CN108911102A - A kind of method that high-efficiency electrochemical restores uranium in enriching and recovering uranium-containing waste water and underground water - Google Patents
A kind of method that high-efficiency electrochemical restores uranium in enriching and recovering uranium-containing waste water and underground water Download PDFInfo
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- CN108911102A CN108911102A CN201810765731.3A CN201810765731A CN108911102A CN 108911102 A CN108911102 A CN 108911102A CN 201810765731 A CN201810765731 A CN 201810765731A CN 108911102 A CN108911102 A CN 108911102A
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/70—Treatment of water, waste water, or sewage by reduction
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/006—Radioactive compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
Abstract
The invention discloses the methods of uranium in a kind of high-efficiency electrochemical reduction enriching and recovering uranium-containing waste water and underground water.The present invention constructs electrochemical system using metal electrode as anode and cathode, the property that electronics is reduced to the insoluble uranium dioxide of tetravalence can be obtained using sexavalence uranyl ion, without outer source additive, hexavalent uranium is reduced to by uranium dioxide by electrode and is enriched in electrode surface.The hexavalent uranium that uranous coating can be further catalyzed in reducing waste water forms new uranous coating.After the completion of electrochemical reduction enrichment, the electrode for being enriched with uranium dioxide is taken out from solution, the efficient reduction removal of uranium in waste water and underground water can be realized.It is aoxidized by further putting the electrodes into dilute nitric acid solution, the high efficiente callback that can be further realized.The present invention has a wide range of application, and efficiently removal and recycling can be achieved to uranyl carbonate in low concentration, high concentration uranium-containing waste water and underground water containing carbonate.
Description
Technical field
The invention belongs to field of waste water treatment, it is related to a kind of high-efficiency electrochemical reduction enriching and recovering uranium-containing waste water and underground water
The method of middle uranium.
Background technique
With the exploitation of uranium ore and being widely used for nuclear energy, the uranium pollution situation in global range is got worse.Uranium is made
Heavy metal toxicity and radioactive pollutant are had both for one kind, the migration in water environment causes ecological environment and human health
Great threat.Uranium content has been well beyond the drinking water of the World Health Organization in the earth's surface or underground water of many countries
Standard (30 μ g/L), if part uranium mining area Uranium in Waste Water is at concentrations up to 50mg/L.The effective uranium pollution control technology of exploiting economy
It is the key that solve uranium pollution.Meanwhile with the increase of global nuclear power source demand, the demand of uranium member is also increasing, needs
Develop efficient uranium enriching and recovering technology.Therefore, the uranium in removal uranium-containing waste water and the synchronous recovery process for realizing uranium are established,
Uranium contamination control and two aspect of resource reclaim all have very important significance.
The method of reported uranium removal mainly has absorption method, chemical precipitation method, ion-exchange and membrane technology at this stage
Method etc..Absorption method is by way of adding adsorbent, using chemical coordination effect or physical absorption by uranium absorption at attached dose
Surface.It is undesirable to the treatment effect of the uranium-containing waste water of high concentration since absorption method processing capacity is limited, and in underground water
The uranium of complex status, such as uranyl carbonate treatment effeciency are very low；Further, since there are adsorption equilibriums for adsorbent, for low dense
The uranium-containing waste water system treatment effeciency of degree is lower.Chemical precipitation method is by addition flocculant and flocculation aid, by uranium from water environment
In be fixed up in the form of precipitating, but this method is bad for the uranium of complex state, such as uranyl carbonate treatment effect, and big
The flocculant and waste residue of amount will also result in secondary pollution.Ion-exchange is similar with absorption method, passes through addition ion-exchanger
Mode is enriched with uranium, but the treatment effect of ion-exchange is limited by ion concentration competitive in water body environment.Film
Partition method is the method penetrated using selectivity of the film to uranium, there is a problem of separation difficulty, and film for the uranium of complex state
It easily causes obstruction that processing capacity is caused to decline by the Assessment of Organic Pollution in water, is unfavorable for large-scale application.
Electrochemical method is with its rapid reaction, controllability is strong, the advantages such as easy to operate, has obtained extensively in contamination control field
General application.There are mainly two types of the methods for the electrochemical system removal uranium announced at this stage：A kind of method is generation in situ
It is co-deposited agent, such as using electric flocculation technique, so that iron anode is generated the uranium progress in free ferrous ion and water body coprecipitated
Product；Another method is artificial addition complexing agent, mainly adds the organic molecule of some short chains, is generated in anodic oxidation small
The low price uranium that molecule intermediate can be generated with cathodic reduction forms complex-precipitation, is deposited on electrode surface.Both the above method
It is substantially to be improved to chemical deposition, and the introducing of electrode system is only to facilitate this process.
Summary of the invention
The object of the present invention is to provide the sides of uranium in a kind of high-efficiency electrochemical reduction enriching and recovering uranium-containing waste water and underground water
Method.
The enrichment method of uranium, the enrichment include in a kind of claimed uranium-containing waste water and/or underground water：
It is higher than the uranium-containing waste water and/or underground water of 2mg/L for uranic concentration, it is high with stable and electrically conductive property
Metal material carries out electroreduction as cathode and anode material, using DC power supply, is enriched with to obtain uranous in cathode surface；
It is less than or equal to the uranium-containing waste water and/or underground water of 2mg/L for uranic concentration, is covered with surface
The high metal electrode of the stable and electrically conductive property of uranium dioxide coating is as cathode material, with the high metal material of stable and electrically conductive property
As anode material, electroreduction is carried out using DC power supply, is enriched with to obtain uranous in cathode surface, completes the uranium-containing waste water
And/or in underground water uranium enrichment.
In the above method, the high metal material of the stable and electrically conductive property is titanium sheet or stainless steel substrates.
The voltage of the DC power supply is 2-5V；
In the electroreduction step, temperature is room temperature；Time is 0.5-15h.
The metal electrode that the surface is covered with uranium dioxide coating is made according to the method included the following steps：
Described to contain in uranium solution, uranic concentration is higher than 2mg/L；Specially 20-100mg/L；；More specifically 55mg/
L。
In the reduction step, temperature is room temperature；Time is 0.5-20 hours；Specially 15 hours；PH value is 2-10.
A kind of recovery method of uranium in uranium-containing waste water and underground water is also claimed in the present invention, and this method includes：
There is uranous cathode to be placed in recovered liquid surface enrichment obtained by aforementioned enrichment method and carry out oxid-reclamatiom, reacts
It finishes and completes the uranous recycling.
In the above method, the recovered liquid is dust technology；The mass percentage concentration of the dust technology is 5-40%；Specially
20%.
In the oxid-reclamatiom step, the time is 0.5-5 hours；Specially 2 hours；Temperature is room temperature.
This method is suitable for various low concentrations and the uranic uranium-containing waste water of high concentration and various low concentrations and high concentration
Uranic enrichment and recycling containing uranium in carbonate underground water.
A kind of method that enrichment and the recycling of uranium in uranium-containing waste water and underground water is also claimed in the present invention.This method packet
It includes：The step of the step of aforementioned enrichment method and recovery method.
Electronics, which can be obtained, the present invention is based on existing sexavalence uranyl ions a large amount of in water body environment is reduced to tetravalence not
Hexavalent uranium is reduced to uranium dioxide simultaneously by electrode without outer source additive by the property of soluble uranium dioxide
It is enriched in electrode surface.After the completion of electrochemical reduction enrichment, the electrode for being enriched with uranium dioxide is taken out from solution, can be realized
The efficient reduction removal of uranium in waste water and underground water.It is aoxidized by further putting the electrodes into dilute nitric acid solution, it can be further
Realize the high efficiente callback of uranium.In addition electrode surface restore the uranium dioxide coating to be formed electrochemical reduction is not caused it is unfavorable
It influences, on the contrary, the uranium dioxide coating formed has suction-operated to hexavalent uranium, results in batch process with titanium dioxide
The accumulation of uranium coating, it is higher and higher that electrode restores removal efficiency.Therefore, the electrode for generating uranium dioxide coating, which can be repeated several times, to be made
With without influencing removal effect.Using this feature, this method can be realized low concentration, high concentration uranium-containing waste water and contain carbonic acid
Uranic removal and recycling in salt underground water.
The principle of the present invention：
According to calculation of thermodynamics, in uranium-bearing solution system, when the external world applies certain potentials, cathode can be by solubilised state
Hexavalent uranium is reduced to insoluble uranous (uranium dioxide), and the uranium dioxide for restoring generation can be deposited on electricity in the form of coating
Electrode is taken out the uranium that can be removed in solution by pole surface after the completion of reduction.
Generating uranium dioxide coating has catalytic action to electrochemical reduction hexavalent uranium, can greatly accelerate sequential reduction mistake
Journey generates more uranium dioxide coating.Therefore, electrode has great reduction capacity in this method.
Since uranium dioxide coating has catalytic action to electrochemical reduction hexavalent uranium, existing uranium dioxide coating is utilized
The quick reduction removal of extremely low concentration uranium may be implemented as cathode for electrode.
Hexavalent uranium is oxidized in uranium dioxide the being oxidized easily property substance that electrode surface is formed.After reduction enriched uranium
Electrode is put into 20% nitric acid the quick recycling, it can be achieved that uranium.Meanwhile the electrode recycled after uranium can reuse.
The invention has the advantages that：
1, the efficient quick removal and recycling of the achievable Uranium in Waste Water of the present invention, without carrying out, net is caught and deposit is located again
The complex steps such as reason, it is simple to operate, it is at low cost, it is without secondary pollution, and electrode can be long-term without treatment processes such as sintering
Recycling.
2, have a wide range of application, the present invention is useless to low concentration (0.02mg/L-2mg/L) and high concentration (being greater than 2mg/L) uranium-bearing
Water all has preferable removal and recovering effect.
3, carbonate is usually contained in underground water, forms stable uranyl carbonate complex compound, traditional absorption with hexavalent uranium
The methods of be difficult to remove the uranyl carbonate complex compound.The present invention has preferable removal effect to uranium in the underground water containing carbonate
Fruit.
4, pH of the present invention is applied widely, for pH within the scope of 2-10 waste water, without adjusting initial pH value.Due to titanium sheet
Sufficiently stable, no replacement is required anode material, entire treatment process is without secondary pollution, and operating condition is convenient, and normal temperature and pressure can be real
It is existing.
5, the uranium coating of electrode surface reduction enrichment will not only inhibit the further reduction of uranium, can be catalyzed acceleration uranium instead
Recycling so that the technology have huge uranium reduction removal capacity.
Specific embodiment
The present invention is further elaborated combined with specific embodiments below, but the present invention is not limited to following embodiments.Institute
State method is conventional method unless otherwise instructed.The raw material can obtain unless otherwise instructed from public commercial source.
Embodiment 1, certain high concentration uranium-containing waste water
100ml uranium-containing waste water (U (VI) concentration is 55mg/L, pH value 7.5) is added to reaction tank, using titanium plate as yin
Anode carries out electroreduction under the conditions of the DC power supply of 2V or so and removes uranium.Under normal temperature and pressure conditions after electroreduction 8 hours, water body
The concentration of middle uranium is down to 0.07mg/L, and the removal efficiency of uranium reaches 99.9%.After electrode is used continuously five times, titanium plate surface is big
Deposit covering is measured, the removal efficiency of uranium does not reduce.It will be placed in 20% nitric acid solution of electrode investment 100mL at normal temperature
After 2 hours, titanium plate electrode surface restores silvery white, and the uranium rate of recovery of electrode surface reaches 99.9%.
Embodiment 2, certain high concentration, high-carbon hydrochlorate uranium-containing waste water
By 100ml high concentration, high-carbon hydrochlorate uranium-containing waste water (U (VI) concentration be 50mg/L, carbonate concentration is about 30mM,
PH value is 7.5) to be added to reaction tank, using titanium plate as anode and cathode, carries out electroreduction under the conditions of the DC power supply of 2V or so and removes
Uranium.Under normal temperature and pressure conditions after electroreduction 15 hours, the concentration of uranium is down to 0.02mg/L in water body, and the removal efficiency of uranium reaches
99.9%.After electrode is used continuously five times, titanium plate surface is covered by a large amount of deposits, and the removal efficiency of uranium does not reduce.Normal
After placing 2 hours in 20% nitric acid solution of electrode investment 100mL under temperature, titanium plate electrode surface restores silvery white, electrode table
The uranium rate of recovery in face reaches 99.9%.
Embodiment 3, certain low concentration uranium-bearing wastewater
High concentration first is added containing (U (VI) concentration is 55mg/L) under normal temperature and pressure conditions in uranium solution in titanium electrode
After carrying out electroreduction 15 hours, the titanium mesh electrode for being covered with uranium dioxide coating is obtained and as cathode.By 100ml
Low concentration uranium-bearing wastewater (U (VI) concentration is 0.1mg/L, and carbonate concentration is about 30mM, pH value 7.5) is added to reaction tank,
Using the titanium mesh with uranium dioxide coating as cathode, the clean titanium mesh in surface makees anode, in the straight of 2.5V or so
Electroreduction is carried out under the conditions of galvanic electricity source removes uranium.Under normal temperature and pressure conditions after electroreduction 13 hours, the concentration of uranium is down in water body
The removal efficiency of 0.001mg/L, uranium reach 99.9%.After electrode is used continuously five times, the removal efficiency of uranium is not reduced.Normal
After placing 2 hours in 20% nitric acid solution of electrode investment 100mL under temperature, titanium plate electrode surface restores silvery white, electrode table
The rate of recovery of face uranium reaches 99.9%.
Claims (9)
1. the enrichment method of uranium in a kind of uranium-containing waste water and/or underground water, including：
It is higher than the uranium-containing waste water and/or underground water of 2mg/L, for uranic concentration with the high metal of stable and electrically conductive property
Material carries out electroreduction as cathode and anode material, using DC power supply, is enriched with to obtain uranous in cathode surface；
It is less than or equal to the uranium-containing waste water and/or underground water of 2mg/L for uranic concentration, dioxy is covered with surface
Change the high metal electrode of stable and electrically conductive property of uranium coating as cathode material, the metal material high using stable and electrically conductive property as
Anode material, using DC power supply carry out electroreduction, be enriched with to obtain uranous in cathode surface, complete the uranium-containing waste water and/
Or in underground water uranium enrichment.
2. according to the method described in claim 1, it is characterized in that：The high material of the stable and electrically conductive property is titanium sheet or stainless
Steel disc.
3. method according to claim 1 or 2, it is characterised in that：The voltage of the DC power supply is 2-5V；
In the electroreduction step, temperature is room temperature；Time is 0.5-20h.
4. method according to claim 1 to 3, it is characterised in that：The surface is covered with uranium dioxide coating
Metal electrode is made according to the method included the following steps：
The high metal material of the stable and electrically conductive property is restored in containing uranium solution；It is described to contain in uranium solution, it is uranic dense
Degree is higher than 2mg/L；Specially 20-100mg/L；More specifically 55mg/L.
5. according to the method described in claim 4, it is characterized in that：In the reduction step, temperature is room temperature；Time is 1-20
Hour；Specially 15 hours.
6. the recovery method of uranium in a kind of uranium-containing waste water and underground water, including：
There is uranous cathode to be placed in recovered liquid surface enrichment obtained by any the method for claim 1-5 to aoxidize back
It receives, end of reaction completes the uranous recycling.
7. according to the method described in claim 6, it is characterized in that：The recovered liquid is dust technology；The quality of the dust technology
Percentage concentration is 5-40%；Specially 20%.
8. method according to claim 6 or 7, it is characterised in that：In the oxid-reclamatiom step, the time is that 0.5-5 is small
When；Temperature is room temperature.
9. a kind of method of enrichment and the recycling of uranium in uranium-containing waste water and underground water, including：Any side in claim 1-5
In the step of method and claim 2-8 the step of any the method.
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| CN201810765731.3A CN108911102B (en) | 2018-07-12 | 2018-07-12 | Method for recycling uranium in uranium-containing wastewater and underground water through efficient electrochemical reduction and enrichment |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109867333A (en) * | 2019-04-01 | 2019-06-11 | 中国科学院生态环境研究中心 | The method with uranium in recycle-water is efficiently removed using titanium-based titanium dioxide nanotube array electrode |
| CN109942076A (en) * | 2019-04-01 | 2019-06-28 | 中国科学院生态环境研究中心 | Utilize the method for uranium in microbiological fuel cell removal-recycle-water and synchronous electrogenesis |
| CN109972173A (en) * | 2019-05-09 | 2019-07-05 | 东华理工大学 | A kind of modification NZVI three-dimensional electrochemical method based on solar energy recycles the device of uranium in nuclear waste water |
| CN113089016A (en) * | 2021-03-10 | 2021-07-09 | 西南科技大学 | Preparation method of high-performance single-center uranium-based supported catalyst |
| CN113707351A (en) * | 2020-11-24 | 2021-11-26 | 核工业北京化工冶金研究院 | Static uranium removing method for sponge iron filter material |
| CN113880234A (en) * | 2021-10-14 | 2022-01-04 | 中国科学院生态环境研究中心 | Method for continuously and efficiently removing and recycling uranium in water by using microbial electrolysis cell |
| CN114031157A (en) * | 2021-11-18 | 2022-02-11 | 中国科学院生态环境研究中心 | Method for removing and recycling heavy metals in water by using porous three-dimensional wood-based electrode |
| CN114214635A (en) * | 2021-11-29 | 2022-03-22 | 哈尔滨工程大学 | Method for efficiently preparing uranium dioxide by adopting electrodeposition |
| CN114380361A (en) * | 2021-12-10 | 2022-04-22 | 中国科学院生态环境研究中心 | Method for recovering uranium from uranium-containing wastewater and underground water through electrochemical reduction and enrichment in coexistence of nitrates |
| CN116282176A (en) * | 2022-09-09 | 2023-06-23 | 哈尔滨工程大学 | Method for directly recovering high-purity uranium oxide from uranium-containing wastewater |
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| CN109942076A (en) * | 2019-04-01 | 2019-06-28 | 中国科学院生态环境研究中心 | Utilize the method for uranium in microbiological fuel cell removal-recycle-water and synchronous electrogenesis |
| CN109942076B (en) * | 2019-04-01 | 2020-08-28 | 中国科学院生态环境研究中心 | Method for removing and recycling uranium in water and synchronously generating electricity by utilizing microbial fuel cell |
| CN109867333A (en) * | 2019-04-01 | 2019-06-11 | 中国科学院生态环境研究中心 | The method with uranium in recycle-water is efficiently removed using titanium-based titanium dioxide nanotube array electrode |
| CN109972173B (en) * | 2019-05-09 | 2024-02-27 | 东华理工大学 | Device for recycling uranium in nuclear wastewater by using solar-based modified NZVI three-dimensional electrochemical method |
| CN109972173A (en) * | 2019-05-09 | 2019-07-05 | 东华理工大学 | A kind of modification NZVI three-dimensional electrochemical method based on solar energy recycles the device of uranium in nuclear waste water |
| CN113707351A (en) * | 2020-11-24 | 2021-11-26 | 核工业北京化工冶金研究院 | Static uranium removing method for sponge iron filter material |
| CN113089016A (en) * | 2021-03-10 | 2021-07-09 | 西南科技大学 | Preparation method of high-performance single-center uranium-based supported catalyst |
| CN113880234A (en) * | 2021-10-14 | 2022-01-04 | 中国科学院生态环境研究中心 | Method for continuously and efficiently removing and recycling uranium in water by using microbial electrolysis cell |
| CN113880234B (en) * | 2021-10-14 | 2023-10-20 | 中国科学院生态环境研究中心 | Microbial electrolysis method for continuously and efficiently removing and recycling uranium in water |
| CN114031157A (en) * | 2021-11-18 | 2022-02-11 | 中国科学院生态环境研究中心 | Method for removing and recycling heavy metals in water by using porous three-dimensional wood-based electrode |
| CN114214635A (en) * | 2021-11-29 | 2022-03-22 | 哈尔滨工程大学 | Method for efficiently preparing uranium dioxide by adopting electrodeposition |
| CN114380361A (en) * | 2021-12-10 | 2022-04-22 | 中国科学院生态环境研究中心 | Method for recovering uranium from uranium-containing wastewater and underground water through electrochemical reduction and enrichment in coexistence of nitrates |
| CN116282176A (en) * | 2022-09-09 | 2023-06-23 | 哈尔滨工程大学 | Method for directly recovering high-purity uranium oxide from uranium-containing wastewater |
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