This disclosure relates generally to metal hydride structures and to methods of forming the metal hydride structures. More specifically, this disclosure relates to neutron moderators including the metal hydride structures, to methods of forming the metal hydride structures, and to methods of regenerating the metal hydride structures.
Neutron moderators are a class of compounds that scatter neutrons, thus slowing their velocity (e.g., for neutrons emitted from a fissile compound within a nuclear reactor). Neutron moderators may optimize fission chain reactions because slower neutrons can increase nuclear reaction efficiency and output. Metal hydrides, which may be used as neutron moderators, are important for accessing high temperature nuclear reactor implementation, owing to their high thermal stability and high hydrogen density when compared to lower temperature nuclear reactor moderators such as water. However, conventional high temperature nuclear reactors that use metal hydrides as moderators may be lifetime limited by both fuel source and moderator efficacy since the effectiveness of the moderator may degrade over time due to hydrogen loss at higher temperatures. The potential for irreversible hydrogen depletion may occur over time under normal operating conditions, and/or if the heat transfer properties of the metal hydride moderator are altered because of swelling, blister formation, delamination, or in the case of an off-normal temperature excursion.
Nuclear reaction moderators that have conventionally been used include metal hydrides, water, heavy water, beryllium oxide, and graphite. A common quality of some effective neutron moderators is the presence of hydrogen atoms in the moderator. One consequence of collisions between neutrons and the neutron moderator containing hydrogen atoms may be that the hydrogen atoms are expelled from the neutron moderator, leading to eventual hydrogen depletion and loss of effectiveness of the substance as a neutron moderator, especially at higher temperatures.
In accordance with embodiments of the disclosure, a neutron moderator includes a porous metal hydride comprising channels within the porous metal hydride.
Further, in accordance with embodiments of the disclosure, a nuclear reactor includes one or more neutron moderator regions in a core of a reactor, one or more fuel regions, one or more heat transfer regions, control drums adjacent to the core, and a control rod adjacent to the core. The one or more of the one or more neutron moderator regions include a neutron moderator. The neutron moderator has a porous metal hydride article with channels. The one or more fuel regions are adjacent to the one or more neutron moderator regions. The one or more heat transfer regions are adjacent to the one or more fuel regions.
Further, in accordance with other embodiments of the disclosure, a method of forming a metal hydride includes forming a porous network scaffold, infiltrating a metal hydride material into the porous network scaffold, and removing the porous network scaffold to form a porous metal hydride article.
Additionally, in accordance with other embodiments of the disclosure, a method of regenerating a neutron moderator includes providing an at least partially depleted metal hydride article, and introducing a hydrogen-containing gas into the at least partially depleted metal hydride article. The at least partially depleted metal hydride article has channels.
The following description provides specific details, such as material compositions, shapes, and sizes, in order to provide a thorough description of embodiments of the disclosure. However, a person of ordinary skill in the art would understand that the embodiments of the disclosure may be practiced without employing these specific details. Indeed, the embodiments of the disclosure may be practiced in conjunction with conventional techniques employed in the industry.
Drawings presented herein are for illustrative purposes only, and are not meant to be actual views of any particular material, component, structure, or system. Variations from the shapes depicted in the drawings as a result, for example, of manufacturing techniques and/or tolerances, are to be expected. Thus, embodiments described herein are not to be construed as being limited to the particular shapes. The drawings are not necessarily to scale.
As used herein, the singular forms “a,” “an,” and “the” are intended to include the plural forms as well, unless the context clearly indicates otherwise. As used herein, “and/or” includes any and all combinations of one or more of the associated listed items.
As used herein, the term “substantially” in reference to a given parameter, property, or condition means and includes to a degree that one of ordinary skill in the art would understand that the given parameter, property, or condition is met with a degree of variance, such as within acceptable tolerances. By way of example, depending on the particular parameter, property, or condition that is substantially met, the parameter, property, or condition may be at least 90.0 percent met, at least 95.0 percent met, at least 99.0 percent met, at least 99.9 percent met, or even 100.0 percent met.
As used herein, “about” or “approximately” in reference to a numerical value for a particular parameter is inclusive of the numerical value and a degree of variance from the numerical value that one of ordinary skill in the art would understand is within acceptable tolerances for the particular parameter. For example, “about” or “approximately” in reference to a numerical value may include additional numerical values within a range of from 80.0 percent to 120.0 percent of the numerical value, such as within a range of from 90.0 percent to 110.0 percent of the numerical value, within a range of from 95.0 percent to 105.0 percent of the numerical value, within a range of from 97.5 percent to 102.5 percent of the numerical value, within a range of from 99.0 percent to 101.0 percent of the numerical value, within a range of from 99.5 percent to 100.5 percent of the numerical value, or within a range of from 99.9 percent to 100.1 percent of the numerical value.
As used herein, porosity of a given material or article is described as a percentage of a volume of voids (e.g., empty pore space) in the material or article divided by a total volume of the material or article (e.g., the combined volume of both the material or article and the voids). As such, porosity may be described as a volumetric percentage (“vol. %”).
As used herein, the term “moderator” (e.g., “neutron moderator”) means a material that is configured to be placed within a nuclear reactor core and formulated to decrease the velocity of high-energy neutrons within the nuclear reactor.
As used herein, the term “MHx” refers to a metal hydride, where “x” may refer to the number of hydrogen atoms per unit lattice. The MHx may be a stoichiometric compound of the metal atoms and hydrogen atoms, or a non-stoichiometric compound of the metal atoms and hydrogen atoms. The metal hydride may be configured as an MHx material, an MHx intermediate structure, and/or an MHx article.
Conventionally, MHx neutron moderators may be formed by exposing a metal (e.g., yttrium) to a gas (e.g., hydrogen) at high temperature. Over time (e.g., several days), the metal may uniformly hydride by reaching a hydrogen concentration sufficient to be utilized for a neutron moderator. However, hydriding the metal at too fast of a rate may result in cracking and mechanical failure of the metal hydride. Use of the neutron moderator at a high temperature may be limited in effectiveness by the eventual loss of hydrogen from the MHx neutron moderator, which may be exacerbated by the high operating temperatures of a nuclear microreactor in which the MHx neutron moderator is used.
Attempts to re-hydride conventional MHx neutron moderators by introducing hydrogen into the MHx neutron moderator in situ (e.g., within the nuclear reactor) may be ineffective, as hydride processes typically cause expansion of the MHx neutron moderator, which can cause cracking and eventual disintegration of the MHx neutron moderator.
Disclosed is a method of regenerating a depleted MHx article that enables control over hydride concentration in the MHx article. The MHx article may, for example, be configured as a MHx moderator (e.g., a MHx neutron moderator) in a nuclear reactor, such as in a microreactor. Microreactors are compact nuclear reactors that are capable of generating a power output from approximately 1 megawatt (“MW”) to approximately 20 MW and operate at a temperature from about 400° C. to about 1,000° C. Using the MHx article according to embodiments of the disclosure may increase the effective lifetime over which reliable operation of the nuclear reactor may occur. More specifically, the MHx article may be used as a neutron moderator that is formulated and configured to regenerate its hydrogen density. The MHx article may be porous such that a flow of gas therethrough regenerates the MHx article following hydrogen depletion.
The operating temperatures of nuclear reactors above certain temperatures (e.g., greater than or equal to about 400° C., such as greater than or equal to about 600° C. or greater than or equal to about 800° C.) may be limited by neutron moderator selection and long-term efficacy. Metal hydrides may provide efficient neutron moderation in nuclear reactors, but may be limited in long-term efficacy by hydride loss, which decreases a moderating ratio of the MHx article. Neutron moderator performance is quantified by a moderating ratio, defined as the macroscopic slowing-down power (the product of the average logarithmic energy loss per collision and the macroscopic neutron scattering cross section) to the macroscopic cross section for neutron absorption.
An MHx neutron moderator (e.g., the MHx article) may be porous (e.g., may exhibit pores), such as including channels (e.g., internal channels) throughout the bulk of the MHx article. Porous regions of the MHx article may enable a gas to flow through the MHx article, which enables regeneration of the MHx article (e.g., an increase of hydrogen content in the MHx article). The channels extend through the MHx article and may be substantially uniformly distributed through the MHx material, providing porosity to the MHx article. The channels may be substantially linear, as shown in
Referring to
The porous network scaffold 110 may be formed by impregnating a precursor foam (e.g., a polyurethane open-cell foam) with resin (e.g., a thermal setting resin, such as a carbonaceous resin or a carbonaceous thermal setting resin). The resin-impregnated precursor foam may be heated to cure (e.g., thermally set) the resin, while maintaining the precursor foam at temperatures below the decomposition temperature of the precursor foam. The resin-impregnated precursor foam may be subjected to one or more temperature gradients to cure the resin. By way of non-limiting example, the resin-impregnated precursor foam may be subjected to a first temperature gradient comprising heating the resin-impregnated precursor foam at rates from approximately 0.05° C. per minute to approximately 0.7° C. per minute until reaching approximately 50° C. to approximately 90° C. In one embodiment, the resin-impregnated precursor foam is subjected to heating at a rate of approximately 0.16° C. per minute until reaching approximately 70° C.
Following the first temperature gradient, the resin-impregnated precursor foam may be maintained at holding temperatures at or below an exothermic temperature of the resin in order to control (e.g., limit) the amount of heat released into the precursor foam. As a non-limiting example, holding temperatures may range from approximately 50° C. to approximately 120° C. for a duration of from approximately 1 hour to approximately 15 hours. In one embodiment, the resin-impregnated precursor foam is held at a temperature of approximately 70° C. for approximately 3 hours.
Following subjecting the resin-impregnated precursor foam to a prolonged holding temperature, the resin-impregnated precursor foam may be subjected to a second or other subsequent temperature gradient.
By way of non-limiting example, the resin-impregnated precursor foam may be subjected to a second temperature gradient comprising heating the resin-impregnated precursor foam at rates from approximately 0.03° C. per minute to approximately 0.13° C. per minute until reaching approximately 150° C. to approximately 190° C. In one embodiment, the resin-impregnated precursor foam is subjected to heating at a rate of approximately 0.09° C. per minute until reaching approximately 170° C. The second temperature gradient may enable a substantially complete thermal setting of the resin, while allowing exothermic heat of the thermal setting of the resin to dissipate without substantially affecting the cell shape of the resin-impregnated precursor foam. Following the second temperature gradient ramp, the resin-impregnated precursor foam may be allowed to cool to room temperature (e.g., approximately 20° C. to approximately 22° C.).
Curing the resin within the resin-impregnated precursor foam may comprise forming crosslinks in the resin impregnated within the precursor foam. Curing the resin impregnated within the precursor foam article may be performed in an inert atmosphere (e.g., nitrogen or argon), in a non-oxidizing atmosphere (e.g., hydrogen), or in a vacuum.
Following curing the resin in the precursor foam, the precursor foam may be heated to pyrolyzing temperatures of the precursor foam for a sufficient duration of time to convert the carbonaceous resin impregnated within the precursor foam to, for example, vitreous carbon (e.g., by vitrifying the resin), resulting in the porous network scaffold 110. As a non-limiting example, pyrolyzing temperatures may range from approximately 400° C. to approximately 2200° C. As a further non-limiting example, the pyrolyzing duration may range from approximately 1 hour to approximately 60 hours. Pyrolyzing the precursor foam may be performed in an inert atmosphere (e.g., nitrogen or argon), in a non-oxidizing atmosphere (e.g., hydrogen), or in a vacuum.
The porosity of the later-formed porous MHx article 100 (
Following formation of the porous network scaffold 110, a protective interlayer (not depicted) may optionally be applied to the scaffold members 112 of the porous network scaffold 110 (e.g., foam ligaments of an RVC foam structure) to protect the scaffold members 112 from subsequent acts carried out in forming an MHx intermediate structure 130 (e.g., melt infiltration of MHx material 140 into the porous network scaffold 110 as depicted in
Referring to
The metal of the MHx material 140 of the MHx intermediate structure 130 and of the MHx article 100 may be an alkali metal, a transition metal, an actinide, or an alloy (including, as examples, a conventional alloy or a high-entropy alloy) thereof. The metal may include, but is not limited to, one or more of yttrium, cerium, zirconium, chromium, titanium, lithium, thorium, or uranium. By way of example, the MHx material 140 may comprise one or more of yttrium hydride, cerium hydride, yttrium zirconium hydride, yttrium chromium hydride, titanium hydride, zirconium hydride, lithium hydride, thorium hydride, uranium hydride, thorium zirconium hydride, or thorium titanium hydride. In some embodiments, the MHx material 140 is yttrium hydride.
Following formation of the MHx intermediate structure 130, the porous network scaffold 110 may be removed. Referring to
The formation of the MHx article 100 may, for example, be performed under vacuum conditions, such as under ultrahigh vacuum conditions. By way of example only, the MHx intermediate structure 130 may be formed (e.g., by melt infiltration of the MHx material into the porous network scaffold 110) at a pressure from approximately 1×10−8 mbar to approximately atmospheric pressure (e.g., in an inert gas such as argon). If the MHx intermediate structure 130 is subjected to deposition (e.g., chemical vapor deposition), such processing acts may be carried out at a pressure from approximately 0.1 mbar to approximately 100 mbar. Removal (e.g., oxidation) of the porous network scaffold 110 may be carried out at atmospheric pressure followed by substantially outgassing residual matter of the porous network scaffold 110 at ultrahigh vacuum conditions (e.g., at or below approximately 1×10−8 mbar). The formation of the MHx article 100 may alternatively be formed under atmospheric conditions. The formation of the MHx article 100 may be performed under high pressure conditions. By way of further example, the formation of the MHx article 100 may be performed at a pressure from about 1×103 mbar to about 1×109 mbar. The formation of the MHx article 100 may also be performed under a gas atmosphere (e.g., hydrogen).
Alternatively, the MHx article 100 may be formed from an MHx precursor material that is infiltrated around the porous network scaffold 110 to form a porous MHx precursor (not shown). The MHx article 100 may be formed following the formation of such a porous MHx precursor. More specifically, the porous network scaffold 110 may be infiltrated with a non-hydride precursor material of the MHx, to form a porous non-hydride metal (e.g., the porous MHx precursor), which may subsequently be converted to the MHx article 100. For instance, the MHx article 100 may be formed by hydriding the porous MHx precursor (e.g., by exposing the porous MHx precursor to hydrogen over time at high temperature). Hydriding the porous MHx precursor may be carried out by introducing hydrogen gas into the porous MHx precursor at a pressure from approximately 1×10−10 mbar to approximately 1000 mbar. The hydrogen gas pressure may be provided at a substantially constant pressure, or may be gradually increased (e.g., from approximately 1×10−10 mbar to approximately 1000 mbar).
Referring to
Methods for forming an MHx article 100, 200, as disclosed herein, may enable formation of the pores 132, 232 of the MHx article 100, 200 to have sizes and shapes that may be configured for use in an MHx moderator 300 (e.g., an MHx neutron moderator) of a nuclear reactor.
Referring to
Although the foregoing descriptions are provided with reference to formation of an MHx article (e.g., MHx articles 100, 200, 310) by melt infiltration of the MHx material (e.g., MHx material 140) into a porous network scaffold (e.g., porous network scaffold 110), other embodiments of the disclosure include MHx articles that are formed using a variety of techniques and processes to result in porous MHx articles comprising a porosity of between about 0.01 vol. % and about 20 vol. %. As non-limiting examples, the MHx article (e.g., MHx articles 100, 200, 310) may be formed by additive manufacturing techniques. For example, partial sintering may be carried out to form a porous MHx article having a desired porosity and other physical characteristics appropriate for use as an MHx moderator. Other techniques of forming an MHx article configured to allow a gas (e.g., hydrogen) to flow therethrough are within the scope of the disclosure.
Processes as described herein may enable selection and variation in the extent of porosity and flow characteristics of the MHx articles (e.g., MHx articles 100, 200, 310) in combination with the moderator neutron efficacy. The moderator regions 410 may be present in the core 400 and configured to allow the gas (e.g., hydrogen gas) to flow through the moderator regions 410. By adjusting the thickness and configuration of the porous network scaffold 110, dimensions (e.g., a width, a length) of the pores 132, 232 may be tailored. The porosity of the moderator regions 410 of the core 400 may allow for in situ regeneration of the MHx article 100, 200, 310, which may improve the effectiveness and lifetime of the MHx articles 100, 200, 310 of the reactor. By regenerating the MHx article 100, 200, 310 according to embodiments of the disclosure, lifetime limitations observed with conventional MHx moderators may be overcome. In contrast, conventional MHx moderators are not easily and reliably regenerated following hydride loss. Instead, core replacement is necessary when the conventional MHx moderators are depleted.
Referring to
In operation, the moderator articles (e.g., MHx article 100, MHx article 200, MHx article 310) of the moderator regions 410 may be used at a high temperature (e.g., at or above about 400° C.) within the reactor core 500 or during an unplanned temperature excursion. During such use, the MHx material 140 may experience a loss of hydrogen over time, becoming depleted. Gas flow (e.g., hydrogen gas) through the MHx articles 100, 200, 310 may enable regeneration of the hydrogen within the MHx articles 100, 200, 310. By way of example, about 20% or more of the depleted hydrogen may be regenerated, such as about 40% or more of the depleted hydrogen, about 60% or more of the depleted hydrogen, about 80% or more of the depleted hydrogen, or about 100% of the depleted hydrogen may be regenerated. The regeneration of the hydrogen may be performed at a temperature at or above about 400° C. The gas (e.g., hydrogen) may be flowed through the MHx articles (e.g., MHx article 100, MHx article 200, MHx article 310) at a flow rate sufficient to regenerate the hydrogen, which depends on the extent of hydrogen depletion and the dimensions of the pores (e.g., pores 132, 232). The flow of gas through the moderator regions 410 may also function as a heat transfer medium. Conditions (e.g., temperature, pressure, hydrogen flow rate) for regenerating the MHx articles (e.g., MHx article 100, MHx article 200, MHx article 310) may be selected to minimize and/or stop cracking or mechanical failure in the MHx articles (e.g., MHx article 100, MHx article 200, MHx article 310). By way of non-limiting example, the MHx article (e.g., MHx article 100, MHx article 200, MHx article 310) may be regenerated (e.g., hydrided) by either static hydrogen gas or flowing hydrogen gas. For any given MHx article (e.g., MHx article 100, MHx article 200, MHx article 310), there may be a hydrogen gas equilibrium pressure for rejuvenation and/or maintenance of hydrogen content in the MHx article. Introducing hydrogen gas at least at the equilibrium pressure into the MHx article may result in hydridation of the MHx article, which may at least offset depletion of hydrogen from the MHx article that occurs during operation of the nuclear reactor. The equilibrium pressure of introduced hydrogen may be less than or equal to approximately 1000 torr. Alternatively, the MHx article may be regenerated by introducing hydrogen gas into the MHx article at a pressure from approximately 1×10−10 mbar to approximately 1000 mbar. The hydrogen gas pressure may be provided at a substantially constant pressure, or may be gradually increased (e.g., from approximately 1×10−10 mbar to approximately 1000 mbar). Additional equilibrium processing conditions (e.g., temperature, gas flow rate) may likewise contribute to rejuvenation of the MHx article.
Regenerating the hydrogen in the moderator regions 410 may be achieved by flowing the gas through the MHx material 140, MHx material 240 of the moderator regions 410. Regeneration of the MHx material may be limited by diffusion and thermodynamic (e.g., temperature, pressure) processes. The hydrogen may be regenerated in situ during use and operation of the nuclear reactor core 500. Alternatively, the moderator regions 410 may be regenerated when the nuclear reactor is offline (e.g., inactive). Interaction of the gas (e.g., hydrogen) with the hydrogen-depleted MHx material of the moderator regions 410 may regenerate the moderator efficacy since the MHx material of the moderator regions 410 is structurally porous. Therefore, the MHx article (e.g., MHx article 100, MHx article 200, MHx article 310) in the moderator region 410 may be formulated and configured to continuously replenish their hydrogen content. The reactor core 500, thus configured to operate at a high temperature (e.g., above about 400° C.), that includes the MHx article (e.g., MHx article 100, MHx article 200, MHx article 310) according to embodiments of the disclosure may enable the lifetime of the reactor core 500 to be fuel limited rather than moderator lifetime limited.
While certain illustrative embodiments have been described in connection with the figures, those of ordinary skill in the art will recognize and appreciate that embodiments encompassed by the disclosure are not limited to those embodiments explicitly shown and described herein. Rather, many additions, deletions, and modifications to the embodiments described herein may be made without departing from the scope of embodiments encompassed by the disclosure, such as those hereinafter claimed, including legal equivalents. In addition, features from one disclosed embodiment may be combined with features of another disclosed embodiment while still being encompassed within the scope of the disclosure.
This application claims the benefit under 35 U.S.C. § 119(e) of U.S. Provisional Patent Application Ser. No. 63/268,298, filed Feb. 21, 2022, the disclosure of which is hereby incorporated herein in its entirety by this reference.
This invention was made with government support under Contract Number DE-AC07-05-ID14517 awarded by the United States Department of Energy. The government has certain rights in the invention.
Number | Date | Country | |
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63268298 | Feb 2022 | US |