CN112875770A - Microwave denitration device - Google Patents
Microwave denitration device Download PDFInfo
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- CN112875770A CN112875770A CN202011525242.4A CN202011525242A CN112875770A CN 112875770 A CN112875770 A CN 112875770A CN 202011525242 A CN202011525242 A CN 202011525242A CN 112875770 A CN112875770 A CN 112875770A
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- microwave
- plutonium
- cavity
- neptunium
- material container
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G56/00—Compounds of transuranic elements
- C01G56/004—Compounds of plutonium
- C01G56/005—Oxides; Hydroxides
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G56/00—Compounds of transuranic elements
- C01G56/007—Compounds of transuranic elements
- C01G56/008—Compounds of neptunium
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C19/00—Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
- G21C19/42—Reprocessing of irradiated fuel
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Abstract
The invention discloses a microwave denitration device, which is used for converting a neptunium nitrate/plutonium solution into neptunium oxide/plutonium powder; the device consists of a microwave generator, a microwave transmission line, a control system, a radioactive sealed box chamber, a microwave cavity and a material container. The device provided by the invention uses microwave heating for concentration and solidification of the tail end product solution in the nuclear fuel post-treatment process, thereby simplifying the post-treatment process of spent fuel.
Description
Technical Field
The invention relates to the field of spent fuel post-treatment, in particular to a microwave denitration device.
Background
During spent fuel reprocessing, it is often necessary to convert neptunium nitrate or plutonium nitrate from a nitrate solution state to an oxide solid state that is easy to transport and store for subsequent processing. For the batch or continuous operation of the neptunium and plutonium tail end process, the currently adopted technical route in foreign countries and China is the process of precipitation and calcination of neptunium and plutonium oxalate, which mainly comprises the following working procedures: 1) preparation of precipitation feed liquid (valence state adjustment and acid regulation); 2) neptunium oxalate and plutonium precipitate; 3) neptunium oxalate and plutonium are filtered; 4) drying and roasting the neptunium oxalate and the plutonium; 5) pouring, weighing and packaging the neptunium dioxide and plutonium products; 6) treating mother liquor obtained after plutonium oxalate precipitation and filtration; 7) pre-purifying the waste gas of the roasting furnace.
The process has the advantages that: (1) the method has a certain purification effect on neptunium and plutonium, the purification coefficient of the split sheet can reach 2-3, and the purity of the obtained neptunium and plutonium products is higher; (2) the obtained oxide has high activity and is beneficial to post-treatment.
However, this process also has the following disadvantages: the process and equipment are complex, more dilute solution is generated, the loss of nuclear materials is caused, and the waste liquid treatment is difficult.
The microwave oven heating process is that an electronic vacuum tube-magnetron generates ultrashort wave electromagnetic waves, the ultrashort wave electromagnetic waves are transmitted to various places in the oven through a microwave transmission element-waveguide tube, polar molecules of materials are caused to vibrate at a very high speed of billions of times per second through transmission, conduction and absorption by materials in the oven, and friction caused by vibration enables the interior of the materials to generate high heat, so that the materials are heated and transformed. The microwave denitration of partial nitrate comprises different stages of solution evaporation and concentration, concentrated solution acid decomposition, denitration and the like, wherein the specific temperature rise process is that the solution starts to boil, the temperature of the solution is increased (120-120 ℃) in boiling, the nitric acid starts to decompose (approximately equal to 200 ℃), the volume of the solution is expanded and solidified (approximately equal to 220 ℃), and the denitration reaction is performed (approximately equal to 230 ℃) and the temperature is reduced (approximately equal to 200 ℃).
The method for heating and denitrating by microwaves has many advantages, such as simple denitration process, easy equipment operation, good powder property of products, no addition of chemical reagents, minimum waste amount in the process and the like. It can avoid the difficulties in precipitation filtration or fluidized bed control. Meanwhile, microwave heating is only for materials absorbing microwaves, other environments can not be heated, and material transformation is energy-saving. A microwave heating denitration device is developed and used for concentrating and solidifying a tail end product solution in the nuclear fuel post-treatment process, so that the spent fuel post-treatment process can be simplified, the dependence on chemical reagents in the process is reduced, and the spent fuel post-treatment process is more energy-saving and environment-friendly.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a microwave heating denitration device, which uses microwave heating for concentrating and solidifying a tail end product solution in the nuclear fuel post-treatment process and simplifies the treatment process.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a microwave denitration apparatus for converting a neptunium/plutonium nitrate solution into neptunium oxide/plutonium powder; the device consists of a microwave generator, a microwave transmission line, a control system, a radioactive sealed box chamber, a microwave cavity and a material container;
the microwave generator, the microwave transmission line and the control system are positioned outside the radioactive sealed box chamber;
the microwave cavity and the material container are positioned in the radioactive sealed box chamber;
the material container is positioned in the microwave cavity;
the microwave generator is used for generating high-power microwaves;
the microwave transmission line is used for transmitting high-power microwaves to the microwave cavity;
the material container is used for containing a neptunium nitrate/plutonium solution.
Further, the material of the microwave cavity is 316L stainless steel;
further, a monitoring system is arranged in the microwave cavity.
Further, the monitoring system comprises a temperature sensor, a humidity sensor, a liquid level sensor and a camera.
Further, the control system can control and change the generation of the microwave and the output power according to the data feedback of the monitoring system.
Furthermore, a wall tube is arranged to penetrate through the side wall of the microwave cavity for the microwave transmission line to enter the microwave cavity.
Further, the material container is a crucible.
The invention has the beneficial effects that:
1) the microwave denitration device has simple operation, can avoid the difficulties in precipitation filtration or fluidized bed control, does not need to add chemical reagents, and has small waste amount in the process.
2) The microwave denitration device can adjust the process parameters according to the properties and the volumes of different salt solutions, evaporate and solidify the solutions, and achieve the purpose of treating the different salt solutions.
Drawings
FIG. 1 is a schematic diagram of a microwave denitration apparatus according to the present invention.
Detailed Description
The invention is described in further detail below with reference to the drawings and the detailed description.
Example 1
As shown in fig. 1, a microwave denitration apparatus for converting a neptunium nitrate/plutonium solution into neptunium oxide/plutonium powder; the device consists of a microwave generator, a microwave transmission line, a control system, a radioactive sealed box chamber, a microwave cavity and a material container.
The microwave generator, the microwave transmission line and the control system are positioned outside the radioactive sealed box chamber (non-radioactive area); the microwave cavity and the material container are positioned inside the radioactive sealed box chamber (radioactive area); the material container is located inside the microwave cavity, is a crucible and is used for containing the neptunium nitrate/plutonium solution, is a main place for denitration reaction, and gradually converts the neptunium nitrate/plutonium solution into an oxide through microwave heating. The material of the microwave cavity is 316L stainless steel, which can restrain the microwave inside the cavity.
The microwave generator is used for generating high-power microwaves; the microwave transmission line is used for transmitting high-power microwaves to the microwave cavity, is of a waveguide transmission structure, and is provided with a wall tube penetrating through the side wall of the microwave cavity so that the microwave transmission line enters the microwave cavity.
A monitoring system is arranged in the microwave cavity. The monitoring system comprises a temperature sensor, a humidity sensor, a liquid level height sensor and a camera. The temperature sensor, the humidity sensor, the liquid level height sensor, the camera and other sensors have the main functions of monitoring the temperature, the humidity of generated water vapor, the thickness of a liquid layer and the working state in the material reaction process and simultaneously utilizing the monitored data; the control system mainly realizes the control function, and controls and changes the generation of microwaves, the output power, the heating temperature, the feedback image, the humidity, the liquid level height information and the like according to the data feedback of the monitoring system.
The microwave denitration device is a continuous heating process and is controlled by a control system, and can complete temperature and time length control of different stages of solution evaporation concentration, concentrated solution acid decomposition, denitration and the like. The microwave denitration device can adjust technological parameters according to the properties and the volumes of different salt solutions, and achieve the purposes of evaporating, solidifying and the like on the solutions.
The typical microwave denitration device has the length of 600-. By adopting the microwave denitration device provided by the invention, a cerium nitrate solution with a certain concentration, with the nitric acid concentration of 1-3mol/L, is placed in a quartz material container, then is placed in a microwave cavity, and a microwave generator is opened to carry out microwave denitration reaction. The microwave pulse width is manually adjusted to provide different microwave powers for materials at different reaction stages, a thermocouple is used for measuring the temperature in the experimental process, a prototype collects a series of temperature data and automatically records the temperature data, and then a temperature rise curve can be generated. The final product is cerium dioxide solid with qualified nitrogen content, the highest temperature is freely adjusted, the whole experiment time is automatically controlled and uniformly controlled by a control system, and the obtained product is sampled, inspected and stored after the experiment is finished.
The temperature control curve shows that each stage of microwave denitration is obvious, the nitrogen fixation content of the microwave denitration product reaches the standard, the equipment can realize microwave denitration of nitrate such as neptunium nitrate (plutonium) and the like, and qualified neptunium oxide (plutonium) powder is obtained. The equipment operates normally in the process, can realize remote control, and is suitable for places such as a hot room with radioactive shielding.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations.
Claims (7)
1. A microwave denitration apparatus for converting a neptunium/plutonium nitrate solution into neptunium oxide/plutonium powder; the device consists of a microwave generator, a microwave transmission line, a control system, a radioactive sealed box chamber, a microwave cavity and a material container;
the microwave generator, the microwave transmission line and the control system are positioned outside the radioactive sealed box chamber;
the microwave cavity and the material container are positioned in the radioactive sealed box chamber;
the material container is positioned in the microwave cavity;
the microwave generator is used for generating high-power microwaves;
the microwave transmission line is used for transmitting high-power microwaves to the microwave cavity;
the material container is used for containing a neptunium nitrate/plutonium solution.
2. The microwave denitration apparatus of claim 1, wherein the material of the microwave cavity is 316L stainless steel.
3. The microwave denitration device of claim 1, wherein a monitoring system is arranged in the microwave cavity.
4. The microwave denitration device of claim 3, wherein the monitoring system comprises a temperature sensor, a humidity sensor, a liquid level sensor and a camera.
5. The microwave denitration apparatus according to claim 4, wherein the control system is capable of controlling and changing the generation of the microwave and the output power according to the data feedback of the monitoring system.
6. The microwave denitration apparatus of claim 1, wherein a wall-through pipe is provided to pass through a side wall of the microwave cavity for the microwave transmission line to enter the microwave cavity.
7. The microwave denitration apparatus of claim 1, wherein the material container is a crucible.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202011525242.4A CN112875770A (en) | 2020-12-22 | 2020-12-22 | Microwave denitration device |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202011525242.4A CN112875770A (en) | 2020-12-22 | 2020-12-22 | Microwave denitration device |
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| CN112875770A true CN112875770A (en) | 2021-06-01 |
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| CN202011525242.4A Pending CN112875770A (en) | 2020-12-22 | 2020-12-22 | Microwave denitration device |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113241208A (en) * | 2021-06-22 | 2021-08-10 | 中国原子能科学研究院 | Accommodating device for plutonium tail end processing, evaporation and calcination system and method |
| CN113447614A (en) * | 2021-06-21 | 2021-09-28 | 中国原子能科学研究院 | Method for measuring denitration rate in radioactive waste liquid calcination process |
| CN115452543A (en) * | 2022-09-21 | 2022-12-09 | 中国原子能科学研究院 | Rapid preprocessing device and method for total alpha and beta measurement |
Citations (6)
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|---|---|---|---|---|
| JPS57188417A (en) * | 1981-05-13 | 1982-11-19 | Toshiba Corp | Microwave heating and denitrating apparatus |
| US4563335A (en) * | 1982-12-21 | 1986-01-07 | Doryokuro Kakunenryo Kaihatsu Jigyodan | Apparatus for continuously concentrating and denitrating nitrate solution by microwave |
| CN106582474A (en) * | 2016-10-20 | 2017-04-26 | 核工业理化工程研究院 | Semicontinuous and automatic microwave denitration device |
| CN106629854A (en) * | 2016-10-20 | 2017-05-10 | 核工业理化工程研究院 | Method for producing uranium trioxide by heating uranyl nitrate solution in microwave manner |
| CN109592714A (en) * | 2018-11-19 | 2019-04-09 | 中核二七二铀业有限责任公司 | A kind of method of uranyl nitrate thermal denitration preparation high activity orange oxide |
| CN111020244A (en) * | 2020-01-09 | 2020-04-17 | 中国原子能科学研究院 | Method for extracting plutonium-238 from irradiated neptunium target and recovering neptunium-237 |
-
2020
- 2020-12-22 CN CN202011525242.4A patent/CN112875770A/en active Pending
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS57188417A (en) * | 1981-05-13 | 1982-11-19 | Toshiba Corp | Microwave heating and denitrating apparatus |
| US4563335A (en) * | 1982-12-21 | 1986-01-07 | Doryokuro Kakunenryo Kaihatsu Jigyodan | Apparatus for continuously concentrating and denitrating nitrate solution by microwave |
| CN106582474A (en) * | 2016-10-20 | 2017-04-26 | 核工业理化工程研究院 | Semicontinuous and automatic microwave denitration device |
| CN106629854A (en) * | 2016-10-20 | 2017-05-10 | 核工业理化工程研究院 | Method for producing uranium trioxide by heating uranyl nitrate solution in microwave manner |
| CN109592714A (en) * | 2018-11-19 | 2019-04-09 | 中核二七二铀业有限责任公司 | A kind of method of uranyl nitrate thermal denitration preparation high activity orange oxide |
| CN111020244A (en) * | 2020-01-09 | 2020-04-17 | 中国原子能科学研究院 | Method for extracting plutonium-238 from irradiated neptunium target and recovering neptunium-237 |
Non-Patent Citations (2)
| Title |
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| ZHAO, YUNFENG ET AL.: "《PROGRESS IN NUCLEAR ENERGY》", 31 January 2008 * |
| 鲍卫民等: "微波脱硝用于高加浓铀转型的研究", 《原子能科学技术》 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113447614A (en) * | 2021-06-21 | 2021-09-28 | 中国原子能科学研究院 | Method for measuring denitration rate in radioactive waste liquid calcination process |
| CN113241208A (en) * | 2021-06-22 | 2021-08-10 | 中国原子能科学研究院 | Accommodating device for plutonium tail end processing, evaporation and calcination system and method |
| CN115452543A (en) * | 2022-09-21 | 2022-12-09 | 中国原子能科学研究院 | Rapid preprocessing device and method for total alpha and beta measurement |
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Application publication date: 20210601 |