US20110091004A1 - Triso fuel for high burn-up nuclear engine - Google Patents

Triso fuel for high burn-up nuclear engine Download PDF

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US20110091004A1
US20110091004A1 US12/681,339 US68133908A US2011091004A1 US 20110091004 A1 US20110091004 A1 US 20110091004A1 US 68133908 A US68133908 A US 68133908A US 2011091004 A1 US2011091004 A1 US 2011091004A1
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Prior art keywords
fuel
layer
silicon carbide
particle
kernel
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Joseph C. Farmer
Magdelana Serrano de Caro
Jaime Marian
Paul P. Demange
Athanasios Arsenlis
Joe H. Satcher, Jr.
Jeffery F. Latkowski
Ryan P. Abbott
Tomas Dias de la Rubia
Edward I. Moses
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Lawrence Livermore National Security LLC
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Lawrence Livermore National Security LLC
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Priority to US12/681,339 priority Critical patent/US20110091004A1/en
Assigned to L\\ reassignment L\\ ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: FARMER, JOSEPH C., MOSES, EDWARD I., DIAZ DE LA RUBIA, TOMAS, DEMANGE, PAUL P., ABBOTT, RYAN P., ARSENLIS, TOM, LATKOWSKI, JEFFERY F., SERRANO DE CARA, MAGDALENA, MARIAN, JAMIE, SATCHER, JOE H.
Assigned to U.S. DEPARTMENT OF ENERGY reassignment U.S. DEPARTMENT OF ENERGY CONFIRMATORY LICENSE (SEE DOCUMENT FOR DETAILS). Assignors: LAWRENCE LIVERMORE NATIONAL SECURITY, LLC
Publication of US20110091004A1 publication Critical patent/US20110091004A1/en
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21B—FUSION REACTORS
    • G21B1/00—Thermonuclear fusion reactors
    • G21B1/01—Hybrid fission-fusion nuclear reactors
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21B—FUSION REACTORS
    • G21B1/00—Thermonuclear fusion reactors
    • G21B1/11—Details
    • G21B1/19—Targets for producing thermonuclear fusion reactions, e.g. pellets for irradiation by laser or charged particle beams
    • 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
    • G21C3/626—Coated fuel particles
    • 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
    • Y02E30/10—Nuclear fusion reactors
    • 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
    • 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
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T50/00—Aeronautics or air transport
    • Y02T50/60—Efficient propulsion technologies, e.g. for aircraft
    • Y02T50/678—Aviation using fuels of non-fossil origin

Definitions

  • IPCC Intergovernmental Panel on Climate Change
  • Nuclear energy a non-carbon emitting energy source
  • nuclear reactors In the United States alone, nuclear reactors have already generated more than 55,000 metric tons (MT) of spent nuclear fuel (SNF).
  • ICF Inertial Confinement Fusion
  • D deuterium
  • T tritium
  • MFE Magnetic Fusion Energy
  • an embodiment of the present invention provides an enhanced fuel particle suitable for use in a laser inertial confinement fusion-fission power plant.
  • the invention has been applied to the design and fabrication of a robust tristructural-isotropic (TRISO) particle capable of high burn-up as well as a fuel pebble including a plurality of the robust TRISO particles.
  • TRISO tristructural-isotropic
  • the methods and systems described herein are also applicable to other nuclear power plant designs.
  • a fuel particle for use in a fusion-fission nuclear engine includes a fuel kernel and a buffer layer surrounding the fuel kernel.
  • the fuel particle also includes a pyrolytic carbon layer surrounding the buffer layer and a silicon carbide layer surrounding the buffer layer.
  • the silicon carbide is characterized by a stress less than 450 MPa at 95% burn-up.
  • the intrinsic tensile strength of the SiC capsule is assumed to be approximately 450 MPa. Of course this value may change for different types of silicon carbide.
  • the fuel particle further includes a second pyrolytic carbon layer surrounding the silicon carbide layer.
  • a method of fabricating a fuel particle for a fusion-fission nuclear engine includes forming a fuel kernel and forming a buffer layer surrounding the fuel kernel. The method also includes forming a first pyrolytic carbon layer surrounding the buffer layer and forming a silicon carbide layer surrounding the first pyrolytic carbon layer. The silicon carbide layer is characterized by a thickness greater than 60 ⁇ m. The method further includes forming a second pyrolytic carbon layer surrounding the silicon carbide layer.
  • a fuel pebble for use in a fusion-fission nuclear engine includes a plurality of fuel particles disposed in a matrix material.
  • Each of the fuel particles includes a fuel kernel, a buffer layer surrounding the fuel kernel, and a pyrolytic carbon layer surrounding the buffer layer.
  • Each of the fuel particles also includes a silicon carbide layer surrounding the buffer layer and a second pyrolytic carbon layer surrounding the silicon carbide layer.
  • the silicon carbide layer is characterized by a thickness greater than 60 ⁇ m.
  • the fuel pebble also includes a cladding layer enclosing the plurality of fuel particles and the matrix material.
  • the present technique provides a robust fuel for Laser Inertial-confinement Fusion-fission Energy (often referred to herein as LIFE) nuclear engines that is able to achieve high (e.g., over 95% and up to 99.9%) burn-up of the fissile material in the kernel of the fuel.
  • LIFE Laser Inertial-confinement Fusion-fission Energy
  • fuel particles described herein provide a mechanism for disposing of weapons grade plutonium and highly enriched uranium. Depending upon the embodiment, one or more of these benefits may be achieved.
  • FIG. 1 is a diagram illustrating a conventional TRISO fuel particle
  • FIG. 2A is a simplified diagram of a high burn-up TRISO fuel particle according to an embodiment of the present invention
  • FIG. 2B is a simplified diagram of a fuel pebble including high burn-up TRISO fuel particles according to an embodiment of the present invention
  • FIG. 3 is a simplified flowchart illustrating a method of fabricating a high burn-up fuel pebble according to an embodiment of the present invention
  • FIG. 4 is a diagram illustrating operational experience with TRISO fuels
  • FIG. 5 is a plot illustrating the wall stress in the high burn-up TRISO fuel particle and fuel pebble illustrated in FIGS. 2A and 2B ;
  • FIG. 6 shows a plot of the swelling of SiC as a function of irradiation temperature
  • FIG. 7 is a plot of wall stress as a function of burn-up percentage according to an embodiment of the present invention.
  • FIG. 8 is a simplified plot of temperature of portions of the enhanced TRISO particle as a function of time.
  • FIG. 9 is a table illustrating various design studies for fuel pebbles including high burn-up TRISO particles.
  • an embodiment of the present invention provides an enhanced fuel particle suitable for use in a laser inertial confinement fusion-fission power plant.
  • a laser inertial confinement fusion-fission power plant Such an engine is described in more detail in our commonly assigned copending U.S. patent application Ser. No. ______, entitled “Control of a Laser Inertial Confinement Fusion-Fission Power Plant,” filed contemporaneously with this application, the contents of which are incorporated by reference.
  • the invention has been applied to the design and fabrication of a robust tristructural-isotropic (TRISO) particle capable of high burn-up as well as a fuel pebble including a plurality of the robust TRISO particles.
  • TRISO tristructural-isotropic
  • FIG. 1 is a diagram illustrating a conventional tristructural-isotropic (TRISO) fuel particle 100 .
  • TRISO fuel which is a type of micro fuel particle, consists of a fuel kernel 110 coated with four layers of three isotropic materials.
  • the fuel kernel 110 in the center of the fuel particle 100 is typically made of uranium dioxide (UO 2 ) or uranium oxy-carbide (UOC).
  • the fuel kernel is coated with a porous buffer layer made of carbon 110 , followed by a dense inner layer of pyrolytic carbon (PyC) 120 , followed by a ceramic layer of silicon carbide (SiC) 130 .
  • the outer layer of the TRISO fuel particle is a dense layer of PyC 140 .
  • the TRISO fuel particles described herein are designed to resist cracking, which results from stresses associated with processes such as fission gas pressure.
  • An example of a reactor design in which TRISO fuel particles are utilized is the pebble bed reactor (PBR), in which thousands of TRISO fuel particles are dispersed into graphite pebbles.
  • PBR pebble bed reactor
  • the PBR is a high temperature reactor.
  • FIG. 2A is a simplified diagram of a high burn-up TRISO fuel particle according to an embodiment of the present invention.
  • the high burn-up TRISO fuel particle is approximately 1 mm in diameter and comprises a number of layers and includes a fuel kernel 210 coated with multiple layers of isotropic materials.
  • the fuel kernel 210 is typically made of uranium oxy-carbide (UOC) although other materials including uranium oxide (UO), uranium dioxide (UO 2 ), weapons-grade plutonium, spent nuclear fuel, depleted uranium, natural uranium, highly enriched uranium, and the like can be used in the fuel kernel.
  • UOC uranium oxy-carbide
  • the fuel kernel is surrounded by a porous carbon buffer layer 220 that attenuates fission recoils and reacts with the gaseous fission products to lower the pressure within the fuel particle.
  • a feature of this approach is the minimal SiC wall thickness capable of maintaining the fission gas pressure at high Fissions per Initial Metal Atom (FIMA), and the corresponding buffer layer thickness, providing volume for the fission gas expansion.
  • FIMA Fissions per Initial Metal Atom
  • the porous buffer layer not only serves to provide space for entrapment of fission gases, but may include sacrificial silicon carbide that can react with palladium and other fission products, thereby preventing these deleterious elements from reacting with the silicon carbide encapsulation shell 240 .
  • the sacrificial carbon can be formed as a layer or can be distributed throughout the porous buffer layer.
  • a zirconium carbide (ZrC) diffusion barrier is positioned surrounding the fuel kernel in order to prevent direct contact of fission products from the kernel with the SiC containment shell 240 . This ZrC diffusion barrier could be positioned either on the inner surface of layer 230 , the inner surface of layer 240 , or both. Additionally, ZrC can serve as an oxygen getter to reduce the oxygen pressure due to the generation of free oxygen from, for example, UOC.
  • the silicon carbide sacrificial material and/or the zirconium carbide diffusion barrier may be formed, either as sequential single layers or as a multi-layer stack in which each of the layers, which may be referred to as sub-layers, is deposited one or more times in a periodic or non-periodic manner.
  • each of the layers which may be referred to as sub-layers
  • several layers of the zirconium carbide diffusion barrier may be deposited in conjunction with the other sub-layers to form the multipurpose buffer “layer” 220 .
  • An inner high thermal conductivity ( ⁇ ) pyrolytic carbon (PyC) layer 230 , a silicon carbide layer 240 , an outer, low p PyC layer 232 , and a protective layer of PyC 250 complete the structure of the fuel particle 200 .
  • the inner PyC layer 230 protects the SiC layer 240 by limiting the interaction between the SiC layer and the fuel kernel.
  • the PyC layer 230 provides structural support to the SiC layer 240 in addition to reducing or preventing reactions between the metallic fission products and the SiC shell 240 .
  • the outer PyC layer 232 and the protective PyC layer 250 protect the particle. If a particle were to crack internally, these layers will serve to prevent the molten salt coolant from leaching radioactive materials, such as UOC, from the fuel particles.
  • the SiC shell 240 is preferably substantially thicker than corresponding layers found in conventional TRISO fuel particles.
  • the thickness of the SiC shell 240 (sometimes referred to as a containment shell or vessel) ranges from about 60 ⁇ m to about 200 ⁇ m.
  • the thickness of the SiC shell 240 is 120 ⁇ m.
  • the thickness is about 70 ⁇ m, about 80 ⁇ m, about 100 ⁇ m, about 120 ⁇ m, or thicker than 120 ⁇ m. In other embodiments, the thickness varies as appropriate to the particular application.
  • the SiC shell 240 serves as a pressure vessel to contain the gaseous and metallic fission products.
  • the SiC layer is formed using a chemical vapor deposition (CVD) process, although other layer formation processes are included within the scope of the present invention.
  • CVD chemical vapor deposition
  • the thickness of the SiC shell is increased in comparison to conventional particles and is sufficient to resist stress from the fission gases as they accumulate with the burning of the fuel kernel in the particle during a high burn-up fuel cycle. Without the protection provided by the SiC shell of the present invention, it is possible that fission gases can escape from the fuel particle and then circulate in the coolant loop.
  • the enhanced TRISO particles described herein are optimized to provide mechanical strength against cracking or failure of the particle during a high burn-up cycle.
  • the burn-up may progress to 99.9% FIMA utilizing embodiments of the present invention.
  • the enhanced or high burn-up TRISO particles described herein provide a high mass fraction of fissile material.
  • the design of the various materials and layer dimensions provides for a kernel of sufficient size, a buffer layer able to absorb fission gases and other byproducts produced during the high burn-up fuel cycle, a SiC containment shell able to withstand the fission gas accumulation pressure at high burn-up percentages (e.g., in excess of 95% FIMA), and the like.
  • the inventors have balanced the strength of the TRISO particle to withstand high burn-up and the accompanying fission gas pressures against the mass fraction of fissile material in the particle and the fuel pebble.
  • the mass fraction of fissile fuel in the enhanced TRISO particle is increased as illustrated in FIG. 9 .
  • FIG. 2B is a simplified diagram of a fuel pebble including high burn-up TRISO fuel particles according to an embodiment of the present invention.
  • the fuel pebble 260 includes a number of TRISO particles 200 that are grouped together into the fuel pebble.
  • a 2-cm diameter pebble can contain many 2-mm diameter enhanced TRISO fuel particles that are embedded in a graphite or a similar inert matrix material.
  • the fuel pebble includes a cladding layer 270 made of a material compatible with molten salt coolants, i.e., a material that is resistant to attack from the molten salt coolant utilized to remove heat from the fuel pebble.
  • Tritium fluoride which behaves like hydrofluoric acid is formed in the molten salt coolant as a result of the transmutation of lithium by the neutron flux. Therefore, the cladding layer 270 is incorporated into the design to provide resistance to attack by hydrofluoric acid.
  • embodiments of the present invention utilize cladding layers including refractory metals such as tungsten and vanadium, refractory metal carbides, oxide-dispersion strengthened (ODS) ferritic steels, or the like.
  • the fuel particles 200 are supported in the cladding 270 by an inert matrix material 280 such as graphite, zirconium carbide, ODS ferritic steels, or the like.
  • the fuel particles and pebble described herein are only exposed to temperatures below the melting point of the fuel particles and pebble, typically between 500° C. and 750° C.
  • the fuel pebbles are marked or encoded with a unique identifier, for example, a bar code, an individual number, or the like.
  • This unique identifier can be used to individually track the fuel pebbles for accounting of the fuel. Because the fuel pebbles can be individually marked and tracked, diversion of large numbers of fuel pebbles is difficult. It should be noted that such individual marking and tracking is not generally possible with conventional TRISO particles.
  • each fuel pebble contains enough of the TRISO fuel particles to emit enough radiation to prevent manual removal without personal harm.
  • the pebbles are self protecting.
  • One fuel pebble emits more radiation than a convention fuel rod, yet to accumulate enough nuclear material to be of concern, on the order of 30,000 fuel pebbles need to be acquired. Therefore, an attempt to refine the fuel kernel from the fuel particles is a difficult task at best.
  • FIG. 3 is a simplified flowchart illustrating fabrication of a fabricating a high burn-up fuel pebble according to an embodiment of the present invention.
  • the fabrication of an enhanced TRISO particle begins with the process of making the fissile kernel.
  • uranium ore either from natural uranium, or depleted uranium (DU) is provided 310 .
  • DU depleted uranium
  • WG-Pu weapons-grade plutonium
  • HEU highly enriched uranium
  • LWR light water reactor
  • SNF spent nuclear fuel
  • the uranium ore is pelletized ( 312 ) and dissolved in a broth, typically utilizing nitric acid (HNO 3 ), Urea, or the like.
  • the uranium broth is flowed through a drop column ( 316 ), washed in water ( 318 ) and alcohol ( 320 ).
  • the uranium fuel is kiln dried ( 322 ), sintered ( 324 ), calcined ( 326 ), tabled ( 328 ), and screened ( 330 ).
  • the screening is the final step in the fabrication of the kernel in the embodiment illustrated in FIG. 3 .
  • Other fertile or fissile materials will be made into kernels utilizing other processes as will be evident to one of skill in the art. Also note the possible use of porous foams of fertile material such as uranium in enhanced TRISO fuels.
  • the kernel illustrated as element 210 in FIG. 2A , is coated with a buffer layer 220 that can include a porous material configured to absorb fission gases, a sacrificial SiC material that serves as a palladium getter ( 331 ), a zirconium carbide diffusion barrier and getter ( 333 ), combinations of these materials, and the like.
  • the porous buffer layer is preferably a nano-porous foam material.
  • the foam materials may include carbon aerogels, silica aerogels, and uranium foams.
  • the foam material includes a metal foam. In some embodiments, this foam material provides a source of sacrificial silicon carbide as well as providing regions for storage of fission gases generated in the kernel via chemisorption on the surface of the foam.
  • the buffer layer can include a sacrificial silicon carbide material.
  • the sacrificial silicon carbide can react with palladium produced as a fission byproduct to form Pd 5 Si. Since the LIFE engine typically operates at a temperature of less than 800° C., the Pd 5 Si remains in a solid form and does not melt. Thus, even if the palladium gas reaches layer 240 , it can react to form a stable, solid material. The consumption of the palladium in the buffer prevents the palladium from reacting with and thereby degrading the silicon carbide layer 240 .
  • Embodiments using a ZrC diffusion barrier prevent or reduce the ability of fission products to react with the SiC containment shell.
  • the sacrificial SiC will react with palladium to form the high-melting 1:3:3:5 Pd:U:Si:C compound.
  • the fuel kernel and buffer layer combination are placed in a chemical vapor deposition (CVD) reactor to deposit the inner pyrolytic carbon layer ( 332 ).
  • the CVD reactor may utilize a reduced or atmospheric pressure, plasma enhancement, or the like.
  • the thickness and resistivity of the inner PyC layer are predetermined depending on the particular application.
  • Either the same or a different CVD reactor is utilized 334 to form the silicon carbide layer 240 .
  • trimethyl silicon chloride (SiCl(CH 3 ) 3 ) is used in depositing the silicon carbide containment layer.
  • the thickness of the containment layer is a predetermined value that provides for mechanical strength sufficient to withstand the fission gas pressure at high burn-up percentages.
  • Either the same or a different CVD reactor 332 or 336 is utilized to form the outer PyC layer 232 .
  • the interfaces between various layers of the structure are not exposed to an ambient environment during the CVD process, improving the fuel performance.
  • a single CVD reactor is utilized with multiple gas sources.
  • multiple CVD reactors joined by a load-lock vacuum interface can be utilized to achieve results similar to those achieved with a single reactor.
  • embodiments of the present invention utilize the equivalent to a single CVD process to form fuel particles that avoid interfacial problems. Additional protective PyC layers (e.g., layer 250 ) may be formed as appropriate.
  • the inventors have determined that the anisotropic swelling of the inner and outer pyrolytic graphite layers 230 and 232 , as well as the graphite binder in the pebbles, may adversely affect the lifetime of high burn-up TRISO fuels. It has been determined that the swelling of the lattice normal to the hexagonal planes (along the c-axis) is substantially greater than that parallel to the planes (along the a-axis). Thus, a material that swells isotropically, and to a lesser extent, is preferable. Thus, in some embodiments, the deposition processes utilized to form the PyC layers is modified to result in smaller grain sizes in the graphite, which can result in less anisotropy. Additionally, the inventors have noted that continuous growth processes tend to produce smaller grain sizes.
  • the particles with the outer PyC layer are tabled ( 338 ), screened ( 340 ), and put through elutriation columns ( 342 ) to purify and separate the particles on the basis of particle density.
  • the particles are combined with a binder in a compaction press ( 344 ) and/or the inert matrix material 280 .
  • the compacted fuel particles/matrix material forms a portion of the fuel pebble, which is about 2-4 cm in diameter.
  • the partially formed pebble is placed in a carburization furnace ( 346 ) and heat treated ( 348 ) before formation of the cladding layer ( 350 ).
  • the cladding layer which is typically a refractory metal, is resistant to dissolution in the molten salt coolants utilized in some engine designs.
  • FIG. 3 provides a particular method of fabricating a high burn-up TRISO fuel pebble 352 according to an embodiment of the present invention.
  • Other sequences of steps may also be performed according to alternative embodiments.
  • alternative embodiments of the present invention may perform the steps outlined above in a different order.
  • the individual steps illustrated in FIG. 3 may include multiple sub-steps that may be performed in various sequences as appropriate to the individual step.
  • additional steps may be added or removed depending on the particular applications.
  • One of ordinary skill in the art would recognize many variations, modifications, and alternatives.
  • FIG. 4 is a diagram illustrating operational experience with TRISO fuels, notably low-enrichment uranium (LEU) and highly enriched uranium (HEU). Note that for the low-enrichment uranium operational experience with conventional TRISO fuels has been at temperatures well above 1000° C., but with neutron fluence appreciably less than 2 ⁇ 10 22 n/cm 2 . A similar experience has occurred with HEU fuels, that is low neutron fluences at high temperature.
  • the high burn-up TRISO fuel particles described herein and configured for use in Laser Inertial-confinement Fusion-fission Energy (LIFE) engines is subjected to considerably different conditions.
  • LIFE Laser Inertial-confinement Fusion-fission Energy
  • the LIFE engine is designed to operate at much lower temperatures, e.g., below 800° C. Because most of the energy content of the fuel will be burned over the operational lifetime of a LIFE engine (thus the term “high burn-up”), the neutron fluence will be substantially higher for fuels used in a LIFE engine than for conventional TRISO fuels, that is, on the order of 1.2 ⁇ 10 23 n/cm 2 . Thus, in the LIFE engine, the temperature of the fuel pebbles will be lower than in conventional nuclear reactors but the pebbles will experience an increased neutron flux.
  • FIG. 5 is a plot illustrating the wall stress in the high burn-up TRISO fuel particle and fuel pebble illustrated in FIGS. 2A and 2B .
  • the high neutron fluence used in the LIFE engine causes an about 99.9% burn-up of the TRISO fuel, creating stress in the high burn-up TRISO fuel particles illustrated in FIG. 2A and the fuel pebble illustrated in FIG. 2B .
  • the stress in the SiC shell 240 as a function of time (burn-up) is shown by curve 510 in FIG. 5 (triangle symbols).
  • the pressure in the SiC shell is primarily due to the build up of fission gases including krypton and xenon.
  • the peak wall stress for the SiC shell or layer 240 reaches a level of 250 Mpa about 40 years after the high burn-up TRISO fuel particles in the fuel pebble are introduced to the LIFE engine. This is well below the intrinsic strength of silicon carbide (SiC).
  • the stress in the cladding layer of the fuel pebble illustrated in FIG. 2B as curve 520 also reaches a maximum at about the same time the stress in the SiC containment layer of the fuel particles, in this case at a level of 350 Mpa.
  • the pressure build up is primarily due to the build up of fission gases, primarily krypton and xenon, as the fuel in the kernel is consumed.
  • the SiC capsule inside individual TRISO particles, and the pebble cladding provide a redundant fission gas containment, known as defense in depth.
  • the wall stress in the SiC layers is less than the published strength of SiC, which is about 450 Mpa. It should be noted that after the fuel pebbles are removed from the LIFE engine, at approximately year 40, the stresses in the SiC layers drop substantially during interim storage and repository conditions. Thus, by operating the LIFE engine at relatively lower temperatures (e.g., below 800° C.), the wall stress from fission gas accumulation remains significantly below the published strength of silicon carbide. Therefore, the fuel particles and fuel pebble provided by embodiments of the present invention prevent cracking of the SiC layers and thereby release of materials from the fuel kernel into the LIFE engine.
  • FIG. 6 is a plot of the swelling of SiC as a function of irradiation temperature.
  • the swelling behavior of SiC is a function of temperature.
  • the swelling percentage of the SiC increases as shown by the plot in FIG. 6 .
  • the temperature region from about 150° C. to about 1000° C. is the saturable regime characterized by point defect swelling.
  • the temperature region over 1000° C. is the non-saturable region characterized by void swelling.
  • Embodiments of the present invention maintain the fuel particles and the fuel pebbles at temperatures less than about 1000° C., preferably in a range from about 600° C. to about 1000° C.
  • the swelling of the SiC remains below the non-saturable void-swelling regime.
  • FIG. 6 operating the LIFE engine at sub-1000° C. temperatures, swelling of the SiC layers in the fuel particles and/or fuel pebbles can be maintained at less that 1%.
  • FIG. 7 is a plot of wall stress as a function of burn-up percentage measured in FIMA according to an embodiment of the present invention.
  • the fission gas pressure in the fuel particle is proportional to the burn-up percentage.
  • the plots shown in FIG. 7 are based on experimental measurements of fission gas pressure.
  • the wall stress in the SiC shell 240 increases as a function of burn-up percentage, as the amount of fission gases and other fission byproducts increase.
  • the SiC wall strength at which the SiC material will fail by cracking or other means is approximately 450 MPa.
  • the wall stress becomes greater than the wall strength at a burn-up of about 60%. Beyond this burn-up percentage, the SiC shell will develop cracks or otherwise fail, with the leakage of fission gases from the fuel kernel, which would cause undesirable effects.
  • the high burn-up TRISO fuel particles provided according to embodiments of the present invention are characterized by reduced wall stress as a function of burn-up in comparison with conventional designs.
  • the wall stress in SiC capsules (or shells) as described herein e.g., a 60 ⁇ m thick SiC layer 240 and a 120 ⁇ m thick SiC layer
  • the stress in the containment shell reaches the failure point at 100% FIMA, likely placing a lower bound on the thickness of SiC containment capsule.
  • the SiC shell will be damaged to some extent by the neutron flux present in the LIFE engine, resulting in some designs utilizing a thicker SiC containment capsule in order to provide a safety margin.
  • complete burn-up of the fuel kernel can occur before the fission gas pressure will cause the SiC capsule to fail.
  • embodiments of the present invention provide benefits not available using conventional designs.
  • Embodiments of the present invention are utilized in LIFE engines that avoid operating above the eutectic temperature of palladium silicide and similar compounds formed during fission of heavy elements in TRISO fuels. If the engine were operated at a temperature above the eutectic temperature, there is a propensity for some of the inner containment of the TRISO particles to liquefy as particular fission products are created by the neutron fluence. If liquefication occurs, the kernel of the TRISO particle can migrate within the particle to contact the silicon carbide shell. This will likely cause damage to the particle, and possibly damage to the pebble containing the TRISO particles.
  • the propensity of the silicon carbide to swell when irradiated is overcome by designing the LIFE engine to operate at a low enough temperature to avoid the non-saturable void-swelling regime as discussed in relation to FIG. 6 .
  • the high stresses in the silicon carbide shell 240 due to the fission gases produced during fuel burn-up is overcome in some embodiments described herein by manufacturing the high burn-up TRISO fuel particle with a thicker silicon carbide wall than in conventional designs.
  • the inventors have determined that the enhanced TRISO fuels described herein overcome a number of challenges, both scientific and engineering, inherent in conventional fuel particle designs.
  • the reaction of carbon and oxygen released from the kernel of the TRISO particle as a result of fission processes can form carbon monoxide.
  • the production of CO is minimized by the use of a zirconium carbide oxygen getter, thereby capturing liberated oxygen in place of the formation of CO.
  • UOC for UO 2 in the fuel kernel, fuel kernel migration up the temperature gradient is minimized.
  • the reduction in fuel kernel migration results in less interaction between the palladium produced by the fission processes and the silicon carbide containment layer and thereby prolongs the lifetime of the fuel particle, enabling high burn-up. Additionally, since UOC has one half the oxygen content of UO 2 , the amount of free oxygen generated during fission processes is approximately half for UOC fuels, reducing the reactions between oxygen and elements of the fuel particle.
  • Some embodiments provide sacrificial silicon carbide material in the vicinity of the fuel kernel, enabling the formation of the stable compound 1:3:3:5 U:Pd:Si:C.
  • This stable compound has a melting point of approximately 1952° C. and serves to absorb palladium that would otherwise react with the silicon carbide containment shell. Since the LIFE engine is designed to operate at a lower operating temperature in order to avoid the non-saturable void-swelling regime, irradiation swelling of SiC and PyC layers is kept at acceptable levels.
  • the wall stress in the SiC containment shell due to fission gas (e.g., Kr and Xe) pressure is less than the failure stress of the containment vessel.
  • a sacrificial SiC material is positioned close to the fissile kernel in some embodiments to provide a reactant to form the stable compound 1:3:3:5 U:Pd:Si:C.
  • a ZrC diffusion barrier can be utilized to prevent fission products from contacting the SiC containment shell.
  • FIG. 8 is a simplified plot of temperature of portions of the enhanced TRISO particle as a function of time.
  • the inventors have determined that the enhanced TRISO particle will experience dynamic stress due to thermal pulsing at 10 to 20 Hz during operation of the LIFE engine. The thermal pulsing may lead to thermal fatigue. Numerical analysis performed by the inventors indicates that the fuel design described herein will endure the thermal pulsing at the rate of 10 to 20 Hz. For this analysis, the kernel was pulsed 20,000 times and the PyC and SiC layers were pulsed about 7,000 times.
  • FIG. 9 is a table illustrating various design studies for fuel pebbles including high burn-up TRISO particles.
  • six different designs are presented based on variations in the design parameters for the enhanced TRISO particle.
  • various elements of the particle are varied, including the diameter of the fertile or fissile kernel 210 , the thickness of the buffer layer 220 , and the thickness of the SiC containment layer or shell 240 .
  • the overall diameter of the particle will vary.
  • the inventors have computed the fission gas pressure present in the particle at approximately 99.9% burn-up.
  • the computed stress in the SiC containment shell will vary as illustrated by the use of Formula 1 and Formula 2. Since the failure stress of SiC is approximately 450 MPa, all six designs provide stress levels less than or equal to this failure strength. Wall thickness will vary with strength.
  • the design of the various elements of the particle will result in a volume ratio between the fissile kernel and the fuel pebble.
  • the latter designs illustrated in FIG. 9 include a higher ratio of kernel to pebble volume and are preferable.
  • the stress in the containment shell is also increasing with design number, which enables the system designer to trade off the kernel to pebble volume ratio against particle strength, and the like.
  • high burn-up TRISO particles and fuel pebbles including such particles are provided by embodiments of the present invention.

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