CN107245588B - A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid - Google Patents
A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid Download PDFInfo
- Publication number
- CN107245588B CN107245588B CN201710259170.5A CN201710259170A CN107245588B CN 107245588 B CN107245588 B CN 107245588B CN 201710259170 A CN201710259170 A CN 201710259170A CN 107245588 B CN107245588 B CN 107245588B
- Authority
- CN
- China
- Prior art keywords
- neptunium
- extraction
- organic
- phase
- stripped
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Active
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
- C22B60/02—Obtaining thorium, uranium, or other actinides
- C22B60/0204—Obtaining thorium, uranium, or other actinides obtaining uranium
- C22B60/0217—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes
- C22B60/0252—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries
- C22B60/026—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries liquid-liquid extraction with or without dissolution in organic solvents
Landscapes
- Life Sciences & Earth Sciences (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Geology (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Extraction Or Liquid Replacement (AREA)
Abstract
The invention belongs to nuclear waste transmutation recovery technology fields, are related to a kind of method of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid.The method includes the steps that following optional, replaceable sequence and repeats, and finally collect water phase and be stripped object: (1) neptunium in the aqueous phase solution containing neptunium being oxidized to sexavalence with oxidant, and the organic solvent containing methylphosphonic acid two (1- first heptan) ester is added under strongly acidic conditions and is extracted；It collects and organic is added to reducing agent, it is stripped under the conditions of dilute acidic, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase, (2) neptunium in the aqueous phase solution containing neptunium is reduced to tetravalence with reducing agent, and the organic solvent containing methylphosphonic acid two (1- first heptan) ester is added under strongly acidic conditions and is extracted；Organic phase is collected, is stripped under the conditions of dilute acidic, the neptunium back extraction of tetravalence in organic phase is entered into water phase.Utilize the neptunium nitrate solution up to standard method of the invention, it is possible to obtained purity.
Description
Technical field
The invention belongs to nuclear waste transmutation recovery technology fields, are related to a kind of extraction and recovery from spentnuclear fuel post-processing waste liquid
The method of neptunium.
Background technique
Contain a certain amount of neptunium, content different, burnup according to the burnup difference of spentnuclear fuel in the spentnuclear fuel of power reactor of nuclear power plant
- 237 content of neptunium is about 500-600g/tU in spentnuclear fuel in 33000.Spentnuclear fuel mainly recycled in last handling process plutonium and
Uranium, neptunium -237 stay in radioactive liquid waste.If the neptunium -237 stayed in radioactive liquid waste does not extract, then can enter solid
Change body.The migration in solidified body of neptunium -237 is strong, is unfavorable for the safety in geological disposal library.Meanwhile neptunium -237 can be used as raw material warp
Irradiation is converted to plutonium -238, becomes the important isotope material of space power and heat source.Therefore neptunium -237 from Spent Radioactive
It is extracted in liquid, security risk caused by -237 migration of neptunium is strong when on the one hand can be reduced waste processing；On the other hand it extracts
Neptunium -237 out can be used as the important source material for preparing plutonium -238.Therefore, neptunium is extracted from spentnuclear fuel reprocessing plant waste liquid
To have great significance.
However, neptunium is recycled without separation and Extraction to recycle uranium, plutonium as the spentnuclear fuel reprocessing plant of target, mainly all into
Enter reprocessing plant high activity liquid waste and in put it is buried after wastewater treatment.The high activity liquid waste and intermediate level liquid waste of spentnuclear fuel reprocessing plant are main
It is the aqueous solution of nitric acid of 2-3mol/L, wherein the ingredient for also thering is a certain amount of last handling process to introduce, such as sodium, zirconium, fission product
Element, the remaining uranium of extraction, plutonium and other actinides such as neptunium, americium, curium etc..Therefore, it to be put in radioactivity, complicated component
Neptunium -237 is isolated and purified in penetrating property waste liquid and is extracted with certain technical difficulty.
The United States, Russia, English, method, day etc., the process that neptunium -237 is extracted in spentnuclear fuel reprocessing plant was studied by country, realized
The extraction recycling of neptunium -237 is carried out from high activity liquid waste and intermediate level liquid waste in spentnuclear fuel reprocessing plant.The side of neptunium is extracted in high activity liquid waste
Method is general are as follows: in spentnuclear fuel reprocessing plant codecontamination separative unit, try to catch up with neptunium in high activity liquid waste (1AW), then from
Neptunium is extracted in high activity liquid waste.Typically extracting the external producer of neptunium with this method includes the U.S. Sa Fanna He Chang and Xi Guchang, Britain
Wen Cikaier factory etc..Another kind extracts the conventional method of neptunium in intermediate level liquid waste are as follows: in the codecontamination of spentnuclear fuel reprocessing plant
In separative unit, uranium, neptunium, plutonium are extracted jointly and fed them into organic phase (1AP), subsequent so that neptunium is entered radioactivity lower useless
Separation and Extraction in liquid.It typically include the Chinese Ford factory and Midwest factory, France in the U.S. with the external producer that this method extracts neptunium
Ma Kuer factory and A Gechang, the RT-1 factory of Russia, the factory, East Sea village of Japan etc..
The technique that spentnuclear fuel reprocessing plant extracts neptunium in the world mainly has ion-exchange and solvent extraction.Ion exchange
The principle of method is to realize to divide using difference of the ion exchange resin to the adsorption capacity between neptunium and other actinides, fission product
From.One of method is under given conditions, neptunium -237 to be allowed to be adsorbed on ion exchange column, elutes fission using detergent and produces
The other elements such as matter-element element, uranium plutonium and then neptunium is eluted.It is required according to the decontamination of -237 pairs of other elements of neptunium, it may
Need progress duplicate operation for the second time or for the third time also to further increase the purity of neptunium -237.
It is using organic extractant to not that solvent extraction extracts the principle of neptunium -237 from spentnuclear fuel reprocessing plant waste liquid
Neptunium from waste liquid is isolated and purified out by the difference with the neptunium of valence state, plutonium and fission product extracting power.Publication No.
103305702A, entitled " recycled in a kind of 2AW+2DW intermediate level liquid waste from Purex flow and the technique of purifying neptunium "
Chinese patent application, which is disclosed, extracts process using the neptunium that tributyl phosphate (TBP) is extractant.This method is in certain condition
Under, spy higher to Np (IV, VI) distribution coefficient using TBP, low to Np (V), Pu (III), fission product distribution coefficient
Property, it can be achieved that uranium, neptunium, plutonium extraction and recovery, and separated with fission product.But 30%TBP- diluent organic extractant phase is deposited
In a problem, i.e. 30%TBP- diluent organic phase extracts distribution coefficient in the higher situation of acidity to tetravalent neptunium and is also only
1-2 needs to be designed as multitple extraction there are under strong salting out in highly acidity (4mol/L or more nitric acid), high salt concentration,
Can guarantee has enough extraction yields to tetravalent neptunium.In this way when extracting tetravalent neptunium, needs using higher concentration of nitric acid or add
Enter many salinities, this is totally unfavorable for the generation for reducing radioactive waste.
Methylphosphonic acid two (1- first heptan) ester is a kind of neutral organophosphine extractant, code name P350, and structural formula is as follows:
Summary of the invention
The object of the present invention is to provide a kind of methods of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid, can pass through
Extraction and back extraction circulation, efficiently make neptunium and other impurities, such as plutonium, uranium, fission product element technetium, strontium, caesium separation are simultaneously
Neptunium is concentrated, purity neptunium nitrate solution up to standard is made.
In order to achieve this, the present invention provides a kind of post-process in waste liquid from spentnuclear fuel and extracts in the embodiment on basis
The method for taking neptunium recovery, the method include the steps that following optional, replaceable sequence and repeatable (step (1), step
(2) optionally one or both includes；Step (1), the sequence of step (2) are variable；Step (1), step (2) are repeatable more
It is secondary), and finally collect water phase and be stripped object:
(1) neptunium in the aqueous phase solution containing neptunium is oxidized to sexavalence with oxidant, and is added contains first under strongly acidic conditions
The organic solvent of base phosphonic acids two (1- first heptan) ester is extracted；Collect it is organic be added to reducing agent, carried out under the conditions of dilute acidic
Back extraction, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase,
(2) neptunium in the aqueous phase solution containing neptunium is reduced to tetravalence with reducing agent, and is added contains first under strongly acidic conditions
The organic solvent of base phosphonic acids two (1- first heptan) ester is extracted；Organic phase is collected, is stripped under the conditions of dilute acidic, it will
The neptunium back extraction of tetravalence enters water phase in organic phase.
The countercurrent extraction equipments such as multistage mixer-settler, pulse extraction column can be used in above-mentioned extraction and back extraction process.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method wherein the method in turn includes the following steps, and finally collects water phase and is stripped object:
(1) neptunium in the aqueous phase solution (spentnuclear fuel post-processing waste liquid) containing neptunium is oxidized to sexavalence with oxidant, and strong
The organic solvent containing methylphosphonic acid two (1- first heptan) ester is added under acid condition to be extracted；Collect it is organic be added to reducing agent,
It is stripped under the conditions of dilute acidic, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase,
(2) neptunium in the aqueous phase solution containing neptunium is reduced to tetravalence with reducing agent, and is added contains first under strongly acidic conditions
The organic solvent of base phosphonic acids two (1- first heptan) ester is extracted；Organic phase is collected, is stripped under the conditions of dilute acidic, it will
The neptunium back extraction of tetravalence enters water phase in organic phase.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method wherein the method in turn includes the following steps, and finally collects water phase and is stripped object:
(1) neptunium in the aqueous phase solution (spentnuclear fuel post-processing waste liquid) containing neptunium is reduced to tetravalence with reducing agent, and strong
The organic solvent containing methylphosphonic acid two (1- first heptan) ester is added under acid condition to be extracted；Organic phase is collected, in dilute acidic item
It is stripped under part, the neptunium back extraction of tetravalence in organic phase is entered into water phase,
(2) neptunium in the aqueous phase solution containing neptunium is oxidized to sexavalence with oxidant, and is added contains first under strongly acidic conditions
The organic solvent of base phosphonic acids two (1- first heptan) ester is extracted；Collect it is organic be added to reducing agent, carried out under the conditions of dilute acidic
Back extraction, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein oxidant described in step (1) is sodium metavanadate, ammonium metavanadate, potassium permanganate.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein the concentration of oxidant described in step (1) is 0.05-0.5mol/L.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein the concentration of the acid of strong acidic condition described in step (1) and step (2) is 2-8mol/L.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein the organic solvent containing methylphosphonic acid two (1- first heptan) ester described in step (1) and step (2) is methylphosphonic acid two
The mixture of (1- first heptan) ester and inert diluent, the inert diluent are selected from kerosene, n-dodecane.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, the volume hundred of (1- first heptan) ester wherein methylphosphonic acid two in the described organic solvent containing methylphosphonic acid two (1- first heptan) ester
Dividing than content is 5-50%.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein reducing agent described in step (1) is hydrazine and/or methyl hydrazine, and reducing agent described in step (2) is that nitric acid is sub-
Iron.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein the concentration of reducing agent described in step (1) be 0.05-1.0mol/L, reducing agent described in step (2) it is dense
Degree is 0.1-1.0mol/L.
In a preferred embodiment, the present invention provides a kind of extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid
Method, wherein the concentration of the acid of dilute acidic condition described in step (1) and step (2) is 0.10-0.40mol/L.
The beneficial effects of the present invention are utilize the side of the extraction and recovery neptunium of the invention from spentnuclear fuel post-processing waste liquid
Method, can by extraction and back extraction circulation, efficiently make neptunium and other impurities, as plutonium, uranium, fission product element technetium, strontium,
Caesium etc. separates and neptunium is concentrated, and purity neptunium nitrate solution up to standard is made.
Detailed description of the invention
Fig. 1 is the illustrative flow chart of the invention that the method for extraction and recovery neptunium in waste liquid is post-processed from spentnuclear fuel.
Fig. 2 is that illustrative of the invention post-process in waste liquid from spentnuclear fuel extracts for the first time in the method for extraction and recovery neptunium
The flow chart for taking-being stripped.
Fig. 3 is that illustrative of the invention post-process in waste liquid from spentnuclear fuel extracts for the second time in the method for extraction and recovery neptunium
The flow chart for taking-being stripped.
Specific embodiment
A specific embodiment of the invention is further illustrated with attached drawing with reference to embodiments.
Research of the embodiment 1:P350 to the extracting power and reducing agent of neptunium to the reducing power of neptunium
By the study found that P350 is more much higher than tributyl phosphate to the extracting power of sexavalence neptunium, tetravalent neptunium.It is specific next
It says, when concentration of nitric acid is 3mol/L in water phase neptunium solution, when neptunium concentration is 0.05g/L, respectively with 5% (v/v) P350- diluent
Extraction system and 5% (v/v) TBP- diluent extraction system aqueous phase extracted (being comparably 1: 1, extraction time is 5 minutes), and
The water phase of certain volume and the concentration of organic phase alpha energy spectrum method measurement wherein neptunium are taken after extraction respectively.A certain valence state in organic phase
Neptunium concentration and water phase in correspond to the ratio between concentration of neptunium of the valence state i.e. distribution coefficient of the valence state neptunium.Using single valence neptunium point
Extraction distribution experiment is not carried out, and experiment show that 5% (v/v) P350- diluent extraction system extracts than 5% (v/v) TBP- diluent
The high 1-2 magnitude of system distribution coefficient is taken, 5% (v/v) P350-Np (IV), Np (VI) distribution coefficient are respectively 5.5,10.6, and
5% (v/v) TBP-Np (IV), Np (VI) distribution coefficient are respectively 0.2,0.9.The distribution coefficient of 5% (v/v) P350-Np (V) is
0.1。
Different using reduction effect of the different reducing agents to neptunium with plutonium, final choice reduction Np (VI) is fast to Np (V) speed,
And Pu (IV) to Pu (III) slow hydrazine and its derivative is restored as reducing agent, specific reducing agent performance is as shown in table 1.
1 hydrazine of table and methyl hydrazine restore neptunium (VI) and Pu (IV) Speedometer Drive
Note: (1) 1mol/L HNO3Medium
(2)3mol/L HNO3Medium
k′NpThe observed rate constant of neptunium (Np (VI) reverts to Np (V)) is restored for reducing agent；
k′puThe observed rate constant of plutonium (Pu (IV) reverts to Pu (III)) is restored for reducing agent；
k′Np/k′PuFor k 'NpWith k 'PuThe ratio between；
t99The Np (VI) that-Np (VI) is 99% reverts to the time required for Np (V).
Based on above the study found that being extraction the invention proposes P350 is used from nuclear fuel reprocessing plant's radioactive liquid waste
The process flow of agent extraction and recovery purifying neptunium is taken, as shown in Figure 1.
Embodiment 2: pass through the method (one) of extraction and back extraction process neptunium recovery twice from spentnuclear fuel post-processing waste liquid
Experimental stand is installed in glove box, extraction and recovery is carried out to the neptunium in spentnuclear fuel reprocessing plant waste liquid.
First time, extraction and back extraction process was as shown in Fig. 2, processing step are as follows:
(1) sodium metavanadate will be used as oxidant condiment after spentnuclear fuel reprocessing plant waste liquid is concentrated by evaporation, 15mol/L's
HNO3Adjusting acidity is 4mol/L, obtains feed liquid 2NAF to be purified.In 2NAF include Np, U, Pu and fission product, Np mainly with
Np (VI) form exists, and Pu mainly exists with Pu (IV).
(2) 2NAF is introduced into 2NA extraction tank, 5% (v/v) P350- kerosene is also introduced in 2NA extraction tank as extractant
2NAX, 3mol/L HNO3It is 2: 1 that stream as detergent 2NAS, 2NAF and 2NAX, which compares,.After extraction greater than 99.9% U, Np,
Pu is extracted jointly enters organic phase 2NAP, and fission product enters water phase 2NAW.
(3) it is introduced into organic phase 2NAP obtained in step (2) as 2NBF in 2NB back extraction slot, 2NB is stripped in slot also
Introduce 0.2mol/L hydrazine -0.3mol/LHNO3As reduction reextraction agent 2NBX, 5% (v/v) P350- kerosene is introduced as benefit extraction agent
2NBS (further extracts uranium, plutonium), and 2NBF and 2NBX stream are than being 2: 1.Np (VI) is reduced to Np by the hydrazine in reduction reextraction agent
(V), it is stripped Np to water phase (2NBP), uranium and plutonium from organic phase to be retained in organic phase (2NBW), realizes the separation of neptunium and uranium plutonium.
Water-phase product 2NBP is neptunium crude product liquid.
Second of extraction and back extraction process is as shown in figure 3, processing step are as follows:
(1) reducing agent (0.1-1.0mol/L Fe (NO is added in 2NBP feed liquid3)2) Np is reduced into tetravalence, Pu reduction
At trivalent, with 5mol/L HNO3Adjusting concentration of nitric acid in 2NBP is 4mol/L, then introduces neptunium for 2NBP as 3NAF feed liquid
Second of extraction and back extraction process 3NA extraction tank in；
(2) 3NAF is introduced into 3NA extraction tank, 5% (v/v) P350- kerosene is also introduced in 3NA extraction tank as extractant
3NAX, 3mol/L HNO3It is 2: 1 that stream as detergent 3NAS, 3NAF and 3NAX, which compares,.It is total greater than 99.9% U, Np after extraction
Enter organic phase 3NAP with extraction, micro Pu and fission product enter water phase 3NAW.
(3) it is introduced into organic phase 3NAP obtained in step (2) as 3NBF in 3NB back extraction slot, 3NB is stripped in slot also
Introduce 0.1mol/LHNO3As stripping agent 3NBX, 5% (v/v) P350- kerosene is introduced as benefit extraction agent 3NBS (further extraction
Uranium, plutonium), 3NBF and 3NBX stream are than being 2:1.In this way, Np is stripped from organic phase (3NBW) to water phase (3NBP).Water-phase product 3NBP
For neptunium product liquid.
Platform experiment the result shows that: total neptunium rate of recovery be greater than 99.5%.
Embodiment 3: pass through the method (two) of extraction and back extraction process neptunium recovery twice from spentnuclear fuel post-processing waste liquid
First time, extraction and back extraction process was as shown in Fig. 2, processing step are as follows:
(1) reducing agent (0.1-1.0mol/LFe (NO is added after being concentrated by evaporation spentnuclear fuel reprocessing plant waste liquid3)2) by Np
It is reduced into tetravalence, Pu is reduced into trivalent, with 5mol/L HNO3Adjusting concentration of nitric acid is 4mol/L, obtains feed liquid 2NAF to be purified.
(2) 2NAF is introduced into 2NA extraction tank, 5% (v/v) P350- kerosene is also introduced in 2NA extraction tank as extractant
2NAX, 3mol/L HNO3It is 2: 1 that stream as detergent 2NAS, 2NAF and 2NAX, which compares,.It is total greater than 99.5% U, Np after extraction
Enter organic phase 2NAP with extraction.
(3) it is introduced into organic phase 2NAP obtained in step (2) as 2NBF in 2NB back extraction slot, 2NB is stripped in slot also
Introduce 0.1mol/LHNO3As stripping agent 2NBX, 5% (v/v) P350- kerosene is introduced as benefit extraction agent 2NBS (further extraction
Uranium, plutonium), 2NBF and 2NBX stream are than being 2: 1.In this way, Np is stripped from organic phase (2NBW) to water phase (2NBP).Water-phase product 2NBP
For neptunium crude product liquid.
Second of extraction and back extraction process is as shown in figure 3, processing step are as follows:
(1) use sodium metavanadate as oxidant condiment, the HNO of 15mol/L water phase 2NBP3Adjusting acidity is 4mol/L,
Np is oxidized to sexavalence in this way, obtains feed liquid 3NAF to be purified, is introduced into the 3NA of second of extraction and back extraction process of neptunium
In extraction tank.
(2) 3NAF is introduced into 3NA extraction tank, 5% (v/v) P350- kerosene is also introduced in 3NA extraction tank as extractant
3NAX, 3mol/L HNO3It is 2: 1 that stream as detergent 3NAS, 3NAF and 3NAX, which compares,.After extraction greater than 99.9% U, Np,
Pu is extracted jointly enters organic phase 3NAP.
(3) it is introduced into organic phase 3NAP obtained in step (2) as 3NBF in 3NB back extraction slot, 3NB is stripped in slot also
Introduce 0.2mol/L hydrazine -0.3mol/LHNO3As reduction reextraction agent 3NBX, 5% (v/v) P350- kerosene is introduced as benefit extraction agent
3NBS (further extracts uranium, plutonium), and 3NBF and 3NBX stream are than being 2: 1.Np (VI) is reduced to Np by the hydrazine in reduction reextraction agent
(V), it is stripped Np to water phase (3NBP), uranium and plutonium from organic phase to be retained in organic phase (3NBW), realizes the separation of neptunium and uranium plutonium.
Water-phase product 3NBP is neptunium product liquid.
Platform experiment the result shows that: the rate of recovery of total neptunium be greater than 99.5%.
Obviously, various changes and modifications can be made to the invention without departing from essence of the invention by those skilled in the art
Mind and range.If in this way, belonging to the model of the claims in the present invention and its equivalent technology to these modifications and changes of the present invention
Within enclosing, then the present invention is also intended to include these modifications and variations.Above-described embodiment or embodiment are only to the present invention
For example, the present invention can also be implemented with other ad hoc fashions or other particular form, without departing from of the invention
Main idea or substantive characteristics.Therefore, the embodiment of description is regarded as illustrative and non-limiting in any way.This
The range of invention should be illustrated that any variation equivalent with the intention and range of claim also should include by appended claims
Within the scope of the invention.
Claims (10)
1. a kind of method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid, which is characterized in that the method includes as follows
Replaceable sequence and repeatable step, and finally collect water phase and be stripped object:
(1) neptunium in the aqueous phase solution containing neptunium is oxidized to sexavalence with oxidant, and is added contains methylphosphine under strongly acidic conditions
The organic solvent of acid two (1- first heptan) ester is extracted；Collect it is organic be added to reducing agent, be stripped under the conditions of dilute acidic
It takes, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase,
(2) neptunium in the aqueous phase solution containing neptunium is reduced to tetravalence with reducing agent, and is added contains methylphosphine under strongly acidic conditions
The organic solvent of acid two (1- first heptan) ester is extracted；Organic phase is collected, is stripped under the conditions of dilute acidic, it will be organic
The neptunium back extraction of tetravalence enters water phase in phase.
2. the method according to claim 1, wherein the method in turn includes the following steps, and finally receiving
Catchment opposite extract:
(1) neptunium in the aqueous phase solution containing neptunium is oxidized to sexavalence with oxidant, and is added contains methylphosphine under strongly acidic conditions
The organic solvent of acid two (1- first heptan) ester is extracted；Collect it is organic be added to reducing agent, be stripped under the conditions of dilute acidic
It takes, as pentavalent and being stripped the neptunium selective reduction of sexavalence in organic phase into water phase,
(2) neptunium in the aqueous phase solution containing neptunium is reduced to tetravalence with reducing agent, and is added contains methylphosphine under strongly acidic conditions
The organic solvent of acid two (1- first heptan) ester is extracted；Organic phase is collected, is stripped under the conditions of dilute acidic, it will be organic
The neptunium back extraction of tetravalence enters water phase in phase.
3. method according to claim 1 or 2, it is characterised in that: oxidant described in step (1) be sodium metavanadate,
Ammonium metavanadate, potassium permanganate.
4. method according to claim 1 or 2, it is characterised in that: the concentration of oxidant described in step (1) is
0.05-0.5mol/L。
5. method according to claim 1 or 2, it is characterised in that: highly acid item described in step (1) and step (2)
The concentration of the acid of part is 2-8mol/L.
6. method according to claim 1 or 2, it is characterised in that: contain methylphosphine described in step (1) and step (2)
The organic solvent of acid two (1- first heptan) ester is the mixture of methylphosphonic acid two (1- first heptan) ester and inert diluent, the inertia
Diluent is selected from kerosene, n-dodecane.
7. method according to claim 1 or 2, it is characterised in that: described to have containing methylphosphonic acid two (1- first heptan) ester
The volume percent content of methylphosphonic acid two in solvent (1- first heptan) ester is 5-50%.
8. method according to claim 1 or 2, it is characterised in that: reducing agent described in step (1) is hydrazine and/or first
Base hydrazine, reducing agent described in step (2) are ferrous nitrate.
9. method according to claim 1 or 2, it is characterised in that: the concentration of reducing agent described in step (1) is
0.05-1.0mol/L, the concentration of reducing agent described in step (2) are 0.1-1.0mol/L.
10. according to the method described in claim 1, it is characterized by: dilute acidic condition described in step (1) and step (2)
Acid concentration be 0.10-0.40mol/L.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201710259170.5A CN107245588B (en) | 2017-04-19 | 2017-04-19 | A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201710259170.5A CN107245588B (en) | 2017-04-19 | 2017-04-19 | A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN107245588A CN107245588A (en) | 2017-10-13 |
| CN107245588B true CN107245588B (en) | 2019-03-12 |
Family
ID=60016556
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201710259170.5A Active CN107245588B (en) | 2017-04-19 | 2017-04-19 | A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN107245588B (en) |
Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110144471B (en) * | 2019-05-15 | 2020-10-09 | 中国原子能科学研究院 | Method for extracting technetium from nuclear fuel post-treatment waste liquid |
| CN110656247B (en) * | 2019-11-05 | 2020-11-10 | 中国原子能科学研究院 | Method for extracting and recovering plutonium from plutonium-containing nitric acid solution |
| CN111020244B (en) * | 2020-01-09 | 2021-03-09 | 中国原子能科学研究院 | Method for extracting plutonium-238 from irradiated neptunium target and recovering neptunium-237 |
| CN111199808B (en) * | 2020-01-09 | 2022-03-11 | 中国原子能科学研究院 | Neptunium dioxide-plutonium dioxide dissolver for hot chamber |
| CN111640520B (en) * | 2020-04-26 | 2022-07-01 | 中国原子能科学研究院 | Device and method for adjusting valence states of neptunium and plutonium in hot chamber |
| CN111863298B (en) * | 2020-06-10 | 2022-08-05 | 中国原子能科学研究院 | Deep purification method of PUREX process polluted solvent |
Family Cites Families (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1012771B (en) * | 1988-07-14 | 1991-06-05 | 清华大学 | Electrolytic reduction-extraction method for reclaiming np from waste radio active liquor |
| JP3050359B2 (en) * | 1994-03-10 | 2000-06-12 | 核燃料サイクル開発機構 | Separation method of neptunium and plutonium |
| CN103305702B (en) * | 2013-07-08 | 2014-12-24 | 中国原子能科学研究院 | Process for recovering and purifying neptunium from waste liquor discharged from 2AW+2DW in Purex flow |
| CN106555062B (en) * | 2015-09-29 | 2020-07-31 | 中国科学院上海应用物理研究所 | Uranium recovery method |
| CN106555054B (en) * | 2015-09-29 | 2019-08-13 | 中国科学院上海应用物理研究所 | A kind of separation and recovery method of thorium and uranium |
-
2017
- 2017-04-19 CN CN201710259170.5A patent/CN107245588B/en active Active
Also Published As
| Publication number | Publication date |
|---|---|
| CN107245588A (en) | 2017-10-13 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN107245588B (en) | A method of the extraction and recovery neptunium from spentnuclear fuel post-processing waste liquid | |
| Malmbeck et al. | Partitioning of minor actinides from HLLW using the DIAMEX process. Part 2-´´ Hot´´ continuous counter-current experiment | |
| Nash et al. | Separations chemistry for actinide elements: recent developments and historical perspective | |
| Morita et al. | Actinide partitioning from HLW in a continuous DIDPA extraction process by means of centrifugal extractors | |
| US8795610B2 (en) | Process for reprocessing spent nuclear fuel not requiring a plutonium-reducing stripping operation | |
| US3374068A (en) | Irradiated fuel reprocessing | |
| CN101449338A (en) | Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide | |
| CN110656247B (en) | Method for extracting and recovering plutonium from plutonium-containing nitric acid solution | |
| CN85105352B (en) | Method for Separating Actinides from Radioactive Waste Liquid | |
| Serrano-Purroy et al. | Towards a DIAMEX process using high active concentrate. Production of genuine solutions | |
| Liljenzin et al. | Reducing the long-term hazard of reactor waste through actinide removal and destruction in nuclear reactors | |
| US10297355B1 (en) | Reduction-oxidation of actinides extraction process (ROANEX) for used nuclear fuel recycling | |
| Gray et al. | Separation of plutonium from irradiated fuels and targets | |
| Achuthan et al. | Aqueous reprocessing by THOREX process | |
| Malmbeck et al. | EURO-GANEX, a Process for the Co-separation of TRU | |
| JP2002243890A (en) | Method for separating, storing and using all actinide from spent nuclear fuel | |
| Castano | Nuclear fuel reprocessing | |
| Xu et al. | An overview of R&D activities on high level liquid waste partitioning at Tsinghua University, China | |
| Abdel-Fattah et al. | Thermodynamics of the solvent extraction of Zr (IV) by Amberlite LA-2, TBP and HDEHP from different aqueous media | |
| JP7108519B2 (en) | Isolation method for minor actinides | |
| Keller Jr | The chemistry of protactinium, neptunium, americium, and curium in the nuclear fuel cycle | |
| Kubota | Development of the partitioning process at JAERI | |
| Deshingkar et al. | Partitioning of actinide from simulated high level wastes arising from reprocessing of PHWR fuels: counter current extraction studies using CMPO | |
| Schulz | Trilaurylamine extraction of neptunium and plutonium from Purex process waste | |
| Tsygankova et al. | Spent nuclear fuel as a resource of future |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant |