Ultrasonics - Sonochemistry 64 (2020) 105039

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Ultrasonics - Sonochemistry
journal homepage: www.elsevier.com/locate/ultson

Ultrasound-assisted cyanide extraction of gold from gold concentrate at low T

temperature
Shimin Yua, Tingting Yub,c, Wenping Songa, , Xiyang Yua, Jianxin Qiaoa, Wuyi Wanga,
⁎

Huijuan Donga, Zhiguang Wua,d, Lizhou Daia, Tianlong Lia,d,

⁎

a
School of Mechatronics Engineering, Harbin Institute of Technology, Harbin 150001, China
b
Max Planck Institute for Intelligent Systems, Heisenbergstr. 3, 70569 Stuttgart, Germany
c
Institute of Physical Chemistry, University of Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany
d
Institute of Pharmacy, Sechenov University, Moscow 119991, Russia

ARTICLE INFO ABSTRACT

Keywords: A sonochemical reactor was developed to study the ultrasound-assisted cyanide extraction of gold from gold ore
Ultrasound-assisted cyanide extraction at low temperature. The effects of ultrasound on gold leaching in low temperature and conventional conditions
Extraction rate of gold were investigated. At the low temperature of 10 °C, ultrasound-assisted extraction increased extraction rate of
Unit consumption of NaCN gold by 0.6%–0.8% and reduced the gold content of cyanide tailings to 0.28 g/t in the leaching of gold con-
centrate and cyanide tailings, respectively. At the conventional temperature of 25 °C, ultrasound-assisted ex-
traction obtained a 0.1% higher extraction rate of gold compared with conventional extraction, with the unit
consumption of NaCN reduction of 15%. The analysis of kinetic model also demonstrated that sonication indeed
improved the reaction of gold leaching greatly. The mineralogy and morphology of ore were further analyzed by
X-ray diffraction (XRD), scanning electron microscope (SEM) and particle size analyzer to explore the
strengthening mechanism of gold leaching. The results showed that the ore particles were smashed, the ore
particle surface was peeled, the passive film was destroyed and the reaction resistance decreased under ultra-
sonic processing. Therefore, the extraction rate of gold was improved and the extraction time was shortened
significantly in ultrasound-assisted cyanide extraction.

1. Introduction However, non-cyanide lixiviants mostly stay in the stage of laboratory

Gold has been widely used in the field of electrical devices, preci-
sion detection and bio-pharmacy for the excellent physical and che-
mical properties (e.g. high melting, good electrical conductivity and
strong acid resistance) [1–3]. However, extracting gold efficiently from
ore is still an urgent difficulty due to the extremely low gold con-
centration, minuscule gold particles and containment of other active
metals. Recently, efficient and environment-friendly exploitation of the
gold resource has become the main challenge to the gold-producing
industry.
Many methods have been used to improve the extraction rate of
gold and reduce environmental pollution, they can be divided into two
categories of non-cyanide method and cyanide method based on the
type of lixiviants. As for non-cyanide method, many new alternative
non-cyanide lixiviants (such as ammoniacal thiosulfate [4], chloride/
hypochlorite [5], halide [6,7], thiourea [8], thiocyanate [9] and aqu-
eous ozone [10]) have been studied for gold leaching in recent years.
research due to the low extraction rate (mostly less than 92% [11,12]
and less than 60% for refractory ore [13]).
Cyanide has been widely used in the gold-producing industry as a
leach reagent for its high efficiency and relatively low cost [14,15].
Many new cyanide methods (such as pre-oxidation [16], the addition of
mercury ions [17] and microwave pretreatment [18]) have been re-
ported to enhance the gold cyanidation recently. Nonetheless, two
substantial drawbacks in the present gold cyanidation still need to be
solved. First, the cyanide extraction rate of gold is limited dramatically
at low temperatures (< 10 °C), and much extra energy is consumed for
heating the leaching tank in winter. Second, the barren liquor and
tailing produced by gold cyanidation contain a large amount of cya-
nide, which brings great difficulties to the subsequent processing [19].
Therefore, an extraction method with high efficiency and lower toxicity
at low temperature is important to be discovered.
Ultrasound technology has been actively studied and widely applied
into the industry for the last few decades, such as nanostructured

⁎
Correspondence authors.
E-mail addresses: songwenping@hit.edu.cn (W. Song), tianlongli@hit.edu.cn (T. Li).

https://doi.org/10.1016/j.ultsonch.2020.105039
Received 23 October 2019; Received in revised form 1 February 2020; Accepted 14 February 2020
Available online 15 February 2020
1350-4177/ © 2020 Elsevier B.V. All rights reserved.
S. Yu, et al.
Table 1
Chemical composition and content of the gold concentrate.
Element Au, g/t Ag, g/t S Fe
Percentages (%) 44.84 104 22.73 24.33
Fig. 1. Sonochemical reactor for cyanide leaching of gold. The inset shows the internal schematic of the extraction vessel with a volume of 3L.
materials synthesis [20], imaging and acoustic microscopy [21,22],
high-precision medical treatment [23] and micro-/nanomotors
[24–26]. Ultrasonic cavitation can produce high-speed micro-jets
(300–1000 m/s) [27], strong shear forces [28] and high local tem-
perature. These effects can clean the particle surface [29], enhance
mass transfer, accelerate reaction rates and avoid the use of high re-
action temperatures [30]. Ambulgekar studied the low temperature
recyclable catalyst for Heck reactions using ultrasound, finding that
presence of ultrasound allows reaction at low temperature and in-
creases the reaction rate as compared to conventional Pd/C catalysed
Heck reactions [31]. Yin used the ultrasound to leach rare earths from
the weathered crust elution-deposited ore [32]. The result showed that
the leaching efficiency of rare earths was substantially increased by
introducing ultrasound. In addition, some attempts on ultrasound-as-
sisted leaching gold have been reported [33–35]. However, few studies
have been conducted on leaching effect and sodium cyanide con-
sumption in ultrasound-assisted cyanide extraction at low temperature.
In this work, we developed a sonochemical reactor for ultrasound-
assisted cyanide leaching gold from gold concentrate at low tempera-
ture. Simulation and experimental studies on ultrasound-assisted cya-
nide gold leaching were conducted. The effects of ultrasound on gold
leaching in conventional conditions and secondary leaching of cyanide
tailings were also investigated. Reaction kinetic models were further
built to analyze the influence of ultrasound on reaction of gold
leaching. Moreover, the strengthening mechanism of ultrasound-as-
sisted extraction was explored.
2. Experiment
2.1. Materials
The gold ore was obtained from the gold mine in Shandong, China.
The free-milling gold ore was pretreated by grinding, flotation and filter
pressing to obtain the gold concentrate in the experiments of this study.
The particle size of the gold concentrate is less than 400 mesh. The
2
Ultrasonics - Sonochemistry 64 (2020) 105039
As Si Al2O3 CaO K2 O Na2O
0.03 18.76 6.92 1.45 1.54 0.9
elemental composition of the gold concentrate obtained by atomic ab-
sorption spectrometer (AAS, Agilent, American) and X Ray fluorescence
(XRF, Pw4400, Panalytical, Netherlands) is shown in Table 1. As can be
seen, the main elements of gold concentrate include sulfur, iron, silicon,
aluminium, calcium, potassium and sodium. The gold content is
44.84 g/t. Sodium cyanide (NaCN), barren liquor (pH≈10.5, CN−
concentration was 371.6 mg/L), calcium oxide (CaO) and cyanide
tailings in the experiments were provided by Shandong Zhongkuang
Group CO., Ltd.
2.2. Experimental method
In order to investigate the effect of ultrasound on cyanide leaching
of gold, experiments were implemented in a sonochemical reactor
shown in Fig. 1. The stirring paddle was driven by a motor to prevent
the ore slurry from depositing. Water inlet and outlet were connected
with a constant temperature cooling circulating pump, providing the
cooling water to keep ore slurry at a constant temperature. The tem-
perature of ore slurry was monitored in real-time by a thermometer
probe, which was obtained by averaging the temperatures of three lo-
cations from the transducer to the extraction vessel. The leached ore
samples can be conveniently taken through the sample connection at
the bottom of the extraction vessel. An ultrasound processor (HH3000B,
Xinxiang Relaxation Ultrasonic Equipment Co., Ltd, China) was em-
ployed in the ultrasound-assisted extraction process. The ultrasonic
transducer was driven by an ultrasonic generator and worked at a re-
sonant frequency of 20 kHz and a power of 650 W.
Firstly, we mixed 600 g of gold concentrate and 1200 mL of barren
liquor to obtain the mixed ore slurry with the solid–liquid ratio of 1:2.
Then we measured the cyanide ion (CN−) of the mixed ore slurry and
added a certain amount of NaCN to make the CN− concentration 0.04,
0.06, 0.08, 0.1 and 0.12 mol/L, respectively. The PH of the mixed ore
slurry was adjusted to 10.5–11 by adding CaO powder. After that, the
mixed ore slurry was extracted in the sonochemical and conventional
reactor, respectively. Finally, the residual cyanide tailings after
S. Yu, et al.
Fig. 2. Agitation and heat transfer of ore slurry. (a) The velocity distribution of
ore slurry under mechanical stirring at 10 °C. (b) The velocity distribution of
ore slurry under ultrasound-assisted mechanical stirring at 10 °C. (c) The
temperature distribution of ore slurry under sonication at 10 °C.
extraction were dried and detected using AAS. In all the experiments,
the same batch of gold concentrate was used. Therefore, we directly
used the gold content of the cyanide tailings after extraction to evaluate
the strengthening effect of ultrasound on gold cyanidation. In addition,
3
Ultrasonics - Sonochemistry 64 (2020) 105039
Fig. 3. Effect of ultrasound on the extraction rate of gold at the (a) low tem-
perature of 10 °C and (b) conventional temperature of 25 °C. The reaction time
of each group of leaching reactions was 24 h. Sonication was executed in the
first 4 h in the ultrasound-assisted extraction.
the unit consumption of NaCN was investigated to evaluate the cost of
gold cyanidation. The unit consumption of NaCN is defined as the mass
of NaCN consumed per kilogram of gold ore leached. After the ex-
periment, the leachate and the remaining tailings were recovered and
subsequently poured into the leaching tank in the industrial process, so
the gold and CN− in the leachate were reused without causing en-
vironmental impact.
2.3. Characterization
The gold content in the cyanide tailings was detected by AAS. The
phase species of raw ore and cyanide tailings were analyzed by X-ray
diffraction (XRD, PERT, Panalytical, Netherlands). The microcosmic
morphology of samples was characterized by scanning electron micro-
scope (SEM, S-4300, HITACHI, Japan). The particle size of ores and
cyanide tailings were measured by laser particle size analyzer
(Mastersize 2000, Malvern, Britain). A portable ion concentrator (Bante
320, BANTE, China) was used to detect the CN− concentration of ore
slurry and barren liquor.
S. Yu, et al.
Fig. 4. Effect of ultrasound on the unit consumption of NaCN of gold at the (a)
low temperature of 10 °C and (b) conventional temperature of 25 °C. The re-
action time of each group of leaching reactions was 24 h. Sonication was exe-
cuted in the first 4 h in the ultrasound-assisted extraction.
3. Results and discussion
3.1. Mechanism of ultrasound treatment on slurry at low temperature
The essence of gold cyanidation is that gold dissolves in the alkaline
cyanide solution and forms a gold cyanide complex (Au(CN)2 ). This
dissolution mechanism is essentially an electrochemical reaction pro-
cess. The overall reaction is shown in Eq. (1) [36].
4Au + 8CN + O2 + 2H2 O 4Au(CN)2 + 4OH (1)
It can be seen that the gold extraction reaction is directly related to
the cyanide concentration. In general, at the optimal gold extraction pH
of 10.5 or higher, most of the cyanide is presented in the CN−, where
cyanide loss by volatilization of hydrogen cyanide acid (HCN) is limited
effectively. Ultrasonic cavitation can accelerate certain physical and
chemical reactions and may even trigger new reactions. Therefore, the
effect of ultrasonic treatment on the loss of CN− by volatilization of
HCN was investigated before the experiments. The result showed that
the CN− concentration of barren liquor remained the same after 20-
minute sonication at the temperature of 10 °C and 25 °C, respectively.
This illustrates that ultrasonic treatment will not cause loss of CN−.
Besides the CN− concentration, the electrochemical reaction
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Ultrasonics - Sonochemistry 64 (2020) 105039
process of gold cyanidation is dramatically affected by reaction tem-
perature [37,38]. The optimal temperature for cyanide leaching gold in
industrial production processes is 25–30 °C. Although higher tempera-
tures can improve the efficiency of leaching, it will take large amounts
of energy to heat large gold cyanidation systems. Higher temperatures
also intensify the HCN volatilization in extraction process, which will
bring much extra consumption of NaCN and environmental pollution
[39,40]. In contrast, the extraction rate of gold is significantly limited at
low extraction temperature. Hence the cyanide reaction tanks have to
be heated to ensure the efficiency of gold cyanidation in winter, which
consumes a large amount of additional energy. In order to solve these
problems, a sonochemical reactor was employed to study the ultra-
sound assisted cyanide leaching gold from gold concentrate at low
temperature. Ultrasonic cavitation was generated at low temperatures
and then produced mixing, chipping, corrosion, wetting and sound-
capillaries, which can effectively promote physical and chemical reac-
tion at low temperature.
To explore the mechanism of ultrasound promoting gold cyanida-
tion at low temperature, the agitation and heat transfer of ore slurry
were simulated using the commercial software (COMSOL Multiphysics).
The velocity distribution of ore slurry under mechanical stirring and
ultrasound-assisted mechanical stirring at 10 °C are shown in Fig. 2(a)
and (b), respectively. The ren vector arrows in the figures symbolizes
the velocity direction of the slurry. It can be seen that the velocity of ore
slurry was effectively improved by the ultrasound-assisted treatment,
which means that mass transfer and extraction reaction were enhanced
significantly. Moreover, the change in the red vector arrows indicates
an obvious growth in the radial velocity of the slurry, which facilitates a
more uniform mixing and sonication of the slurry.
In addition to mechanical mixing, ultrasonic treatment can cause
local temperature rise. Therefore, the temperature distribution of ore
slurry under sonication at 10 °C was also assessed. As shown in
Fig. 2(c), ore slurry was heated under sonication, and the temperature
of the ore slurry near the horn of transducer even reached 15 °C. Me-
chanical stirring caused most of ore slurry to be sonicated to increase its
temperature. The temperature values of ore slurry near the horn mea-
sured repeatedly in the experiment were 13–16 °C, which corresponded
to the results shown in Fig. 2(c). In order to weaken the effect of
temperature rise caused by ultrasonic treatment, the circulating cooling
water was lower than 10 °C (~7–8 °C) and 25 °C (~21–23 °C) to
maintain the average temperature in ultrasound-assisted extraction
experiments at low temperature and normal temperature, respectively.
During the ultrasound-assisted extraction, the temperature values of ore
slurry near the horn were about two degrees higher than the average
temperature, which had little effect on extraction reaction.
The results of Fig. 2 illustrate that the intense mechanical mixing
caused by ultrasound can counteract the limitation of low temperature
on gold leaching reaction, which will in turn enhance the extraction
rate of gold significantly at low temperature. Ultrasound cavitation also
produced high-speed micro-jets and strong shear force, which deeply
destroyed the surface of extremely fine ore particles and promoted the
gold leaching.
3.2. Effect of ultrasound on the extraction rate of gold and consumption of
NaCN
Although the results of Fig. 2 demonstrate the potentiation of ul-
trasound on gold leaching reaction at low temperature, the specific law
of this effect is still unclear. Therefore, the effect of ultrasound on cy-
anide leaching of gold at low temperature is investigated experimen-
tally in this section. As shown in Fig. 3 (a), the black line and blue line
represent the extraction rate of gold at different cyanide concentration
after 24 h of conventional extraction at 25 °C and 10 °C, respectively.
The red line represents the extraction rate of gold after 24 h of ultra-
sound-assisted extraction at 10 °C, in which the sonication was only
applied for the first 4 h. As can be seen, the extraction rate in
S. Yu, et al.
Fig. 5. Gold content of secondary extracted cyanide tailings at different ex-
traction process. Cyanide tailings after 48 h of industrial extraction were ex-
tracted for 9 h using different methods, keeping the CN− concentration of
0.1 mol/L. Sonication was executed in the first 1 h in the ultrasound-assisted
extraction.
Fig. 6. Effect of ultrasound on the reaction rate of gold leaching. Gold con-
centrate was extracted at the temperature of 25 °C and CN− concentration of
0.1 mol/L. Sonication was executed in the first 4 h in the ultrasound-assisted
extraction.
conventional extraction at 10 °C was much lower than that in con-
ventional extraction at 25 °C. This is because the rate and yield of ex-
traction reaction were severely limited at low temperature. However,
ultrasound-assisted treatment increased the extraction rate of gold by
0.6%–0.8% at 10 °C, which was close to the extraction rate in con-
ventional extraction at 25 °C. The reason is that the bubble collapse
caused by ultrasonic cavitation created high-speed liquid jets and hot
spots with temperatures of up to tens of thousands of Kelvin [41,42],
which enhanced the mass transfer and heated slurry to a certain extent.
In consequence, the rate and yield of extraction reaction were effec-
tively promoted by ultrasound at low temperature.
It can be seen from Fig. 3(a) that the extraction rate of gold in
conventional extraction at 25 °C was already high. However, the gold
content of the cyanide tailings was even high and some of the valuable
gold could be extracted [43,44]. The global gold production will in-
crease by 3 t for every 0.1% enhancement in gold extraction rate, and
the corresponding growth of gold industry's income is considerable.
Therefore, the effect of ultrasound on the gold cyanidation in
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Ultrasonics - Sonochemistry 64 (2020) 105039
Fig. 7. Evaluation of reaction rate constant of (a) conventional extraction and
ultrasound-assisted extraction at 10 °C and conventional extraction at 25 °C of
the secondary extraction. (b) conventional extraction and ultrasound-assisted
extraction at 25 °C.
conventional conditions was studied in this work. Fig. 3(b) further
presents the effect of sonication on the extraction rate of gold at the
conventional temperature of 25 °C. The black line and green line re-
present the extraction rate of gold at different cyanide concentration in
conventional extraction and ultrasound-assisted extraction, respec-
tively. The extraction rate of gold rose with an increase in CN− con-
centration. At the CN− concentration of 0.04–0.1 mol/L, ultrasound-
assisted treatment increased the extraction rate of gold by 0.1%–0.2%.
However, the ultrasound-assisted extraction had no obvious promotion
effect on gold cyanidation when the CN− concentration reached
0.12 mol/L or higher. This is because almost all of the non-wrapped
gold contacted with CN− and was leached at extremely high CN−
concentration.
The results of Fig. 3 also indicate that the extraction rate of gold rose
with a growth of CN− concentration. However, the high CN− con-
centration will cause excessive consumption of NaCN and increase the
difficulty of subsequent cyanide-containing wastewater treatment. The
consumption of NaCN is also an important indicator for evaluating the
profitability of gold production. Hence, the effect of ultrasound on the
consumption of NaCN at low temperature was further studied. Fig. 4
shows the unit consumption of NaCN after different extraction reaction.
In Fig. 4(a), the red and blue columns represent the unit consumption of
S. Yu, et al. Ultrasonics - Sonochemistry 64 (2020) 105039

Table 2
Performance of ultrasound-assisted extraction and conventional extraction.
Terms 10 °C 25 °C

Conventional extraction ultrasound-assisted extraction Conventional extraction ultrasound-assisted extraction

Extraction rate (%) 98.01 98.66 98.72 98.86

Unit consumption of NaCN (g/kg) 1.063 1.623 2.074 2.260
Gold content of second extraction cyanide tailings (g/t) 0.36 0.28 0.35 /
Requirement of extra heat in industrial process Yes No No No

Fig. 8. X-ray diffraction pattern of raw gold ore and cyanide tailings.

NaCN at different cyanide concentration after 24 h of conventional
extraction at 25 °C and 10 °C, respectively. The green column represents
the unit consumption of NaCN after 24 h of ultrasound-assisted ex-
traction at 10 °C. As can be seen, the unit consumption of NaCN in
conventional extraction at 10 °C was low and hardly changed with an
increase of CN− concentration, while the unit consumption of NaCN in
ultrasound-assisted extraction at 10 °C was higher and increased with
increasing of CN− concentration. This phenomenon corresponds to the
higher extraction rate in ultrasound-assisted extraction in Fig. 3(a).
When the CN− concentration was higher than 0.06 mol/L, ultrasound-
assisted extraction at 10 °C achieved a much lower unit consumption of
NaCN and a similar extraction rate of gold comparing to the conven-
tional extraction at 25 °C. For example, ultrasound-assisted extraction
at a CN− concentration of 0.12 mol/L and temperature of 10 °C
achieved the same extraction rate to the conventional extraction at the
CN− concentration of 0.1 mol/L and temperature of 25 °C, while the
unit consumption of NaCN was 16% lower. This means that ultrasound-
assisted extraction can obtain high extraction rate of gold and obviously
reduce NaCN consumption at low temperature.
The unit consumption of NaCN after different extraction at 25 °C is
presented in Fig. 4 (b). The unit consumption of NaCN increased with
an increase of the CN− concentration. At the same CN− concentration,
the unit consumption of NaCN in ultrasound-assisted extraction was
higher than that in conventional extraction. This is because ultrasonic
cavitation promoted the progress of extraction reaction and other
chemical reactions, and consequently more gold and other substances
reacted with NaCN in the ultrasound-assisted extraction. Fig. 4(b) il-
lustrates that ultrasound-assisted extraction increased the extraction of
gold in conventional conditions and reduced the consumption of NaCN.
For example, ultrasound-assisted extraction at a CN− concentration of
0.06 mol/L achieved the 0.1% higher extraction rate than the con-
ventional extraction at a CN− concentration of 0.08 mol/L, and the unit
consumption of NaCN was 15% lower.

6
S. Yu, et al.
Fig. 9. Scanning electron microscope (SEM) images of (a) raw gold ore, (b)
cyanide tailings after conventional extraction and (c) cyanide tailings after
ultrasound-assisted extraction.
3.3. Effect of ultrasound on the limit and reaction rate of gold leaching
It is believed that strong cavitation can also enhance the gold cya-
nidation by destroying the surface of ore particles, which can break
through the limits of conventional leaching, extracting the portion of
the unextracted deep-wrapped gold. To demonstrate this, the cyanide
tailings after 48 h of industrial extraction were used to study the effect
of ultrasound on secondary leaching of cyanide tailings. Gold content of
the cyanide tailings was as low as 0.4 g/t and almost all of the exposed
gold had been extracted. In this case, the enhancement of intense me-
chanical mixing and heating on gold leaching could be ignored.
Effect of ultrasound on secondary leaching of cyanide tailings was
7
Ultrasonics - Sonochemistry 64 (2020) 105039
investigated, keeping the CN-concentration of 0.1 mol/L. As showed in
Fig. 5, the black and blue lines represent the gold content of cyanide
tailings after different conventional extraction time at 25 °C and 10 °C,
respectively. The red line represents the gold content of cyanide tailings
after different ultrasound-assisted extraction time at 10 °C, in which the
sonication was only applied for the first hour. The use of gold content in
the tailings after secondary leaching to demonstrate the advantages of
ultrasound-assisted extraction is more intuitive. As can be seen, the gold
content of the secondary leached cyanide tailings reached the limit
value (~0.36 g/t) after conventional extraction. However, the gold
content of the cyanide tailings was further reduced to 0.28 g/t after
ultrasound assisted extraction. The corresponding extraction rate was
higher than 99%. The reason is that high-speed micro-jets and strong
shear force produced by ultrasound cavitation destroyed the surface of
the ore particles, and exposed the wrapped gold to the lixiviants. It’s
worth noting that this phenomenon will be significant in the extraction
of refractory ore.
Most industrial production processes greatly extend the extraction
time and even more than 60 h to obtain a high extraction rate of gold.
Longer extraction times increase the cost of cyanide extraction of gold.
Therefore, the effect of the ultrasound on the rate of extraction reaction
was investigated, keeping the temperature of 25 °C and CN− con-
centration of 0.1 mol/L. During the ultrasound-assisted extraction, so-
nication was only applied during the first 4 h. Fig. 6 shows the ex-
traction rate of gold after different extraction time. The black line and
green line present the extraction rate of gold after different extraction
time of conventional extraction and ultrasound-assisted extraction, re-
spectively. As can be seen, most of the gold was extracted from ore after
12-hour conventional extraction, while it took only 4 h in ultrasound-
assisted extraction. It can be found that the rate of extraction reaction
was effectively increased with the ultrasound-assisted treatment. This is
because that the high-speed micro-jets generated by ultrasonic cavita-
tion accelerated the mass transfer and improved the diffusion rate of
gold ore particles [45].
Reaction kinetic models of different temperatures and different
leaching methods were built to better identify the mechanisms that
occur during the leaching process. In the reaction of Eq. (1), the re-
actant CN−, O2 and H2O were in large excess. The kinetic order of the
reaction can thus be decreased to a first-order reaction. The reaction
rate constant is evaluated by plotting ln([Au]) against extraction time
as can be seen in Fig. 7(a) and (b). The slope of the plot refers to the
additive inverse of the reaction rate constant respectively, and it’s listed
in the table A1. It can be noticed that the higher the reaction tem-
perature is, the higher the reaction rate constant is. The ultrasound
indeed helped to increase the reaction rate constant dramatically. In
addition, taking the plot of the natural logarithm of two reaction rate
constants at 10 °C and 25 °C under the same experimental condition
against 1/T, the activation energy of the reaction under this condition
can be analyzed to be 2.2 kJ/mol. An activation energy of less than
10 kJ/mol implies that with increasing temperature the reaction can
only be limitedly accelerated. This also indicated that in the low tem-
perature, especially for the gold concentrates with low gold content,
promotion effect of sonication on gold leaching is significant.
In order to more intuitively compare the performance of ultrasound-
assisted and conventional extraction, the extraction yields and costs of
the two leaching processes at a CN− concentration of 0.1 mol/L were
compared in Table 2. As can be seen, at the low temperature of 10 °C,
the extraction rate of gold after ultrasonic-assisted extraction was
greatly improved. Although the unit consumption of NaCN was also
increased, its value is negligible compared to the increased leached
gold. Similarly, ultrasound-assisted extraction also increased the ex-
traction rate to a certain extent at the conventional temperature of
25 °C. In addition, ultrasonic-assisted leaching eliminates the need for
extra heat for gold leaching at low temperatures.
S. Yu, et al. Ultrasonics - Sonochemistry 64 (2020) 105039

Fig. 10. The particle size distribution of raw gold ore and cyanide tailings. The
average particle sizes were shown in the legend.

3.4. Mineralogical and morphology analysis

Fig. 8 shows the X-ray diffraction pattern of the raw gold ore and
cyanide tailings. As can be seen, the phase species of gold ore were not
changed after cyanide leaching while the peak intensity of SiO2 and
FeS2 was changed. After conventional extraction of 8 h, the peak in-
tensity of SiO2 increased to some extent and the peak intensity of FeS2
changed inconspicuously, which indicates that a certain amount of
substances in raw gold ore had been dissolved. However, the peak in-
tensities of SiO2 and FeS2 rose obviously after 4-hour ultrasound-as-
sisted extraction, which indicates that more other substances had been
dissolved. Hence, the relative content of SiO2 and FeS2 in the cyanide
tailings increased [44]. It indicates that the liquid–solid reaction rate
was accelerated obviously in the ultrasound-assisted extraction.
In addition to the solubility of gold ore, the rate and yield of gold
cyanidation are affected by the ore particle size [46]. Fig. 9 shows the
SEM images of raw gold ore, cyanide tailing after conventional ex-
traction and cyanide tailing after ultrasound-assisted extraction. As
described in Fig. 9, the raw gold ore contains a large number of large
particles that were wrapped by tiny particles, which hindered the re-
action of cyanide ion and gold wrapped in ore particle. After conven-
tional extraction, many large particles still existed in cyanide tailings
and the change of particle surface was not obviously. Nonetheless, the
ore particles were significantly smashed and the particle surface was
washed effectively after ultrasound-assisted extraction. It means that
ultrasound-assisted extraction accelerated the liquid–solid reaction and
promoted gold leaching.
In order to investigate the effect of ultrasound on ore particle size Fig. 11. Scanning electron microscope (SEM) images of FeS2 in (a) raw gold
accurately, the particle size analysis of ore before and after extraction ore, (b) cyanide tailings after conventional extraction and (c) cyanide tailings
after ultrasound-assisted extraction.
was studied. Fig. 10 shows the particle size distribution of raw gold ore,
cyanide tailings after conventional extraction and cyanide tailings after
ultrasound-assisted extraction, respectively. As can be seen, many large ore in this research is wrapped in pyrite (FeS2), which hinders the ex-
particles with a particle size larger than 300 μm existed in the raw gold traction rate of gold [47]. Therefore, destroying the FeS2 is crucial for
ore. The average particle size of ore decreased from 32.15 μm to leaching gold from gold ore effectively. The morphology of pyrite in the
28.60 μm after conventional extraction, and the large particles with a ore before and after extraction is shown in Fig. 11. The number of edge
particle size larger than 300 μm had disappeared. The average particle angles and attachments on surface decreased while the pyrite was not
size of the ore was further reduced to 22.27 μm after ultrasound-as- fully opened after conventional extraction, so the wrapped gold could
sisted extraction. In addition, the number of particles with particle size not be effectively exposed to the solution. However, after ultrasound-
larger than 70 μm significantly reduced while the number of particles assisted extraction, the surface of pyrite became cleaner and smoother,
with particle size of 10–20 μm increased. It indicates that sonication and even some wispy fissures were produced. Hence, more refractory
broke up the large particles and homogenized the ore particles, which gold wrapped in pyrite was exposed to the solution and leached through
also demonstrates the results of Fig. 9. the pores and fissure in ultrasound-assisted extraction. This is because
It can be seen from Table 1 and Fig. 8 that the refractory gold in the the high-speed micro jet produced by ultrasonic cavitation generated a

8
S. Yu, et al.
continuous and dramatic impact force on ore particles, which can
change the surface morphology of pyrite and open pyrite to promote
gold leaching [32,48]. Moreover, the intensely ultrasonic cavitation can
destroy the passive film of extraction reaction and enhance the mass
transfer in the extraction solution. It is proved that ultrasound assisted
cyanide extraction can enhance the extraction rate of gold and shorten
extraction time.
4. Conclusion
This study developed a sonochemical reactor to explore the effect of
ultrasound on cyanide leaching of gold at low temperature. Simulation
results demonstrated that the velocity and temperature of ore slurry
were enhanced under ultrasound treatment. Ultrasound-assisted cya-
nide leaching gold in conventional and low temperature extraction
were carried out. The ultrasound-assisted extraction rate of gold at the
low temperature of 10 °C was similar to the one in conventional ex-
traction at 25 °C, and the unit consumption of NaCN reduced by 16%.
Gold content of cyanide tailings decreased to a minimum limit of
0.28 g/t using ultrasound-assisted secondary leaching at 10 °C, sug-
gesting the corresponding extraction rate of gold exceeded 99%.
Moreover, the ultrasound-assisted extraction rate of gold at the con-
ventional temperature of 25 °C was 0.1% higher compared with the one
in conventional extraction at 25 °C, and the unit consumption of NaCN
declined by 15%. Extraction time was also shortened significantly at
ultrasound-assisted processing. Reaction rate constants and activation
energy obtained from kinetics analysis indicated the enhanced effect of
sonication during gold cyanidation.
The XRD results showed that ultrasonic treatment accelerated the
mass transfer and liquid–solid reaction in a slurry. The SEM and particle
size analysis indicated that the ore particles were smashed, the passive
film was destroyed and reaction resistance was decreased by ultra-
sound. In consequence, ultrasound-assisted cyanide extraction can ef-
Appendix A
Table A1
The reaction rate constant of the reaction under different conditions.
k (extraction of gold concentrate, Fig. 6)
Conventional extraction at 0.267
25 °C
Ultrasound-assisted extraction 0.855
at 25 °C
References
[1] T. Sato, H. Watanabe, The extraction of zirconium (IV) from hydrochloric acid
solutions by high-molecular-weight amines, Anal. Chim. Acta. 54 (1971) 439–446.
[2] H. Murakami, S. Nishihama, K. Yoshizuka, Separation and recovery of gold from
waste LED using ion exchange method, Hydrometallurgy 157 (2015) 194–198.
[3] N. Das, Recovery of precious metals through biosorption-a review, Hydrometallurgy
103 (2010) 180–189.
[4] M. Lampinen, A. Laari, I. Turunen, Ammoniacal thiosulfate leaching of pressure
oxidized sulfide gold concentrate with low reagent consumption, Hydrometallurgy
151 (2015) 1–9.
[5] M. Baghalha, Leaching of an oxide gold ore with chloride/hypochlorite solutions,
Int. J. Miner. Process. 82 (2007) 178–186.
[6] S.R.L. Brooy, H.G. Linge, G.S. Walker, Review of gold extraction from ores, Miner.
Eng. 7 (1994) 1213–1241.
[7] B. Donmez, F. Sevim, S. Colak, A study on recovery of gold from decopperized
anode slime, Chem. Eng. Technol. 24 (2001) 91–95.
9
Ultrasonics - Sonochemistry 64 (2020) 105039
fectively promote the full leaching of gold and dose will have a good
application prospect in gold smelting.
CRediT authorship contribution statement
Shimin Yu: Writing-Original draft, Methodology. Tingting Yu:
Writing - original draft. Wenping Song: Methodology,
Conceptualization, Writing - review & editing. Xiyang Yu: Data cura-
tion. Jianxin Qiao: Software. Wuyi Wang: Visualization. Huijuan
Dong: Investigation. Zhiguang Wu: Formal analysis. Lizhou Dai:
Formal analysis. Tianlong Li: Methodology, Conceptualization, Writing
- review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgements
This work was supported by the National Natural Science
Foundation of China, China (No. 51675140). China Postdoctoral
Science Foundation Grant (Nos. 2017 M621257 and 2018 T110285),
General Financial Grant from the Heilongjiang Postdoctoral Science
Foundation, China (Nos. LBH-Z17055, LBH-TZ12), Fundamental
Research Funds for Central Universities, China (No. HIT. NSRIF.
2019051), State Key Laboratory of Robotics and System, China
(SKLRS201807B), State Key laboratory of Advanced Technology for
Materials Synthesis and Processing, China (Wuhan University of
Technology) and Key Laboratory of Micro-systems and Microstructures
Manufacturing of Ministry of Education, China (No. 2018KM009).
k (extraction of cyanide tailings, Fig. 5)
Conventional extraction at 0.013
10 °C
Ultrasound-assisted extraction 0.052
at 10 °C
Conventional extraction at 0.021
25 °C
[8] T.L. Deng, M.X. Liao, M.H. Wang, Y.-M. Chen, N. Belzile, Enhancement of gold
extraction from biooxidation residues using an acidic sodium sulphite-thiourea
system, Miner. Eng. 14 (2001) 263–268.
[9] O.E. Kuzugudenli, C. Kantar, Alternatives to gold recovery by cyanide leaching, Erc.
Univ. Fen. Bil. Derg. 15 (1999) 119–127.
[10] J. Viñals, E. Juan, M. Ruiz, E. Ferrando, M. Cruells, A. Roca, J. Casado, Leaching of
gold and palladium with aqueous ozone in dilute chloride media, Hydrometallurgy
81 (2006) 142–151.
[11] X.M. Zhang, G. Senanayake, A review of ammoniacal thiosulfate leaching of gold:
an update useful for further research in non-cyanide gold lixiviants, Miner. Process
Extr. Metall. Rev. 37 (2016) 385–411.
[12] S.S. Konyratbekova, A. Baikonurova, A. Akcil, Non-cyanide leaching processes in
gold hydrometallurgy and iodine-iodide applications: a review, Miner. Process Extr.
Metall. Rev. 36 (2015) 198–212.
[13] L. Fu, L. Zhang, S. Wang, W. Cui, J. Peng, Synergistic extraction of gold from the
refractory gold ore via ultrasound and chlorination-oxidation, Ultrason. Sonochem.
37 (2017) 471–477.
[14] G. Hilson, A.J. Monhemius, Alternatives to cyanide in the gold mining industry:
S. Yu, et al.
what prospects for the future? J. Clean Prod. 14 (2006) 1158–1167.
[15] Y. Guan, E.J. Hensen, Cyanide leaching of Au/CeO2: highly active gold clusters for
1,3-butadiene hydrogenation, Phys. Chem. Chem. Phys. 11 (2009) 9578–9582.
[16] T.O. Nunan, I.L. Viana, G.C. Peixoto, H. Ernesto, D.M. Verster, J.H. Pereira,
J.M. Bonfatti, L.A.C. Teixeira, Improvements in gold ore cyanidation by pre-oxi-
dation with hydrogen peroxide, Miner. Eng. 108 (2017) 67–70.
[17] Q. Li, T. Jiang, Y. Yang, G. Li, Y. Guo, G. Qiu, Co-intensification of cyanide leaching
gold by mercury ions and oxidant, Trans. Nonferrous Met. Soc. China 20 (2010)
1521–1526.
[18] R.K. Amankwah, A.U. Khan, C.A. Pickles, W.T. Yen, Improved grindability and gold
liberation by microwave pretreatment of a free-milling gold ore, Miner. Process
Extr. Metall. 114 (2005) 30–36.
[19] N. Kuyucak, A. Akcil, Cyanide and removal options from effluents in gold mining
and metallurgical processes, Miner. Eng. 50 (2013) 13–29.
[20] J.J. Hinman, K.S. Suslick, Nanostructured materials synthesis using ultrasound,
sonochemistry 375 (2017) 59–94.
[21] A. Fenster, D.B. Downey, 3-D ultrasound imaging: a review, IEEE Eng. Med. Biol. 15
(1996) 41–51.
[22] H.K. Wickramasinghe, Scanning acoustic microscopy: a review, J. Microsc. 129
(1983) 11.
[23] T. Lee, W. Luo, Q. Li, H. Demirci, L. Guo, Laser-induced focused ultrasound for
cavitation treatment: toward high-precision invisible sonic scalpel, Small 13 (2017)
1701555.
[24] J. Li, T. Li, T. Xu, M. Kiristi, W. Liu, Z. Wu, J. Wang, Magneto–acoustic hybrid
nanomotor, Nano Lett. 15 (2015) 4814–4821.
[25] T. Xu, F. Soto, W. Gao, V. Garcia-Gradilla, J. Li, X. Zhang, J. Wang, Ultrasound-
modulated bubble propulsion of chemically powered microengines, J. Am. Chem.
Soc. 136 (2014) 8552–8555.
[26] T. Xu, F. Soto, W. Gao, R. Dong, V. Garcia-Gradilla, E. Magaña, X. Zhang, J. Wang,
Reversible swarming and separation of self-propelled chemically powered nano-
motors under acoustic fields, J. Am. Chem. Soc. 137 (2015) 2163–2166.
[27] I. Tzanakis, G.S.B. Lebon, D.G. Eskin, K.A. Pericleous, Characterizing the cavitation
development and acoustic spectrum in various liquids, Ultrason. Sonochem. 34
(2017) 651–662.
[28] N.S.M. Yusof, B. Babgi, Y. Alghamdi, M. Aksu, J. Madhavan, M. Ashokkumar,
Physical and chemical effects of acoustic cavitation in selected ultrasonic cleaning
applications, Ultrason. Sonochem. 29 (2015) 568–576.
[29] D. Radziuk, H. Möhwald, Ultrasonically treated liquid interfaces for progress in
cleaning and separation processes, Phys. Chem. Chem. Phys. 18 (2015) 21–46.
[30] R.R. Deshmukh, R. Rajagopal, K.V. Srinivasan, Ultrasound promoted C-C bond
formation: Heck reaction at ambient conditions in room temperature ionic liquids,
Chem. Commun. 17 (2001) 1544–1545.
[31] G.V. Ambulgekar, B.M. Bhanage, S.D. Samant, Low temperature recyclable catalyst
for Heck reactions using ultrasound, Tetrahedron Lett. 46 (2005) 2483–2485.
[32] S. Yin, J. Pei, F. Jiang, S. Li, J. Peng, L. Zhang, S. Ju, C. Srinivasakannan,
Ultrasound-assisted leaching of rare earths from the weathered crust elution-
10
Ultrasonics - Sonochemistry 64 (2020) 105039
deposited ore using magnesium sulfate without ammonia-nitrogen pollution,
Ultrason. Sonochem. 41 (2018) 156–162.
[33] P. Zhu, X. Zhang, K. Li, G. Qian, M. Zhou, Kinetics of leaching refractory gold ores
by ultrasonic-assisted electro-chlorination, Int. J. Min. Met. Mater. 19 (2012)
473–477.
[34] I.D.L. Calle, N. Cabaleiro, M. Costas, F. Pena, S. Gil, I. Lavilla, C. Bendicho,
Ultrasound-assisted extraction of gold and silver from environmental samples using
different extractants followed by electrothermal-atomic absorption spectrometry,
Microchem J. 97 (2011) 93–100.
[35] L. Xiong, S. Shen, L. Liu, L. Zhang, Selective and effective reduction of gold Ions
from acidic HCl–NaClO3 leachate with oxalic acid, Ind. Eng. Chem. Res. 53 (2014)
16672–16677.
[36] E.A. Oraby, J.J. Eksteen, Gold dissolution and copper suppression during leaching
of copper–gold gravity concentrates in caustic soda-low free cyanide solutions,
Miner. Eng. 87 (2016) 10–17.
[37] Z.L. Wu, Z.S. Huang, R.M. Ruan, S.P. Zhong, B.K.C. Chan, Effect of temperature on
column bioleaching of a refractory gold ore, Adv. Mater. Res. 825 (2013) 352–355.
[38] J.S.J. van Deventer, P.F. van der Merwe, The effect of temperature on the deso-
rption of gold cyanide from activated carbon, Thermochim. Acta 221 (1993)
99–113.
[39] S.C. Bouffard, D.G. Dixon, Evaluation of kinetic and diffusion phenomena in cya-
nide leaching of crushed and run-of-mine gold ores, Hydrometallurgy 86 (2007)
63–71.
[40] I. Dobrosz-Gómez, B.D. Ramos García, E. Gilpavas, M.Á. Gómez García, Kinetic
study on HCN volatilization in gold leaching tailing ponds, Miner. Eng. 110 (2017)
185–194.
[41] R. Hiller, S.J. Putterman, B.P. Barber, Spectrum of synchronous picosecond sono-
luminescence, Phys. Rev. Lett. 69 (1992) 1182–1184.
[42] C.D. Ohl, T. Kurz, R. Geisler, O. Lindau, W. Lauterborn, Bubble dynamics, shock
waves and sonoluminescence, Phil. Os. T. R. Soc. A. 357 (1999) 269–294.
[43] I.M.S.K. Ilankoon, Y. Tang, Y. Ghorbani, S. Northey, M. Yellishetty, X. Deng,
D. McBride, The current state and future directions of percolation leaching in the
Chinese mining industry: Challenges and opportunities, Miner. Eng. 125 (2018)
206–222.
[44] B. Liu, Z. Zhang, L. Li, Y. Wang, Recovery of gold and Iron from the cyanide tailings
by magnetic roasting, Rare Metal Mat. Eng. 42 (2013) 1805–1809.
[45] C.D. Ohl, M. Arora, R. Ikink, N. De Jong, M. Versluis, M. Delius, D. Lohse,
Sonoporation from jetting cavitation bubbles, Biophys. J. 91 (2006) 4285–4295.
[46] S. Ellis, G. Senanayake, The effects of dissolved oxygen and cyanide dosage on gold
extraction from a pyrrhotite-rich ore, Hydrometallurgy 72 (2004) 39–50.
[47] A.E. Panyushkina, I.A. Tsaplina, N.V. Grigor’eva, T.F. Kondrat’eva,
Thermoacidophilic microbial community oxidizing the gold-bearing flotation con-
centrate of a pyrite-arsenopyrite ore, Microbiology 83 (2014) 539–549.
[48] J. Rooze, E.V. Rebrov, J.C. Schouten, J.T.F. Keurentjes, Dissolved gas and ultrasonic
cavitation: a review, Ultrason. Sonochem. 20 (2013) 1–11.