CN113981253B - Recovery method of americium-containing waste - Google Patents

Recovery method of americium-containing waste Download PDF

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CN113981253B
CN113981253B CN202111273570.4A CN202111273570A CN113981253B CN 113981253 B CN113981253 B CN 113981253B CN 202111273570 A CN202111273570 A CN 202111273570A CN 113981253 B CN113981253 B CN 113981253B
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americium
acid solution
solution
containing waste
exchange resin
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CN113981253A (en
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邹青
李凯
赵园
王亚星
曾献
胡宸
周桐
罗益玮
段承杰
崔大伟
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China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
Lingdong Nuclear Power Co Ltd
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China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
Lingdong Nuclear Power Co Ltd
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    • 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
    • C22B60/0295—Obtaining thorium, uranium, or other actinides obtaining other actinides except plutonium
    • 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
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/006—Wet processes
    • C22B7/007—Wet processes by acid leaching
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/08—Processing by evaporation; by distillation
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/12—Processing by absorption; by adsorption; by ion-exchange
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/20—Recycling

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  • Environmental & Geological Engineering (AREA)
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  • High Energy & Nuclear Physics (AREA)
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  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Treatment Of Water By Ion Exchange (AREA)

Abstract

The invention relates to a method for recycling americium-containing waste. In the method for recovering the americium-containing waste, firstly, the americium-containing waste is dissolved in hydrochloric acid solution to obtain an americium-containing solution, and the americium-containing waste contains americium elements and complexes thereof; evaporating and drying the americium-containing solution, and then adding a nitric acid solution to obtain an americium-containing nitric acid solution; and (3) adsorbing the nitric acid solution containing the americium by using ion exchange resin, and then desorbing to obtain an americium ion solution, wherein active groups of the ion exchange resin comprise any one of sulfonic acid groups, phosphonic acid groups or amide groups. The method can separate and recycle americium from the americium-containing waste with complex components, has high separation efficiency and mild conditions, and can obtain the high-purity americium ion solution which can be used for the radioactive experiment to realize the reutilization of the waste, thereby reducing the treatment capacity and the treatment cost of the radioactive waste in a laboratory and greatly relieving the pressure of the radioactive waste treatment.

Description

Recovery method of americium-containing waste
Technical Field
The invention relates to the technical field of radioactive metal treatment, in particular to a method for recycling americium-containing waste.
Background
Along with the gradual implementation of carbon peak and carbon neutralization promise in China, the specific gravity of clean energy in the energy structure of China is heavier and heavier. The nuclear energy is used as a clean energy source, has the advantages of high energy density, small carbon emission, large uranium resource reserves and the like, and plays an important role in the process of realizing the carbon neutralization target. The nuclear power operation can generate a large amount of spent fuel, and the spent fuel contains a large amount of recyclable resources such as uranium, plutonium and the like and minor actinides such as americium with long-term radioactivity. In the prior art, a closed circulation nuclear energy utilization strategy is adopted to separate, recycle and reuse uranium and plutonium in spent fuel, and simultaneously separate minor actinides such as americium and the like, so as to reduce the amount of radioactive waste which needs to be treated by a geological treatment method.
Americium (Am) is an important minor actinide nuclide of spent fuel, and in order to solve the separation problem in the post-treatment of spent fuel, technicians widely study physicochemical property analysis and separation behaviors of the spent fuel. In the radiochemistry experiment, when Am element is used for carrying out researches such as oxidization, separation and solid chemistry, a large amount of Am-containing waste is generated, wherein the Am-containing waste comprises Am-containing waste liquid and Am-containing solid waste, and the Am-containing radioactive waste is difficult to treat by the traditional separation and purification technology to reach the standard of direct discharge due to inherent toxicity and strong radioactivity of Am element. In the prior art, the treatment is mainly performed by a centralized storage mode, so as to minimize the radioactive waste containing Am and reduce the storage burden of the radioactive waste containing Am, technicians try to separate and recover Am from the radioactive waste containing Am, however, the traditional spent fuel post-treatment technology still stays in a stage of separating and recovering uranium and plutonium, but actinides such as americium (Am) are difficult to separate and recover effectively. The Am-containing waste generated by radiochemistry experiments is generally a solid-liquid mixture, has complex components and stable solid component properties, contains Am, various ligands capable of complexing or coordinating with Am and complexes formed by the two, and is difficult to effectively separate and recover americium (Am) from the Am-containing waste by a traditional separation technology.
Thus, there is a need in the art for improvement.
Disclosure of Invention
Based on the method, the invention provides a method for recovering the americium-containing waste, which can separate and recover the americium from the americium-containing waste with complex components and has high separation efficiency.
The technical scheme of the invention is as follows.
In one aspect of the invention, a method for recovering americium-containing waste is provided, comprising the steps of:
dissolving americium-containing waste in hydrochloric acid solution to obtain an americium-containing solution, wherein the americium-containing waste contains americium elements and complexes thereof;
evaporating and drying the americium-containing solution, and then adding a nitric acid solution to obtain an americium-containing nitric acid solution;
adsorbing the nitric acid solution containing the americium by ion exchange resin, and then desorbing to obtain an americium ion solution; the active group of the ion exchange resin comprises any one of sulfonic acid group, phosphonic acid group or amide group.
In some of these embodiments, the active groups of the ion exchange resin are sulfonic acid groups.
In some of these embodiments, the ion exchange resin is a sulfonic acid group-containing styrene-divinylbenzene copolymer.
In some of these embodiments, the step of adsorbing treatment employs dynamic adsorption; in the step of adsorption treatment, the flow rate of the nitric acid solution containing americium is 0.5-1.5 mL/min.
In some of these embodiments, the dynamic adsorption contact time of the americium-containing nitric acid solution with the ion exchange resin is between 3 minutes and 10 minutes.
In some embodiments, the desorption step uses hydrochloric acid solution with the concentration of 4-7 mol/L as eluent, and the flow rate of the eluent is 0.3-0.7 mL/min.
In some of these embodiments, after the step of adsorption treatment and before the step of desorption, the method further comprises the steps of:
and pre-eluting the ion exchange resin after the adsorption treatment by adopting hydrochloric acid solution with the concentration of 0.5 mol/L-1.5 mol/L.
In some of these embodiments, the step of desorbing is repeated 3-6 times; and/or
Repeating the pre-elution step for 3-6 times.
In some of these embodiments, the method further comprises the steps of:
evaporating the americium ion solution, and then adding nitric acid solution to obtain Am (NO) 3 ) 3 A solution.
In some of these embodiments, the concentration of the hydrochloric acid solution used in the step of dissolving the americium-containing waste in the hydrochloric acid solution is between 4 and 7 moles/liter; the volume ratio of the americium-containing waste to the hydrochloric acid liquid is 1 (0.1-1); and/or
The temperature of the step of dissolving the americium-containing waste in the hydrochloric acid solution is between 180 and 210 ℃.
In some embodiments, the concentration of the nitric acid solution is 1mol/L to 3mol/L.
In some of these embodiments, before the step of adsorbing treatment, further comprising the steps of:
and pre-leaching the ion exchange resin by adopting hydrochloric acid solution with the concentration of 0.3 mol/L-0.7 mol/L.
In the method for recycling the americium-containing waste, firstly, the americium-containing waste is dissolved in hydrochloric acid solution, the complex containing americium in the americium-containing solution is fully dissociated by the hydrochloric acid solution, and solid matters such as the complex containing americium in the americium-containing waste are dissolved in the hydrochloric acid solution, so that americium elements in the nitric acid solution containing americium exist in the form of americium ions, and a uniform americium-containing solution is obtained; then evaporating and drying the americium-containing solution, and adding a nitric acid solution to obtain an americium-containing nitric acid solution; then the nitric acid solution containing the americium is adsorbed by a specific ion exchange resin, in the process, the nitric acid solution containing the americium provides an acid system which is favorable for separating the americium ions from other impurities, the method is favorable for fully adsorbing the americium ions in the nitric acid solution containing the americium by the ion exchange resin, and other impurities flow out along with effluent; and then, recovering the americium ions adsorbed by the ion exchange resin through desorption to obtain a high-purity americium ion solution. Therefore, the americium can be separated and recovered from the americium-containing waste with complex components, the separation efficiency is high, the conditions are mild, the obtained high-purity americium ion solution can be used for a radioactive experiment, and the reutilization of the waste is realized, so that the treatment capacity and the treatment cost of radioactive waste in a laboratory are reduced, and the pressure of radioactive waste treatment is greatly relieved.
Detailed Description
The present invention will be described more fully hereinafter in order to facilitate an understanding of the present invention, and preferred embodiments of the present invention are set forth. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used herein in the description of the invention is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. The term "and/or" as used herein includes any and all combinations of one or more of the associated listed items.
An embodiment of the present invention provides a method for preparing ultrapure ceria, comprising the following steps S10 to S40.
And step S10, dissolving americium-containing waste in hydrochloric acid solution to obtain an americium-containing solution, wherein the americium-containing waste contains americium elements and complexes thereof.
And step S20, evaporating and drying the americium-containing solution obtained in the step S10, and adding a nitric acid solution to obtain an americium-containing nitric acid solution.
And step S30, adsorbing the americium-containing nitric acid solution obtained in the step S20 by using ion exchange resin, and then desorbing to obtain an americium ion solution.
The active groups of the ion exchange resin include any one of sulfonic acid groups, phosphonic acid groups or amide groups.
In the method for recycling the americium-containing waste, firstly, the americium-containing waste is dissolved in hydrochloric acid solution, the americium-containing complex in the americium-containing solution is fully dissociated, and solid matters such as the americium-containing complex in the americium-containing waste are completely dissolved, so that americium elements in the nitric acid solution containing the americium are in the form of americium ions, and a uniform americium-containing solution is obtained; then evaporating and drying the americium-containing solution, and adding a nitric acid solution to obtain an americium-containing nitric acid solution; then the nitric acid solution containing the americium is adsorbed by a specific ion exchange resin, in the process, the nitric acid solution containing the americium provides an acid system which is favorable for separating the americium ions from other impurities, the method is favorable for fully adsorbing the americium ions in the nitric acid solution containing the americium by the ion exchange resin, and other impurities flow out along with effluent; and then, recovering the americium ions adsorbed by the ion exchange resin through desorption to obtain a high-purity americium ion solution. Therefore, the americium can be separated and recovered from the americium-containing waste with complex components, the separation efficiency is high, the conditions are mild, the obtained high-purity americium ion solution can be used for a radioactive experiment, and the reutilization of the waste is realized, so that the treatment capacity and the treatment cost of radioactive waste in a laboratory are reduced, and the pressure of radioactive waste treatment is greatly relieved.
It is understood that the americium-containing waste contains americium elements, ligands capable of complexing or coordinating with Am, and complexes formed by both.
Further, the americium-containing waste may also contain other impurities, such as other metal salts, and the like.
The americium-containing waste is a solid-liquid mixture, has complex components, contains Am, various ligands capable of complexing or coordinating with Am and complex solid components formed by the Am and the ligands, has stable properties, can obtain uniform americium-containing solution by adopting hydrochloric acid solution, lays a foundation for the subsequent separation and recovery steps, and can not be well dissolved by other acids.
In some of these embodiments, the americium-containing waste contains Am (NO 3 ) 3 A phenylhexaic acid ligand (mel) and Am-mel solid state crystals.
In a specific example, the americium-containing waste is radioactive waste generated during the synthesis of the metal-organic framework material of Am.
In some of these embodiments, in step S10, the concentration of the hydrochloric acid solution used in the step of dissolving the americium-containing waste in the hydrochloric acid solution is between 4 and 7mol/L;
further, the volume ratio of the americium-containing waste to the hydrochloric acid solution is 1 (0.1-1).
In some of these embodiments, in step S10, the step of dissolving the americium-containing waste in the hydrochloric acid solution is at a temperature ranging from 180 ℃ to 210 ℃; further, the time is 1d to 3d. In a specific example, in step S10, the conditions of the step of dissolving the americium-containing waste in the hydrochloric acid solution are: incubate at 180℃for 3d.
The concentration, the dosage and the dissolution condition of the hydrochloric acid solution are controlled, so that solid matters in the americium-containing waste are further completely dissolved, a uniform americium-containing solution is obtained, a foundation is laid for the subsequent steps, and the recovery efficiency is further improved.
In some embodiments, the concentration of the nitric acid solution is 1mol/L to 3mol/L in the step S20.
By controlling the concentration of the nitric acid solution, the obtained americium-containing nitric acid solution has a specific acidic system, and the sufficient adsorption of americium ions in the americium-containing nitric acid solution in the subsequent step by the ion exchange resin is further promoted, so that the recovery efficiency is further improved.
In some embodiments, in step S20, the volume ratio of the americium-containing solution to the nitric acid solution is 1:0.1 to 1.
Further, in step S20, the evaporation drying step is performed under heating conditions, and the heating is performed to a temperature at which the liquid in the americium-containing solution evaporates, without any particular limitation. Specifically, the temperature is raised to a temperature that causes the liquid in the americium-containing solution to return.
Preferably, in step S30, the active group of the ion exchange resin is a sulfonic acid group.
The skilled person in the present invention, after a number of experiments, found that: when sulfonic acid groups or phosphonic acid groups or amide groups are used as active groups of the ion exchange resin, the americium ions are adsorbed by ionic action. Wherein, when the sulfonic acid group is used as an active group of the ion exchange resin, the adsorption and separation effects on americium ions are particularly excellent.
Further, the ion exchange resin is a styrene-divinylbenzene copolymer containing sulfonic acid groups.
The ion exchange resin can further improve the adsorption and separation effects on americium ions.
Specifically, the ion exchange resin is AG50W-X8.
It is to be understood that the ion exchange resin may be any one of resins of styrene-divinylbenzene copolymers having sulfonic acid groups, and is not limited to the specific commercial types mentioned above.
In some embodiments, the step of the adsorption treatment described above employs dynamic adsorption.
Further, in the step of adsorption treatment, the flow rate of the nitric acid solution containing americium is between 0.5mL/min and 1.5mL/min.
In some of these embodiments, the dynamic adsorption contact time of the americium-containing nitric acid solution with the ion exchange resin is between 3 minutes and 10 minutes.
Further, the volume/mass ratio of the americium-containing nitric acid solution to the ion exchange resin is 1g (1 mL-50 mL).
By controlling the specific adsorption treatment conditions, the penetration adsorption capacity in the adsorption treatment step is 50 mg/g-100 mg/g; am has an adsorption rate of 98% or more.
Further, the ion exchange resin has a particle size unit of 100 to 200 mesh.
In some of these embodiments, the adsorption step described above is performed in an exchange column; specifically, an ion exchange resin is packed into an exchange column to form an ion exchange column.
Further, the material of the exchange column is polytetrafluoroethylene.
In some embodiments, before the step of adsorbing treatment, the method further comprises the following steps:
and pre-leaching the ion exchange resin by adopting hydrochloric acid solution with the concentration of 0.3 mol/L-0.7 mol/L.
The ion exchange resin can be activated by a specific pre-leaching step, and the adsorption capacity of the ion exchange resin can be further improved.
Further, the pre-leaching treatment is repeated a plurality of times. Specifically, the pre-rinsing treatment was repeated 3 times.
In some embodiments, in the step S30, hydrochloric acid solution with the concentration of 4-7 mol/L is used as eluent in the desorption step, and the flow rate of the eluent is 0.3-0.7 mL/min.
The method comprises the steps of adopting hydrochloric acid solution with specific concentration as eluent, controlling the flow rate of the eluent, and desorbing the americium ions adsorbed by the ion exchange resin, thereby recovering and obtaining the high-purity americium ion solution.
In some of these embodiments, in step S30, the desorption step is repeated 3 to 6 times.
To further fully desorb the americium ions adsorbed by the ion exchange resin.
In a specific example, in step S30, the desorption step is repeated 5 times.
It is understood that the adsorption-desorption steps described above may be performed in the same column.
In some of these embodiments, in step S30, after the step of adsorption treatment and before the step of desorption, the method further comprises the steps of:
and pre-eluting the ion exchange resin after adsorption treatment by adopting hydrochloric acid solution with the concentration of 0.5 mol/L-1.5 mol/L.
In some of these embodiments, the use of a specific pre-elution step can further increase the efficiency of desorption.
Further, the above pre-elution step is repeated 3 to 6 times.
Specifically, the above-described pre-elution step was repeated 6 times.
The desorption rate in the desorption step reaches 88% -99% through specific desorption treatment conditions. Further, the recovery rate of Am in the americium-containing waste reaches 86.24-97.02%, and the purity of the recovered americium ion solution is high.
In some of these embodiments, the following step S40 is further included.
Step S40: evaporating and drying the americium ion solution obtained in the step S30, and then adding a nitric acid solution to obtain Am (NO) 3 ) 3 A solution.
Thus, the high-purity americium ion solution is converted into Am (NO) with higher purity 3 ) 3 The solution can be continuously used for the radioactive experiment, realizes the reutilization of wastes, reduces the treatment capacity and the treatment cost of radioactive wastes in laboratories, and greatly relieves the pressure of radioactive waste treatment.
Specifically, the concentration of the nitric acid solution used in step S40 is 0.1mol/L.
The invention will be described in connection with specific embodiments, but the invention is not limited thereto, and it will be appreciated that the appended claims outline the scope of the invention, and those skilled in the art, guided by the inventive concept, will appreciate that certain changes made to the embodiments of the invention will be covered by the spirit and scope of the appended claims.
DETAILED DESCRIPTION OF EMBODIMENT (S) OF INVENTION
Example 1
(1) Providing americium-containing waste: a radioactive waste solid-liquid mixture generated in the process of synthesizing the metal organic framework material of Am. The americium-containing waste contains Am (NO) 3 ) 3 A phenylhexaic acid ligand (mel) and Am-mel solid state crystals.
(2) 1.5mL of 5mol/L hydrochloric acid solution is added into 2mL of the americium-containing waste, and then the mixture is heated to 180 ℃ in a reaction kettle, and the mixture is subjected to heat preservation for 3 days, so that a uniform americium-containing solution is obtained.
(3) Then the americium-containing solution is placed in a reflux device for heating and evaporating until the solution is dried, and then 5mL of nitric acid solution with the concentration of 1mol/L is added to obtain the americium-containing nitric acid solution.
(4) Filling cation exchange resin AG50W-X8 (2 g; 100-200 meshes) into 10mL of polytetrafluoroethylene adsorption column to form a cation exchange column; taking 30mL of HCl solution with the concentration of 0.5mol/L as eluent, equally dividing into 3 parts, and pre-leaching the cation exchange resin in the cation exchange column for three times; then, carrying out dynamic adsorption experiments, wherein during adsorption treatment, the flow rate of the nitric acid liquid containing the americium is controlled to be 1mL/min, and the dynamic adsorption contact time of the nitric acid liquid containing the americium and the cation exchange resin is 5 minutes; then, 30mL of HCl solution with the concentration of 1mol/L is used as eluent, and is divided into 6 parts, and the cation exchange resin which has absorbed Am is pre-eluted for 6 times; finally, 5mL of hydrochloric acid solution with the concentration of 5mol/L is used as eluent, and is divided into 5 parts, the cation exchange resin after pre-elution is analyzed and attached for 5 times, and the flow rate of the eluent is controlled to be 0.5mL/min in the process of analysis and attachment, so that pure Am ion hydrochloric acid solution is obtained.
(5) The obtained Am ion hydrochloric acid solution is placed in a reflux device for heating and evaporation until the solution is dried, and then 1mL of nitric acid solution with the concentration of 0.1mol/L is added into the system to obtain Am (NO) 3 ) 3 A solution.
(6) Further detection of Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Thereby obtaining the molar quantity of recovered Am element, and the percentage of the molar quantity of recovered Am element to the molar quantity of Am element in the americium-containing waste is the recovery rate of Am element. Specifically, the recovery rate of Am element in example 1 was 93% by detection calculation.
Ultraviolet-visible absorption spectroscopy was used for Am (NO 3 ) 3 The purity of the solution was checked, am (NO 3 ) 3 Occupy Am (NO 3) 3 The mass percentage of the solute in the solution is Am (NO) 3 ) 3 Purity, results indicate that: am (NO) 3 ) 3 The mass percentage of the solute in the Am (NO 3) 3 solution is 99.9 percent.
Example 2
(1) Providing americium-containing waste: a radioactive waste solid-liquid mixture generated in the process of synthesizing the metal organic framework material of Am. The americium-containing waste contains Am (NO) 3 ) 3 A phenylhexaic acid ligand (mel) and Am-mel solid state crystals.
(2) 1.5mL of 5mol/L hydrochloric acid solution is added into 2mL of the americium-containing waste, and then the mixture is heated to 180 ℃ in a reaction kettle, and the mixture is subjected to heat preservation for 3 days, so that a uniform americium-containing solution is obtained.
(3) Then the americium-containing solution is placed in a reflux device for heating and evaporating until the solution is dried, and then 5mL of nitric acid solution with the concentration of 1mol/L is added to obtain the americium-containing nitric acid solution.
(4) Filling cation exchange resin HDEHP extraction resin (2 g; 100-200 meshes) into 10mL polytetrafluoroethylene adsorption columns to form cation exchange columns; taking 30mL of HCl solution with the concentration of 0.5mol/L as eluent, equally dividing into 3 parts, and pre-leaching the cation exchange resin in the cation exchange column for three times; then, carrying out dynamic adsorption experiments, wherein during adsorption treatment, the flow rate of the nitric acid liquid containing the americium is controlled to be 1mL/min, and the dynamic adsorption contact time of the nitric acid liquid containing the americium and the cation exchange resin is 5 minutes; then, 30mL of HCl solution with the concentration of 1mol/L is used as eluent, and is divided into 6 parts, and the cation exchange resin which has absorbed Am is pre-eluted for 6 times; finally, 5mL of hydrochloric acid solution with the concentration of 5mol/L is used as eluent, and is divided into 5 parts, the cation exchange resin after pre-elution is analyzed and attached for 5 times, and the flow rate of the eluent is controlled to be 0.5mL/min in the process of analysis and attachment, so that pure Am ion hydrochloric acid solution is obtained.
(5) The obtained Am ion hydrochloric acid solution is placed in a reflux device for heating and evaporation until the solution is dried, and then 1mL of nitric acid solution with the concentration of 0.1mol/L is added into the system to obtain Am (NO) 3 ) 3 A solution.
(6) As in step (6) of example 1, the recovery rate of Am element in example 2 was calculated by detection and found to be 90%. Obtained Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Occupy Am (NO 3) 3 SolutionThe mass percentage of the solute in the water is 99.9%.
Example 3
(1) Providing americium-containing waste: a radioactive waste solid-liquid mixture generated in the process of synthesizing the metal organic framework material of Am. The americium-containing waste contains Am (NO) 3 ) 3 A phenylhexaic acid ligand (mel) and Am-mel solid state crystals.
(2) 1.5mL of 5mol/L hydrochloric acid solution is added into 2mL of the americium-containing waste, and then the mixture is heated to 180 ℃ in a reaction kettle, and the mixture is subjected to heat preservation for 3 days, so that a uniform americium-containing solution is obtained.
(3) Then the americium-containing solution is placed in a reflux device for heating and evaporating until the solution is dried, and then 5mL of nitric acid solution with the concentration of 1mol/L is added to obtain the americium-containing nitric acid solution.
(4) Filling cation exchange resin amide resin (DGA) resin (2 g; 100-200 meshes) into 10mL of polytetrafluoroethylene adsorption column to form a cation exchange column; taking 30mL of HCl solution with the concentration of 0.5mol/L as eluent, equally dividing into 3 parts, and pre-leaching the cation exchange resin in the cation exchange column for three times; then, carrying out dynamic adsorption experiments, wherein during adsorption treatment, the flow rate of the nitric acid liquid containing the americium is controlled to be 1mL/min, and the dynamic adsorption contact time of the nitric acid liquid containing the americium and the cation exchange resin is 5 minutes; then, 30mL of HCl solution with the concentration of 1mol/L is used as eluent, and is divided into 6 parts, and the cation exchange resin which has absorbed Am is pre-eluted for 6 times; finally, 5mL of hydrochloric acid solution with the concentration of 5mol/L is used as eluent, and is divided into 5 parts, the cation exchange resin after pre-elution is analyzed and attached for 5 times, and the flow rate of the eluent is controlled to be 0.5mL/min in the process of analysis and attachment, so that pure Am ion hydrochloric acid solution is obtained.
(5) The obtained Am ion hydrochloric acid solution is placed in a reflux device for heating and evaporation until the solution is dried, and then 1mL of nitric acid solution with the concentration of 0.1mol/L is added into the system to obtain Am (NO) 3 ) 3 A solution.
(6) As in step (6) of example 1, the recovery rate of Am element in example 3 was 88% by detection and calculation. Obtained Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Occupy Am (NO) 3 ) 3 The mass percentage of the solute in the solution was 99.9%.
Example 4
Example 4 is identical to example 1, except that: step (3) then places the americium-containing solution in a reflux unit, heating it to evaporate until the solution dries, and then adding 5mL of nitric acid solution with a concentration of 3mol/L.
The remaining steps and conditions were the same as in example 1.
The recovery of Am element in example 4 was calculated to be 91% by detection. Obtained Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Occupy Am (NO) 3 ) 3 The mass percentage of the solute in the solution was 99.9%.
Example 5
Example 5 is identical to example 1, except that: in the desorption step in the step (4), a hydrochloric acid solution of 7mol/L was used as an eluent.
The remaining steps and conditions were the same as in example 1.
The recovery rate of Am element in example 5 was 89% as calculated by detection. Obtained Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Occupy Am (NO) 3 ) 3 The mass percentage of the solute in the solution was 99.9%.
Comparative example 1
(1) Providing americium-containing waste: a radioactive waste solid-liquid mixture generated in the process of synthesizing the metal organic framework material of Am. The americium-containing waste contains Am (NO) 3 ) 3 A phenylhexaic acid ligand (mel) and Am-mel solid state crystals.
(2) 1.5mL of 5mol/L hydrochloric acid solution is added into 2mL of the americium-containing waste, and then the mixture is heated to 180 ℃ in a reaction kettle, and the mixture is subjected to heat preservation for 3 days, so that a uniform americium-containing solution is obtained.
(3) Then the americium-containing solution is placed in a reflux device for heating and evaporating until the solution is dried, and then 5mL of nitric acid solution with the concentration of 1mol/L is added to obtain the americium-containing nitric acid solution.
(4) Filling ion exchange resin D113 resin (2 g; 100-200 meshes) into 10mL of polytetrafluoroethylene adsorption column to form a cation exchange column; taking 30mL of HCl solution with the concentration of 0.5mol/L as eluent, equally dividing into 3 parts, and pre-leaching the cation exchange resin in the cation exchange column for three times; then, carrying out dynamic adsorption experiments, wherein during adsorption treatment, the flow rate of the nitric acid liquid containing the americium is controlled to be 1mL/min, and the dynamic adsorption contact time of the nitric acid liquid containing the americium and the cation exchange resin is 5 minutes; then, 30mL of HCl solution with the concentration of 1mol/L is used as eluent, and is divided into 6 parts, and the cation exchange resin which has absorbed Am is pre-eluted for 6 times; finally, 5mL of hydrochloric acid solution with the concentration of 5mol/L is used as eluent, and is equally divided into 5 parts, the cation exchange resin after pre-elution is analyzed and attached for 5 times, and the flow rate of the eluent is controlled to be 0.5mL/min in the process of analysis and attachment treatment, so that pure Am ion hydrochloric acid solution is obtained.
(5) The obtained Am ion hydrochloric acid solution is placed in a reflux device for heating and evaporation until the solution is dried, and then 1mL of nitric acid solution with the concentration of 0.1mol/L is added into the system to obtain Am (NO) 3 ) 3 A solution.
(6) Further detection of Am (NO) 3 ) 3 Am in solution (NO) 3 ) 3 Thereby obtaining the molar quantity of recovered Am element, and the percentage of the molar quantity of recovered Am element to the molar quantity of Am element in the americium-containing waste is the recovery rate of Am element. Specifically, the recovery rate of Am element in comparative example 1 was 30% as calculated by detection.
Comparative example 2
Comparative example 2 in step (2), 5mol/L hydrochloric acid solution was replaced with 5mol/L sulfuric acid solution, and then heated to 180℃in a reaction kettle, and heat-preserved for 3 days, as a result, it was found that: the residue exists at the bottom of the reaction kettle, the solid waste is not completely dissolved, the dissolution efficiency is below 50%, and the subsequent steps are difficult to carry out.
The foregoing examples illustrate only a few embodiments of the invention, which are described in detail and are not to be construed as limiting the scope of the invention. It should be noted that it will be apparent to those skilled in the art that several variations and modifications can be made without departing from the spirit of the invention, which are all within the scope of the invention. Accordingly, the scope of protection of the present invention is to be determined by the appended claims.

Claims (11)

1. A method for recovering americium-containing waste, comprising the steps of:
dissolving americium-containing waste in hydrochloric acid solution to obtain an americium-containing solution, wherein the americium-containing waste contains americium elements and complexes thereof;
evaporating and drying the americium-containing solution, and then adding a nitric acid solution to obtain an americium-containing nitric acid solution; the concentration of the nitric acid solution is 1 mol/L-3 mol/L;
and (3) adsorbing the americium-containing nitric acid solution by using ion exchange resin, and then desorbing to obtain an americium ion solution, wherein the active group of the ion exchange resin comprises any one of sulfonic acid group, phosphonic acid group or amide group.
2. The method for the recovery of americium-containing waste as claimed in claim 1, characterized in that the active groups of the ion exchange resin are sulphonic acid groups.
3. The method for recovering americium-containing waste according to claim 1, characterized in that said ion exchange resin is a styrene-divinylbenzene copolymer containing sulfonic acid groups.
4. A method for recovering americium-containing waste as claimed in any one of claims 1 to 3, wherein the step of adsorption treatment uses dynamic adsorption; in the adsorption treatment step, the flow rate of the americium-containing nitric acid solution is 0.5 mL/min-1.5 mL/min.
5. The method for recovering americium-containing waste as claimed in claim 4, wherein the dynamic adsorption contact time of the nitric acid solution containing americium and the ion exchange resin is 3-10 minutes.
6. A method for recovering americium-containing waste as claimed in any one of claims 1 to 3, wherein in the desorption step, a hydrochloric acid solution with a concentration of 4 to 7mol/L is used as the eluent, and the flow rate of the eluent is 0.3 to 0.7mL/min.
7. The method for recovering americium-containing waste as claimed in claim 6, characterized in that it comprises, after said step of adsorption treatment and before said step of desorption, the further steps of:
and pre-eluting the ion exchange resin after the adsorption treatment by adopting hydrochloric acid solution with the concentration of 0.5mol/L to 1.5 mol/L.
8. The method for recovering americium-containing waste as claimed in claim 7, wherein said step of desorbing is repeated 3-6 times; and/or
Repeating the pre-elution step for 3-6 times.
9. A method for the recovery of americium-containing waste as claimed in any one of claims 1 to 3, further comprising the steps of:
evaporating the americium ion solution, and then adding nitric acid solution to obtain Am (NO) 3 ) 3 A solution.
10. The method for recovering americium-containing waste according to any one of claims 1 to 3, wherein the concentration of the hydrochloric acid solution used in the step of dissolving the americium-containing waste in the hydrochloric acid solution is 4mol/L to 7mol/L, and the volume ratio of the americium-containing waste to the hydrochloric acid solution is 1 (0.1 to 1); and/or
The temperature of the step of dissolving the americium-containing waste in the hydrochloric acid solution is 180-210 ℃.
11. A method for recovering americium-containing waste as claimed in any one of claims 1 to 3, further comprising, before the step of adsorption treatment, the steps of:
and pre-leaching the ion exchange resin by adopting hydrochloric acid solution with the concentration of 0.3 mol/L-0.7 mol/L.
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