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Bromic acid-thiourea synergistic leaching of sulfide gold ore

  • Zhang Qiang , Duan Jing-Ze and Xiang Peng-Zhi EMAIL logo
Published/Copyright: October 29, 2024
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Green Processing and Synthesis
From the journal Green Processing and Synthesis Volume 13 Issue 1

Abstract

Bromate–thiourea coordinated leaching of gold sulfide ore for gold sulfide ore as leaching object. The effects of leaching reagent, stirring speed, and leaching time on gold leaching were investigated in this article. The results showed that the optimum leaching conditions were potassium bromate 0.1 M, thiourea 0.6 g·L−1, hydrochloric acid 0.2 M, agitation speed 250 rpm, ratio of liquid to solid 4, and leaching time 10 min. Under these conditions, high efficiency and rapid leaching of gold can be achieved, and reagent consumption is reduced. The research results have theoretical and practical significance for expanding new green gold extraction technology.

Keywords: bromate; thiourea; synergistic leaching; green gold extraction

1 Introduction

It is difficult to extract gold from refractory sulfur-bearing gold ore by cyanidation. At the same time, the highly toxic cyanide will cause serious environmental pollution and ecological damage, some countries have banned the use of cyanide gold extraction [1,2]. Therefore, it is urgent to find a non-cyanide leaching method that can deal with this kind of gold ore effectively. The exposure of gold in sulfide ore should be considered first. The direct leaching of sulfide ore is usually in the range of acidity, and the gold can be directly leached by a suitable oxidant. As a strong oxidant, bromate is more Standard electrode potential than most oxidants under acidic conditions. Due to the oxidizing property of bromate, it can completely satisfy the dissolution of gold. After the leaching of gold, the bromate reduction product is a bromide, which is usually non-toxic. Therefore, the method is also a green gold extraction method [3,4,5].

Thiourea process is a non-cyanide technology that can be applied in the future because of its quick leaching kinetics and non-toxicity [6]. In the thiourea process, the iron ion is usually used as an oxidant, but this method has the problems of difficult leaching and a slow leaching rate. In addition to iron, bromic acid as a strong oxidant can also be used for gold leaching. The potential at the initial stage of gold leaching is greater than 1.131 V, which satisfies the reduction potential of oxidant required for the bromination leaching system. Therefore, it is feasible to extract gold from raw ore by this method. However, due to the preservation of bromic acid, potassium bromate is usually acidified to form bromic acid which acts as an oxidant, in the leaching system, thiourea was used as a coordination agent for gold leaching [7]. The chemical reaction of the method is as follows:

Pre-leaching stage:

6 H + + BrO 3 − + 6 Au + 12 SC ( NH 2 ) 2 = 6 Au ( SC ( NH 2 ) 2 ) 2 + + Br − + 3 H 2 O

Later stage of leaching:

2 A u + B r O 3 − + 7 B r − + 6 H + = 2 A u B r 4 − + 3 H 2 O Δ r G m Θ = − 584.296 k J · m o l − 1

From the above chemical equations, it can be seen that the system has good gold-dissolving ability in both the early and late stages of leaching. It not only overcomes the weakness of traditional thiourea for gold dissolution of sulfide ores, but also reduces the excessive reagent consumption of the Bromic acid-thiourea system. In this article, the bromate–thiourea synergistic leaching of gold from refractory gold sulfide ore was studied. The effects of leaching reagent, stirring speed, and leaching time on gold leaching were investigated, and the experimental results have theoretical and practical significance for extending the new green gold extraction technology [8].

2 Experiment

2.1 Reagent

Potassium bromate, hydrochloric acid, thiourea, ferric chloride, and other reagents are analytical pure, experimental water for distilled water. The research object is a gold ore in Yunnan province. From Figure 1, it can be seen that the main minerals in the ore are quartz, dolomite, calcite, pyrite, chalcocite, etc. As can be seen from Table 1, the main recoverable valuable element in the ore is gold with a grade of 2.66 g·t−1. Among other elements, the content of S and As is higher. Due to the high content of S and As, the ore is refractory to leaching, and the gold grade is relatively low, but it still has a certain economic value.

Figure 1 XRD diagram of raw ore.
Figure 1

XRD diagram of raw ore.

Table 1

Elemental analysis of raw gold ore

Element Au (g·t−1) Cu Fe S As C MgO Al2O3 CaO K2O SiO2
Content (%) 2.66 0.15 2.62 1.88 0.29 6.76 1.51 9.50 3.45 4.57 67.57

2.2 Equipment

TAS-990 atomic absorption spectrophotometer (Beijing Puxi); PHS-3C acidity meter (Shanghai Yidian Scientific Instrument Co., Ltd.).

2.3 Leaching of gold

The ore is leached directly without roasting. The gold leaching test of the ore is carried out at room temperature by weighing a certain amount of ore sample and placing it in a conical flask. The leaching solution was prepared by mixing corresponding leaching reagent with deionized water. Adjust the pH of the pulp with sodium hydroxide or hydrochloric acid. During the leaching process, the pulp is stirred at a constant rate. At the end of the leaching test, the ore slurry is separated by solid and liquid to get the leached slag, and the leached slag is washed several times with deionized water, dried, and crushed, and then the gold content in the leached slag is analyzed, the leaching rate of gold was calculated. The formula for the gold leaching rate is as follows:

θ = m α − m 1 β m α × 100 %

Here, α is the gold content in the sample (g·t−1), β is the gold content in the leach residue (g·t−1), m is the weight of the sample (g), and m 1 is the weight of the leach residue (g).

3 Results and discussion

3.1 Effect of bromate concentration

In order to study the effect of the concentration of potassium bromate on gold leaching rate, the effect of different concentrations of potassium bromate on gold extraction was investigated. The other test conditions were: Hydrochloric acid 0.2 M, thiourea 0.6 g·L−1, the leaching time was 30 min and the stirring speed was 250 rpm. The results are shown in Figure 2. With the increase in the concentration of potassium bromate, the leaching rate of gold increased significantly. When the concentration of potassium bromate is 0.1 M, the leaching rate of gold is 90.5%. At the same time, when the concentration of potassium bromate is more than 0.1 M, the leaching rate of gold has little relation with the concentration of potassium bromate. Therefore, 0.1 M was chosen as the optimum concentration of potassium bromate.

Figure 2 Effect of potassium bromate concentration on gold extraction rate.
Figure 2

Effect of potassium bromate concentration on gold extraction rate.

3.2 Effect of thiourea concentration

When only potassium bromate is used as an oxidant, its consumption is larger [7]. In order to reduce the consumption of potassium bromate, thiourea was used as a leaching aid to oxidize sulfide ore. The design of the experiment is as follows: thiourea has the characteristics of a fast gold leaching rate and good selectivity. However, potassium bromate as an oxidant has a strong oxidation ability and can oxidize thiourea [9]. Therefore, it is necessary to control the concentration of thiourea. The effect of thiourea concentration on gold leaching from raw ore was studied at room temperature. The other test conditions were potassium bromate 0.1 M, hydrochloric acid 0.2 M, liquid–solid ratio of 4, reaction time of 30 min, and agitation speed of 250 rpm; the test results are shown in Figure 3. It was found that the leaching rate of gold reached 91.7% when the concentration of thiourea was 0.6 g·L−1. When the concentration of thiourea exceeds 0.6 g·L−1, the leaching rate of gold no longer increases. Therefore, 0.6 g·L−1 is the optimum concentration of thiourea for leaching of raw ore.

Figure 3 The effect of thiourea concentration on gold extraction rate.
Figure 3

The effect of thiourea concentration on gold extraction rate.

3.3 Effect of hydrochloric acid concentration

Thiourea is relatively stable in the acidic range, but potassium bromate has strong oxidation under acidic conditions. In order to reduce the over-oxidation of thiourea, it is necessary to keep suitable acidic conditions in the leaching system. In the leaching test, hydrochloric acid provided hydrogen ions, thus creating suitable acidic conditions and promoting the reaction. In order to investigate the influence of hydrochloric acid concentration on gold dissolution, the experimental conditions were set as follows: potassium bromate, 0.1 M; thiourea, 0.6 g·L−1; liquid–solid ratio, 4; leaching time, 30 min; agitation speed, 250 rpm; the result is shown in Figure 4. The leaching rate of gold increases rapidly with the increase in the concentration of hydrochloric acid, but when the concentration of hydrochloric acid is more than 0.2 M, the leaching rate of gold does not change significantly, so the optimum concentration of hydrochloric acid is 0.2 M.

Figure 4 The effect of hydrochloric acid concentration on gold extraction rate.
Figure 4

The effect of hydrochloric acid concentration on gold extraction rate.

3.4 The effect of liquid–solid ratio

In the process of gold leaching, the liquid–solid ratio has an important effect on the gold leaching rate [10]. The immobilization conditions were as follows: potassium bromate 0.1 M; thiourea, 0.6 g·L−1; hydrochloric acid, 0.2 M; leaching time, 30 min; and agitation speed, 250 rpm. Higher liquid–solid ratio is beneficial to the continuous improvement of the gold leaching rate. But the increase in liquid–solid ratio will lead to an increase in equipment cost. As can be seen from Figure 5, the leaching rate of gold does not increase when the liquid–solid ratio is greater than 4. Therefore, the optimal liquid–solid ratio is 4.

Figure 5 Effect of L/S on gold extraction rate.
Figure 5

Effect of L/S on gold extraction rate.

3.5 The influence of stirring speed

Generally speaking, the agitation speed has a great influence on gold leaching, by increasing the agitation speed and increasing the mass transfer rate [11]. Therefore, moderately increasing the stirring speed can promote the contact between the leaching solution and the solid particles, thus improving the gold leaching rate. The effect of stirring speed on gold leaching rate was studied. The reaction was carried out under the conditions of 0.1 M, fixed potassium bromate, 0.6 g·L−1 thiourea, 0.2 M hydrochloric acid, 30 min of reaction time, and 4 liquid–solid ratio. As shown in Figure 6, the gold leaching rate reaches its maximum at 250 rpm with the increase in stirring speed. When the stirring speed was further increased, the gold leaching rate did not change. The results show that the leaching effect of gold ore is best when the stirring speed is 250 rpm under the conditions.

Figure 6 Effect of stirring speed on gold extraction rate.
Figure 6

Effect of stirring speed on gold extraction rate.

3.6 Effect of leaching time

The leaching rate of gold increases with the prolongation of leaching time. But prolonged leaching time will lead to increased capital and reagent costs after a certain time [12]. Therefore, the selection of appropriate leaching time is the key to guarantee the efficient leaching of gold. The experimental conditions were as follows: potassium bromate, 0.1 M; thiourea, 0.6 g·L−1; hydrochloric acid, 0.2 M; agitation speed, 250 rpm; and liquid–solid ratio, 4. As can be seen from Figure 7, the leaching rate of the system is very fast, and the gold extraction rate can reach 92.3% in 10 min. Fast leaching rate is the biggest advantage of the bromate–thiourea synergistic leaching of gold sulfide ore. Secondly, compared with the literature [13,14,15], it can be found that this method reduces reagent consumption. But the reagent consumption is still large. Further optimization is needed.

Figure 7 Effect of leaching time on gold extraction rate.
Figure 7

Effect of leaching time on gold extraction rate.

3.7 Compared with thiourea methods

The test conditions of thiourea method are as follows [10,16]: thiosulfate concentration is 0.1 M, copper ion concentration is 0.05 M, ammonia concentration is 0.4 M, agitation speed is 250 rpm, liquid–solid ratio is 4, leaching time is 12 h, and pH is 2. The leaching rate of the same gold sample is 33.4%. The experimental conditions of the thiourea method were as follows: reaction temperature, 30°C; thiourea concentration, 1.5 g·L−1; iron ion concentration, 1.5 g·L−1, pH 1.5; leaching process with air, ratio of liquid to solid 4, leaching time 6 h, and the leaching rate of gold was only 43.1%. Due to the high content of S and As, the two methods did not achieve good leaching results. The reason is that the oxidizing agent has weak oxidizing ability and cannot fully oxidize sulfides in gold ore.

3.8 Characterization of gold ore before and after leaching

From the comparison of the surface of gold ore before and after leaching (Figure 8), the surface of gold ore becomes smooth and rough after leaching, and there are many pores. This shows that the surface of the gold ore was strongly corroded. Gold is leached by contact with the leaching solution of gold after the surface of the ore is corroded.

Figure 8 Characterization of gold ore before and after leaching (a) before leaching, (b) after leaching.
Figure 8

Characterization of gold ore before and after leaching (a) before leaching, (b) after leaching.

3.9 Comparison of thiourea consumption

The consumption of reagents is an important content in the leaching process. Thiourea concentration is the most important reagent in this method, and the amount of thiourea determines whether gold can be further leached. The consumption of two kinds of process reagents was compared. The two processes are potassium bromate, 0.1 M, thiourea, 0.6 g·L−1; hydrochloric acid, 0.2 M; agitation speed, 250 rpm; ratio of liquid to solid, 4; and leaching time, 10 min; thiourea concentration, 1.5 g·L−1, iron ion concentration, 1.5 g·L−1, pH 1.5; leaching process with air: ratio of liquid to solid, 4; leaching time, 6 h. The consumption of thiourea was investigated after leaching under the optimum experimental conditions. The results are shown in the Table 2.

Table 2

Comparison of leaching results and thiourea consumption by two different methods

System Leaching rate of gold (%) Leaching time Thiourea consumption (%)
Bromate–thiourea 92.3 10 min 88.7
Fe3+–thiourea 43.1 6 h 53.1

The results show that thiourea is consumed more than other methods, but this method still has a high leaching rate and short leaching time. Although the leaching time is very short, the oxidation of bromic acid is so strong that thiourea is oxidized quickly.

From the results of previous tests, the gold leaching rate is very high; the reason is that bromic acid can leach gold even at a low concentration of thiourea. The chemical reaction of the method is as follows:

BrO 3 − + 6 SC ( NH 2 ) 2 = 3 ( SCN 2 H 3 ) 2 + Br − + 3 H 2 O

BrO 3 − + 5 Br − + 6 H + = Br 2 + 3 H 2 O

2 Au + BrO 3 − + 7 Br − + 6 H + = 2 AuBr 4 − + 3 H 2 O

Compared with the bromic acid method, the concentration of potassium bromate used in this method is relatively less, so it is more environmentally friendly. But it is undeniable that the composition of the leaching solution is more complex, which will bring trouble for the next step of gold recovery.

4 Conclusion

In this article, bromate–thiourea synergistic leaching of gold sulfide ore has been studied. This method reduces the consumption of reagents, and the leaching time is greatly reduced compared with other gold extraction methods such as cyanidation and thiosulfate. The gold leaching effect is satisfactory. Through the experiment, the conditions of bromate–thiourea synergistic leaching of gold sulfide ore are as follows: the concentration of potassium bromate is 0.1 M, the concentration of thiourea is 0.6 g·L−1, the concentration of hydrochloric acid is 0.2 M, the agitation speed is 250 rpm, the ratio of liquid to solid is 4, and the leaching time was 10 min. Although the reagent consumption of this method is large, the leaching rate is high, and the leaching time is short; compared with the cyanide method, this method is still a green gold extraction method.

Acknowledgements

This work was financially supported by the Rare and Precious Metals Extraction and Mine Ecological Management Team Foundation(22YNOUTD02).

  1. Author contributions: Zhang Qiang: resources, writing – original draft, writing – review and editing; Duan Jing-ze: project administration and funding acquisition; Peng-Zhi Xiang: methodology and formal analysis.

  2. Conflict of interest: Authors state no conflict of interest.

  3. Data availability statement: The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.

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Received: 2024-04-09
Accepted: 2024-08-26
Published Online: 2024-10-29

© 2024 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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  91. Green synthesis and effective utilization of biogenic Al2O3-nanocoupled fungal lipase in the resolution of active homochiral 2-octanol and its immobilization via aluminium oxide nanoparticles
  92. Eco-friendly RP-HPLC approach for simultaneously estimating the promising combination of pentoxifylline and simvastatin in therapeutic potential for breast cancer: Appraisal of greenness, whiteness, and Box–Behnken design
  93. Use of a humidity adsorbent derived from cockleshell waste in Thai fried fish crackers (Keropok)
  94. One-pot green synthesis, biological evaluation, and in silico study of pyrazole derivatives obtained from chalcones
  95. Bio-sorption of methylene blue and production of biofuel by brown alga Cystoseira sp. collected from Neom region, Kingdom of Saudi Arabia
  96. Synthesis of motexafin gadolinium: A promising radiosensitizer and imaging agent for cancer therapy
  97. The impact of varying sizes of silver nanoparticles on the induction of cellular damage in Klebsiella pneumoniae involving diverse mechanisms
  98. Microwave-assisted green synthesis, characterization, and in vitro antibacterial activity of NiO nanoparticles obtained from lemon peel extract
  99. Rhus microphylla-mediated biosynthesis of copper oxide nanoparticles for enhanced antibacterial and antibiofilm efficacy
  100. Harnessing trichalcogenide–molybdenum(vi) sulfide and molybdenum(vi) oxide within poly(1-amino-2-mercaptobenzene) frameworks as a photocathode for sustainable green hydrogen production from seawater without sacrificial agents
  101. Magnetically recyclable Fe3O4@SiO2 supported phosphonium ionic liquids for efficient and sustainable transformation of CO2 into oxazolidinones
  102. A comparative study of Fagonia arabica fabricated silver sulfide nanoparticles (Ag2S) and silver nanoparticles (AgNPs) with distinct antimicrobial, anticancer, and antioxidant properties
  103. Visible light photocatalytic degradation and biological activities of Aegle marmelos-mediated cerium oxide nanoparticles
  104. Physical intrinsic characteristics of spheroidal particles in coal gasification fine slag
  105. Exploring the effect of tea dust magnetic biochar on agricultural crops grown in polycyclic aromatic hydrocarbon contaminated soil
  106. Crosslinked chitosan-modified ultrafiltration membranes for efficient surface water treatment and enhanced anti-fouling performances
  107. Study on adsorption characteristics of biochars and their modified biochars for removal of organic dyes from aqueous solution
  108. Zein polymer nanocarrier for Ocimum basilicum var. purpurascens extract: Potential biomedical use
  109. Green synthesis, characterization, and in vitro and in vivo biological screening of iron oxide nanoparticles (Fe3O4) generated with hydroalcoholic extract of aerial parts of Euphorbia milii
  110. Novel microwave-based green approach for the synthesis of dual-loaded cyclodextrin nanosponges: Characterization, pharmacodynamics, and pharmacokinetics evaluation
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  112. Green synthesis and characterization of CuO/ZnO nanocomposite using Musa acuminata leaf extract for cytotoxic studies on colorectal cancer cells (HCC2998)
  113. Review Articles
  114. Materials-based drug delivery approaches: Recent advances and future perspectives
  115. A review of thermal treatment for bamboo and its composites
  116. An overview of the role of nanoherbicides in tackling challenges of weed management in wheat: A novel approach
  117. An updated review on carbon nanomaterials: Types, synthesis, functionalization and applications, degradation and toxicity
  118. Special Issue: Emerging green nanomaterials for sustainable waste management and biomedical applications
  119. Green synthesis of silver nanoparticles using mature-pseudostem extracts of Alpinia nigra and their bioactivities
  120. Special Issue: New insights into nanopythotechnology: current trends and future prospects
  121. Green synthesis of FeO nanoparticles from coffee and its application for antibacterial, antifungal, and anti-oxidation activity
  122. Dye degradation activity of biogenically synthesized Cu/Fe/Ag trimetallic nanoparticles
  123. Special Issue: Composites and green composites
  124. Recent trends and advancements in the utilization of green composites and polymeric nanocarriers for enhancing food quality and sustainable processing
  125. Retraction
  126. Retraction of “Biosynthesis and characterization of silver nanoparticles from Cedrela toona leaf extracts: An exploration into their antibacterial, anticancer, and antioxidant potential”
  127. Retraction of “Photocatalytic degradation of organic dyes and biological potentials of biogenic zinc oxide nanoparticles synthesized using the polar extract of Cyperus scariosus R.Br. (Cyperaceae)”
  128. Retraction to “Green synthesis on performance characteristics of a direct injection diesel engine using sandbox seed oil”
https://doi.org/10.1515/gps-2024-0079
Keywords for this article
bromate; thiourea; synergistic leaching; green gold extraction
Creative Commons
BY 4.0

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  102. A comparative study of Fagonia arabica fabricated silver sulfide nanoparticles (Ag2S) and silver nanoparticles (AgNPs) with distinct antimicrobial, anticancer, and antioxidant properties
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  113. Review Articles
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  115. A review of thermal treatment for bamboo and its composites
  116. An overview of the role of nanoherbicides in tackling challenges of weed management in wheat: A novel approach
  117. An updated review on carbon nanomaterials: Types, synthesis, functionalization and applications, degradation and toxicity
  118. Special Issue: Emerging green nanomaterials for sustainable waste management and biomedical applications
  119. Green synthesis of silver nanoparticles using mature-pseudostem extracts of Alpinia nigra and their bioactivities
  120. Special Issue: New insights into nanopythotechnology: current trends and future prospects
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  125. Retraction
  126. Retraction of “Biosynthesis and characterization of silver nanoparticles from Cedrela toona leaf extracts: An exploration into their antibacterial, anticancer, and antioxidant potential”
  127. Retraction of “Photocatalytic degradation of organic dyes and biological potentials of biogenic zinc oxide nanoparticles synthesized using the polar extract of Cyperus scariosus R.Br. (Cyperaceae)”
  128. Retraction to “Green synthesis on performance characteristics of a direct injection diesel engine using sandbox seed oil”
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