JP3434091B2 - How to treat spent nuclear fuel - Google Patents
How to treat spent nuclear fuelInfo
- Publication number
- JP3434091B2 JP3434091B2 JP19953195A JP19953195A JP3434091B2 JP 3434091 B2 JP3434091 B2 JP 3434091B2 JP 19953195 A JP19953195 A JP 19953195A JP 19953195 A JP19953195 A JP 19953195A JP 3434091 B2 JP3434091 B2 JP 3434091B2
- Authority
- JP
- Japan
- Prior art keywords
- nuclear fuel
- uranium
- nitrogen
- spent nuclear
- fuel
- 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 - Fee Related
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
-
- 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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
Landscapes
- Inorganic Compounds Of Heavy Metals (AREA)
Description
【０００１】[0001]
【発明の属する技術分野】本発明は原子炉で使用した核
燃料（使用済核燃料）の処理方法に関する。TECHNICAL FIELD The present invention relates to a method for treating nuclear fuel (spent nuclear fuel) used in a nuclear reactor.
【０００２】[0002]
【従来の技術】従来、原子炉で使用した使用済核燃料を
加熱して気体と接触することにより、該核燃料中の不純
物を分離する方法としては、主成分がウラン酸化物であ
るペレット状の燃料に対して、酸素を含む気体と水素を
含む気体を交互に接触させる方法が知られている。この
技術は、 Nuclear Technology 誌第４１巻１３７〜１４
８頁で紹介され公知となっている。2. Description of the Related Art Conventionally, as a method for separating impurities in a nuclear fuel by heating spent nuclear fuel used in a nuclear reactor and contacting it with a gas, a pellet fuel containing uranium oxide as a main component is used. On the other hand, a method is known in which a gas containing oxygen and a gas containing hydrogen are alternately contacted. This technology is known as Nuclear Technology, Vol. 41, 137-14.
It is introduced on page 8 and is publicly known.
【０００３】[0003]
【発明が解決しようとする問題点】上記した従来の使用
済核燃料の処理方法では、ペレット状の酸化物燃料のみ
が対象となっており、原子炉で使用した使用済核燃料の
主成分がウラン窒化物であるときには、該核燃料に含ま
れるウランの化学的または物理的形態変化による体積膨
張と収縮が十分に生起しないため、該核燃料から水素、
ヘリウム、クリプトン、キセノン、ヨウ素を分離するこ
とができないという問題があり、またウラン窒化物燃料
から生じた窒素を回収して再利用できないという問題も
あった。更に、窒化物として核燃料中に含まれるネプツ
ニウム、プルトニウム及びアメリシウムを再び原子炉で
利用するためには、ウラン窒化物燃料を硝酸または溶融
塩に溶解した後に湿式法または乾式法による使用済核燃
料の再処理を行い、該核燃料中に含まれるネプツニウ
ム、プルトニウム及びアメリシウムをウランと分離して
回収する必要があるため処理が複雑になるとの問題があ
った。The above-mentioned conventional method for treating spent nuclear fuel is intended only for pelletized oxide fuel, and the main component of spent nuclear fuel used in the nuclear reactor is uranium nitriding. When it is a substance, since the volume expansion and contraction due to the chemical or physical shape change of uranium contained in the nuclear fuel do not sufficiently occur, hydrogen from the nuclear fuel,
There was a problem that helium, krypton, xenon, and iodine could not be separated, and that nitrogen generated from uranium nitride fuel could not be recovered and reused. Furthermore, in order to reuse the neptunium, plutonium and americium contained in the nuclear fuel as nitrides in the nuclear reactor again, after dissolving the uranium nitride fuel in nitric acid or molten salt, the spent nuclear fuel is regenerated by the wet method or the dry method. There is a problem that the process becomes complicated because it is necessary to separate and recover the neptunium, plutonium and americium contained in the nuclear fuel from the uranium.
【０００４】[0004]
【課題を解決するための手段】本発明は（１）主成分が
ウラン窒化物であるペレット状または球状の使用済核燃
料を加熱した状態で、水蒸気と酸素を含む気体と反応さ
せた後、水素を含む気体と反応させ、核燃料に含まれる
ウランの化学的または物理的形態変化による体積膨張と
収縮を生起させて、該核燃料中の水素、ヘリウム、クリ
プトン、キセノン、ヨウ素、窒素を分離することを特徴
とする使用済核燃料の処理方法（第１発明）、（２）上
記（１）記載の処理方法で分離された水素、ヘリウム、
クリプトン、キセノン、ヨウ素、窒素等を混合気体から
物理的または化学的分離方法により窒素を回収すること
を特徴とする使用済核燃料の処理方法（第２発明）、
（３）上記（１）記載の処理方法により使用済核燃料を
処理し、該核燃料中に含まれるネプツニウム、プルトニ
ウム及びアメリシウムをウランと分離することなく、燃
料として再加工し、再び原子炉で使用する使用済核燃料
の処理方法（第３発明）である。According to the present invention, (1) a pellet-shaped or spherical spent nuclear fuel whose main component is uranium nitride is heated and reacted with a gas containing water vapor and oxygen, and then hydrogen. Of hydrogen, helium, krypton, xenon, iodine, and nitrogen in the nuclear fuel by causing a volume expansion and contraction of the uranium contained in the nuclear fuel due to a chemical or physical shape change of the uranium. Characteristic spent nuclear fuel treatment method (first invention), (2) hydrogen and helium separated by the treatment method described in (1) above,
A method for treating spent nuclear fuel, which comprises recovering nitrogen from a mixed gas by physical or chemical separation of krypton, xenon, iodine, nitrogen and the like (second invention),
(3) The spent nuclear fuel is treated by the treatment method described in (1) above, and the neptunium, plutonium and americium contained in the nuclear fuel are reprocessed as fuel without being separated from uranium and used again in a nuclear reactor. It is a method for treating spent nuclear fuel (third invention).
【０００５】本発明をさらに詳述するに、原子炉で使用
した主成分がウラン窒化物であるペレット状または顆粒
状の使用済核燃料を加熱した状態で、まず水蒸気と酸素
の混合気体と反応させる処理を行い、該核燃料に含まれ
るウランを気体中で窒化物から主成分はＵ3 Ｏ8 で部分
的にＵＯ2 を含む酸化物へ変化させ、この際の体積膨張
により最初直径：０．５〜２ｃｍ、長さ：０．５〜３ｃ
ｍのペレット状または直径：１μｍ〜２ｍｍの球状の該
核燃料を部分的に粉砕する。この処理過程で該核燃料に
含まれていた水素、ヘリウム、クリプトン、キセノン、
ヨウ素、窒素が気体中に移行するため、気体中の窒素は
再使用のために回収する。次に、部分的に粉砕された前
記核燃料を加熱した状態で水素を含む気体と反応させ、
核燃料に含まれるウランをＵＯ2 に還元し、この際の体
積の収縮により核燃料の粉砕を進展するとともに、水
素、ヘリウム、クリプトン、キセノン、ヨウ素、窒素の
気体中への移行を促進し、また、核燃料の再加工に適し
た原料を得る。この処理過程においても、核燃料に含ま
れていた水素、ヘリウム、クリプトン、キセノン、ヨウ
素、窒素が気体中に移行するため、気体中の窒素化合物
を再使用のために回収する。この処理により、核燃料中
に含まれるネプツニウム、プルトニウム及びアメリシウ
ムはウランとともに酸化物として得ることができるもの
である。To explain the present invention in more detail, pelletized or granular spent nuclear fuel whose main component is uranium nitride used in a nuclear reactor is first reacted with a mixed gas of steam and oxygen in a heated state. performs processing, the main component of a nitride uranium contained in the nucleic fuel in gas is changed to oxides containing partially UO 2 with U 3 O 8, the first diameter by volume expansion at this time: 0.5 ~ 2cm, length: 0.5-3c
m of pellet or diameter: 1 μm to 2 mm of spherical nuclear fuel is partially crushed. Hydrogen, helium, krypton, xenon, which were contained in the nuclear fuel during this treatment process,
Since iodine and nitrogen are transferred to the gas, the nitrogen in the gas is recovered for reuse. Next, the partially crushed nuclear fuel is reacted with a gas containing hydrogen in a heated state,
The uranium contained in the nuclear fuel is reduced to UO 2 , and the contraction of the volume at this time progresses the pulverization of the nuclear fuel and promotes the transfer of hydrogen, helium, krypton, xenon, iodine and nitrogen into the gas. Obtain raw materials suitable for reprocessing nuclear fuel. Also in this process, hydrogen, helium, krypton, xenon, iodine, and nitrogen contained in the nuclear fuel are transferred into the gas, so that the nitrogen compound in the gas is recovered for reuse. By this treatment, neptunium, plutonium and americium contained in the nuclear fuel can be obtained as oxides together with uranium.
【０００６】[0006]
【発明の実施の形態】本発明の第１発明によれば、原子
炉で使用されたウラン窒化物に水蒸気と酸素の混合気体
を作用させることにより、窒化ウラン（ＵＮ）が迅速に
水蒸気と反応してウラン酸化物となり、このウラン酸化
物が酸素により酸化され最終的にＵ3Ｏ8 となるもので
あり、１４．３ｇ／ｃｍ3 の理論密度をもつＵＮが８．
３８の理論密度しかもたないＵ3 Ｏ8 に変化する際の約
７０％の体積膨張によりペレット状や顆粒状の核燃料の
破砕が進み、燃料中に含まれる水素、ヘリウム、クリプ
トン、キセノン、ヨウ素、窒素の気体中への移行を促進
するものである。破砕の程度は酸素添加量により変化
し、反応生成物がＵＯ2 であるかＵ3 Ｏ8 であるかによ
り、理論密度比で約３０％から約７０％の間で可変とで
きる。ウラン窒化物に水蒸気と酸素の混合気体を作用さ
せて製造したＵＯ2 とＵ3 Ｏ8 の混合物に水素を含む気
体を作用させてＵＯ2 とすることにより最大の理論密度
比で約２０％の収縮を起こし、ペレット状や顆粒状の核
燃料の破砕が進み、燃料中に含まれる水素、ヘリウム、
クリプトン、キセノン、ヨウ素、窒素の気体中への移行
を更に促進する。BEST MODE FOR CARRYING OUT THE INVENTION According to the first aspect of the present invention, uranium nitride (UN) reacts rapidly with steam by causing a mixed gas of steam and oxygen to act on uranium nitride used in a nuclear reactor. The resulting uranium oxide is the uranium oxide that is oxidized by oxygen to finally become U 3 O 8, and UN having a theoretical density of 14.3 g / cm 3 is 8.
Due to the volume expansion of about 70% when changing to U 3 O 8 having only a theoretical density of 38, crushing of pelletized or granular nuclear fuel progresses, and hydrogen, helium, krypton, xenon, iodine contained in the fuel, It promotes the transfer of nitrogen into the gas. The degree of crushing varies depending on the amount of oxygen added, and can be varied between about 30% and about 70% in theoretical density ratio depending on whether the reaction product is UO 2 or U 3 O 8 . A mixture of UO 2 and U 3 O 8 produced by reacting a mixed gas of steam and oxygen on uranium nitride is treated with a gas containing hydrogen to form UO 2, and the maximum theoretical density ratio is about 20%. Due to contraction, the pelletized or granular nuclear fuel is crushed, and hydrogen, helium,
It further promotes the transfer of krypton, xenon, iodine and nitrogen into gas.
【０００７】本発明の第２発明によれば、核燃料中に窒
素化合物として含まれていた窒素は水蒸気と酸素の混合
気体と反応することによりＮ2 、ＮＨ3 または窒素酸化
物として気相中に移行するため、これを回収して再利用
に供することができる。また、本発明の第３発明によれ
ば、核燃料中に含まれるネプツニウム、プルトニウム及
びアメリシウムはウランとともに十分に蒸気圧が低いた
め固相中に残り、酸化物として得ることができるもので
ある。このためネプツニウム、プルトニウム及びアメリ
シウムは、ウランとともに酸化物粉末として核燃料とし
て再利用可能となる。According to the second aspect of the present invention, nitrogen contained as a nitrogen compound in nuclear fuel reacts with a mixed gas of water vapor and oxygen to form N 2 , NH 3 or a nitrogen oxide in the gas phase. Since it is transferred, it can be collected and reused. Further, according to the third aspect of the present invention, neptunium, plutonium and americium contained in the nuclear fuel, together with uranium, have a sufficiently low vapor pressure that they remain in the solid phase and can be obtained as oxides. Therefore, neptunium, plutonium and americium can be reused as nuclear fuel as oxide powder together with uranium.
【０００８】[0008]
（例１）図１は本発明の第１発明及び第２発明に係わる
処理の流れを示す。１は発電または核変換を目的とする
原子炉であり、ここでは主成分がウラン窒化物である直
径：０．５〜２ｃｍ、長さ：０．５〜３ｃｍのペレット
状または直径：１μｍ〜２ｍｍの球状の使用済核燃料２
が使用されている。使用済核燃料２を反応容器３の中で
加熱し、水蒸気と酸素を含む気体４と反応させる。次
に、同一の反応容器３または別の反応容器５の中で核燃
料を加熱し、水素を含む気体６と反応させる。核燃料中
の水素、ヘリウム、クリプトン、キセノン、ヨウ素、窒
素はオフガス７中に９９〜１００％移行し反応容器３ま
たは５よりのオフガス７として回収する。上記の処理に
よると、使用済核燃料２を反応容器３中で水蒸気と酸素
を含む気体４と反応させる際の使用済核燃料２の体積膨
張により、該燃料２の被覆管の物理的破砕を行うことも
可能であり、オフガス７に含まれる水素、ヘリウム、ク
リプトン、キセノン、ヨウ素、窒素等の混合気体から物
理的または化学的分離方法８により窒素を回収する。(Example 1) FIG. 1 shows a processing flow according to the first and second aspects of the invention. Reference numeral 1 denotes a nuclear reactor for the purpose of power generation or transmutation, in which the main component is uranium nitride, diameter: 0.5 to 2 cm, length: 0.5 to 3 cm pellet or diameter: 1 μm to 2 mm Spherical spent nuclear fuel 2
Is used. The spent nuclear fuel 2 is heated in the reaction container 3 and reacted with the gas 4 containing water vapor and oxygen. Next, the nuclear fuel is heated in the same reaction container 3 or another reaction container 5 and reacted with the gas 6 containing hydrogen. Hydrogen, helium, krypton, xenon, iodine, and nitrogen in the nuclear fuel are transferred to the offgas 7 by 99 to 100% and recovered as the offgas 7 from the reaction vessel 3 or 5. According to the above processing, the physical expansion of the cladding of the spent nuclear fuel 2 is performed by the volume expansion of the spent nuclear fuel 2 when the spent nuclear fuel 2 is reacted with the gas 4 containing water vapor and oxygen in the reaction vessel 3. It is also possible to recover nitrogen from the mixed gas of hydrogen, helium, krypton, xenon, iodine, nitrogen, etc. contained in the offgas 7 by the physical or chemical separation method 8.
【０００９】（例２）図２は本発明の第３発明に係わる
実施例を示すものである。９は発電または核変換を目的
とする原子炉であり、ここでは主成分がウラン窒化物で
ある直径：０．５〜２ｃｍ、長さ：０．５〜３ｃｍのペ
レット状または直径：１μｍ〜２ｍｍの球状の使用済核
燃料１０が使用されている。使用済核燃料１０に含まれ
るネプツニウム、プルトニウム及びアメリシウムをウラ
ンと分離することなく、図１に示す処理工程１１で処理
した後、燃料として振動充填法等により燃料の再加工施
設１２で再加工し、再び原子炉９で利用することができ
る。(Example 2) FIG. 2 shows an embodiment according to the third invention of the present invention. Reference numeral 9 denotes a nuclear reactor for the purpose of power generation or transmutation, in which the main component is uranium nitride, diameter: 0.5 to 2 cm, length: 0.5 to 3 cm pellet or diameter: 1 μm to 2 mm The spherical spent nuclear fuel 10 is used. Neptunium, plutonium and americium contained in the spent nuclear fuel 10 are processed in the processing step 11 shown in FIG. 1 without being separated from uranium, and then reprocessed in the fuel reprocessing facility 12 as a fuel by a vibration filling method, It can be used again in the nuclear reactor 9.
【００１０】[0010]
【発明の効果】
（１）本発明によれば、原子炉で使用した主成分がウラ
ン窒化物である直径：０．５〜１ｍｍ、長さ：０．５〜
３ｃｍのペレット状または直径：１μｍ〜２ｍｍの球状
の使用済核燃料から、硝酸や溶融塩で溶解する処理を行
わずに核燃料中の水素、ヘリウム、クリプトン、キセノ
ン、ヨウ素、窒素を分離できるため、従来の処理工程を
簡単化でき、処理設備を単純化できる効果がある。ま
た、従来の処理に伴って発生する硝酸溶液や溶融塩等の
液体状の放射性２次廃棄物が発生しない効果がある。EFFECTS OF THE INVENTION (1) According to the present invention, the main component used in a nuclear reactor is uranium nitride. Diameter: 0.5-1 mm, length: 0.5-
Since it is possible to separate hydrogen, helium, krypton, xenon, iodine, and nitrogen in nuclear fuel from spent nuclear fuel in the form of pellets with a diameter of 3 cm or spherical particles with a diameter of 1 μm to 2 mm without performing treatment to dissolve with nitric acid or molten salt, This has the effect of simplifying the processing steps of and the processing equipment. Further, there is an effect that liquid radioactive secondary waste such as nitric acid solution and molten salt generated by the conventional treatment is not generated.
【００１１】（２）また、本発明によれば、原子炉で使
用したウラン等の窒化物中の窒素を気体中に回収するこ
とができ、窒素の再利用がきわめて容易となる効果があ
る。(2) Further, according to the present invention, the nitrogen in the nitride such as uranium used in the nuclear reactor can be recovered into the gas, and there is an effect that the recycling of the nitrogen is extremely easy.
【００１２】（３）更に本発明によれば、原子炉で使用
した主成分がウラン窒化物である直径：０．５〜２ｃ
ｍ、長さ：０．５〜３ｃｍのペレット状または直径：１
μｍ〜２ｍｍの球状の使用済核燃料中に含まれるネプツ
ニウム、プルトニウム及びアメリシウムをウランと分離
することなく、燃料として再加工できるため、核拡散抵
抗性に優れた核燃料のリサイクル形態を構築することが
できる効果がある。(3) Further according to the present invention, the main component used in the nuclear reactor is uranium nitride Diameter: 0.5-2c
m, length: 0.5-3 cm pellets or diameter: 1
Neptunium, plutonium and americium contained in spherical nuclear fuel with a diameter of μm to 2 mm can be reprocessed as fuel without separation from uranium, and thus a nuclear fuel recycling form with excellent nuclear diffusion resistance can be constructed. effective.
【図１】本発明の一実施例に係わる流れ図。FIG. 1 is a flow chart according to an embodiment of the present invention.
【図２】本発明の他の一実施例に係わる流れ図。FIG. 2 is a flowchart according to another embodiment of the present invention.
フロントページの続き (72)発明者 波多野 守 東京都千代田区丸の内二丁目５番１号 三菱重工業株式会社本社内 (56)参考文献 特開 平６−94888（ＪＰ，Ａ) ＲＡＭＡ ＲＡＯ Ｇ Ａ， ＭＵＫ ＥＲＪＥＥ Ｓ Ｋ， ＶＡＩＤＹＡ Ｖ Ｎ， ＶＥＮＵＧＯＰＡＬ Ｖ， ＳＯＯＤ Ｄ Ｄ，Ｏｘｉｄａｔｉｏｎ ａｎｄ ｈｙｄｒｏｌｙｓｉｓ ｋｉ ｎｅｔｉｃ ｓｔｕｄｉｅｓ ｏｎ Ｕ Ｎ，Ｊｏｕｒｎａｌ ｏｆ Ｎｕｃｌｅ ａｒ Ｍａｔｅｒｉａｌｓ，ＮＬ，1991 年11月，Ｖｏｌ．185 Ｎｏ．２，Ｐ231 −241 (58)調査した分野(Int.Cl.7，ＤＢ名) G21C 19/44 Front Page Continuation (72) Inventor Mamoru Hatano 2-5-1, Marunouchi, Chiyoda-ku, Tokyo Mitsubishi Heavy Industries, Ltd. Head office (56) Reference JP-A-6-94888 (JP, A) RAMA RAO GA, MUK ERJEE SK, VAIDYA VN, VENUGOPAL V, SOOD D D, Oxidation and hydrolysis ki netiques on U N, Journal of Nuclear, 11th November, 11th November, November 1 Material. 185 No. 2, P231-241 (58) Fields investigated (Int.Cl. 7 , DB name) G21C 19/44
Claims (3)
または球状の使用済核燃料を加熱した状態で、水蒸気と
酸素を含む気体と反応させた後、水素を含む気体と反応
させ、核燃料に含まれるウランの化学的または物理的形
態変化による体積膨張と収縮を生起させて、該核燃料中
の水素、ヘリウム、クリプトン、キセノン、ヨウ素、窒
素を分離することを特徴とする使用済核燃料の処理方
法。1. A pelletized or spherical spent nuclear fuel whose main component is uranium nitride is heated and reacted with a gas containing water vapor and oxygen, and then with a gas containing hydrogen to be contained in the nuclear fuel. A method for treating spent nuclear fuel, characterized in that hydrogen, helium, krypton, xenon, iodine and nitrogen in the nuclear fuel are separated by causing volume expansion and contraction of uranium due to a change in chemical or physical form.
素、ヘリウム、クリプトン、キセノン、ヨウ素、窒素等
の混合気体から物理的または化学的分離方法により窒素
を回収することを特徴とする使用済核燃料の処理方法。2. A use characterized by recovering nitrogen from a mixed gas of hydrogen, helium, krypton, xenon, iodine, nitrogen and the like separated by the treatment method according to claim 1 by a physical or chemical separation method. How to treat spent nuclear fuel.
燃料を処理し、該核燃料中に含まれるネプツニウム、プ
ルトニウム及びアメリシウムをウランと分離することな
く、燃料として再加工し、再び原子炉で使用する使用済
核燃料の処理方法。3. A spent nuclear fuel is treated by the treatment method according to claim 1, and neptunium, plutonium and americium contained in the nuclear fuel are reprocessed as fuel without being separated from uranium, and used again in a nuclear reactor. Spent nuclear fuel treatment method.
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| JP19953195A JP3434091B2 (en) | 1995-08-04 | 1995-08-04 | How to treat spent nuclear fuel |
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|---|---|
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| JP3434091B2 true JP3434091B2 (en) | 2003-08-04 |
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Non-Patent Citations (1)
| Title |
|---|
| ＲＡＭＡ ＲＡＯ Ｇ Ａ， ＭＵＫＥＲＪＥＥ Ｓ Ｋ， ＶＡＩＤＹＡ Ｖ Ｎ， ＶＥＮＵＧＯＰＡＬ Ｖ， ＳＯＯＤ Ｄ Ｄ，Ｏｘｉｄａｔｉｏｎ ａｎｄ ｈｙｄｒｏｌｙｓｉｓ ｋｉｎｅｔｉｃ ｓｔｕｄｉｅｓ ｏｎ ＵＮ，Ｊｏｕｒｎａｌ ｏｆ Ｎｕｃｌｅａｒ Ｍａｔｅｒｉａｌｓ，ＮＬ，１９９１年１１月，Ｖｏｌ．１８５ Ｎｏ．２，Ｐ２３１−２４１ |
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| JPH0943390A (en) | 1997-02-14 |
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