METHOD FOR RECOVERING NICKEL FROM IRON-ALUMINUM SLAG OBTAINED BY BATTERY POWDER LEACHING

Abstract

Disclosed in the present invention is a method for recovering nickel from iron-aluminum slag obtained by battery powder leaching. The method comprises the following steps: adding a sulfuric acid solution into an iron-aluminum slag to dissolve, so as to obtain a sulfate solution; then adding an oxidizing agent; adding ammonia water and carbonate into the oxidized sulfate solution; adjusting the pH to 1.0-3.2 for reaction; separating ferric hydroxide to precipitate to obtain an iron-removed solution; adding carbonate into the iron-removed solution, adjusting the pH to 3.2-5.5 for reaction; separating aluminum hydroxide to precipitate to obtain an aluminum-removed solution; adding ammonia water to the aluminum-removed solution, adjusting the pH to 7.0-8.8 for reaction; washing and removing impurities to obtain a nickel complex; adding an oxidizing agent to the nickel complex to break the complex, so as to obtain a nickel-containing solution. By means of the present method, efficient separation of iron, aluminum and nickel in the iron-aluminum slag is efficiently achieved, the separation effect of iron, aluminum and nickel is improved, the loss of nickel is reduced, and the recovery rate of nickel is improved.

Claims

1. A method for recovering nickel from iron-aluminum residue obtained by leaching battery powder, comprising the following steps: S1: adding sulfuric acid solution to the iron-aluminum residue for dissolving the same to obtain a sulfate solution, then adding an oxidizing agent; S2: adding ammonia water and carbonate to oxidized sulfate solution, adjusting pH to 1.0-3.2 for reaction, and separating iron hydroxide precipitate to obtain iron-removed liquid; S3: adding carbonate to the iron-removed liquid, adjusting pH to 3.2-5.5 for reaction, and separating aluminum hydroxide precipitate to obtain aluminum-removed liquid; S4: adding ammonia water to the aluminum-removed liquid, adjusting pH to 7.0-8.8 for reaction, and obtaining nickel complex after washing and removing impurities; S5: adding an oxidizing agent to the nickel complex to break complexation to obtain nickel-containing solution.

2. The method according to claim 1, wherein in step S1, the oxidizing agent is hydrogen peroxide; preferably, the volume ratio of the sulfate solution to the hydrogen peroxide is 1: (0.01-0.5), and the mass fraction of the hydrogen peroxide is 1-35%.

3. The method according to claim 1, wherein in step S2, molar ratio of Fe.sup.3+ and CO.sub.3.sup.2?in reaction system is 1:(1-8).

4. The method according to claim 1, wherein in step S2, ratio of molar amount of nickel element to NH.sub.3 in reaction system is 1:(1-10).

5. The method according to claim 1, wherein in step S3, molar ratio of Al.sup.3+ and CO.sub.3.sup.2?in reaction system is 10:(5-50).

6. The method according to claim 1, wherein in step S4, ratio of molar amount of nickel element to NH.sub.3 in reaction system is 1:(4-20).

7. The method according to claim 1, wherein in step S2 and/or step S4, the concentration of the ammonia water is 0.1-5 mol/L.

8. The method according to claim 1, wherein in step S2 and/or step S3, the carbonate is one or more of ammonium carbonate, sodium carbonate or sodium bicarbonate; preferably, the concentration of the carbonate is 0.01-5 mol/L.

9. The method according to claim 1, wherein in step S5, the oxidizing agent is one or two of hydrogen peroxide or sodium hypochlorite.

10. The method according to claim 1, wherein in step S5, the nickel complex is further subjected to ultraviolet light treatment when the complexation is broken.

Description

BRIEF DESCRIPTION OF DRAWINGS

[0028] The present invention will be further described below in conjunction with the accompanying drawings and embodiments, in which:

[0029] FIG. 1 is a process flow diagram of the present invention.

DETAILED DESCRIPTION

[0030] Hereinafter, the concept and technical effects of the invention will be clearly and completely described below in combination with embodiments, so that the purpose, characteristics and effects of the invention can be fully understood. Obviously, the described examples are only part of the examples of the invention, not all of the examples. Based on the embodiments of the invention, other examples obtained by those skilled in the art without creative work belong to the protection scope of the invention.

Example 1

[0031] A method for recovering nickel in iron-aluminum residue obtained by leaching battery powder, referring to FIG. 1, the specific process was: [0032] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1400 ml of sulfuric acid with a concentration of 0.46 mol/L to obtain sulfate solution, and then 70 ml of 30 wt % hydrogen peroxide was added. [0033] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.233 mol, 0.165 mol, 0.094 mol respectively. 320 ml of 0.55 mol/L ammonia water was added as a complexing agent in advance to the sulfate solution, and then 355 ml of 1.50 mol/L sodium carbonate was added as a precipitant, stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated and separated. 130 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.5, and aluminum hydroxide precipitate was generated and separated. 685 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged and was allowed to stand, supernatant liquid was removed and nickel complex was separated. [0034] (3) Separation of nickel from nickel complex: 45 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min. Nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Example 2

[0035] A method for recovering nickel in iron-aluminum residue obtained by leaching battery powder, the specific process was: [0036] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1500 ml of sulfuric acid with a concentration of 0.74 mol/L to obtain sulfate solution, and then 70 ml of 30 wt % hydrogen peroxide was added. [0037] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.233 mol, 0.165 mol, 0.094 mol respectively. 340 ml of 0.55 mol/L ammonia water was added as a complexing agent in advance to the sulfate solution, and then 360 ml of 1.50 mol/L sodium carbonate was added as a precipitant, stirred. The pH was adjusted to 2.9, and iron hydroxide precipitate was generated and separated. 115 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.4, and aluminum hydroxide precipitate was generated and separated. 725 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged and was allowed to stand, supernatant liquid was removed and nickel complex was separated. [0038] (3) Separation of nickel from nickel complex: 50 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min. Nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Example 3

[0039] A method for recovering nickel in iron-aluminum residue obtained by leaching battery powder, the specific process was: [0040] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1100 ml of sulfuric acid with a concentration of 0.87 mol/L to obtain sulfate solution, and then 70 ml of 30 wt % hydrogen peroxide was added. [0041] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.237 mol, 0.166 mol, 0.092 mol respectively. 330 ml of 0.55 mol/L ammonia water was added as a complexing agent in advance to the sulfate solution, and then 370 ml of 1.50 mol/L sodium carbonate was added as a precipitant, stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated and separated. 130 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.5, and aluminum hydroxide precipitate was generated and separated. 685 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged and was allowed to stand, supernatant liquid was removed and nickel complex was separated.

[0042] (3) Separation of nickel from nickel complex: 40 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min. Nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Example 4

[0043] A method for recovering nickel in iron-aluminum residue obtained by leaching battery powder, the specific process was: [0044] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 2000 ml of sulfuric acid with a concentration of 0.24 mol/L to obtain sulfate solution, and then 75 ml of 30 wt % hydrogen peroxide was added. [0045] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.233 mol, 0.163 mol, 0.094 mol respectively. 330 ml of 0.55 mol/L ammonia water was added as a complexing agent in advance to the sulfate solution, and then 355 ml of 1.50 mol/L sodium carbonate was added as a precipitant, stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated and separated. 130 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.5, and aluminum hydroxide precipitate was generated and separated. 710 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged and was allowed to stand, supernatant liquid was removed and nickel complex was separated. [0046] (3) Separation of nickel from nickel complex: 60 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 12 min. Nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Example 5

[0047] A method for recovering nickel in iron-aluminum residue obtained by leaching battery powder, the specific process was: [0048] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 2200 ml of sulfuric acid with a concentration of 0.35 mol/L to obtain sulfate solution, and then 80 ml of 30 wt % hydrogen peroxide was added. [0049] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.234 mol, 0.165 mol, 0.094 mol respectively. 320 ml of 0.55 mol/L ammonia water was added as a complexing agent in advance to the sulfate solution, and then 355 ml of 1.50 mol/L sodium carbonate was added as a precipitant, stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated and separated. 130 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.5, and aluminum hydroxide precipitate was generated and separated. 690 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged and was allowed to stand, supernatant liquid was removed and nickel complex was separated. [0050] (3) Separation of nickel from nickel complex: 50 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min. Nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Comparative Example 1

[0051] A method for recovering nickel in the iron-aluminum residue obtained by leaching battery powder, which differs from the Examples in that sodium carbonate was not added. The specific process was: [0052] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1400 ml of sulfuric acid with a concentration of 0.64 mol/L to obtain sulfate solution, and then 70 ml of 30 wt % hydrogen peroxide was added. [0053] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.233 mol, 0.165 mol, 0.094 mol. 320 ml of 0.55 mol/L ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated, separated, and stirred. 195 ml of ammonia water was further added to the sulfate solution to adjust pH to 3.8, and aluminum hydroxide precipitate was generated, separated, and stirred. 675 ml of ammonia water was added to the sulfate solution. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed with water, centrifuged, and allowed to stand, supernatant liquid was removed and nickel complex was separated. [0054] (3) Separation of nickel from nickel complex: 45 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min, nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.7, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

Comparative Example 2

[0055] A method for recovering nickel in the iron-aluminum residue obtained by leaching battery powder, which differs from the Examples in that sodium carbonate was not added. The specific process was: [0056] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1600 ml of sulfuric acid with a concentration of 0.55 mol/L to obtain sulfate solution, and then 80 ml of 30 wt % hydrogen peroxide was added. [0057] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.234 mol, 0.164 mol, 0.094 mol. 750 ml of 0.50 mol/L sodium hydroxide was added to the sulfate solution, and stirred. The pH was adjusted to 2.5, and iron hydroxide precipitate was generated, separated, and stirred. 130 ml of sodium hydroxide was further added to the sulfate solution to adjust pH to 3.7, and aluminum hydroxide precipitate was generated, separated, and stirred. 195 ml of sodium hydroxide was added to the sulfate solution. The pH was adjusted to 7.8, and nickel hydroxide precipitate was generated.

Comparative Example 3

[0058] A method for recovering nickel in the iron-aluminum residue obtained by leaching battery powder, which differs from the Example 1 in that sodium carbonate was not added. The specific process was: [0059] (1) Iron-aluminum residue pretreatment: 200 g of iron-aluminum residue was dissolved in 1400 ml of sulfuric acid with a concentration of 0.55 mol/L to obtain a sulfate solution. [0060] (2) Sulfate solution: the moles of iron, aluminum, and nickel in the sulfate solution were determined to be 0.233 mol, 0.165 mol, 0.094 mol respectively. 320 ml of 0.55 mol/L ammonia water was added to the sulfate solution in advance, and then 355 ml of 1.50 mol/L sodium carbonate was added, and stirred. The pH was adjusted to 2.8, and iron hydroxide precipitate was generated and separated. 130 ml of sodium carbonate was further added to the sulfate solution, and stirred. The pH was adjusted to 3.5, and aluminum hydroxide precipitate was generated and separated. 685 ml of ammonia water was added to the sulfate solution, and stirred. The pH was adjusted to 7.6, and nickel-containing complex solution was generated. The nickel-containing complex solution was washed to remove impurities and a nickel complex was obtained. [0061] (3) Separation of nickel from nickel complex: 45 ml of 30 wt % hydrogen peroxide was added to the nickel complex. 400 w ultraviolet light was applied to the top of the solution for 15 min, and nickel sulfate solution was obtained, and stirred. 1.0 mol/L sodium hydroxide was added to adjust pH to 7.4, and nickel hydroxide precipitate was obtained. Solid-liquid separation was performed to obtain nickel hydroxide and sodium sulfate solution. The sodium sulfate solution was evaporated at 110? C. to obtain crude sodium sulfate.

[0062] The iron hydroxide, aluminum hydroxide, and nickel sulfate obtained in Examples 1-5 and Comparative Examples 1-3 were all calcinated to constant weight at 160? C. (the iron hydroxide and aluminum hydroxide were dehydrated and decomposed into iron oxide, aluminum oxide, and nickel sulfate dehydrated crystal water respectively). The test data was shown in Table 1.

TABLE-US-00001 TABLE 1 Data of Examples 1-5 and Comparative Examples 1-2. separated product nickel (%) iron (%) aluminum (%) Example 1 iron oxide 1.06 67.83 0.11 aluminum oxide 0.63 0.76 51.36 nickel sulfate 36.14 0.07 <0.01 Example 2 iron oxide 1.14 68.36 0.17 aluminum oxide 0.89 0.71 51.36 nickel sulfate 35.86 0.06 <0.01 Example 3 iron oxide 1.36 68.02 0.20 aluminum oxide 0.75 0.50 51.36 nickel sulfate 35.79 0.05 <0.01 Example 4 iron oxide 1.30 68.17 0.12 aluminum oxide 0.41 0.76 51.36 nickel sulfate 36.02 0.03 <0.01 Example 5 iron oxide 1.22 68.26 0.13 aluminum oxide 0.57 0.98 51.36 nickel sulfate 36.23 0.08 <0.01 Comparative iron oxide 4.36 68.83 0.10 Example 1 aluminum oxide 7.33 3.66 51.36 nickel sulfate 35.14 7.85 <0.01 Comparative iron oxide 5.58 62.65 0.19 Example 2 aluminum oxide 7.98 3.46 51.36 nickel sulfate 35.28 6.03 <0.01 Comparative iron oxide 4.36 62.40 0.33 Example 3 aluminum oxide 13.34 3.46 51.36 nickel sulfate 35.43 5.86 <0.01

[0063] It can be seen from Table 1 that, through measuring, all of the nickel contents in iron oxide and aluminum oxide obtained by dehydration in the Examples were less than 1.4%, the iron content in nickel sulfate was less than 0.10%, and the aluminum content in nickel sulfate was less than 0.01%. The data is better than the method of directly separating iron, aluminum and nickel by alkaline precipitation in Comparative Examples 1 and 2 (nickel content in iron oxide was more than 4.36%, the nickel content in aluminum oxide was more than 7.33%). It shows that the present invention has well realized high-efficiency separation of iron, aluminum, and nickel in iron-aluminum residue, improved the separation effect of iron, aluminum, and nickel, reduced the loss of nickel, and increased the recovery rate of nickel.

[0064] The preferred examples of the present disclosure have been described in detail above with reference to the accompanying drawings, but the present disclosure is not limited to the described examples. Within the scope of knowledge possessed by the ordinary skilled person in the art, various modifications can be made without departing from the purpose of the present invention. In addition, in the case of no conflict, the examples of the present invention and the features in the examples can be combined with each other.