JPH08239220A - Production of uranium dioxide powder - Google Patents
Production of uranium dioxide powderInfo
- Publication number
- JPH08239220A JPH08239220A JP7041913A JP4191395A JPH08239220A JP H08239220 A JPH08239220 A JP H08239220A JP 7041913 A JP7041913 A JP 7041913A JP 4191395 A JP4191395 A JP 4191395A JP H08239220 A JPH08239220 A JP H08239220A
- Authority
- JP
- Japan
- Prior art keywords
- ammonium
- particles
- salt
- gas
- uranate
- 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.)
- Granted
Links
Classifications
-
- 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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Landscapes
- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、原子炉燃料の製造に適
した二酸化ウラン（ＵＯ2）粉末を六フッ化ウラン（Ｕ
Ｆ6）の変換により製造する方法に関する。更に詳しく
は結晶粒径の大きな核燃料ペレットを製造するに適した
二酸化ウラン粉末の製造方法に関するものである。BACKGROUND OF THE INVENTION The present invention relates to a uranium dioxide (UO 2 ) powder suitable for the production of a nuclear fuel, and a uranium hexafluoride (U) powder.
F 6 ) conversion method. More specifically, it relates to a method for producing a uranium dioxide powder suitable for producing a nuclear fuel pellet having a large crystal grain size.
【０００２】[0002]
【従来の技術】従来、この種の製造方法として、湿式法
と乾式法が知られており、湿式法の中ではＡＤＵ（重ウ
ラン酸アンモニウム）法が最も多く用いられている。Ａ
ＤＵ法は、ＵＦ6ガスを気液反応で加水分解してウラニ
ルイオン含有液とし、この含有液にアンモニア水溶液を
添加して重ウラン酸アンモニウムを沈殿させ、これを濾
過し、乾燥し、焙焼・還元して二酸化ウラン粉末を得る
方法である。しかしこの方法では、アンモニア水が目的
とする中間生成物であるＡＤＵの沈殿反応の他に、上記
加水分解において副生するＨＦとも反応するために、本
来目的とする量より過剰のアンモニア水を必要とし、か
つ上記アンモニアの添加によってＮＨ4Ｆが副生し、こ
れが上記濾過工程で濾液中に移行する等の問題点があ
る。2. Description of the Related Art Conventionally, as a manufacturing method of this kind, a wet method and a dry method are known, and the ADU (ammonium diuranate) method is most often used among the wet methods. A
In the DU method, UF 6 gas is hydrolyzed by a gas-liquid reaction to give a uranyl ion-containing solution, and an aqueous ammonia solution is added to this solution to precipitate ammonium diuranate, which is filtered, dried, and roasted. -It is a method of reducing to obtain uranium dioxide powder. However, in this method, in addition to the precipitation reaction of ADU, which is the intended intermediate product of ammonia water, and the reaction with HF, which is a by-product of the above hydrolysis, an excess of ammonia water over the originally intended amount is required. In addition, there is a problem that NH 4 F is produced as a by-product due to the addition of the ammonia, and this is transferred to the filtrate in the filtration step.
【０００３】これらの問題点を解決する方法として特開
昭６２−１９７３１８号公報による二酸化ウランを製造
する方法が提案されている。この方法はＵＦ6ガスと水
蒸気の気相反応によりＵＯ2Ｆ2粒子とＨＦガスに分離
し、このＵＯ2Ｆ2粒子を水に溶解してＵＯ2Ｆ2水溶液を
生成させ、これにアンモニア水溶液を添加して重ウラン
酸アンモニウムを沈殿させ、これを濾過し、乾燥させ、
乾燥した重ウラン酸アンモニウムを焙焼・還元してＵＯ
2粉末を得ることを特徴とする。一方、近年の原子力発
電における技術革新の試みのひとつとして、原子炉燃料
をより長期間使用する、いわゆる高燃焼度化の計画が検
討されている。この高燃焼度化に伴って燃料からの核分
裂生成ガス（ＦＰガス）の放出が増大し、これによる燃
料棒内の内圧上昇及びペレット−被覆管ギャップの熱伝
導度の低下が起こり、燃料の健全性が低下する可能性が
あるため、高燃焼度化を実現するにはＦＰガスのペレッ
ト外への放出を低減することが必要である。このＦＰガ
スの保持効果を高めるためには、ペレットの結晶粒径を
大きくするのが有効であることが判っている。As a method for solving these problems, a method for producing uranium dioxide according to Japanese Patent Laid-Open No. 62-197318 has been proposed. This method separates UO 2 F 2 particles and HF gas by a gas phase reaction of UF 6 gas and water vapor, dissolves these UO 2 F 2 particles in water to generate a UO 2 F 2 aqueous solution, and an aqueous ammonia solution is added to this. To precipitate ammonium biuranate, which was filtered, dried,
UO by roasting and reducing dried ammonium heavy uranate
It is characterized in that 2 powders are obtained. On the other hand, as one of recent technological innovations in nuclear power generation, a so-called high burnup plan, which uses a reactor fuel for a longer period of time, is under study. As the burnup increases, the release of fission product gas (FP gas) from the fuel increases, which causes an increase in internal pressure in the fuel rod and a decrease in the thermal conductivity of the pellet-cladding gap. Therefore, it is necessary to reduce the emission of FP gas outside the pellets in order to achieve high burnup. It has been found that increasing the crystal grain size of the pellet is effective for enhancing the FP gas holding effect.
【０００４】[0004]
【発明が解決しようとする課題】しかし上記特開昭６２
−１９７３１８号公報に示される方法では従来のＡＤＵ
法に比べてアンモニア水の使用量及び副生ＮＨ4Ｆの発
生量を減少させることは可能であるが、得られるＵＯ2
粉末のハンドリング性（成形性）及び焼結特性が不十分
であり、結晶粒径の更に大きな核燃料ペレットを製造す
るには限界がある等の問題点が残されている。本発明の
目的は、ハンドリング性及び焼結特性に優れ、かつ結晶
粒径の大きな核燃料ペレットの製造に適したＵＯ2粉末
を得ることができる二酸化ウラン粉末の製造方法を提供
することにある。However, the above-mentioned Japanese Patent Application Laid-Open No. 62-62
In the method shown in Japanese Patent Laid-Open No. 197318, the conventional ADU is used.
Although it is possible to reduce the amount of ammonia water used and the amount of by-produced NH 4 F generated compared to the method, the UO 2 obtained
The handling properties (formability) and sintering characteristics of the powder are insufficient, and there are problems such as a limit to the production of nuclear fuel pellets having a larger crystal grain size. An object of the present invention is to provide a method for producing a uranium dioxide powder, which is excellent in handleability and sintering characteristics, and which can obtain UO 2 powder suitable for producing a nuclear fuel pellet having a large crystal grain size.
【０００５】[0005]
【課題を解決するための手段】上記目的を達成するため
に、本発明の二酸化ウラン粉末の製造方法はＵＦ6ガス
と水蒸気とを反応させてＵＯ2Ｆ2粒子を生成する工程
と、このＵＯ2Ｆ2粒子とアンモニウム塩とを水相中で反
応させてウラン酸アンモニウム塩を生成する工程と、生
成したウラン酸アンモニウム塩を固液分離する工程と、
固液分離されたウラン酸アンモニウム塩を焙焼・還元し
てＵＯ2粉末を生成する工程とを含むことを特徴とす
る。本発明において、水相中でのＵＯ2Ｆ2粒子とアンモ
ニウム塩との反応がアンモニウム塩水溶液へのＵＯ2Ｆ2
粒子の混合添加により行われるか、又はＵＯ2Ｆ2粒子を
水に溶解して生成したＵＯ2Ｆ2水溶液とアンモニウム塩
水溶液との混合により行われることが望ましい。In order to achieve the above object, the method for producing uranium dioxide powder according to the present invention comprises the steps of reacting UF 6 gas with steam to produce UO 2 F 2 particles, and A step of reacting 2 F 2 particles and an ammonium salt in an aqueous phase to produce an ammonium uranate salt; and a step of solid-liquid separating the produced ammonium uranate salt,
Roasting and reducing the solid-liquid separated ammonium uranate to produce UO 2 powder. In the present invention, UO 2 F 2 reaction with UO 2 F 2 particles and ammonium salt in the aqueous phase is the aqueous solution of ammonium
It is preferable to carry out by mixing and adding particles, or by mixing UO 2 F 2 aqueous solution produced by dissolving UO 2 F 2 particles in water and ammonium salt aqueous solution.
【０００６】アンモニウム塩は炭酸アンモニウム及び有
機酸のアンモニウム塩のいずれか又は双方であることが
望ましく、この場合有機酸のアンモニウム塩は酢酸アン
モニウム、シュウ酸アンモニウム又はコハク酸アンモニ
ウムのいずれかを包含する。従って、生成するウラン酸
アンモニウム塩は好ましくは炭酸ウラニルアンモニウ
ム、酢酸ウラニルアンモニウム、シュウ酸ウラニルアン
モニウム及びコハク酸ウラニルアンモニウムからなる群
から選ばれた１種又は２種以上の化合物である。The ammonium salt is preferably either or both ammonium carbonate and an ammonium salt of an organic acid, where the ammonium salt of an organic acid includes either ammonium acetate, ammonium oxalate or ammonium succinate. Therefore, the resulting ammonium uranate salt is preferably one or more compounds selected from the group consisting of uranyl ammonium carbonate, uranyl ammonium acetate, uranyl ammonium oxalate and uranyl ammonium succinate.
【０００７】次に本発明の二酸化ウラン粉末の製造方法
の一例を図１に示す装置に基づいて説明する。図１に示
すように、ＵＦ6ガスは導入管１０を通じて、また水蒸
気は導入管１１を通じてそれぞれ流動層反応装置１２内
に導入され、この内部で反応してＵＯ2Ｆ2粒子を生成す
る。流動層反応装置１２の好ましい操作温度は２００〜
５００℃である。流動層反応装置１２で副生するＨＦガ
スは凝縮器１３によってＨＦ水溶液として回収され、容
器１４に受けられる。Next, an example of the method for producing the uranium dioxide powder of the present invention will be described based on the apparatus shown in FIG. As shown in FIG. 1, the UF 6 gas is introduced into the fluidized bed reactor 12 through the introduction pipe 10 and the water vapor is introduced into the fluidized bed reactor 12 through the introduction pipe 11, and reacts therein to produce UO 2 F 2 particles. The preferred operating temperature of the fluidized bed reactor 12 is 200-
500 ° C. The HF gas produced as a by-product in the fluidized bed reactor 12 is recovered by the condenser 13 as an HF aqueous solution and received in the container 14.
【０００８】生成したＵＯ2Ｆ2粒子は反応装置１２の流
動層からオーバーフローして排出され、溶解装置１６に
導入し、そこに導管１７から導入される水によって溶解
される。溶解装置１６で生成したＵＯ2Ｆ2水溶液は反応
容器１８に送られ、そこに導管１９から導入されるアン
モニウム塩水溶液と反応してウラン酸アンモニウム塩の
沈殿を生成する。ウラン酸アンモニウム塩の沈殿を含む
液体は濾過装置２１に移送されて、沈殿と濾液に分離さ
れ、濾別された沈殿は乾燥装置２２に送られて乾燥され
る。乾燥されたウラン酸アンモニウム塩は焙焼・還元装
置２３に送られ、導管２４より導入される水素ガス、窒
素ガス及び水蒸気よりなる混合ガスと反応して、焙焼・
還元され、ＵＯ2を生成し、製品の二酸化ウランとして
容器２６に受容される。なお２７は排気処理系である。The produced UO 2 F 2 particles overflow from the fluidized bed of the reactor 12 and are discharged, introduced into the dissolving device 16 and dissolved therein by the water introduced from the conduit 17. The UO 2 F 2 aqueous solution generated in the dissolving device 16 is sent to the reaction vessel 18 and reacts with the ammonium salt aqueous solution introduced from the conduit 19 to generate a precipitate of ammonium uranate. The liquid containing the ammonium uranate salt precipitate is transferred to the filter device 21 to be separated into a precipitate and a filtrate, and the filtered precipitate is sent to the dryer device 22 to be dried. The dried ammonium uranate salt is sent to the roasting / reducing device 23 and reacts with a mixed gas consisting of hydrogen gas, nitrogen gas and steam introduced from a conduit 24 to roast / reduce.
It is reduced to form UO 2 and is received in container 26 as the product uranium dioxide. Reference numeral 27 is an exhaust treatment system.
【０００９】次に本発明の二酸化ウラン粉末の製造方法
の別の例を図２に示す装置に基づいて説明する。図２に
示すように、ＵＦ6ガスは導入管１０を通じて、また水
蒸気は導入管１１を通じてそれぞれ流動層反応装置１２
内に導入され、この内部で反応してＵＯ2Ｆ2粒子を生成
する。流動層反応装置１２の好ましい操作温度は２００
〜５００℃である。流動層反応装置１２で副生するＨＦ
ガスは凝縮器１３によってＨＦ水溶液として回収され、
容器１４に受けられる。Next, another example of the method for producing uranium dioxide powder of the present invention will be described based on the apparatus shown in FIG. As shown in FIG. 2, UF 6 gas is introduced through the introduction pipe 10 and steam is introduced through the introduction pipe 11 in the fluidized bed reactor 12 respectively.
It is introduced into and reacts inside to produce UO 2 F 2 particles. The preferred operating temperature of the fluidized bed reactor 12 is 200
~ 500 ° C. HF by-produced in the fluidized bed reactor 12
The gas is recovered by the condenser 13 as an HF aqueous solution,
It is received in the container 14.
【００１０】生成したＵＯ2Ｆ2粒子は流動層反応装置１
２の流動層からオーバーフローして排出され、アンモニ
ウム塩水溶液が収納されている反応容器３１に送られ
る。このアンモニウム塩水溶液は導管３２を通じて反応
容器３１に導入される。反応容器３１内において、ＵＯ
2Ｆ2粒子はアンモニウム塩水溶液に添加され、撹拌器３
３で混合されてウラン酸アンモニウム塩の沈殿を生成す
る。ウラン酸アンモニウム塩の沈殿を含む液体は濾過装
置２１に移送されて、沈殿と濾液に分離され、濾別され
た沈殿は乾燥装置２２に送られて乾燥される。乾燥され
たウラン酸アンモニウム塩は焙焼・還元装置２３に送ら
れ、導管２４より導入される水素ガス、窒素ガス及び水
蒸気よりなる混合ガスと反応して、焙焼・還元され、Ｕ
Ｏ2を生成し、製品の二酸化ウラン粉末として容器２６
に受容される。なお２７は排気処理系である。The UO 2 F 2 particles produced are in a fluidized bed reactor 1
It is overflowed from the fluidized bed of No. 2 and discharged, and sent to the reaction vessel 31 in which the ammonium salt aqueous solution is stored. This ammonium salt aqueous solution is introduced into the reaction vessel 31 through the conduit 32. In the reaction vessel 31, UO
2 F 2 particles were added to the ammonium salt aqueous solution and stirred 3
Mix at 3 to produce a precipitate of ammonium uranate salt. The liquid containing the ammonium uranate salt precipitate is transferred to the filter device 21 to be separated into a precipitate and a filtrate, and the filtered precipitate is sent to the dryer device 22 to be dried. The dried ammonium uranate salt is sent to the roasting / reducing device 23 and reacted with a mixed gas consisting of hydrogen gas, nitrogen gas and steam introduced from a conduit 24 to be roasted / reduced, and U
A container 26 that produces O 2 and is used as the product uranium dioxide powder
Accepted by. Reference numeral 27 is an exhaust treatment system.
【００１１】[0011]
【作用】ＵＯ2Ｆ2粒子とアンモニウム塩との水相中での
反応によって生成したウラン酸アンモニウム塩は固液分
離された後の流動性が良好であるため、このウラン酸ア
ンモニウム塩を焙焼・還元すると、ハンドリング性及び
焼結特性に優れたＵＯ2粉末が得られる。The ammonium uranate salt produced by the reaction of UO 2 F 2 particles with the ammonium salt in the aqueous phase has good fluidity after solid-liquid separation. Therefore, this ammonium uranate salt is roasted. -When reduced, UO 2 powder having excellent handling properties and sintering characteristics is obtained.
【００１２】[0012]
【実施例】次に本発明の具体的態様を示すために、本発
明の実施例を図１及び図２の装置に基づいて説明する。 ＜実施例１＞上述のように構成された図１の装置を下記
の操作条件で操作してＵＯ2粉末を製造した。 流動層反応装置１２の操作温度 ： ３００℃ ＵＦ6ガスの供給速度 ： ２００ｇ／分 水蒸気供給速度 ： ７０ｇ／分 ＵＯ2Ｆ2粒子の生成速度 ： １６７ｇ／分 ＵＯ2Ｆ2粒子と水との混合比（重量） ： ０．１３ アンモニウム塩 ： 炭酸アンモニウム アンモニウム塩水溶液の濃度 ： ２０％ ＵＯ2Ｆ2水溶液とアンモニウム塩水溶液 の混合比（ＮＨ3／Ｕモル比） ： ５ ウラン酸アンモニウム塩 ： 炭酸ウラニルアンモニウム 焙焼・還元装置２３の操作温度 ： ６５０℃ 水素ガス及び水蒸気 よりなる混合ガスの混合比（容量） ： Ｈ2／水蒸気＝１／１ ＜実施例２＞アンモニウム塩として炭酸アンモニウムの
代わりに酢酸アンモニウムを用いた以外は実施例１と実
質的に同じ操作を繰返してＵＯ2粉末を製造した。EXAMPLES Next, examples of the present invention will be described with reference to the apparatus shown in FIGS. 1 and 2 in order to show specific embodiments of the present invention. <Example 1> UO 2 powder was manufactured by operating the apparatus of FIG. 1 configured as described above under the following operating conditions. The operating temperature of the fluidized bed reactor 12: a 300 ° C. UF 6 gas feed rate: mixing with 167 g / min UO 2 F 2 particles and water: 200 g / min steam supply rate: 70 g / min UO 2 F 2 particles production rate of Ratio (weight): 0.13 Ammonium salt: Ammonium carbonate Concentration of ammonium salt aqueous solution: 20% Mixing ratio of 20% UO 2 F 2 aqueous solution and ammonium salt aqueous solution (NH 3 / U molar ratio): 5 Ammonium uranate: Uranyl carbonate Ammonium roasting / reducing device 23 operating temperature: 650 ° C. Mixing ratio (volume) of mixed gas consisting of hydrogen gas and steam: H 2 / steam = 1/1 <Example 2> Acetic acid instead of ammonium carbonate as ammonium salt Substantially the same operations as in Example 1 were repeated except that ammonium was used to produce UO 2 powder.
【００１３】＜実施例３＞上述のように構成された図２
の装置を下記の操作条件で操作してＵＯ2粉末を製造し
た。 流動層反応装置１２の操作温度 ： ３００℃ ＵＦ6ガスの供給速度 ： ２００ｇ／分 水蒸気供給速度 ： ７０ｇ／分 ＵＯ2Ｆ2粒子の生成速度 ： １６７ｇ／分 アンモニウム塩 ： 炭酸アンモニウム ＵＯ2Ｆ2粒子の添加速度 ： １６７ｇ／分 アンモニウム塩水溶液の濃度 ： ２０％ ＵＯ2Ｆ2粒子とアンモニウム塩水溶液 の混合比（ＮＨ3／Ｕモル比） ： ５ ウラン酸アンモニウム塩 ： 炭酸ウラニルアンモニウム 焙焼・還元装置２３の操作温度 ： ６５０℃ 水素ガス及び水蒸気 よりなる混合ガスの混合比（容量） ： Ｈ2／水蒸気＝１／１ ＜実施例４＞アンモニウム塩として炭酸アンモニウムの
代わりにシュウ酸アンモニウムを用いた以外は実施例３
と実質的に同じ操作を繰返してＵＯ2粉末を製造した。<Embodiment 3> FIG. 2 constructed as described above.
UO 2 powder was produced by operating the above apparatus under the following operating conditions. Operating temperature of the fluidized bed reactor 12: 300 ° C. UF 6 gas supply rate: 200 g / min Water vapor supply rate: 70 g / min UO 2 F 2 particle production rate: 167 g / min Ammonium salt: Ammonium carbonate UO 2 F 2 particles Addition rate: 167 g / min Ammonium salt aqueous solution concentration: 20% UO 2 F 2 particles / ammonium salt aqueous solution mixing ratio (NH 3 / U molar ratio): 5 Ammonium uranate: Uranyl ammonium carbonate roasting / reducing device Operation temperature of 23: 650 ° C. Mixing ratio (volume) of mixed gas consisting of hydrogen gas and steam: H 2 / steam = 1/1 <Example 4> Other than using ammonium oxalate instead of ammonium carbonate as ammonium salt Is Example 3
Substantially the same operation was repeated to produce UO 2 powder.
【００１４】＜比較例＞反応容器３１内において、ＵＯ
2Ｆ2粉末とアンモニウム塩水溶液とを反応させる代わり
に流動層反応装置１２で生成したＵＯ2Ｆ2粉末を水に溶
解してＵＯ2Ｆ2水溶液を調製し、このＵＯ2Ｆ2水溶液を
反応容器３１に導入し、かつアンモニア水溶液を導管３
２から反応容器３１に導入して重ウラン酸アンモニウム
（ＡＤＵ）の沈殿を生成させ、このＡＤＵ沈殿を濾過装
置２１及び乾燥装置２２を経由して焙焼・還元装置２３
に移送し、ここで焙焼・還元した。それ以外は実施例３
と実質的に同じ操作を繰返してＵＯ2粉末を製造した。<Comparative Example> In the reaction vessel 31, UO
The UO 2 F 2 powder produced by fluidized bed reactor 12 instead of reacting the 2 F 2 powder and an ammonium salt solution to UO 2 F 2 aqueous solution was prepared by dissolving in water, reacting the UO 2 F 2 aqueous solution It is introduced into the container 31 and the aqueous ammonia solution is introduced into the conduit 3
2 is introduced into the reaction vessel 31 to generate a precipitate of ammonium heavy uranate (ADU), and this ADU precipitate is roasted / reduced by the filtration device 21 and the drying device 22.
And then roasted and reduced there. Otherwise, Example 3
Substantially the same operation was repeated to produce UO 2 powder.
【００１５】＜評価＞実施例１〜実施例４及び比較例か
ら製造したＵＯ2粉末の代表的物性及びこれらのＵＯ2粉
末から同一条件でペレットを製造したときのペレットの
結晶粒径を表１に示す。<Evaluation> Table 1 shows typical physical properties of UO 2 powders produced in Examples 1 to 4 and Comparative Example and the crystal grain size of the pellets produced from these UO 2 powders under the same conditions. Shown in.
【００１６】[0016]
【表１】 [Table 1]
【００１７】表１から明らかなように、比較例と比べて
実施例１〜４は成形性及び焼結特性に優れ、かつ結晶粒
径の大きなペレットが得られることが判った。As is clear from Table 1, it was found that Examples 1 to 4 were superior in moldability and sintering characteristics to Comparative Examples and pellets having a large crystal grain size were obtained.
【００１８】[0018]
【発明の効果】以上述べたように、本発明によれば、Ｕ
Ｆ6ガスと水蒸気とを反応させてＵＯ2Ｆ2粒子を生成さ
せ、このＵＯ2Ｆ2粒子とアンモニウム塩とを水相中で反
応させてウラン酸アンモニウム塩を生成させ、生成した
ウラン酸アンモニウム塩を固液分離し、固液分離された
ウラン酸アンモニウム塩を焙焼・還元してＵＯ2粉末を
生成させるようにしたから、成形性及び焼結特性に優
れ、かつ結晶粒径の大きなペレットの製造に適したＵＯ
2粉末を得ることができる。As described above, according to the present invention, U
F 6 by reacting a gas and water vapor to produce a UO 2 F 2 particles, the UO 2 F 2 is reacted with particles and an ammonium salt in the aqueous phase by generating a uranium ammonium salts, uranium Ammonium generated The salt is solid-liquid separated, and the solid-liquid separated ammonium uranate salt is roasted / reduced to generate UO 2 powder. Therefore, pellets having excellent moldability and sintering characteristics and a large crystal grain size are formed. UO suitable for manufacturing
2 powders can be obtained.
【図１】本発明の方法の一例を実施するのに用いる装置
の構成図。FIG. 1 is a block diagram of an apparatus used to carry out an example of the method of the present invention.
【図２】本発明の方法の別の例を実施するのに用いる装
置の構成図。FIG. 2 is a block diagram of an apparatus used to carry out another example of the method of the present invention.
１０ ＵＦ6ガスの導入管 １１ 水蒸気の導入管 １２ 流動層反応装置 １３ ＨＦガスの凝縮器 １４ 容器 １６ 溶解装置 １７ 水の導管 １８，３１ 反応容器 １９，３２ アンモニウム塩水溶液の導管 ２１ 濾過装置 ２２ 乾燥装置 ２３ 焙焼・還元装置 ２４ 混合ガスの導管 ２６ 二酸化ウランの容器 ２７ 排気処理系 ３３ 撹拌器10 UF 6 Gas Introducing Pipe 11 Water Vapor Introducing Pipe 12 Fluidized Bed Reactor 13 HF Gas Condenser 14 Container 16 Dissolver 17 Water Pipeline 18,31 Reaction Vessel 19,32 Ammonium Salt Aqueous Pipeline 21 Filtration Device 22 Drying Equipment 23 Roasting / reducing equipment 24 Mixed gas conduit 26 Uranium dioxide container 27 Exhaust treatment system 33 Stirrer
───────────────────────────────────────────────────── フロントページの続き (72)発明者 橋本 知彦 茨城県那珂郡那珂町大字向山字六人頭1002 番地の14 三菱マテリアル株式会社那珂エ ネルギー研究所内 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Tomohiko Hashimoto 14 Nakamura-cho, Naka-gun, Ibaraki Pref.
Claims (6)
Ｆ2粒子を生成する工程と、 前記ＵＯ2Ｆ2粒子とアンモニウム塩とを水相中で反応さ
せてウラン酸アンモニウム塩を生成する工程と、 前記ウラン酸アンモニウム塩を固液分離する工程と、 前記固液分離されたウラン酸アンモニウム塩を焙焼・還
元してＵＯ2粉末を生成する工程とを含む二酸化ウラン
粉末の製造方法。1. UO 2 is produced by reacting UF 6 gas with water vapor.
Generating F 2 particles; reacting the UO 2 F 2 particles with an ammonium salt in an aqueous phase to generate an ammonium uranate salt; solid-liquid separating the ammonium uranate salt; And a step of roasting and reducing the solid-liquid separated ammonium uranate to produce UO 2 powder.
塩との反応がアンモニウム塩水溶液へのＵＯ2Ｆ2粒子の
混合添加により行われる請求項１記載の二酸化ウラン粉
末の製造方法。2. The method for producing a uranium dioxide powder according to claim 1, wherein the reaction of the UO 2 F 2 particles and the ammonium salt in the aqueous phase is carried out by mixing and adding the UO 2 F 2 particles to the aqueous ammonium salt solution.
塩との反応がＵＯ2Ｆ2粒子を水に溶解して生成したＵＯ
2Ｆ2水溶液とアンモニウム塩水溶液との混合により行わ
れる請求項１記載の二酸化ウラン粉末の製造方法。3. UO produced by the reaction of UO 2 F 2 particles with an ammonium salt in an aqueous phase by dissolving the UO 2 F 2 particles in water.
The method for producing a uranium dioxide powder according to claim 1, which is carried out by mixing an aqueous 2 F 2 solution and an aqueous ammonium salt solution.
有機酸のアンモニウム塩のいずれか又は双方である請求
項１ないし３いずれか記載の二酸化ウラン粉末の製造方
法。4. The method for producing a uranium dioxide powder according to claim 1, wherein the ammonium salt is one or both of ammonium carbonate and an ammonium salt of an organic acid.
ウム、シュウ酸アンモニウム又はコハク酸アンモニウム
のいずれかである請求項４記載の二酸化ウラン粉末の製
造方法。5. The method for producing a uranium dioxide powder according to claim 4, wherein the ammonium salt of the organic acid is ammonium acetate, ammonium oxalate or ammonium succinate.
アンモニウム、酢酸ウラニルアンモニウム、シュウ酸ウ
ラニルアンモニウム及びコハク酸ウラニルアンモニウム
からなる群から選ばれた１種又は２種以上の化合物であ
る請求項１ないし３いずれか記載の二酸化ウラン粉末の
製造方法。6. The ammonium uranate is one or more compounds selected from the group consisting of uranyl ammonium carbonate, uranyl ammonium acetate, uranyl ammonium oxalate and uranyl ammonium succinate. The method for producing a uranium dioxide powder as described above.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04191395A JP3339536B2 (en) | 1995-03-01 | 1995-03-01 | Method for producing uranium dioxide powder |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04191395A JP3339536B2 (en) | 1995-03-01 | 1995-03-01 | Method for producing uranium dioxide powder |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH08239220A true JPH08239220A (en) | 1996-09-17 |
| JP3339536B2 JP3339536B2 (en) | 2002-10-28 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP04191395A Expired - Lifetime JP3339536B2 (en) | 1995-03-01 | 1995-03-01 | Method for producing uranium dioxide powder |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009035432A (en) * | 2007-07-31 | 2009-02-19 | Mitsubishi Materials Corp | Manufacturing process of uranium dioxide granules |
| KR20210064250A (en) * | 2018-10-09 | 2021-06-02 | 후라마통 | Nuclear Fuel Powder Manufacturing Equipment |
-
1995
- 1995-03-01 JP JP04191395A patent/JP3339536B2/en not_active Expired - Lifetime
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009035432A (en) * | 2007-07-31 | 2009-02-19 | Mitsubishi Materials Corp | Manufacturing process of uranium dioxide granules |
| KR20210064250A (en) * | 2018-10-09 | 2021-06-02 | 후라마통 | Nuclear Fuel Powder Manufacturing Equipment |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3339536B2 (en) | 2002-10-28 |
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