TRISO FUEL FOR HIGH BURN-UP NUCLEAR ENGINE

Abstract

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 fuel particle further includes a second pyrolytic carbon layer surrounding the silicon carbide layer.

Description

CROSS-REFERENCE TO RELATED APPLICATIONS

The present application claims benefit under 35 U.S.C. §119(e) of U.S. Provisional Patent Application No. 60/997,780, filed on Oct. 4, 2007, entitled “Hybrid Fusion-Fission Reactor,” and U.S. Provisional Patent Application No. 61/130,200, filed on May 29, 2008, entitled “Hybrid Fusion-Fission Reactor Using Laser Inertial Confinement Fusion,” the disclosures of which are hereby incorporated by reference in their entirety for all purposes.

STATEMENT AS TO RIGHTS TO INVENTIONS MADE UNDER FEDERALLY SPONSORED RESEARCH AND DEVELOPMENT

The United States Government has rights in this invention pursuant to Contract No. DE-AC52-07NA27344 between the United States Department of Energy and Lawrence Livermore National Security, LLC.

BACKGROUND OF THE INVENTION

Projections by the Energy Information Agency and current Intergovernmental Panel on Climate Change (IPCC) scenarios expect worldwide electric power demand to double from its current level of about 2 terawatts electrical power (TWe) to 4 TWe by 2030, and could reach 8-10 TWe by 2100. They also expect that for the next 30 to 50 years, the bulk of the demand of electricity production will be provided by fossil fuels, typically coal and natural gas. Coal supplies 41% of the world's electric energy today, and is expected to supply 45% by 2030. In addition, the most recent report from the IPCC has placed the likelihood that man-made sources of CO₂ emissions into the atmosphere are having a significant effect on the climate of planet earth at 90%. “Business as usual” baseline scenarios show that CO₂ emissions could be almost two and a half times the current level by 2050. More than ever before, new technologies and alternative sources of energy are essential to meet the increasing energy demand in both the developed and the developing worlds, while attempting to stabilize and reduce the concentration of CO₂ in the atmosphere and mitigate the concomitant climate change.

Nuclear energy, a non-carbon emitting energy source, has been a key component of the world's energy production since the 1950's, and currently accounts for about 16% of the world's electricity production, a fraction that could—in principle—be increased. Several factors, however, make its long-term sustainability difficult. These concerns include the risk of proliferation of nuclear materials and technologies resulting from the nuclear fuel cycle; the generation of long-lived radioactive nuclear waste requiring burial in deep geological repositories; the current reliance on the once through, open nuclear fuel cycle; and the availability of low cost, low carbon footprint uranium ore. In the United States alone, nuclear reactors have already generated more than 55,000 metric tons (MT) of spent nuclear fuel (SNF). In the near future, we will have enough spent nuclear fuel to fill the Yucca Mountain geological waste repository to its legislated limit of 70,000 MT. The commercial spent nuclear fuel destined for the repository is approximately 90% of this value, or approximately 63,000 metric tons of heavy-metal uranium (MTHM).

Fusion is an attractive energy option for future power generation, with two main approaches to fusion power plants now being developed. In a first approach, Inertial Confinement Fusion (ICF) uses lasers, heavy ion beams, or pulsed power to rapidly compress capsules containing a mixture of deuterium (D) and tritium (T). As the capsule radius decreases and the DT gas density and temperature increase, DT fusion reactions are initiated in a small spot in the center of the compressed capsule. These DT fusion reactions generate both alpha particles and 14.1 MeV neutrons. A fusion burn front propagates from the spot, generating significant energy gain. A second approach, Magnetic Fusion Energy (MFE) uses powerful magnetic fields to confine a DT plasma and to generate the conditions required to sustain a burning plasma and generate energy gain.

Important technology for ICF is being developed primarily at the National Ignition Facility (NIF) at Lawrence Livermore National Laboratory (LLNL), assignee of this invention, in Livermore, Calif. There, a laser-based inertial confinement fusion project designed to achieve thermonuclear fusion ignition and burn utilizes laser energies of 1 to 1.3 MJ. Fusion yields of the order of 10 to 20 MJ are expected. Fusion yields in excess of 200 MJ are expected to be required in central hot spot fusion geometry if fusion technology, by itself, were to be used for cost effective power generation. Thus, significant technical challenges remain to achieve an economy powered by pure inertial confinement fusion energy.

SUMMARY OF THE INVENTION

According to the present invention, techniques related to nuclear engine fuel are provided. More particularly, an embodiment of the present invention provides an enhanced fuel particle suitable for use in a laser inertial confinement fusion-fission power plant. Merely by way of example, 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. The methods and systems described herein are also applicable to other nuclear power plant designs.

According to an embodiment of the present invention, a fuel particle for use in a fusion-fission nuclear engine is provided. The fuel particle 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. In this case, 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. As the strength increases above this level, the required wall thickness will decrease. As the strength decreases below this level, the required wall thickness will increase. The fuel particle further includes a second pyrolytic carbon layer surrounding the silicon carbide layer.

According to another embodiment of the present invention, a method of fabricating a fuel particle for a fusion-fission nuclear engine is provided. The method 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 μm. The method further includes forming a second pyrolytic carbon layer surrounding the silicon carbide layer.

According to an alternative embodiment of the present invention, a fuel pebble for use in a fusion-fission nuclear engine is provided. The fuel pebble 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 μm. The fuel pebble also includes a cladding layer enclosing the plurality of fuel particles and the matrix material.

Numerous benefits are achieved by way of the present invention over conventional techniques. For example, 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. Additionally, 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. These and other benefits will be described in more detail throughout the present specification and more particularly below.

These and other objects and features of the present invention and the manner of obtaining them will become apparent to those skilled in the art, and the invention itself will be best understood by reference to the following detailed description read in conjunction with the accompanying drawings.

BRIEF DESCRIPTION OF THE DRAWINGS

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; and

FIG. 9 is a table illustrating various design studies for fuel pebbles including high burn-up TRISO particles.

DETAILED DESCRIPTION OF SPECIFIC EMBODIMENTS

According to the present invention, techniques related to nuclear engine fuel are provided. More particularly, an embodiment of the present invention provides an enhanced fuel particle suitable for use in 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. Merely by way of example, 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. The methods and systems described herein are also applicable to other nuclear power plant designs. Additional discussion related to nuclear fusion-fission engines is provided in U.S. patent application Ser. No. ______, entitled “Control of a Laser Inertial Confinement Fusion-Fission Power Plant” (Attorney Docket No. 027512-000400) and U.S. patent application Ser. No. ______ (Attorney Docket No. 027512-000700US), entitled “Solid Hollow Core Fuel for Fusion-Fission Engine,” the disclosures of which are hereby incorporated by reference in their entirety for all purposes.

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 (UO₂) 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. 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. As illustrated in FIG. 2A, 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 (UO₂), weapons-grade plutonium, spent nuclear fuel, depleted uranium, natural uranium, highly enriched uranium, and the like can be used in the fuel kernel. 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.

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. In some embodiments, 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. Thus, for example, 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 (ρ) 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. In an embodiment, the thickness of the SiC shell 240 (sometimes referred to as a containment shell or vessel) ranges from about 60 μm to about 200 μm. In a particular embodiment, the thickness of the SiC shell 240 is 120 μm. In another embodiment, the thickness is about 70 μm, about 80 μm, about 100 μm, about 120 μm, or thicker than 120 μm. 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. Typically, 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. In embodiments of the present invention, 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.

In contrast with conventional fuel particles, 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. As an example, the burn-up may progress to 99.9% FIMA utilizing embodiments of the present invention. Additionally, the enhanced or high burn-up TRISO particles described herein provide a high mass fraction of fissile material. Thus, 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.

In contrast with conventional TRISO particles, in order to achieve high burn-up, 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. As an example, in an embodiment, 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. Referring to FIG. 2B, the fuel pebble 260 includes a number of TRISO particles 200 that are grouped together into the fuel pebble. As an example, 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. Accordingly, 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.

During typical use, 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.

According to an embodiment of the present invention, 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. In addition each fuel pebble contains enough of the TRISO fuel particles to emit enough radiation to prevent manual removal without personal harm. Thus, 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. As illustrated in FIG. 3, the fabrication of an enhanced TRISO particle begins with the process of making the fissile kernel. In the embodiment illustrated in FIG. 3, uranium ore, either from natural uranium, or depleted uranium (DU) is provided 310. Although these two particular types of fissile material are illustrated in this particular embodiment, the enhanced TRISO particles are not limited to these particular fuels. Other fuels including weapons-grade plutonium (WG-Pu), highly enriched uranium (HEU), light water reactor (LWR) spent nuclear fuel (SNF), or the like can be utilized to form enhanced TRISO particles. The primary difference in comparison to the conventional TRISO fabrication process is the unit operation where the pebble is coated with the protective cladding material. Other process steps are very similar to the conventional TRISO process. It should be noted that some fuels provide benefits in comparison with other fuels since, for example, fuel particles including DU may pose lifetime problems not present in WG-Pu, since WG-Pu is mostly fissile material and thus the fuel particle including WG-Pu is not damaged by neutrons during breeding up of plutonium during the fuel cycle.

The uranium ore is pelletized (312) and dissolved in a broth, typically utilizing nitric acid (HNO₃), Urea, or the like. The uranium broth is flowed through a drop column (316), washed in water (318) and alcohol (320). After these processes, 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. As described in relation to layer 220 in FIG. 1, the porous buffer layer is preferably a nano-porous foam material. The foam materials may include carbon aerogels, silica aerogels, and uranium foams. In a particular embodiment, 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.

In addition to providing an expansion volume for fission gases, the buffer layer can include a sacrificial silicon carbide material. For example, the sacrificial silicon carbide can react with palladium produced as a fission byproduct to form Pd₅Si. Since the LIFE engine typically operates at a temperature of less than 800° C., the Pd₅Si 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. As illustrated in FIG. 3, trimethyl silicon chloride (SiCl(CH₃)₃) is used in depositing the silicon carbide containment layer. The thickness of the containment layer, as discussed above, 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. It should be appreciated that in some embodiments, the interfaces between various layers of the structure are not exposed to an ambient environment during the CVD process, improving the fuel performance. Thus, in some embodiments, a single CVD reactor is utilized with multiple gas sources. In other embodiments, multiple CVD reactors joined by a load-lock vacuum interface can be utilized to achieve results similar to those achieved with a single reactor. Thus, 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.

Additionally, 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.

Once the particles with the outer PyC layer have been fabricated, they are tabled (338), screened (340), and put through elutriation columns (342) to purify and separate the particles on the basis of particle density. After elutriation, 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.

It should be appreciated that the specific steps illustrated in FIG. 3 provide 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. For example, alternative embodiments of the present invention may perform the steps outlined above in a different order. Moreover, 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. Furthermore, 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 2×10²² n/cm². 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. (high fluence, but low temperature) 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 1.2×10²³ n/cm². 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. As previously discussed in relation to FIG. 4, 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. Referring to FIG. 5, 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).

Similarly to the fuel particles, 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. As discussed previously, 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. Together, the SiC capsule inside individual TRISO particles, and the pebble cladding provide a redundant fission gas containment, known as defense in depth.

For both the fuel particles and the fuel pebble, 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. As shown by the plot in FIG. 6, the swelling behavior of SiC is a function of temperature. As the irradiation temperature increases from 0° C. to about 1100° C., SiC the swelling percentage decreases from about 10% to less than 1% depending on the irradiation damage, quantified as displacements per atom (dpa). At temperatures greater than about 1100° C., 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. Thus, by maintaining the fuel for the LIFE engine at relatively low temperatures (e.g., on the order of 800° C.), the swelling of the SiC remains below the non-saturable void-swelling regime. As illustrated by 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. To a first approximation, 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. Similarly, 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. For a SiC shell in a conventional TRISO particle with a SiC layer thickness of 30 μm, 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.

Since the LIFE engine is designed to operate at high burn-up levels, the inventors have appreciated that conventional TRISO particles utilizing thin layers of SiC are unsuitable for long lived operation at the high fission gas pressures associated with LIFE engines. Based on the determination that failure of the SiC layer as a result of fission gas pressure makes conventional particles unsuitable, the inventors have developed new designs that provide long life operation at high burn-up levels.

In contrast with the conventional TRISO particle, 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. As shown in FIG. 7, the wall stress in SiC capsules (or shells) as described herein (e.g., a 60 μm thick SiC layer 240 and a 120 μm thick SiC layer) does not exceed the wall strength of SiC throughout the burn-up process. For the fuel particle with a 60 μm SiC containment capsule, 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. In actual use, 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. Thus, complete burn-up of the fuel kernel can occur before the fission gas pressure will cause the SiC capsule to fail. As a result, 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.

Thus, 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. As discussed in relation to FIG. 2A, 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. For example, in some embodiments, the reaction of carbon and oxygen released from the kernel of the TRISO particle as a result of fission processes, can form carbon monoxide. Accordingly, in these embodiments, 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. Furthermore, by substituting UOC for UO₂ 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 UO₂, 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.

Since the wall thickness of the SiC containment layer is thicker than in conventional designs, 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. In order to reduce the impact of fission products attacking the SiC containment shell, 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. Additionally, in some embodiments 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. In FIG. 9, six different designs are presented based on variations in the design parameters for the enhanced TRISO particle. As illustrated in the table, 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. Depending on the values selected for these elements, the overall diameter of the particle will vary. Given these physical dimensions, the inventors have computed the fission gas pressure present in the particle at approximately 99.9% burn-up. Depending on the particular formula utilized, 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. At the same time, 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. Thus, by proper particle design, high burn-up TRISO particles and fuel pebbles including such particles are provided by embodiments of the present invention.

It is also understood that the examples and embodiments described herein are for illustrative purposes only and that various modifications or changes in light thereof will be suggested to persons skilled in the art and are to be included within the spirit and purview of this application and scope of the appended claims.

Claims

1. A fuel particle for use in a fusion-fission nuclear engine, the fuel particle comprising:

a fuel kernel;

a buffer layer surrounding the fuel kernel;

a pyrolytic carbon layer surrounding the buffer layer;

a silicon carbide layer surrounding the buffer layer, wherein the silicon carbide is characterized by a stress less than its intrinsic strength at high burn-up; and

a second pyrolytic carbon layer surrounding the silicon carbide layer.

2. The fuel particle of claim 1 further comprising a third pyrolytic carbon layer surrounding the second pyrolytic carbon layer.

3. The fuel particle of claim 1 wherein the fuel kernel comprises uranium dioxide.

4. The fuel particle of claim 1 wherein the fuel kernel comprises at least one of low enriched uranium or high enriched uranium.

5. The fuel particle of claim 1 wherein the buffer layer comprises a porous carbon layer.

6. The fuel particle of claim 1 wherein the silicon carbide layer is characterized by a thickness greater than 30 μm.

7. The fuel particle of claim 6 wherein the thickness is greater than 60 μm.

8. The fuel particle of claim 7 wherein the thickness is greater than 90 μm.

9. The fuel particle of claim 1 wherein the silicon carbide layer is characterized by a stress of less than 450 Mpa at 50% burn-up.

10. A method of fabricating a fuel particle for a fusion-fission nuclear engine, the method comprising:

forming a fuel kernel;

forming a buffer layer surrounding the fuel kernel;

forming a first pyrolytic carbon layer surrounding the buffer layer;

forming a silicon carbide layer surrounding the first pyrolytic carbon layer, wherein the silicon carbide layer is characterized by a thickness greater than 60 μm; and

forming a second pyrolytic carbon layer surrounding the silicon carbide layer.

11. The method of claim 10 wherein the fuel kernel comprises uranium oxy-carbide.

12. The method of claim 10 wherein the buffer layer comprises at least one of a SiC material or a ZrC material.

13. The method of claim 10 wherein forming the silicon carbide layer comprises using a chemical vapor deposition process.

14. The method of claim 10 wherein forming the first pyrolytic carbon layer and forming the second pyrolytic carbon layer comprises using a chemical vapor deposition process.

15. A fuel pebble for use in a fusion-fission nuclear engine, the fuel pebble comprising:

a plurality of fuel particles disposed in a matrix material, each of the fuel particles comprising: a fuel kernel; a buffer layer surrounding the fuel kernel; a pyrolytic carbon layer surrounding the buffer layer; a silicon carbide layer surrounding the buffer layer, wherein the silicon carbide layer is characterized by a thickness greater than 60 μm; and a second pyrolytic carbon layer surrounding the silicon carbide layer; and

a cladding layer enclosing the plurality of fuel particles and the matrix material.

16. The fuel pebble of claim 15 wherein the inert material comprises graphite.

17. The fuel pebble of claim 15 wherein the cladding layer comprises a refractory metal.

18. The fuel pebble of claim 15 wherein the cladding layer comprises a refractory metal carbide material.

19. The fuel pebble of claim 15 wherein the silicon carbide layer is characterized by a stress of less than 450 Mpa at 50% burn-up.

20. The fuel pebble of claim 19 wherein the silicon carbide layer is characterized by a stress of less than 450 Mpa at 70% burn-up.

21. The fuel pebble of claim 20 wherein the silicon carbide layer is characterized by a stress of less than 450 Mpa at 90% burn-up.

22. The fuel pebble of claim 15 wherein the matrix material comprises at least one of graphite or zirconium carbide.