CN1287364A - Microwave heating process to solidify high radioactive waste liquid - Google Patents

Microwave heating process to solidify high radioactive waste liquid Download PDF

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Publication number
CN1287364A
CN1287364A CN00124466A CN00124466A CN1287364A CN 1287364 A CN1287364 A CN 1287364A CN 00124466 A CN00124466 A CN 00124466A CN 00124466 A CN00124466 A CN 00124466A CN 1287364 A CN1287364 A CN 1287364A
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China
Prior art keywords
high activity
liquid waste
activity liquid
microwave
reaction vessel
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CN00124466A
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CN1121045C (en
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鲍卫民
宋崇立
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Tsinghua University
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Tsinghua University
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00Energy generation of nuclear origin
    • Y02E30/30Nuclear fission reactors
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02WCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00Technologies for solid waste management
    • Y02W30/50Reuse, recycling or recovery technologies

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  • Processing Of Solid Wastes (AREA)
  • Heat Treatment Of Water, Waste Water Or Sewage (AREA)

Abstract

The present invention features that microwave from microwave source is utilized in heated evaporation and denitration of high radioactive waste liquid to obtain solidified material, which is further burnt and packed as solidified intermediate of waste liquid. the solidified intermediate is easy to store and transport with less safety risk.

Description

Method with microwave heating intermediate solidification high activity liquid waste
The invention belongs to the radioactive waste process field, specially refer to the process field of the intermediate solidification of being convenient to temporary or transportation high activity liquid waste.
High activity liquid waste is the refuse that nuclear power plant and aftertreatment factory produce, because waste liquid brings risk for the leakage of high activity liquid waste to corrosion (intense radiation corrosion is down strengthened), disaster (for example earthquake, water, fire, meteorite hit etc.) or the artificial factor (war, riot, accident etc.) of reservoir vessel.Its leakage will cause great pollution to environment, cause great harm to biology.The railway line of the traffic requirements special use of high activity liquid waste, special-purpose haulage vehicle and cask, all these must pay a high price for.
Is the high activity liquid waste solidification that safe handling is necessary.The glass solidification method of France has been represented the solidified prior art of high activity liquid waste (seeing Commissariat A L'Energie Atomique's report " CEA-CONF-12277 ").It is the glass blocks of selecting different formulations at the concrete composition of different high activity liquid wastes, high activity liquid waste is cast to the glass blocks fusion in proportion again solidifies in the rustless steel container.Russia also has business-like glass solidification device (to see the monograph that SIA " Radon " (" Enomar ") 1996 publishes: holy " thunder is stepped on " experience " SIA " Radon " experience in radioactive waste vitrification " aspect the radioactive waste glass solidification).They are purpose with the high activity liquid waste final disposal all.Do not having huge fund input, do not grasping before the complex technology of glass solidification high activity liquid waste, all can not build glass solidification factory.Therefore, not that each unit that produces high activity liquid waste can both maybe must build glass solidification factory.But, high activity liquid waste is done middle curing processing does not see as yet so far that to be suitable for temporarily depositing or be transported to other local relevant technologies of handling report is arranged.
The object of the present invention is to provide a kind of method of microwave heating intermediate solidification high activity liquid waste, the firming body that utilizes this method to obtain is suitable for the temporary or transportation of radioactive liquid waste.Avoid the security risk of high activity liquid waste when storing or transport.
The present invention is achieved like this:
(1), utilize volume pump to send in the reaction vessel of microwave heating chamber with the high activity liquid waste in the high activity liquid waste holding tank.
(2) open microwave power supply, its microwave that sends is input to the microwave heating chamber, the high activity liquid waste in the reaction vessel is wherein heated.Regulate the power of microwave power supply, the temperature of control heating high activity liquid waste makes the high activity liquid waste evaporation, concentrates at 95-105 ℃, per hour remove the estimation of 0.5-1.0 kilogram moisture by every kilowatt of microwave power, select the concentrated time, after high activity liquid waste concentrated, temperature raise rapidly.
(3) power of adjusting microwave power supply, the temperature of control high activity liquid waste decompose the nitrate in the high activity liquid waste, i.e. denitration reaction at 190-450 ℃.The oxides of nitrogen gas NO that denitration produces xSend into device for absorbing tail gas, it is multiplexing that water absorbs the formation salpeter solution.
(4) after above-mentioned reaction vessel treats that the material of denitration is done admittedly, stop to import microwave, reaction vessel is sent into the swift electron stove, above-mentioned material is carried out calcination, calcination temperature is controlled at 700-800 ℃, calcination time 10-30 minute.
(5) after the cooling of the material of above-mentioned calcination, from reaction vessel, take out, send into the discharging packer's bay and pack, can obtain high activity liquid waste intermediate solidification body.
The salt content of above-mentioned high activity liquid waste is the 80-400 grams per liter, acidity the 0.5-5.5 molar nitric acid/liter.
Fig. 1 is a process flow diagram of the present invention.Among Fig. 1: 1 is the high activity liquid waste holding tank; 2 is volume pump; 3 are the microwave heating chamber; 4 is microwave power supply; 5 is the swift electron stove; 6 are the discharging packer's bay; 7 is device for absorbing tail gas, the microwave of A for sending from microwave power supply 4, and B is water and oxides of nitrogen gas, C is a high activity liquid waste intermediate solidification body.
Fig. 2 has provided microwave heating chamber 3 among Fig. 1, microwave power supply 4, the principle of operation figure of swift electron stove 5 and device for absorbing tail gas 7.Among Fig. 2: 8 waveguides; 9 circulators; 10 water loads; 11 infrared thermometers; 12 pumps; 13 air pumps; 14 travelling bogies; 15 feeding tubes; 16 reaction vessels; 17 is pallet.
In conjunction with Fig. 1, Fig. 2 specific descriptions are done in technological operation of the present invention:
The reactor 16 of high activity liquid waste and the fixed position that travelling bogie 14 is positioned at heating using microwave chamber 3 are housed, Reaction vessel 16 is placed on the pallet 17 of travelling bogie 14, and the high activity liquid waste in the high activity liquid waste collecting tank 1 utilizes Measuring pump 2 imports feeding tubes 15 and sends in the reaction vessel 16 in the heating using microwave chamber 3, opens microwave power supply 4, Microwave is by in the waveguide 8 input microwave heating chamber 3, to being positioned at the high activity liquid waste in the reaction vessel 16 wherein Heat, travelling bogie 14 can come and go operation at trapped orbit, and the pallet 17 on the travelling bogie 14 has certainly Moving whirligig can make the even absorbing microwave of material in the reaction vessel, and the microwave that feeds back after the load variations passes through circulation Device 9 usefulness loads 10 absorb in case stop loss bad microwave power supply. Measure temperature of charge with infrared radiation thermometer 11, regulate little The power of ripple power supply, control high activity liquid waste temperature make the high activity liquid waste evaporation and concentration at 95-105 ℃, at this moment high put useless The liquid surface boiling can not splash. The solution concentration process is per hour removed moisture 0.5-1.0 according to every kilowatt of microwave power Kilogram calculates, and can select to evaporate the required time of high activity liquid waste. After solution concentrates, regulate the power of microwave power supply 4, The fast rise of control high activity liquid waste temperature, in 190-450 ℃ of scope, the nitrate in the high activity liquid waste can decompose, Emit a large amount of oxides of nitrogen gas NOx These NOxWith air exhauster 13 suction device for absorbing tail gas 7, by pump 12 The recyclable nitric acid of shower water solution is multiplexing. Disengage NOxRear material is done solid immediately. Temperature also descends immediately. Stop this moment Only import microwave, by travelling bogie 14 reaction vessel 16 is sent into swift electron stove 5. Swift electron stove 5 adopts The tungsten filament heating of quartz ampoule protection, heating element heater is protected not by sour gas corrosion, and firing rate is 200-300 ℃/minute. A few minutes, the temperature of afterreaction container reached 700-800 ℃, can keep like this thing of microwave denitration product The reason characteristic. Calcination 10-30 minute, obtain loose porous cellular agglomerate height after the cooling and put material, hold with reaction Not phase adhesion of device is very easily taken out from reaction vessel, and material is followed travelling bogie 14 and entered discharging packer's bay 6 from unloading After the material packer's bay takes out, package, can obtain the oxide intermediate solidification body C of high activity liquid waste, namely be suitable for temporary transient Deposit and transport.
Advantage of the present invention provides a kind of solidifying much waster liquid based short-cut method. The block cured product of output is fit to In temporary or transportation. Face huge security risk when having avoided high activity liquid waste to deposit or transport. The present invention is suitable for the intermediate solidification of the different Acidic High-level Liquid Waste of various compositions, and technological operation is easy, and is needed Technology and equipment are that the unit of each generation high activity liquid waste can possess. Therefore the present invention has very big practicality Be worth.
Embodiment one
1 liter of reaction vessel useful volume
Simulated high-level radioactive waste is composition (salinity 320 grams per liters, the about 2 moles of HNO of acidity according to China typical case high activity liquid waste 3/ liter) configuration.Analog material liquid measures 0.5 lifting goes in the reaction vessel, under 99 ℃, concentrates 50-65 minute with 0.5-2.1 kilowatt of microwave heating, at 380 ℃ of following denitration 4-5 minutes, obtains 87 gram agglomerate solids.Water and nitric acid become gas to be collected at device for absorbing tail gas, and the agglomerate solid is sent into the swift electron stove 700 ℃ of following calcinations 10 minutes, obtains efficient waste liquid intermediate solidification body 77 grams.This firming body is the oxide of efficient waste liquid, and this is oxide porous loose, very easily takes out from reaction vessel, can keep in or transport after the packing.
Embodiment two
4.5 liters of reaction vessel volume
3 liters of simulated high-level radioactive wastes (forming with example one) are put into reaction vessel.Concentrate 3-4 hour with 2.1-4.2 kilowatt of microwave heating down at 105 ℃, at 400 ℃ of following denitration 10-20 minutes.Obtain 560 gram agglomerate solids.Again through the swift electron stove 750 ℃ of following calcinations 30 minutes, obtain the efficient waste liquid intermediate solidification body of 482 grams, this firming body is loose agglomerate, takes out the back packing from reactor, can keep in or transport.
Embodiment three
1.6 liters of reaction vessel volume
Selecting typical high activity liquid waste mainly to form 1 lifting of preparation analog material liquid (salt 115 grams per liters, acidity 5 mol) goes in the reaction vessel.
With 0.5-2.1 kilowatt of microwave heating, concentrate 60-90 minute down at 100 ℃, obtained 76 gram agglomerate solids at 450 ℃ of following denitration 5-10 minutes, obtained the efficient waste liquid intermediate solidification body of 62 grams through the swift electron stove in 20 minutes 800 ℃ of following calcinations again, this firming body is loose agglomerate, monoblock is taken out from container at an easy rate, is suitable for temporary after the packing or transportation.

Claims (2)

1. the method with microwave heating intermediate solidification high activity liquid waste is characterized in that
(1) utilize volume pump that the high activity liquid waste in the high activity liquid waste holding tank is sent in the indoor reaction vessel of microwave heating chamber;
(2) microwave that microwave power supply sent imports in the microwave heating chamber, and the high activity liquid waste in the reaction vessel is wherein heated;
(3) power of adjusting microwave power supply, with control high activity liquid waste heating-up temperature at 95-105 ℃, make the high activity liquid waste evaporation and concentration, regulate the power of microwave power supply again, with control high activity liquid waste heating-up temperature at 190-450 ℃, nitrate in the high activity liquid waste is decomposed, i.e. denitration reaction, the oxides of nitrogen gas NO that denitration produces x, it is multiplexing to send into device for absorbing tail gas water absorption formation salpeter solution;
(4) material for the treatment of denitration in the above-mentioned reaction vessel do solid after, stop to import microwave, reaction vessel is sent in the swift electron stove, carry out calcination to doing solid material, calcination temperature is controlled at 700-800 ℃, calcination 10-30 minute;
(5) after the cooling of the material after the above-mentioned calcination, from reaction vessel, take out and send into discharging packer's bay inner packing, can obtain high activity liquid waste intermediate solidification body.
2. in accordance with the method for claim 1, the salt content that it is characterized in that described high activity liquid waste is the 80-400 grams per liter, acidity the 0.5-5.5 molar nitric acid/liter between.
CN00124466A 2000-09-08 2000-09-08 Microwave heating process to solidify high radioactive waste liquid Expired - Fee Related CN1121045C (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102201271A (en) * 2011-03-30 2011-09-28 西北核技术研究所 System for processing radioactive wastes
CN102201272A (en) * 2011-03-30 2011-09-28 西北核技术研究所 Method for processing radioactive wastes
CN102436859A (en) * 2011-11-29 2012-05-02 清华大学 Transformation method for neodymium peracid solution
CN102522135A (en) * 2011-11-29 2012-06-27 清华大学 Method for transformation of zirconium base oxalic acid solution
CN102584018A (en) * 2012-03-15 2012-07-18 西南科技大学 Method for preparing high-radioactivity effluent glass-ceramic solidified body in microwave process

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102201271A (en) * 2011-03-30 2011-09-28 西北核技术研究所 System for processing radioactive wastes
CN102201272A (en) * 2011-03-30 2011-09-28 西北核技术研究所 Method for processing radioactive wastes
CN102201271B (en) * 2011-03-30 2013-10-30 西北核技术研究所 System for processing radioactive wastes
CN102436859A (en) * 2011-11-29 2012-05-02 清华大学 Transformation method for neodymium peracid solution
CN102522135A (en) * 2011-11-29 2012-06-27 清华大学 Method for transformation of zirconium base oxalic acid solution
CN102436859B (en) * 2011-11-29 2013-12-04 清华大学 Transformation method for neodymium peracid solution
CN102522135B (en) * 2011-11-29 2014-11-26 清华大学 Method for transformation of zirconium base oxalic acid solution
CN102584018A (en) * 2012-03-15 2012-07-18 西南科技大学 Method for preparing high-radioactivity effluent glass-ceramic solidified body in microwave process
CN102584018B (en) * 2012-03-15 2015-07-29 西南科技大学 A kind of method of preparing high-radioactivity effluent glass-ceramic solidified body in microwave process

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