Minerals Engineering 174 (2021) 107231

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Minerals Engineering
journal homepage: www.elsevier.com/locate/mineng

Lime use in gold processing – A review

C.A. du Plessis a, *, H. Lambert b, R.S. Gärtner b, K. Ingram c, W. Slabbert d, J.J. Eksteen e
a
Lhoist, Australia
b
Lhoist, Belgium
c
Lhoist, USA
d
Hatch, Australia
e
Curtin University, Australia

A R T I C L E I N F O A B S T R A C T

Keywords: The gold processing industry is a large consumer of lime reagents in various forms. Its role in gold processing is
Cyanide mainly as a pH control agent for optimal cyanidation leaching of gold, as well as a neutralization agent in re­
CaO fractory gold processing via acidic oxidation routes. There are, however, a range of conditions upstream of
Ca(OH)2
cyanidation that influence lime consumption and its functionality in the overall process. Lime also positively
Activated carbon
Scaling
impacts gold absorption onto carbon in CIP/CIL circuits compared to other pH modifiers. The quantity of lime
Scale consumed depends upon several factors, including (1) lime reagent properties, (2) methods of preparation, (3)
gold ore type, and (4) processing flow sheet. This article provides a comprehensive review of lime functionality in
gold processing and process features that influence its consumption.

1. Introduction therefore, explicitly focuses on lime use in gold processing applications.

The large variety of gold processing methods necessitated limiting the
Gold extractive metallurgy has arguably been the subject of more scope of this review to current industrial applications and to cyanide as
studies and publications than any other metal. Pyrometallurgical pro­ the dominant gold lixiviant.
cessing and physical separation methods were the earliest forms of gold
processing, followed by mercury amalgamation in the more recent past, 2. Lime reagent formats and features
but these were overtaken by use of cyanide as chemical lixiviant. Early
industrial mining applications using cyanide date back to 1887 Lime is the generic term used to describe various formats of the re­
(Maclaurin, 1895; Gray and McLachlen, 1933). Cyanide use has become agent (National Lime Association, 1995; du Plessis et al., 2021). Formats
ubiquitous, with about 80% of global gold extraction being facilitated by include: quicklime – a dry reagent with calcium oxide (CaO) as the main
this lixiviant, despite the large number of other lixiviants that have been component, produced from the calcination of limestone containing
proposed (Aylmore, 2016). Globally, more than a billion tons of ore per calcium carbonate (CaCO3); hydrate or hydrated lime – a dry reagent
year are treated using cyanide (Habashi, 2016). In addition to the comprising mainly Ca(OH)2, produced from the stoichiometric hydra­
beneficial gold-lixiviant features of cyanide, its associated hazards also tion of quicklime with water; and slaked lime or milk of lime – a slurry of
became known in the 19th Century, and with it the critical importance Ca(OH)2 particles typically in the range of 10–25 %wt produced from
of pH control. Lime is typically the most cost-efficient reagent to achieve slaking quicklime in a stoichiometric excess of water, although specialty
this. The natural abundance of limestone from which lime is produced, product formulations may contain up to 45 %wt solids content.
the cost competitiveness of lime and its chemical features have Quicklime (with active ingredient CaO), the starting reagent mate­
entrenched it as a critical reagent, alongside cyanide, in the gold pro­ rial for all other forms of lime reagent, is produced by calcination of
cessing industry. A significant body of scientific literature has been limestone (CaCO3) at temperatures ranging from 900 to 1300 ◦ C (Kumar
devoted to the industrial use of cyanide in gold processing (Adams, et al., 2007) using a variety of kiln types and fuel sources (Piringer,
1990; Marsden and House, 2006), in contrast to the dearth of publica­ 2017). Calcination is typically outsourced to lime producing companies,
tions on the use of lime in this important industry. This review, usually located some distance from the mining location. The calcination

* Corresponding author.
E-mail address: chris.duplessis@lhoist.com (C.A. du Plessis).

https://doi.org/10.1016/j.mineng.2021.107231
Received 8 July 2021; Received in revised form 18 September 2021; Accepted 22 September 2021
Available online 27 October 2021
0892-6875/© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

conditions, as well as the fuel used as energy source, significantly in­ provide loss on ignition values, upon heating to 950 ◦ C, on the fresh
fluence the properties of the resulting quicklime (Boynton, 1980). These quicklime shipment leaving its production site. From the loss on ignition
factors include the impact on quicklime porosity, reactivity, slaking value (to 950 ◦ C), the amount of residual CaCO3 (typically unburned
characteristics, and ultimately the Ca(OH)2 particle size generated after limestone) can be calculated (EN12485:2017; ASTM C25-17). As the loss
reacting with water (Zanin et al., 2019). The remote locations of most on ignition (to 950 ◦ C), or the difference between the loss-on-ignition up
mine sites make transport logistics a significant cost component, to 950 ◦ C and 550 ◦ C for “air-slaked” lime, is equivalent to the amount of
particularly given the fairly low cost of the lime raw material at the point CO2 liberated by decomposition of calcium carbonate, this value is
of production. Quicklime is typically used for long distance transport commonly also referred to as “CO2 content”. In the same fashion, the loss
because of its lower mass per unit of reactive ingredient, compared to of ignition upon heating to 550 ◦ C is commonly referred to as the “H2O
hydrate and slaked formats. content”, i.e. the water vapor liberated by decomposition of calcium
hydroxide. Analytical methods for characterizing lime, also include
3. Quicklime composition determination of quicklime reactivity (not shown in Table 1, because of
different determination methods used in different regions), measured by
Several similar international standard methods have been developed a temperature increase upon reaction with water. A rapid increase in
and are widely used to characterize lime reagents (AS 4489.6.1-1997; temperature indicates a higher reactivity. Reactivity is influenced by a
ASTM C25 – 19; EN, 2017). The parameter ranges of typical industrial range of factors, including the quicklime purity and the calcination
quicklimes are illustrated in Table 1, and the relevance of each briefly temperature (Boynton, 1980; Oates, 2008; Zanin et al., 2019). Lime­
discussed. stone calcination at 900⁰C results in highly reactive quicklime compared
The total CaO content is typically determined by X-ray fluorescence to ultra-low reactivity from calcination at 1,300 ◦ C. Reactivity loss from
spectroscopy (XRF) and is indicative of the calcium present in different calcination at increased temperatures is typically (Boynton, 1980)
mineral forms, mainly as quicklime (CaO). This metric is distinguished explained by sintering and grain growth and thus loss of reactive in­
from available CaO, determined by acid titration of a slaked sample. ternal surface area. As grain growth is thought to be driven by surface
The available CaO value is an indicator of the active reagent component diffusion during calcination, increased temperatures accelerate this
that is available for the target reaction and is, therefore, less than the process.
total CaO. A portion of the total CaO is unreactive, with this proportion Lime reagent utilization efficiency can be defined as the mass per­
increasing with calcination time and temperature (Boynton, 1980; Zanin centage of the lime reagent participating in the target reaction(s). Uti­
et al., 2019). Some magnesium is unavoidably present in virtually all lization efficiency is not generally explicitly determined in gold
quicklime, because of the inherent association of magnesium with cal­ processing operations, although it is an important consideration when
cium in limestone. The magnesium content of limestone is of lesser re­ comparing lime reagents and can readily be determined under labora­
agent value in gold processing than the calcium content. This is for a tory conditions, using relevant proxy reactions (Ineich et al., 2017). It
number of reasons: (1) MgO in lime is significantly less reactive than should be noted that although the available CaO content of lime pro­
CaO; (2) MgO cannot raise solution pH above 10.5, compared to 12.4 in vides an indication of potential active reagent, this metric is determined
the case of CaO; and (3) the reaction product of MgO in most gold for quicklime and does not take into consideration the factors that in­
processing applications is soluble MgSO4, which acts as a buffer against fluence slaking and thus the properties of the Ca(OH)2 particles. It is the
pH increases above 10.5, thereby increasing overall lime consumption. properties of hydrated Ca(OH)2 particles, rather than the starting
The silica and iron content of lime is typically low and inconsequential quicklime, that determine utilization efficiency. Lime utilization effi­
in gold processing, as it mainly remains inert. Most of the sulfur content ciency is, therefore, a combination of lime impurities, unreactive CaO,
originates from the calcination fuel used, rather than from the limestone. application inefficiencies and properties of the Ca(OH)2 particles
Sulfur containing fuels, therefore, increase the sulfur content of the lime. (Fig. 1).
An elevated sulfur content of lime, particularly if it exceeds 0.5 %wt may
have a detrimental effect during slaking of quicklime, as it has a 4. Dry quicklime versus slaked lime reagent use
coarsening effect on the slaked Ca(OH)2 particles (Potgieter et al., 2003;
du Plessis et al., 2020). Loss on ignition is defined as the weight loss due Lime reagent dosing methods in gold processing are typically
to thermal decomposition from heating to a defined temperature. For dependent on the extent of acid consuming reactions and the accuracy of
lime it typically covers two different metrics: Most commonly, it de­ pH control required. The simplest dosing format is where dry quicklime
scribes the loss on ignition up to 950 ◦ C, i.e. the weight loss is caused by (of particle size < 25 mm) is directly applied to ore on a conveyor-belt
the decomposition of both the calcium carbonate and calcium hydroxide ball mill feed via a dosing screw attached to a lime silo. The dosing
in the sample to quicklime (CaO). The other metric is the loss on ignition screw feed rate is controlled by a feedback mechanism based on the pH
up to 550 ◦ C, caused by the decomposition of calcium hydroxide to CaO. measurement in the cyanidation process unit. Such dosing methods are
This metric becomes important when a quicklime shipment has been typically applied in scenarios where the lime consumption demand of
exposed during transport, handling or storage and has reacted with air processed ore is relatively low (i.e. < 2 kg per ton of ore treated), pre­
humidity. This reaction decreases quicklime reactivity, as well as the dictable and stable. Lime dosing via this method is based on the ratio­
available CaO to a minor degree. A lime supplier will typically only nale that the ball mill provides sufficient agitation and residence time to
achieve slaking (i.e. hydration) of the quicklime into Ca(OH)2. A similar
dosing method is applied to gold heap leaching operations where dry
Table 1
quicklime is dosed directly from a silo, via a screw feeder, onto the ore
Parameter ranges of typical industrial quicklime.
on the back of a truck before the ore is stacked onto a heap (Kappes,
Parameter Range (%wt) 2002). The latter method does not provide for precise pH control or
Total CaO content 80–95 adjusting pH after lime has been added to the ore. Despite these limi­
CaO available 75–92 tations, such dry addition methods are relatively simple to implement
MgO 1–5
with minimal operational or capital cost. In most gold processing op­
SiO2 1–5
Al2O3 0.07–0.7 erations and applications, however, dry quicklime is slaked resulting in a
Fe2O3 0.08–0.4 suspension of Ca(OH)2 particles that can be pumped and dosed into
SO3 0.1–1.3 multiple process operations for flexible and accurate pH control. Slaking
Loss on ignition (LOI) 0.5–2.5 can be achieved in a variety of slaking reactors including ball mill
CO2 0.4–2.0
slakers, detention slakers, and stirred tank slakers (Oates, 1998).

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

Fig. 1. Illustration of mass step-down components from initial lime to that utilized in the application process.

5. Ca(OH)2 as active reagent format oxidation of zero valance metallic gold (Au0) into monovalent gold
(Au+), with which cyanide forms a stable complex [Au(CN)2]− , Reaction
A feature of virtually all non-pyrometallurgical gold processing is (1), referred to as aurocyanide. Calcium cyanide is less commonly used
that it occurs in aqueous media. In such conditions, Ca(OH)2 is always and then only where production occurs close to the point of use. This is
the active reagent component of lime, regardless of the format in which because dry powdered cyanide is prone to hydrolysis when in contact
lime is dosed into the process. Even in scenarios where dry quicklime is with most air, which causes release of HCN gas and the use of slurries/
used, the CaO does not directly react in target reactions. Instead, CaO solutions limit the economical transport distances of cyanided in this
first reacts with water (hydrates) to form slightly soluble (~1.4 g.l− 1) Ca format.
(OH)2 particles, or more precisely Ca2+ and OH− (Oates, 2008). It is the
4Au0 + 8NaCN + O2 + 2H2 O→4NaAu(CN)2 + 4NaOH (1)
soluble calcium (Ca2+) and hydroxide ions (OH− ), rather than the solid
Ca(OH)2, that participate in target reactions (Giles et al., 1993). Disso­ The cyanide reagent used in gold processing significantly exceeds the
lution of Ca2+ and OH− from the surface of solid Ca(OH)2 particles is the stoichiometric gold content in the ore/concentrate being treated. This is
limiting step in the reaction (Johannsen and Rademacher, 1999). Finer because most of the added cyanide is either consumed by unwanted side-
Ca(OH)2 particles result in improved kinetics and utilization efficiency, reactions (Bakatula and Tutu, 2016) and/or rendered ineffective due to
compared to larger Ca(OH)2 particles. Typically, a Ca(OH)2 particle size the pH-dependent HCN/CN− speciation of cyanide illustrated in Fig. 2a,
with d50 below 15 µm kinetically performs optimally, even though it is with a pKa of 9.2, Reaction (2). Importantly, CN− is the desirable species
rarely explicitly measured in gold processing plants. Ca(OH)2 particle for gold cyanidation leaching, thus requiring the pH of the solution to be
size is mainly determined by the following factors (Ineich et al., 2017): maintained, preferably above pH 10.5, where > 90% of the cyanide is
present as CN− , to enable the gold dissolution reaction. Below this pH,
• Reactivity of the lime (influenced by the calcination process condi­ soluble cyanide is increasingly present as hydrogen cyanide (HCN),
tions and fuel), with more reactive lime typically resulting in finer Ca which is ineffective as a leaching agent and prone to volatilization as a
(OH)2 particles (National Lime Association, 1995). highly toxic and hazardous gas (Perry et al., 1999). Chloride in saline
• Soluble elements contained in the slaking water, e.g. high concen­ gold processing solutions, ubiquitous in the Western Australian gold
trations (>500 mg.l− 1) of sulfate in the water will coarsen the milk of fields (Turner et al., 1994; Ali and Turner, 2004), causes a shift in
lime (Potgieter et al., 2003). equilibrium between HCN and CN− towards lower pH values (Verho­
• Operating temperature of the slaker, i.e. higher slaking temperatures even et al., 1990) (Fig. 2b).
(65–85 ◦ C) generally result in finer Ca(OH)2 particles (Zinck and
Aube, 2000). This phenomenon is particularly relevant for low [CN − ] 1
Mole fraction of CN − = = (2)
reactivity lime, but less relevant for higher reactivity lime. For a [HCN] + [CN − ] 10(pK a − pH) + 1
continuous production process, the slaking temperature is primarily The cost of cyanide is typically a major expense for many gold op­
controlled by the lime-to-water feed ratio of the slaker (typically at erations. The use of lime, therefore, enhances the utilization efficiency of
mass ratio of 1:8 to 1:4) and the reactivity of the lime. cyanide via pH modification. In scenarios where process solutions are
• Extent of mechanical abrasion or comminution during or after buffered, often with dissolved magnesium (detailed in the next section),
slaking. Some slakers, for example, make use of comminution the lime reagent requirement to attain a pH level higher than 10.5 be­
methods (as in ball mill slakers) to reduce the particle size of the comes a high operating cost component. Under such conditions, oper­
slaked lime. This is particularly used in scenarios, where other fac­ ational lime-cyanide trade-off decisions have to be made weighing up
tors would otherwise result in coarse Ca(OH)2 (Gärtner and Diaz the cost of: (a) operating at a pH level of 10.5 with increased lime re­
Chavez, 2019). agent to increase the cyanide utilization efficiency (and thereby the cost
efficiency) compared to (b) operating at a pH of, say, 9 (below the
6. Cyanide as driver for lime use buffering capacity of magnesium) saving on lime reagent but increasing
cyanide consumption due to lower utilization efficiency.
The use of cyanide as the predominant gold lixiviant reagent, Re­
action (1), is the key driver for the use of lime in gold processing (Perry 7. The main alkali consumption reactions in gold processing
et al., 1999). Cyanide, commonly used in the form of sodium cyanide (at circuits
solution concentrations ranging from 200 to 600 mg.l− 1 or dosages of
0.1 to 1.0 kg per ton of ore (in the case of non-refractory ore), acts as a In the absence of alkali consuming reactions, the relationship be­
lixiviant for gold in the presence of oxygen, where oxygen facilitates tween Ca(OH)2 concentration and solution pH is illustrated in Fig. 3.

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

Fig. 2. CN− and HCN speciation as a function of pH (a) and CN− speciation at different chloride concentrations (b).

which the return water is used as process water, and within the process
circuit before sufficient lime reagent has been added to achieve the
target pH for cyanidation. Once magnesium is in solution, usually with
sulfate as the counter-anion, it buffers the pH and consumes alkali when
upward control of pH is required. This soluble magnesium starts reacting
with lime, Reactions (5a) and (5b), from pH 9.3 to 9.5, and continues to
consume lime until a pH of 10.5 is reached (Ineich et al., 2017). Stoi­
chiometrically, each ton of dissolved Mg2+, will consume 3.1 tons of Ca
(OH)2 (equivalent to 2.3 ton of CaO). An important consideration for
plant operators is to conduct an inventory of dissolved magnesium input
into the entire plant water circuit. If magnesium inputs into the water
circuit can be minimized, the lime-cyanide trade-off consideration
mentioned earlier may favour an operational pH > 10.5. Initial lime
consumption in the process circuit may be high, as the initial process
water inventory of magnesium is precipitated from solution, but would
subsequently be reduced to the extent that further magnesium input into
the water circuit can be minimized. If soluble magnesium is continu­
ously and unavoidably entering the solution circuit at high concentra­
tions, the resulting high lime consumption it would induce (as well as
the increased viscosity due to precipitation of large quantities of Mg
(OH)2 and CaSO4⋅2H2O) may force a plant to operate at pH values in the
Fig. 3. Indicative relationship between soluble Ca(OH)2 concentration and pH
in an unbuffered solution (maximum solubility of Ca(OH)2 at ambient condi­ range 9.0–9.2 (Costello, 1986) to avoid this reaction, and incur higher
tions is approximately 1.4 g.l− 1). cyanide consumption instead.
MgSO4 + Ca(OH)2 + 2H2 O→Mg(OH)2 + CaSO4 .2H2 O (5a)
Empirically the relationship can be estimated from reactions (3) and (4),
where Ca(OH)2 concentration is in grams per liter, within the pH range MgCl2 + Ca(OH)2 →Mg(OH)2 + CaCl2 (5b)
7–12 and soluble Ca(OH)2 concentration < 1 g.l− 1. These empirical
Acid generation from pyrite oxidation – The presence of pyrite
equations generally fit the Ca(OH)2 versus pH titration curve better than
(FeS2) or other sulfide minerals results in acid generation when exposed
the theoretical calculation based on the OH− concentration, in unbuf­
to water and oxygen, Reaction (6). This reaction may occur within the
fered solutions (Lhoist internal data).
processing plant, in waste dumps or in tailings storage facilities (Dold,
Ca(OH)2 = e(pH− 12.05)
(3) 2014), and may be significantly accelerated by the presence of bio-
catalytic microbes (Duncan et al., 1967; Livesey-Goldblatt, 1986). The
[ ]
pH = ln Ca(OH)2 + 12.05 (4) acid from this reaction is neutralized by lime resulting in the formation
of gypsum precipitate, Reaction (7). Stoichiometrically, each ton of
In addition to raising the pH to the operational setpoint for optimal oxidized pyrite requires 1.24 tons of Ca(OH)2 (equivalent to 0.93 ton of
cyanidation, lime is also required to neutralize and counter acid- CaO). The fact that gypsum precipitates in the process means that both
generating reactions or to overcome the effects of dissolved pH- the sulfate anion in sulfuric-acid and alkali cation are removed from
buffering elements. The main lime consuming reactions that, in com­ solution, thus preventing their accumulation in the circuit. This is an
bination, contribute to the overall lime consumption of gold processing important distinguishing feature of using lime as alkali reagent. By
plants, are briefly discussed: comparison, the use of any sodium-based neutralizing reagent leaves the
Magnesium pH buffering – Magnesium is an abundant element sodium soluble and without a chemical precipitation sink within the
contained in gangue ore minerals (Chryssoulis and McMullen, 2016) and processing circuit. Sodium can, therefore, only exit the circuit via un­
in process solutions. Magnesium is solubilized at pH levels below 9.5 and controlled seepage from tailings storage facilities (Zhang et al., 2020),
particularly under more acidic conditions. Conditions conducive to unless deliberately removed from a side-stream by evaporation or
magnesium dissolution may occur in tailings storage facilities, from

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

reverse osmosis with the concentrate brines contained or treated, pro­ phosphonates, polyacrylate or polyacrylate-polymaleate (Alfano and
cesses that are generally uneconomical for these applications. Apart Boffardi, 1994).
from cost factors, the operational trade-off decision, between using
calcium versus sodium alkali reagent (or other alkalis such as potassium 8. Lime interaction with activated carbon
or magnesium), is based on the following two options: (1) removal of
most cations and anions from solution and dealing with the disposal of Adsorbing cyanide-solubilized gold onto activated carbon was a
precipitated gypsum and metal hydroxides, compared with (2) dealing critically important development step in gold processing (Nicol et al.,
with soluble sodium sulfate as reaction product, that cannot readily be 1984a, 1984b, 1984c) and played a significant role in expanding gold
removed from solution. Pyrrhotite also occurs in some gold ores and is a production. Lime and the consequences of its use, also play an important
significantly more reactive iron sulfide mineral than pyrite. The net acid role in the performance of this process step and are briefly summarized.
generation, and therefore the lime consumption effect of its oxidation, is Adsorption onto activated carbon – Cyanidation results in gold
dependent upon a number of complex factors, including the ratio of solubilized as negatively charged aurocyanide [AuCN2]− . Activated
contained iron to sulfur, the extent of oxidation of iron and sulfur, and carbon has no surface charge and does not adsorb aurocyanide as a
the nature of precipitation products (Belzile et al., 2004). negatively charged gold-cyanide ion complex. The predominance of
dissolved Ca2+ from the use of lime, despite the addition of cyanide in
4FeS2 + 15O2 + 14H2 O→4Fe(OH)3 + 8H2 SO4 (6)
the sodium form, results in the formation, Reaction (9), of a weakly-
soluble calcium aurocyanide non-ionic covalent coordination complex,
Ca(OH)2 + H2 SO4 →CaSO4 .2H2 O (7)
Ca[Au(CN)2]2, that adsorbs onto the surface of activated carbon
Reactions with clays contained in laterites - Substantial gold (Davidson and Sole, 2007). The degree to which the aurocyanide com­
mineralization occurs in some relatively shallow weathered tropical plexes are adsorbed follows the series Ca > Mg > Li > Na > K, with
laterites (Colin and Vieillard, 1991; Larizzatti et al., 2008; Kioe-A-Sen calcium aurocyanide most strongly adsorbed (Davidson, 1974). The
et al., 2016). Due to extensive weathering over geological time, such reasons for this phenomenon could be inferred from fundamental studies
laterites contain an abundance of hydrated alumina and silica, often in conducted on highly ordered pyrolytic graphite (HOPG) (Poinen et al.,
clay-like format (Obonyo et al., 2014). The reactions of hydrated lime 1998) that found Ca2+ to have a higher charge-to-size ratio than Na+
with clays contained in weathered laterites is well known in civil engi­ and K+, and a higher coulombic attraction for aurocyanide anions, once
neering soil stabilization applications (Little, 1987; Transportation intercalated amongst the graphene layers.
Research Board, 1987). In the context of gold processing, the available [ ]− [ ]
time frame determines the most relevant lime consuming reactions with 2 Au(CN)2 + Ca2+ → Ca Au(CN)2 2 (9)
this ore material. The relatively short time period (i.e. hours), from lime Scaling on activated carbon – The precipitation of calcium car­
addition to cyanidation leaching occurring in a gold processing plant, bonate, referred to earlier, Reaction (8), also occurs on activated carbon,
causes cation exchange capacity interactions to be the most prominent causing surface fouling and reducing adsorption capacity (Davidson
lime consuming phenomenon (Little, 1987). When lime is added to such et al., 1979; Cevallos Toledo et al., 2020). Calcium carbonate scaling
clay-containing laterite slurries, the divalent calcium cation displaces occurs on the outer surface of activated carbon particles, thereby pre­
most other cations already adsorbed onto the negatively charged clay venting both adsorption and elution of gold from the internal meso- and
surfaces. Ca2+ displaces all of the cations to its left in the Lyotropic series micro pores (Fig. 4) that generally have a surface area exceeding 400 m2.
(Little, 1987): Li+ < Na+ < H+ < K+ <NH4+ ≪ Mg2+ < Ca2+ ≪ Al3+. g− 1 (McDougall, 1991). Most commercial activated carbon has a specific
Once adsorbed onto the clay surface, the calcium cations act to adsorb surface area of 800 to 1200 m2.g− 1, which is predominantly contained
negatively charged hydroxyl anions. The net effect is that clay minerals within micropores <2 nm in diameter. To counter this effect, a portion
adsorb both Ca2+ and OH− from solution, thus increasing the con­ of the activated carbon inventory is continuously subjected to an acid
sumption of Ca(OH)2 added to the process. The clays contained in washing step, to reverse the CaCO3 scaling effect. Acid washing is
laterite gold ores effectively act as a physico chemical adsorption buffer typically conducted using either hydrochloric or nitric acid at 3% con­
against lime-induced pH increase to a level optimal for cyanidation centration for 20 to 60 min at ambient temperatures, although some
leaching. Such ores have been reported to consume lime to levels as high plants use more aggressive temperature conditions (i.e. 60 ◦ C). In in­
as 12 kg per ton (IAMGOLD, 2018). Over extended time periods, as dustrial practice, acid washing is commonly conducted before gold
prevails in tailings storage facilities, pozzolanic-type reactions of resid­ elution, i.e. with the aurocyanide present on the activated carbon
ual lime with silica and alumina clay minerals may occur to form cal­ (Stange, 1999). Acid washing makes the elution more efficient as it al­
cium silicate hydrate (CSH), CaO.SiO2⋅H2O, and calcium aluminate lows aurocyanide, adsorbed in the internal pores of the activated car­
hydrate (CAH), CaO.Al2O3⋅H2O, respectively (Attoh-Okine, 1995; Fir­ bon, to be eluted for subsequent electrowinning.
oozi et al., 2017; Saing et al., 2017). One way to reduce calcium carbonate formation is to reduce carbon
Carbonation – The fact that the cyanidation reaction requires oxy­ dioxide input by sparging pure oxygen rather than air into the cyani­
gen, Reaction (1), necessitates the introduction of either pure oxygen dation process, although at significant cost. An alternative is to use lime
gas, active air sparging, or passive aeration in the case of gold heap in a CO2 scrubbing system, Reaction (8), (Samari et al., 2020) prior to
leaching operations. The contained CO2 in air dissolves into solution sparging the scrubbed air into the cyanidation reactor.
from the liquid/air contact and reacts with lime to form calcium car­
bonate, Reaction (8), although this is the smallest contributor to overall 9. Lime use in gold processing flow sheets
lime reagent consumption. The product of this reaction is more relevant
than the reagent consumption effect, because of the operational impli­ The diversity of gold ores has given rise to many process flow sheet
cations of calcium carbonate precipitate formation and very low solu­ configurations (La Brooy et al., 1994). Lime reagent consumption is
bility (<50 mg.l− 1) (Plummer and Busenberg, 1982). determined by the ore characteristics rather than the small fraction of
CO2 + Ca(OH)2 →CaCO3 + H2 O (8) contained gold. From a lime consumption perspective, hydrometallur­
gical gold processing can broadly be classified using three ore features:
Calcium carbonate causes scaling effects that manifest most prob­ (1) gold grade, (2) copper mineral content and (3) pyrite content, as
lematically on the surface of activated carbon, which is used to adsorb illustrated in Table 2, with typical lime consumption ranges given as a
the aurocyanide complex from solution (discussed in more detail in the function of ore feed (Lhoist data). The combination of these features
next section). General carbonate scaling in plant circuits may be influences the lime consumption relative to gold production output.
addressed using anti-scalants such as polyether polyamino methylene

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

Fig. 4. Diagrammatic representation of a carbon granule section (left) and scanning electron micrograph (right) of an extreme case (not typical of industrial op­
erations) of calcium carbonate (CaCO3) precipitate scaling on activated carbon particle surface (courtesy Lhoist R&D).

a free-milling ore is illustrated in Fig. 5. In most plant circuits, gravity-

Table 2
recoverable gold is catered for in the flow sheet, as this fraction of the
A simplified empirical representation of the three main ore characteristics (gold
gold incurs the least operational effort (Bath et al., 1973; McGrath et al.,
grade, copper content and pyrite content, at high H, medium M or low L relative
concentrations) influencing the choice of gold processing method and impact on
2018; Lowes et al., 2020). The gravity recoverable gold process is not
typical lime consumption. lime-intensive and is, therefore, not discussed here. This flow sheet
(Fig. 5) is typical for ores with reasonable gold grade (i.e. > 1 g Au per
Processing flow sheet Gold Copper Pyrite Lime consumption
method grade content content (kg.t− 1 of ore)
ton ore) and have sufficiently low concentrations of iron and copper
sulfide minerals that do not interfere with the processing in terms of
Simple tank leaching H L L 0.8 to 1.5
cyanide consumption or copper dissolution. Lime is added, usually in
Tank leaching with H M L 0.8 to 1.5
nuisance copper dry quicklime form, to crushed ore via a screw feeder from a lime silo
Copper-gold H H L 0.2 to 0.8 onto the conveyor belt feed of a ball mill. Lime dose rates are typically
sequential relatively low, i.e. 0.5 – 2 kg per ton of dry ore feed. Process water is also
flotation fed into the mill together with the crushed ore to facilitate milling at the
Conventional heap L L L 1 to 5
leaching
appropriate solids concentration and viscosity that are suitable for direct
Refractory treatment H L H 2.5 to 10 cyanide leaching. This method of lime addition relies on lime slaking (i.
processes e. hydration) occurring within the ball mill, where the residence time
and attritioning effect is adequate for hydration of CaO to Ca(OH)2. In
circuits that use dilute comminution, where the mill classification
Each of the main processing flow sheet methods is discussed in more
product solids content is too dilute for direct cyanidation, a thickening
detail, with specific reference to lime consumption.
stage (not shown in Fig. 5) is used to increase the concentration to
around 50 %wt (depending on viscosity limitations) before cyanidation.
9.1. Simple tank leaching Some lime may be used to facilitate flocculation in the thickener
(Stange, 1999), although such lime addition requires slaking for effec­
The simplest (and commonly occurring) flow sheet configuration for tive use. In the leaching circuit, the ore slurry, commonly referred to as

Fig. 5. Simplified process flow sheet of uncomplicated gold process with gravity recovery followed by cyanidation. Variations of this flow sheet include ore directly
to milling (i.e. no crushing), lime addition after the milling step, and the use of resin instead of activated carbon.

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

“pulp”, is then subjected to leaching in a series of sequential agitated range of copper–cyanide complexes, thereby consuming more cyanide
cyanidation tanks, to which cyanide is added and air is sparged into, to than is necessary for gold leaching only. The copper–cyanide complexes
enable gold leaching (Adams, 1989). Once solubilized, gold adsorption are also quite stable under typical tailings conditions, when compared to
occurs in a separate series of agitated tanks, in the case of carbon-in-pulp free cyanide. These complexes compete with and reduce gold adsorption
(CIP) processing. In these tanks, activated carbon flows counter-current onto activated carbon (Dai and Breuer, 2009). This phenomenon also
to the flow direction of the pulp, with screens used to separate the causes a range of operational problems including the increase of cyanide
mineral pulp from the gold-loaded activated carbon. In some scenarios content in the leached tails and contamination of the final dore gold
the processing flow sheet may be configured to facilitate aurocyanide metal, amongst others (Shantz and Reich, 1978; Nguyen et al., 1997;
adsorption onto activated carbon simultaneous with (i.e. in the same Kyle and Hefter, 2015; Bakatula and Tutu, 2016). The sulfidization
vessels as) the leaching process, a process known as carbon-in-leach acidification recycle thickening (SART) process, is a way to deal with
(CIL). This technique is used where particular characteristics of the such copper and high cyanide consumption in gold processing circuits.
ore increase the risk of gold loss by so-called preg-robbing or preg- SART has been incorporated in a variety of flow sheets, since its first
borrowing (Dunne et al., 2012; Snyders et al., 2017). Preg-robbing re­ installation at the Telfer gold mine in Western Australia, including tank
fers to the phenomenon where cyanide-solubilized gold is adsorbed onto and heap leaching operations (Barter et al., 2001; Adams et al., 2008;
carbonaceous components contained in the mineral being treated, Stewart and Kappes, 2012; Estay et al., 2018). A simplified diagram of
thereby “robbing” the pregnant solution of its soluble gold and the main flow sheet components of SART processing of the cyanidation
rendering it unrecoverable. Some make-up lime may also be added to tailings solution is illustrated in Fig. 6, although several variants have
the cyanidation tanks for minor pH adjustment to maintain the target pH been deployed. The most stable, and therefore most prevalent, cop­
during cyanidation. Some plants perform milling in circumneutral pH per–cyanide species at typical gold-process operational pH (i.e. 9 – 11) is
(or the prevailing pH according to the water source) and add slaked lime [Cu(CN)3]2− , with copper in the cuprous valance state (Cu+). The first
slurry only to the cyanidation section. step of the SART process (i.e., sulfidization) is based on the high affinity
of sulfide for copper, resulting in a very low solubility of copper sulfide
precipitate (Ksp = 2.3 × 10− 48) (Lewis, 2010; Estay, 2018). Using this
9.2. Nuisance copper treatment
phenomenon under acidic conditions (pH 4–5) allows for cyanide to be
displaced from [Cu(CN)3]2− by sulfide reagents (NaSH or H2S) while
All sulfide minerals react with cyanide, although to varying extents
cyanide is protonated to HCN, Reactions (10) and (11), (Buisman and
(Aghamirian, 1997; Deschênes et al., 2002), with copper minerals
Dijkman, 2005; Adams et al., 2008). Acidification also promotes the
generally having a more detrimental impact on gold recovery. Some
breakage of the Cu-cyanide complex, as well as other weak acid disso­
gold ores contain significant concentrations of copper minerals, (such as
ciable (WAD) cyanide complexes with Zn, Ni, Ag, and Hg that may occur
chalcocite, covellite, bornite, cuprite, chrysocolla, enargite, tetrahe­
(Estay, 2018). The process results in the precipitation of Cu2S that is
drite, malachite and azurite) that are cyanide-soluble and significantly
subjected to a thickening step to concentrate it, and releases cyanide
complicate the gold recovery (Kyle and Hefter, 2015), referred to as
back into solution as aqueous hydrogen cyanide (HCN). The thickened
“nuisance copper”. The main reason for this “nuisance” is because such
underflow, with the addition of NaOH, is filtered to produce the final
copper minerals often occur in much greater quantities (even if not in
Cu2S product. NaOH is used to increase the pH well above the 7.2 pKa of
economic quantities) than gold and therefore result in significant cya­
H2S/HS− , preferably to pH 10, to reduce the risk of H2S evolution from
nide consumption. The front-end flow sheet configuration for gold ores
the Cu2S product. Lime can also be used for this purpose, but will result
with nuisance copper is typically the same as illustrated in Fig. 5.
in gypsum co-precipitation in the product, that negatively affects the
Gravity gold is also often extracted, although the presence of native
saleability of the Cu2S product.
copper may also cause complications. Gold ores with nuisance copper
differ from free-milling oxide ores in the back-end treatment of the 2Na2 Cu(CN)3 + H2 S + 2H2 SO4 →Cu2 S + 6HCN + 2Na2 SO4 (10)
cyanide-leached slurry. Cyanide reacts with copper minerals to form a

Fig. 6. Simplified block flow diagram of the SART process components.

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

4Na2 Cu(CN)3 + 2NaSH + 5H2 SO4 →2Cu2 S + 12HCN + 5Na2 SO4 (11) Medina and Anderson, 2020). In scenarios where gold is preferentially
associated with pyrite, methods are required to separate copper minerals
The acid solution, from both the Cu2S thickener overflow and Cu2S from gold-bearing pyrite. Though many different flow sheet combina­
filtration step, containing HCN is neutralized using lime, typically in an tions have been used commercially, a simplified block flow diagram of a
agitated reactor under slight negative pressure. This process step is used typical flow sheet is illustrated in Fig. 7, showing the main lime addition
to both neutralize the acid, Reaction (7), and to increase the pH to fully points. Lime is added to the copper rougher flotation, typically to control
convert HCN back to CN− , Reaction (12). The resulting gypsum the pH at approximately 9–10. Pyrite floats readily in acid and neutral
(CaSO4⋅2H2O) is thickened, filtered and disposed to tailings, while the conditions with xanthate as collector, while high pH values depress
high pH treated solution, containing CN− , is recycled back to cyanida­ pyrite (Mu et al., 2016). Additionally, the high pH is also necessary
tion. The main factors governing lime consumption are: (1) the quantity because the oxidation of pyrite would otherwise cause a pH decrease in
of acid used and (2) the buffering elements contained in solution. It the copper rougher circuit, Reaction (6). Such a reduction in pH would
should also be noted that the SART process contains two important facilitate some copper dissolution, causing copper activation of pyrite
gaseous hazards, HCN and H2S, both of which are pH species dependent, making it difficult to depress the pyrite (Zanin et al., 2019). In the Cu
that require scrubbing (not shown in the diagram) and careful cleaner stage, the objective is to float and produce a high-grade copper
management. concentrate, while the gold-containing pyrite is depressed (i.e. rejected
to tails) (Bulatovic, 1997). This separation is pH dependent and typically
2HCN + Ca(OH)2 →Ca(CN)2 + 2H2 O (12)
requires a pH of 11, achieved by further lime addition (Akop, 2014;
Zanin et al., 2019). The tails from this process report to the pyrite
9.3. Cyanide recovery by acidification, volatilization and recovery (AVR) flotation circuit where pyrite is reactivated (i.e. the depression effect is
reversed so that it will float), typically using potassium amyl xanthate
The AVR process, or different versions thereof, such as CRP (cyanide (PAX). The gold-containing pyrite concentrate then reports to the cya­
recovery process) and Cyanisorb, may be used to recover cyanide from nidation circuit for gold leaching and recovery (Benson et al., 2007;
process solutions with total cyanide concentrations exceeding 150 mg Akop, 2014).
l− 1, for re-use (Riveros et al., 1993; Stevenson et al., 1998). The process The copper concentrate inevitably contains some gold, of which the
is generally more suitable to solutions rather than mineral slurries value is mainly lost commercially, while the gold-bearing pyrite
(Fleming, 2016). It can be used to recover cyanide from solution streams concentrate unavoidably also contains some copper minerals (Bulatovic,
exiting the SART process, or as a standalone unit in scenarios where 1997). The cyanidation of such gold-bearing pyrite, with residual copper
residual cyanide (i.e. after cyanidation leaching) is not significantly minerals, incurs a high cyanide consumption due to undesirable side-
complexed by copper. In the AVR process, sulfuric acid is added to the reactions of cyanide with these copper minerals, as elaborated in the
alkaline cyanide containing solution to reduce the pH below 7, thereby previous section (Zhang et al., 1997; Kianinia et al., 2018), including
converting contained cyanide to HCN. If cyanide is mainly present as reactions that result in cyanide-soluble copper such as [Cu(CN)3]2− . A
WAD cyanide, a pH of 4 is required. The HCN is stripped or vapourised high concentration of cyanide-solubilized copper poses operational
from the acid solution. The stripped acid solution is treated with lime difficulties that may warrant explicit treatment as outlined in the
reagent, to increase the pH to a suitable level for re-use within the description of the SART process.
processing plant and to precipitate soluble metals as hydroxides. The
extent of lime use is dependent upon the acid addition used, as well as 9.5. Heap leaching of low-grade (uncomplicated) ore (low pyrite and
the quantity and extent of metal precipitation required. The HCN vapour copper mineral content)
is recovered by scrubbing into a NaOH solution. The cyanide concen­
tration in the scrubbing solution can be built up to almost 100 g.l− 1 as a Heap leaching and dump leaching are well-known metallurgical
maximum operational limit (Fleming, 2016). Lime may also be used in processing methods used to extract gold from low-grade ore (Kappes,
the HCN adsorption scrubbing unit, if sufficient measures are taken to 2002). This method is typically used for ore containing <1 g gold per
overcome scaling. The net effect of using the AVR is that both WAD and metric ton of ore where the contained gold value does not warrant the
free cyanides are separated and recovered from process solution streams increased cost of milling, flotation and subsequent use of tank leaching
for re-use in the cyanidation leaching step. methods (Petersen, 2016). Stacked ore heaps vary in height from 6 m to
20 m and may contain several lifts. Heaps are typically constructed using
9.4. Sequential flotation recovery of copper and gold containing ore run-of-mine ore or crushed-and-agglomerated ore. The decision to crush
ore is dependent upon the natural liberation of the run-of-mine (ROM)
Orebodies that contain both copper and gold in economic quantities, ore compared with crushed ore and takes into consideration the cost of
require flow sheet configurations tailored to their specific circum­ crushing and its impact on the hydraulic percolation properties of a
stances. The factors affecting the optimal configuration are: (1) the heap. The objective of heap leaching is to provide a low-cost method of
extent to which gold is associated with copper minerals or pyrite min­ contacting cyanide solution with ore surfaces containing liberated gold
eral, (2) the payable value of gold contained in the copper concentrate, particles. The basic process components of a heap leaching circuit with
and (3) country regulatory policies. The latter is relevant because low sulfide content, is illustrated in Fig. 8 (for simplicity, the elution,
regulation in some countries may compel companies to recover the full acid washing, activated carbon regeneration and electrowinning process
value of contained metals before exporting. The payable gold contained
in copper concentrate is a function of the treatment charges – refining
charges (TC-RC) that the mine operator can contractually secure for its
copper concentrate (Malewski, 2016; Díaz-Borrego et al., 2019). Gold
contained in copper concentrate is not payable at full value and, in some
instances, attracts zero payable value. This provides a powerful incen­
tive for mining companies to consider implementing process flow sheets
that separately generate a copper concentrate as well as a gold value
stream.
Copper-gold process flow sheets typically involve the combination of
complex flotation circuits, combined with subsequent cyanidation Fig. 7. Simplified process units for sequential flotation recovery of copper and
leaching for gold recovery (Benson et al., 2007; Zheng et al., 2010; gold-bearing pyrite concentrates.

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

9.6. Refractory gold

The term “refractory” in this context refers to gold ores from which
gold is not readily recoverable by direct lixiviant leaching, such as cy­
anide leaching (Asamoah et al., 2019; Asamoah, 2021). Several factors
may cause this poor recovery, such as the presence of so-called “preg-
robbing” carbonaceous minerals (this means the gold leaches with cy­
anide, but it is re-adsorbed onto a component of the ore). Most refractory
gold ores, however, are deemed refractory because the fine gold parti­
cles are contained and occluded within a matrix of sulfide minerals,
most commonly pyrite (FeS2) or arsenopyrite (FeAsS), or when the gold
is in solid solution with other minerals, typically sulfide minerals. Such
gold is typically not sufficiently liberated by milling and is therefore not
sufficiently accessible to lixiviants. If gold liberation can be achieved,
Fig. 8. Simplified heap leaching circuit components. the presence of pyrite has a limited impact on cyanidation gold recovery
(Deschênes et al., 2002), because of the minimal direct reaction of pyrite
components are not shown). The cyanide solution (typically containing with cyanide to produce thiocyanate, SCN− , Reaction (13), (Kianinia
300–500 mg.l− 1) is irrigated onto the heap surface (at irrigation rates et al., 2018).
ranging from 10 to 18 l.m− 2.h− 1) allowing it to flow via gravity though
4FeS2 + 8NaCN + 3O2 + 6H2 O→8NaSCN + 4Fe(OH)3 (13)
the ore channels and pores, acting as a lixiviant for gold (Kappes, 2002).
Cyanide solution flow occurs as unsaturated percolation, meaning that To overcome the problems posed by refractory gold, pretreatment in
flow channels and pores are not saturated with solution, thereby the form of oxidative destruction (also referred to as pre-oxidation) of
allowing air ingress carrying oxygen for the cyanidation reaction with the occluding sulfide mineral, or ultrafine grinding (UFG), is required to
gold, Reaction (1). Dissolved aurocyanide reports to the pregnant leach enable sufficient gold liberation for cyanidation (as long as the gold is
solution from which it is recovered by carbon adsorption. The leach not in solid solution, i.e. invisible as a separate phase, when viewed with
solution is relatively free from mineral particulates. This allows the use a scanning electron microscope). UFG of pyritic concentrates for sub­
of carbon-in-column (CIC) adsorption columns (Heinen et al., 1978) that sequent leaching is used in ores where refractoriness to direct cyanida­
reduce activated carbon attrition and the problem of activated carbon tion arises from fine to ultrafine (0.02 – 20 μm) gold mineral inclusions
fines. in the pyrite and/or arsenopyrite (Ellis and Gao, 2003). Several well-
To facilitate the cyanide leach process, an elevated pH within the known pretreatment process options have been implemented commer­
heap is generally achieved by direct dry addition of quicklime (CaO) to cially, all of which involve the pre-oxidation of the sulfide mineral either
the ore via a screw feeder from a silo directly onto the ore on the back of via pyrometallurgical roasting or hydrometallurgical methods (La Brooy
dump trucks before they tip the ore to stack the heap. For mechanized et al., 1994; Aylmore and Jaffer, 2012; Marsden and House, 2006). All
stacking, the lime is transferred from a silo directly onto one of the these pre-treatment methods involve the oxidation of the concentrate
conveyor belts. Using this direct addition method, the quicklime is (typically pyrite or pyrite and arsenopyrite), resulting in acid genera­
incorporated into the stacked ore bed, although not well dispersed tion, while subsequent cyanidation occurs at elevated pH conditions.
within the ore. Added to the ore in this manner, the lime does not pro­ This acid-generating feature of refractory ore processing is the main
vide for ideal contact with the percolating cyanide solution. Solution driver for high lime reagent consumption. Each of the main refractory
flow channels are uneven and often not well distributed, particularly ore pre-oxidation methods, and their impact on lime consumption, are
with run-of-mine rather than crushed-and-agglomerated ore (Bouffard discussed in turn.
and Dixon, 2007; Ghorbani et al., 2016). This means that solution flow
may by-pass quicklime-containing niches within the ore, reducing the 9.6.1. Roasting of refractory ore
utilization efficiency of the added lime reagent. Typically lime additions Pyrite (FeS2), as well as arsenopyrite (FeAsS), roasting is a well-
range from 1 to 3 kg per ton for ores containing low sulfide content, but known technology occurring at temperatures between 600 and 1000
may increase with increasing pyritic sulfur content. A general phe­ ◦
C (Runkel and Sturm, 2009). In addition to reactions (14) and (15),
nomenon of gold heap leaching is that the pH of the pregnant leach various reactions occur during the roasting process, depending on the
solution emanating from the bottom of a heap, has a lower pH than the operating temperature and oxygen partial pressure. Roasting is a
irrigation solution applied to the surface. The reason for the pH gradient preferred option for treating refractory ores also containing carbona­
is because of the alkali consuming reactions within the heap, Reactions ceous matter that causes preg-robbing effects (Afenya, 1991). The
(5)–(8). As the solution percolates it encounters the cumulative alkali roasting process effectively converts the contained sulfide minerals to
consuming demand of the ore, thereby resulting in a pH gradient. This SO2 gas, and carbonaceous matter to CO2 gas, thereby expelling both
pH gradient, in turn, impacts the speciation of cyanide, resulting in a sulfur and carbon from the treated material and enabling subsequent
reduction in the fraction of cyanide available in desirable CN− form. The conventional gold cyanidation leaching of the mineral residue
overall impact of the unfavourable cyanide speciation, down the heap, is (Fernández et al., 2000). The roasting of ores containing arsenopyrite
dependent on the cyanide concentration and pH prevailing in the presents greater difficulties than straight pyritic ores mainly because of
percolating solution. Lime addition to the pregnant solution before the tendency toward the formation of insoluble arsenites and arsenates,
carbon adsorption is not typically practiced because an increased pH which have a detrimental effect on gold recovery. In addition to arsenic
(from 9 to 11 for example) has a detrimental effect on both the rate and trioxide (the basis for arsenites), arsenic pentoxide may also form
capacity of aurocyanide adsorption onto activated carbon (Fleming and (which reacts with metal oxides to form arsenates). Ferric arsenate is
Nicol, 1984). However, lime addition is practiced in circumstances particularly problematic and is to be avoided, as it forms a non-porous
where: (1) adsorption carbon columns are enclosed within buildings layer that tends to occlude the gold in the calcine and reduces subse­
(typically to protect against winter freezing conditions) to reduce the quent recovery of gold. To prevent this, the arsenic removal stages are
safety hazard of HCN and (2) to precipitate dissolved elements in the normally done in an oxygen-deficient roasting stage. As the sulfur and
pregnant liquor that may interfere with aurocyanide adsorption onto arsenic removal optimally requires two different levels of oxygen partial
activated carbon. pressure, a two-stage roast is typically performed (Thomas and Cole,
2005).

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

4FeS2 + 11O2 →2Fe2 O3 + 8SO2 (14) As the reaction, Reaction (18), proceeds, the resulting NaOH causes an
increase in pH that further inhibits the dissolution of calcium and hy­
2FeAsS + 5O2 →Fe2 O3 + As2 O3 + 2SO2 (15) droxide ions from solid particles when the pH exceeds 12. This pH is
reached with as little as 0.4 g.l− 1 of NaOH. Practically it means that the
SO2 emissions directly to atmosphere pose obvious environmental
process only works effectively if the pH of the reaction is limited to 11.8
hazards and although this has been a past practice at many roasters,
(Bezuidenhout et al., 2012), thus requiring a large volume of dilute
particularly in remote locations, its use is being increasingly phased out.
solution circuit inventory. More importantly, under these conditions the
The presence of trace amounts of volatile mercury, arsenic and volatile
solubility of gypsum is greater than that of Ca(OH)2 (Hansen and
heavy metals have also proven to add to the challenges of roaster gas
Pressler, 1947), thereby constraining the forward reaction. This limita­
handling (Nyavor and Egiebor, 1991; Hylander and Herbert, 2008,
tion makes the dual alkali scrubbing process impractical for large-scale
Department of Environment and Conservation, Air Quality Management
refractory gold operations that may generate hundreds of tons of SO2 per
Branch, Government of Western Australia, 2010; Martin et al., 2014).
day.
Various process strategies have been deployed to deal with the resulting
Conversion to sulfuric acid – In most modern roasting plants, SO2 is
SO2 gas emissions, ranging from adsorption and chemical reaction
converted into sulfuric acid and sold as a reagent for other applications.
processes to conversion into sulfuric acid as a saleable product. The main
The conversion process is based on three main process steps (Crundwell
process strategies that have been used to treat roasting SO2 off-gasses are
et al., 2011): (1) cooling, cleaning and drying of gases, (2) catalytic
briefly outlined below, with specific reference to implications for lime
oxidation of SO2 to SO3 with oxygen, and (3) generating 98.5% H2SO4.
use.
In the absence of arsenic-containing minerals, this SO2 treatment pro­
Adsorption within the roasting process – Early studies and applica­
cess does not consume any lime reagent.
tions reported SO2 emissions mitigation by using lime (as co-feed)
Treatment of arsenic-containing sulfuric acid streams – Roasting of
together with sulfide containing ore or concentrate in the roasting
sulfide minerals that contain some arsenic, typically in the form of
process (Nyavor and Egiebor, 1991; Cole et al., 2001). The rationale for
arsenopyrite, requires explicit arsenic treatment process (Taylor et al.,
this approach is that lime acts as an adsorbent of SO2 within the process,
2014). Even with such treatment processes in place, some arsenic
thereby preventing emissions. This approach is, however, impractical
contamination of the sulfuric acid, produced via the process described
and uneconomical because of the high lime-reagent consumption
above, may occur. In such scenarios, the sulfuric acid needs to be pu­
needed for the process to be sufficiently effective at adsorbing all SO2
rified of residual arsenic to ensure sale ability. Solvent extraction
and preventing its emission.
methods are used to remove arsenic from the sulfuric acid solution,
Dual alkali scrubbing process – The dual alkali process makes use of
resulting in an arsenic-containing acidic side-stream (Wiśniewski, 1997;
both (i.e. dual) NaOH and Ca(OH)2 alkalis and has mainly been applied
Jantunen et al., 2019). This arsenate (As5+) or arsenite (As3+) contained
at platinum group metals (PGM) mineral processing operations and coal-
within this side-stream can be treated in several ways (Feng et al., 2017,
fired power plants (VanNess et al., 1979), based on concerns that
2018), including with lime to precipitate either calcium arsenate, Re­
calcium-based adsorbents in wet scrubbing systems would cause
action (19), or arsenite, Reaction (20), at pH levels of approximately 12.
excessive scaling. The process can be summarized (Fig. 9) as using NaOH
This precipitation reaction consumes more lime than the precipitation of
as a gas scrubbing solution to remove SO2 in a gas/liquid contactor with
arsenic under acidic conditions as scorodite, FeAsO4⋅2H2O (Demopou­
sodium sulfite solution as the reaction product, Reaction (16), (Lunt
los, 2005). Calcium arsenate Ca3(AsO4)2 is insoluble in alkaline media,
et al., 2003). If the sodium sulfite is not fully oxidized within the gas/
while calcium arsenite Ca3(AsO3)2 is partially soluble, therefore
liquid contactor, an air-sparged oxidation reactor is used to facilitate its
requiring deliberate disposal consideration and precautions (Stefanakis
oxidation to sodium sulfate, Reaction (17). Sodium sulfate is reacted
and Kontopoulos, 1990).
with lime, Reaction (18), to regenerate soluble NaOH and gypsum pre­
cipitate. The gypsum is removed in a solid/liquid separation step and the 2H3 AsO4 + 3Ca(OH)2 →Ca3 (AsO4 )2 + 6H2 O (19)
NaOH is re-used in the SO2 scrubbing process.
2H3 AsO3 + 3Ca(OH)2 →Ca3 (AsO3 )2 + 6H2 O (20)
SO2 + 2NaOH→Na2 SO3 + H2 O (16)
Ca(OH)2 dry sorbent use – The efficiency of SO2 conversion to sale
2Na2 SO3 + O2 →2Na2 SO4 (17) able sulfuric acid means that there is no substantial requirement for SO2
gas adsorption in modern roasting plants that would use lime or other
Na2 SO4 + Ca(OH)2 + 2H2 O→CaSO4 .2H2 O + 2NaOH (18) adsorption reagents. Small quantities of fugitive SO2 emissions may,
A severe operational constraint on the dual alkali process is the self- however, occur in some locations within such plants and may be
limiting nature of the reaction of Ca(OH)2 with Na2SO4, Reaction (18). It extracted and directed towards a treatment system using Ca(OH)2 as a
is important to note that Ca(OH)2 is only slightly soluble (National Lime dry scrubbing reagent, similar to that widely used at large scale in flue-
Association, 1995) and that it is the soluble calcium (Ca2+) and hy­ gas treatment of coal-fired power plants (Chisholm and Rochelle, 1999).
droxide ions (OH− ), rather than the solid Ca(OH)2 particles that react In such systems SO2 is contacted with hydrated lime and converted to
with NaOH. Dissolution of Ca2+ and OH− from the surface of solid Ca CaSO3, Reaction (21), and, depending on the extent of oxidation, may be
(OH)2 particles is the limiting step in the reaction and is pH dependent. partially converted to gypsum, Reaction (22).
SO2 + Ca(OH)2 →CaSO3 + H2 O (21)

2CaSO3 + O2 + 4H2 O→2CaSO4 .2H2 O (22)

9.6.2. Pre-oxidation of refractory ore in tanks or autoclaves

Hydrometallurgical processing in tanks or autoclaves is commonly
applied to high-grade refractory ore, particularly where the ore does not
exhibit “preg-robbing” features. High grade is required to sustain the
considerable cost of milling (typically to < 150 μm), flotation, oxidation
and neutralization required to for ecomomic gold recovery. A wide
Fig. 9. Simplified dual alkali process for SO2 removal from gas streams using range of hydrometallurgical process flow sheets are used (La Brooy
NaOH as primary scrubbing reagent and Ca(OH)2 to precipitate gypsum and et al., 1994; Aylmore and Jaffer, 2012; Marsden and House, 2006) based
regenerate NaOH.

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C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

on location and ore-specific conditions, but generally contain the pro­ (24). Reaction (24) illustrates the reaction for potassium jarosite,
cess components illustrated in Fig. 10. although potassium may be substituted by sodium, ammonium, silver or
The ore is crushed, milled and subjected to flotation to produce a hydronium cations (Gramp et al., 2008; Fleming, 2010; Kaksonen et al.,
concentrate in which both the gold and sulfide mineral content is 2014). By this mechanism, the limestone and lime reagent requirements
increased, relative to that of the original ore feed. A low-grade tailings within the process circuit are influenced by the pre-oxidation method.
stream is also produced. A concentrate regrind and gravity circuit is
commonly used to recover any gravity gold (Laplante et al., 1995). The 12FeS2 + 45O2 + 24H2 O→6Fe2 O3 + 24H2 SO4 (23)
concentrate is thickened and subjected to some form of sulfide oxida­
tion. This sulfide oxidation step, also referred to as pre-oxidation, is the 12FeS2 + 45O2 + 2K2 SO4 + 30H2 O→4KFe3 (OH)6 (SO4 )2 + 18H2 SO4 (24)
distinguishing and most prominent feature of refractory process flow
The acidic mineral slurry resulting from the pre-oxidation process is
sheets in which pyrite, and sometimes arsenopyrite, is oxidized to render
then subjected to counter current decantation (CCD), where wash water
the concentrate amenable to subsequent cyanidation and gold recovery.
flows counter current to the solids in a series of thickeners (Thomas and
The pre-oxidation reaction is most often conducted in either pressure
Pearson, 2016). The purpose of the CCD circuit is to separate and
oxidation autoclaves or biological oxidation reactors. Oxidation in au­
remove sulfuric acid and dissolved elements from the solids residue,
toclaves occurs at 180 ◦ C to 235 ◦ C and pressures of up to 3,500 kPa for
before neutralization and cyanidation of the gold-containing mineral
up to 60 min using pure oxygen (Rusanen et al., 2013; Tiihonen et al.,
residue pulp. The CCD underflow reports to a pulp liming step in which
2013; Thomas and Pearson, 2016). Biological oxidation (also called
the pH in increased to > 10.5 to facilitate effective cyanidation.
biooxidation), using chemo-lithotrophic bacteria that catalyze the
Through the use of a CCD circuit, most acid and dissolved elements
oxidation of reduced iron and sulfur, occurs at atmospheric pressure
are separated from the mineral slurry and report to the first CCD over­
conditions and temperatures ranging from 35 to 45 ◦ C with oxygen
flow. The overflow solution is typically neutralized in two stages (Dew
provided by air sparging. Indeed, the CO2 contained in air is required as
et al., 1997). Due to the high level of acidity, primary neutralization
carbon source for the chemo-lithotrophic bacteria that catalyze the
makes use of milled limestone (CaCO3) to neutralize sulfuric acid and to
mineral oxidation reactions (du Plessis et al., 2001; Rawlings et al.,
precipitate soluble iron and many other soluble metals, such as
2003). The absence of cyanide during the oxidation step ensures the gold
aluminium. Lime (CaO), rather than limestone, is required to achieve
remains unoxidized as solid Au0, during the sulfide oxidation process
sufficiently high pH values to precipitate elements such as manganese
(Cheng et al., 2021). The purpose of the oxidation step is to (1) liberate
and magnesium in secondary neutralization. The lime reagent con­
the gold, and (2) reduce the sulfide content that would otherwise react
sumption of this step is typically high (i.e., exceeding 100,000 tons per
with cyanide, although the former is the principal operational consid­
annum for large plants), causing plant operators to seek alternative
eration. The extent of sulfide oxidation is the main driver for acid gen­
disposal mechanisms for these acidic waste streams that do not consume
eration and subsequent lime consumption, though some operations
lime. Some plants substitute the use of flotation tailings for lime in
perform direct whole-ore alkaline pressure oxidation. The form of iron
secondary neutralization to reduce reagent costs. The reaction of tail­
precipitation also plays a role, although to a lesser extent. Pre-oxidation
ings, however, generates soluble magnesium and other sulfates, such as
processes result in sulfuric acid and precipitation of ferric iron, either as
sodium and potassium, that remain soluble, leak into the environment
hematite, Reaction (23), or jarosite, Reaction (24), depending on the
and cause detrimental effects (Canham et al., 2020). By contrast, the use
acidity level, pressure, temperature and cation composition (Fleming,
of lime results in the precipitation of sulfates as insoluble gypsum.
2010). Pressure oxidation, because of its higher pressure conditions,
results mainly in hematite, while biooxidation yields jarosite because of
9.6.2.1. Silver recovery after pre-oxidation in pressure oxidation
the ambient pressure conditions. Hematite formation does not result in
autoclaves. In scenarios where substantial quantities of silver are pre­
sulfate incorporation into the iron precipitate, whereas in the case of
sent, together with gold, additional process steps may be required to
jarosite it does, thus reducing the residual sulfuric acid in solution
enable optimal silver recovery. This is because of silver’s tendency to be
requiring neutralization, i.e. H2SO4 production from reaction (23) vs.
oxidized (to Ag+) during the autoclave pre-oxidation process and to
precipitate as argento-jarosite, AgFe3(SO4)2(OH)6, rendering subse­
quent recovery by cyanidation ineffective. (Chan et al., 2015; Gunar­
atnam et al., 2018). This problem can be remedied by subjecting the
washed oxidized residue to a so-called lime boil process, before cyani­
dation. During this process the oxidized solids residue from the auto­
clave is digested in the presence of lime with pH maintained as high as
12.4, at 90 to 95 ◦ C for 4 h, Reaction (25), (Kasaini et al., 2008; Aylmore
and Jaffer, 2012; Gunaratnam et al., 2018). This reaction decomposes
the jarosite and renders the silver amenable to conventional cyanidation
in a subsequent process step.
AgFe3 (SO4 )2 (OH)6 + 2Ca(OH)2 + 2H2 O
(25)
→3Fe(OH)3 + AgOH + 2CaSO4 .H2 O

9.6.2.2. Ultrafine grinding. Ultrafine grinding is another method to

process selected refractory ores/concentrates (where refractoriness to
direct cyanidation arises from fine to ultrafine (>0.02 μm, <20 μm) gold
mineral inclusions in the pyrite and/or arseno-pyrite). This technology
can be applied where gold remains a separate, albeit colloidal phase, in
the sulfide rather than in solid solution, where no separate gold phase is
identifiable, irrespective of microscope magnification. KCGM was the
Fig. 10. Simplified hydrometallurgical process components for processing first gold mine to use ultrafine grinding followed by cyanidation. The
high-grade refractory ore. (In the case of whole-ore oxidation treatment, the Fimiston plant in Western Australia commissioned a large UFG mill to
flotation and concentrate steps are absent. In some flow sheets the gravity completely replace roasting, thereby eliminating atmospheric emissions
circuit is before the flotation step).

11
 C.A. du Plessis et al. Minerals Engineering 174 (2021) 107231

from the Gidji Processing Plant (Ellis and Gao, 2003). UFG typically least amenable. A wide range of industrial methods have been developed
increases the reactivity of the sulfides in the milled ore/concentrate, to treat telluride-containing gold ores (Ellis and Deschênes, 2016). A
thereby increasing the lime demand to maintain a stable pH for cyani­ common feature is cyanidation at high lime dose and pH levels above
dation, and it also increases cyanide consumption (Hourn et al., 1995). 11.5 (Deschênes et al., 2006) and even above 12 (Rumball et al., 2008),
to improve leaching kinetics (indicatively summarized in reaction (26),
9.6.3. Heap leaching of refractory ore by biooxidation pre-treatment for calaverite).
The pre-oxidation methods described above are applied to relatively
4AuTe2 + 8NaCN + 8Ca(OH)2 + 9O2
high-grade ores where the comminution and flotation cost are justified. (26)
→4NaAu(CN)2 + 8CaTeO3 + 6H2 O + 4NaOH
Lower-grade refractory ores are treated by heap leaching processes,
because the low grade does not warrant the rather high cost of
comminution, flotation and pre-oxidation processes described earlier. 9.8. Treatment of sulfide-containing tailings and waste dumps
The heap leaching methods applied to refractory ore differ in important
ways from those of conventional heap leaching of non-refractory ore. All mining operations have mine plans that delineate the economi­
The latter is applicable to scenarios where the pH gradient in a heap can cally extractable ore, determined by the ore grade, processing method
reasonably be controlled in such a manner that the pH remains above 9 and associated costs, as well as the prevailing metal price. Mining
in the leach solution. Refractory ores that contain a high concentration economical ore requires excavation and disposal of ore that falls below
of pyrite or arseno-pyrite are therefore unsuitable to such treatment and the economic cut-off grade. The dumps in which this waste is contained,
are instead subjected to a two-step heap leaching process (Brierley and as well as the tailings and residues rejected from ore processing, often
Hill, 1993) relying on: (1) biooxidation, followed by (2) cyanidation contain minerals that may give rise to well-documented acid generation,
leaching. Similar approaches to heap leaching have also been applied to so called acid rock drainage or acid mine drainage (AMD) from a wide
precious- and base metal sulfide combinations, e.g. (Mwase et al., 2012; range of sources, including oxidation of pyrite, Reaction (6), jarosite
Mwase et al., 2012; Mwase et al., 2014). Biooxidation in heaps are decomposition, Reactions (27a), (27b), and others (Dold, 2014; Li et al.,
similar to reactions in tanks, Reaction (6), discussed earlier, however, 2014; Parbhakar-Fox et al., 2018). Lime reagents play a key role in both
heap biooxidation pretreatment operations are significantly different prevention and remediation of acid generation effects (Pozo-Antonio
than that of conventional cyanide heap leaching operations (Holtum and et al., 2014; Qian et al., 2017). The use of lime for this purpose is
Murray, 1994; Brierley and Rawlings, 1997). The biooxidation heap pad particularly relevant to ore deposits, tailings and waste dumps that
is aerated from below (but above the level of solution collection) to contain high sulfide concentrations, i.e. sulfide refractory gold ores.
provide oxidation and is irrigated to provide a solution within the heap, (H3 O)Fe3 (SO4 )2 (OH)6 + 2H2 O
as bioleaching bacteria require a solution film on the mineral surface to (27a)
→3Fe(OH)3 + 2H2 SO4
oxidize the sulfide minerals (Bartlett, 1990; Bouffard and Dixon, 2004).
2NaFe3 (SO4 )2 (OH)6 + 6H2 O
Aeration is required not only to provide oxygen for the oxidation re­ (27b)
→6Fe(OH)3 + 3H2 SO4 + Na2 SO4
actions, but also to provide CO2, as the bacteria and archaea used in such
heap leaching require CO2 as a carbon source for growth and metabolic
functions (Petersen et al., 2010). The oxidation reaction, Reaction (6), is 10. Conclusion
acid-generating causing the process to operate at pH levels of 2 and
below (Bosecker, 1997). Indeed, the biooxidation process is more effi­ Together with cyanide, lime is the most-used reagent in gold pro­
cient at such low pH levels where ferric iron is maintained in soluble cessing. These two reagents are typically responsible for a large portion
form and facilitates sulfide mineral oxidation, while being continuously of the operating costs of the surface facilities at a gold processing
regenerated by biooxidation processes (Schippers and Sand, 1999; operation. Ore mineralogy, mineral associations, and degree of
Kaksonen et al., 2014). The acid conditions also cause dissolution of dissemination, as well as the choice of processing flow sheet and tech­
gangue mineral elements, such as silicate and magnesium (Crundwell, nologies, and the chemistry of the process water, all impact where and
2014; Chetty, 2018). Once biooxidation has sufficiently oxidized sulfide how much lime is utilized in the process. The article reviewed the factors
minerals to render the contained gold amenable to cyanidation recov­ that influence and inform operational trade-off decisions between the
ery, the ore in the biooxidation heap pad is drained, washing cycles use (and cost) of lime relative to other process efficiencies/inefficiencies
applied, and the ore transferred to a separate heap leaching pad where that may influence gold recovery and costs.
cyanidation occurs (Brierley and Hill, 1993). Lime, in the form of dry
quicklime, is added to the ore during the transfer process, typically via Declaration of Competing Interest
screw feeder from a lime silo directly onto an ore transfer conveyer belt,
before being stacked on the cyanidation heap leaching pad. The pH The authors declare that they have no known competing financial
target and subsequent cyanidation leaching is then similar to that of interests or personal relationships that could have appeared to influence
non-refractory ore heap leaching. The acidic solution drained and the work reported in this paper.
washed from the biooxidation heap stage, typically containing mainly
iron, alumina, silica, magnesium and sulfate, is neutralized sequentially Acknowledgements
by use of limestone (CaCO3) to neutralize acid and remove mainly iron
and aluminium, followed by the use of lime to precipitate the remaining The authors thank W. Staunton, R. Dunne, D. Lyons, D. Ballard, N.
dissolved elements for safe disposal (Brierley and Hill, 1993). Kramadhati, J. Heiszwolf, I. Pareys, F. Losma, and G. Herrier for valu­
able information sourcing, inputs and reviews.
9.7. Telluride-containing gold
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