EP0160831A2 - Procédé pour décontaminer chimiquement les parties métalliques des installations de réacteur nucléaire - Google Patents

Procédé pour décontaminer chimiquement les parties métalliques des installations de réacteur nucléaire Download PDF

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Publication number
EP0160831A2
EP0160831A2 EP85103900A EP85103900A EP0160831A2 EP 0160831 A2 EP0160831 A2 EP 0160831A2 EP 85103900 A EP85103900 A EP 85103900A EP 85103900 A EP85103900 A EP 85103900A EP 0160831 A2 EP0160831 A2 EP 0160831A2
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EP
European Patent Office
Prior art keywords
dicarboxylic acids
permanganic acid
nuclear reactor
treatment
acid
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
Application number
EP85103900A
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German (de)
English (en)
Other versions
EP0160831B1 (fr
EP0160831A3 (en
Inventor
Horst-Otto Bertholdt
Hans Dipl.-Ing. Hirning
Rudolf Papesch
Hubert Dipl.-Ing. Stamm
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Areva GmbH
Original Assignee
Kraftwerk Union AG
Siemens AG
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Publication date
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Application filed by Kraftwerk Union AG, Siemens AG filed Critical Kraftwerk Union AG
Publication of EP0160831A2 publication Critical patent/EP0160831A2/fr
Publication of EP0160831A3 publication Critical patent/EP0160831A3/de
Application granted granted Critical
Publication of EP0160831B1 publication Critical patent/EP0160831B1/fr
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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
    • 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

Definitions

  • the invention relates to a process for the chemical decontamination of metallic components of nuclear reactor plants, in which an oxidative treatment with a permanganate solution is carried out before dicarboxylic acids are used for further treatment.
  • an alkaline permanganate solution at a temperature of about 100 ° C. is used for the oxidative treatment. It is then rinsed out with deionate before continuing with a citrate oxalate solution which is adjusted to a pH of 3.5 with ammonia and which contains an inhibitor and ethylenediaminetetraacetic acid.
  • the inhibitor is iron III formate.
  • the known method with its individual stages and the rinsing steps in between works with high chemical concentrations and is relatively time-consuming. It has also not yet been used for primary systems of nuclear reactors which would have to be practically emptied for this purpose and which would have to be refilled after the treatment.
  • the invention is therefore based on the object of reducing the dose burden on inspection and repair personnel by chemical decontamination of the primary system To enable nuclear reactors or parts thereof, which can be carried out with less effort. As an important secondary condition, it should be ensured that chemical decontamination results in only a small amount of secondary waste, which in turn must be eliminated in a radiation-safe manner.
  • permanganic acid is used for the oxidative treatment. As has been found, this can be used for the same effect with significantly lower concentrations and, moreover, it can be achieved that the subsequent treatment with dicarboxylic acids also requires much smaller amounts of acid, so that there is correspondingly less secondary waste. Above all, however, the treatment can be carried out by introducing the permanganic acid into the primary coolant of a water-cooled nuclear reactor. It is therefore no longer necessary to drain the primary coolant. Rather, the new process can be carried out in such a way that the primary coolant is cleaned by ion exchange resins and remains in the nuclear reactor for further operation.
  • the permanganic acid is advantageously produced by converting potassium permanganate. This can be done by withdrawing potassium using an ion exchanger. The conversion can take place outside the system to be treated in special containers, but also during the decontamination of entire primary circuits with the auxiliary systems available in the nuclear power plant (such as primary coolant cleaning). The permanganic acid is then in a concentration range of 20 to 400 mg / kg.
  • An advantageous development of the invention consists in that a mixture with an oxalic acid content of at most 1/3 is used as the dicarboxylic acids.
  • Dicarboxylic acids with a chain length of C 3 and hydroxidicarboxylic acids can be used as further dicarboxylic acids of the mixture.
  • the dicarboxylic acids are introduced directly into the permanganic acid solution, especially for cleaning primary circuits. This saves the usual rinsing processes and the draining and discarding or processing of the permanganate solution.
  • 1 shows the primary cooling circuit of a pressurized water reactor that is to be decontaminated, and the auxiliary power plants required for this purpose.
  • 2 shows the time course of the decontamination treatment for a first cycle.
  • the pressurized water reactor comprises a reactor pressure vessel 2, a steam generator 3 and a main coolant pump 4. This promotes this from the reactor pressure vessel 2 via the hot line 5 in the primary cooling water reaching the steam generator 3 via the cold strand 6 back into the reactor pressure vessel 2.
  • a volume control system 8 is used to treat the primary cooling water. It is connected to the cold line 6 in the area between the pump 4 and the steam generator 3 with an outlet line 10. It runs via a recuperative heat exchanger 12 and a cooler 13 to a shut-off valve 14. This is followed by control valves 15, 16 and 17 which lead to a storage tank 18. The coolant can be conveyed back from the storage tank 18 into the primary circuit 1 via a high-pressure feed pump 20. The cooled and cleaned primary coolant passes through the recuperative heat exchanger 12 before it returns to the cold line 6 via the line 21 behind the pump 4.
  • Devices for coolant treatment are located parallel to valves 15 to 17. They include an indicated with 24 coolant cleaning as well as a gasification g ühlstoffent- 25. For the ingestion of large amounts of refrigerant is provided a coolant storage 26th The devices 24 to 26, like a coolant preparation 27, are connected to an exhaust gas system 28, which receives the gaseous activity carriers that occur during the coolant treatment.
  • boron is removed from the coolant, which is used for combustion control.
  • the boron and the boron-free deionate can be fed to a boric acid and deionate feed 30, which is connected to the volume control system 8 via a line 31 sen, into which a chemical feed 32 also feeds.
  • the liquid waste produced in the coolant cleaning can be passed on to a treatment plant 35 for radioactive waste water, which is followed by the treatment of radioactive concentrates indicated at 36.
  • the temperature in the primary system is reduced to 60 60 ° C. and the dicarboxylic acid mixture is introduced directly into the permanganic acid solution.
  • dicarboxylic acids or hydroxidicarboxylic acids which are entered up to a concentration of 300 mg / kg in the primary coolant, as shown by curve part 41, and further 100 mg / kg parts of oxalic acid, as curve part 42 is intended to show .
  • dicarboxylic acids are mesoxalic acid, malonic acid and dihydroxyfumaric acid and dihydroxy tartaric acid are used.
  • the HMnP 4 and MnO 2 present in the system react with the oxalic acid and are reduced to Mn ++ ions.
  • the oxalic acid is oxidized to C0 2 , the C0 2 being removed via the degasser.
  • the contents of the primary circuit are heated to 100 ° C again. Parts of the primary coolant are then shunted over ion exchange filters that are part of the coolant cleaning 24 or coolant preparation 27, so that the facilities already present in the power plant are used.
  • the chemical concentration can be reduced to practically zero (curve 44).
  • the manganese content originating from the oxidative conversion is reduced, as indicated by the dashed curve part 45.
  • the components of the oxide layer are also filtered out. This happens after the curve 46, which represents the content of iron, chromium, nickel and possibly cobalt.
  • the withdrawal of the cations and the dicarboxylic acid via the ion exchanger is controlled in such a way that the dicarboxylic acid is present in excess, equivalent to the dissolved cations. This is crucial in order to prevent the activity from failing again.

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  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Food Science & Technology (AREA)
  • Electrochemistry (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Cleaning By Liquid Or Steam (AREA)
  • Apparatus For Disinfection Or Sterilisation (AREA)
  • Cleaning And De-Greasing Of Metallic Materials By Chemical Methods (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)
  • Treatment Of Water By Ion Exchange (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
EP85103900A 1984-04-12 1985-04-01 Procédé pour décontaminer chimiquement les parties métalliques des installations de réacteur nucléaire Expired - Lifetime EP0160831B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3413868 1984-04-12
DE19843413868 DE3413868A1 (de) 1984-04-12 1984-04-12 Verfahren zur chemischen dekontamination von metallischen bauteilen von kernreaktoranlagen

Publications (3)

Publication Number Publication Date
EP0160831A2 true EP0160831A2 (fr) 1985-11-13
EP0160831A3 EP0160831A3 (en) 1987-11-25
EP0160831B1 EP0160831B1 (fr) 1991-12-04

Family

ID=6233426

Family Applications (1)

Application Number Title Priority Date Filing Date
EP85103900A Expired - Lifetime EP0160831B1 (fr) 1984-04-12 1985-04-01 Procédé pour décontaminer chimiquement les parties métalliques des installations de réacteur nucléaire

Country Status (8)

Country Link
US (1) US4756768A (fr)
EP (1) EP0160831B1 (fr)
JP (1) JPS60235099A (fr)
BR (1) BR8501711A (fr)
CA (1) CA1254113A (fr)
DE (2) DE3413868A1 (fr)
ES (1) ES8702726A1 (fr)
FI (1) FI84118C (fr)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1989003113A1 (fr) * 1987-10-02 1989-04-06 Abb Reaktor Gmbh Procede de decontamination de surfaces
EP0355477A1 (fr) * 1988-08-12 1990-02-28 Siemens Aktiengesellschaft Procédé et dispositif pour la décontamination du système primaire d'une centrale nucléaire
BE1002593A3 (nl) * 1988-11-09 1991-04-02 Lemmens Godfried Werkwijze voor de dekontaminatie van radioaktief besmette materialen.
DE102007038947A1 (de) 2007-08-17 2009-02-26 Areva Np Gmbh Verfahren zur Dekontamination von mit Alphastrahlern kontaminierten Oberflächen von Nuklearanlagen
US8608861B2 (en) 2005-11-29 2013-12-17 Areva Np Gmbh Method for the decontamination of an oxide layer-containing surface of a component or a system of a nuclear facility
CN107170503A (zh) * 2017-06-02 2017-09-15 苏州热工研究院有限公司 一种降低在役压水堆核电厂集体剂量的化学清洗方法

Families Citing this family (27)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ES2045298T3 (es) * 1988-08-24 1994-01-16 Siemens Ag Procedimiento para la descontaminacion quimica de la superficie de un componente metalico de una instalacion de reactor nuclear.
US5170840A (en) * 1992-06-15 1992-12-15 Grunwald James L Method for detecting breaches in heat exchanger tubing
DE4232246A1 (de) * 1992-09-25 1994-03-31 Siemens Ag Verfahren zur Zerstörung einer organischen Substanz
DE19818772C2 (de) * 1998-04-27 2000-05-31 Siemens Ag Verfahren zum Abbau der Radioaktivität eines Metallteiles
US6635232B1 (en) 1999-05-13 2003-10-21 Kabushiki Kaisha Toshiba Method of chemically decontaminating components of radioactive material handling facility and system for carrying out the same
DE19851852A1 (de) * 1998-11-10 2000-05-11 Siemens Ag Verfahren zur Dekontamination einer Oberfläche eines Bauteiles
RU2132579C1 (ru) * 1998-11-13 1999-06-27 Косарева Инэсса Михайловна Способ химической дезактивации поверхности металлических изделий, зараженных радиоактивными веществами
JP3977963B2 (ja) 1999-09-09 2007-09-19 株式会社日立製作所 化学除染方法
TW529041B (en) * 2000-12-21 2003-04-21 Toshiba Corp Chemical decontamination method and treatment method and apparatus of chemical decontamination solution
JP2003098294A (ja) * 2001-09-27 2003-04-03 Hitachi Ltd オゾンを用いた除染方法及びその装置
KR100724710B1 (ko) * 2002-11-21 2007-06-04 가부시끼가이샤 도시바 방사화 부품의 화학적 오염제거 시스템 및 방법
JP4131814B2 (ja) * 2002-11-21 2008-08-13 株式会社東芝 放射化部品の化学除染方法および装置
KR101086600B1 (ko) * 2006-02-09 2011-11-23 가부시끼가이샤 도시바 화학 제염 장치 및 그 제염 방법
RU2340965C1 (ru) * 2007-03-29 2008-12-10 Федеральное государственное унитарное предприятие "Научно-исследовательский технологический институт имени А.П. Александрова" Способ химической дезактивации оборудования атомных электрических станций
DE102008063941A1 (de) * 2008-12-19 2010-07-01 Forschungszentrum Jülich GmbH Verfahren zur Reduzierung oder zumindest teilweisen Entfernung spezifischer Radiotoxika aus einer kerntechnischen Anlage
DE102009047524A1 (de) * 2009-12-04 2011-06-09 Areva Np Gmbh Verfahren zur Oberflächen-Dekontamination
DE102010028457A1 (de) * 2010-04-30 2011-11-03 Areva Np Gmbh Verfahren zur Oberflächen-Dekontamination
ES2576187T3 (es) 2011-09-20 2016-07-06 Horst-Otto Bertholdt Método para descomponer una capa de óxido
DE102013102331B3 (de) 2013-03-08 2014-07-03 Horst-Otto Bertholdt Verfahren zum Abbau einer Oxidschicht
JP6249916B2 (ja) * 2014-09-24 2017-12-20 三菱重工業株式会社 過マンガン酸の調製装置
JP6937348B2 (ja) * 2015-02-05 2021-09-22 フラマトム ゲゼルシャフト ミット ベシュレンクテル ハフツング 原子炉の冷却システムで金属表面を除染する方法
KR102272949B1 (ko) * 2015-02-05 2021-07-06 프라마톰 게엠베하 원자로의 냉각 시스템에서의 금속 표면 오염 제거 방법
DE102016104846B3 (de) * 2016-03-16 2017-08-24 Areva Gmbh Verfahren zur Behandlung von Abwasser aus der Dekontamination einer Metalloberfläche, Abwasserbehandlungsvorrichtung und Verwendung der Abwasserbehandlungsvorrichtung
MX370759B (es) * 2017-01-19 2019-12-13 Framatome Gmbh Metodo para descontaminar superficies metalicas de una instalacion nuclear.
WO2018149862A1 (fr) 2017-02-14 2018-08-23 Siempelkamp NIS Ingenieurgesellschaft mbH Procédé de décomposition d'une couche d'oxyde contenant des radionucléides
CN107101525A (zh) * 2017-03-21 2017-08-29 华电电力科学研究院 一种对发电厂锅炉过热器循环化学清洗的方法
CN107481772B (zh) * 2017-08-22 2019-07-02 深圳中广核工程设计有限公司 核电站放射性浓缩液排放管路的冲洗系统及冲洗方法

Family Cites Families (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3013909A (en) * 1960-03-31 1961-12-19 Guyon P Pancer Method of chemical decontamination of stainless steel nuclear facilities
US3496017A (en) * 1966-04-28 1970-02-17 Atomic Energy Commission Method and composition for decontamination of stainless steel surfaces
US3615817A (en) * 1969-02-04 1971-10-26 Atomic Energy Commission Method of decontaminating radioactive metal surfaces
US3873362A (en) * 1973-05-29 1975-03-25 Halliburton Co Process for cleaning radioactively contaminated metal surfaces
JPS5293900A (en) * 1976-02-02 1977-08-06 Hitachi Ltd Purififying method and device for nuclear reactor
US4226640A (en) * 1978-10-26 1980-10-07 Kraftwerk Union Aktiengesellschaft Method for the chemical decontamination of nuclear reactor components
GB2077482B (en) * 1980-06-06 1983-06-08 Us Energy Coolant system decontamination
EP0071336B1 (fr) * 1981-06-17 1986-03-26 Central Electricity Generating Board Procédé pour la dissolution chimique des dépôts d'oxyde

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1989003113A1 (fr) * 1987-10-02 1989-04-06 Abb Reaktor Gmbh Procede de decontamination de surfaces
EP0313843A1 (fr) * 1987-10-02 1989-05-03 ABB Reaktor GmbH Procédé pour décontaminer des surfaces
EP0355477A1 (fr) * 1988-08-12 1990-02-28 Siemens Aktiengesellschaft Procédé et dispositif pour la décontamination du système primaire d'une centrale nucléaire
BE1002593A3 (nl) * 1988-11-09 1991-04-02 Lemmens Godfried Werkwijze voor de dekontaminatie van radioaktief besmette materialen.
US8608861B2 (en) 2005-11-29 2013-12-17 Areva Np Gmbh Method for the decontamination of an oxide layer-containing surface of a component or a system of a nuclear facility
DE102007038947A1 (de) 2007-08-17 2009-02-26 Areva Np Gmbh Verfahren zur Dekontamination von mit Alphastrahlern kontaminierten Oberflächen von Nuklearanlagen
CN107170503A (zh) * 2017-06-02 2017-09-15 苏州热工研究院有限公司 一种降低在役压水堆核电厂集体剂量的化学清洗方法
CN107170503B (zh) * 2017-06-02 2019-04-02 苏州热工研究院有限公司 一种降低在役压水堆核电厂集体剂量的化学清洗方法

Also Published As

Publication number Publication date
ES542157A0 (es) 1986-12-16
ES8702726A1 (es) 1986-12-16
DE3584790D1 (de) 1992-01-16
CA1254113A (fr) 1989-05-16
FI84118B (fi) 1991-06-28
JPS60235099A (ja) 1985-11-21
EP0160831B1 (fr) 1991-12-04
DE3413868A1 (de) 1985-10-17
US4756768A (en) 1988-07-12
FI84118C (fi) 1991-10-10
JPH0310919B2 (fr) 1991-02-14
BR8501711A (pt) 1985-12-10
FI850780L (fi) 1985-10-13
FI850780A0 (fi) 1985-02-26
EP0160831A3 (en) 1987-11-25

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