Method and device for dry treatment of irradiated nuclear fuel
专利摘要:
Irradiated nuclear fuels consisting primarily of plutonium compounds and/or uranium compounds such as oxides, carbides, nitrides are converted in accordance with the method to plutonium hexafluoride and/or uranium hexafluoride. In a first step, the compounds are contacted within a first zone of an enclosure with a gas mixture containing at least one fluorination reagent. In a second step, the remainder of the compounds which have not been converted to fluorides during the first step is contacted directly within a second zone of the enclosure with a bed which has been fluidized by means of a gas mixture containing at least one fluorination reagent. 公开号:SU791271A3 申请号:SU772523052 申请日:1977-09-20 公开日:1980-12-23 发明作者:Буржуа Мишель;Маневи Жорж;Ру Жан-Пьер 申请人:Коммиссариат А Л"Энержи Атомик (Фирма); IPC主号:
专利说明:
(54) METHOD FOR DRY TREATMENT OF IRRADIATED NUCLEAR FUEL AND DEVICE FOR ITS IMPLEMENTATION one The invention relates to the nuclear industry, namely to the processing of irradiated nuclear fuel. A known method for repeated dry treatment of fuel used in fast reactors or light water, which are mixed oxides of plutonium, consists in exposing the above mentioned oxides to gaseous fluorine-containing Yu reagents, such as fluorine, bromine pentafluoride, chlorine trifluoride, in the reaction zone fluidized bed -1, However, the fluorination of plutonium oxide 5 or plutonium tetrafluoride (an intermediate in the reaction between PuO and Pu) takes place slowly, and in the presence of an inert component, such as hydroxide aluminum 20, these reactions become even slower. This method does not take place at temperatures higher due to the danger of corrosion of equipment materials .25 There is also known a method of dry treatment of irradiated nuclear fuel, formed, in particular, of plutonium compounds and / or uranium compounds selected in the group, including oxides, carbides and nitrides, according to which these compounds plutonium and / or uranium are converted into plutonium and / or uranium hexafluorides by fluorination reactions carried out in a plasma reactor. A device for dry processing of the obtained nuclear fuel is known, which contains chambers for carrying out fluorination 2. However, with this process, the reactions are incomplete, i.e. the unburned products are in the solid state. The purpose of the invention is to increase the yield of the fluorides formed and to maximize the loss of participation. The RCT in the reaction products. This goal is achieved in that the method of dry treatment of irradiated nuclear fuel, formed, in particular, plutonium compounds and / or uranium compounds, selected in the group, including oxides, carbides and nitrides, according to which these compounds plutonium and / or uranium in hexa, plutonium and / or uranium fluorides by fluorination reactions carried out in a plasma reactor include two steps in one and in the same chamber, the combination of fluorination reactions occurring in the plasma reactor with the fluorination reaction taking place in the fluidized bed reactor, the first step being to bring Vkontakt in the first zone of the above chamber of plutonium and / or uranium compounds with a gas mixture containing at least one fluorinated reagent, and separating the gaseous fluorides formed from solid compounds, and the second stage consists in bringing the solid compounds, not p eobrazovavshihs during fluorides during the first phase, fluidized bed through a gas mixture containing at least one fluorinated reagent, and wherein the formed compartment fluorides from the last residues of solid compounds. In an apparatus for carrying out a dry treatment of irradiated nuclear fuel containing a chamber for carrying out fluorination reactions, the latter is divided into zones: the first for converting a part of solids into gases, an intermediate separation zone of the formed gases and solids that have not been converted to gases, the second reaction zone of solid substances that are not converted in the first zone, with a layer that is fluidized by a gas mixture that has the ability to complete the conversion of the above solid substances in gases at high temperature, said second zone being provided with means for supplying the fluidized bed and the output means remaining solid residues, and the intermediate zone is provided with means output the formed gases formed as Tsilya schricheskogo channel opening into the separation zone, within which is located a block filtration output gases. Means are also provided for heating and / or cooling the walls of the chamber. The drawing shows a diagram of the proposed device. The device for dry treatment of irradiated nuclear fuel comprises a chamber 1, which has a first zone 2, called the combustion zone, an intermediate zone 3 (separation zone), a second zone 4 (fluidized zone). The upper part of chamber 1 contains a closing plate 5 through which a channel 6 for supplying powdered irradiated nuclear fuel and an inert gas and another channel 7 for supplying fluorine-containing reagent passes. The lower part 8 of channel b is a burner port. The combustion zone 2 contains windows 9 located at the ends of the side pipelines. 10, below the burner exit plane, so as to observe the occurrence of the flame. The walls of the burning zone 2 contain either heating means 11 (e.g., resistance windings) or cooling means 12 (e.g., coolant circulation in the second shell) outside the chamber. The use of heating means 11 or cooling means 12 depends on the nature of the fuel being processed and on the operating speeds, which are in accordance with the characteristics of the device. In the intermediate zone 3 of the chamber 1, called the separation zone, there is an outlet of a cylindrical channel 13 intended to discharge the gaseous fluorides formed. In this separation zone 3, solid compounds that have not been converted to gas are separated from the gaseous fluorides formed and fall under the force of gravity into the lower part of the chamber, which is a fluidized bed zone 4, whereas the gaseous fluorides formed are passed through channel 13 This channel is equipped with filters 14, which are designed to trap fine solid particles, which can together with gases. fall to the exit from the separation zone. This channel 13 also has cooling means, similar to cooling means 12, or heating means, similar to heating means 11. The lower end 15 of the fluidized bed zone 4 ends in a truncated cone. At this end 15 there is an outlet of a channel 16 for feeding a mixture of fluorine-containing reagent and an inert gas and a channel 17 for diverting the last remaining solid residues. The walls of the fluidized bed zone 4 are also provided with heating means or cooling means. The device works as follows. The powder mixture of oxides U02 and PuO with decomposition products is injected into the inert gas through channel b and simultaneously fluorine is introduced through channel-7. At the level of part 8 of channel B, a flame spontaneously arises, which is maintained by itself until most of the products burn, this flame is observed through the windows 9. The burner 8, in addition to the central opening of the supply of combustible powder, contains one or several other openings concentrically relative to the central openings and which form rings for insertion into the chamber of various co. relevant gas. Waste gas leaving the combustion zone 2, as well as solids, not fully converted into the gas, or remaining solid during combustion, is cooled during its passage through zone 2 by means of 12. In the separation zone, the separation of the remaining solid compounds from the resulting gases is due to decantation. If a large part of the solid particles falls under the action of its own weight into the zone 4 of the chamber, then the gas waste consisting of a mixture of excess fluorine, oxygen, UF, Pu and several volatile salts of decomposition products is directed yo to channel 13 to the filters 14. Fluidized bed zone 4 has a layer of solid aluminum hydroxide particles mixed with particles of solid compounds not converted to fluorides; this layer is fluidized using a mixture of fluorine and inert gas fed through channel 16. Solid forms are mixed in the lower part 15 of zone 4. components of the Liquefied Layer. This is necessary because incomplete mixing, due to the potential for exothermic reactions with solid compounds not yet converted to fluorides, causes a rise in temperature that promotes the sintering of solid particles and interferes with the reaction. This fluidized bed zone is heated by means of heating during the passage of the fluidization mixture through the bed of solids. It is cooled by any suitable device. The waste gas generated in the upper part of the fluidized bed zone 4, which is a mixture of gaseous fluorine and gaseous puP, is directed through channel 13 to the filters 14. The plutonium depletion rate of the fluidized bed is kept high and uniform due to external vibration of the chamber or by frequently blowing back inert gas or fluorine through the filters 14. These filters 14 are installed in parallel — one is working while the other is cleared from clogging by the back gas flow. The reactions carried out in the combustion zone 2 and in the fluidized bed zone 4 are carried out simultaneously. They are also made independently, for example, with variable operation of the combustion zone 2, and then the fluidized bed zone 4, and the mixing of this fluidized bed is always carried out by the appropriate inert gas flows during the operation of the burning zone 2. During periodic outages in one or another zone, the inoperative zone is cleaned by flushing the appropriate inert gas. The device operates almost continuously or semi-continuously if an appropriate power supply device for the powder-burning zone 2 is used, such as a bunker-feed device or a screw, an appropriate mechanism for introducing into the zone 4 the solid component of the fluidized bed, as well as an appropriate mechanism for continuous output or intermittent output of depleted fluid bed load, Thus, in accordance with 5, and due to the use of the device, the first treatment stage in the combustion zone 2 allows to convert almost completely uranium oxide and most of the plutonium oxide into hexafluorides, the second stage in the fluidized zone 4 is extremely reliable, since the amount of oxides which remains to be processed in this fluidized bed NOM layer, is much smaller than when the nuclear fuel is directly processed in this fluidized bed, therefore a very significant decrease occurs the seizure capabilities of the fluidized bed due to the exothermic nature of the reactions.
权利要求:
Claims (1) [1] 1. Method for dry treatment of irradiated nuclear fuel formed, in particular, plutonium compounds and / or uranium compounds selected in the group comprising oxides, carbides and nitrides, according to which these plutonium and / or uranium compounds are converted to plutonium hexafluorides and / or uranium by fluorination reactions are carried out .1 And in a plasma reactor, characterized in that / in order to increase the yield of fluorides formed and to maximize products involved in the reaction, it involves a combination of fluorination reactions in the plasma reactor, carried out in two stages in the same chamber, with the reaction fluorination, which takes place in the fluidized bed reactor; the first stage consists in bringing into contact in the first zone of the above chamber of the compounds of plutonium and / or uranium with a gas mixture containing, by at least one fluorinated reagent, and separating gaseous fluorides formed from solid compounds, and the second stage consists in contacting directly
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同族专利:
公开号 | 公开日 BE858830A|1978-01-16| DE2741402A1|1978-03-23| GB1576657A|1980-10-15| US4202861A|1980-05-13| FR2365187B1|1981-05-08| FR2365187A1|1978-04-14| JPS5338896A|1978-04-10|
引用文献:
公开号 | 申请日 | 公开日 | 申请人 | 专利标题 FR72440E|1957-11-05|1960-04-13|Commissariat Energie Atomique|Improvements in processes and apparatus of the kind for obtaining uranium fluoride| BE621972A|1961-10-26|1900-01-01| DE1244143B|1964-11-21|1967-07-13|Kernforschungsanlage Juelich D|Process for processing nuclear fuel containing uranium| US3294493A|1966-04-18|1966-12-27|Albert A Jonke|Method of separating uranium and plutonium| BE729289A|1968-03-09|1969-08-18| GB1219528A|1968-10-24|1971-01-20|Atomic Energy Commission|Fluoride reprocessing of nuclear fuels| US3790493A|1971-04-06|1974-02-05|Gen Electric|Post oxidation process for uranium dioxide rich compositions|FR2391782B1|1976-09-02|1980-02-15|Pechiney Ugine Kuhlmann| US4522794A|1983-08-25|1985-06-11|The United States Of America As Represented By The Department Of Energy|Fluorination process using catalyst| US4555318A|1984-01-06|1985-11-26|The United States Of America As Represented By The United States Department Of Energy|Removal of fluoride impurities from UF6 gas| JPS60184526U|1984-05-18|1985-12-07| FR2687140B1|1992-02-11|1994-05-13|Pechiney Uranium|METHOD FOR RECOVERING AND PURIFYING A HIGHLY ENRICHED URANIUM-BASED METAL ALLOY.| FR2692880B1|1992-06-29|1994-09-02|Pechiney Uranium|Process for the selective electro-fluorination of alloys or metallic mixtures based on uranium.| ZA938990B|1992-12-04|1994-08-03|Atomic Energy South Africa|Production of uranium hexafluoride| US8192704B1|2011-02-25|2012-06-05|The United States Of America As Represented By The Department Of Energy|Spent nuclear fuel recycling with plasma reduction and etching|
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申请号 | 申请日 | 专利标题 FR7628147A|FR2365187B1|1976-09-20|1976-09-20| 相关专利
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