JP2012166983A - Method for producing particle for producing nuclear fuel pellet - Google Patents
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本発明は、原子力発電などの燃料に用いられる核燃料ペレットを形成するためのペレット製造用粒子の製造方法に関する。 The present invention relates to a method for producing pellet production particles for forming nuclear fuel pellets used in fuels such as nuclear power generation.
原子力発電などの燃料には、二酸化ウラン燃料や二酸化ウランにプルトニウムを混合したＭＯＸ燃料が用いられる。これらの核燃料は、二酸化ウラン粉末などの原料粉末をペレットに成形して還元雰囲気下で焼結し、この焼結ペレットを燃料棒に封入し、多数の燃料棒を束ねた燃料集合体として使用される。 As fuel for nuclear power generation, uranium dioxide fuel or MOX fuel in which uranium dioxide is mixed with plutonium is used. These nuclear fuels are used as a fuel assembly in which raw powders such as uranium dioxide powder are formed into pellets and sintered in a reducing atmosphere, and the sintered pellets are sealed in fuel rods and bundled with many fuel rods. The
二酸化ウランなどの核燃料粉末を製造する方法としてマイクロ波加熱を利用した方法が知られている。この製造方法は、硝酸にウランを溶解させた硝酸ウラニル溶液などをマイクロ波によって加熱脱硝し、ウラン酸化物（主成分：ＵＯ3）のケーキ状乾固体とし、これを焙焼還元することによって、揮発性不純物を除去すると共に、酸化度を調整して二酸化ウラン（ＵＯ2）を主成分にし、この乾固体から焼結ペレットの原料となる核燃料粉末を製造している。 As a method for producing nuclear fuel powder such as uranium dioxide, a method using microwave heating is known. In this production method, a uranyl nitrate solution in which uranium is dissolved in nitric acid is heated and denitrated by microwaves to form a cake-like dry solid of uranium oxide (main component: UO 3 ), which is roasted and reduced. Volatile impurities are removed and the degree of oxidation is adjusted to make uranium dioxide (UO 2 ) the main component, and nuclear fuel powder that is a raw material for sintered pellets is produced from this dry solid.
一般的に、工業的に効率よく核燃料の焼結ペレットを製造するためには、ペレットの金型に入れやすいように、乾固体からペレット製造用の粒子を製造する。例えば、焙焼還元した乾固体を微細に粉砕し、この粉砕粉に水などのバインダを添加して粒径数百μmの粒子に造粒し、これを篩分けをしてペレット製造用粒子とし、規格外の粒子径のものは前工程にリサイクルして再利用している。 Generally, in order to produce sintered pellets of nuclear fuel efficiently industrially, particles for producing pellets are produced from dry solids so that they can be easily put into a pellet mold. For example, the dry solid that has been roasted and reduced is finely pulverized, and a binder such as water is added to the pulverized powder to form particles having a particle size of several hundreds of μm. Non-standard particle sizes are recycled and reused in the previous process.
特開２０１０−１９０７１８号公報（特許文献１）には、プルトニウムとウランの混合硝酸溶液をマイクロ波加熱して脱硝粉末にし、この脱硝粉末を焙焼還元した後にバインダを加えて造粒し、この造粒体をペレットに成形することが記載されている（図１（Ｂ）参照）。また、特開２０１０−１９０７２０号公報（特許文献２）には、プルトニウムとウランの混合硝酸溶液をマイクロ波加熱して脱硝粉末にし、これにバインダを加えて造粒した後に、造粒体を焙焼還元してペレット製造用粒子にすることが記載されている。 In JP 2010-190718 (Patent Document 1), a mixed nitric acid solution of plutonium and uranium is microwave-heated to obtain a denitration powder, the denitration powder is roasted and reduced, a binder is added and granulated. It is described that the granulated body is formed into pellets (see FIG. 1B). In JP 2010-190720 A (Patent Document 2), a mixed nitric acid solution of plutonium and uranium is microwave-heated to form a denitration powder, and after adding a binder to the granulated powder, the granulated product is roasted. It is described that it is subjected to calcination reduction to produce particles for pellet production.
特許文献１および特許文献２に記載されている方法は、何れもマイクロ波加熱によって脱硝して得た乾固体の粉砕粉末を造粒してペレット製造用粒子を製造している。一方、特開２００３−４８８３号公報（特許文献３）には、プルトニウムとウランの混合硝酸溶液をマイクロ波加熱して脱硝粉末にし、これを造粒せずに気流搬送して成形機に供給してペレットに成形する方法が記載されている。 In each of the methods described in Patent Document 1 and Patent Document 2, pelletized particles are manufactured by granulating a dry solid pulverized powder obtained by denitration by microwave heating. On the other hand, in Japanese Patent Application Laid-Open No. 2003-4883 (Patent Document 3), a mixed nitric acid solution of plutonium and uranium is microwave-heated to obtain a denitration powder, which is air-flowed without being granulated and supplied to a molding machine. The method of forming into pellets is described.
二酸化ウラン粉末にバインダの水を加えて造粒する場合、一般に水分量を数wt％以下の精度にコントロールするなど非常に厳密な運転条件を守る必要がある。また、造粒手法によっては、原料粉末の粒度分布や比表面積、あるいは水分量の僅かな差異が造粒体に大きな変化を与えることが知られている。 When granulating by adding binder water to uranium dioxide powder, it is generally necessary to observe very strict operating conditions such as controlling the water content to an accuracy of several wt% or less. In addition, it is known that, depending on the granulation technique, a slight difference in the particle size distribution, specific surface area, or moisture content of the raw material powder greatly changes the granulated body.
例えば、原料粉末の条件にもよるが、造粒のバインダに水を用いる場合、許容される水分量の誤差は数wt％以下、多くの場合には１wt％以下であり、水分量の管理は非常に難しい条件下にある。さらに、水は中性子の速度を減速させる効果があり、中性子がある速度まで減速されると核分裂反応（臨界）が起こりやすい環境になるため、臨界安全上は水を使用しないことが望ましい。このように、バインダに水を用いる場合には、臨界安全の観点から禁水区域としている施設における適用が困難である。 For example, depending on the conditions of the raw powder, when water is used for the granulating binder, the allowable moisture content error is several wt% or less, and in many cases 1 wt% or less. It is in a very difficult condition. Furthermore, water has the effect of reducing the speed of neutrons, and when neutrons are decelerated to a certain speed, a fission reaction (criticality) is likely to occur. Therefore, it is desirable not to use water for critical safety. As described above, when water is used for the binder, it is difficult to apply to a facility that is a water-prohibited area from the viewpoint of critical safety.
また、特許文献２の方法では、脱硝後の乾固体の粉末にバインダの水を加えた後に強力な混練を処して水が均一に分散した塊にし、この塊を解砕羽根で砕くことによって造粒し、この造粒体を焙焼還元してペレット製造用粒子を製造している。しかし、この造粒体は水和性のUO3粉体に水を添加しているので強固な水和物が形成されており、取扱が困難となる場合がある。 In addition, in the method of Patent Document 2, the water of the binder is added to the dry solid powder after denitration, and then powerful kneading is performed to form a lump in which water is uniformly dispersed, and the lump is crushed with a crushing blade. The granulated product is roasted and reduced to produce particles for pellet production. However, in this granulated body, water is added to the hydratable UO 3 powder, so that a strong hydrate is formed, and it may be difficult to handle.
本発明は、核燃料ペレットの製造方法における従来の上記問題を解決したものであり、ウラン酸化物の乾固体粉末に水を加えて造粒する工程を必要とせずにペレット製造用の粒子を製造する方法を提供する。 The present invention solves the above-mentioned conventional problems in the method of producing nuclear fuel pellets, and produces particles for pellet production without requiring a step of granulating by adding water to a dry solid powder of uranium oxide. Provide a method.
本発明は、以下の構成からなる核燃料ペレット製造用粒子の製造方法に関する。
〔１〕ウラン含有硝酸溶液をマイクロ波によって加熱脱硝してケーキ状乾固体を製造し、該乾固体を解砕することによってペレット製造用粒子を製造することを特徴とする核燃料ペレット製造用粒子の製造方法。
〔２〕ケーキ状乾固体を解砕した後に焙焼還元し、またはケーキ状乾固体を焙焼還元した後に解砕する上記[１]に記載する核燃料ペレット製造用粒子の製造方法。
〔３〕ケーキ状乾固体を粗砕した後に解砕し、該解砕粒子を篩分けして粒径が数百μmの粒子を選択してペレット製造用粒子にし、一方、篩分けから外れた解砕粒子を溶液の調整工程、粗砕工程または解砕工程に戻して再利用する上記[１]または上記[２]に記載する核燃料ペレット製造用粒子の製造方法。
〔４〕ウラン含有硝酸溶液が硝酸ウラニル溶液であり、または硝酸ウラニルと硝酸プルトニウムの混合溶液である上記[１]〜上記[３]の何れかに記載する核燃料ペレット製造用粒子の製造方法。
The present invention relates to a method for producing particles for producing nuclear fuel pellets having the following configuration.
[1] A nuclear fuel pellet manufacturing particle characterized in that a uranium-containing nitric acid solution is heated and denitrated by microwaves to produce a cake-like dry solid, and the dry solid is crushed to produce pellet-producing particles. Production method.
[2] The method for producing particles for producing nuclear fuel pellets according to the above [1], wherein the cake-like dry solid is crushed and reduced, or the cake-like dry solid is baked and reduced and then crushed.
[3] The cake-like dry solid was crushed and then crushed, and the crushed particles were sieved to select particles having a particle size of several hundreds of μm to produce pellets. The method for producing particles for producing nuclear fuel pellets according to the above [1] or [2], wherein the pulverized particles are returned to the solution adjustment step, the coarse pulverization step or the pulverization step and reused.
[4] The method for producing particles for producing nuclear fuel pellets according to any one of [1] to [3] above, wherein the uranium-containing nitric acid solution is a uranyl nitrate solution or a mixed solution of uranyl nitrate and plutonium nitrate.
本発明の製造方法によれば、ウラン含有硝酸溶液をマイクロ波加熱して砕きやすいケーキ状乾固体にし、これを解砕することによってペレット製造用の粒子を製造するので、乾固体を微細に粉砕する工程および水を加えて造粒する工程が無く、水の添加に起因する従来の課題を解決することができる。従って、安全性の高い製造方法であり、実用に適している。 According to the production method of the present invention, the uranium-containing nitric acid solution is heated in a microwave to form a cake-like dry solid that can be easily crushed. By crushing this, the particles for pellet production are produced, so the dry solid is finely pulverized. There is no step of granulating and adding water and granulating, so that the conventional problems caused by the addition of water can be solved. Therefore, it is a highly safe manufacturing method and is suitable for practical use.
また、本発明の製造方法は、乾固体を微粉末に粉砕する工程が無いので、微粉の発生量を軽減することができ、放射性物質の微粉末が周囲に付着・滞留する問題を低減することができる。 In addition, since the production method of the present invention does not have a step of pulverizing dry solids into fine powders, the amount of fine powders generated can be reduced, and the problem of radioactive substance fine powders adhering and staying around can be reduced Can do.
さらに、本発明の製造方法は造粒工程が無いので、造粒時の粒径制御などの操作が不要であり、製造工程を簡略化することができ、製造コストを低減することができる。 Furthermore, since the production method of the present invention does not have a granulation step, operations such as particle size control at the time of granulation are unnecessary, the production step can be simplified, and the production cost can be reduced.
以下、本発明を実施形態に基づいて具体的に説明する。
本発明の製造方法は、ウラン含有硝酸溶液をマイクロ波によって加熱脱硝してケーキ状乾固体を製造し、該乾固体を解砕することによってペレット製造用粒子を製造することを特徴とする核燃料ペレット製造用粒子の製造方法である。
Hereinafter, the present invention will be specifically described based on embodiments.
The production method of the present invention is a nuclear fuel pellet characterized by producing a cake-like dry solid by heating and denitrating a uranium-containing nitric acid solution by microwaves, and producing pelletized particles by crushing the dry solid It is a manufacturing method of the particle for manufacture.
本発明の製造方法の概略を図１（Ａ）に示す。
本発明の製造方法において、ウラン含有硝酸溶液として硝酸ウラニル溶液、または硝酸ウラニルと硝酸プルトニウムの混合溶液を用いることができる。硝酸ウラニル溶液からウラン燃料が製造される。また、硝酸ウラニルと硝酸プルトニウムの混合溶液からＭＯＸ燃料が製造される。
An outline of the production method of the present invention is shown in FIG.
In the production method of the present invention, a uranyl nitrate solution or a mixed solution of uranyl nitrate and plutonium nitrate can be used as the uranium-containing nitric acid solution. Uranium fuel is produced from uranyl nitrate solution. Also, MOX fuel is produced from a mixed solution of uranyl nitrate and plutonium nitrate.
本発明の製造方法は、ウラン含有硝酸溶液をマイクロ波によって加熱することによってウラン酸化物の乾固体にする。ウラン含有硝酸溶液をマイクロ波で加熱すると、水分が蒸発すると共に約２００℃を超えた付近で硝酸が分解してＮＯXガスが生じ、被加熱物の温度の上昇に伴って脱硝が進み、約３００℃を超えた付近でウラン酸化物の乾固体（主成分ＵＯ3）になる。 In the production method of the present invention, the uranium-containing nitric acid solution is heated by microwaves to form a uranium oxide dry solid. When the uranium-containing nitric acid solution is heated with microwaves, the water evaporates and the nitric acid decomposes in the vicinity of about 200 ° C. to generate NO x gas. Denitration proceeds as the temperature of the heated object increases, It becomes a uranium oxide dry solid (main component UO 3 ) near 300 ° C.
ウラン含有硝酸溶液を、例えば毎分３〜５℃程度の遅い昇温速度で加熱すると、結晶が成長した硬い乾固体になる。一方、マイクロ波加熱によって、例えば毎分１５〜３５℃程度の早い昇温速度で加熱すると、発生したＮＯXガスや水蒸気によって内部に多数の気泡が形成されたケーキ状乾固体になる。このケーキ状乾固体は人手で押し潰す程度の圧力で容易に解砕することができる。 When the uranium-containing nitric acid solution is heated at a slow heating rate of, for example, about 3 to 5 ° C. per minute, it becomes a hard dry solid with crystals grown. On the other hand, when heated at a high heating rate of, for example, about 15 to 35 ° C. per minute by microwave heating, a cake-like dry solid in which a large number of bubbles are formed inside by the generated NO x gas or water vapor is obtained. This cake-like dry solid can be easily crushed with a pressure that is crushed manually.
本発明は、上記マイクロ波加熱によって砕きやすいケーキ状乾固体を形成する。具体的には、例えば、０.５〜４Ｎ程度の硝酸ウラニル溶液（３００ｇ/L程度）８５０mLについて、マイクロ波を約３０〜約５０分照射して約４００℃〜約５００℃に加熱することによって、砕きやすいケーキ状乾固体を形成することができる。 The present invention forms a cake-like dry solid that is easily crushed by the microwave heating. Specifically, for example, about 850 mL of a uranyl nitrate solution (about 300 g / L) of about 0.5 to 4N is irradiated with microwaves for about 30 to about 50 minutes and heated to about 400 ° C. to about 500 ° C. It is possible to form a cake-like dry solid that is easy to crush.
ケーキ状乾固体を解砕してペレット製造用粒子に適する粒径の粒子を回収する。図２に示したように、脱硝した乾固体２０を粗砕した後に解砕しても良い。解砕は解砕装置３０を用いることができる。 The cake-like dry solid is crushed to collect particles having a particle size suitable for pellet production particles. As shown in FIG. 2, the denitrated dry solid 20 may be crushed and then crushed. The crushing apparatus 30 can be used for crushing.
解砕粒子４０を篩分けして粒径が数百μmの粒子を選択してペレット製造用粒子にし、一方、篩分けから外れた解砕粒子４０を溶液の調整工程、粗砕工程または解砕工程に戻して再利用することができる。 The pulverized particles 40 are sieved to select particles having a particle size of several hundreds of μm to produce pellets. On the other hand, the crushed particles 40 that are out of the sieving are adjusted in the solution, crushed or crushed. It can be returned to the process and reused.
解砕粒子（主成分ＵＯ3）は焙焼還元して酸化度を下げ二酸化ウラン粒子にする。ケーキ状乾固体を解砕した後に焙焼還元し、あるいはケーキ状乾固体を焙焼還元した後に解砕してもよい。焙焼は空気雰囲気下で５５０〜７５０℃の温度で行い、還元は水素雰囲気下で５５０〜７５０℃の温度で行えばよい。 The pulverized particles (main component UO 3 ) are roasted and reduced to reduce the degree of oxidation to uranium dioxide particles. The cake-like dry solid may be crushed and reduced after pulverization, or the cake-like dry solid may be crushed and reduced. The roasting may be performed at a temperature of 550 to 750 ° C. in an air atmosphere, and the reduction may be performed at a temperature of 550 to 750 ° C. in a hydrogen atmosphere.
〔実施例１〕
４Ｎ程度の硝酸ウラニル溶液（３００ｇ/L程度）８５０mLにマイクロ波を約３０分〜約５０分照射して約４００〜約４５０℃に加熱してケーキ状乾固体２５０ｇを得た。この乾固体を水素雰囲気下で６５０℃に加熱して還元し、粗砕粒を１０ｇ/分の割合で解砕装置に供給して粒径数百μmの粒子２５０ｇを回収し、二酸化ウランを主成分とするペレット製造用粒子を得た。解砕粒子の顕微鏡写真を図３、図４に示す。また、その粒度分布を図５に示す。図５の粒度分布は乾式レーザによる測定であり、その体積平均粒径は６２６.８μmである。
[Example 1]
850 mL of about 4N uranyl nitrate solution (about 300 g / L) was irradiated with microwaves for about 30 minutes to about 50 minutes and heated to about 400 to about 450 ° C. to obtain 250 g of a cake-like dry solid. This dry solid is reduced by heating to 650 ° C. in a hydrogen atmosphere, and coarsely crushed particles are supplied to a pulverizer at a rate of 10 g / min to recover 250 g of particles having a particle size of several hundred μm. The particles for pellet production were obtained. The micrographs of the crushed particles are shown in FIGS. The particle size distribution is shown in FIG. The particle size distribution in FIG. 5 is measured by a dry laser, and the volume average particle size is 626.8 μm.
２０−脱硝乾固体、３０−解砕装置、４０−解砕粒子。 20-Denitrated dry solid, 30-Crushing device, 40-Crushing particles.
Claims (4)
A method for producing particles for producing nuclear fuel pellets, comprising producing a cake-like dry solid by heating and denitrating a uranium-containing nitric acid solution by microwaves, and then pulverizing the dry solid.
The method for producing particles for producing nuclear fuel pellets according to claim 1, wherein the cake-like dry solid is crushed and then reduced by baking, or the cake-like dry solid is baked and reduced and then crushed.
After crushing the cake-like dry solid, it is crushed, and the crushed particles are sieved to select particles with a particle size of several hundreds of μm to produce pellets. On the other hand, the crushed particles deviated from sieving The method for producing particles for producing nuclear fuel pellets according to any one of claims 1 and 2, wherein the particles are recycled after being returned to the solution adjustment step, the coarse crushing step or the crushing step.
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| JPS54121442A (en) * | 1978-03-13 | 1979-09-20 | Power Reactor & Nuclear Fuel Dev Corp | Microwave heating device for radioactive material |
| JPS57100920A (en) * | 1980-12-16 | 1982-06-23 | Toshiba Corp | Converting apparatus of nuclear fuel |
| JP2001215295A (en) * | 2000-02-02 | 2001-08-10 | Japan Nuclear Cycle Development Inst States Of Projects | Denitrification-roasting-reduction system |
| JP2003004883A (en) * | 2001-06-26 | 2003-01-08 | Japan Nuclear Cycle Development Inst States Of Projects | Production method for nuclear fuel pellet |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP4054981A4 (en) * | 2019-11-04 | 2024-02-14 | X Energy Llc | Preparation of acid-deficient uranyl nitrate solutions |
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