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Chapter

Hydrometallurgical Recovery of
Gold from Mining Wastes
Emilia Neag, Eniko Kovacs, Zamfira Dinca,
Anamaria Iulia Török, Cerasel Varaticeanu
and Erika Andrea Levei

Abstract

Gold is a highly required material for a wide range of personal and industrial
applications. The high demand for gold, together with the shortage of natural
resources and high pollution potential of wastes generated during mining and
ore processing activities led to search for alternative sources of gold. A possible
source is represented by mine wastes resulting from the processing of polymetallic
or sulfidic ores. The reprocessing of wastes and old tailings with moderate to low
content of gold offers not only a business opportunity, but also enhances the quality
of the surrounding environment, changes the land use and offers a wide range of
socio-economic benefits. Cyanidation, the most widespread Au leaching option, is
progressively abandoned due to the high risk associated with its use and to the low
public acceptance. Therefore, alternative methods such as thiocyanate, thiourea,
thiosulphate and halide leaching gained more and more interest. This chapter
presents the most important features of some Au leaching methods, emphasizing
their advantages, limitations and potential applications.

Keywords: gold recovery, nonferrous mining wastes, leaching, technology,

circular economy

1. Introduction

From ancient times, gold was associated with power and wealth, being used for
the manufacture of tools and weapons, decorative objects and jewelries. Nowadays,
gold is a highly required element in the field of electronics, nanotechnology, medicine,
food, cosmetics, decorative or creative fashion, as well as in space technology [1–4].
Despite their economic importance, mining and ore processing have a low
public acceptance and a high environmental pollution potential as they generate
great amounts of wastes consisting in a mixture of solid waste materials (sand,
fine grained ground-up rock with a size of 1–600 μm), water, chemicals and high
concentrations of hazardous metals (Cu, Cd, Fe, Mn, Pb, Zn), metalloids (As, Se),
together with precious metals (Au, Ag) [5–9].
The mining waste disposal and the long-term management of tailing storage
facilities are critical issues of the mining process, as they can cause landscape dam-
ages and can lead to severe environmental contamination and destruction of living

1
Strategies of Sustainable Solid Waste Management

ecosystems [10, 11]. Worldwide, several tailing dam accidents with significant
environmental damages and sometimes also with human lives loss were reported
[11, 12]. One of the most important tailings dam failures occurred in 2000 in Baia
Mare, Romania, due to an improper design and lack of effective management of the
tailings impoundment, causing catastrophic damages to the environment [13, 14].
Another severe mining failure was reported in 1971 in the Certej River catchment,
Romania, where a large volume of mine tailings flooded the valley and generated
a significant pollution of the surrounding environment, together with 100 human
lives loss [15]. An important pollution accident occurred in Spain in 1998, when a
massive amount of acid water and mud containing toxic metals were released into
the Agrio and Guadiamar River from the dam of the Aznalcollar tailings pond [16].
Mining wastes and by-products are valuable secondary resources since they
contain important amounts of base, precious or strategic metals that can be
recovered [17]. Beside their economic importance, the wastes valorization by
reprocessing could improve the quality of the environment. The recycling, reuse
and recovery of extractive wastes is also encouraged in the Extractive Waste
Directive 2006/21/EC as it could lead to sustainable mining by resources conser-
vation and reduced environmental impact [17, 18]. Therefore, new processing
methods and technologies need to be developed and implemented. The most
used method for Au leaching from wastes is based on cyanidation. However, in
the context of raising social awareness and straightening environmental regula-
tion, cyanide has become a socially and environmentally undesirable method
for Au recovery. Therefore, the interest in finding other alternatives to cyanide,
with low impact on the environment increased [19–22]. There are a considerable
number of gold leaching methods which are currently tested or developed as
pilot-scale studies, but only a few are available on commercial scale. The most
tested leaching agents for gold are thiosulfate, thiourea, thiocyanate and halides
[19–21]. An effective Au recovery process from mining wastes could provide new
resources for various industrial fields [23]. This chapter presents an overview
of the most used leaching methods for Au recovery with their advantages and
limitations.

2. Gold leaching methods

2.1 Cyanide leaching

Cyanide is a cheap but highly toxic reagent that is very effective in leaching
gold from low-grade minerals and mining wastes. Therefore, cyanidation is the
most widely used method for the extraction of gold from mining wastes. Despite
its advantages, is considered an unacceptable and highly hazardous approach.
The health and safety concerns related to the use of cyanide as a leaching agent
were raised after the occurrence of several technological accidents that severely
damaged the environment [20, 24, 25]. Such incidents led to the development of a
voluntary program in the gold mining industry entitled the “International Cyanide
Management Code” with the objective to safely manage cyanide and safeguard
human health and the environment [26, 27].
The cyanide leaching is based on the Au complexation with cyanide ions in the
presence of oxygen in an alkaline solution according to Eq. (1) [22].

−
4Au + 8CN − + O
=2 + 2H2 O 4  Au ( CN )2  + 4OH− (1)

2
Hydrometallurgical Recovery of Gold from Mining Wastes
DOI: [Link]

Cyanide compounds are classified into three main types: free cyanides
(hydrogen cyanide (HCN), ionic cyanide (CN−)), weak acid dissociable (WAD)
cyanide complexes (with Cd, Cu, Ni, and Zn) and strong cyanide complexes (with
Co, Au, Ag, and Fe). The chemistry of these compounds offers perspectives on their
actions regarding performance, safety and environment [28]. There are a couple
of main ways through which cyanide can damage the environment: leakages, spills
and evaporation from open leaching basins [21]. To reduce the negative impact on
the environment, the naturally occurring cyanide dissociation mechanisms such as
volatilization, complexation, precipitation, adsorption, biological transformation,
and sulfidation can be artificially enhanced [27]. By complexation, most often
with formation of iron cyanocomplexes, cyanide can be removed from wastes.
However, considering that these complexes can dissociate photochemically into free
cyanides, some concerns regarding the environmental risks were raised [27]. The
adsorption of weak and strong cyanometallic complexes on goethite, manganese
oxides, aluminum oxides, silica, and clays is another option for cyanide reduction
[27]. Biological transformations assisted by bacteria, fungi or plant species may
break down cyanide via oxidative, reductive, hydrolytic or assimilatory pathways to
carbon and nitrogen species used for their growth [27]. The rate of cyanide attenua-
tion in tailings is influenced by cyanide speciation, pH of the solution, temperature,
redox conditions, exposure to sunlight and microbial activity [27].

2.2 Thiourea leaching

Thiourea (SC(NH2)2) dissolves gold by forming a complex in acidic solution

according to Eq. (2) [20, 22, 29, 30]. In the leaching process, ferric sulfate is added
as a catalyst to enhance the gold oxidation [20, 22].

Au ( SC ( NH2 )2 )2
+
Au + + 2SC ( NH2 )2 = (2)

Gold dissolution in thiourea is faster than in cyanide, but high volumes of

thiourea solutions are needed in the dissolution process [22]. This shortcoming is
avoided by using a mixture of thiourea, thiocyanate and ferric sulfate [21]. Thiourea
presents low sensitivity to base metals present in mining wastes and tailings used
as raw material for Au recovery [29]. Regardless of its low toxicity compared to
cyanide, thiourea is classified as a potential carcinogen [20, 29].
Extensive research has been carried out on Au leaching using acid thiourea
solution at laboratory scale. Moreover, thiourea leaching of Au was tested in pilot
plants and industrial operations [28, 30]. The pH of the solution, leaching potential,
ferric sulfate concentration, thiourea concentration and leaching time are critical
parameters for the leaching efficiency [20]. The optimum conditions for thiourea
leaching can be achieved by using an appropriate quantity of oxidant to ensure the
oxidation of 50% of the thiourea to formamidine disulfide. An excessive amount
of oxidant will lead to high thiourea consumptions. High consumptions combined
with the use of reagents for pH adjustment and potential control will increase the
cost of the leaching process [28].

2.3 Thiocyanate leaching

Thiocyanate (SCN−) forms two stable and soluble complexes with gold,
Au(SCN)2− (aurothiocyanate) and Au(SCN)4− (aurithiocyanate), out of which
Au(SCN)4− is the most stable (Eqs. (3) and (4)) [28, 31].

3
Strategies of Sustainable Solid Waste Management

Au ( SCN )2 + e−
− −
Au + 2SCN
= (3)

Au ( SCN )4 + 3e−
− −
Au + 4SCN
= (4)

Thiocyanate has low toxicity, high stability, but also slow leaching rate. Thus,
ferric ion as an oxidant is used to increase the leaching rate. Gold leaching using
thiocyanate takes place in the presence of ferric ions, according to Eq. (5) [19].

Au ( SCN )4 + 3Fe2 +
−
Au + 4SCN − + 3Fe
= 3+
(5)

The thiocyanate/ferric sulfate system proved to be suitable for a wide range

of ferric ion/thiocyanate molar ratios and slowed the rate of thiocyanate decom-
position [32]. Generally, gold leaching using thiocyanate (0.01–0.05 M) occurs
at a potential of 0.4–0.45 V, pH 1–3, in the presence of an oxidant like ferric ions
(2–5 g/L) or peroxide. It has been shown that, under optimal conditions, a gold
extraction yield of 95% can be achieved [21]. Thiocyanate concentrations in the
range of 0.5 to 5 g/L and Fe (III) concentrations in the range of 6 to 12 g/L have
been used in laboratory and small-scale pilot tests. The thiocyanate concentration
must be maintained for the effective leaching of Au [28]. Thiocyanate leaching
has not yet been commercialized due to its complex operating process [32]. As
the leaching takes place at low pH, special reactors are required to resist in highly
corrosive and oxidizing media [29]. Before its large-scale implementation, more
research is needed to identify the optimum conditions of the process and to reduce
the thiocyanate consumption.

2.4 Thiosulfate leaching

The thiosulphate leaching proved to be a very promising, environmental-

friendly alternative to cyanide leaching for Au and Ag recovery [20]. Usually it is
used under alkaline conditions to avoid thiosulfate decomposition in the presence
of oxygen as oxidation agent (Eq. (6)) [20, 21, 28].

4Au ( S2O3 )2 + 4OH−

3−
4Au + 8S2O32 − + O=
2 + 2H2 O (6)

Generally, the dissolution rate of Au in alkaline thiosulphate is slow, but it can be

enhanced in the presence of ammonia and Cu2+ [20, 21]. The stability of thiosulfate
and copper complexes depends on the pH of the solution [22]. The Au dissolution in
ammoniacal-copper thiosulfate takes place according to Eq. (7) [28].

Au + 5S2O32 − + Cu ( NH=
3 )4 Au ( S2O3 )2 + 4NH3 + Cu ( S2O3 )3
2+ 3− 5−
(7)

The main advantages of thiosulphate leaching compared with other methods are
the low toxicity, high reaction selectivity, ability to recirculate the leaching solu-
tions, lower reagent cost and the possibility to recover the dissolved gold by adsorp-
tion and electrodeposition [8, 33]. The main disadvantage of alkaline thiosulphate
leaching is the high reagent consumption and low extraction rates [21].

4
Hydrometallurgical Recovery of Gold from Mining Wastes
DOI: [Link]

Recently, Ubaldini investigated the use of thiosulphate for Au extraction

using mine tailings from Ribita and Criscior [8]. A gold extraction of 75% after
leaching and a recovery of 90% Au after purification (adsorption–desorption–
electrodeposition cycle) was obtained, while the overall process achieved a recovery
of 65–67% Au [8]. The Au and Ag recovery from mineral tailings using glycine and
sodium thiosulphate showed a leaching recovery of Au more than 80% after 48 h
leaching tests with thiosulfate at a solid–liquid ratio of 1:1 [34].
Several studies have been carried out over the last decades to establish the
commercial feasibility of Au leaching using thiosulphate. The high consumption
of thiosulfate during Au leaching represents a disadvantage for scaling up the
process as thiosulphate is easily oxidized by the copper ions added as catalyzer
[33]. Moreover, the low affinity of activated carbon for the gold complex makes the
recovery of Au more difficult [33].
Mahmoud and Awad studied the recovery of Au from thiosulfate solution on
activated carbon in the presence of ammonium persulfate [35]. The obtained results
showed that increasing the ammonium persulfate concentrations to 0.01 M, an effi-
ciency of 85% for gold adsorption after only 10 min was obtained, and 95% of Au
was recovered after 90 min [36]. The recovery of Au from the thiosulphate leachate
using strong base anion resins compared with weak base anion resins presents
several advantages such as higher adsorption capacities of gold complex and inde-
pendence of the adsorption performances on the pH of the solution. However, their
selectivity for [Au(S2O3)2]3− against [Cu(S2O3)3]5− is low and complex processes are
required for the complete separation of gold and copper from the anion resin [33].

2.5 Halide leaching

2.5.1 Chlorination

Before the large-scale use of cyanide leaching, chlorination was widely applied
for gold recovery [20, 21]. Gold dissolution occurs in two stages according to Eqs.
(8) and (9) [28].

Au + Cl − = AuCl + e− (8)

AuCl2 − + 2Cl −= AuCl 4 − + 2e− (9)

Compared to alkaline cyanide leaching, chlorination offers a high dissolution

rate, but requests acidic media, high temperatures and high concentrations of
chloride [21]. In the case of minerals containing silver and lead the metal recovery
is low. Moreover, during the leaching process highly toxic and corrosive chlorine
gases are released [21]. The reagent consumption is high when low concentrations
of sulfides are present in the wastes, leading to the reduction of the gold complex to
metallic gold [20].
Recently, Ahtiainen and Lundstrom studied cyanide-free gold leaching in mild
chloride media obtaining a gold extraction of 72% at a redox potential <520 mV vs.
Ag/AgCl [37].
The combination of chlorination with roasting for the Au extraction showed
that 91.6% of Au was recovered using 4% CaCl2, while heating at 1323 K for 2 h
[38]. Li studied the gold extraction from tailings using sulfuric acid as a pretreat-
ment before calcium hypochlorite leaching [39]. The obtained results showed that
the leaching rate of Au was 81% using 8% calcium hypochlorite, 333 K chlorination

5
Strategies of Sustainable Solid Waste Management

temperature and 2 h chlorination time [39]. The use of chlorine for gold extrac-
tion remains difficult to use due to the high reagent consumption, its corrosive
effect, high cost of the overall process and challenges experienced in Au recovering
process [28].

2.5.2 Bromine

Gold dissolution in bromide (Eq. (10)) is influenced by the concentration

of bromide and Au, the pH and the electrochemical potential of the anodic and
cathodic processes [21, 40].

Au + 4Br −= AuBr4 − + 3e− (10)

Bromide leaching has the advantages of short extraction time, high dissolution
rates, high selectivity and adaptation to a wide range of pH values. However,
bromide is not suitable to be used as a large-scale industrial process as it is difficult
to handle and has high reagent costs [20–22, 40].
Over the last years, gold dissolution was investigated using different oxidants
like ferric ion, hydrogen peroxide and hypochlorite. The results showed a slow
dissolution of gold using hydrogen peroxide and ferric ion [40]. The efficiency of
bromine produced in-situ using NaBr, NaOCl and HCl to dissolve auriferous gold
ore from the Castromil deposit (Portugal) was proven to be comparable with that of
cyanide leaching and twice higher than of thiosulfate [40].

2.5.3 Iodine

Triiodide ion formed by iodine (I2) and iodide ions (I−) acts as an oxidant
complexing gold (Eq. (11)) [21, 29].

Au + 4I−= AuI4 − + 3e− (11)

Iodine gold leaching can be a promising alternative to cyanide leaching because

of its low volatility and hazardousness [22]. The process presents high leaching rates
and the formed gold iodide complexes are more stable in aqueous solutions than
the complexes with other halogens [20]. However, iodine was not used at industrial
scale due to its high cost [22]. The electrolytic deposition could be an efficient
method to reduce the costs through electrolytic recovery of gold and regeneration
of iodine [29]. Recently, electrodeposition of gold from iodine leaching solution
using response surface methodology was used to study the interactions between
variables and their effect on gold deposition rate. The proposed method showed a
high deposition rate (94.02%), but a low coulombic efficiency (2.53%) [41].
Presently, the application of halide systems is limited due to the difficulties
encountered in maintaining the gold complex in the solution [20].

2.6 Aqua regia leaching

Aqua regia is a mixture of concentrated nitric acid (HNO3) and hydrochloric

acid (HCl). The dissolution of gold with aqua regia is a simple, fast and effective
process, but the amount of NOx released in the atmosphere can be a significant

6
Hydrometallurgical Recovery of Gold from Mining Wastes
DOI: [Link]

source of air pollution [42]. The HNO3 favors the formation of trivalent gold ions,
which further react with chloride to form tetrachloroaurate anions, according to
Eq. (12) [21, 43].

= AuCl − 4 + H + + NO + 2H2O
Au + HNO3 + 4HCl (12)

The aqua regia leaching is mostly used for alloys with high gold content [36]. In
case of higher Ag content, it is necessary to reduce the amount of Ag to prevent the
incomplete dissolution of gold by blending doré materials with feedstocks contain-
ing low amounts of Ag or by pretreatment with HNO3 for Ag removal before disso-
lution. Aqua regia is known as an effective leaching agent due to its high dissolution
rate, but is extremely corrosive [21]. During the leaching process, toxic NOx gases
are released. The NOx emissions depend on the acid concentrations, temperature
and air flow rates of the dissolution process [42]. The effectiveness of the dissolu-
tion process in aqua regia is influenced by the material granulation which can offer
a large surface area to enable the reaction kinetics. In addition, the solution can be
heated during dissolution to allow a rapid reaction.

2.7 Microbial leaching

Recovery of value-added metals from various wastes using microbial species has
attracted much interest in recent years due to the long-term decline of ore grades
and concentrates. Microorganisms play an important role especially in the gold
recovery process from mining wastes and tailings. Some specialized bacteria, fungi,
yeasts, algae or actinomycetes are increasingly being used to facilitate the extraction
of gold from low-grade auriferous ore [44]. These microorganisms can enhance the
oxidation of metallic minerals and may be used as flotation agents or as biosorbents
in the gold recovery process [24, 45].
In recent years, two different types of biomining processes have attracted
researchers’ interest as alternatives to conventional methods: bioleaching and
biological oxidation, as they proved to be cost-efficient, sustainable and non-
hazardous [46–48].
Bioleaching is a solubilization process in which bacteria help to dissolve gold
from ores or wastes, while in the biooxidation process, the acidophilic microor-
ganisms release gold from minerals during sulfide oxidation [49]. Biooxidation
of gold can be applied as heap or dump leaching and stirred tank leaching. The
static biooxidation techniques are based on the principle of circulating water and
air through waste heaps to activate the growth of microorganisms that amplify
the oxidation [50]. Cyanogenic microorganisms as Chromobacterium violaceum,
Pseudomonas fluorescens and Pseudomonas plecoglossicida were able to mobilize gold
when grown in the presence of various metal-containing solids. Compared to
chemical oxidation, biological oxidation offers the advantages of low production
costs, low temperatures, low pressures, partial sulfide oxidation, decreased leachate
consumption and no atmospheric pollution [51]. In polymetallic sulfidic ores sev-
eral acidophilic, chemolithotrophic iron and sulfur oxidizing bacteria are present.
Mesophilic iron and sulfur oxidizing bacteria as Acidithiobacillus ferroxidans, sulfur-
oxidizing Acidithiobacillus thioxidans, iron-oxidizing Leptospirillum ferriphilum
and Leptospirillum ferrooxidans, moderately thermophilic bacteria, such as sulfur-
oxidizing Acidithiobacillus caldus and sulfur and iron oxidizing Sulfobacillus spp. has
been reported to assist in the oxidation of sulfides [44, 52].

7
Strategies of Sustainable Solid Waste Management

Various microorganisms were tested for gold biomining [51]. A recent study has
reported the Au recovery from polymetallic sulfide minerals using biooxidation
followed by acid washing and citrate leaching [53]. Thus, the biooxidation stage
removed the refractory ores, increasing the gold extraction from 17.3 to 86.4% [53].
In the biooxidation process, sulfides are oxidized by mixed mesophilic culture
mainly consisting of Acidithiobacillus ferrooxidans. A combined procedure for Au,
Ag and Pb recovery from sulfide minerals was proposed by Lorenzo-Tallafigo [54].
Biosorption by microbial biomass is another promising, cost efficient and eco-
friendly method for the gold recovery from wastes [23, 54]. Biosorption is a passive
sorption and/or complexation method of gold in the cell wall of diverse algae,
fungi and bacteria biomass [54, 55]. Stationary or dead microbial biomass bind
and concentrate gold ions from pregnant leachates [56]. In biosorption processes
a series of green and brown algae (Chlorella vulgaris, Fucus vesiculosus, Sargassum
natans), fungi (Aspergillus niger, Mucor rouxii, Rhizopus arrihus, Aspergillus
oryzae, Chaetomium globosum, Gibberella fujikuroi, Mucor hiemalis, Penicillium
chrysogenum, Purpureocillium lilacinum), yeast (Candida krusei, Candida robusta,
Candida utilis, Cryptococcus albidus, Cryptococcus laurentii, Debaryomyces hansenii,
Endomycopsis fibuligera, Hansenula anomala, Hansenula saturnas, Kluyveromyces
spp., Saccharomyces cerevisiae, Sporobolomyces salmonicolor, Torulopsisaeria) or bac-
teria (Streptomyces phaeochromogenes HUT6013, Acinetobacter calcoaceticus, Erwinia
herbicola, Pseudomonas aeruginosa, Pseudomonas maltophilia) are used for gold recov-
ery [24]. Some microbial species (Bacillus subtilis, Escherichia coli, Streptomyces albus,
Candida utilis, Aspergillus niger) can contribute to the passive sorption of gold from
solution or have the capacity to accumulate gold in an EPS capsule (Hyphomonas
adhaerens MHS-3) [51]. A gold recovery rate of 85% has been reported by Kenney
when non-metabolizing bacteria cells of Bacillus subtilis and Pseudomonas putida
were used [57].
Recent studies revealed effective results for Au recovery with other biomining
methods as bioprecipitation, biomineralization, bioflotation, bioflocculation, bio-
sorption and bioaccumulation [58–60]. All these methods are based on gold harvest-
ing microorganisms, which are either isolated from the gold enriched areas and
domesticated or bioengineered strains with exceptional gold retrieval efficiency [48].
Due to the fact that various microbial communities have different structure, func-
tions and dynamics in the gold metabolization, their use in bio-hydrometallurgical
processes still remain a challenge. Even if many thermophilic or acidophilic bacteria,
archaea or other types of microorganisms have been isolated, characterized, and
even used for extracting precious metals, new strains isolated from different sources
of wastes are needed [47]. At the same time, it is necessary to find combinations
of chemicals compatible with efficient microbial agents to recover high levels of
gold [61].
In the mining industry, naturally-occurring microorganisms which can be
exploited through different strategies for the extraction and recovery of gold have a
great potential [62]. The use of microorganisms for the recovery of precious metals
from waste is economical and can avoid environmental pollution [44]. Furthermore,
microbe driven technologies based on processes like biofiltration using specialized
biofilters can assure a specific recovery of the gold ions [63]. Future gold recovery
processing systems based on microorganisms will revolutionize the gold production.

3. Conclusions

Mining wastes represent a valuable resource for various elements, among which
precious metals like gold. These wastes present both challenges and opportunities,

8
Hydrometallurgical Recovery of Gold from Mining Wastes
DOI: [Link]

as it require long term management to reduce the environmental risks, but could
act as important resources for base and precious metals. In order to secure the high
global demand for gold, new, low-cost, highly efficient but also environmentally
friendly methods need to be developed. Although there is a lot of research in the
field of developing less-toxic alternatives to cyanide and several leaching agents
proved their efficiency, till now, there is no viable industrial scale alternative to cya-
nide. Another important challenge is the recovery of Au from mine waste leachates
containing several soluble metals in various concentrations.

Acknowledgements

This research was funded by a grant of the Romanian National Authority for
Scientific Research and Innovation, CCCDI-UEFISCDI, project number 52/2018,
COFUND-ERANET-ERAMIN-MINTECO-2, within PNCDI III.

Conflict of interest

The authors declare no conflict of interest.

Author details

Emilia Neag1, Eniko Kovacs1,2, Zamfira Dinca1, Anamaria Iulia Török1,

Cerasel Varaticeanu1 and Erika Andrea Levei1*

1 INCDO-INOE 2000, Research Institute for Analytical Instrumentation,

Cluj-Napoca, Romania

2 University of Agricultural Sciences and Veterinary Medicine, Cluj-Napoca,

Romania

*Address all correspondence to: [Link]@[Link]

© 2020 The Author(s). Licensee IntechOpen. This chapter is distributed under the terms
of the Creative Commons Attribution License ([Link]
by/3.0), which permits unrestricted use, distribution, and reproduction in any medium,
provided the original work is properly cited.

9
Strategies of Sustainable Solid Waste Management

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