The present invention relates generally to fluidized bed processing and, more particularly, to embodiments of a fluidized bed fluorination system including a conical gas distributor that improves solids-gas mixing and eliminates dead zones within a reaction vessel, as well to fluorination methods carried-out utilizing such a fluidized bed fluorination system.
Fuel for nuclear power plants is commonly produced by uranium enrichment processes requiring uranium hexafluoride (UF6) as a feed/input. UF6 is, in turn, commonly produced by the fluorination of uranium hexafluoride (UF4). During one known fluorination process, solid UF4 is introduced into a fluidized bed reaction vessel (commonly referred to as a “fluorinator”) and reacted with fluorine gas at elevated temperatures to yield the desired product, gaseous UF6. The fluidized bed commonly contains an inert diluent material, such as calcium fluoride (CaF2; also commonly referred to as “fluorspar”), magnesium fluoride, or alumina, to improve the quality of fluidization and to moderate the reaction kinetics (e.g., to dissipate the considerable amounts of heat generated during the fluorination process). A gas distributor, which has traditionally assumed the form of a flat perforated or sintered plate (or grate) positioned near the bottom of the reaction vessel, is utilized to introduce the fluorine gas along with other fluidizing gases into the reaction vessel. The flat plate gas distributor provides high velocity gas flow into the reaction vessel to enhance fluidization of the bed material and to discourage back flow of the gaseous and solid materials through the distributor. The gaseous UF6 produced by the fluorination reaction is withdrawn from the reaction vessel through an upper manifold and then subjected to further downstream processing (e.g., filtering, purification, scrubbing, desubliming, condensation, and distillation).
During the above-described fluorination process, solids may aggregate within the reaction vessel and form relatively large, rock-like particles due to the highly reactive nature of fluorine, the heat released by the fluorination reaction, and impurities present within the bed material and UF4. Such aggregate masses tend to accumulate on the flat plate gas distributor and, specifically, within dead zones along the upper face of the gas distributor that remain relatively undisturbed by high velocity gas flow (note that the gas distributor dead zones generally cannot be eliminated by simply increasing the density of the gas flow openings through the gas distributor without negatively impacting the overall quality of fluidization). The solid aggregates may gradually grow so large as to cause critical operational issues within the reaction vessel, such as the obstruction of gas flow openings in the flat plate gas distributor and the development of hot spots within the reaction vessel. While some reaction vessels employ vertically-extending, sidewall-mounted drain pipes to remove solid aggregates from an area above the flat plate gas distributor, such drain pipes are typically limited in the amount of solid aggregates they are able to remove. Thus, even when the reaction vessel is equipped with such a sidewall-mounted drain pipe, solids may still aggregate on the flat plate gas distributor, particularly in sections far removed from the sidewall-mounted drain pipe, and eventually grow sufficiently large to force shutdown of the reaction vessel and cleaning of the gas distributor, which adds undesired expense and delay to the fluorination process.
It would thus be desirable to provide embodiments of fluidized bed fluorination reactor wherein the aggregation of solids within a reaction vessel is minimized. Ideally, embodiments of such a fluidized bed fluorination reactor would employ a unique fluorine gas distributor providing improved gas flow characteristics within the reaction vessel, such as improved solids-gas mixing within the reaction vessel to increase the mass and heat transfer between solids and gas phases during fluorination. It would further be desirable to provide embodiments of a fluidized bed reactor suitable for carrying-out such a fluorination process or other fluidized reaction wherein the accumulation of solids is minimized and wherein solids-gas mixing is improved. It would still further be desirable to provide embodiments of a fluorination process performed utilizing a fluidized bed fluorination reactor and providing the above-noted advantages. Other desirable features and characteristics of the present invention will become apparent from the subsequent Detailed Description and the appended Claims, taken in conjunction with the accompanying Drawings and the foregoing Background.
Embodiments of a fluidized bed fluorination reactor are provided. In one embodiment, the fluidized bed fluorination reactor includes a source of fluorine gas, a reaction vessel, a windbox fluidly coupled to the source of fluorine gas, and a conical gas distributor fluidly coupled between the reaction vessel and the windbox. The conical gas distributor has a plurality of gas flow openings directing fluorine gas flow from the windbox into the fluorination reaction vessel during the fluorination process.
Embodiments of a fluidized bed reactor are further provided. In one embodiment, the fluidized bed reactor includes a source of gaseous reactant, a reaction vessel, a windbox fluidly coupled to the source of gaseous reactant, and a conical gas distributor fluidly coupled between the reaction vessel and the windbox. The conical gas distributor has a plurality of gas flow openings directing gaseous reactant flow from the windbox and into the reaction vessel during the reaction.
Embodiments of a fluorination process are further provided, which are carried-out utilizing a fluidized bed fluorination reactor of the type that includes a reaction vessel and a conical gas distributor having a plurality of gas flow openings formed therein. In one embodiment, the fluorination process includes the steps of supplying uranium tetrafluoride to the reaction vessel, and directing fluorine gas into the reaction vessel through the conical gas distributor and along a plurality of gas flow paths that are non-parallel with the longitudinal axis of the reaction vessel to support a fluorination reaction yielding uranium hexafluoride.
At least one example of the present invention will hereinafter be described in conjunction with the following figures, wherein like numerals denote like elements, and:
The following Detailed Description is merely exemplary in nature and is not intended to limit the invention or the application and uses of the invention. Furthermore, there is no intention to be bound by any theory presented in the preceding Background or the following detailed description.
Although described below in conjunction with a particular type of fluidized bed reactor, namely, a fluorination reactor, embodiments of the fluidized bed reactor can be utilized to carry-out other types of fluidized bed reactions, such as fluidized bed hydro-fluorination and reduction reactions, oxidation reactions, or chlorination reactions. This notwithstanding, embodiments of the fluidized bed reactor described below are particularly well-suited for carrying-out fluorination reactions wherein aggregation of solids is especially problematic due, at least in part, to the highly reactive nature of fluorine and the tremendous amounts of heat generated by the fluorination reaction. Thus, in preferred embodiments, and by way of non-limiting example only, the fluidized bed reactor is implemented as a fluidized bed fluorination reactor suitable for carrying-out the fluorination of, for example, uranium tetrafluoride (UF4) to yield uranium hexafluoride (UF6).
Windbox 14 includes a shell 28 defining an interior chamber, which is fluidly coupled to a source of fluorine gas 30 by way of a fluorine inlet pipe 32. As utilized herein, the term “pipe” encompasses all types of flow conduits, as well as assemblies of flow conduits joined in fluid communication. The fluorine gas, which may be generically referred to as a “fluidizing gas” herein, flows through inlet pipe 32 into windbox 14, through a conical gas distributor (hidden from view in
A perforated flat plate gas distributor has traditionally been employed to conduct the fluorine gas from windbox 14 into reaction chamber 18 of reaction vessel 12. The flat plate gas distributor, which typically assumes the form of a disk or grate-like structure, also supports the fluidized bed held within reaction vessel 12. As noted above, such perforated flat plate gas distributors do not achieve optimal gas-solids mixing and are prone to the accumulation of solid aggregates thereon. The aggregation of solids is especially problematic in the context of fluorination reactions due, at least in part, to the highly reactive nature of fluorine, to the highly exothermic nature of the fluorination reaction, and to impurities unavoidably present within the UF4 and bed materials. To mitigate the above-described problems, and specifically to provide improved gas-solids mixing and a significant reduction in the accumulation of solids within the reaction vessel and over the gas distributor, fluidized bed fluorination reactor 10 is equipped with a unique conical gas distributor and, in preferred embodiments, further with a solids drain pipe fluidly coupled to a central opening provided in the conical gas distributor. An example of such a conical gas distributor and central solids drain pipe is described more fully below in conjunction with
While conical gas distributor 38 can be mounted between reaction vessel 12 (
The dimensions of conical gas distributor 38, the material or materials from which gas distributor 38 is formed, and the manner in which gas distributor 38 is fabricated will inevitably vary amongst different embodiments. However, by way of non-limiting example, it is noted that gas distributor 38 is preferably formed from a high temperature metal or alloy and fabricated to have a single piece or unitary construction. Gas flow openings 46 can be formed through conical support wall 44 of gas distributor 38 utilizing a suitable drilling process, such as mechanical drilling or laser drilling. If desired, the mouths or inlets of gas flow openings 46 (i.e., the bottom ends of openings 46 in the illustrated orientation) may be chamfered. While by no means limited to a particular range of thicknesses, conical support wall 44 and annular mounting flange 62 of gas distributor 38 are preferably fabricated to be sufficiently thick to support the fluidized bed held within reaction vessel 12 (
With continued reference to the exemplary embodiment illustrated in
As noted above, the shape of conical support wall 44 and the shape, size, disposition, and dimensions of gas flow openings 46 are optimized to promote solids-gas mixing within reaction vessel 12 and drainage of aggregate solids through solids drain pipe 40. With respect to conical support wall 44, in particular, it will be readily appreciated that conical support wall 44 converges toward solids opening 48 and, thus, the inlet of solids drain pipe 40. Conical support wall 44 preferably has a substantially smooth outer surface and a sufficient slant or declination to promote gravity flow of solids into solids openings 48 and, therefore, into solids drain pipe 40 for reliable and continual removal of the aggregate solids from reaction vessel 12 (
Gas flow openings 46 are preferably configured to provide high velocity gas flow from windbox 14 into reaction vessel 12 (
In a preferred embodiment, gas flow openings 46 cooperate to create vortices-like fluorine flow within a bottom portion of reaction vessel 12 immediately above conical gas distributor 38 to increase agitation of the fluidized bed and further improve solids-gas mixing. The creation of gas flow vortices within a bottom portion of reaction vessel 12 may be enhanced by imparting gas flow openings with a distribution or spatial arrangement that is non-symmetrical. The creation of gas flow vortices, along with a substantially widespread distribution of gas flow openings 46, also helps reduce or eliminate the formation of dead zones across the upper surface of conical gas flow distributor 38. Each gas flow opening 46 preferably has a substantially straight or non-tortuous geometry to optimize gas flow velocity. Although not shown in
The foregoing has thus provided embodiments of a fluidized bed reactor, such as a fluidized bed fluorination reactor, employing a conical gas distributor, preferably in conjunction with a solids drain pipe fluidly coupled to a central opening in the conical gas distributor, to promote the continual removal of solid aggregates from within a reaction vessel and to thereby deter the accumulate of such solid aggregates to sizes that could otherwise interfere with operation of fluidized bed reactor and ultimately force reactor shutdown. Notably, the above-described conical gas distributor also improves overall fluidization quality, gas residence time, gas-solids mixing, and heat and mass transfer as compared to traditional perforated flat plate gas distributors. The foregoing has also provided embodiments of a fluorination process carried-out utilizing a fluidized bed fluorination reactor of the type that includes a reaction vessel and a conical gas distributor having a plurality of gas flow openings formed therein. In one embodiment, the fluorination process includes the steps of supplying uranium tetrafluoride to the reaction vessel and directing fluorine gas into the reaction vessel through the conical gas distributor and along a plurality of gas flow paths that are non-parallel with the longitudinal axis of the reaction vessel to support a fluorination reactor yielding uranium hexafluoride.
By way of non-limiting illustration, an exemplary implementation of the fluidized bed reactor has been described above wherein the reactor assumed the form of a fluorine reactor utilized to covert uranium tetrafluoride to uranium hexafluoride. Embodiments of the fluidized bed reactor are especially well-suited for usage as fluorine reactors, such as the fluidized bed fluorination reactors utilized to convert uranium tetrafluoride to uranium hexafluoride, as the fluorination reaction is especially prone to the aggregation of solids due to the highly reactive nature of fluorine, the large amounts of heat generated by the fluorination reaction, and impurities present in the uranium tetrafluoride and fluidized bed materials. This notwithstanding, embodiments of fluidized bed reactor are by no means limited to usage in conjunction with fluorination processes. In this regard, the foregoing description has provided embodiments of a fluidized bed reactor for use in conjunction with a fluidizing gas, which may or may not be a fluorination reactor utilized in conjunction with a fluorine gas. Thus, the foregoing has generally provided embodiments of a fluidized bed reactor that includes a source of gaseous reactant, a reaction vessel, and a windbox fluidly coupled to the source of gaseous reactant, and a conical gas distributor fluidly coupled between the reaction vessel and the windbox. The conical gas distributor having a plurality of gas flow openings directing gaseous reactant flow from the windbox and into the reaction vessel during the reaction. In certain embodiments, and depending upon the desired reactions, the gaseous reactant may be fluorine, chlorine, hydrogen fluoride, hydrogen, hydrogen chloride, oxygen, air, steam, and mixtures thereof. In certain cases, the gaseous reactant may be diluted by an inert gas, such as nitrogen, argon, or helium.
While multiple exemplary embodiments have been presented in the foregoing Detailed Description, it should be appreciated that a vast number of variations exist. It should also be appreciated that the exemplary embodiment or exemplary embodiments are only examples, and are not intended to limit the scope, applicability, or configuration of the invention in any way. Rather, the foregoing Detailed Description will provide those skilled in the art with a convenient road map for implementing an exemplary embodiment of the invention. It being understood that various changes may be made in the function and arrangement of elements described in an exemplary embodiment without departing from the scope of the invention as set-forth in the appended Claims.