CN102491554A - Method for treating alkali wastewater containing uranium - Google Patents
Method for treating alkali wastewater containing uranium Download PDFInfo
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- CN102491554A CN102491554A CN2011103937741A CN201110393774A CN102491554A CN 102491554 A CN102491554 A CN 102491554A CN 2011103937741 A CN2011103937741 A CN 2011103937741A CN 201110393774 A CN201110393774 A CN 201110393774A CN 102491554 A CN102491554 A CN 102491554A
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Abstract
The invention provides a method for treating alkali wastewater containing uranium, which comprises the following steps: (a) adding Ca(OH)2 into the alkali wastewater containing uranium and enabling concentration of CO32- and HCO3- in the alkali wastewater containing uranium to be reduced be less than 0.1mg/L, (b) filtering obtained the alkali wastewater containing uranium in the step (a), adding FeSO4 into filtrate and adjusting potential of hydrogen (pH) value in a range of 7.0-9.0, (c) adding BaCl2 into obtained alkali liquid containing uranium in the step (b) to performing coprecipitation and radium removing, and (d) aging obtained alkali liquid containing uranium in the step (c), performing the step (b) to aged alkali liquid containing uranium, and performing neutralization reaction together with the filtrate. After 5-10 times of cycling aging, finally-obtained alkali liquid containing uranium is filtered to obtain filtrate and filter residues. By means of the method, uranium content in wastewater can be reduced to be less than 0.05 mg/L, radium content can be reduced to be less than 1.1 Bq/L, standard wastewater discharge can be completely achieved, and residues are small in quantity and easy to dispose.
Description
Technical field
The present invention relates to the hydrometallurgy of uranium field, be specifically related to the removal method of uranium, radium in the uranium mine alkalescence uranium-containing waste water.
Background technology
The uranium ore alkaline process leaches with the acid system leaching and compares; Can optionally dissolve the uranium in the ore; Wherein iron, aluminium, titanium etc. are dissolved in the carbonate solution hardly, have only some a spot of molybdate, silicate, vannadate, phosphoric acid salt and some metal carbonate complex compound in the leach liquor.The radionuclide thorium soaks at alkali and is actually insoluble in the process, and radium then dissolves 1.5~3%, and other radionuclide is obviously all dumped mine tailing and suffered.Therefore the uranium mine of handling for alkaline process, the principal pollutant of waste water are radioactive nucleus uranium and radium.
See that from the explored uranium resources of China the ratio of alkaline ore resource amount reaches 30%, adopt alkaline process (carbonate) to leach usually, often use NaCl+NaHCO because uranium reclaims the drip washing operation of technology for this type ore
3, bring Cl to system
-, and progressively accumulation, cause the tail washings uranium concentration of absorption process to run height, influence the recovery of uranium.Therefore, need a part of waste water be effluxed, normally move to guarantee technology.CO in the alkalescence uranium-containing waste water
3 2-And Cl
-Coexistence, prior art remove uranium, remove the radium weak effect, are difficult to reach the highest allowable value of discharge of wastewater: uranium 0.3mg/L, radium 1.1Bq/L.This is the major cause that China's alkalescence ore uranium resources does not obtain large-scale development as yet.
Summary of the invention
The object of the present invention is to provide a kind of alkaline uranium-containing waste water treatment process that solves the environmental protection problem of uranium mine.
Realize the technical scheme of the object of the invention: a kind of alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization: add Ca (OH) in the alkalitropism uranium-containing waste water
2, Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L;
(b) neutralization: the alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value stirs and makes Fe
2+Oxidation generates Fe (OH)
3Deposition, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 7.0~9.0;
(c) remove radium: in the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 20~60g/m
3
(d) circulation ageing: the alkaline uranium-bearing slurry to step (c) gained carries out ageing, 20~30 ℃ of ageing temperature, digestion time 16~22h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 5~10 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
Aforesaid a kind of alkaline uranium-containing waste water treatment process, its described Ca (OH)
2Through the digestion of unslaked lime water is processed.
Aforesaid a kind of alkaline uranium-containing waste water treatment process, in its step (a), Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.1~1.3 times of molar weight sum, 20~30 ℃ of temperature of reaction, 0.5~2 hour reaction times.
Aforesaid a kind of alkaline uranium-containing waste water treatment process, its step (b) adopt pneumatic blending to add FeSO
4, 20~30 ℃ of neutralization reaction temperature, neutralization reaction time 1~3h.
BaCl in the aforesaid a kind of alkaline uranium-containing waste water treatment process, its step (c)
2The molar weight that adds is SO
4 2-5 ‰ of molar weight~15 ‰, 20~30 ℃ of temperature of reaction, reaction times 1~3h.
Aforesaid a kind of alkaline uranium-containing waste water treatment process, CO in its described alkaline uranium-containing waste water
3 2-Content is 3.5~12.0gL
-1HCO
3 -Content is 2.0~3.0gL
-1PH value 9.0~10.5, uranium content 1.0~10.0mgL
-1Radium content 10~40BqL
-1
Aforesaid a kind of alkaline uranium-containing waste water treatment process is in its step (b), if HCO in the waste water
3 -Content is more is transferred to 7 with waste water ph, CO in waste water
3 2-Content is more is transferred to 9 with waste water ph.
Effect of the present invention is: the present invention is according to containing and UO in the alkaline uranium-containing waste water
2 2+The CO that complex ability is strong
3 2-And HCO
3 -Characteristics, earlier remove CO with chemical precipitation method
3 2-And HCO
3 -, and deposition is removed most of uranium simultaneously, removes uranium and coprecipitation method except that radium with the chemical carrier distillation method degree of depth then.Handle alkaline uranium-containing waste water application the present invention the waste water uranium content is reduced to below the 0.05mg/L, radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard fully.The dirty quantity of slag is less, is easy to dispose.Cost for wastewater treatment is controlled at lower level, and cost for wastewater treatment is lower than the acid waste water processing cost in the ton ore.The inventive method is used for the wastewater treatment of uranium mine, has solved the environmental problem that exists for many years, makes to efflux the environmental pollution that alkaline waste water causes and be curbed, and the environment of mining area quality improves.
Description of drawings
Fig. 1 is the schema of a kind of alkaline uranium-containing waste water treatment process of the present invention.
Embodiment
Below in conjunction with accompanying drawing and specific embodiment a kind of alkaline uranium-containing waste water treatment process of the present invention is further described.
Embodiment 1
Certain uranium ore alkaline waste water is formed U:3.91mgL
-1CO
3 2-: 4.54gL
-1HCO
3 -: 2.32gL
-1Ra:18.2BqL
-1Cl
-: 7.54gL
-1Ca:0.006gL
-1Mg:0.034gL
-1
Above-mentioned alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, described Ca (OH)
2Through the digestion of unslaked lime water is processed.Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition.Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.1 times of molar weight sum, 25 ℃ of temperature of reaction, 1 hour reaction times.Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L;
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value adopts pneumatic blending to make Fe
2+Oxidation generates Fe (OH)
3Deposition, neutralizing agent FeSO
47H
2O consumption 5kgm
-3, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 8.0; 25 ℃ of neutralization reaction temperature, neutralization reaction time 2h.
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 40g/m
3BaCl
2The molar weight that adds is SO
4 2-10 ‰ of molar weight, 25 ℃ of temperature of reaction, reaction times 2h.
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 25 ℃ of ageing temperature, digestion time 20h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 8 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.0Bq/L, can realize discharged wastewater met the national standard.
Certain uranium ore alkaline waste water is formed U:0.70mgL
-1CO
3 2-: 5.10gL
-1HCO
3 -: 1.56gL
-1Ra:15.2BqL
-1Cl
-: 3.92gL
-1Ca:0.010gL
-1Mg:0.042gL
-1
Above-mentioned alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, described Ca (OH)
2Through the digestion of unslaked lime water is processed.Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L;
Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.1 times of molar weight sum, 25 ℃ of temperature of reaction, 1 hour reaction times.
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value adopts pneumatic blending to make Fe
2+Oxidation generates Fe (OH)
3Deposition, neutralizing agent FeSO
47H
2O consumption 5.2kgm
-3, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 8.2; 25 ℃ of neutralization reaction temperature, neutralization reaction time 2h.
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 35g/m
325 ℃ of temperature of reaction, reaction times 2h.
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 25 ℃ of ageing temperature, digestion time 18h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 6 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
Embodiment 3
Certain uranium ore alkaline waste water is formed U:9.49mgL
-1CO
3 2-: 11.6gL
-1Ra:34.5BqL
-1Cl
-: 16.24gL
-1Ca<0.005gL
-1Mg<0.005gL
-1
Above-mentioned alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L;
Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.1 times of molar weight sum, 25 ℃ of temperature of reaction, 1 hour reaction times.
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value adopts pneumatic blending to make Fe
2+Oxidation generates Fe (OH)
3Deposition, neutralizing agent FeSO
47H
2O consumption 5.6kgm
-3, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 8.1; 25 ℃ of neutralization reaction temperature, neutralization reaction time 2h.
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 45g/m
325 ℃ of temperature of reaction, reaction times 2h.
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 20~30 ℃ of ageing temperature, digestion time 16~22h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 7 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
Embodiment 4
Certain uranium ore alkaline waste water is formed: CO
3 2-Content is 3.5gL
-1HCO
3 -Content is 3.0gL
-1PH value 9.0, uranium content 1.0mgL
-1Radium content 10BqL
-1
Above-mentioned alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L; Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.2 times of molar weight sum, 20 ℃ of temperature of reaction, 0.5 hour reaction times.
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value adopts pneumatic blending to make Fe
2+Oxidation generates Fe (OH)
3Deposition, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 7.0; 20 ℃ of neutralization reaction temperature, neutralization reaction time 1h.
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 20g/m
3BaCl
2The molar weight that adds is SO
4 2-5 ‰ of molar weight, 20 ℃ of temperature of reaction, reaction times 1h.
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 20 ℃ of ageing temperature, digestion time 16h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 5 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
Embodiment 5
Certain uranium ore alkaline waste water is formed: CO
3 2-Content is 12.0gL
-1HCO
3 -Content is 2.0gL
-1PH value 10.5, uranium content 10.0mgL
-1Radium content 40BqL
-1
Above-mentioned alkaline uranium-containing waste water treatment process, it comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L; Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.3 times of molar weight sum, 30 ℃ of temperature of reaction, 2 hours reaction times.
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value adopts pneumatic blending to make Fe
2+Oxidation generates Fe (OH)
3Deposition, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 9.0; 30 ℃ of neutralization reaction temperature, neutralization reaction time 3h.
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 60g/m
3BaCl
2The molar weight that adds is SO
4 2-15 ‰ of molar weight, 30 ℃ of temperature of reaction, reaction times 3h.
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 30 ℃ of ageing temperature, digestion time 22h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 10 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
The present invention is according to containing and UO in the alkaline uranium-containing waste water
2 2+The CO that complex ability is strong
3 2-And HCO
3 -Characteristics, earlier remove CO with chemical precipitation method
3 2-And HCO
3 -, and deposition is removed most of uranium simultaneously, removes uranium and coprecipitation method except that radium with the chemical carrier distillation method degree of depth then.The concrete operations step is following:
(1) Ca (OH)
2In the alkalization process, with CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition makes CO in the waste water
3 2-And HCO
3 -Reduce to below the 0.1mg/L, thereby make it complexing UO
2 2+Amount very limited, most of uranium precipitates in this process in the waste water.In order to guarantee to remove CO
3 2-Effect, Ca (OH)
2Consumption is controlled at stoichiometric 1.1~1.3 times.
(2) remove CO
3 2-And HCO
3 -Waste water also need the degree of depth to remove uranium and remove radium, and need adjustment pH, the present invention selects a kind of weak acid, i.e. FeSO
4(can use anhydrous FeSO
4, also available FeSO
47H
2O), it can not cause the CaCO that generates when the neutralization bases wastewater
3Deposition is returned molten, therefore, and the CaCO of generation
3Deposition can be filtered, and also can not filter.This process adopts pneumatic blending, makes Fe
2+Oxydrolysis generates fresh Fe (OH)
3Deposition is used for adsorbing the remaining uranium of carrier band, reaches the purpose that the degree of depth is removed uranium.FeSO
47H
2The add-on of O is a benchmark to regulate pH<9 usually, with CO in the waste water
3 2-And HCO
3 -Amount relevant, approximately be 1/3~2/3 of sum of the two.If HCO in the waste water
3 -Content is more is transferred to 7 with waste water ph, CO in waste water
3 2-Content is more is transferred to 9 with waste water ph.
(3) through adding FeSO
4Replenish SO
4 2-After, add BaCl
2Carry out co-precipitation and remove radium, in order to guarantee to remove radium effect, BaCl
2Add-on and the SO that replenishes
4 2-Amount is relevant, the SO that replenishes
4 2-Few, the BaCl that then need add
2Many, be controlled at 20~60g/m usually
3
(4) Fe
2+Oxydrolysis has generated loose gelationus Fe (OH)
3, more sad filter, and the slurry volume is relatively large.Through slurry circulation and aged method, concrete operation method: the slurry of last time is returned neutralization procedure next time, and circulation repeatedly reduces the slurry volume, and improves its strainability.
Claims (7)
1. alkaline uranium-containing waste water treatment process, it is characterized in that: this method comprises the steps:
(a) alkalization:
Add Ca (OH) in the alkalitropism uranium-containing waste water
2, Ca (OH)
2With CO
3 2-And HCO
3 -Reaction generates CaCO
3Deposition, Ca (OH)
2Add-on make CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -Concentration is reduced to below the 0.1mg/L;
(b) neutralization:
The alkaline uranium-containing waste water of step (a) gained is filtered, obtain filtrating and filter residue; In filtrating, add FeSO then
4Adjustment pH value stirs and makes Fe
2+Oxidation generates Fe (OH)
3Deposition, FeSO
4Add-on make alkaline uranium-containing waste water pH be controlled at 7.0~9.0;
(c) remove radium:
In the alkaline uranium-bearing slurry of step (b) gained, add BaCl
2Carry out co-precipitation and remove radium, BaCl
2Add-on is controlled at 20~60g/m
3
(d) circulation ageing:
Alkaline uranium-bearing slurry to step (c) gained carries out ageing, 20~30 ℃ of ageing temperature, digestion time 16~22h; Ageing gained alkalescence uranium-bearing slurry returns in the step (b), carries out neutralization reaction with filtrating;
Through 5~10 circulation ageings, the alkaline uranium-bearing slurry of last gained is filtered, obtain filtrating and filter residue, this filtrating uranium content is reduced to below the 0.05mg/L, and radium content is reduced to below the 1.1Bq/L, can realize discharged wastewater met the national standard.
2. a kind of alkaline uranium-containing waste water treatment process according to claim 1 is characterized in that: described Ca (OH)
2Through the digestion of unslaked lime water is processed.
3. a kind of alkaline uranium-containing waste water treatment process according to claim 1 is characterized in that: in the step (a), and Ca (OH)
2The molar weight that adds is CO in the alkaline uranium-containing waste water
3 2-And HCO
3 -1.1~1.3 times of molar weight sum, 20~30 ℃ of temperature of reaction, 0.5~2 hour reaction times.
4. want 1 described a kind of alkaline uranium-containing waste water treatment process according to right, it is characterized in that: step (b) adopts pneumatic blending to add FeSO
4, 20~30 ℃ of neutralization reaction temperature, neutralization reaction time 1~3h.
5. a kind of alkaline uranium-containing waste water treatment process according to claim 1 is characterized in that: BaCl in the step (c)
2The molar weight that adds is SO
4 2-5 ‰ of molar weight~15 ‰, 20~30 ℃ of temperature of reaction, reaction times 1~3h.
6. a kind of alkaline uranium-containing waste water treatment process according to claim 1 is characterized in that: CO in the described alkaline uranium-containing waste water
3 2-Content is 3.5~12.0gL
-1HCO
3 -Content is 2.0~3.0gL
-1PH value 9.0~10.5, uranium content 1.0~10.0mgL
-1Radium content 10~40BqL
-1
7. a kind of alkaline uranium-containing waste water treatment process according to claim 1 is characterized in that: in the step (b), if HCO in the waste water
3 -Content is more is transferred to 7 with waste water ph, CO in waste water
3 2-Content is more is transferred to 9 with waste water ph.
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