EP0160831B1 - Verfahren zur chemischen Dekontamination von metallischen Bauteilen von Kenreaktoranlagen - Google Patents

Verfahren zur chemischen Dekontamination von metallischen Bauteilen von Kenreaktoranlagen Download PDF

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Publication number
EP0160831B1
EP0160831B1 EP85103900A EP85103900A EP0160831B1 EP 0160831 B1 EP0160831 B1 EP 0160831B1 EP 85103900 A EP85103900 A EP 85103900A EP 85103900 A EP85103900 A EP 85103900A EP 0160831 B1 EP0160831 B1 EP 0160831B1
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EP
European Patent Office
Prior art keywords
process according
nuclear reactor
coolant
acid
acids
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 - Lifetime
Application number
EP85103900A
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German (de)
English (en)
French (fr)
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EP0160831A3 (en
EP0160831A2 (de
Inventor
Horst-Otto Bertholdt
Hans Dipl.-Ing. Hirning
Rudolf Papesch
Hubert Dipl.-Ing. Stamm
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Siemens AG
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Siemens AG
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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 approximately 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.
  • a process for chemical decontamination is known from EP-A 0 071 336, which provides for the use of a permanganate salt in acidic solution as the first stage.
  • a mixture of potassium permanganate and nitric acid is used in particular.
  • Such a process step produces chemicals such as manganese dioxide and potassium nitrate, which are ineffective for cleaning and to increase the undesirable Contribute secondary waste.
  • the secondary waste contains ions, such as K NO and NO3 ⁇ , which have to be removed in the secondary waste disposal with expensive ion exchangers.
  • the invention is based on the object of making it possible to reduce the dose burden on inspection and repair personnel by chemical decontamination of the primary system of nuclear reactors or of parts thereof, which can be carried out with little 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, which is produced by converting permanganate salt by means of ion exchangers.
  • 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.
  • the permanganic acid can be present 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 returned to the primary circuit 1 from the storage tank 18 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.
  • 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 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.
  • 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 HMnO4 and MnO2 present in the system reacts with the oxalic acid and is reduced to Mn++ ions.
  • the oxalic acid is oxidized to CO2, the CO2 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. In the course of 20 hours to the time T3, the chemical concentration can be practically zero (curve 44). The manganese content originating from the oxidative conversion is reduced, as indicated by the dashed curve part 45. At the same time, 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)
  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Food Science & Technology (AREA)
  • Electrochemistry (AREA)
  • Physics & Mathematics (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Cleaning By Liquid Or Steam (AREA)
  • Cleaning And De-Greasing Of Metallic Materials By Chemical Methods (AREA)
  • Apparatus For Disinfection Or Sterilisation (AREA)
  • Treatment Of Water By Ion Exchange (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)
EP85103900A 1984-04-12 1985-04-01 Verfahren zur chemischen Dekontamination von metallischen Bauteilen von Kenreaktoranlagen Expired - Lifetime EP0160831B1 (de)

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 EP0160831A2 (de) 1985-11-13
EP0160831A3 EP0160831A3 (en) 1987-11-25
EP0160831B1 true EP0160831B1 (de) 1991-12-04

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ID=6233426

Family Applications (1)

Application Number Title Priority Date Filing Date
EP85103900A Expired - Lifetime EP0160831B1 (de) 1984-04-12 1985-04-01 Verfahren zur chemischen Dekontamination von metallischen Bauteilen von Kenreaktoranlagen

Country Status (8)

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

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1968075A1 (de) 2005-11-29 2008-09-10 Areva NP GmbH Verfahren zur Dekontamination einer eine Oxidschicht aufweisenden Oberfläche einer Komponente oder eines Systems einer kerntechnischen Anlage
DE102007038947A1 (de) * 2007-08-17 2009-02-26 Areva Np Gmbh Verfahren zur Dekontamination von mit Alphastrahlern kontaminierten Oberflächen von Nuklearanlagen
WO2013041595A1 (de) 2011-09-20 2013-03-28 Nis Ingenieurgesellschaft Mbh Verfahren zum abbau einer oxidschicht
DE102013102331B3 (de) * 2013-03-08 2014-07-03 Horst-Otto Bertholdt Verfahren zum Abbau einer Oxidschicht
WO2018149862A1 (de) 2017-02-14 2018-08-23 Siempelkamp NIS Ingenieurgesellschaft mbH Verfahren zum abbau einer radionuklidhaltigen oxidschicht

Families Citing this family (28)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CH673545A5 (enrdf_load_stackoverflow) * 1987-10-02 1990-03-15 Industrieorientierte Forsch
EP0355477A1 (de) * 1988-08-12 1990-02-28 Siemens Aktiengesellschaft Verfahren und Einrichtung zur Dekontamination des Primärsystems eines Kernkraftwerkes
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.
BE1002593A3 (nl) * 1988-11-09 1991-04-02 Lemmens Godfried Werkwijze voor de dekontaminatie van radioaktief besmette materialen.
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
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
EP1054413B1 (en) * 1999-05-13 2013-07-17 Kabushiki Kaisha Toshiba Method of chemically decontaminating components of radioactive material handling facility and system for carrying out the same
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
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
HUE047725T2 (hu) * 2015-02-05 2020-05-28 Framatome Gmbh Eljárás fém felületek szennyezõdés-mentesítésére nukleáris reaktor hûtõrendszerében
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
EP3446316B1 (en) * 2017-01-19 2020-04-15 Framatome GmbH Method for decontaminating metal surfaces of a nuclear facility
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
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
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

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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
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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
US4481040A (en) * 1981-06-17 1984-11-06 Central Electricity Generating Board Of Sudbury House Process for the chemical dissolution of oxide deposits

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Gmelin Handbuch der Anorganischen Chemie, Springer Verlag, 1975, 8. Auflage, Band MANGAN, Seiten 85-86 *
H. Remy, Lehrbuch der Anorganischen Chemie, Akademische Verlagsgesellschaft, 1973, 12. und 13. Auflage, Band II, Seiten 285 *

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1968075A1 (de) 2005-11-29 2008-09-10 Areva NP GmbH Verfahren zur Dekontamination einer eine Oxidschicht aufweisenden Oberfläche einer Komponente oder eines Systems einer kerntechnischen Anlage
US8021494B2 (en) 2005-11-29 2011-09-20 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
US8702868B2 (en) 2007-08-17 2014-04-22 Areva Gmbh Method for decontaminating surfaces of nuclear plants which have been contaminated with alpha emitters
WO2013041595A1 (de) 2011-09-20 2013-03-28 Nis Ingenieurgesellschaft Mbh Verfahren zum abbau einer oxidschicht
DE102013102331B3 (de) * 2013-03-08 2014-07-03 Horst-Otto Bertholdt Verfahren zum Abbau einer Oxidschicht
EP2787509A1 (de) 2013-03-08 2014-10-08 Horst-Otto Bertholdt Verfahren zum Abbau einer Oxidschicht
WO2018149862A1 (de) 2017-02-14 2018-08-23 Siempelkamp NIS Ingenieurgesellschaft mbH Verfahren zum abbau einer radionuklidhaltigen oxidschicht

Also Published As

Publication number Publication date
JPS60235099A (ja) 1985-11-21
CA1254113A (en) 1989-05-16
FI84118B (fi) 1991-06-28
FI850780A0 (fi) 1985-02-26
FI850780L (fi) 1985-10-13
FI84118C (fi) 1991-10-10
DE3584790D1 (de) 1992-01-16
US4756768A (en) 1988-07-12
EP0160831A3 (en) 1987-11-25
EP0160831A2 (de) 1985-11-13
ES8702726A1 (es) 1986-12-16
DE3413868A1 (de) 1985-10-17
BR8501711A (pt) 1985-12-10
ES542157A0 (es) 1986-12-16
JPH0310919B2 (enrdf_load_stackoverflow) 1991-02-14

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