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Reuse and Stabilization of Sulphide Mine
Reuse and Stabilization of Sulphide Mine
Reuse and Stabilization of Sulphide Mine
A R T I C L E I N F O A B S T R A C T
Handling Editor: M.T. Moreira The processing of low-grade sulphide gold ores generates a significant volume of tailings which impacts the
environment. The reuse of sulphide mine tailings as a substitute for sand in construction mortar offers the ad-
Keywords: vantages of reducing costly tailings management whilst promoting sustainable construction. However, the
Sulphide mine tailings acceptance of mine tailings as alternative sand for construction depends on its effective stabilization during use.
Stabilization
In this study, hardened mortar cubes have been prepared by varying the substitution of river sand with sulphide
River sand
mine tailings. The stabilization effects of cement, cement-lime and cement-pozzolana on sulphide mine tailings
Fine aggregate
Masonry mortar have been investigated. The water demand, slump behaviour, bulk density, water absorption, compressive
strength, and X-ray diffraction (XRD) were examined to observe the physical and mechanical properties of the
mortars. The water demand and bulk density decreased whilst the slump value and water absorption increased
with increased tailings replacement. The highest 28-day compressive strength of 12.2 MPa was achieved at 25%
tailing replacement with a cement binder. Cement proved to be the best binder for the stabilization of the tailings
which was followed by cement-pozzolana and cement-lime respectively.
* Corresponding author.
E-mail address: aandrews.coe@knust.edu.gh (A. Andrews).
https://doi.org/10.1016/j.jclepro.2022.131971
Received 2 December 2021; Received in revised form 9 March 2022; Accepted 22 April 2022
Available online 27 April 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
processing routes selected. Furthermore, the properties of mortar and 2. Materials and methods
concrete produced from mine tailings depend on the tailings charac-
teristics and substitution level, water-to-cement ratio, and other addi- 2.1. Sampling and sample preparation
tives (Benarchid et al., 2019).
Gold mining at Obuasi in Ghana dates back over a century and re- Tailings samples were collected from the decommissioned Kokotea-
mains one of the oldest viable mines on the continent of Africa. In sua Tailings Storage Facility (TSF) located at Obuasi in the Ashanti re-
Anglogold Ashanti, Obuasi Mine, a total of 14,726,019 Mt sulphide gion of Ghana. The entire TSF surface area was divided into four main
tailings from the Pompora Treatment Plant have been stored in a areas as shown in Fig. 1. The area marked “A” is the main sampling area
decommissioned tailings storage facility (TSF) located at Kokoteasua, a which was gridded into a 100 m × 100 m plot. Area marked “B” was
suburb in Obuasi. From 2004, the mine began re-mining the tailings and gridded into two irregular blocks of approximately 80 m2. No further
depositing its tailings in Pompora Tailings Storage Facility until the gridding was possible at area “B” due to the presence of huge erosion
operation was halted in 2010 due to TSF stability issues. The Kokoteasua gullies and unstable slopes towards the east of the area. Area marked “C”
TSF currently holds about 4,870,478 Mt of tailings at a grade and is a partially re-mined area that was not sampled due to its low tailings
complexity which makes it currently uneconomical for re-mining. Since content and erosion of lateritic material from the surrounding highlands.
the stoppage of the re-mining exercise, the Kokoteasua TSF has Area marked “D” is a completely mined out area that is used as a water
remained a major environmental liability to the mine. The mine has to impoundment for incident water and was therefore not sampled. The
pump incident water and runoffs off the Kokoteasua TSF for treatment remaining areas were steeply sloped which were inaccessible for sam-
through reverse osmosis (RO) plant before discharge due to its high pling. Two bulk samples were randomly picked within each grid ac-
levels of total dissolved solids (TDS), arsenic and other metals beyond cording to USEPA EPA530-D-02-002, 2002. The sample points in each
the Ghana Environmental Protection Agency (EPA) effluent discharge grid were however not less than 50 m apart in each case to get as much
standards. Notwithstanding, seepage of this incident water in the cause variability as possible within the sampling grids. A backhoe was used to
of its temporary storage poses the threat of pollution to groundwater in dig out about 100 kg of tailings at each location up to depths of 0.7–0.8
the area. m. About 20 kg bulk sample was then representatively taken from the
Studies conducted in Obuasi indicate that soils around active and dug-out at each sample point by quartering with a shovel. A hand-held
decommissioned tailings dams contain arsenic and high amounts of Global Positioning System (GPS) using Geo tracker android Software
sulphide minerals, such as arsenopyrite, which can generate acid mine was used to record the exact location of each sample point. Samples
drainage (AMD) and thus have become an environmental concern in the were packaged into labelled transparent plastic bags, sealed to avoid
catchment areas (Antwi-Agyei et al., 2009). Additionally, inactive tail- losses and cross-contamination, and stored for further analysis. A 500 g
ings impoundments are receiving more attention due to the long-term representative sample was composited in the laboratory from the two
effects of windblown dispersal and groundwater contamination bulk samples from each grid by coning and quartering. A total of eleven
(Aucamp and van Schalkwyk, 2003). The traditional management of test samples of 500 g each were formulated. The samples were air-dried
hazardous tailings after the end of life of the tailings dam has been to for 6–7 days to ensure moisture levels are uniform for mortar formula-
adequately cover them with silty or clayey material that minimizes tions. The air-dried samples were then packed into zip lock bags for
percolation and erosion of the tailings during storms for closure. How- further analysis. River sand was obtained from the locality and used as
ever, the large demand of land for these tailings impoundments in the fine aggregate.
first place, combined with the expensiveness and scarcity of natural
material for covering these tailings deposits makes them an uneco- 2.2. Physical and chemical characterization of soil samples
nomical and often difficult venture (Lyu et al., 2019). The above con-
cerns make it worth the while to investigate options of stabilizing the 2.2.1. Specific gravity and particle size distribution
tailings material for use in a sustainable way to eradicate its liability and Specific gravity determination was carried out on a single composite
also make the land available for the community for development. For sub-sample of 500 g. The sample was first sieved through a 4.75 mm
instance, sulphide mine tailings have been used as alkali-activated ma- sieve and dried for 24 h in a Genlab SPIO 12001S drying oven at 80 ◦ C to
terial with ground granulated blast furnace slag to produce a C-S-H avoid the oxidation of sulphides and other oxidizable components of the
phase with a 10% increase in early strength (Kotwica et al., 2018b). tailings. A 35 g test sample was analyzed in a 250 ml pyconometer ac-
Reuse of the Kokoteasua sulphide mine tailings as fine aggregate for cording to ASTM D854-14.
construction mortar works is considered in this work. Particle size distribution was carried out by sieve analyses using 1.18
In Ghana, river sand is one of the primary sources of sand used in the mm, 0.6 mm, 0.3 mm, 0.212 mm, 0.15 mm, 0.075 mm, 0.053 mm sieves
preparation of construction mortar. Due to the rapid growth in the in an Endecotts EFL 2000 electromagnetic sieve shaker. Particles that
construction industry, demand for river sand has increased enormously, were finer than 0.053 mm were analyzed by a hydrometer using BS
leading to its deficiency, and thus increasing the cost of construction. 1377-1-2016 standard protocols.
The mining of river sand is also destroying rivers by deepening the
riverbeds and causing bank slides, loss of vegetation on the banks of 2.2.2. Chemical and mineralogical analyses
rivers, and disturbing aquatic life (Yifru and Mitikie, 2020). Therefore, The chemical compositions of tailings, sand and binders were
there is a need to look for an alternative material to partially replace determined using a VMR-Olympus X-ray fluorescence spectrometer
river sand for sustainable construction. The objective of this research is whilst their mineralogical compositions were determined using PAN
to investigate the stabilization of the Kokoteasua tailings and their analytical Empyrean Series 2 X-ray diffractometer. The XRD analysis
sustainable use as fine aggregate for construction mortar. The physical, was carried out using Cu K-alpha radiations of wavelength 1.54060 nm
chemical and mineralogical characterization of the mine tailings was operating at 45 kV and 40 mA. Identification of the mineral phases
conducted. Three different binders (cement, cement-lime, and present was done with the Jade software package.
cement-pozzolana) were used to stabilize the tailing material. River sand
was substituted with tailings at varying proportions to produce mortars 2.2.3. Soil pH and electrical conductivity (EC)
and the physical and mechanical properties were determined. Remobi- Soil pH and electrical conductivity (EC) were determined according
lization studies were conducted to assess the effectiveness of to APHA 4500 and APHA 2510 methods respectively. 10 g of soil sample
stabilization. passing through 1.7 mm sieve was weighed into a beaker and 50 ml of
deionized water was added to achieve a soil-to-water ratio of 1:5. The
mixture was allowed to stand for 1 h. The pH and EC of the supernatant
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A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
solution were measured using a calibrated Jenway 3505 pH meter and 2.3. Mortar preparation, casting, curing and testing
Eutech CON2700 conductivity meter, respectively.
2.3.1. Mixing ratios
2.2.4. Anions determination in soil samples Table 1 shows the mix design for the formulation of mortars. A
The presence of sulphates, chlorides, and phosphates in the soil was cement:sand ratio of 1:5 was used following the BS 5628-3 mortar
analyzed using KONELAB 20i Aquakem Discrete Analyzer as per ASTM designation (iii) suitable for general purpose application. Portable water
4500 (2017). 50 ml of deionized water was added to 10 g of soil sample was used for mixing. Sand and tailings samples were thoroughly dried
and shaken for 2 h using an orbital shaker. The solids were allowed to prior to mixing to ensure exact moisture levels in the mortars. Mortar
settle and the decant filtered. The Aquakem Konelab 20i was used to mixes were composed of cement-tailings-sand, cement-lime-tailings-
measure the concentration of the analyte in the filtrate by photometric sand, and cement-pozzolana-tailings-sand. For each binder, different
analyses using the appropriate calibrators, controls and reagents. tailings:sand proportions of 0%:100%, 25%:75%, 50%:50%, 75%:25%
and 100%:0% were used to formulate the mortars. Mixing of the mortars
2.2.5. Arsenic, metals and cyanide determination in soil samples was conducted manually in a 1m diameter steel mixing tub. The tub was
Arsenic and metals in soils were determined using the aqua regia rinsed thoroughly and dried after each mix. Mortars prepared were cast
digestion method according to the EPA 3050B (1996). A 1 g soil sample into 100 mm × 100 mm wooden moulds (Fig. 2) following BS
was weighed into a 50 ml digestion tube to which 6 ml of conc. HNO3 8500–2:2015 and ensuring compaction by filling in two layers each
and 3 ml conc. HCl was added. The mixture was heated on a hot block receiving 25 strokes with a tamper. Triplicate specimens were generated
which had been pre-heated to 105 ◦ C for 40 min 10 ml of deionized with each mortar mix for the different curing ages to be tested. After 24
water was added to the mixture and heated again for 80 min. The h, mortar specimens were demoulded, placed in a water bath at room
mixture was then cooled and filtered through Whatman 1 filter paper temperature and cured for 7, 14, 28 and 56 days respectively.
into a 50 ml flask. Deionized water was added to obtain the 50 ml mark.
Metal concentrations were then determined in mg/kg with Agilent 7900 2.3.2. Bulk density and water absorption test
Inductively Coupled Plasma Mass Spectrometer (ICP MS) using the Bulk density was determined following BS EN 1015-6 procedure
appropriate blanks and standard solutions for each metal. The free and whilst the water absorption of mortar cubes was determined according
total cyanide concentration was determined using Skalar Segmented to ASTM C 642–13. Three samples were tested and recorded after 28
Flow Autoanalyzer following APHA 4500 (2017) procedure. days of curing. An average value of the three was subsequently
determined.
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A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
Table 1
Mortar mixing design.
Replacement of Gold Tailings (%) Binder: Aggregate Constituents (g)
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A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
The chemical compositions (wt %) of the tailings and binders are Table 3
presented in Table 2. Quartz was the major oxide in the tailing (62.65%) Physicochemical parameters of tailings and sand.
with high fractions of Al2O3 and Fe2O3 and a low fraction of CaO. Parameter Unit Tailings Sand
Furthermore, the tailings contain a minimum of 70% of primary oxides
pH – 7.9–8.9 7.9–8.00
(SiO2, Al2O3 and Fe2O3). Consequently, the tailings could possess hy- EC μS/cm 222 3.41
draulic properties (Simonsen et al., 2020). The river sand consisted Chloride mg/kg <5 3.30
mainly of quartz (88.12%) with minor fractions of Al2O3, Fe2O3. The Sulphate mg/kg 437.37 0.32
Ordinary Portland Cement (42.5R) contained CaO (60%), SiO2 Phosphate mg/kg 0.78 0.085
Calcium mg/kg 17727 147.71
(26.15%), Al2O3 (2.91%), and Fe2O3 (2.97%). These oxides enhance Magnesium mg/kg 8763.64 98.03
hydration in mixtures to achieve a desirable compressive strength (sta- Sodium mg/kg 102.09 63.78
bilization). Minor oxides such as MgO (1.48%) and SO3 (3.51%) were Potassium mg/kg 300.00 167.55
also present. For pozzolana, an adequate amount of active ingredients Sulphur mg/kg 2590 ———
Cyanide-Free mg/kg 0.37 ———
SiO2 (67.99%), Al2O3 (11.97%), and Fe2O3 (2.85%) were present.
Cyanide-Total mg/kg 0.42 ———
Higher content (>70%) of the active ingredient (SiO2 + Al2O3 + Fe2O3)
makes it possible to achieve a higher compressive strength due to
improved hydraulic reactivities (Simonsen et al., 2020). The major ox-
Table 4
ides in lime were CaO and SiO2 with minor fractions of SO3 and Fe2O3.
Mean concentration of arsenic and heavy metals in tailings and sand.
The mineralogical composition of tailings consists of quartz (SiO2),
feldspar mineral albite (NaAlSi3O8) and iron (II, III) oxide Fe3O4. The Element Tailings (mg/kg) Sand (mg/kg) WHO Guideline
sand and pozzolana consisted mainly of quartz. As 766.36 4.32 20
Fe 38636.36 10630.24 50000
Al 4145.45 1428.73 ——
3.2. Physicochemical properties Mn 389.09 181.1 2000
Pb 24.81 2.80 50
Ni 38.81 2.32 50
Table 3 shows the physicochemical properties of the tailings and Cr 27.45 20.94 100
sand. The pH of tailings ranged from 7.9 to 8.9 whilst that of sand was Co 16.54 3.40 50
from 7.9 to 8.00. A higher EC value was observed for tailings (222 μS/ Cu 70.36 2.96 100
cm) relative to sand (3.41 μS/cm). The mean concentration of Ca, Mg, Zn 81.90 1.9 300
Na, K and S2− in tailings samples were respectively 17,727, 8763.64,
102.09, 300, 2590 mg/kg. A high concentration of Ca may be attributed
are reportedly among the highest in the world and have been linked to
to lime (CaO) used to condition the pH during gold ore extraction. High
the principal gold-bearing ore in the region, arsenopyrite (FeAsS).
sulphide content in the tailing was due to the sulphidic nature of Obuasi
Hence, tailings can therefore be a potential source of As contamination
gold ore (FeS, FeAsS). Sulphate (SO2−4 ) concentration was high (437.37 to nearby environmental receptors that may pose an environmental
mg/kg) due to the oxidation of sulphide minerals during storage health concern. The mean concentrations of Mn, Pb, Ni, Cr, Co, Cu and
(Bempah et al., 2013). Free and total cyanide were both detected in the Zn in sand samples (Table 4) were also below the WHO maximum
tailings samples with mean concentrations of 0.37 mg/kg and 0.42 permissible limits. The mean arsenic concentration in the sand is also
mg/kg respectively. The mean concentrations of Ca, Mg, Na and K in well below the WHO limit.
sand samples were 147.71, 98.03, 63.78, and 167.55 mg/kg respec-
tively. Free and total cyanide in the sand were below the laboratory
detection limit. The concentration of chloride in tailings was below the 3.3. Water demand
laboratory detection limit (<5 mg/kg) whilst a mean concentration of
3.30 mg/kg was observed in the sand. The water to cement ratio (w/c) is a critical parameter affecting the
Table 4 shows the mean concentrations of arsenic, Fe, Al, Mn, Pb, Ni, strength of cementitious materials. The estimation of water demand is
Cr, Co, Cu and Zn in the tailings and sand samples. The concentrations important for two main reasons: (1) for effective hydration of cement
have been compared with WHO guidelines. Iron concentration was the and (2) serves as a lubricant for fine aggregates based on its specific area
highest in the tailing sample (38,636.36 mg/kg). The mean concentra- (Singh et al., 2015). Water demand, in this context, is the amount of
tion of Mn, Pb, Ni, Cr, Co, Cu and Zn in tailings samples were all below mixing water required to produce a specified consistency of mortar. The
WHO maximum permissible limits. However, the presence of these water requirements for the preparation of mortar samples with varying
metals in the tailings can be a source of contamination to adjoining tailings substitution with different binder types are presented in Fig. 4.
environmental receptors (soils, river water and sediments) through The results show that both sand and binder types have a strong influence
moisture movement or wind erosion of dried tailings (Antwi-Agyei et al., on the water demand and therefore the properties of the mortar pro-
2009). Mean arsenic concentration of 766.36 mg/kg far exceeded the duced. Generally, the water demand is found to decrease with increasing
WHO maximum permissible limit. Gold ore deposits in Obuasi are rich amounts of tailings for both cement and cement-lime binders (Fig. 4). An
in iron and are characterized by sulphide minerals in arsenopyrite form increase in tailings replacement increases the surface area of the fine
(Kumi-Boateng, 2007). A high concentration (542 mg/kg) of As in aggregate and thus decreases the water demand. For the
tailings was also observed by Bempah et al. (2013) in tailings from the cement-pozzolana binder, however, the water demand remained at
AngloGold-Ashanti, Obuasi Mine. Arsenic levels in ores found at Obuasi about the same level with increasing amounts of tailings. This could be
Table 2
Chemical compositions (wt%) of tailings, sand, and binders.
Sample SiO2 Al2O3 MgO P2O5 SO3 K2O CaO MnO Fe2O3 LOI
Tailings 62.65 9.96 1.01 0.05 0.24 1.41 2.08 0.11 5.90 14.9
Sand 88.12 2.53 - - - 0.25 - 0.04 2.73 3.33
Cement 26.15 2.91 1.48 0.07 3.51 0.42 60.00 0.05 2.97 2.27
Pozzolana 67.99 11.97 - - 0.03 0.38 - 0.02 2.85 4.39
Lime 0.11 - - - 0.08 - 55.35 - 0.05 43.90
5
A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
due to the high water demand for pozzolana which counters the low
water demand for cement (SABIR et al., 2001). Additionally, for the
same percent tailings replacement, water demand is highest in
cement-lime binder followed by cement and cement-pozzolana respec-
tively. Thamboo et al. (2018) reported that lime-cement mortars are less
workable than cement mortars and thus require high water demand. It is
also evident from Fig. 4 that the water demand at 0% tailings (i.e. 100%
sand) were high for cement (2.1) and cement-lime (3.0) binders. This
could be attributed to the porous nature (coarser particles of sand) of the
mixture as shown in Fig. 3. A similar observation has been reported
elsewhere (Thamboo et al., 2018).
Fig. 6. Effect of tailings substitution on (a) bulk density and (b) water ab-
Fig. 5. Effect of tailings substitution on slump value for different binders. sorption for different binders.
6
A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
water absorption of hardened mortar for the different binders after 28d
curing are shown in Fig. 6. The average densities of mortars for all kinds
of binders did not change for tailings substitutions up to 25%. There-
after, the average densities decreased with increasing tailings substitu-
tion. Again, the highest average density (8.4 g/cm3) was observed in
mortar produced with cement binder only, followed by cement-
pozzolana (8.3 g/cm3) and lastly cement-lime (8.2 g/cm3). The
average densities of the sand, tailings and binders were measured as
follows: sand ~1.61, tailings ~1.38, cement ~1.43, lime ~1.14, and
pozzolana ~1.15 g/cm3. Sand is denser than the binder and tailings. For
the same binder type, increasing tailings would decrease the bulk den-
sity whilst for the same tailing substitution, cement would have the
highest bulk density followed by cement-pozzolana and cement-lime
respectively.
On the other hand, the average amount of water absorbed for each
mortar under the different binder types steadily increased with
increasing tailings content in the mortar (Fig. 6b). For cement binder,
mortar prepared using 0% tailings (100% sand) absorbed the least water
of 7.4% relative to mortar prepared using different tailings substitutions.
Accordingly, there was a steady rise of water absorbed for each mortar
prepared with 25%, 50% and 75% tailings substitutions with water
absorption values of 9.1%, 13.5%, 17.1% respectively, which were all
below 20%. However, the mortar with 100% tailings substitution had
water absorption above 20%. Similar patterns of water absorption were
also observed for mortar prepared using cement-lime and cement-
pozzolana binders. Again, 100% tailings substitution exceeded water
absorption of 20%. The increasing water absorption could be related to
the nature of tailings, which present higher fine content and thus absorb
more water due to the large surface area (Argane et al., 2016). It has
been reported that the durability of cement-based mortars is dependent
on the amount of fluid penetrating the mortar (Aparna et al., 2018).
Thus the durability of mortars can be improved by reducing the pene-
tration of water or fluids which can cause a chemical attack (Sicakova
et al., 2017). From Fig. 6, penetration resistance can be improved by
increasing the density of the mortar through the reduction of fines in the
mortar mix.
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A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
8
A. Andrews et al. Journal of Cleaner Production 357 (2022) 131971
Table 5
Chemical analyses (ppm) of leachate.
Tailings (%) As Ca Na K Mg Cl SO₄2 PO₄3 NO−
3
Cement
0 0.058 3 96.9 46.2 <0.5 1.8 20 1.2 5.23
25 0.58 2 124 39.8 <0.5 7.4 18 0.94 6.57
100 1.1 3 93.6 20.6 <0.5 17.9 53 0.7 7.1
Cement-Lime
0 0.002 623 53.1 104 <0.5 7.3 3 1.26 2.11
25 0.009 15 76.1 59.3 <0.5 3.2 6 0.93 2.36
100 0.021 200 66.9 72.9 <0.5 4.3 1 0.39 6.04
Cement-Pozzolana
0 0.085 4 53.1 53.2 <0.5 6.3 53 1.1 1.25
25 0.67 2 76.9 76.9 <0.5 11.8 20 1.81 9.7
100 0.89 43 38.4 25 <0.5 44.4 128 0.86 2.9
GHEPA 0.1 250 200 5 2 250 300 — 50
Declaration of competing interest Kotwica, Ł., Chorembała, M., Kapeluszna, E., Stępień, P., Deja, J., Illikainen, M.,
Gołek, Ł., 2018a. Influence of calcined mine tailings on the properties of alkali
activated slag mortars. Key Eng. Mater. 761, 83–86.
The authors declare that they have no known competing financial Kotwica, Ł., Kapeluszna, E., Stępień, P., Deja, J., Illikainen, M., Gołek, Ł., 2018b.
interests or personal relationships that could have appeared to influence Influence of sulphides on hydration of ground granulated slag alkali activated
the work reported in this paper. mortars and pastes. Key Eng. Mater. 761, 92–95.
Kumi-Boateng, B., 2007. Assessing the spatial distribution of arsenic concentration from
goldmine for environmental management at Obuasi, Ghana. MSc Thesis. Int. Institute for
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