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Article

Alkaline Leaching and Concurrent Cementation of Dissolved Pb and Zn from Zinc Plant Leach Residues

1
Department of Metallurgical Engineering, School of Mines, University of Zambia, P.O. Box 32379, Lusaka 10101, Zambia
2
Division of Sustainable Resources Engineering, Graduate School of Engineering, Hokkaido University, Sapporo 060-8628, Japan
3
Division of Sustainable Resources Engineering, Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japan
4
School of Minerals and Energy Resources Engineering, The University of New South Wales, Sydney, NSW 2052, Australia
5
Geology Department, School of Mines, The University of Zambia, P.O. Box 32379, Lusaka 10101, Zambia
6
Faculty of Veterinary Medicine, Hokkaido University, Sapporo 060-0818, Japan
7
School of Veterinary Medicine, The University of Zambia, P.O. Box 32379, Lusaka 10101, Zambia
*
Author to whom correspondence should be addressed.
Minerals 2022, 12(4), 393; https://doi.org/10.3390/min12040393
Submission received: 23 February 2022 / Revised: 14 March 2022 / Accepted: 19 March 2022 / Published: 23 March 2022
(This article belongs to the Special Issue Sustainable Production of Metals for Low-Carbon Technologies)

Abstract

:
Zinc plant leach residues (ZPLRs), particularly those produced using old technologies, have both economic importance as secondary raw materials and have environmental impacts because they contain hazardous heavy metals that pose risks to human health and the environment. Therefore, the extraction and recovery of these metals from ZPLRs has both economic and environmental benefits. In this study, we investigated the removal of lead (Pb) and zinc (Zn) from ZPLRs by alkaline (NaOH) leaching and the concurrent cementation of dissolved Pb and Zn using aluminum (Al) metal powder. The effects of the leaching time, NaOH concentration, solid-to-liquid ratio (S/L), and dosage of Al metal powder on the extraction of Pb and Zn were investigated. Pb and Zn removal efficiencies increased with increasing NaOH concentrations and decreasing S/Ls. The Pb and Zn removal efficiencies were 62.2% and 27.1%, respectively, when 2.5 g/50 mL (S/L) of ZPLRs were leached in a 3 M NaOH solution for 30 min. The extraction of Pb and Zn could be attributed to the partitioning of these metals in relatively more mobile phases—water-soluble, exchangeable, and carbonate phases—in ZPLRs. Around 100% of dissolved Pb and less than 2% of dissolved Zn were cemented in leaching pulp when Al metal powder was added. Minerals in the solid residues, particularly iron oxides minerals, were found to suppress the cementation of extracted Zn in leaching pulp, and when they were removed by filtration, Zn was recovered by Al metal powder via cementation.

1. Introduction

The increase in the global population, the rapid development of cities, and the current push to decarbonize society are all contributing to the unprecedentedly high demand for metals. For example, the renewable energy and clean energy technologies needed to decarbonize society are more metal and material intensive than conventional fossil-fuel-based technologies [1,2,3]. In a recent report by the World Bank, zinc (Zn) and lead (Pb) were two of the 17 materials/metals identified as critical for the clean energy transition to succeed [4]. Unfortunately, high-grade, primary metal resources have become scarce, so alternative sources such as submarine deposits and wastes are currently being explored [5,6].
Zinc plant leach residues (ZPLRs), especially those that were produced using old technologies, are regarded as environmental nuisances and hazardous wastes due to their high amounts of leachable residual hazardous elements such as Pb, Zn, cadmium (Cd), copper (Cu), and arsenic (As) [7,8,9,10]. Lead, Cd, and As can cause various illnesses that affect the central nervous system, skin, lungs and kidneys, even in minute amounts, while Cu and Zn are essential micronutrients that are toxic at high concentrations [11,12,13]. Aside from Zn and Pb, ZPLRs can also contain other critical metals such as cobalt (Co), indium (In), gallium (Ga), and germanium (Ge) [14,15,16]. The extraction of these metals from ZPLRs serves two purposes: (1) exploitation for economic benefits and (2) the detoxification and clean-up of ZPLRs-impacted sites.
Metal extraction from ZPLRs by hydrometallurgical processes is preferred because they are less energy-intensive (especially for low-grade metallurgical wastes such as ZPLRs) compared to their counterpart, pyrometallurgical processes. Most hydrometallurgical techniques involve the use of strong acids to extract metals of interest. Because these acids are nonselective, they dissolve unwanted elements, the majority of which interferes with succeeding recovery processes, so purification processes (e.g., solvent extraction) are required [17,18,19,20].
The leaching of ZPLRs using alkaline lixiviants achieves the selective solubilization of amphoteric elements—Al, Pb, and Zn—leaving iron (Fe), calcium (Ca), and magnesium (Mg) host minerals that constitute a large percentage of ZPLRs undissolved. The dissolution of Pb and Zn under alkaline conditions is due to the formation of complexes with hydroxyl ions (OH) [21]. In weak to moderately strong alkaline solutions (i.e., pH 6–12), Pb and Zn dissolve as Pb(OH)3 with small amounts of Pb(OH)42− and Zn(OH)3 with small amounts of Zn(OH)42−, respectively. In a strong alkaline solution (i.e., pH > 12), the dominant species are Pb(OH)42− for Pb and Zn(OH)42− for Zn. Many researchers have investigated and successfully extracted Pb and Zn from ZPLRs using alkaline solutions [14,22,23,24]. The alkaline extractive processes studied are as follows: leaching → solid–liquid separation → metal recovery stages. However, solid–liquid separation by filtration, especially for strong alkaline, is difficult [25]. Thus, some dissolved Pb and Zn from ZPLRs remain in residues if thorough filtration and the washing of leaching residues are not carried out. The residual metals in produced residues are economic losses and at the same time render the produced residues hazardous.
The authors previously developed concurrent-extraction cementation (CEC)—a new metals recovery technique that extracts metals and captures/sequesters them by cementation before solid–liquid separation. Cementation or reductive precipitation is an electrochemical process whereby zero-valent metals or alloys are used to selectively recover redox-sensitive dissolved metals from solution [26,27]. The CEC technique eliminates the need for thorough filtration and extensive washing to remove residual toxic elements in the leaching residues [28,29]. These previous studies, however, were conducted in acidic solutions and Zn could not be cemented by Al metal powder from the leaching pulp or filtered solution because of the competitive effects of proton reduction on cementation [30]. This study, therefore, investigates the CEC of dissolved Pb and Zn from ZPLRs in alkaline (NaOH) leaching pulp using Al metal powder as the cementation agent.

2. Materials and Methods

2.1. Materials

Zinc plant leach residues (ZPLRs) from a historic Pb-Zn mine dumpsite in Kabwe, Zambia were used in this study. The total amounts of Pb and Zn in the ZPLRs were around 6.19 wt% and 2.53 wt%, respectively. The major crystalline minerals of Pb were anglesite (PbSO4), cerussite (PbCO3), and esperite (PbCa2Zn3(SiO4)3). Meanwhile, only one crystalline mineral for Zn, zinkosite (ZnSO4), was detected. Ultra-pure Al metal powder with a median particle size (D50) of 126.8 µm (>99.99%, +50–150 µm, Wako Pure Chemical Industries, Ltd., Osaka, Japan) was used to cement dissolved Pb and Zn from ZPLRs. Detailed characterizations of Al powder and ZPLRs are reported elsewhere [28,31]. Reagent grade NaOH (Wako Pure Chemical Industries, Ltd., Osaka, Japan) was used to prepare the alkaline leaching solutions of different concentrations by dissolving and diluting in deionized (DI) water (18 MΩ·cm, Milli-Q® Integral Water Purification System, Merck Millipore, Burlington, VT, USA).

2.2. Methods

All batch experiments were done using 200-mL Erlenmeyer flasks, and the volume of leaching solutions of different concentrations (i.e., 0–6 M) was fixed at 50 mL. A leaching solution of known volume was added in a flask before the addition of ZPLRs to obtain a predetermined solid-to-liquid ratio (S/L). In the case of CEC experiments, 0.25 g of Al powder was added together with ZPLRs. The pulp was then shaken in a temperature-controlled water bath shaker maintained at 25 °C at a shaking speed of 120 strokes/min and a shaking amplitude of 40 mm. After shaking for preplanned durations, the pulp was carefully collected and filtered through 0.20 µm syringe-driven membrane filters. The filtrate was analyzed for Pb and Zn using an inductively-coupled plasma-atomic emission spectrometer (ICP-AES) (ICPE-9820, Shimadzu Corporation, Kyoto, Japan) (margin of error = ±2%). For the CEC experiments, one more step was added to remove cemented and agglomerated Pb and Zn by sieving using a stainless-steel sieve with an aperture size of 150 µm. The cementation products (i.e., +150 µm) were dried in a vacuum oven, digested by aqua regia in a microwave-assisted acid digestion system (Ethos Advanced Microwave Lab station, Milestone Inc., Sorisole, Italy), and the leachates were analyzed for Pb, Zn, and Fe by ICP-AES. Additionally, the cementation products were analyzed by a scanning electron microscope with an energy-dispersive X-ray spectrometer (SEM-EDX) (JSM-IT200, JEOL Ltd., Tokyo, Japan).
To calculate the Pb and Zn removal efficiencies ( η M e ) from ZPLRs with and without the addition of Al powder, Equations (1) and (2), respectively, were used.
η M e = ( V   ×   C M e ) + ( W c m e ×   M c m e ) W S     ×     M s   ×     100
η M e = V   ×   C M e W S     ×     M s ×   100
where C M e is the concentration (g/L) of Pb and Zn, V is the volume (L) of the leaching solution, W S is the weight % of either Pb and Zn in ZPLRs, M s is the mass (g) of the leached ZPLRs, M c m e is the mass (g) of cemented and agglomerated particles, and W c m e is the weight % of Pb and Zn in cemented and agglomerated particles calculated based on the digested fraction of M c m e in aqua regia and analysis of the solution by ICP-AES.

3. Results and Discussions

3.1. Leaching of ZPLRs in NaOH without the Addition of Al Powder

The effects of leaching time, NaOH concentration, and S/L on Pb and Zn removal efficiencies from ZPLRs were investigated by batch leaching experiments without the addition of Al powder.
The leaching duration effects on Pb and Zn removal was investigated using 3 M NaOH, a 2.5 g/50 mL S/L ratio, and a temperature of 25 °C. The results show that the removal efficiencies for Pb and Zn increased with time up to 15 min, beyond which they changed only insignificantly (Figure 1a). At 15 min of leaching time, the Pb removal efficiency was 60.4% and remained the same even when the leaching time was increased to 120 min (i.e., 59.6%). Similarly, the removal efficiency for Zn was around 28% for 15 min of leaching and 25% when the leaching time was prolonged to 120 min. The Pb and Zn removal efficiencies corroborated and correlated with the water-soluble, exchangeable, and carbonate phases of Pb and Zn approximated by sequential extraction (experimental method and detailed discussion reported by the authors elsewhere [31]) (Figure 2). It is thermodynamically difficult to dissolve Pb and Zn bound to relatively stable phases (e.g., Fe/Mn oxyhydroxide, Fe oxide, and sulfides/organic) in NaOH leaching solution [32,33].
To investigate the effects of the NaOH concentration on Pb and Zn removal efficiencies, NaOH in solution was varied from 0 to 6 M, the S/L maintained at 2.5 g/50 mL, and the temperature was maintained at 25 °C for 30 min of leaching time. The removal efficiencies of Pb and Zn increased with higher NaOH concentrations up to 3 M (i.e., Pb and Zn removal of around 60% and 25%), after which, the change in the removal efficiencies of Pb and Zn became insignificant (Figure 1b). The reactions between Pb- and Zn-hosting minerals and NaOH in the solution can be described by Equations (3)–(6) [22,32].
PbSO 4 + 3 NaOH     Pb ( OH ) 3 +   SO 4 2 + 3 Na +
2 PbO + 2 NaOH +   H 2 O     2 Pb ( OH ) 3 + 2 Na +
ZnSO 4 + 3 NaOH     Zn ( OH ) 3 +   SO 4 2 + 3 Na +
2 ZnO + 2 NaOH +   H 2 O     2 Zn ( OH ) 3 + 2 Na +
In weak to moderately strong alkaline solutions (pH 6–12), the dominant species for Pb and Zn are Pb ( OH ) 3 and Zn ( OH ) 3 . When the NaOH concentration increases (strong alkaline solution, pH > 12) the equilibrium shifts and the more soluble Pb and Zn hydroxyl complexes Pb ( OH ) 4 2 and Zn ( OH ) 4 2 , respectively, become more dominant [21]. This explains why Pb and Zn removal efficiencies increased at higher concentrations of NaOH (i.e., 3 M NaOH). Increasing the NaOH concentration beyond 3 M did not improve the Pb and Zn removal efficiencies because almost all the easily extractable Pb and Zn (as determined by sequential extraction) from the ZPLRs were already exhausted.
The S/L is another parameter that affects Pb and Zn removal efficiencies from ZPLRs due to changes in the ratio of hydroxyl concertation to Pb and Zn. To investigate the effects of the S/L ratio on Pb and Zn removal efficiencies, leaching experiments were carried out by varying the amounts of ZPLRs (i.e., 1–10 g) added in 50 mL of 3 M NaOH solution and shaking for 30 min in the water bath at 25 °C. The results show that Pb and Zn removal efficiencies decrease with increasing amounts of ZPLRs in a 50 mL of 3 M NaOH (Figure 1c). The Pb removal efficiency decreased from 62.5% for 1 g to 22.7% for 10 g of ZPLRs. Similarly, the Zn removal efficiency was negatively affected by the S/L. The Zn removal efficiency decreased from 27.1% for 1 g to 13.3% for 10 g of ZPLRs. This decrease in Pb and Zn removal efficiencies with an increase in the S/L can be attributed to the limited hydroxyl ions available to extract Pb and Zn [34], as highlighted above.

3.2. Concurrent Cementation of Dissolved Pb and Zn in Leaching Pulp of ZPLRs

The concurrent cementation of dissolved Pb and Zn in leaching pulp was conducted using Al metal powder. Al is not only environmentally friendly as a cementation agent, but it also has a very low standard electrode potential (i.e., −2.35 V vs. NHE in basic solution), which makes it a thermodynamically good candidate for the cementation of dissolved Pb and Zn [35,36,37]. The oxide layer (Al2O3) which covers and insulates Al and suppresses the transfer of electrons dissolves at a high pH [30,38]. As previously discussed, Pb and Zn oxides equally dissolve and are complexed with hydroxide, as shown in Figure 3.

3.2.1. Effects of Time and NaOH Concentration on Cementation and Distribution of Pb in Leaching Pulp

When 0.25 g of Al powder was added during the leaching of ZPLRs in 3 M NaOH solution, the overall chemical reaction that was thermodynamically expected is expressed by Equation (9), and the net reaction of anodic and cathodic half-reactions are expressed by Equations (7) and (8).
Al + 4 OH     Al ( OH ) 4 + 3 e 2.35   V
Pb + 4 OH   Pb ( OH ) 4 2 + 2 e 0.54   V
2 Al + 3 Pb ( OH ) 4 2   2 Al ( OH ) 4 + 4 OH + 3 Pb
Equation (9) is the cementation reaction of dissolved Pb by added Al powder. The standard Gibbs free energy change, Δ G 0 (i.e., Δ G 0 = n F Δ E 0 , n is number of electrons transferred, F is Faraday’s constant, and Δ E 0   (   E Al Al ( OH ) 4 0 E Pb Pb ( OH ) 4 2 0 )   is the galvanic cell potential of Equation (9)), is −1047.82 kJ/mol, implying that cementation of dissolved Pb2+ from ZPLRs by Al powder is thermodynamically feasible. The distribution of Pb among the cementation product, solution (i.e., dissolved Pb but uncemented), and undissolved Pb from ZPLRs for different leaching times and NaOH concentrations are shown in Figure 4. Figure 4a shows that the amount of dissolved but uncemented Pb decreased with an increase in leaching time of up to 30 min, where almost 100% of the dissolved Pb was cemented by Al metal powder. This entails that dissolved Pb from ZPLRs was cemented as described in the chemical reaction represented by Equation (9). However, a leaching period longer than 30 min led to an increase in the Pb remaining in the solution. This trend could be attributed to the redissolution of cemented Pb after all the Al has been dissolved and consumed by cementation and other side reactions.
The effects of the NaOH concentration on the Pb distribution for concurrent cementation of dissolved Pb at 30 min of leaching time is shown in Figure 4b. As expected, the amount of Pb dissolved from ZPLRs and cemented by 0.25 g of Al powder increased with the increase in the NaOH concentration. The cemented Pb increased from 27% for 1 M NaOH to 66.1% for 6 M NaOH, with no dissolved Pb remaining in the solution.

3.2.2. Effects of Time and NaOH Concentration on Cementation and Distribution of Zn in Leaching Pulp

The half-reactions represented by Equations (10) and (11) that add up to the overall chemical reaction depicted in Equation (12) were thermodynamically expected when 0.25 g of Al powder was added during the leaching of ZPLRs in 3 M NaOH solution.
Al + 4 OH     Al ( OH ) 4 + 3 e 2.35   V
Pb + 4 OH   Pb ( OH ) 4 2 + 2 e 1.285   V
2 Al + 3 Zn ( OH ) 4 2   2 Al ( OH ) 4 + 4 OH + 3 Zn
Equation (12) is the cementation reaction of dissolved Zn as ZnOH)42− from ZPLRs is cemented by Al whose standard Gibbs free energy change, G 0 (i.e., Δ G 0 = n F Δ E 0 , n is number of electrons transferred, F is Faraday’s constant, and Δ E 0   ( E Al Al ( OH ) 4 0 E Zn Zn ( OH ) 4 2 0 )   is the galvanic cell potential of Equation (9)), is −616.57 kJ/mol. This means that the cementation of dissolved Zn2+ from ZPLRs by Al powder is thermodynamically favorable. However, the results show that little Zn was cemented by Al metal powder from 7.5 up to 120 min using various NaOH concentrations because most of the dissolved Zn remained in solution (Figure 5a,b). This could mean that there were some counter-reactions to the cementation reaction. These reactions could arise from co-dissolved elements in the leachate and/or solid residues.
When the cementation product was analyzed by SEM-EDX, it was shown that both Pb and Zn were cemented but the intensity for Zn was much lower than Pb (Figure 6).
To investigate the effects of co-dissolved elements and solid residues on the cementation of dissolved Zn from leaching solution using Al metal powder, simulated (model) 3 M NaOH solutions containing both 8 mM Pb2+ and 10 mM Zn2+ and filtrate (to eliminate solid residues interference) after the initial addition of Al powder during ZPLR leaching, respectively, were used. The model solution was prepared by dissolving ZnCl2 and PbCl2 (Wako Pure Chemical Industries, Ltd., Osaka, Japan) in 3 M NaOH. For the model solution, 0.15 g of Al metal powder was added to cement both Pb and Zn. For the filtrate after the concurrent cementation of dissolved Pb and Zn experiments, 0.1 g of Al metal powder was added to the cement residual Zn in the presence of other co-dissolved elements from ZPLRs. Figure 7a shows that 100% of Pb and 100% of Zn in the model solution were cemented out of the solution by Al metal powder. This confirms the thermodynamic feasibility discussed above and that Al metal powder can cement Zn. Likewise, the dissolved Zn in the filtrate after the concurrent cementation experiment was recovered (around 96.9%) by the second portion of Al metal powder added in the filtrate (Figure 7b). This implies that the co-dissolved elements from ZPLRs and from cementation experiments do not affect the cementation of Zn in NaOH solution. The results, however, highlight that solid residue could possibly interfere with and suppress the cementation of Zn during the concurrent cementation of dissolved Pb and Zn experiments.
To investigate the effects of minerals in the solid residues from ZPLRs that could affect the cementation of dissolved Zn from leaching pulp using Al metal powder, 2.5 g (to maintain the same S/L ratio) of the three most abundant minerals in the ZPLRs we used. This included SiO2 (quartz), Fe2O3 (hematite), and Fe3O4 (magnetite), and each mineral was added in a model solution of 3 M NaOH solutions containing both 8 mM Pb2+ and 10 mM Zn2+. To mimic the ZPLR concurrent cementation experiments, 0.25 g of Al metal powder was added to the solution and shaken for 30 min in a temperature-controlled bash shaker. For all of the three solid residues, around 98% of Pb was cemented by Al metal powder (Figure 8). However, Zn cementation was slightly reduced by SiO2 (93%) and significantly suppressed by Fe2O3 (28.5%) and Fe3O4 (27.9%). The slight decrease in cementation in the case of Zn in 2.5 g could be ascribed to dissolved silicate anions that exhibit the properties of nanoparticles suspension (colloid) hence affecting viscosity and the transportation of metal ions on the surface of the Al metal and cementation Al ions away from the surface of Al metals [40]. Meanwhile, the significant suppression by Fe2O3 and Fe3O4 could be attributed to preferential consumption of electrons from Al metal powder to reduce Fe3+ to Fe2+ (i.e., Fe(OH)3 to Fe(OH)2), whose standard electrode potential in basic solution is around −0.54 V. This deduction is also supported by other works highlighting the participation of Fe2O3 and Fe3O4 in electrochemical reactions such as pyrite dissolution, arsenite oxidation to arsenate, and the recovery of gold ions from chloride solutions [41,42]
The concurrent cementation of both dissolved Pb and Zn can be applied for the remediation of Pb-Zn mine waste materials or Pb-Zn contaminated soil that do not contain a substantial amount of iron oxide. The most toxic metal, Pb, can be cemented in pulp with less suppression by Fe oxides. Meanwhile, the dissolved Zn can be recovered after filtration by either cementation using Al or precipitation as ZnS [21].

4. Conclusions

This study investigated Pb and Zn removal from ZPLRs in alkaline solution by the concurrent cementation of dissolved Pb and Zn in leaching pulp. The findings are summarized as below:
(1)
Pb and Zn removal efficiencies were affected by the leaching time, the NaOH concentration, and the S/L ratio. The Pb and Zn removal efficiencies were 62.2% and 27.1%, respectively, when 2.5 g/50 mL (S/L) of ZPLRs were leached in a 3 M NaOH solution for 30 min.
(2)
The amounts Pb (62.2%) and Zn (27.1%) that were removed from ZPLRs using NaOH solution correlated and corroborated with the mobile phase fraction (i.e., Pb and Zn bound to water, exchangeable, and carbonates) approximated by sequential extraction.
(3)
Around 100% of the dissolved Pb was cemented by Al metal powder for the concurrent cementation of dissolved Pb in the leaching pulp.
(4)
The dissolved Zn was not cemented out in leaching pulp by the addition of Al metal powder. However, around 96.9% was cemented by Al after filtration. The suppression of cementation by Al metal was attributed to solid residues, in particular Fe oxides.
(5)
The concurrent cementation of both dissolved Pb and Zn in alkaline leaching pulp has the potential to be applied for the remediation of Pb-Zn mine wastes or Pb-Zn contaminated soil, provided they contain minimal amounts of iron oxides, which were found to suppress Zn cementation.

Author Contributions

Conceptualization, M.S.; methodology, M.S., T.F. and R.H.; formal analysis, M.S., M.I. (Mayumi Ito), N.H., S.J., I.P. and C.B.T.; investigation, M.S.; writing—original draft preparation, M.S.; writing—review and editing, M.S., M.I. (Mayumi Ito), N.H., C.B.T., S.J., I.P., I.N., T.S. and T.I.; supervision, M.I. (Mayumi Ito) and N.H.; project administration, M.I. (Mayumi Ishizuka), S.N. and H.N.; funding acquisition, M.I. (Mayumi Ishizuka)., S.N. and H.N. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported partly by the Japan Society for the Promotion of Science (JSPS) CORE to CORE program (M.I. (Mayumi Ishizuka)), Hokkaido University SOUSEI-TOKUTEI Specific Research Projects (M.I. (Mayumi Ishizuka)), JSPS Bilateral Open Partnership Joint Research Projects (grant number: JPJSBP120209902) (S.N.), The Japan Prize Foundation (S.N.), and Grants-in-Aid for Scientific Research from the Ministry of Education, and Culture, Sports, Science and Technology of Japan (grant number 20K20633) (S.N.).

Data Availability Statement

Data is available on request because of the restrictions, as the research is ongoing.

Conflicts of Interest

The authors declare no conflict of interest.

References

  1. Dahan, A.M.E.; Alorro, R.D.; Pacaña, M.L.C.; Baute, R.M.; Silva, L.C.; Tabelin, C.B.; Resabal, V.J.T. Hydrochloric Acid Leaching of Philippine Coal Fly Ash: Investigation and Optimisation of Leaching Parameters by Response Surface Methodology (RSM). Sustain. Chem. 2022, 3, 76–90. [Google Scholar] [CrossRef]
  2. Park, I.; Kanazawa, Y.; Sato, N.; Galtchandmani, P.; Jha, M.K.; Tabelin, C.B.; Jeon, S.; Ito, M.; Hiroyoshi, N. Beneficiation of Low-Grade Rare Earth Ore from Khalzan Buregtei Deposit (Mongolia) by Magnetic Separation. Minerals 2021, 11, 1432. [Google Scholar] [CrossRef]
  3. Tabelin, C.B.; Park, I.; Phengsaart, T.; Jeon, S.; Villacorte-Tabelin, M.; Alonzo, D.; Yoo, K.; Ito, M.; Hiroyoshi, N. Copper and Critical Metals Production from Porphyry Ores and E-Wastes: A Review of Resource Availability, Processing/Recycling Challenges, Socio-Environmental Aspects, and Sustainability Issues. Resour. Conserv. Recycl. 2021, 170, 105610. [Google Scholar] [CrossRef]
  4. Hund, K.; La Porta, D.; Fabregas, T.P.; Laing, T.; Drexhage, J. World Bank Minerals for Climate Action—The Mineral Intensity of the Clean Energy Transition 2020; World Bank Publications: Washington, DC, USA, 2020. [Google Scholar]
  5. Tabelin, C.B.; Dallas, J.; Casanova, S.; Pelech, T.; Bournival, G.; Saydam, S.; Canbulat, I. Towards a Low-Carbon Society: A Review of Lithium Resource Availability, Challenges and Innovations in Mining, Extraction and Recycling, and Future Perspectives. Miner. Eng. 2021, 163, 106743. [Google Scholar] [CrossRef]
  6. Aikawa, K.; Ito, M.; Segawa, T.; Jeon, S.; Park, I.; Tabelin, C.B.; Hiroyoshi, N. Depression of Lead-Activated Sphalerite by Pyrite via Galvanic Interactions: Implications to the Selective Flotation of Complex Sulfide Ores. Miner. Eng. 2020, 152, 106367. [Google Scholar] [CrossRef]
  7. Mufalo, W.; Tangviroon, P.; Igarashi, T.; Ito, M.; Sato, T.; Chirwa, M.; Nyambe, I.; Nakata, H.; Nakayama, S.; Ishizuka, M. Solid-Phase Partitioning and Leaching Behavior of Pb and Zn from Playground Soils in Kabwe, Zambia. Toxics 2021, 9, 248. [Google Scholar] [CrossRef]
  8. Behnajady, B.; Moghaddam, J. Selective Leaching of Zinc from Hazardous As-Bearing Zinc Plant Purification Filter Cake. Chem. Eng. Res. Des. 2017, 117, 564–574. [Google Scholar] [CrossRef]
  9. Tabelin, C.B.; Silwamba, M.; Paglinawan, F.C.; Mondejar, A.J.S.; Duc, H.G.; Resabal, V.J.; Opiso, E.M.; Igarashi, T.; Tomiyama, S.; Ito, M.; et al. Solid-Phase Partitioning and Release-Retention Mechanisms of Copper, Lead, Zinc and Arsenic in Soils Impacted by Artisanal and Small-Scale Gold Mining (ASGM) Activities. Chemosphere 2020, 260, 127574. [Google Scholar] [CrossRef]
  10. Abo Atia, T.; Spooren, J. Microwave Assisted Chloride Leaching of Zinc Plant Residues. J. Hazard. Mater. 2020, 398, 122814. [Google Scholar] [CrossRef]
  11. Ho, G.D.; Tabelin, C.B.; Tangviroon, P.; Tamamura, S.; Igarashi, T. Effects of Cement Addition on Arsenic Leaching from Soils Excavated from Projects Employing Shield-Tunneling Method. Geoderma 2021, 385, 114896. [Google Scholar] [CrossRef]
  12. Igarashi, T.; Herrera, P.S.; Uchiyama, H.; Miyamae, H.; Iyatomi, N.; Hashimoto, K.; Tabelin, C.B. The Two-Step Neutralization Ferrite-Formation Process for Sustainable Acid Mine Drainage Treatment: Removal of Copper, Zinc and Arsenic, and the Influence of Coexisting Ions on Ferritization. Sci. Total Environ. 2020, 715, 136877. [Google Scholar] [CrossRef]
  13. Tabelin, C.B.; Igarashi, T.; Villacorte-Tabelin, M.; Park, I.; Opiso, E.M.; Ito, M.; Hiroyoshi, N. Arsenic, Selenium, Boron, Lead, Cadmium, Copper, and Zinc in Naturally Contaminated Rocks: A Review of Their Sources, Modes of Enrichment, Mechanisms of Release, and Mitigation Strategies. Sci. Total Environ. 2018, 645, 1522–1553. [Google Scholar] [CrossRef] [PubMed]
  14. Rao, S.; Wang, D.; Liu, Z.; Zhang, K.; Cao, H.; Tao, J. Selective Extraction of Zinc, Gallium, and Germanium from Zinc Refinery Residue Using Two Stage Acid and Alkaline Leaching. Hydrometallurgy 2019, 183, 38–44. [Google Scholar] [CrossRef]
  15. Fattahi, A.; Rashchi, F.; Abkhoshk, E. Reductive Leaching of Zinc, Cobalt and Manganese from Zinc Plant Residue. Hydrometallurgy 2016, 161, 185–192. [Google Scholar] [CrossRef]
  16. Koleini, S.M.J.; Mehrpouya, H.; Saberyan, K.; Abdolahi, M. Extraction of Indium from Zinc Plant Residues. Miner. Eng. 2010, 23, 51–53. [Google Scholar] [CrossRef]
  17. Jeon, S.; Tabelin, C.B.; Takahashi, H.; Park, I.; Ito, M.; Hiroyoshi, N. Interference of Coexisting Copper and Aluminum on the Ammonium Thiosulfate Leaching of Gold from Printed Circuit Boards of Waste Mobile Phones. Waste Manag. 2018, 81, 148–156. [Google Scholar] [CrossRef]
  18. Jeon, S.; Tabelin, C.B.; Park, I.; Nagata, Y.; Ito, M.; Hiroyoshi, N. Ammonium Thiosulfate Extraction of Gold from Printed Circuit Boards (PCBs) of End-of-Life Mobile Phones and Its Recovery from Pregnant Leach Solution by Cementation. Hydrometallurgy 2020, 191, 105214. [Google Scholar] [CrossRef]
  19. Choi, S.; Yoo, K.; Alorro, R.D.; Tabelin, C.B. Cementation of Co Ion in Leach Solution Using Zn Powder Followed by Magnetic Separation of Cementation-Precipitate for Recovery of Unreacted Zn Powder. Miner. Eng. 2020, 145, 106061. [Google Scholar] [CrossRef]
  20. Phengsaart, T.; Ito, M.; Hamaya, N.; Tabelin, C.B.; Hiroyoshi, N. Improvement of Jig Efficiency by Shape Separation, and a Novel Method to Estimate the Separation Efficiency of Metal Wires in Crushed Electronic Wastes Using Bending Behavior and “Entanglement Factor”. Miner. Eng. 2018, 129, 54–62. [Google Scholar] [CrossRef]
  21. Liu, Q.; Zhao, Y.; Zhao, G. Production of Zinc and Lead Concentrates from Lean Oxidized Zinc Ores by Alkaline Leaching Followed by Two-Step Precipitation Using Sulfides. Hydrometallurgy 2011, 110, 79–84. [Google Scholar] [CrossRef]
  22. Şahin, M.; Erdem, M. Cleaning of High Lead-Bearing Zinc Leaching Residue by Recovery of Lead with Alkaline Leaching. Hydrometallurgy 2015, 153, 170–178. [Google Scholar] [CrossRef]
  23. Huang, Y.; Geng, Y.; Han, G.; Cao, Y.; Peng, W.; Zhu, X.; Zhang, T.; Dou, Z. A Perspective of Stepwise Utilization of Hazardous Zinc Plant Purification Residue Based on Selective Alkaline Leaching of Zinc. J. Hazard. Mater. 2020, 389, 122090. [Google Scholar] [CrossRef] [PubMed]
  24. Seyed Ghasemi, S.M.; Azizi, A. Alkaline Leaching of Lead and Zinc by Sodium Hydroxide: Kinetics Modeling. J. Mater. Res. Technol. 2018, 7, 118–125. [Google Scholar] [CrossRef]
  25. Zhang, Y.; Feng, X.; Qian, L.; Luan, J.; Jin, B. Separation of Arsenic and Extraction of Zinc and Copper from High-Arsenic Copper Smelting Dusts by Alkali Leaching Followed by Sulfuric Acid Leaching. J. Environ. Chem. Eng. 2021, 9, 105997. [Google Scholar] [CrossRef]
  26. Jeon, S.; Bright, S.; Park, I.; Tabelin, C.B.; Ito, M.; Hiroyoshi, N. The Effects of Coexisting Copper, Iron, Cobalt, Nickel, and Zinc Ions on Gold Recovery by Enhanced Cementation via Galvanic Interactions between Zero-Valent Aluminum and Activated Carbon in Ammonium Thiosulfate Systems. Metals 2021, 11, 1352. [Google Scholar] [CrossRef]
  27. Jeon, S.; Bright, S.; Park, I.; Tabelin, C.B.; Ito, M.; Hiroyoshi, N. A Simple and Efficient Recovery Technique for Gold Ions from Ammonium Thiosulfate Medium by Galvanic Interactions of Zero-Valent Aluminum and Activated Carbon: A Parametric and Mechanistic Study of Cementation. Hydrometallurgy 2022, 208, 105815. [Google Scholar] [CrossRef]
  28. Silwamba, M.; Ito, M.; Hiroyoshi, N.; Tabelin, C.B.; Hashizume, R.; Fukushima, T.; Park, I.; Jeon, S.; Igarashi, T.; Sato, T.; et al. Recovery of Lead and Zinc from Zinc Plant Leach Residues by Concurrent Dissolution-Cementation Using Zero-Valent Aluminum in Chloride Medium. Metals 2020, 10, 531. [Google Scholar] [CrossRef] [Green Version]
  29. Silwamba, M.; Ito, M.; Tabelin, C.B.; Park, I.; Jeon, S.; Takada, M.; Kubo, Y.; Hokari, N.; Tsunekawa, M.; Hiroyoshi, N. Simultaneous Extraction and Recovery of Lead Using Citrate and Micro-Scale Zero-Valent Iron for Decontamination of Polluted Shooting Range Soils. Environ. Adv. 2021, 5, 100115. [Google Scholar] [CrossRef]
  30. Choi, S.; Jeon, S.; Park, I.; Ito, M.; Hiroyoshi, N. Addition of Fe3O4 as Electron Mediator for Enhanced Cementation of Cd2+ and Zn2+ on Aluminum Powder from Sulfate Solutions and Magnetic Separation to Concentrate Cemented Metals from Cementation Products. J. Environ. Chem. Eng. 2021, 9, 106699. [Google Scholar] [CrossRef]
  31. Silwamba, M.; Ito, M.; Hiroyoshi, N.; Tabelin, C.B.; Fukushima, T.; Park, I.; Jeon, S.; Igarashi, T.; Sato, T.; Nyambe, I. Detoxification of Lead-Bearing Zinc Plant Leach Residues from Kabwe, Zambia by Coupled Extraction-Cementation Method. J. Environ. Chem. Eng. 2020, 8, 104197. [Google Scholar] [CrossRef]
  32. Orhan, G. Leaching and Cementation of Heavy Metals from Electric Arc Furnace Dust in Alkaline Medium. Hydrometallurgy 2005, 78, 236–245. [Google Scholar] [CrossRef]
  33. Dutra, A.J.B.; Paiva, P.R.P.; Tavares, L.M. Alkaline Leaching of Zinc from Electric Arc Furnace Steel Dust. Miner. Eng. 2006, 19, 478–485. [Google Scholar] [CrossRef]
  34. Zhang, Y.; Deng, J.; Chen, J.; Yu, R.; Xing, X. Leaching of Zinc from Calcined Smithsonite Using Sodium Hydroxide. Hydrometallurgy 2013, 131–132, 89–92. [Google Scholar] [CrossRef]
  35. Tabelin, C.B.; Resabal, V.J.T.; Park, I.; Villanueva, M.G.B.; Choi, S.; Ebio, R.; Cabural, P.J.; Villacorte-Tabelin, M.; Orbecido, A.; Alorro, R.D.; et al. Repurposing of Aluminum Scrap into Magnetic Al0/ZVI Bimetallic Materials: Two-Stage Mechanical-Chemical Synthesis and Characterization of Products. J. Clean. Prod. 2021, 317, 128285. [Google Scholar] [CrossRef]
  36. Seng, S.; Tabelin, C.B.; Kojima, M.; Hiroyoshi, N.; Ito, M. Galvanic Microencapsulation (GME) Using Zero-Valent Aluminum and Zero-Valent Iron to Suppress Pyrite Oxidation. Mater. Trans. 2019, 60, 277–286. [Google Scholar] [CrossRef] [Green Version]
  37. Jeon, S.; Tabelin, C.B.; Takahashi, H.; Park, I.; Ito, M.; Hiroyoshi, N. Enhanced Cementation of Gold via Galvanic Interactions Using Activated Carbon and Zero-Valent Aluminum: A Novel Approach to Recover Gold Ions from Ammonium Thiosulfate Medium. Hydrometallurgy 2020, 191, 105165. [Google Scholar] [CrossRef]
  38. Djokić, S.S. Cementation of Copper on Aluminum in Alkaline Solutions. J. Electrochem. Soc. 1996, 143, 1300. [Google Scholar] [CrossRef]
  39. Bethke, C.M. The Geochemist’s Workbench—A User’s Guide to Rxn, Act2, Tact, React, and Gtplot; University of Illinois: Urbana, IL, USA, 2002. [Google Scholar]
  40. Yang, X.; Zhu, W.; Yang, Q. The Viscosity Properties of Sodium Silicate Solutions. J. Solut. Chem. 2008, 37, 73–83. [Google Scholar] [CrossRef]
  41. Calderon, A.R.M.; Alorro, R.D.; Tadesse, B.; Yoo, K.; Tabelin, C.B. Evaluation of Maghemite-Rich Iron Oxide Composite Prepared from Magnetite as Adsorbent for Gold from Chloride Solution. JOM 2019, 71, 4639–4646. [Google Scholar] [CrossRef]
  42. Tabelin, C.B.; Corpuz, R.D.; Igarashi, T.; Villacorte-Tabelin, M.; Ito, M.; Hiroyoshi, N. Hematite-Catalysed Scorodite Formation as a Novel Arsenic Immobilisation Strategy under Ambient Conditions. Chemosphere 2019, 233, 946–953. [Google Scholar] [CrossRef]
Figure 1. Pb and Zn removal efficiencies from ZPLRs: (a) Effects of leaching time when 2.5 g ZPLRs was leached in 50 mL of concentration 3 M NaOH and shaken at 120 strokes per minute in the water bath at 25 °C; (b) effects of NaOH concentration when 2.5 g ZPLRs was leached in 50 mL of different NaOH concentration and shaken at 120 strokes per minute in the water bath at 25 °C; and (c) effects of S/L ratio when various amounts ZPLRs were leached in 50 mL of 3M NaOH concentration and shaken at 120 strokes per minute in the water bath at 25 °C.
Figure 1. Pb and Zn removal efficiencies from ZPLRs: (a) Effects of leaching time when 2.5 g ZPLRs was leached in 50 mL of concentration 3 M NaOH and shaken at 120 strokes per minute in the water bath at 25 °C; (b) effects of NaOH concentration when 2.5 g ZPLRs was leached in 50 mL of different NaOH concentration and shaken at 120 strokes per minute in the water bath at 25 °C; and (c) effects of S/L ratio when various amounts ZPLRs were leached in 50 mL of 3M NaOH concentration and shaken at 120 strokes per minute in the water bath at 25 °C.
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Figure 2. Phase partitioning by sequential extraction of Pb and Zn for ZPLRs (reprinted with permission from Silwamba et al., [31] copyright (2020) Elsevier) (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 2. Phase partitioning by sequential extraction of Pb and Zn for ZPLRs (reprinted with permission from Silwamba et al., [31] copyright (2020) Elsevier) (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 3. Log activity-pH predominant diagram for (a) 0.1 mM Al3+ and 0.1 mM SO42−, (b) 0.1 mM Zn2+ and 0.1 mM SO42−, and (c) 0.1 mM Pb2+ and 0.1 mM SO42− at 25 °C and 1.013 bar created using the Geochemist’s Workbench® with MINTEQ database [39] (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 3. Log activity-pH predominant diagram for (a) 0.1 mM Al3+ and 0.1 mM SO42−, (b) 0.1 mM Zn2+ and 0.1 mM SO42−, and (c) 0.1 mM Pb2+ and 0.1 mM SO42− at 25 °C and 1.013 bar created using the Geochemist’s Workbench® with MINTEQ database [39] (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 4. Effects of (a) leaching time and (b) NaOH concentration on cementation and distribution of Pb in leaching pulp when Al powder was added during ZPLR leaching (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 4. Effects of (a) leaching time and (b) NaOH concentration on cementation and distribution of Pb in leaching pulp when Al powder was added during ZPLR leaching (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 5. Effects of (a) leaching time and (b) NaOH concentration on cementation and distribution of Zn in leaching pulp when Al powder was added during ZPLR leaching (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 5. Effects of (a) leaching time and (b) NaOH concentration on cementation and distribution of Zn in leaching pulp when Al powder was added during ZPLR leaching (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 6. SEM-EDX of cementation product when 2.5 g ZPLRs were leached in 3 M NaOH solution for 30 min with the addition of 0.25 g Al powder: (a) SEM microphotography, (b) EDX map of Pb, (c) EDX map of Zn, and (d) EDX map of Al (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 6. SEM-EDX of cementation product when 2.5 g ZPLRs were leached in 3 M NaOH solution for 30 min with the addition of 0.25 g Al powder: (a) SEM microphotography, (b) EDX map of Pb, (c) EDX map of Zn, and (d) EDX map of Al (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 7. Amounts of Pb and Zn cemented out from (a) 3 M NaOH model solution containing Pb and Zn ions and treated for 15 and 30 min, and (b) concurrent cementation of dissolved Pb and Zn ions and cementation of Zn in the filtrate solution after concurrent cementation experiment (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 7. Amounts of Pb and Zn cemented out from (a) 3 M NaOH model solution containing Pb and Zn ions and treated for 15 and 30 min, and (b) concurrent cementation of dissolved Pb and Zn ions and cementation of Zn in the filtrate solution after concurrent cementation experiment (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Figure 8. Effects of SiO2, Fe2O3, and Fe3O4 on cementation of Pb and Zn when 2.5 of a given mineral was mixed in 3 M NaOH solution containing 8 mM of Pb2+ and Zn2+ for 30 min (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
Figure 8. Effects of SiO2, Fe2O3, and Fe3O4 on cementation of Pb and Zn when 2.5 of a given mineral was mixed in 3 M NaOH solution containing 8 mM of Pb2+ and Zn2+ for 30 min (for interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).
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Silwamba, M.; Ito, M.; Hiroyoshi, N.; Tabelin, C.B.; Hashizume, R.; Fukushima, T.; Park, I.; Jeon, S.; Igarashi, T.; Sato, T.; et al. Alkaline Leaching and Concurrent Cementation of Dissolved Pb and Zn from Zinc Plant Leach Residues. Minerals 2022, 12, 393. https://doi.org/10.3390/min12040393

AMA Style

Silwamba M, Ito M, Hiroyoshi N, Tabelin CB, Hashizume R, Fukushima T, Park I, Jeon S, Igarashi T, Sato T, et al. Alkaline Leaching and Concurrent Cementation of Dissolved Pb and Zn from Zinc Plant Leach Residues. Minerals. 2022; 12(4):393. https://doi.org/10.3390/min12040393

Chicago/Turabian Style

Silwamba, Marthias, Mayumi Ito, Naoki Hiroyoshi, Carlito Baltazar Tabelin, Ryota Hashizume, Tomoki Fukushima, Ilhwan Park, Sanghee Jeon, Toshifumi Igarashi, Tsutomu Sato, and et al. 2022. "Alkaline Leaching and Concurrent Cementation of Dissolved Pb and Zn from Zinc Plant Leach Residues" Minerals 12, no. 4: 393. https://doi.org/10.3390/min12040393

APA Style

Silwamba, M., Ito, M., Hiroyoshi, N., Tabelin, C. B., Hashizume, R., Fukushima, T., Park, I., Jeon, S., Igarashi, T., Sato, T., Nyambe, I., Nakata, H., Nakayama, S., & Ishizuka, M. (2022). Alkaline Leaching and Concurrent Cementation of Dissolved Pb and Zn from Zinc Plant Leach Residues. Minerals, 12(4), 393. https://doi.org/10.3390/min12040393

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