtained from two parallel analyses of leachate. Measurement uncertainty for ICP-MS is better than ±3% and, for spectrophotometry, it is ±5%. Figure 1. Concentrations of Cr and Mo in aqueous leachates (a liquid-to-solid ratio of 10 L/kg) of bulk mixed aggregates from aged EAF slag aggregate of the same batch, applying different natural aggregate-to-slag aggregate ratios. Notes: Bars represent mean Cr and Mo concentrations determined by ICP-MS, while the error bars indicate the minimum and maximum concentrations from two parallel determinations in the leachate by ICP-MS. Environmental Impacts of Mixed Aggregates for use in Unbound Layers in Road Construction 9 (0.5 mg/kg Mo) [28]. Cr concentration in the leachate at natural aggregate-to-slag aggre- gate ratio 30/70 is 0.95 mg/kg and gradually decreases with decrease in the amount of slag aggregate in the mixed aggregate. A concen- tration that is below the limit for inert waste (0.5 mg/kg Cr) [28] is reached at ratio 85/15. In order to evaluate the variability of Cr leach- ing from mixed aggregates, aged slag aggregate from different batches was used for the prepa- ration of mixed aggregates, applying natural aggregate-to-slag aggregate ratio 90/10. These results are presented in Figure 2. The pH values of the leachates in the samples from Figure 2 were around 10. As evident from the data of Figure 2, the leaching of Cr from 13 mixed aggregates ranged from 0.1 mg/kg up to 0.65 mg/kg. Only two samples exceeded the maximal legislative value set for inert waste. High variability in leached Cr concentrations in the aggregates prepared from aged EAF slag at the same natural aggregate-to-slag aggregate ratio (90/10), with constant pH (10), but from different slag aggregate batches, indicates the high variability of Cr content in the slag aggre- gate samples from different batches. Cr content in the EAF slag aggregate is related to different compositions of Cr in steel. Finally, the influence of EAF slag ageing on leaching of Cr from mixed aggregates was esti- mated. For this purpose, mixed aggregates from four different batches were prepared from fresh and aged EAF slag aggregates, applying natural aggregate-to-slag aggregate ratio 90/10. The results of this experiment are shown in Fig- ure 3. The pH of the leachates investigated was around 10. The data in Figure 3 demonstrate that, as a consequence of variable Cr content in different slag batches, leached Cr concentrations varied significantly. The ageing of EAF slag, which sta- bilises its mineralogical phases, results in low- er leachability of Cr. Leaching of Cr from mixed aggregates made of aged EAF slag aggregate is 30–60% lower than that of aggregates pre- pared from fresh slag aggregate from the same batch. It is further evident that Cr leaching from mixed aggregates made of aged EAF slag aggregate (natural aggregate-to-slag aggregate ratio 90/10) from different EAF slag aggregate batches did not exceed 0.3 mg/kg. Conclusions The results from the present study revealed that in bulk mixed aggregates (0/32 mm), made of dolomite natural aggregate and EAF slag aggregate, only Cr, among all elements and anions investigated, may exceed the concentra- tion limit for inert waste (0.5 mg/kg Cr). To find the conditions for safe use of mixed aggregates from natural aggregate and EAF slag aggregate, leaching of Cr from samples with different nat- ural aggregate-to-EAF slag aggregate ratios was studied, applying fresh and aged (28 days) EAF Figure 2. Concentrations of Cr in aqueous leachates (a liquid- to-solid ratio of 10 L/kg) of bulk mixed aggregates from aged EAF slag of different slag batches, applying natural aggregate- to-slag aggregate ratio 90/10. Notes: Bars represent mean Cr concentrations determined by ICP-MS, while the error bars indicate the minimum and maximum concentrations from two parallel determinations in the leachate by ICP-MS. Figure 3. Concentrations of Cr in aqueous leachates (a liquid- to-solid ratio of 10 L/kg) of bulk mixed aggregates from fresh and aged EAF slags of different slag batches, applying natural aggregate-to-slag aggregate ratio 90/10. Notes: Bars represent mean Cr concentrations determined by ICP-MS, while the error bars indicate the minimum and maximum concentrations from two parallel determinations in the leachate by ICP-MS. Gostečnik M., Šinik P ., Mladenovič A., Ščančar J., Milačič R. RMZ – M&G | 2020 | Vol. 67 | pp. 003–012 10 slag aggregate from different batches. High pH of mixed aggregates (pH 10–12) enabled the leaching of Cr in the form of oxyanion chromate. Due to variable Cr content in the EAF slag ag- gregate from different batches, which is related to the composition of steel (different amounts of Cr added in the process to obtain the steel of desired properties), the extent of Cr leach- ing from mixed aggregates varied significantly. Leaching of Cr from mixed aggregates made from aged EAF slag aggregate was 30–60% low- er than that from fresh EAF slag aggregate. Data of the present investigation demonstrated that mixed aggregates prepared from natural aggre- gate and EAF slag aggregate may be safely used in unbound materials for road construction if aged slag is used for preparation of mixed ag- gregates at natural aggregate-to-EAF slag ag- gregate ratio 90/10. The safe reuse of EAF slag leads to the protection of the environment and preservation of natural resources. Acknowledgements This work was supported by the Ministry of Education, Science and Sport, the Republic of Slovenia, by co-financing the doctoral studies of Metka Gostečnik at the Jožef Stefan Interna- tional Postgraduate School (contract number C3330-16-500190). We also acknowledge the financial support received from the Slovenian Research Agency (ARRS) (programme groups P2-0273 and P1-0143). References [1] Banaitė, D., Tamošiūnienė, R. (2016): Sustainable development: the circular economy indicators’ selection model. Journal of Security and Sustain- ability Issues, 6(2), http://dx.doi.org/10.9770/ jssi.2016.6.2(10). [2] Regulation (EU) No 305/2011 of the European par- liament and of the council, of 9 March 2011, Official Journal of the European Union, 4.4.2011. [3] Official Journal of the European Union. (2011). Reg- ulation (EU) No 305/2011 of the European parlia- ment and of the council laying down harmonised conditions for the marketing of construction prod- ucts and repealing Council Directive 89/106/EEC, 88, pp. 5–43. [4] ARSO annual report (2019): The type and quantity of waste generated in manufacturing and service ac- tivities and the ways of managing (2018), https:// www.arso.gov.si/varstvo%20okolja/odpadki/po- ro%c4%8dila%20in%20publikacije/. Last assessed march 2020. [5] Yildirim, I., Prezzi, M. (2011): Chemical, miner- alogical, and morphological properties of steel slag. Advances in Civil Engineering, pp. 1–13, doi:10.1155/2011/463638. [6] Milačič, R., Zuliani, T ., Oblak, T ., Mladenovič, A., Ščančar, J. (2011): Environmental impacts of as- phalt mixes with electric arc furnace steel slag. Journal of Environmental Quality, 40, pp. 115–1161, doi:10.2134/jeq2010.0516. [7] Oblak, T ., Ščančar, J., Vahčič, M., Zuliani, T ., Mlade- novič, A., Milačič, R. (2011): Environmental impacts of asphalt and cement composites with addition of EAF dust. RMZ - Materials and Geoenvironment, 58(2), pp. 181–192. [8] National Slag Association, Steel slag: A premier construction aggregate, Assessed on March 2020, from http://www.acobrasil.org.br/siderurgiaemfo- co/CCABrasil/NSA%20Steel%20Furnace%20Bro- chure.pdf. Last assessed March 2020. [9] Lim, J.W., Chew, L.H., Choong, T .S.Y., Tezara, C., Yazdi, M.H. (2016): Overview of Steel Slag Application and Utilization, MATEC Web of Conferences 74, 00026, pp. 1–5, DOI: 10.1051/matecconf/20167400026. [10] Arribas, I., Vegas, J., San-José, J., Manso, J.M. (2014): Durability studies on steelmaking slag concretes. Materials & Design, 63, pp. 168–176, https://doi. org/10.1016/j.matdes.2014.06.002. [11] Arribas, I., Santamaría, A., Ruiz, E., Ortega-López, Manso, J.M. (2015): Electric arc furnace slag and its use in hydraulic concrete. Construction and Building Materials, 15, pp. 68–79, https://doi.org/10.1016/j. conbuildmat.2015.05.003. [12] Roslan, N.H., Ismail, M., Abdul-Majid, Z., Ghoreishi- amiri, S., Muhammad, B. (2016): Performance of steel slag and steel sludge in concrete. Construction and Building Materials, 104, pp. 1–24, https://doi. org/10.1016/j.conbuildmat.2015.12.008. [13] Penteado, C.S.G., Evangelista, B.L., dos Santos Fer- reira, G.C., Borges, P .H.A., Lintz, R.C.C. (2019): Use of electric arc furnace slag for producing concrete pav- ing blocks. Ambiente Construído, Porto Alegre, 19(2), pp. 21–32, http://dx.doi.org/10.1590/s1678- 86212019000200305. Environmental Impacts of Mixed Aggregates for use in Unbound Layers in Road Construction 11 [14] Wang, G.C. (2016): 8 - Unbound slag aggregate use in construction. In: The Utilization of Slag in Civil Infrastructure Construction, Woodhead Publishing Series in Civil and Structural Engineering: Number 68, Wang, G.C. (ed.). Elsevier Ltd., SPi Global: India, pp. 155–184, https://doi.org/10.1016/B978-0-08- 100381-7.00008-2. [15] Gonawala, R.J., Kumar, R., Chauhan, K.A. (2019): Us- age of Crushed EAF Slag in Granular Sub-base Layer Construction. In: Proceedings of ICIIF 2018, Spring- er Nature, Singapore, Gateway East Singapore, pp. 257–266. [16] Skaf, M., Manso, J.M., Aragón, Á., Fuente-Alonso, J.A., Ortega-López, V. (2017): EAF slag in asphalt mixes: A brief review of its possible re-use. Resources, Con- servation and Recycling, 120, pp. 176–185. http:// dx.doi.org/10.1016/j.resconrec.2016.12.009. [17] Maharaj, C., White, D., Maharaj, R., Morin, C. (2017): Reuse of steel slag as an aggregate to asphaltic road pavement surface. Cogent Engineering, 4(1), pp. 1–12, doi.org/10.1080/23311916.2017.1416889. [18] Vaiana, R., Balzano, F., Iuele, T ., Gallelli, V. (2019): Microtexture performance of EAF slags used as ag- gregate in asphalt mixes: A comparative study with surface properties of natural stones. Applied Scienc- es, 9(15), 3197, pp. 1–14, https://doi.org/10.3390/ app9153197. [19] Češnovar, M., Traven, K., Horvat, B., Ducman, V. (2019): The Potential of Ladle Slag and Electric Arc Furnace Slag use in Synthesizing Alkali Activat- ed Materials; the Influence of Curing on Mechan- ical Properties. Materials, 12(7), 1173, pp. 1–18, doi:10.3390/ma12071173. [20] Vahčič, M., Milačič, R., Mladenovič, A., Murko, S., Zuliani, T ., Zupančič, M., Ščančar, J. (2008): Leach- ability of Cr(VI) and other metals from asphalt composites with addition of filter dust. Waste Man- agement, 28, pp. 2667–2674, doi:10.1016/j.was- man.2008.01.003. [21] Šturm, T ., Milačič, R., Murko, S., Vahčič, M., Mlad- enovič, A., Strupi Šuput, J., Ščančar, J. (2009): The use of EAF dust in cement composites: Assess- ment of environmental impact. Journal of Hazard- ous Materials, 166, pp. 277–283, doi:10.1016/j. jhazmat.2008.11.015. [22] Zalar Serjun, V., Mladenovič, A., Mirtič, B., Meden, A., Ščančar, J., Milačič, R. (2015): Recycling of ladle slag in cement composites: environmental impacts. Waste Management, 43, pp. 376–385, http://dx.doi. org/10.1016/j.wasman.2015.05.006. [23] Milačič, R., Zuliani, T ., Oblak, T ., Mladenovič, A., Ščančar, J. (2011): Environmental impacts of as- phalt mixes with electric arc furnace steel slag. Journal of Environmental Quality, 40, pp. 115–1161, doi:10.2134/jeq2010.0516. [24] Wang, G.C. (2016): 7 - Environmental aspects of slag utilization. In: The Utilization of Slag in Civil Infrastructure Construction, Woodhead Publishing Series in Civil and Structural Engineering: Number 68, Wang, G.C. (ed.). Elsevier Ltd., SPi Global: India, pp. 131–153, https://doi.org/10.1016/B978-0-08- 100381-7.00007-0. [25] SIST EN 1744-3 (2002). Tests for chemical properties of aggregates. Part 3, Preparation of eluents by leach- ing of aggregates. [26] SIST EN 12457-4 (2004). Characterisation of waste – Leaching – Compliance test for leaching of granular waste materials and sludges. Part 4, One stage batch test at a liquid to solid ratio of 10 L/kg for materials with particle size below 10 mm (without or with size reduction). [27] Vidmar, J., Zuliani, T ., Novak, P ., Drinčić, A., Ščančar, J., Milačič, R. (2017): Elements in water, suspended particulate matter and sediments of the Sava River. Journal of Soils and Sediments, 17(7), pp. 1917–1927, doi 10.1007/s11368-016-1512-4. [28] Decree on waste (2015): Official Gazette of Republic Slovenia RS, No. 37/15 and No. 69/15.