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Original Article
DOI: 10.1016/j.jmrt.2020.01.068
Open Access
Available online 30 January 2020
Study on thermodynamic model of arsenic removal from oxidative acid leaching
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Yang Wanga,1, Xiong Fanga,1, Pin Dengc, Zhihao Ronga, Xincun Tanga,
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tangxincun@csu.edu.cn

Corresponding authors.
, Shan Caob,
Corresponding author
cs1988@qlu.edu.cn

Corresponding authors.
a College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China
b School of Light Industry and Engineering, Qilu University of Technology, Shandong, 250353, China
c Hunan Research Institute of Nonferrous Metals, Changsha, 410100, China
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Tables (5)
Table 1. The content of main ingredient in the sample (wt.%).
Table 2. The reaction and φ/V.
Table 3. The test results of pre-experiment (g·L−1).
Table 4. Ksp of some arsenate and sulfate.
Table 5. The composition analysis (wt.%) (W-YX1, W-YX2, W-XJ respectively represent waste residues of Yongxing and Xinjiang).
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Additional material (1)
Abstract

In this paper, we propose a new strategy to remove arsenic from arsenic-containing waste residues by oxidation-acid leaching. The experimental results show the example is effective for different types of arsenic-containing waste residues. Chemical thermodynamic calculations provide guidance for leaching of oxidizing acids, while theoretical calculations and experimental data have successfully proven the shielding layer of AsH3. The acid leaching characteristics of different types of arsenate were analyzed, a multi-metal ion equilibrium system in acid leaching was established, and a model of arsenic removal by oxidizing acid was established. An in-depth understanding of the relationship between the amount of acid required to leaching different arsenic-containing waste residues and the pH of the leachate provides new perspectives on how to efficiently collect hazardous materials from industrial waste residues.

Keywords:
Arsenic-bearing waste residues
Oxidation-acid leaching
Arsenic removal model
Thermodynamic calculation
Full Text
1Introduction

Arsenic is widely distributed in nature, and natural arsenic compounds are often associated with other minerals, for example domeykite, chloanthite and carminite [1,2]. In recent years, with the rapid development of energy storage devices usually composed of non-ferrous metals, more and more arsenic has been enriched and entered the human living environment, posing a huge threat to human living environment and physical health [1,2]. Most arsenic compounds will volatilize into the flue gas and collide with elements such as lead, antimony and zinc in the high temperature furnace gas during the smelting process of nonferrous metals to form arsenate or arsenite.

Because high arsenic dust usually contains a large amount of valuable metals, such as lead, antimony, tin, indium, etc., it still has economic value [3]. However, despite the increasing achievements in arsenic removal, there are still some difficulties in removing arsenic. Chemists face many difficulties in processing high arsenic dust, separating and removing arsenic, and simultaneously increasing the content of valuable metals [4,5]. On the other hand, if the dust is returned directly to the smelter to recover valuable metals, it will reduce the efficiency of the equipment and increase the energy consumption required for the smelting process. Therefore, it is urged to establish a simple and efficient method to recover high arsenic dust with fine particle size, valence and composition.

So far, the main treatment methods are divided into pyrolysis arsenic by fire roasting [6] and wet leaching arsenic [7]. Wet leaching of arsenic is mainly divided into hot water leaching, acid leaching and alkali leaching. Roasting arsenic removal has low cost, short process, simple process, large scale, low arsenic removal rate, poor working environment, and serious air pollution [8]. Compared with fire roasting, wet arsenic removal has the advantages of high arsenic removal rate and complicated processing [9–11], high arsenic removal rate and less environmental pollution.

In addition, the subsequent treatment of arsenic-containing liquids after leaching should be considered [12–14]. At present, the method of adding iron salt or calcium salt to the solution is widely used to treat high-concentration arsenic wastewater [15–17]. In order to match the process, the filtrate after alkali leaching requires not only oxidation treatment, but also acid to adjust the pH, which further increases the treatment process and cost.

At the same time, due to the wide range of sources and complex components of arsenic-containing waste residues, the theoretical analysis of leaching of arsenic in arsenic-containing waste residues is less, and it is difficult to find suitable arsenic removal methods for different methods. The type of arsenic-containing waste residue. This article takes high arsenic dust as an example, introduces a simple method for large-scale recovery of arsenic, improves the traditional acid leaching process, and the leaching rate is more than 95%, which solves the problem of producing highly toxic arsenic gas from sulfuric acid. Leaching. Then the theoretical research on the leaching process was carried out, and a multi-metal ion-acid leaching equilibrium system model was established to provide guidance for the oxidation-acid leaching process of various arsenic-containing waste residues.

2Materials and methods2.1Materials

The arsenic-containing sample used in all experiments was smelting dust. The dust was generated by oxidized blowing and reduction smelting of fog copper, provided by the lead-copper smelting company in Jiyuan, Henan province, China. The main components of the dust were analyzed by phase analysis. The ICP results are shown in Table 1. The contents of arsenic, lead, copper and zinc were 20.90%, 46.08%, 3.52% and 2.73%, respectively. The XRD pattern shown in Fig. 1 shows that the arsenic exists in the stages of PbHAsO4, Pb5 (AsO4)3Cl, and As2O3, which correspond to the Joint Committee on Powder Diffraction Standards (JCPDS) card No. 29-0072, No. 19-0683 and No. 36-1490, respectively. The copper and zinc parts are present as sulfides.

Table 1.

The content of main ingredient in the sample (wt.%).

Element  Content (wt.%) 
As  20.90 
Pb  46.08 
Cu  3.52 
Zn  2.73 
Fig. 1.

The XRD pattern of the sample.

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Sulfuric Acid (Analytical Pure), Hydrogen Peroxide (Analytical Pure), Mercury bromide (Analytical Pure) used in this study were supplied by Sinopharm Chemical Reagent Co., Ltd, China.

2.2Experimental

All leaching experiments were performed in 500 mL three-necked flasks, and the openings of the flasks were completely closed with mechanical stirrers, pH/ORP test electrodes and exhaust pipes leading to AsH3 absorption bottles. 200 mL of a hydrogen peroxide-sulfuric acid leaching solution (0–4% (volume ratio) H2O2 + 0–98 g·L−1 (0–1 M) H2SO4) was introduced into the flask. The temperature was then adjusted from 293 K to 363 K to find the best experimental conditions. Add 50 g of arsenic-containing sample. The resulting slurry was then stirred at 300 rpm for 4 h. An AsH3 absorption bottle containing a 50 mL, 6% (volume) hydrogen peroxide solution. Before the AsH3 absorption bottle, a mercury bromide test paper was added to detect the generation of arsenide, and the arsenic in the absorption solution was measured by mercury in Gutzeit Content (II) bromide method. At the end of each experimental run, the solids were separated from the solution by filtration. The filtrate and residue were analyzed for chemical composition and chemical phase. Estimate the leaching rate of arsenic according to the following formula:

Where η  is the leaching rate of the element, %; m0 is the sample mass before leaching, g; ω0 is the content of the element in the sample, %; m  is the sample mass after leaching, g; ω  is the content of the element in the residue, %.

2.3Characterization and analyses

The XRD patterns were collected using a Bruker D8 diffraction instrument with Cu Kα radiation (40 kV, 40 mA). X-ray photoelectron spectroscopy (XPS, ESCALAB 250 Xi, Thermo Fisher Scientifific, USA) was used to elucidate the oxidation state and the composition of the dust sample and leach residue. Slurry solution pH were measured for every test using laboratory pH/ORP meters (FE28, METTLER TOLEDO, Switzerland). All solution and solid analysis were conducted using an Inductively Coupled Plasma optical emission spectrometer (ICP-OES, Optima 5300DV, PerkinElmer, USA). The detection limit of ICP-OES for the elements was 0.01 mg L−1.

3Results and discussion3.1The analysis of Hydrogen peroxide treatment

Due to the presence of zinc, reducing metals such as As (III) and As (V) are reduced to AsH3, and the traditional acid leaching process may lead to safety accidents [18]. The reaction equation is as follows:

To ensure the safety of the leaching operation and avoid the generation of AsH3, the safety of the treatment was evaluated using hydrogen peroxide as a shielding agent in the experiments. Taking Zn in waste as an example, when the concentration of As (III) or As (V) in the solution is 0.7 mol·L−1 and 10-6 Pa, the H+ concentration c (H+) is 0.1 mol·L−1, 1 mol·L−1, and 2 mol·L−1, respectively. The calculated equilibrium potentials of the relevant reactions and their results are shown in Table 2[19,20]. According to the analysis of the data in this table, when H2O2 is not added, As (III) or As (V) is reduced as an oxidant in the presence of a reducing metal such as Zn, and AsH3 toxic gas is easily generated. After adding H2O2, due to the strong oxidizing property of H2O2, Zn must preferentially react with it to prevent Zn from reducing As (III) or As (V). At the same time, if AsH3 is generated, H2O2 can also oxidize AsH3 to As (III) or As (V) to prevent AsH3 from escaping. The test results before the experiment are shown in Table 3. Only before the experiment, an additional 0.1 g of Zn was added to the dust. The experiments were performed with 293 K, 328 K and 363 K water immersion, hydrogen peroxide immersion (4% H2O2), acid leaching (98 g·L−1 H2SO4), and oxidizing acid leaching (4% H2O2, 98 g·L−1 H2SO4), respectively. It can be seen from Table 3 that both the acid leaching and the oxidizing acid leaching have achieved a good leaching effect. The leaching rate of arsenic exceeds 95%, but AsH3 is generated during the acid leaching process, and the shielding of AsH3 can be achieved after adding hydrogen peroxide. At the same time, due to the rapid decomposition of hydrogen peroxide at high temperatures, the shielding effect is weakened. Therefore, it is possible to perform oxidation-acid leaching at normal temperature while ensuring operation safety to achieve a high arsenic leaching rate.

Table 2.

The reaction and φ/V.

nReactionφ/Va(H+)
0.1 
(1)  H3AsO4+2H++2e=HAsO2+2H2O  φ/V=0.560-0 .0591p+0.0295lgaH3AsO4 -0.0295lga(HAsO2)  0.505  0.565  0.583 
(2)  H3AsO4+8H++8e=AsH3+4H2O  φ/V=0.144-0 .0591p+0.0074lgaH3AsO4 -0.0074lgp(AsH3)  0.128  0.187  0.205 
(3)  HAsO2+6H++6e=AsH3+2H2O  φ/V=0.005-0 .0591pH+0.0098lgaHAsO2-0.0098lgp(AsH3)  −0.056  0.003  0.021 
(4)  Zn2++2e=Zn  φ/V=-0.762+0.0295lgaZn2+   −0.792  −0.792  −0.792 
(5)  H2O2+2H++2e=2H2O  φ/V=1.776-0 .0591pH+0.0295lgaH2O2   1. 717  1.776  1.794 
Table 3.

The test results of pre-experiment (g·L−1).

ConditionConcentration in leachateGenerate AsH3 or not  As concentration in absorption solution 
As  Zn  Cu  Pb  Fe     
Water leaching20℃  9.357  0.110  0.001  0.000  0.000  no  0.00 
55℃  10.534  0.111  0.000  0.000  0.000  no  0.00 
90℃  13.947  0.083  0.000  0.000  0.000  no  0.05 
Hydrogen peroxide leaching20℃  14.001  1.432  0.982  0.000  0.000  no  0.00 
55℃  14.455  2.432  1.297  0.000  0.000  no  0.05 
90℃  16.476  1.602  1.065  0.001  0.000  no  0.10 
Acid leaching20℃  42.512  6.564  8.221  0.000  0.004  yes  1.55 
55℃  51.923  6.654  8.875  0.000  0.074  yes  1.75 
90℃  50.112  6.032  8.445  0.000  0.022  yes  1.75 
Oxidizing acid leaching20℃  50.265  7.098  8.946  0.0004  0.023  no  0.00 
55℃  45.337  6.435  8.456  0.000  0.054  no  0.10 
90℃  44.297  6.553  8.043  0.000  0.033  no  0.75 

In order to obtain detailed information about the chemical composition and valence state of the original dust, the dust treated with only H2O2 and the dust treated with oxidizing acid were used in turn. As can be seen from Fig. 2a, As, Cu, Zn and Pb are the main phases in all three samples. Obviously, compared with the original dust, the As, Cu and Zn content in the dust after the oxidative acid leaching treatment is significantly reduced. As shown in Fig. 2b, the peaks centered at 139.39 eV (Pb 4f7/2) and 144.19 eV (Pb 4f5/2) are attributed to the characteristic peaks of Pb (II). Fig. 2c and d also show that there are two peaks in the XPS spectrum of As. One focusing on 1326.44 eV (As 2p3) and 45.21 eV (As 3d) was regarded as the characteristic peak of As in the 3+ oxidation state, and the other focusing on 1327.85 eV and 46.44 eV was designated as As5+. In addition, in the original dust, the value of As3+/ As5+ is about 1/4. In the dust treated with H2O2, the proportion of As3+ decreases and the percentage of As5+ increases, which means that a large amount of As3+ has been oxidized to As5+ during the oxidation process using hydrogen peroxide. In addition, in the dust after the oxidative acid leaching treatment, the peak area of As decreases sharply, which indicates that As is almost completely leached by the formation of H3AsO4. Fig. 2e and f show that the Zn 2p peak at 1022.34 eV is a typical Zn peak in the 2+ oxidation state. It indicates that most of the Zn and Cu species are present in the 2+ state in all three samples.

Fig. 2.

The XPS pattern of original dust, dust treated by H2O2 and dust treated by oxidation-acid leaching, and b), c), d), e), f) are XPS spectra of Pb 4f, As 2p3, As 3d, Zn 2p, Cu 2p Separately.

(0.89MB).

In short, after the hydrogen peroxide treatment, the As3+ species in the dust is oxidized to As5+ species, and the metal is oxidized to a high-valent cation state. Then, the insoluble arsenate material can be converted into soluble arsenic acid by adding an acid, and then the As material can be leached.

3.2Establishment of oxidative acid leaching model

Since the low-value substance is oxidized to a high-valence state in the oxidizing acid leaching reaction, the leaching process can be simply simulated. As shown in Fig. 3, a multi-metal ion equilibrium system can be established. The substances in the oxidized system can be divided into: (1) M1: substances that do not react with acids, such as CuSO4, ZnSO4, etc. ; (2) M2: with acids Non-arsenate reacting, such as CaCO3, Fe2O3, etc. ; (3) M3: Arsenate reacting with acid, such as PbHAsO4, FeAsO4, etc. After the equilibrium of oxidizing acid leaching, there is mainly a balance between arsenate ions, sulfate ions and cations in the system, so the metal ions in the solution can be divided into: (1) M4: can react with arsenate and sulfate to form Precipitation, such as Pb2+, Ca2+, Ba2+, etc.; (2) M5: Only react with arsenate to form a precipitate that does not react with sulfate, such as Fe3+, Zn2+, Cu2+, etc. After filtration, the main component of the filter residue is sulfate precipitation. Since the acid consumed by M2 is negligible, the effects of M3 and M4 are mainly considered when calculating the amount of acid added in the extract.

Fig. 3.

Model of oxidative acid leaching.

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Setting that the liquid-solid ratio of the leaching process is n, the free hydrogen ion in the leach solution after leaching is cH, that is, the pH of the leach solution is –lgcH. Since arsenic acid is a weak acid [21], there are:

H3AsO4 → H2AsO4 + H+ ka1 = 6.2 × 10−3
H2AsO4 → HAsO2−4 + H+ ka2 = 1.2 × 10−7
HAsO2−4 → AsO3−4 + H+ ka3 = 3.1 × 10−12

For the leaching of arsenate, setting that the content of MAsO4 or MHAsO4 in waste residue is x (mass fraction), the molar mass of MAsO4 or MHAsO4 is M, the concentration of M3+ or M2+in the leachate is cM, and the concentrations of H3AsO4, H2AsO4, HAsO42-, and AsO43- are y0, y1, y2, y3.

Considering that in the acidic environment, the precipitation is mainly acid arsenate, the leaching of arsenate species (MAsO4) can be divided into the following categories:

a) FeAsO4 species

The dissolution of MAsO4 is:

MAsO4 → AsO3−4 + M3+ Ksp(MAsO4) = K1

According to Eqs. (1–4), there are:

For incomplete leaching :

Calculated according to Eq. (5–9):

At this point cM≤1000xMn, then the concentration of sulfuric acid in the leachate should be:

When K1+cHK1ka3+cH2K1ka2ka3+cH3K1ka1ka2ka3>1000xMn, there are: cM=1000xMn ;

So for complete leaching:

Calculated according to Eq. (5–8 and 12):

The concentration of sulfuric acid in the leach solution should be:

b) ZnHAsO4 species

The concentration of sulfuric acid in the leach solution is:

C) PbHAsO4 species

Sulfate precipitates will be produced, so there is:

MSO4 → SO2−4 + M2+ Ksp(MSO4) = K2
WhencH(cH2K1ka1ka2K2+cHK1ka2K2+K1K2+ka3K1cHK2)2+cHK1ka2K2+2K1K2+3ka3K1cHK2<1000xMn,

Please refer to the support information 1∼3 for the detailed calculation process.

According to Eqs. (11),(14),(15),(16),(18) and (19), When 1000x/Mn is taken from 0.00–1.75, taking the FeAsO4, ZnHAsO4 and PbHAsO4 as examples, Dust-Free Hydrogen- Sulfuric Acid Concentration Chart can be obtained. The result is shown in Fig. 4.

Fig. 4.

Dust-Free Hydrogen-Sulfuric Acid Concentration Chart: a), c), e) are surface map of leaching of FeAsO4, ZnHAsO4 and PbHAsO4; b), d), f) are leaching curve of FeAsO4, ZnHAsO4 and PbHAsO4.

(1MB).

As can be seen from Fig. 4, different types of arsenate dust require different sulfuric acid consumption and the concentration of free hydrogen ions in the leachate is also different. As shown in Fig. 4a, c and e, the dissolution and leaching process is divided into two phases: the dissolving acid consumption phase and the acid excess phase. When the acid is too much, Δc(H2SO4)/Δa becomes smaller and gradually approaches 0.5, so whether the leaching is completed can be judged by the pH change rate of the solution. It can be seen from Fig. 4b, d, and f that when it is completely leached, the amount of free hydrogen in the leachate increases with the amount of leaching dust, but the increase rate of Δa/n(dust) is the same, As the quantity n(dust) increases, c(H2SO4)/n(dust) decreases. Therefore, the higher the leaching amount, the higher the acid utilization. Consider real arsenic species in dust:

We assume here that the MAsO4 substances in the original dust are arranged in the order of leaching: M1AsO4, M2AsO4, M3AsO4, …, MpAsO4, and when MiAsO4 is being leached, M1AsO4, M2AsO4, M3AsO4, … Mi-1AsO4 has been completely leached. Setting that the concentration of MiAsO4 species in the leaching is c(MiAsO4)=ci (i = l,2,3…,p), and the concentration of Mi3+ in the leachate is bi.

When MiAsO4 belongs to FeAsO4 species:

Since y0, y1, y2 are relatively small, it can be simplified as:

Then:

It can be seen that the leaching at this time is only related to MiAsO4, so the content of As in the dust is set to be ω (mass fraction), and when the concentration of Mi3+ in the leachate is bi, the leaching rate of As is η,:

And because hydrogen peroxide is added during the leaching process, the calculation results will be somewhat biased. Therefore, a factor ε was introduced to correct the actually required sulfuric acid concentration. The correction factor ε can be approximated as:

η0 is the leaching rate of arsenic by hydrogen peroxide leaching.

Then:

When MiAsO4 belongs to ZnHAsO4 species:

When MiAsO4 belongs to PbHAsO4 species:

Please refer to the support information 4∼6 for the detailed calculation process.

3.3Comparison between theoretical model and experiments

Many experts have done a lot of research on arsenate [22–24]. Table 4 illustrates the solubility constants of some arsenate and sulfate (Ref: [1][25], [2][26], [3][27], [4][28], [5][21], [6][29] ).

Table 4.

Ksp of some arsenate and sulfate.

Formula  Ksp  Formula  Ksp  Formula  Ksp 
BiAsO4[1]  4.40 × 10−10  CrAsO4[1]  7.70 × 10−21  AlAsO4[2]  8.70 × 10−19 
FeAsO4[3,4]  5.70 × 10−21  CaHAsO4[5]  1.60 × 10−5  BaHAsO4[5]  1.60 × 10−5 
ZnHAsO4[5]  2.30 × 10−7  CuHAsO4[5]  6.80 × 10−8  PbHAsO4[6]  2.00 × 10−10 
CaSO4[1]  4.93 × 10−5  BaSO4[1]  1.08 × 10−10  PbSO4[1]  2.53 × 10−8 

According to the above calculation formula, the relationship between the leaching rate and the required sulfuric acid concentration in the leaching solution, and the relationship between the leaching rate and the pH (-lg) of the leaching solution (considering that the leaching of PbHAsO4 can be divided into dissolution and reprecipitation processes The leaching order is ZnHAsO4, PbHAsO4, FeAsO4. As shown in Fig. 5, the results are consistent with the experiment. Fig. 6 is the trend of the concentration of Cu, Zn, Fe and As in the solution as the sulfuric acid concentration increases. As can be seen from Fig. 5, the leaching process can be divided into several stages:

Fig. 5.

Comparison between theoretical model and experiments (the solid lines are results of theoretical calculation and points are results of experiments).

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Fig. 6.

The concentration trend of Cu, Zn, Fe and As in solution with the change of sulfuric acid concentration.

(0.16MB).

The a–b zone is the oxidation zone, in this zone, hydrogen peroxide oxidizes As3+ to As5+, CuS, ZnS and the like are oxidized to CuSO4, ZnSO4, etc., and the pH of the solution is significantly decreased:

Compared with Fig. 6, it can be found that the concentration of copper, zinc and arsenic ions in the solution is increased after oxidation. This is because most of the CuSO4, ZnSO4, etc. generated during this process directly enter the leachate, and only a small amount of CuHAsO4 and ZnHAsO4 are generated.

The b–c zone is a Cu-Zn-As leaching zone, in which CuHAsO4 and ZnHAsO4 are dissolved and leached, and the rate of decrease in pH gradually becomes slower. It can be seen from Fig. 6 that with the increase of the sulfuric acid concentration in this region, the leaching rate of Cu, Zn, and As increases, and the sum of the increase in Cu and Zn concentrations is equal to the increase in As concentration, which further proves that the region is copper zinc arsenate Dissolution and leaching.

The c–d area is a Pb-As leaching area. During this interval, PbHAsO4 dissolves and forms PbSO4, and the pH value slowly decreases. It can be seen from Fig. 6 that as the concentration of As in the solution continuously increases, the concentration of sulfuric acid increases, and the concentration of other metal ions does not change much. This indicates that the lead arsenate precipitate in this area has been converted into a sulfate precipitate, and As has been leached into the solution. Due to the leaching of a large amount of arsenic, the solution forms a buffer system and the pH value slowly decreases.

The d–e region is an Fe-As leaching region. Because the Ksp precipitation of FeAsO4 is too small, the amount of sulfuric acid required in this region increases sharply, and the pH value drops significantly. According to the difference between the calculated results and the experimental results, the model conforms to the actual situation and can provide guidance for actual leaching. For this batch of slag, leaching in the Pb-As leaching zone is the most economical and effective. When the source of the waste residue is different, the model can also be used for simulation to predict the leaching rate of arsenic, the consumption of acid and the pH value of the leaching solution, and provide a basis for selecting the optimal leaching conditions.

Table 5 shows the composition analysis results of three different waste residues. And as shown in Fig. 7, the theoretical leaching curves of these waste residues are also in agreement with the experiments, indicating that the model can also be applied to different arsenic-containing residues. Among them, the acid consumption is large, and the effect on W-YX1 is small, because the arsenic content of W-YX1 is high, and most of it is trivalent arsenic. For waste residues such as W-YX1, it is more suitable for multiple leaching.

Table 5.

The composition analysis (wt.%) (W-YX1, W-YX2, W-XJ respectively represent waste residues of Yongxing and Xinjiang).

  As(III)  As(V)  Pb  Cu  Zn  Fe 
W-YX1 (wt.%)  44.16  2.33  14.38  0.05  0.52  2.29 
W-YX2 (wt.%)  6.61  12.27  13.69  0.03  1.37  0.97 
W-XJ (wt.%)  6.11  14.25  9.55  2.18  16.17  2.43 
Fig. 7.

Comparison between theoretical model and experiments (W-YX1, W-YX2, W-XJ respectively represent waste residues of Yongxing and Xinjiang).

(0.7MB).
4Conclusions

This paper introduces a simple and efficient method that can remove arsenic from high arsenic dust with fine-grained complex valence. The results of this study are summarized as follows:

  • (1)

    The theoretical feasibility of avoiding the production of AsH3 in acid (H2SO4 system) leaching arsenic is analyzed. The calculation of relevant thermodynamics and practical experiments shows that during the leaching process, hydrogen peroxide can avoid the production of toxic AsH3. The optimal concentration of H2O2 is 4% by volume.

  • (2)

    Through analysis, arsenic in dust mainly exists in the form of PbHAsO4, Pb5(AsO4)3Cl, As2O3. Copper and zinc exist mainly in divalent forms. After the hydrogen peroxide treatment, the arsenic is leached into the solution in the form of arsenate acid.

  • (3)

    According to the results of the phase analysis of the residue, the leaching of oxidizing acid into arsenate can be simulated, and the amount of acid and the leaching process can be calculated.

If this research is expanded, it will be possible to perform automatic analysis and automatic leaching of different arsenic-containing waste residues in the future.

Conflict of interest

The authors declare no conflict of interest.

Acknowledgements

This work was supported by National Natural Science Foundation of China (Grant No. 21476268, 21808170) and Shandong Provincial Natural Science Foundation (Grant No. ZR201807260006).

Appendix A
Supplementary data

The following are Supplementary data to this article:

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