JP2018511037A - 原子炉の冷却システムで金属表面を除染する方法 - Google Patents
原子炉の冷却システムで金属表面を除染する方法 Download PDFInfo
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- 229910052751 metal Inorganic materials 0.000 title claims abstract description 28
- 239000002184 metal Substances 0.000 title claims abstract description 28
- 230000003647 oxidation Effects 0.000 claims abstract description 135
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 135
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- 150000004706 metal oxides Chemical class 0.000 claims abstract description 24
- MUBZPKHOEPUJKR-UHFFFAOYSA-N oxalic acid group Chemical group C(C(=O)O)(=O)O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000007864 aqueous solution Substances 0.000 claims abstract description 19
- 150000007524 organic acids Chemical class 0.000 claims abstract description 18
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims abstract description 12
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- RGHNJXZEOKUKBD-UHFFFAOYSA-N D-gluconic acid Natural products OCC(O)C(O)C(O)C(O)C(O)=O RGHNJXZEOKUKBD-UHFFFAOYSA-N 0.000 claims abstract description 4
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- 229910021645 metal ion Inorganic materials 0.000 description 8
- 230000008859 change Effects 0.000 description 7
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- BFGKITSFLPAWGI-UHFFFAOYSA-N chromium(3+) Chemical compound [Cr+3] BFGKITSFLPAWGI-UHFFFAOYSA-N 0.000 description 5
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 4
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- 238000009835 boiling Methods 0.000 description 4
- 229910052804 chromium Inorganic materials 0.000 description 4
- JOPOVCBBYLSVDA-UHFFFAOYSA-N chromium(6+) Chemical compound [Cr+6] JOPOVCBBYLSVDA-UHFFFAOYSA-N 0.000 description 4
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- 238000000354 decomposition reaction Methods 0.000 description 2
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- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 229910001293 incoloy Inorganic materials 0.000 description 2
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- 230000007246 mechanism Effects 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
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- ZCDOYSPFYFSLEW-UHFFFAOYSA-N chromate(2-) Chemical compound [O-][Cr]([O-])(=O)=O ZCDOYSPFYFSLEW-UHFFFAOYSA-N 0.000 description 1
- KRVSOGSZCMJSLX-UHFFFAOYSA-L chromic acid Substances O[Cr](O)(=O)=O KRVSOGSZCMJSLX-UHFFFAOYSA-L 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
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- AWJWCTOOIBYHON-UHFFFAOYSA-N furo[3,4-b]pyrazine-5,7-dione Chemical compound C1=CN=C2C(=O)OC(=O)C2=N1 AWJWCTOOIBYHON-UHFFFAOYSA-N 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
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- 238000011065 in-situ storage Methods 0.000 description 1
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C17/00—Monitoring; Testing ; Maintaining
- G21C17/02—Devices or arrangements for monitoring coolant or moderator
- G21C17/022—Devices or arrangements for monitoring coolant or moderator for monitoring liquid coolants or moderators
- G21C17/0225—Chemical surface treatment, e.g. corrosion
-
- 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
- G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
- G21F9/002—Decontamination of the surface of objects with chemical or electrochemical processes
- G21F9/004—Decontamination of the surface of objects with chemical or electrochemical processes of metallic surfaces
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23G—CLEANING OR DE-GREASING OF METALLIC MATERIAL BY CHEMICAL METHODS OTHER THAN ELECTROLYSIS
- C23G1/00—Cleaning or pickling metallic material with solutions or molten salts
- C23G1/02—Cleaning or pickling metallic material with solutions or molten salts with acid solutions
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23G—CLEANING OR DE-GREASING OF METALLIC MATERIAL BY CHEMICAL METHODS OTHER THAN ELECTROLYSIS
- C23G1/00—Cleaning or pickling metallic material with solutions or molten salts
- C23G1/28—Cleaning or pickling metallic material with solutions or molten salts with molten salts
-
- 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
- G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
-
- 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
-
- 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
- G21F9/28—Treating solids
-
- 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
- G21F9/28—Treating solids
- G21F9/30—Processing
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C19/00—Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
- G21C19/28—Arrangements for introducing fluent material into the reactor core; Arrangements for removing fluent material from the reactor core
-
- 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
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- Life Sciences & Earth Sciences (AREA)
- General Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Plasma & Fusion (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Cleaning By Liquid Or Steam (AREA)
- Cleaning And De-Greasing Of Metallic Materials By Chemical Methods (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Apparatus For Disinfection Or Sterilisation (AREA)
Abstract
Description
a)ラジオアイソトープを含む金属酸化物を過マンガン酸塩オキシダントの水溶液と接触させる酸化工程(oxidation step)、
b)金属酸化物の少なくとも一部およびラジオアイソトープを溶解させるために、前記酸化工程に付された金属酸化物を、シュウ酸、ギ酸、クエン酸、酒石酸、ピコリン酸、グルコン酸、グリオキシル酸およびそれらの混合物から成る群から選択される有機酸の水溶液と接触させる除染工程(decontamination step)、ならびに、
c)少なくともラジオアイソトープをイオン交換樹脂に固定化する洗浄工程(cleaning step)
を含んで成る除染方法である。
前記酸化工程は、同じまたは異なる処理サイクルの中で次々に実施される、少なくとも1つの酸性の酸化工程(酸性条件下における酸化工程)および少なくとも1つのアルカリ性の酸化工程(アルカリ条件下における酸化工程)を含んで成り、ならびに、前記複数の処理サイクルは、高温酸化工程を含む少なくとも1つの処理サイクルを含んで成り、該高温酸化工程において、オキシダント溶液が少なくとも100℃の温度に保持され、ならびに、高温酸化工程の間、少なくとも1つのリアクター・クーラント・ポンプが主ループ内部でオキシダント溶液を循環および加熱するために用いられ、ならびに残留熱除去システムが、オキシダント溶液の温度を制御するために用いられる。
本実験において、加圧水型原子炉の蒸気発電機からの汚染されたチューブの部位を使用した。各部位は、4×3.5cmの寸法、表面積14cm2を有した2つのサンプルを供するために、長手方向に切断された。それらチューブおよびサンプルは、InconelTM600から成るものであった。サンプルの初期の表面活性は、2.7×103Bq/cm2であった。
同様の実験を、処理サイクルの数の減少に関して、高温酸化工程を含んで成る処理サイクルの性能を示すために実施した。実施例1の2つのサンプルは、全ての処理サイクルで高温酸化工程を用いて実施することを除いては、実施例1で示したのと同一の条件で、合計3つの処理サイクルに付された。さらに、サンプル1は、アルカリ性の酸化工程を含んで成る第1の処理サイクルに付され、続いて、各々酸性の酸化工程を含んで成る2つの処理サイクルに付された。サンプル2は、アルカリ性の条件下での金属酸化物の酸化を含んで成る処理サイクルに続けて、酸性の酸化工程と、後続するアルカリ性の酸化工程を含んで成る処理サイクルとなるように、アルカリ性および酸性の酸化工程を交互に用いる処理サイクルに付された。
Claims (13)
- 原子炉の冷却システムにおける金属表面を除染する方法であって、
前記金属表面が、ラジオアイソトープを含む金属酸化物で被覆されており、
前記冷却システムが、少なくとも1つのリアクター・クーラント・ポンプを含む1またはそれよりも多い主ループおよび残留熱除去システムを有して成り、
前記除染方法が、複数の処理サイクルを実施することを含んで成り、該処理サイクルの各々が、
a)ラジオアイソトープを含む金属酸化物を過マンガン酸塩オキシダントの水溶液と接触させる酸化工程、
b)金属酸化物の少なくとも一部およびラジオアイソトープを溶解させるために、前記酸化工程に付された金属酸化物を、シュウ酸、ギ酸、クエン酸、酒石酸、ピコリン酸、グルコン酸、グリオキシル酸およびそれらの混合物から成る群から選択される有機酸の水溶液と接触させる除染工程、ならびに、
c)少なくともラジオアイソトープをイオン交換樹脂に固定化する洗浄工程
を含んで成り、
前記酸化工程が、同じまたは異なる処理サイクルの中で次々に実施される、少なくとも1つの酸性の酸化工程および少なくとも1つのアルカリ性の酸化工程を含んで成り、
前記複数の処理サイクルが、高温酸化工程を含む少なくとも1つの処理サイクルを含んで成り、前記過マンガン酸塩オキシダント溶液が、少なくとも100℃の温度に保持され、前記高温酸化工程中にて、前記少なくとも1つのリアクター・クーラント・ポンプが、主ループ内のオキシダント溶液を循環および加熱するために用いられ、前記残留熱除去システムが、オキシダント溶液の温度を制御するために用いられる、
除染方法。 - 過マンガン酸塩オキシダントがHMnO4、HMnO4/HNO3、KMnO4/HNO3、KMnO4/KOH、KMnO4/NaOHから成る群から選択される、請求項1に記載の除染方法。
- 酸性の酸化工程において、過マンガン酸塩オキシダントの水溶液のpH値が約6未満であり、好ましくは約4未満である、請求項1または2に記載の除染方法。
- アルカリ性の酸化工程において、過マンガン酸塩オキシダントの水溶液のpH値が少なくとも8であり、好ましくは少なくとも10である、請求項1または2に記載の除染方法。
- 酸性の酸化工程における過マンガン酸塩オキシダントが、HMnO4、HMnO4/HNO3、KMnO4/HNO3または過マンガン酸塩の他の金属塩から成る群から選択される、請求項3に記載の除染方法。
- アルカリ性の酸化工程における過マンガン酸塩オキシダントが、KMnO4/NaOH 、KMnO4/KOHまたは過マンガン酸塩の他の金属塩および金属水酸化物である、請求項4に記載の除染方法。
- 複数の処理サイクルが、酸性の酸化工程を含んで成る第1の処理サイクルに引き続いて、アルカリ性の酸化工程を含んで成る第2の処理サイクルを行う、またはその逆である、交互に順列した処理サイクルを含んで成る、請求項1〜6のいずれかに記載の除染方法。
- 複数の処理サイクル全てが、オキシダント溶液が少なくとも100℃の温度を保持する高温酸化工程を含んで成る、請求項1〜7のいずれかに記載の除染方法。
- オキシダント溶液が120℃〜150℃の温度範囲に保持される、請求項1〜8のいずれかに記載の除染方法。
- 少なくとも1つの酸性の酸化工程が、オキシダント溶液が少なくとも100℃の温度で保持される高温酸化工程を含んで成る、請求項1〜9のいずれかに記載の除染方法。
- 少なくとも1つのアルカリ性の酸化工程が、オキシダント溶液が少なくとも100℃の温度で保持される高温酸化工程を含んで成る、請求項1〜9のいずれかに記載の除染方法。
- 有機酸がシュウ酸である、請求項1〜11のいずれかに記載の除染方法。
- 高温酸化工程の間にてオキシダント溶液が1barよりも高い圧力に保持される、請求項1〜11のいずれかに記載の除染方法。
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