JPH0949892A - Control method for grain diameter of uo2 sintered pellet - Google Patents
Control method for grain diameter of uo2 sintered pelletInfo
- Publication number
- JPH0949892A JPH0949892A JP7199906A JP19990695A JPH0949892A JP H0949892 A JPH0949892 A JP H0949892A JP 7199906 A JP7199906 A JP 7199906A JP 19990695 A JP19990695 A JP 19990695A JP H0949892 A JPH0949892 A JP H0949892A
- Authority
- JP
- Japan
- Prior art keywords
- grain
- powder
- sintered body
- scrap
- oxidation
- 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
- 238000000034 method Methods 0.000 title claims abstract description 18
- 239000008188 pellet Substances 0.000 title claims abstract description 18
- 239000000843 powder Substances 0.000 claims abstract description 27
- 238000005245 sintering Methods 0.000 claims abstract description 7
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000001257 hydrogen Substances 0.000 claims abstract description 5
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 5
- 239000013078 crystal Substances 0.000 claims description 18
- 239000002245 particle Substances 0.000 claims description 18
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 5
- 239000003758 nuclear fuel Substances 0.000 claims description 5
- 230000001590 oxidative effect Effects 0.000 claims description 5
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 4
- 230000003647 oxidation Effects 0.000 abstract description 13
- 238000007254 oxidation reaction Methods 0.000 abstract description 13
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 4
- 239000001301 oxygen Substances 0.000 abstract description 4
- 229910052760 oxygen Inorganic materials 0.000 abstract description 4
- 238000011084 recovery Methods 0.000 abstract description 4
- 238000000280 densification Methods 0.000 abstract description 3
- 239000000463 material Substances 0.000 abstract description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 abstract 4
- 229910018404 Al2 O3 Inorganic materials 0.000 abstract 2
- 229910052681 coesite Inorganic materials 0.000 abstract 2
- 229910052906 cristobalite Inorganic materials 0.000 abstract 2
- 239000000377 silicon dioxide Substances 0.000 abstract 2
- 235000012239 silicon dioxide Nutrition 0.000 abstract 2
- 229910052682 stishovite Inorganic materials 0.000 abstract 2
- 229910052905 tridymite Inorganic materials 0.000 abstract 2
- 238000007781 pre-processing Methods 0.000 abstract 1
- 238000009826 distribution Methods 0.000 description 6
- 239000007858 starting material Substances 0.000 description 6
- 230000007423 decrease Effects 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000011148 porous material Substances 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000005253 cladding Methods 0.000 description 2
- 238000007796 conventional method Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000010297 mechanical methods and process Methods 0.000 description 2
- 239000002253 acid Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- ZAASRHQPRFFWCS-UHFFFAOYSA-P diazanium;oxygen(2-);uranium Chemical compound [NH4+].[NH4+].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[U].[U] ZAASRHQPRFFWCS-UHFFFAOYSA-P 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000005469 granulation Methods 0.000 description 1
- 230000003179 granulation Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
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]
【発明の属する技術分野】本発明は、核燃料ペレット製
造に関し、特にＵＯ２焼結ペレットの結晶粒径を制御す
る方法に関するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to the production of nuclear fuel pellets, and more particularly to a method for controlling the grain size of UO 2 sintered pellets.
【０００２】[0002]
【従来の技術】ＵＯ２燃料の製造において発生するＵＯ
２スクラップは、大別して粉末とペレットに区分される
が、これらは回収して再利用に供される。ＵＯ２スクラ
ップの回収にあたっては、湿式法と乾式法が採用され
る。UO generated in the production of UO 2 fuel
The two scraps are roughly classified into powder and pellets, which are collected and reused. Wet method and dry method are adopted for the recovery of UO 2 scrap.
【０００３】粉末とペレットに適用される湿式法では、
ＵＯ２スクラップを酸で溶解し、二ウラン酸アンモニウ
ム（ＮＨ４）２Ｏ・２ＵＯ３またはＵＯ４として沈澱さ
せ、ＵＯ２粉末を得る。一方、主にペレットに適用され
る乾式法では、ＵＯ２スクラップを酸化雰囲気中で処理
し、Ｕ３Ｏ８粉末を得る。In the wet method applied to powders and pellets,
UO 2 scrap is dissolved with acid and precipitated as ammonium diuranate (NH 4 ) 2 O.2UO 3 or UO 4 to obtain UO 2 powder. On the other hand, in the dry method mainly applied to pellets, UO 2 scrap is processed in an oxidizing atmosphere to obtain U 3 O 8 powder.
【０００４】湿式法によるＵＯ２スクラップの回収には
プラント設備の費用がかかったり、廃液処理等の問題が
あるため、乾式法の採用が好ましい。しかし、乾式法で
得られたＵ３Ｏ８粉末は、これをＵＯ２粉末に添加し、
成形、焼結すると、還元雰囲気中でＵＯ２に相変化を起
し、密度低下の原因となる。[0004] Since the recovery of UO 2 scrap by the wet method involves the cost of plant facilities and waste liquid treatment, the dry method is preferable. However, the U 3 O 8 powder obtained by the dry method was added to UO 2 powder,
When molded and sintered, UO 2 undergoes a phase change in a reducing atmosphere, which causes a decrease in density.
【０００５】従って、安定した焼結密度を有するＵＯ２
粉末を得るには、まず前述したＵ３Ｏ８粉末の粒度を調
整することが必要となる。焼結粒子の大きさを調整する
方法としては、一般には機械的粉砕あるいは造粒が採用
される。しかし、これらの機械的方法では設備投資が必
要であったり、原料である酸化処理前のＵＯ２スクラッ
プの特性が直接大きく影響する等の問題がある。Therefore, UO 2 having a stable sintered density
In order to obtain the powder, it is first necessary to adjust the particle size of the U 3 O 8 powder described above. As a method of adjusting the size of the sintered particles, mechanical pulverization or granulation is generally adopted. However, these mechanical methods have problems that they require equipment investment and that the characteristics of UO 2 scrap before oxidation, which is a raw material, have a great influence directly.
【０００６】[0006]
【発明が解決しようとする課題】本発明は、Ｕ３Ｏ８粉
末の粒径を制御するために、従来採用されていた機械的
方法に代る、確実で生産性の優れた新規な方法を提供す
ることをその目的としている。また、本発明の目的は、
ＵＯ２スクラップの酸化回収粉末の粒度を制御する方法
を見い出し、これにより焼結密度およびデンシフィケー
ション値をコントロールすることにある。DISCLOSURE OF THE INVENTION The present invention provides a reliable and highly productive novel method for controlling the particle size of U 3 O 8 powder, which is an alternative to the mechanical method conventionally used. Its purpose is to provide. The object of the present invention is
It is to find a way to control the particle size of the oxidatively recovered powder of UO 2 scrap and thereby control the sintering density and densification value.
【０００７】[0007]
【課題を解決するための手段】本発明者らは、Ｕ３Ｏ８
粉末の平均粒径を制御するためには、まず出発物質であ
るＵＯ２焼結体の平均結晶粒径を調整すれば良いことを
知見した。すなわち、酸化前のＵＯ２焼結ペレットの結
晶粒径と製造されたＵ３Ｏ８粉末の粒径との間にはある
一定の相関関係があることを見い出したのである。The present inventors have found that U 3 O 8
In order to control the average particle size of the powder, it was first found that the average crystal particle size of the starting material UO 2 sintered body should be adjusted. That is, it was found that there is a certain correlation between the crystal grain size of the UO 2 sintered pellet before oxidation and the grain size of the manufactured U 3 O 8 powder.
【０００８】本発明は、下記の事項をその特徴としてい
る。原子燃料用ＵＯ２焼結ペレットのスクラップを回収
して再使用に供するにあたり、酸化雰囲気内で得られる
Ｕ３Ｏ８粉末の粒径を制御するために、前処理として水
素雰囲気中にて処理ボート内に５％程度のＡｌ２Ｏ３お
よびＳｉＯ２の小片を入れてＵＯ２焼結ペレットのスク
ラップを再焼結する、ＵＯ２焼結ペレットの結晶粒径の
制御方法。The present invention is characterized by the following items. In recovering the scrap of UO 2 sintered pellets for nuclear fuel for reuse, in order to control the particle size of the U 3 O 8 powder obtained in an oxidizing atmosphere, a processing boat in a hydrogen atmosphere is used as a pretreatment. A method for controlling the crystal grain size of UO 2 sintered pellets, which comprises re-sintering scraps of UO 2 sintered pellets by putting small pieces of about 5% Al 2 O 3 and SiO 2 inside.
【０００９】以下に、本発明を詳細に説明する。まず、
ＵＯ２焼結体からＵ３Ｏ８粉末を得るための処理工程に
ついて述べる。出発物質であるＵＯ２焼結体は、５００
〜６００℃で１〜２時間、酸化雰囲気中で酸化される。
その酸化のメカニズムは、まず結晶粒界が酸化され、そ
の後、結晶粒内に酸化が進行する。The present invention will be described in detail below. First,
The processing steps for obtaining the U 3 O 8 powder from the UO 2 sintered body will be described. The starting material, UO 2 sintered body, is 500
It is oxidized in an oxidizing atmosphere at ~ 600 ° C for 1-2 hours.
The mechanism of the oxidation is that the crystal grain boundaries are first oxidized and then the oxidation progresses in the crystal grains.
【００１０】図１に示すように、一般的に焼結体は多結
晶体であり、粒界により区分されている。ＵＯ２焼結体
は、２０μｍ程度の結晶粒により構成されている。空気
雰囲気中で酸化が開始されると、粒界にまず酸素が侵入
し、その後粒内に酸素が侵入して酸化が完了する。粒界
に酸素が侵入し、酸化が始まると粒界のＵＯ２がＵ３Ｏ
８に相変化し、体積膨脹して剥がれ落ちる。従って、出
発物質であるＵＯ２焼結体の粒径を制御することによ
り、最終物質であるＵ３Ｏ８の粒径を制御することが出
来る。As shown in FIG. 1, a sintered body is generally a polycrystalline body and is divided by grain boundaries. The UO 2 sintered body is composed of crystal grains of about 20 μm. When the oxidation is started in the air atmosphere, oxygen first enters the grain boundary and then oxygen enters the grain to complete the oxidation. When oxygen enters the grain boundaries and oxidation starts, UO 2 at the grain boundaries becomes U 3 O.
The phase changes to 8 , and the volume expands and peels off. Therefore, by controlling the particle size of the starting material UO 2 sintered body, the particle size of the final material U 3 O 8 can be controlled.
【００１１】ＵＯ２焼結体の結晶粒径は、一般的な原子
燃料の製造パラメータである温度１７００〜１８００
℃、２〜６時間で焼結した場合、平均で１０〜２０μｍ
程度である。従って、結晶粒界に沿って酸化が進行する
と１０〜２０μｍの結晶粒が基本となって、Ｕ３Ｏ８粉
末の平均粒径が決定される。The crystal grain size of the UO 2 sintered body is the temperature 1700 to 1800 which is a manufacturing parameter of general nuclear fuel.
When sintered at 2 ° C for 2 to 6 hours, the average is 10 to 20 μm.
It is a degree. Therefore, when the oxidation progresses along the grain boundaries, the average grain size of the U 3 O 8 powder is determined on the basis of the crystal grains of 10 to 20 μm.
【００１２】出発物質であるＵＯ２焼結体の平均粒径の
制御は再焼結熱処理により達成される。さらに、再焼結
時にＡｌ２Ｏ３およびＳｉＯ２の蒸気が雰囲気中に存在
すれば、その蒸気が粒界から侵入し、結晶粒の成長がよ
り促進される。The control of the average particle size of the starting material UO 2 sintered body is achieved by the re-sintering heat treatment. Furthermore, if vapors of Al 2 O 3 and SiO 2 are present in the atmosphere during re-sintering, the vapors penetrate from grain boundaries and the growth of crystal grains is further promoted.
【００１３】Ｕ３Ｏ８を添加したＵＯ２成形体を水素雰
囲気で焼結すると、Ｕ３Ｏ８がＵＯ２に相変化し、体積
が減少する。これはＵ３Ｏ８が気孔形成剤になり得るこ
とを意味している。気孔形成剤により出来上がった気孔
は、そのサイズにより原子炉内で挙動の違いを表す。す
なわち、サイズの小さい（一般的に、数μｍ）気孔は消
滅しやすく、その結果、原子炉内燃焼時に収縮する減
少、すなわち、焼きしまり（デンシフィケーション）が
発生する。この現象はペレットから被覆管への熱伝達の
低下や被覆管のつぶれ（コラップス）を誘発するので好
ましくない。粒径を制御されたものは４４μｍ以下の粉
末が少なくなっているので、微細な気孔の発生が抑制さ
れ、品質の向上につながる。[0013] sintering U 3 O 8 UO 2 moldings was added in a hydrogen atmosphere, U 3 O 8 is phase-changed into UO 2, volume decreases. This means that U 3 O 8 can be a pore-forming agent. The pores created by the pore-forming agent show different behavior in the reactor depending on their size. That is, small-sized pores (generally, a few μm) are likely to disappear, and as a result, a decrease in shrinkage during combustion in a nuclear reactor, that is, densification occurs. This phenomenon is unfavorable because it induces a decrease in heat transfer from the pellets to the cladding and collapse of the cladding (collapse). Since the amount of powder having a controlled particle size is less than 44 μm, the generation of fine pores is suppressed, which leads to an improvement in quality.
【００１４】[0014]
【実施例】以下、本発明を実施例により説明する。従来
法により、出発物質として、１７９０℃で４時間焼結し
たＵＯ２焼結体を用意した。この焼結体の平均結晶粒径
は１５μｍであった。次いで、この焼結体を５００℃で
２時間、空気雰囲気中で酸化し、得られたＵ３Ｏ８粉末
を７４μｍ以下のふるいにかけて粉度分布を測定した。
その結果を、図２に示す。The present invention will be described below with reference to examples. According to the conventional method, a UO 2 sintered body that was sintered at 1790 ° C. for 4 hours was prepared as a starting material. The average crystal grain size of this sintered body was 15 μm. Next, this sintered body was oxidized at 500 ° C. for 2 hours in an air atmosphere, and the obtained U 3 O 8 powder was passed through a sieve of 74 μm or less to measure the fineness distribution.
The result is shown in FIG.
【００１５】本発明法により、１７９０℃で８時間、水
素ガス雰囲気中で、かつ容器内のＵＯ２量に対し５％の
Ａｌ２Ｏ３とＳｉＯ２片と共に熱処理して、ＵＯ２焼結
体を得た。この焼結体の平均結晶粒径は３０μｍであっ
た。次いで、この焼結体を５００℃で２時間、空気雰囲
気中で酸化し、得られたＵ３Ｏ８粉末を７４μｍ以下の
ふるいにかけて粒度分布を測定した。その結果を、図３
に示す。According to the method of the present invention, heat treatment was performed at 1790 ° C. for 8 hours in a hydrogen gas atmosphere together with 5% Al 2 O 3 and SiO 2 pieces with respect to the amount of UO 2 in the container to obtain a UO 2 sintered body. Got The average crystal grain size of this sintered body was 30 μm. Next, this sintered body was oxidized at 500 ° C. for 2 hours in an air atmosphere, and the obtained U 3 O 8 powder was passed through a sieve of 74 μm or less to measure the particle size distribution. The result is shown in FIG.
Shown in
【００１６】以下に、図２と図３を比較する。図２から
分るように、粒径の制御をしていないＵＯ２焼結体を酸
化した粉末の粒径はバラツキが大きい。これは出発物質
であるＵＯ２の結晶粒の分布にバラツキがあり、微細な
結晶粒が多く存在していることを示している。一方、図
３から分るように、本発明法により、焼結体の結晶粒径
を制御すると、微細な結晶粒がなくなり、最終物質であ
るＵ３Ｏ８粉末の粒度分布が均一化する。Below, FIG. 2 and FIG. 3 are compared. As can be seen from FIG. 2, the particle size of the powder obtained by oxidizing the UO 2 sintered body whose particle size is not controlled varies greatly. This indicates that the distribution of the crystal grains of UO 2 which is the starting material varies and that many fine crystal grains are present. On the other hand, as can be seen from FIG. 3, when the crystal grain size of the sintered body is controlled by the method of the present invention, fine crystal grains disappear, and the grain size distribution of the final substance, U 3 O 8 powder, becomes uniform.
【発明の効果】本発明により、微細な結晶粒粉末が少な
くなり、かつ密度コントロールも安定的であり、核燃料
ペレットの品質向上に有益である。更に、粒度制御のた
めの粉砕機等への投資も不要となり、その経済効果も大
きい。Industrial Applicability According to the present invention, the amount of fine crystal grain powder is reduced and the density control is stable, which is useful for improving the quality of nuclear fuel pellets. Further, there is no need to invest in a crusher or the like for controlling the particle size, which has a large economic effect.
【図１】ＵＯ２焼結体における酸化のメカニズムを示し
た説明図である。FIG. 1 is an explanatory diagram showing a mechanism of oxidation in a UO 2 sintered body.
【図２】従来法により製造した粉末の粒度分布を示した
グラフである。FIG. 2 is a graph showing a particle size distribution of a powder manufactured by a conventional method.
【図３】本発明法により製造した粉末の粒度分布を示し
たグラフである。FIG. 3 is a graph showing the particle size distribution of the powder produced by the method of the present invention.
Claims (2)
プを回収して再使用に供するにあたり、酸化雰囲気内で
得られるＵ３Ｏ８粉末の粒径を制御するために、前処理
として水素雰囲気中で処理ボート内にＡｌ２Ｏ３とＳｉ
Ｏ２の小片を入れてＵＯ２焼結ペレットのスクラップを
再焼結することを特徴とする、ＵＯ２焼結ペレットの結
晶粒径の制御方法。1. A hydrogen atmosphere as a pretreatment for controlling the particle size of U 3 O 8 powder obtained in an oxidizing atmosphere when scrap of UO 2 sintered pellets for nuclear fuel is collected and reused. Al 2 O 3 and Si in the processing boat in
Put a small piece of O 2, characterized in that re-sintering scrap UO 2 sintered pellets, method of controlling the crystal grain size of UO 2 sintered pellets.
の全量に対し５％であることを特徴とする、請求項１に
記載のＵＯ２焼結ペレットの結晶粒径の制御方法。 2. The amount of small pieces of Al 2 O 3 and SiO 2 is UO 2
Wherein the of based on the total amount is 5%, the control method of the crystal grain size of UO 2 sintered pellet according to claim 1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7199906A JP3071671B2 (en) | 1995-08-04 | 1995-08-04 | Method of controlling grain size of UO2 sintered pellet |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7199906A JP3071671B2 (en) | 1995-08-04 | 1995-08-04 | Method of controlling grain size of UO2 sintered pellet |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0949892A true JPH0949892A (en) | 1997-02-18 |
| JP3071671B2 JP3071671B2 (en) | 2000-07-31 |
Family
ID=16415579
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP7199906A Expired - Fee Related JP3071671B2 (en) | 1995-08-04 | 1995-08-04 | Method of controlling grain size of UO2 sintered pellet |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3071671B2 (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100794071B1 (en) * | 2006-12-05 | 2008-01-10 | 한국원자력연구원 | Method of producing nuclear fuel pellet |
| KR100832567B1 (en) * | 2006-12-05 | 2008-05-27 | 한국원자력연구원 | Method of producing large-grained nuclear fuel pellet |
| US9190179B2 (en) | 2010-10-20 | 2015-11-17 | Korea Atomic Energy Research Institute | Method of controlling solubility of additives at and near grain boundaries, and method of manufacturing sintered nuclear fuel pellet having large grain size using the same |
-
1995
- 1995-08-04 JP JP7199906A patent/JP3071671B2/en not_active Expired - Fee Related
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR100794071B1 (en) * | 2006-12-05 | 2008-01-10 | 한국원자력연구원 | Method of producing nuclear fuel pellet |
| KR100832567B1 (en) * | 2006-12-05 | 2008-05-27 | 한국원자력연구원 | Method of producing large-grained nuclear fuel pellet |
| US9190179B2 (en) | 2010-10-20 | 2015-11-17 | Korea Atomic Energy Research Institute | Method of controlling solubility of additives at and near grain boundaries, and method of manufacturing sintered nuclear fuel pellet having large grain size using the same |
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| JP3071671B2 (en) | 2000-07-31 |
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