JP6796587B2 - 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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- 238000001816 cooling Methods 0.000 title claims description 34
- 229910052751 metal Inorganic materials 0.000 title claims description 26
- 239000002184 metal Substances 0.000 title claims description 26
- 230000003647 oxidation Effects 0.000 claims description 124
- 238000007254 oxidation reaction Methods 0.000 claims description 124
- 238000005202 decontamination Methods 0.000 claims description 80
- 239000007800 oxidant agent Substances 0.000 claims description 70
- 230000001590 oxidative effect Effects 0.000 claims description 68
- 230000003588 decontaminative effect Effects 0.000 claims description 56
- 238000000034 method Methods 0.000 claims description 38
- 230000002378 acidificating effect Effects 0.000 claims description 29
- 239000007864 aqueous solution Substances 0.000 claims description 26
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 21
- 239000002826 coolant Substances 0.000 claims description 21
- 229910044991 metal oxide Inorganic materials 0.000 claims description 21
- 150000004706 metal oxides Chemical class 0.000 claims description 21
- 150000007524 organic acids Chemical class 0.000 claims description 17
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 9
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 claims description 8
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- 239000002253 acid Substances 0.000 claims description 5
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- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 claims description 4
- RGHNJXZEOKUKBD-SQOUGZDYSA-N D-gluconic acid Chemical compound OC[C@@H](O)[C@@H](O)[C@H](O)[C@@H](O)C(O)=O RGHNJXZEOKUKBD-SQOUGZDYSA-N 0.000 claims description 4
- 238000004140 cleaning Methods 0.000 claims description 4
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- 229920003303 ion-exchange polymer Polymers 0.000 claims description 4
- BSKHPKMHTQYZBB-UHFFFAOYSA-N 2-methylpyridine Chemical compound CC1=CC=CC=N1 BSKHPKMHTQYZBB-UHFFFAOYSA-N 0.000 claims description 3
- FEWJPZIEWOKRBE-JCYAYHJZSA-N Dextrotartaric acid Chemical compound OC(=O)[C@H](O)[C@@H](O)C(O)=O FEWJPZIEWOKRBE-JCYAYHJZSA-N 0.000 claims description 3
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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 description 2
- 239000000174 gluconic acid Substances 0.000 claims description 2
- 229910000000 metal hydroxide Inorganic materials 0.000 claims description 2
- 150000004692 metal hydroxides Chemical class 0.000 claims description 2
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- 239000000243 solution Substances 0.000 description 52
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 18
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- 230000000694 effects Effects 0.000 description 14
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 8
- 230000001965 increasing effect Effects 0.000 description 8
- 229910021645 metal ion Inorganic materials 0.000 description 8
- 239000003929 acidic solution Substances 0.000 description 5
- BFGKITSFLPAWGI-UHFFFAOYSA-N chromium(3+) Chemical compound [Cr+3] BFGKITSFLPAWGI-UHFFFAOYSA-N 0.000 description 5
- 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
- 239000012670 alkaline solution Substances 0.000 description 4
- 238000009835 boiling Methods 0.000 description 4
- 230000008859 change Effects 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
- 238000013461 design Methods 0.000 description 4
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- 229910001026 inconel Inorganic materials 0.000 description 4
- 229910052759 nickel Inorganic materials 0.000 description 4
- 239000002901 radioactive waste Substances 0.000 description 4
- VEQPNABPJHWNSG-UHFFFAOYSA-N Nickel(2+) Chemical compound [Ni+2] VEQPNABPJHWNSG-UHFFFAOYSA-N 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000004090 dissolution Methods 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
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- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 229910000990 Ni alloy Inorganic materials 0.000 description 2
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- 238000006243 chemical 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
- 238000002347 injection Methods 0.000 description 2
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- 150000002500 ions Chemical class 0.000 description 2
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 2
- 230000007246 mechanism Effects 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
- 238000012544 monitoring process Methods 0.000 description 2
- 239000012286 potassium permanganate Substances 0.000 description 2
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- 229910000531 Co alloy Inorganic materials 0.000 description 1
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 description 1
- FEWJPZIEWOKRBE-UHFFFAOYSA-N Tartaric acid Natural products [H+].[H+].[O-]C(=O)C(O)C(O)C([O-])=O FEWJPZIEWOKRBE-UHFFFAOYSA-N 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000009390 chemical decontamination Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 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
- 238000010924 continuous production Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 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
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 238000007689 inspection Methods 0.000 description 1
- 239000011344 liquid material Substances 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 235000005985 organic acids Nutrition 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
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- 239000007787 solid Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 229910052566 spinel group Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 235000002906 tartaric acid Nutrition 0.000 description 1
- 239000011975 tartaric acid Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
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- 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
-
- 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
- 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
- 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
-
- 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
-
- 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
-
- 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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- 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)
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 (12)
- 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2つ以上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の水溶液が、少なくとも120℃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、主ループ内の過マンガン酸塩オキシダントの水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、過マンガン酸塩オキシダントの水溶液の温度を制御するために用いられ、
少なくとも1つの酸性の酸化工程が、過マンガン酸塩オキシダントの水溶液が少なくとも120℃の温度で保持される高温酸化工程を含んで成る、
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6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、過マンガン酸塩オキシダントの水溶液が少なくとも120℃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。
- 過マンガン酸塩オキシダントの水溶液が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つのアルカリ性の酸化工程が、過マンガン酸塩オキシダントの水溶液が少なくとも120℃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1〜10のいずれかに記載の除染方法。
- 高温酸化工程の間にて過マンガン酸塩オキシダントの水溶液が1barよりも高い圧力に保持される、請求項1〜10のいずれかに記載の除染方法。
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GB1340276A (en) | 1970-04-21 | 1973-12-12 | Kernforschungsanlage Juelich | Process for decomposing metallic oxide materials |
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DE3413868A1 (de) | 1984-04-12 | 1985-10-17 | Kraftwerk Union AG, 4330 Mülheim | Verfahren zur chemischen dekontamination von metallischen bauteilen von kernreaktoranlagen |
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