US20050135542A1 - Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking - Google Patents

Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking Download PDF

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Publication number
US20050135542A1
US20050135542A1 US10/715,069 US71506903A US2005135542A1 US 20050135542 A1 US20050135542 A1 US 20050135542A1 US 71506903 A US71506903 A US 71506903A US 2005135542 A1 US2005135542 A1 US 2005135542A1
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US
United States
Prior art keywords
alcohol
reactor
boiling water
primary system
water reactor
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.)
Abandoned
Application number
US10/715,069
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English (en)
Inventor
Bernhard Stellwag
Wilfried Ruhle
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.)
EnBW Kraftwerke AG
Areva GmbH
Original Assignee
EnBW Kraftwerke AG
Framatome ANP GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by EnBW Kraftwerke AG, Framatome ANP GmbH filed Critical EnBW Kraftwerke AG
Priority to US10/715,069 priority Critical patent/US20050135542A1/en
Publication of US20050135542A1 publication Critical patent/US20050135542A1/en
Assigned to FRAMATOME ANP GMBH, ENBW KRAFTWERKE AG reassignment FRAMATOME ANP GMBH ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: RUEHLE, WILFRIED, STELLWAG, BERNHARD
Assigned to AREVA NP GMBH reassignment AREVA NP GMBH CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: FRAMATOME ANP GMBH
Priority to US11/820,966 priority patent/US20070263761A1/en
Priority to US13/913,633 priority patent/US9879351B2/en
Abandoned legal-status Critical Current

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Classifications

    • 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
    • C23F—NON-MECHANICAL REMOVAL OF METALLIC MATERIAL FROM SURFACE; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL; MULTI-STEP PROCESSES FOR SURFACE TREATMENT OF METALLIC MATERIAL INVOLVING AT LEAST ONE PROCESS PROVIDED FOR IN CLASS C23 AND AT LEAST ONE PROCESS COVERED BY SUBCLASS C21D OR C22F OR CLASS C25
    • C23F11/00—Inhibiting corrosion of metallic material by applying inhibitors to the surface in danger of corrosion or adding them to the corrosive agent
    • 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
    • C23F—NON-MECHANICAL REMOVAL OF METALLIC MATERIAL FROM SURFACE; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL; MULTI-STEP PROCESSES FOR SURFACE TREATMENT OF METALLIC MATERIAL INVOLVING AT LEAST ONE PROCESS PROVIDED FOR IN CLASS C23 AND AT LEAST ONE PROCESS COVERED BY SUBCLASS C21D OR C22F OR CLASS C25
    • C23F11/00—Inhibiting corrosion of metallic material by applying inhibitors to the surface in danger of corrosion or adding them to the corrosive agent
    • C23F11/08—Inhibiting corrosion of metallic material by applying inhibitors to the surface in danger of corrosion or adding them to the corrosive agent in other liquids
    • C23F11/10—Inhibiting corrosion of metallic material by applying inhibitors to the surface in danger of corrosion or adding them to the corrosive agent in other liquids using organic inhibitors
    • C23F11/12—Oxygen-containing compounds
    • C23F11/122—Alcohols; Aldehydes; Ketones
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C15/00—Cooling arrangements within the pressure vessel containing the core; Selection of specific coolants
    • G21C15/28—Selection of specific coolants ; Additions to the reactor coolants, e.g. against moderator corrosion
    • 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
    • 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
    • G21C19/30—Arrangements for introducing fluent material into the reactor core; Arrangements for removing fluent material from the reactor core with continuous purification of circulating fluent material, e.g. by extraction of fission products deterioration or corrosion products, impurities, e.g. by cold traps
    • G21C19/307—Arrangements for introducing fluent material into the reactor core; Arrangements for removing fluent material from the reactor core with continuous purification of circulating fluent material, e.g. by extraction of fission products deterioration or corrosion products, impurities, e.g. by cold traps specially adapted for liquids
    • 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

Definitions

  • the invention lies in the boiling water reactor technology field. More-specifically, the invention relates to a method for protecting the components of the primary system of a boiling water reactor in particular from stress corrosion.
  • the coolant which comes into contact with the reactor core is known as primary coolant
  • the lines and components which are exposed to the primary coolant are known as the primary system.
  • the primary system of a boiling water reactor includes systems of lines as well as various internal fittings and pumps.
  • the components generally consist of stainless steel, for example of a CrNi steel, or an Ni-base alloy, such as Inconel® 600 (Inco Alloys International, Inc.).
  • Radiolysis of the primary coolant causes, inter alia, the reaction products hydrogen peroxide, oxygen, and hydrogen to form in the boiling water reactor.
  • the oxidizing conditions which result from the excess of oxidizing agents promote corrosion, in particular stress corrosion cracking, of the components.
  • it is known to admix hydrogen with the primary coolant. This bonds oxidizing agents contained in the primary coolant and shifts the electrochemical potential of the component surfaces toward negative values.
  • a drawback of the conventional method is that relatively large quantities of hydrogen are required to ensure sufficient protection against corrosion.
  • European patent disclosure EP 0736878 describes a method in which the oxide layer of the component surfaces in the primary system is doped with precious metal, which makes it possible to use smaller quantities of hydrogen.
  • German published patent application DE 100 30 726 A1 describes a method in which the quantities of hydrogen and precious metal are supposed to be reduced by coating the component surfaces with a film which includes a substance with a photocatalytic action.
  • the substances with photocatalytic action that are used preferably TiO 2 and ZrO 2 —are N-type semiconductors which are excited by the Cherenkov radiation which is present in the reactor, shifting the corrosion potential of the component surfaces toward negative values.
  • the Soviet document discloses corrosion protection measures by way of the addition of alcohol in the coolant/moderator.
  • the specific concentration disclosed is approximately 10 to 10 5 ⁇ mol/kg in order to completely prevent oxygen formation during the radiolysis of the coolant.
  • the disclosed alcohol concentration must necessarily be present at those locations at which the radiolysis processes are the strongest, that is, at the fuel rods in the reactor core.
  • a problem associated with very high alcohol concentration is that a relatively large portion of the alcohol remains unused, i.e., it is not oxidized by radiolysis oxygen or decomposed by the radiolysis, it subsequently passes through a phase change into the vapor phase and then reaches the steam turbine and the condenser downstream of the steam turbine. There, the alcohol is cooled to about 40° C. At this temperature, only a small proportion of the alcohol is dissolved in the liquefied condensate which is fed back into the reactor pressure vessel in the form feedwater. The by far largest proportion is contained in the vapor phase. The latter is not simply let go into the environment but it is transported via an off-gas path within which a catalytic recombination of hydrogen and oxygen to water is effected. An alcohol component in the vapor phase could, on the one hand, disturb the recombination. On the other hand, additional functional elements and processing steps would have to be provided in order to hold back the alcohol or to convert the same into a non-damaging form.
  • a method for protecting components of a primary system of a boiling water reactor having a pressure vessel and a feedwater line opening out into the pressure vessel comprises the following steps:
  • the alcohol concentration is adjusted to less than 10 ⁇ mol per kg.
  • the objects of the invention are achieved by a method in which an alcohol that can be oxidized under the conditions prevailing in the reactor system, preferably in liquid phase, is fed into the primary coolant instead of hydrogen, with the component surfaces being bright or being covered only by a native oxide layer.
  • a native oxide layer is to be understood as meaning an oxide layer which forms as a result of corrosion to the component material, if appropriate with the intercalation of foreign metals or foreign metal oxides, during reactor operation or during an oxidizing pretreatment.
  • the component surfaces are doped with precious metal, for example with Pt, with the result that a lower concentration of alcohol is required in the primary coolant.
  • the alcohol concentration is maintained at between 0.1 and 300 ⁇ mol per kg of the primary coolant and, in a preferred embodiment, it is maintained at less than 10 ⁇ mol/kg. It is expedient for the alcohol to be fed into the condensate or feedwater system.
  • the quantity which is metered in is in this case such that the abovementioned concentration is established in the downcomer of the boiling water reactor.
  • the downcomer is the area in the reactor pressure vessel which extends downward from the opening points of the feed tubes. It is preferable to use methanol, ethanol and propanol. However, formic acid, formaldehyde, and acetaldehyde are also eminently suitable.
  • the metering-in of alcohol may lead to several disadvantageous results. That is, it is in effect a balancing act between the positive and the negative effects thereof.
  • the instantly claimed invention provides a successful compromise with highly improved corrosion protection while the negative effects of the alcohol are virtually unnoticeable. This is particularly so when the alcohol concentration is maintained at below 10 ⁇ mol/kg.
  • FIG. 1 is a diagrammatic longitudinal section taken through a boiling water reactor
  • FIG. 2 is a diagrammatic chart showing the potentials of CrNi steel and Pt in the presence of CH 3 OH and hydrogen as reducing agents.
  • a pressure vessel 1 of the reactor houses fuel assemblies 2 or fuel elements.
  • An alcohol of the above-mentioned type preferably methanol
  • IMSCC stress corrosion cracking
  • the reactor is in an operating state in which the components of the reactor, i.e. for example the pressure vessel 1 and the non-illustrated core grid, which usually consist of CrNi steel or an Ni-base alloy, are bright or are covered only with a native oxide layer.
  • the former case occurs, for example, if an oxide layer has been removed from the component surfaces during maintenance work.
  • the quantity injected into the feedline 3 is such that a concentration of from 0.1 to 300 ⁇ mol/kg of alcohol, in particular methanol, is established in the downcomer 4 which adjoins the feedline 3 at the bottom.
  • the optimum concentration of alcohol is dependent on various factors, such as the component material, the presence of precious metal doping, etc., and is therefore to be determined on a case-by-case basis for each individual reactor.
  • the concentration is set to less than 10 ⁇ mol/kg which, in a given context, provides for an acceptable compromise with regard to good corrosion protection and virtually negligible disadvantages otherwise associated with the alcohol.
  • Tests using Pt and CrNi steel electrodes were carried out in order to test the theoretical effectiveness of the proposed method.
  • the electrodes made from CrNi steel were subjected to preliminary oxidation for 500 hours at 280° C. with a water chemistry that corresponds to the conditions of use in the reactor.
  • the CrNi steel electrodes which have been pretreated in this way and the Pt electrodes were arranged in an autoclave through which hot water at a temperature of 280° C. was flowing.
  • the chemistry of the circulated water was set so as to correspond to the conditions in a boiling water reactor.
  • the oxygen content was kept at between 0.2 and 2 ppm.
  • the reducing agents used were methanol and, for comparison purposes, hydrogen.
  • the potentials of the electrodes were determined as a function of the methanol or hydrogen content and are plotted in the diagram shown in FIG. 2 against the methanol/oxygen or hydrogen/oxygen molar ratio.
  • the indication “CrNi” indicates CrNi steel. It can be seen that metering of methanol results in a protective action which is comparable to that achieved by metering hydrogen. In both cases, the Pt potential is reduced to below the protection potential of ⁇ 230 mV. In the case of the undoped CrNi steel electrode, it is likewise possible to observe similar electrochemical activities with both methanol and hydrogen. However, in order in this case to reduce the potential to below the protection potential, it is necessary to establish significantly higher molar ratios.
  • a potential of ⁇ 500 mV was measured for an oxygen content of less than 10 ppb and a methanol content of 2 ppm ( ⁇ 62.5 ⁇ mol/kg).

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Preventing Corrosion Or Incrustation Of Metals (AREA)
  • Catalysts (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
US10/715,069 2001-05-15 2003-11-17 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking Abandoned US20050135542A1 (en)

Priority Applications (3)

Application Number Priority Date Filing Date Title
US10/715,069 US20050135542A1 (en) 2001-05-15 2003-11-17 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
US11/820,966 US20070263761A1 (en) 2001-05-15 2007-06-21 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
US13/913,633 US9879351B2 (en) 2001-05-15 2013-06-10 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
DE10123690A DE10123690A1 (de) 2001-05-15 2001-05-15 Verfahren zum Schutz der Bauteile des Primärsystems eines Siedewasserreaktors insbesondere vor Spannungsrisskorrosion
DE10123690.5 2001-05-15
PCT/EP2002/005274 WO2002093586A2 (de) 2001-05-15 2002-05-14 Verfahren zum schutz der bauteile des primärsystems eines siedewasserreaktors insbesondere vor spannungsrisskorrosion
US10/715,069 US20050135542A1 (en) 2001-05-15 2003-11-17 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking

Related Parent Applications (1)

Application Number Title Priority Date Filing Date
PCT/EP2002/005274 Continuation WO2002093586A2 (de) 2001-05-15 2002-05-14 Verfahren zum schutz der bauteile des primärsystems eines siedewasserreaktors insbesondere vor spannungsrisskorrosion

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US11/820,966 Continuation US20070263761A1 (en) 2001-05-15 2007-06-21 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking

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US20050135542A1 true US20050135542A1 (en) 2005-06-23

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US10/715,069 Abandoned US20050135542A1 (en) 2001-05-15 2003-11-17 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
US11/820,966 Abandoned US20070263761A1 (en) 2001-05-15 2007-06-21 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
US13/913,633 Expired - Fee Related US9879351B2 (en) 2001-05-15 2013-06-10 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking

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US11/820,966 Abandoned US20070263761A1 (en) 2001-05-15 2007-06-21 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
US13/913,633 Expired - Fee Related US9879351B2 (en) 2001-05-15 2013-06-10 Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking

Country Status (7)

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US (3) US20050135542A1 (de)
EP (1) EP1388151B1 (de)
JP (1) JP3970182B2 (de)
DE (2) DE10123690A1 (de)
ES (1) ES2334647T3 (de)
TW (1) TW554347B (de)
WO (1) WO2002093586A2 (de)

Cited By (8)

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US20070223645A1 (en) * 2004-05-19 2007-09-27 Wilfried Ruehle Bonding Radioactive Iodine in a Nuclear Reactor
US20090086878A1 (en) * 2007-09-28 2009-04-02 Areva Np Inc. Boiling water reactor nuclear power plant with alcohol injection
US20090133772A1 (en) * 2005-12-05 2009-05-28 Lionel Cachon Element for a pipe for transporting hot gases and method of fabricating said element
CN105393309A (zh) * 2013-08-14 2016-03-09 阿海珐有限公司 用于减少核反应堆所用的部件的表面的放射性污染的方法
US9879351B2 (en) * 2001-05-15 2018-01-30 Areva Inc. Method for protecting components of a primary system of a boiling water reactor in particular from stress corrosion cracking
CN108352201A (zh) * 2015-11-30 2018-07-31 法玛通有限公司 核电设备以及核电设备的操作方法
US11469005B2 (en) * 2018-04-13 2022-10-11 Joint Stock Company “State Scientific Centre Of The Russian Federation—Institute For Physics And Power Engineering Named After A.I. Leypunsky” Reactor core having both nuclear fuel and a heat pipe in a module located in a solid neutron moderator
US11476011B2 (en) * 2018-08-16 2022-10-18 Joint Stock Company “State Scientific Centre Of The Russian Federation Institute For Physics And Power Engineering Named After A.I. Leypunsky” Reactor core having both nuclear fuel and a heat pipe in a module located in a solid neutron moderator

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US8233581B2 (en) 2009-03-31 2012-07-31 Westinghouse Electric Company Llc Process for adding an organic compound to coolant water in a pressurized water reactor

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JP3970182B2 (ja) 2007-09-05
TW554347B (en) 2003-09-21
US9879351B2 (en) 2018-01-30
WO2002093586A2 (de) 2002-11-21
US20070263761A1 (en) 2007-11-15
EP1388151A2 (de) 2004-02-11
EP1388151B1 (de) 2009-11-11
DE50213991D1 (de) 2009-12-24
ES2334647T3 (es) 2010-03-15

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