EP1693855A2 - Brennstoffelement für einen schnellen neutronenreaktor (varianten) und mantelung für seine herstellung - Google Patents

Brennstoffelement für einen schnellen neutronenreaktor (varianten) und mantelung für seine herstellung Download PDF

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Publication number
EP1693855A2
EP1693855A2 EP04793751A EP04793751A EP1693855A2 EP 1693855 A2 EP1693855 A2 EP 1693855A2 EP 04793751 A EP04793751 A EP 04793751A EP 04793751 A EP04793751 A EP 04793751A EP 1693855 A2 EP1693855 A2 EP 1693855A2
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EP
European Patent Office
Prior art keywords
cladding
steel
carbides
ferrite
fuel
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EP04793751A
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English (en)
French (fr)
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EP1693855A4 (de
EP1693855B1 (de
Inventor
Alexandr Grigorievich Ioltukhovsky
Maria Vladimirovna Leontieva-Smirnova
Alexandr Viktorovich Vatulin
Viktor Nikolaeyich Golovanov
Valentin Kuzmich Shamardin
Tatyana Mikhailovna Bulanova
Valentin Vladimirovich Tsevelev
Igor Alexeevich Shkabura
Jury Alexandrovich Ivanov
Vladimir Alexandrovich Forstman
Mikhail Ivanovich Solonin
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Federal State Unitarian Enterprise " Aa Bochvar All-Russia Research Institute Of Inorganic Materials"
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Federal State Unitarian Enterprise " Aa Bochvar All-Russia Research Institute Of Inorganic Materials"
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Publication of EP1693855A2 publication Critical patent/EP1693855A2/de
Publication of EP1693855A4 publication Critical patent/EP1693855A4/de
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Classifications

    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/22Ferrous alloys, e.g. steel alloys containing chromium with molybdenum or tungsten
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
    • C21D6/00Heat treatment of ferrous alloys
    • C21D6/002Heat treatment of ferrous alloys containing Cr
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/001Ferrous alloys, e.g. steel alloys containing N
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/005Ferrous alloys, e.g. steel alloys containing rare earths, i.e. Sc, Y, Lanthanides
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/12Ferrous alloys, e.g. steel alloys containing tungsten, tantalum, molybdenum, vanadium, or niobium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/24Ferrous alloys, e.g. steel alloys containing chromium with vanadium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/28Ferrous alloys, e.g. steel alloys containing chromium with titanium or zirconium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/32Ferrous alloys, e.g. steel alloys containing chromium with boron
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
    • C21D2211/00Microstructure comprising significant phases
    • C21D2211/005Ferrite
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
    • C21D2211/00Microstructure comprising significant phases
    • C21D2211/008Martensite

Definitions

  • the present invention relates to nuclear engineering range, specifically, to materials used in nuclear engineering and might be applied to fabricating fuel elements and components of fast nuclear reactor cores (below - BN reactors).
  • Low activation irradiation resistant steel is known (see RU patent N 2135623) that contains carbon, silicon, manganese, chromium, nickel, vanadium, copper, molybdenum, cobalt, tungsten, yttrium, niobium, aluminum and iron at the following ratio between components, percent by weight: carbon - 0.13-0.18; silicon 0.20-0.35; manganese - 0.30-0.60; chromium - 2.0-3.5; tungsten - 1.0-2.0; vanadium - 0.10-0.35; molybdenum 0 0.01-0.05; nickel - 0.01-0.05; cobalt - 0.01-0.05; copper - 0.01-0.10; aluminum - 0.01-0.10; niobium - 0.01-0.05; yttrium - 0.05-0.15; the balance being iron.
  • the total content of nickel, cobalt, molybdenum, niobium and copper makes up not more than 0.2 percent by weight, while the ratio (V+0.3W)C varies within 3 to 6.
  • This steel has low induced activity, however, is not heat resistant at a temperature exceeding 500°C (see M.V.Zakharov, A.M.Zakharov. Heat Resistant Alloys, M.: Metallurgy, 1972).
  • low activation heat resistant (up to 550°C) steel (according to RU patent N 2033461) that contains carbon, silicon, manganese, chromium, tungsten, vanadium, boron, titanium, cerium and iron at the following ratio between components, mass %: carbon - 0.10-0.20; silicon - 0.02-1.00; manganese - 0.50-2.0; chromium - 10.0-13.9; tungsten - 0.8-2.9; vanadium - 0.05-0.45; titanium - 0.01-0.10; boron - 0.0005-0.008; cerium - 0.001-0.100, the balance being iron.
  • EP823 steel A steel that in terms of composition of ingredients and functioning approaches most closely the claimed one is EP823 steel the composition and properties of which are described in the paper by M.I.Solonin., F.G.Reshetnicov, A.G.Ioltukhovsky and others "Novel Structural Materials for Cores of Nuclear Power Installations", in journal “Physics and Chemistry of Material Processing", 2001, N4, pp.17-27.
  • the steel contains, percent by weight: carbon -0.14-0.18; silicon - 1.1-1.3; manganese -0.5-0.8; chromium - 10.0-12.0; nickel - 0.5-0.8; vanadium - 0.2-0.4; molybdenum - 0.6-0.9; tungsten - 0.5-0.8; niobium - 0.2-0.4; boron - 0.006 (as calculated) cerium - not more than 0.1; nitrogen - not more than 0.05; sulphur - not more than 0.010; phosphorus - not more than 0.015; the balance being iron.
  • the major disadvantages of this steel are its high activation ability under neutron irradiation via neutron reactions on Ni, Mo, Nb, Cu, Co and other elements to form long-lived radioactive isotopes as well as low heat resistance at a temperature not lower than 650°C and propensity for LTIE within 270-400°C.
  • the technical objective of the invention is to create a BN reactor fuel element with a cladding having the following properties: low induced activity and a higher rate of its decay after exposure to neutrons, higher resistance to embrittlement in the temperature range from 270 to 400°C under neutron irradiation and a high heat resistance at temperatures up to 700°C.
  • the technical result is to create a fuel element with a cladding having a high resistance to embrittlement in the temperature range from 270 to 400°C as well as a higher level of heat resistance at temperatures up to 700°C and high performance.
  • the set up objective pertaining to the first version of realizing a BN reactor fuel element is put in practice via fabricating its cladding from ferritic-martensitic class steel having a non-uniform structure along a cladding length that consists of at least two zones; with the steel structure in the top zone of a fuel element providing its higher heat resistance and in the bottom zone enhancing its resistance to low temperature irradiation embrittlement.
  • the set up objective pertaining to the second version of realizing a BN reactor fuel element is put in practice via fabricating its cladding from low activation steel containing carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities at the following ratio between components, percent by weight:
  • the structure of the steel along a cladding length consists of at least two zones; with the steel structure in the top zone of a fuel element providing its higher heat resistance and containing ⁇ -ferrite, ⁇ - ferrite, sorbite, chromium carbides M 23 C 6 and M 6 C, carbides and carbonitrides of the steel components (V, Ta, Ti, Zr, W and others), intermetallics of the Fe 2 (W) type while the structure in the bottom zone enhancing its resistance to low temperature irradiation embrittlement consists of sorbite, ⁇ -ferrite, ⁇ -ferrite, residual austenite, carbides and carbonitrides of steel components (Cr, V, Na, W and others); in this case high-angle boundaries of grains are occupied by carbides M 23 C 6 and M 6 C while grains of both sorbite and ⁇ -fer
  • the set up objective is also put in practice via fabricating a cladding for a fast reactor fuel element from low activation steel containing carbon, silicon, manganese, chromium, vanadium, tungsten, boron, cerium and/or yttrium, titanium, tantalum, zirconium, nitrogen, iron and unavoidable impurities at the following ratio of components, percent by weight:
  • the steel structure along a cladding length consists of at least two zones: with the steel structure in the top zone of a fuel element providing its higher heat resistance and containing ⁇ -ferrite, sorbite, chromium carbides M 23 C 6 and M 6 C, carbides and carbonitrides of steel components (V, Ta, Ti, Zr, W and others), intermetallics of the Fe 2 (W) type while the structure in the bottom zone enhancing its resistance to low temperature irradiation embrittlement consists of sorbite, ⁇ -ferrite, ⁇ -ferrite, residual austenite, carbides and carbonitrides of steel components (Cr, V, Ta, W and others); in this case high-angle boundaries of grains are occupied by carbides M 23 C 6 and M 6 C while grains of both sorbite and ⁇ -ferrite have but individual precipitates of carbides and
  • the structure of a steel along a cladding length consists of three zones; with the middle zone structure having intermediate values of heat resistance and resistance to low temperature irradiation embrittlement in comparison to those in the bottom and top zones.
  • the total content of impurities of high activation metals viz., molybdenum, niobium, nickel, copper and cobalt, does not exceed 0.1 %mass. This serves to reduce neutron irradiation induced activation and to accelerate the decay rate of induced activation of steel.
  • the essence of the invention consists in the fact that the steel structure along a cladding length is made non-uniform and is brought in conformity with the actual temperature drop along the length of the BN reactor core which makes up several hundred degrees. That is why, the claimed invention puts in practice a novel principle of placing different requirements for the properties and structure of a fuel cladding along its length.
  • the steel structure in the bottom (low temperature) zone of a fuel cladding includes sorbite, ⁇ -ferrite, residual austenite, carbides of likely strong carbide forming components of the steel (Cr, V, Ti, Ta, W and others), nitrides and carbonitrides of the above mentioned elements; boundaries of large-angle grains are basically free from precipitates of carbides M 23 C 6 and M 6 C and have an intragranular coagulated carbide phase.
  • the low temperature zone of a fuel element is subjected to cycling (up to 10 cycles) which comprises heating to the temperature A C1 + 20°C and cooling to room temperature; in this case the rate of product cooling after tempering and in the process of cycling and after it is finished has not to be below 50°C/min upon cooling in air.
  • the steel is subjected to complex alloying with elements having a prompt decay of irradiation induced activity to attain a specified ratio between ⁇ -stabilizing elements (C, N, Mn) and ⁇ -stabilizing ones (Cr, W, V, Ta, Ti, Zr, Mo, Nb and others).
  • a stable martensitic - ferritic structure of a cladding that contains solid solution strengthening interstitial elements (C,N,B) and substitutional elements (W, V, Cr), strengthening carbide (MC, M 2 C, M 23 C 6 and others), nitride (MN, M 2 N) and carbonitride (MCN) phases as well as Laves phases of the Fe(W) type.
  • This structure in the high temperature zone of a fuel cladding is formed via quenching at a temperature of 1050-1150°C for 40 min followed by tempering at 680-760°C.
  • An increase in the content of tungsten that is introduced in place of molybdenum at an approximately equivalent ratio provides a lower irradiation induced activation of a cladding and its prompt decay with time after neutron exposure due to a lower section of neutron interaction with tungsten nuclei and a lower half-life of irradiation produced isotopes of tungsten, respectively.
  • An increase in the content of tungsten also promotes preservation of a high level of long-term and short-term strength of steel.
  • Cerium and/or yttrium introduced in the quantity of 0.001-0.10 %mass promotes the refining and atomizing of steel grains. In this case cerium and yttrium being low activation elements do not increase the induced activity of the steel claimed.
  • the low levels of cerium and/or yttrium content correspond to the minimal concentration at which its favourable influence on steel refining is noted.
  • the value of the upper limit of cerium and/or yttrium content promotes preservation of the adequate processability by steel at a hot stage.
  • the low limit of zirconium content is determined by the need of binding a part of nitrogen into finely dispersed and thermodynamically stable particles of zirconium nitride.
  • the upper limit of zirconium content is determined by the feasible formation of low melting zirconium-iron eutectic which might reduce the processability of steel.
  • the low limit of titanium content is determined by the need of binding a part of carbon into thermodynamically stable finely dispersed carbides of titanium.
  • the upper level of titanium content is determined by feasible redistribution of nitrogen between zirconium and titanium which is not desired because of a possible decrease in long-term strength of steel.
  • the low level of tantalum content is determined by the need of binding a part of carbon into thermodynamically stable tantalum carbides and ensuring its content in solid solution at the level of ultimate solubility.
  • the upper limit of tantalum content is determined by feasible formation of globular carbide inclusions that reduce the processability of steel.
  • the low limit of nitrogen content is determined by the need of binding zirconium into finely dispersed particles of zirconium nitride.
  • the restriction of the nitrogen upper limit is required to provide the processability of steel during welding: zirconium and tantalum being low activation elements do not increase the induced activity of the claimed steel.
  • Nitrogen as an isotope 14 N becomes activated under neutron irradiation to form a long-lived isotope 14 C that upon decaying (half-life of 5.7x10 3 years) produces ⁇ -particle (stable isotope 6 He) without resulting in ⁇ -radiation, i.e., the availability of nitrogen does not influence the decay of steel radiation activity determined by ⁇ -radiation.
  • the content of silicon ranges from 0.1 to 0.8 to ensure deoxidation of steel.
  • the content of manganese is kept at the level of 0.5-2.0 percent by weight.
  • the chromium content of the claimed steel is kept at the level of 10-13.5 percent by weight.
  • the carbon content of the claimed steel ranges within 0.10-0.21 percent by weight to provide for the high level of structural stability and heat resistance via the process of martensitic transformation.
  • Ingots 25 kg in mass were forged into billets 35 mm in the diameter that were then forged into plates 10mm thick and a bar 12mm in the diameter.
  • Ingots 500kg in mass were forged into billets 90mm in the diameter that were then rolled to produce a sheet 6mm thick and a bar 12mm in the diameter.
  • the bar, sheet and plates were heat treated under the standard conditions, namely, normalizing and tempering.
  • the heat treated metal was used to fabricate cylindrical samples with the effective part size ⁇ 5x25 mm to be tested for long-term strength and creep in compliance with GOST( ⁇ OCT) 10145-81 and GOST( ⁇ OCT) 3248-81.
  • Tensile properties also after irradiation were determined using standard samples in tensile tests according to GOST ( ⁇ OCT) 10446-80.
  • the indicated samples had to simulate the condition of the metal in the high temperature part of a fuel cladding at the operating temperature not lower than 600°C.
  • the samples were subjected to cycling, i.e., heating to the temperature A C1 +20°C, 10 min holding and cooling to room temperature at a rate of not less than 50°C/min within 600 to 20°C. Altogether 10 cycles were carried out. After the cyclic treatment the samples were subjected to tempering at 720°C for 2 h followed by accelerated cooling (not less than 50°C/min) to room temperature.
  • the claimed steel was neutron irradiated in research fast neutron reactor BOR-60 at a temperature of 345-365°C to the fluence of (1.14-2.0) 10 22 n/cm 2 (E>0.1MeV) at the damage dose of 5.8-8.0 dpa.
  • Tensile tests were conducted using remotely operated breaking machine 1794-Y5 in air at a strain rate of ⁇ 1 mm/min. Under the indicated conditions samples were irradiated that had been heat treated under the standard conditions as well as samples that had been subjected to the cyclic heat treatment.
  • the claimed fuel element cladding is usable in cores of fast neutron reactors.
  • the use of a fuel element with a cladding having the claimed properties shall provide for high cost-effectiveness due to a more prompt decay of induced activity and have high properties of heat resistance and resistance to low temperature irradiation embrittlement. This cost-effectiveness effect will manifest in lower contamination of environment effected by operating nuclear power facilities of novel generation and in feasibility of re-using structural materials. Table 2.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
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  • Crystallography & Structural Chemistry (AREA)
  • Heat Treatment Of Steel (AREA)
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  • Materials For Medical Uses (AREA)
EP04793751.1A 2003-10-06 2004-10-04 Brennstoffelement für einen schnellen neutronenreaktor (varianten) und mantelung für seine herstellung Expired - Lifetime EP1693855B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
RU2003129679/02A RU2262753C2 (ru) 2003-10-06 2003-10-06 Твэл реактора на быстрых нейтронах (варианты) и оболочка для его изготовления
PCT/RU2004/000384 WO2005034139A2 (fr) 2003-10-06 2004-10-04 Unite de combustible pour reacteur a neutrons rapides, et gaine permettant sa preparation

Publications (3)

Publication Number Publication Date
EP1693855A2 true EP1693855A2 (de) 2006-08-23
EP1693855A4 EP1693855A4 (de) 2013-01-02
EP1693855B1 EP1693855B1 (de) 2014-12-17

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EP04793751.1A Expired - Lifetime EP1693855B1 (de) 2003-10-06 2004-10-04 Brennstoffelement für einen schnellen neutronenreaktor (varianten) und mantelung für seine herstellung

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EP (1) EP1693855B1 (de)
CN (1) CN1890758B (de)
RU (1) RU2262753C2 (de)
WO (1) WO2005034139A2 (de)

Cited By (5)

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CN102194531A (zh) * 2010-03-11 2011-09-21 中国核动力研究设计院 快中子反应堆燃料双行波自分区燃烧方法
US20160225468A1 (en) * 2013-11-19 2016-08-04 Joint Stock Company "Akme-Engineering" Fuel rod cladding, fuel rod and fuel assembly
WO2017180647A1 (en) * 2016-04-11 2017-10-19 Terrapower, Llc High temperature, radiation-resistant, ferritic-martensitic steels
RU2634867C1 (ru) * 2016-12-28 2017-11-07 Акционерное общество "Научно-производственное объединение "Центральный научно-исследовательский институт технологии машиностроения", АО "НПО "ЦНИИТМАШ" Теплостойкая и радиационно-стойкая сталь
EP2938751B1 (de) * 2012-12-28 2022-07-27 TerraPower LLC Zusammensetzung auf eisenbasis für brennstoffelement

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RU2515716C1 (ru) * 2013-04-26 2014-05-20 Российская Федерация, от имени которой выступает Государственная корпорация по атомной энергии "Росатом" Малоактивируемая жаропрочная радиационностойкая сталь
KR101676243B1 (ko) * 2014-12-02 2016-11-30 현대자동차주식회사 고온 강도 및 내산화성이 우수한 내열주강
RU2615961C1 (ru) * 2015-11-26 2017-04-11 Российская Федерация, от имени которой выступает Государственная корпорация по атомной энергии "Росатом" Узел сварного соединения оболочки тепловыделяющего элемента с заглушкой, выполненных из высокохромистой стали (варианты)
RU2603355C1 (ru) * 2015-11-26 2016-11-27 Российская Федерация, от имени которой выступает Государственная корпорация по атомной энергии "Росатом" Способ герметизации тепловыделяющих элементов ядерного реактора с оболочкой из высокохромистой стали
CN108356263B (zh) * 2018-04-28 2019-09-24 苏州大学 激光增材制造用新型马氏体耐热钢合金粉末及其制备方法
RU2683168C1 (ru) * 2018-05-15 2019-03-26 Акционерное общество "Научно-производственное объединение "Центральный научно-исследовательский институт технологии машиностроения", АО "НПО "ЦНИИТМАШ" Нейтронно-поглощающая сталь
CN112695255B (zh) * 2020-11-27 2021-09-17 中国核动力研究设计院 一种铁素体马氏体钢包壳管材制备方法
CN112695256A (zh) * 2020-11-27 2021-04-23 中国核动力研究设计院 一种铁素体马氏体钢包壳材料及其制备方法
CN113355497B (zh) * 2021-06-04 2022-05-31 西安建筑科技大学 一种低活化钢钢板及其制备工艺
CN114959484B (zh) * 2022-06-06 2023-04-25 武汉钢铁有限公司 一种80级胎圈钢丝用热轧盘条及其制备方法、汽车轮胎

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CN102194531A (zh) * 2010-03-11 2011-09-21 中国核动力研究设计院 快中子反应堆燃料双行波自分区燃烧方法
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US20160225468A1 (en) * 2013-11-19 2016-08-04 Joint Stock Company "Akme-Engineering" Fuel rod cladding, fuel rod and fuel assembly
US10720244B2 (en) * 2013-11-19 2020-07-21 Joint Stock Company “Akme-Engineering” Fuel rod cladding, fuel rod and fuel assembly
WO2017180647A1 (en) * 2016-04-11 2017-10-19 Terrapower, Llc High temperature, radiation-resistant, ferritic-martensitic steels
RU2634867C1 (ru) * 2016-12-28 2017-11-07 Акционерное общество "Научно-производственное объединение "Центральный научно-исследовательский институт технологии машиностроения", АО "НПО "ЦНИИТМАШ" Теплостойкая и радиационно-стойкая сталь

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CN1890758A (zh) 2007-01-03
CN1890758B (zh) 2010-07-21
WO2005034139A3 (fr) 2005-07-28
EP1693855A4 (de) 2013-01-02
WO2005034139A2 (fr) 2005-04-14
EP1693855B1 (de) 2014-12-17
RU2262753C2 (ru) 2005-10-20
RU2003129679A (ru) 2005-04-10

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