WO2016122374A1 - Fuel for water-cooled nuclear reactors - Google Patents

Fuel for water-cooled nuclear reactors Download PDF

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Publication number
WO2016122374A1
WO2016122374A1 PCT/SE2016/000004 SE2016000004W WO2016122374A1 WO 2016122374 A1 WO2016122374 A1 WO 2016122374A1 SE 2016000004 W SE2016000004 W SE 2016000004W WO 2016122374 A1 WO2016122374 A1 WO 2016122374A1
Authority
WO
WIPO (PCT)
Prior art keywords
fuel
water
porosity
uranium
cooled nuclear
Prior art date
Application number
PCT/SE2016/000004
Other languages
French (fr)
Inventor
Mikael Jolkkonen
Kyle Johnson
Janne Wallenius
Original Assignee
Blykalla Reaktorer Stockholm Ab
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 Blykalla Reaktorer Stockholm Ab filed Critical Blykalla Reaktorer Stockholm Ab
Priority to CA3010876A priority Critical patent/CA3010876C/en
Publication of WO2016122374A1 publication Critical patent/WO2016122374A1/en

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Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G21C3/62—Ceramic fuel
    • 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 nuclear fuel is intended to permit longer residence time, alternatively a higher power, or a combination thereof for water-cooled nuclear reactor fuels.
  • the actinide density of the fuel exceeds 9.7 g/cm 3 and its open porosity is sufficiently low to significantly improve the corrosion resistance of the fuel.
  • the fuel pellet is manufactured using conventional sintering, hot pressing, field assisted hot pressing, microwave assisted hot pressing or spark plasma sintering (SPS).
  • SPS spark plasma sintering
  • the fuel consists of more than 80 volume percent uranium nitride (UN), with an open porosity below 0.1 %.
  • the fuel consists of more than 80 volume percent uranium nitride (UN), with an open porosity below 0.1 %. Up to 20 volume percent consists of a secondary phase with a lower melting point than UN, which thanks to higher plasticity acts as pore filler during sintering.
  • UN uranium nitride
  • the purpose of the present invention is to provide a nuclear fuel combining an actinide density higher than 9.7 g/cm 3 with an improved tolerance to water and steam at temperatures exceeding 250°C.
  • a specific purpose of the present invention is to provide a uranium nitride fuel with improved tolerance to water and steam at temperatures exceeding 250°C.
  • the invention offers a solution to problems of corrosion of nuclear fuels with an actinide density higher than 9.7 g/cm 3 that have been observed during exposure to water and steam at temperatures exceeding 250°C, and therefore facilitates the use of this fuel type in commercial water-cooled nuclear power plants.
  • nitride fuels have historically been difficult to manufacture with high density, resulting in a considerable fraction of open porosity in the pellets produced. Therefore, steam and pressurised hot water may penetrate and deeply oxidise the pellet.
  • the larger specific volume of the forming uranium dioxide causes an inner expansion which rapidly fragmentises and eventually powderises the pellet.
  • uranium nitride fuels By manufacturing uranium nitride fuels, uranium silicide fuels and mixtures of these fuels with a sufficiently low fraction of open porosity, the oxidation process is limited to surface corrosion, which considerably delays the decomposition of the fuel.
  • Uranium nitride fuels with very low porosity may be manufactured using spark plasma sintering (SPS) at a temperature exceeding 1600°C [Malkki 2014].
  • SPS spark plasma sintering
  • Another opportunity for eliminating open porosity in a uranium nitride fuel is achieved by blending a certain fraction of uranium silicide, having a melting temperature below 1600°C, into uranium nitride.
  • the uranium silicide will, thanks to its plasticity, constitute a pore filling second phase, reducing the porosity of the pellet.
  • the invention is especially useful in light water and heavy water cooled nuclear power reactors.
  • Example 1 The invention is especially useful in light water and heavy water cooled nuclear power reactors.
  • uranium nitride pellets consisting of more than 80% UN, with a varying degree of porosity and content of UO2, U2N3 and uranium silicide.
  • UO2, U2N3 and uranium silicide During exposure of UN to steam, uranium dioxide, ammonia and hydrogen gas form according to the reaction formula:
  • Figure 1 shows the measured rate of production for hydrogen and total hydrogen production rate as function of time for uranium nitride pellets with 2.3%, 13.0% and 22.4% porosity.
  • uranium nitride pellets with varying degree of open porosity were manufactured using the SPS-method at different temperatures and pressures.
  • the open porosity was measured using Archimedes' method with chloroform as medium.
  • Figure 2 displays the open porosity as function of total porosity. The measurements show that when the total porosity of the uranium nitride pellet is less than 2.5%, open porosity is less than 0.1 %.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Ceramic Engineering (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Ceramic Products (AREA)

Abstract

The invention refers to a nuclear fuel for use in water cooled nuclear reactors. The fuel, which consists of at least 80 % uranium nitride, has an actinide density higher than 9.7 g/cm3 and an open porosity of less than 0.1 %. Consequently, the fuel is resistant to attacks from water and stream and can be used at temperatures above 250 degrees Centigrade.

Description

Fuel for water-cooled nuclear reactors
Description of the invention
The nuclear fuel is intended to permit longer residence time, alternatively a higher power, or a combination thereof for water-cooled nuclear reactor fuels. The actinide density of the fuel exceeds 9.7 g/cm3 and its open porosity is sufficiently low to significantly improve the corrosion resistance of the fuel. The fuel pellet is manufactured using conventional sintering, hot pressing, field assisted hot pressing, microwave assisted hot pressing or spark plasma sintering (SPS). In a preferred embodiment, the fuel consists of more than 80 volume percent uranium nitride (UN), with an open porosity below 0.1 %.
In another preferred embodiment, the fuel consists of more than 80 volume percent uranium nitride (UN), with an open porosity below 0.1 %. Up to 20 volume percent consists of a secondary phase with a lower melting point than UN, which thanks to higher plasticity acts as pore filler during sintering.
Summary of the invention
The purpose of the present invention is to provide a nuclear fuel combining an actinide density higher than 9.7 g/cm3 with an improved tolerance to water and steam at temperatures exceeding 250°C. A specific purpose of the present invention is to provide a uranium nitride fuel with improved tolerance to water and steam at temperatures exceeding 250°C.
This and other objectives are achieved by the invention as defend in the independent claims.
Yet other advantageous embodiments of the invention are specified in the dependent claims. The invention offers a solution to problems of corrosion of nuclear fuels with an actinide density higher than 9.7 g/cm3 that have been observed during exposure to water and steam at temperatures exceeding 250°C, and therefore facilitates the use of this fuel type in commercial water-cooled nuclear power plants. Especially nitride fuels have historically been difficult to manufacture with high density, resulting in a considerable fraction of open porosity in the pellets produced. Therefore, steam and pressurised hot water may penetrate and deeply oxidise the pellet. The larger specific volume of the forming uranium dioxide causes an inner expansion which rapidly fragmentises and eventually powderises the pellet. By manufacturing uranium nitride fuels, uranium silicide fuels and mixtures of these fuels with a sufficiently low fraction of open porosity, the oxidation process is limited to surface corrosion, which considerably delays the decomposition of the fuel.
Experiments on pellets with different porosity confirm that the rate of attack is more dependent on the porosity of the pellet than on reaction temperature, supporting the conclusion that improved protection against corrosion in steam and pressurised hot water is most easily achieved by eliminating the open porosity.
Uranium nitride fuels with very low porosity may be manufactured using spark plasma sintering (SPS) at a temperature exceeding 1600°C [Malkki 2014]. Another opportunity for eliminating open porosity in a uranium nitride fuel is achieved by blending a certain fraction of uranium silicide, having a melting temperature below 1600°C, into uranium nitride. During pellet manufacture at a temperature above 1600°C the uranium silicide will, thanks to its plasticity, constitute a pore filling second phase, reducing the porosity of the pellet. Industrial applicability
The invention is especially useful in light water and heavy water cooled nuclear power reactors. Example 1)
In this example, laboratory tests were conducted on uranium nitride pellets consisting of more than 80% UN, with a varying degree of porosity and content of UO2, U2N3 and uranium silicide. During exposure of UN to steam, uranium dioxide, ammonia and hydrogen gas form according to the reaction formula:
UN + 2H2O -> UO2 + NH3 + 0.5 H2
Parameters of the test:
Steam pressure: 0.5 bar Steam temperature: 400 - 425°C
The lab tests showed that the rate of corrosion attack on the uranium nitride pellet is strongly dependent of its porosity.
Figure 1 shows the measured rate of production for hydrogen and total hydrogen production rate as function of time for uranium nitride pellets with 2.3%, 13.0% and 22.4% porosity.
Example2)
In this example, uranium nitride pellets with varying degree of open porosity were manufactured using the SPS-method at different temperatures and pressures. The open porosity was measured using Archimedes' method with chloroform as medium. Figure 2 displays the open porosity as function of total porosity. The measurements show that when the total porosity of the uranium nitride pellet is less than 2.5%, open porosity is less than 0.1 %.

Claims

Claims
1 . A nuclear fuel for power production in water-cooled nuclear reactors, wherein the actinide density exceeds 9.7 g/cm3, wherein the fuel consists of at least 80 volume percent UN and wherein the open porosity is less than 0.1 %.
2. A nuclear fuel according to claim 1 , wherein up to 20 volume percent consists of a uranium silicide compound.
PCT/SE2016/000004 2015-01-30 2016-01-29 Fuel for water-cooled nuclear reactors WO2016122374A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CA3010876A CA3010876C (en) 2015-01-30 2016-01-29 Nuclear fuel for water-cooled nuclear reactors

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
SE1500058A SE1500058A1 (en) 2015-01-30 2015-01-30 Fuel for water-cooled nuclear reactors
SE1500058-1 2015-01-30

Publications (1)

Publication Number Publication Date
WO2016122374A1 true WO2016122374A1 (en) 2016-08-04

Family

ID=56543844

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/SE2016/000004 WO2016122374A1 (en) 2015-01-30 2016-01-29 Fuel for water-cooled nuclear reactors

Country Status (3)

Country Link
CA (1) CA3010876C (en)
SE (1) SE1500058A1 (en)
WO (1) WO2016122374A1 (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110415845A (en) * 2019-08-06 2019-11-05 中国核动力研究设计院 A kind of high uranium density hybrid fuel pellet and preparation method thereof

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1366923A (en) * 1970-11-12 1974-09-18 Nukem Gmbh Production of nuclear fuel
US20110206174A1 (en) * 2010-02-22 2011-08-25 Westinghouse Electric Sweden Ab Nuclear fuel, a fuel element, a fuel assembly and a method of manufacturing a nuclear fuel
WO2014028731A1 (en) * 2012-08-15 2014-02-20 University Of Florida Research Foundation, Inc. High density uo2 and high thermal conductivity uo2 composites by spark plasma sintering (sps)

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1366923A (en) * 1970-11-12 1974-09-18 Nukem Gmbh Production of nuclear fuel
US20110206174A1 (en) * 2010-02-22 2011-08-25 Westinghouse Electric Sweden Ab Nuclear fuel, a fuel element, a fuel assembly and a method of manufacturing a nuclear fuel
WO2014028731A1 (en) * 2012-08-15 2014-02-20 University Of Florida Research Foundation, Inc. High density uo2 and high thermal conductivity uo2 composites by spark plasma sintering (sps)

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
MALKKI, P. ET AL.: "Manufacture of fully dense uranium nitride pellets using hydride derived powders with spark plasma sintering", JOURNAL OF NUCLEAR MATERIALS, vol. 452, no. 1- 3, 19 June 2014 (2014-06-19), pages 548 - 551 *
MALKKI, P., THE MANUFACTURING OF URANIUM NITRIDE FOR POSSIBLE USE IN LIGHT WATER REACTORS, 8 June 2015 (2015-06-08), Stockholm *
MUTA ET AL.: "Characterization of composite nitride pellet prepared by SPS technique", MATERIALS SCIENCE AND TECNHOLOGY, 5 October 2008 (2008-10-05) *

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110415845A (en) * 2019-08-06 2019-11-05 中国核动力研究设计院 A kind of high uranium density hybrid fuel pellet and preparation method thereof
CN110415845B (en) * 2019-08-06 2021-06-11 中国核动力研究设计院 High-uranium-density composite fuel pellet and preparation method thereof

Also Published As

Publication number Publication date
CA3010876A1 (en) 2016-08-04
SE1500058A1 (en) 2016-07-31
CA3010876C (en) 2023-08-29

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