EP0033091B1 - Process for purifying a nitric-acid u/pu solution - Google Patents

Process for purifying a nitric-acid u/pu solution Download PDF

Info

Publication number
EP0033091B1
EP0033091B1 EP81100235A EP81100235A EP0033091B1 EP 0033091 B1 EP0033091 B1 EP 0033091B1 EP 81100235 A EP81100235 A EP 81100235A EP 81100235 A EP81100235 A EP 81100235A EP 0033091 B1 EP0033091 B1 EP 0033091B1
Authority
EP
European Patent Office
Prior art keywords
solution
impurities
plutonium
americium
ions
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.)
Expired
Application number
EP81100235A
Other languages
German (de)
French (fr)
Other versions
EP0033091A1 (en
Inventor
Volker Dr. Schneider
Gerhard Margraf
Wolf-Günther Dr. Druckenbrodt
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Alkem GmbH
Original Assignee
Alkem GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Alkem GmbH filed Critical Alkem GmbH
Publication of EP0033091A1 publication Critical patent/EP0033091A1/en
Application granted granted Critical
Publication of EP0033091B1 publication Critical patent/EP0033091B1/en
Expired legal-status Critical Current

Links

Images

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
    • C22B60/0265—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries extraction by solid resins
    • 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
    • C22B60/04—Obtaining plutonium
    • 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

Definitions

  • the present invention relates to a method for cleaning a nitric acid U / Pu solution from impurities.
  • solutions arise, for example, in the case of wet scrap return in a fuel element factory. They must be returned to the conversion process, ie the process for the production of nuclear fuels and fuel tablets from U0 2 or PuO z .
  • the impurities contained in them, the z. B. caused by the material of the reaction vessel and the pipelines, ie are preferably metallic, must be removed beforehand.
  • the normal impurities therefore consist of iron and chromium, with plutonium-containing nuclear fuels there is also americium, a decay product of plutonium that arises during the storage of plutonium-containing nuclear fuels, but must not be incorporated as a neutron poison in newly manufactured nuclear fuel tablets.
  • impurities are removed from uranium / plutonium solutions by extraction processes. This is usually divided into a uranium and a plutonium solution at the same time.
  • extraction process the use of organic, flammable solvents is necessary, which should be avoided as far as possible in the context of plutonium processing in glove boxes - the risk of fire must be kept as low as possible.
  • Ion exchangers from processes for cleaning plutonium have also been used in many areas. These are mostly anion exchangers that are loaded with strongly nitric acid solutions.
  • the plutonium (IV) is in this case as a nitrate complex and remains in the ion exchange column, while the impurities, such as. B. Americium, uranium and heavy metals go through the column. Uranium and plutonium are thus separated and the plutonium must be re-mixed with large amounts of dilute acid.
  • the plutonium (111) with all other metal cations is retained in the exchange columns and uranium (IV) as an anion complex passes through the column. Uranium and plutonium are also separated again, which is still loaded with all metallic impurities - as mentioned at the beginning. The plutonium must also be eluted again with large amounts of dilute acid.
  • This process is of particular interest when processing plutonium in a fuel assembly plant.
  • soluble (U / Pu) 0 2 powders are produced. If an americium content has built up in the material during long-term interim storage of plutonium, which must be separated off before further processing, these powders can be dissolved and cleaned and processed further by the process according to the invention. Manufacturing scrap that has been collected over a longer period of time and may also be contaminated can be dissolved and cleaned using the same procedure.
  • the process can advantageously be used to separate americium from nuclear fuel powders or tablets which have been stored for a very long time.
  • This oxidized solution is fed via valve 11 and line 51 with the help of a pump 5 to the ion exchange column 4 and the cation exchange resin contained therein (strongly acidic cation exchanger with SO 3 - as functional groups) is designed in such a way that predominantly the trivalent heavy metal ions do not Uranyl and plutonyl ions are adsorbed.
  • the solution running through the opened valve 46 and the line 45 then has the following composition:
  • the running U / Pu solution can be fed directly back to the conversion system.
  • this is eluted in a targeted manner.
  • the ion exchange column 4 is rinsed with 0.5 l malar nitric acid at medium temperature.
  • the rinsing liquid contains and is supplied from the container 2 via the line 51, the ion exchanger 4 and the opened valve 42 and the line 41 to the evaporator 3.
  • the heating device of the same is not shown for the sake of clarity, since devices of this type are known per se.
  • the rinsing solution is concentrated in this vaporizer and reaches the storage container 2 as distillate. This process step involves concentration of the U / Pu ions in the remaining solution, which is then returned via line 32 to the conversion system.
  • the impurities remain on the ion exchanger column 4. These are then eluted with 1 to 3 molar nitric acid, which was prepared in the tank 2 and was filled into it via the line 25 and the valve 26, and the eluate is fed via the valve 44 and the line 43 to an evaporator 6, the Distillate produced there is fed back to the storage tank 2 via line 62 and the concentrated solution is fed via line 61 either to the americium conversion or to the waste processing known per se. After rinsing with approximately 0.5 molar nitric acid, the ion exchange column 4 is available for a renewed cleaning cycle.
  • this initially discontinuous process can be made quasi-continuous.
  • the apparatuses are state of the art, so that this simple process does not cause any difficulties from this side either.
  • the simple construction of the required equipment also allows it to be installed in glove boxes, as is common in plutonium-processing plants.

Landscapes

  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Mechanical Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Geology (AREA)
  • Materials Engineering (AREA)
  • Environmental & Geological Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Treatment Of Liquids With Adsorbents In General (AREA)

Description

Die vorliegende Erfindung betrifft ein Verfahren zur Reinigung einer salpetersauren U/Pu-Lösung von Verunreinigungen. Solche Lösungen entstehen beispielsweise bei der nassen Schrottrückführung in einer Brennelementfabrik. Sie müssen in den Konversionsprozeß, d. h. in den Prozeß zur Herstellung von Kernbrennstoffen und Brennstofftabletten aus U02 bzw. PuOz zurückgeführt werden. Die in ihnen enthaltenen Verunreinigungen, die z. B. durch das Material der Reaktionsbehälter sowie der Rohrleitungen hervorgerufen werden, also vorzugsweise metallischer Art sind, müssen dabei vorher entfernt werden. Die normalen Verunreinigungen bestehen daher aus Eisen und Chrom, bei plutoniumhaltigen Kernbrennstoffen kommt dabei noch Americium hinzu, einem Zerfallsprodukt des Plutoniums, das während der Lagerung plutoniumhaltiger Kernbrennstoffe entsteht, jedoch als Neutronengift nicht in neuherzustellende Kernbrennstofftabletten eingebaut werden darf.The present invention relates to a method for cleaning a nitric acid U / Pu solution from impurities. Such solutions arise, for example, in the case of wet scrap return in a fuel element factory. They must be returned to the conversion process, ie the process for the production of nuclear fuels and fuel tablets from U0 2 or PuO z . The impurities contained in them, the z. B. caused by the material of the reaction vessel and the pipelines, ie are preferably metallic, must be removed beforehand. The normal impurities therefore consist of iron and chromium, with plutonium-containing nuclear fuels there is also americium, a decay product of plutonium that arises during the storage of plutonium-containing nuclear fuels, but must not be incorporated as a neutron poison in newly manufactured nuclear fuel tablets.

Bei einer längeren Lagerung von PU02-PU[ver besteht ebenfalls die Notwendigkeit für die Abtrennung des aufgebauten Americiums. Dies kann nach dem gleichen Verfahren geschehen.If P U 0 2 -P U [ver is stored for a long time, there is also a need to separate the built-up americium. This can be done using the same procedure.

Nach der bisherigen Technik, siehe z. B. den Purex-Prozeß, werden Verunreinigungen aus Uran/ Plutonium-Lösungen durch Extraktionsverfahren entfernt. Hierbei erfolgt normalerweise gleichzeitig eine Aufteilung in eine Uran- und in eine Plutoniumlösung. Beim Einsatz des Extraktionsverfahrens ist aber die Verwendung von organischen, brennbaren Lösungsmitteln notwendig, was im Rahmen der Plutoniumverarbeitung in Handschuhkästen tunlichst umgangen werden sollte - die Brandgefahr muß so klein als irgend möglich gehalten werden.According to the previous technology, see e.g. B. the Purex process, impurities are removed from uranium / plutonium solutions by extraction processes. This is usually divided into a uranium and a plutonium solution at the same time. When using the extraction process, however, the use of organic, flammable solvents is necessary, which should be avoided as far as possible in the context of plutonium processing in glove boxes - the risk of fire must be kept as low as possible.

Auch wurden bereits Ionentauscher aus Prozessen zur Reinigung von Plutonium in vielen Bereichen eingesetzt. Hier handelt es sich zumeist um Anionentauscher, die mit stark salpetersauren Lösungen beschickt werden. Das Plutonium (IV) liegt in diesem Falle als Nitrato-Komplex vor und bleibt in der lonentauschersäule, während die Verunreinigungen, wie z. B. Americium, Uran und Schwermetalle die Säule durchlaufen. Es kommt somit zu einer Auftrennung von Uran und Plutonium und das Plutonium muß mit großen Mengen verdünnter Säure wieder eiuiert werden.Ion exchangers from processes for cleaning plutonium have also been used in many areas. These are mostly anion exchangers that are loaded with strongly nitric acid solutions. The plutonium (IV) is in this case as a nitrate complex and remains in the ion exchange column, while the impurities, such as. B. Americium, uranium and heavy metals go through the column. Uranium and plutonium are thus separated and the plutonium must be re-mixed with large amounts of dilute acid.

Beim Einsatz von Kationentauschern wird das Plutonium (111) mit allen anderen Metallkationen in den Austauschsäulen zurückgehalten und Uran (IV) als Anionen-Komplex durchläuft die Säule. Es kommt somit ebenfalls wieder zu einer Auftrennung von Uran und Plutonium, das weiterhin noch mit allen metallischen Verunreinigungen - wie eingangs erwähnt - beladen ist. Das Plutonium muß auch hier ebenfalls mit großen Mengen verdünnter Säure wieder eluiert werden.When using cation exchangers, the plutonium (111) with all other metal cations is retained in the exchange columns and uranium (IV) as an anion complex passes through the column. Uranium and plutonium are also separated again, which is still loaded with all metallic impurities - as mentioned at the beginning. The plutonium must also be eluted again with large amounts of dilute acid.

Dieser Stand der Technik erfordert also in jedem Falle einen ziemlichen apparativen Aufwand, zumal die Verunreinigungen anschließend immer noch vom Uran oder Plutonium getrennt werden müssen.In any case, this state of the art requires a lot of equipment, especially since the impurities then still have to be separated from the uranium or plutonium.

Da sowohl Uran als auch Plutonium in ihrer oxidischen Form als Kernbrennstoff Verwendung finden, insbesondere auch als Mischoxide, ergab sich die Aufgabe aus deren Lösungen nur die Verunreinigungen herauszuholen und einer Abfallbehandlung zuzuführen und die so gereinigte Lösung in den Konversionsprozeß zurückzuführen.Since both uranium and plutonium in their oxidic form are used as nuclear fuel, in particular also as mixed oxides, the task arose from their solutions only to remove the impurities and to carry out a waste treatment and to return the cleaned solution to the conversion process.

Diese Aufgabe wird erfindungsgemäß dadurch gelöst, daß die U/Pu-lonen der Ausgangslösung in die sechswertige Form aufoxidiert werden, daß die Lösung sodann über eine Kationenaustauschersäule geleitet wird, die stark saure Kationentauscher mit S03- als funktioneller Gruppe enthält und in der die aus dreiwertigen Schwermetallionen, vorzugsweise Eisen-, Chrom- oder Americiumionen bestehenden Verunreinigungen zurückgehalten werden, und daß die Verunreinigungen durch anschließende Spülung dieser Säule der an sich bekannten Abfallbehandlung bzw. Verwertung zugeführt werden.This object is achieved in that the U / Pu ions of the starting solution are oxidized into the hexavalent form, that the solution is then passed over a cation exchange column which contains strongly acidic cation exchangers with S0 3 - as a functional group and in which the trivalent heavy metal ions, preferably iron, chromium or americium ions existing impurities are retained, and that the impurities by subsequent rinsing of this column are the waste treatment or recycling known per se.

Dieses Verfahren ist von besonderem Interesse bei der Plutoniumverarbeitung in einer Brennelementfabrik. Beim Einsatz moderner Kofällverfahren werden lösliche (U/Pu)02-Pulver hergestellt. Wenn sich bei einer zu langfristigen Zwischenlagerung von Plutonium ein Americiumgehalt im Material aufgebaut hat, der vor der Weiterverarbeitung abgetrennt werden muß, können diese Pulver gelöst und nach dem erfindungsgemäßen Verfahren gereinigt und weiterverarbeitet werden. Nach dem gleichen Verfahren können Fabrikationsschrotte, die über einen längeren Zeitraum gesammelt worden sind und evtl. noch zusätzlich verunreinigt sind, aufgelöst und gereinigt werden. Günstigerweise kann das Verfahren zur Abtrennung von Americium aus sehr lange gelagerten Pu-haltigen Kernbrennstoffpulvern oder Tabletten verwendet werden.This process is of particular interest when processing plutonium in a fuel assembly plant. When using modern co-precipitation processes, soluble (U / Pu) 0 2 powders are produced. If an americium content has built up in the material during long-term interim storage of plutonium, which must be separated off before further processing, these powders can be dissolved and cleaned and processed further by the process according to the invention. Manufacturing scrap that has been collected over a longer period of time and may also be contaminated can be dissolved and cleaned using the same procedure. The process can advantageously be used to separate americium from nuclear fuel powders or tablets which have been stored for a very long time.

Aus FR-A -2 198 902 ist es zwar bekannt eine salpetersaure Lösung von U6+-lonen über eine Kationenaustauschersäule zu leiten, in der Kationenaustauschersäule werden jedoch nicht Verunreinigungen, sondern Uranionen zurückgehalten, die durch Spülen mit verdünnter Säure eluiert werden.From FR-A -2 198 902 it is known to pass a nitric acid solution of U 6 + ions over a cation exchange column, but in the cation exchange column it is not impurities which are retained but uranium ions which are eluted by rinsing with dilute acid.

Zur näheren Veranschaulichung der Erfindung wird auf das in der Figur dargestellte Fließschema verwiesen und dieses anhand eines Beispieles näher erläutert. Zur besseren Demonstration des Verfahrens wurde eine salpetersaure U/Pu-Lösung künstlich mit Verunreinigungen versetzt, sie hatte dann die folgende Zusammensetzung:

Figure imgb0001
Figure imgb0002
 For a more detailed illustration of the invention, reference is made to the flow diagram shown in the figure and this is explained in more detail using an example. To better demonstrate the process, a nitric acid U / Pu solution was artificially mixed with impurities, it then had the following composition:
Figure imgb0001
Figure imgb0002

Diese Lösung wird nun über die Leitung 13 in den Oxidationsbehälter 1 eingelassen, der mit einer Heizeinrichtung 12 versehen ist. Durch' Erhitzen auf 130-150"C wird diese Lösung in einer Zeit von etwa 30 Minuten aufoxidiert und die Salpetersäurekonzentration eingestellt. Die nachfolgende Zusammenstellung zeigt diese Salpetersäurekonzentration sowie die erreichten Wertigkeitsstufen der darin enthaltenen lonen.

Figure imgb0003
This solution is now let in via the line 13 into the oxidation container 1, which is provided with a heating device 12. By heating to 130-150 ° C., this solution is oxidized in a time of about 30 minutes and the nitric acid concentration is adjusted. The following compilation shows this nitric acid concentration and the valence levels of the ions contained therein.
Figure imgb0003

Diese oxidierte Lösung wird über das Ventil 11 und die Leitung 51 mit Hilfe einer Pumpe 5 der lonenaustauschersäule 4 zugeführt und das darin enthaltene Kationenaustauscherharz (stark saurer Kationentauscher mit SO3- als funktionelle Gruppen) ist so ausgelegt, daß vorwiegend die dreiwertigen Schwermetallionen jedoch nicht die Uranyl- und Plutonylionen adsorbiert werden. Die über das geöffnete Ventil 46 und die Leitung 45 ablaufende Lösung hat dann folgende Zusammensetzung:

Figure imgb0004
This oxidized solution is fed via valve 11 and line 51 with the help of a pump 5 to the ion exchange column 4 and the cation exchange resin contained therein (strongly acidic cation exchanger with SO 3 - as functional groups) is designed in such a way that predominantly the trivalent heavy metal ions do not Uranyl and plutonyl ions are adsorbed. The solution running through the opened valve 46 and the line 45 then has the following composition:
Figure imgb0004

Der Vergleich zur Ausgangszusammensetzung zeigt, daß auf der Säule im wesentlichen Americium, Eisen und Chrom und nur äußerst geringe. Mengen von Uran und Plutonium verbleiben.The comparison with the starting composition shows that on the column essentially americium, iron and chromium and only very little. Amounts of uranium and plutonium remain.

Die ablaufende U/Pu-Lösung kann zunächst direkt wieder der Konversionsanlage zugeführt werden. Zur weiteren Rückgewinnung des auf der Säule 4 verbliebenen Urans und Plutoniums wird dieses gezielt eluiert. Dazu wird die lonenaustauschersäule 4 mit 0,5-lmalarer Salpetersäure bei mittlerer Temperierung gespült. Die Spülflüssigkeit enthält dadurch

Figure imgb0005
und wird aus dem Behälter 2 über die Leitung 51, den Ionentauscher 4 und das geöffnete Ventil 42 sowie die Leitung 41 dem Verdampfer 3 zugeführt. Die Heizeinrichtung desselben ist der Übersichtlichkeit halber nicht weiter dargestellt, da Geräte dieser Art an sich bekannt sind. In diesem Verdampfer wird die Spüllösung aufkonzentriert und gelangt als Destillat in den Vorratsbehälter 2. Aus diesem wurde sie auch für den Spülvorgang der lonenaustauschersäule 4 über das Ventil 21 entnommen. Mit diesem Prozeßschritt ist eine Aufkonzentrierung der U/Pu-lonen in der verbleibenden Lösung verbunden, diese wird dann über die Leitung 32 der Konversionsanlage wieder zurückgeführt.The running U / Pu solution can be fed directly back to the conversion system. To further recover the uranium and plutonium remaining on column 4, this is eluted in a targeted manner. For this purpose, the ion exchange column 4 is rinsed with 0.5 l malar nitric acid at medium temperature. As a result, the rinsing liquid contains
Figure imgb0005
 and is supplied from the container 2 via the line 51, the ion exchanger 4 and the opened valve 42 and the line 41 to the evaporator 3. The heating device of the same is not shown for the sake of clarity, since devices of this type are known per se. The rinsing solution is concentrated in this vaporizer and reaches the storage container 2 as distillate. This process step involves concentration of the U / Pu ions in the remaining solution, which is then returned via line 32 to the conversion system.

Nach diesem Arbeitsgang verbleiben auf der lonentauschersäule 4 nur noch die Verunreinigungen. Diese werden alsdann mit 1- bis 3molarer Salpetersäure, die im Tank 2 vorbereitet wurde, und in diesen über die Leitung 25 und das Ventil 26 eingefüllt wurde, eluiert und das Eluat über das Ventil 44 und die Leitung 43 einem Verdampfer 6 zugeführt, wobei das dort entstehende Destillat über die Leitung 62 wieder dem Vorratstank 2 zugeführt wird und die konzentrierte Lösung über die Leitung 61 entweder der Americiumkonversion oder der an sich bekannten Abfallverarbeitung zugeleitet wird. Nach einer Spülung mit ca. 0,5molarer Salpetersäure steht die lonenaustauschersäule 4 für einen erneuten Reinigungszyklus zur Verfügung.After this operation, only the impurities remain on the ion exchanger column 4. These are then eluted with 1 to 3 molar nitric acid, which was prepared in the tank 2 and was filled into it via the line 25 and the valve 26, and the eluate is fed via the valve 44 and the line 43 to an evaporator 6, the Distillate produced there is fed back to the storage tank 2 via line 62 and the concentrated solution is fed via line 61 either to the americium conversion or to the waste processing known per se. After rinsing with approximately 0.5 molar nitric acid, the ion exchange column 4 is available for a renewed cleaning cycle.

Durch eine mehrfache Anordnung der Behälter 1 bis 6 kann dieses zunächst diskontinuierliche Verfahren quasikontinuierlich gestaltet werden. Die apparativen Einrichtungen sind allgemeiner Stand der Technik, so daß diesem einfachen Verfahren auch von dieser Seite her keine Schwierigkeiten erwachsen. Der einfache Aufbau der benötigten Apparaturen gestattet es außerdem, diese in Handschuhboxen einzubauen, wie sie in plutoniumverarbeitenden Betrieben üblich sind.Through a multiple arrangement of the containers 1 to 6, this initially discontinuous process can be made quasi-continuous. The apparatuses are state of the art, so that this simple process does not cause any difficulties from this side either. The simple construction of the required equipment also allows it to be installed in glove boxes, as is common in plutonium-processing plants.

Die zur Überwachung des Verfahrens benötigten Geräte, wie z. B. Temperaturmeßfühler, Säuregradmesser usw. sowie ihre steuerungstechnische Verknüpfung wurden der Übersichtlichkeit halber nicht dargestellt, diese Technik gehört bei Kenntnis des geschilderten Verfahrensablaufes zum selbstverständlichen Wissen eines auf diesem Gebiet tätigen Fachmannes.The devices required to monitor the process, such as. B. temperature sensors, acidity level, etc., and their control-related linkage have not been shown for the sake of clarity, this technique is part of the knowledge of the process described understandable knowledge of a specialist working in this field.

Abschließend seien die mit diesem Verfahren verbundenen Vorteile kurz zusammengestellt:

  • 1. Die Auslegungskapazität der lonenaustauschersäulen 4 muß nicht nach der Uran- und Plutoniummenge, sondern weitgehend nur nach der Menge der zu erwartenden Verunreinigungen ausgelegt werden.
  • 2. Uran und Plutonium, die in den Ausgangsmaterialien bereits vergesellschaftet sind, werden nicht getrennt und können gemeinsam weiterverarbeitet werden.
  • 3. Da der Hauptanteil des Urans und Plutoniums die lonenaustauschersäule 4, ohne adsorbiert zu werden, durchläuft, kann der Anteil der Eluiersäure, der anschließend aufkonzentriert wird, klein gehalten werden. Dies bedeutet eine erhebliche Einsparung und Verdampferkapazität und damit auch an Energiekosten.
  • 4. Da ein Kationenaustauscherharz der erwähnten Art eingesetzt wird, kann dieses nicht nitriert werden und ist somit sehr sicher zu hantieren.
  • 5. Das Austauscherharz ist sehr strahlenbeständig und kann für eine große Anzahl, z. B. mehr als 100 Zyklen ohne Kapazitätsverlust eingesetzt werden.
  • 6. Die spezielle hohe Adsorptionsfähigkeit des Kationenaustauscherharzes für Americium erleichtert die spätere Prozeßführung für die Americiumkonversion, falls diese gewünscht wird.
  • 7. Die Endlagerung der eluierten Verunreinigungen, die bereits in aufkonzentrierter Form anfallen, ist Stand der Technik.
In conclusion, the advantages associated with this procedure are briefly summarized:
  • 1. The design capacity of the ion exchange columns 4 does not have to be designed according to the amount of uranium and plutonium, but largely only according to the amount of the impurities to be expected.
  • 2. Uranium and plutonium, which are already associated in the raw materials, are not separated and can be processed together.
  • 3. Since the main part of the uranium and plutonium passes through the ion exchange column 4 without being adsorbed, the part of the eluting acid which is subsequently concentrated can be kept small. This means a considerable saving and evaporator capacity and thus also in energy costs.
  • 4. Since a cation exchange resin of the type mentioned is used, it cannot be nitrided and is therefore very safe to handle.
  • 5. The exchange resin is very radiation-resistant and can for a large number, for. B. more than 100 cycles can be used without loss of capacity.
  • 6. The special high adsorption capacity of the cation exchange resin for americium facilitates the later process control for the americium conversion, if this is desired.
  • 7. The final storage of the eluted impurities, which already occur in concentrated form, is state of the art.

Claims (3)

1. A process for purifying a nitric acid U/Pu-solution from impurities, characterised in that the U/Pu-ions of the starting solution are oxidized to the hexavalent form; that the solution is then passed through a cation-exchange column which contains strongly acid cation exchangers having S03- as a functional group, and in which the impurities, which consist of trivalent heavy metal ions, especially iron, chromium or americium ions, are retained; and that through subsequent flushing of the column, the impurities are fed to known waste treatment or utilization steps.
2. A process according to claim 1, characterised in that, for the oxidation, the starting solution is heated in known manner to 130-150° C for a period of about 30 minutes.
3. The use of the process according to claim 1 for the separation of americium from Pu-containing nuclearfuel powders or pellets which have been stored for very long time.
EP81100235A 1980-01-29 1981-01-14 Process for purifying a nitric-acid u/pu solution Expired EP0033091B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3003088 1980-01-29
DE19803003088 DE3003088A1 (en) 1980-01-29 1980-01-29 METHOD FOR PURIFYING A NITRIC ACID U / PU SOLUTION

Publications (2)

Publication Number Publication Date
EP0033091A1 EP0033091A1 (en) 1981-08-05
EP0033091B1 true EP0033091B1 (en) 1984-06-06

Family

ID=6093162

Family Applications (1)

Application Number Title Priority Date Filing Date
EP81100235A Expired EP0033091B1 (en) 1980-01-29 1981-01-14 Process for purifying a nitric-acid u/pu solution

Country Status (4)

Country Link
US (1) US4431580A (en)
EP (1) EP0033091B1 (en)
JP (1) JPS5716396A (en)
DE (2) DE3003088A1 (en)

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2002060817A1 (en) * 2000-10-05 2002-08-08 Pcs Nitrogen Fertilizer, L.P. Gypsum decontamination process
KR20160072846A (en) 2008-05-02 2016-06-23 샤인 메디컬 테크놀로지스, 인크. Device and method for producing medical isotopes
WO2012003009A2 (en) 2010-01-28 2012-01-05 Shine Medical Technologies, Inc. Segmented reaction chamber for radioisotope production
US10734126B2 (en) * 2011-04-28 2020-08-04 SHINE Medical Technologies, LLC Methods of separating medical isotopes from uranium solutions
CA2869559C (en) 2012-04-05 2022-03-29 Shine Medical Technologies, Inc. Aqueous assembly and control method

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB812815A (en) * 1954-12-08 1959-04-29 Permutit Co Ltd Improvements relating to the recovery of uranium from solutions
FR2198902A1 (en) * 1972-09-09 1974-04-05 Bayer Ag
DE2733396B1 (en) * 1977-07-23 1978-09-07 Kernforschungsanlage Juelich Method and device for loading cores of weakly acidic cation exchange resins with uranyl ions

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CA526260A (en) * 1956-06-12 G. Harvey Bernard Radioactive compositions
US2875024A (en) * 1946-08-27 1959-02-24 Edward R Tompkins Separation of barium values from uranyl nitrate solutions
US2554476A (en) * 1949-01-25 1951-05-22 Louis B Werner Radioactive product and method of producing the same
GB801743A (en) * 1954-05-18 1958-09-17 Atomic Energy Authority Uk Extraction of plutonium and uranium
US3158577A (en) * 1963-06-20 1964-11-24 Lane A Bray Method of treating radioactive waste
US3880980A (en) * 1972-11-30 1975-04-29 Allied Chem Recovery of uranium from HCl digested phosphate rock solution

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB812815A (en) * 1954-12-08 1959-04-29 Permutit Co Ltd Improvements relating to the recovery of uranium from solutions
FR2198902A1 (en) * 1972-09-09 1974-04-05 Bayer Ag
DE2733396B1 (en) * 1977-07-23 1978-09-07 Kernforschungsanlage Juelich Method and device for loading cores of weakly acidic cation exchange resins with uranyl ions

Also Published As

Publication number Publication date
JPH0128920B2 (en) 1989-06-06
DE3162623D1 (en) 1984-07-12
DE3003088A1 (en) 1981-07-30
EP0033091A1 (en) 1981-08-05
US4431580A (en) 1984-02-14
JPS5716396A (en) 1982-01-27

Similar Documents

Publication Publication Date Title
DE1592427A1 (en) Processing of irradiated nuclear fuel
EP2564394B1 (en) Process for decontamination of surfaces
DE2210106A1 (en) Process for the selective extraction of metalhones from aqueous solutions
DE2154655C3 (en) Process for the separation of uranium, transuranium elements and mixtures containing elements occurring as fission products of nuclear fuels by countercurrent or cross-current electrolysis
DE2839317C2 (en)
DE69402633T2 (en) Process for the separation and recovery of plutonium and neptunium from a nitric acid solution
DE3332954C2 (en)
DE1929512A1 (en) Processing system for irradiated nuclear fuel
CH625363A5 (en)
EP0033091B1 (en) Process for purifying a nitric-acid u/pu solution
DE2556939A1 (en) FUEL FOR NUCLEAR REACTORS AND PROCESS FOR ITS PRODUCTION
DE1592418B2 (en) PROCESS FOR PROCESSING AQUATIC SOLUTIONS OF IRRADIATED REACTOR FUELS
EP0170796B1 (en) Process for separating great amounts of uranium from small amounts of fission products which are present in aqueous basic solutions containing carbonate
EP0170795B1 (en) Method for recovering uranium values in an extractive reprocessing process for irradiated nuclear-fuel materials
DE3345199C2 (en)
DE2520940C2 (en) Device for the continuous, extractive separation of connections by means of electrolytic reduction
EP0112500A1 (en) Process for producing crystals containing plutonium dioxide
EP0033444B1 (en) Process for recovering uranium and/or plutonium from solutions with a high salt load
DE3940401A1 (en) METHOD AND ARRANGEMENT FOR REDUCING THE IODINE CONTENT IN A NUCLEAR FUEL SOLUTION
Schneider et al. Process for cleaning a nitric acid U/Pu-solution
DE2348804A1 (en) METHOD OF REMOVING FISSION PRODUCTS FROM COOLANT FROM NUCLEAR REACTOR PLANTS
DE3642841C2 (en)
DE3147199A1 (en) METHOD FOR SOLVING SOLIDS, ESPECIALLY SOLID CORE REACTOR FUELS, AND SOLUTION VESSEL, ESPECIALLY FOR THIS METHOD
DE1150369B (en) Process for converting masses containing zirconium and uranium into stable solutions
DE3101505C2 (en) Process for treating plutonium nitrate, optionally together with uranyl nitrate

Legal Events

Date Code Title Description
PUAI Public reference made under article 153(3) epc to a published international application that has entered the european phase

Free format text: ORIGINAL CODE: 0009012

AK Designated contracting states

Designated state(s): BE DE FR GB

17P Request for examination filed

Effective date: 19811030

GRAA (expected) grant

Free format text: ORIGINAL CODE: 0009210

AK Designated contracting states

Designated state(s): BE DE FR GB

REF Corresponds to:

Ref document number: 3162623

Country of ref document: DE

Date of ref document: 19840712

ET Fr: translation filed
PLBE No opposition filed within time limit

Free format text: ORIGINAL CODE: 0009261

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: NO OPPOSITION FILED WITHIN TIME LIMIT

26N No opposition filed
PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: GB

Payment date: 19891231

Year of fee payment: 10

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: BE

Payment date: 19900124

Year of fee payment: 10

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: FR

Payment date: 19900125

Year of fee payment: 10

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: DE

Payment date: 19900328

Year of fee payment: 10

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: GB

Effective date: 19910114

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: BE

Effective date: 19910131

GBPC Gb: european patent ceased through non-payment of renewal fee
PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: FR

Effective date: 19910930

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: DE

Effective date: 19911001

REG Reference to a national code

Ref country code: FR

Ref legal event code: ST