CN106847358B - A kind of device and method of supercritical water oxidation processing Radioactive myocardial damage - Google Patents
A kind of device and method of supercritical water oxidation processing Radioactive myocardial damage Download PDFInfo
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- CN106847358B CN106847358B CN201710134047.0A CN201710134047A CN106847358B CN 106847358 B CN106847358 B CN 106847358B CN 201710134047 A CN201710134047 A CN 201710134047A CN 106847358 B CN106847358 B CN 106847358B
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/20—Disposal of liquid waste
- G21F9/22—Disposal of liquid waste by storage in a tank or other container
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Abstract
The invention discloses a kind of device and methods of supercritical water oxidation processing Radioactive myocardial damage, the device integrated high voltage liquid pump, high pressure gas pump, supercritical water oxidation kettle, heating system (tube furnace), check valve, counterbalance valve and hot operation glove box build up supercritical water oxidation apparatus, the oxidation to organic liquid waste is realized by the way of continuous operation, quickly and efficiently converts radioactive wastewater and carbon dioxide for Radioactive myocardial damage.Nowadays many Radioactive myocardial damages for needing to be handled in time, which are generally from, is related to core relevant unit, the liquid scintillation solution etc. generated in used oil, " tributyl phosphate (TBP)+diluent " in spentnuclear fuel last handling process and the nuclear medicine procedures for typically having nuclear power plant's house property raw.The present invention uses supercritical Water Oxidation Technology, and the organic liquid waste containing radionuclide is carried out exhaustive oxidation, is allowed to thoroughly be converted into carbon dioxide, water and inorganic salts.As common radioactive wastewater, processing is facilitated to dispose.
Description
Technical field
The present invention relates to the technical fields of Radioactive myocardial damage processing, and in particular to a kind of processing of supercritical water oxidation is put
The device and method of penetrating property organic liquid waste.
Background technique
It is so-called overcritical, refer to a kind of specialized fluids state of substance.When the substance increasing temperature and pressure for being in vapor liquid equilibrium
When, thermal expansion causes fluid density to reduce, and pressure rise increases density of gas phase, when temperature and pressure reaches certain point
When, the interface of gas-liquid two-phase disappears, and becomes homogeneous system, this point is exactly critical point.The critical point temperature of water is 647.3K
(374.1 DEG C), pressure 22.1MPa.The water of postcritical becomes supercritical water.In the supercritical state, water is physico
It learns property and huge variation has occurred, be not only different from the water of liquid, but also be different from gaseous water.It can by adjusting temperature and pressure
With it is very convenient, efficiently control chemical reaction.Organic matter dissolves in supercritical water, the very low oxygen of solubility in normal-temperature water
Gas, nitrogen, hydrogen, carbon dioxide etc. can also be miscible with it.Solubility and dissociation constant of the inorganic salts in supercritical water are very low.
In addition, the dielectric constant of supercritical water, ionic product, thermal capacitance, heat transfer coefficient etc. have apparent difference with gas and liquid two phases.
Supercritical water oxidation is using supercritical water as reaction medium come oxygenolysis organic matter, and process is similar to wet
Formula oxidation.In supercritical water, organic matter and oxidant can form homogeneous phase, overcome mass transfer between phases resistance, high temperature
High pressure improves the oxidation rate of organic matter again, by control condition, can be achieved within several seconds to a few minutes time organic
The thorough decomposition of object.Product is the small-molecule substances such as carbon dioxide, water, nitrogen and inorganic salts.When organic matter in waste liquid
When mass fraction is more than 2%, self-heating is can be realized in oxidation process.
The characteristics of SCWO technology: 1, homogeneous reaction.SCWO make to occur originally liquid phase or solid phase organic waste materials and gas phase it
Between multinomial reaction be converted into the homogeneous reaction in supercritical water.Therefore reaction rate is fast, and structure of reactor is simple, equipment
It is small in size.2, treatment effeciency is high.In SCWO environment, due to can be formed oxygen, hydrocarbon, aqueous systems homogeneous phase,
There is no resistance to mass tranfer, therefore oxidation efficiency is very high, the removal rate of most of organic matter is up to 99% or more.3, it will be unable to processing
Organic phase-change is water phase.Since reaction is carried out under enclosed environment, organic component is in temperature appropriate, pressure and certain stops
Staying can be fully oxidized as inorganic components such as carbon dioxide, water, nitrogen and phosphate radicals under time conditions.
Currently used SCWO equipment and its process are as shown in Figure 1.
It needs to use TBP+ extractant in spentnuclear fuel last handling process, radiolysis products can be accumulated with access times, to drop
Low extraction ability.Radiolysis products have to pass through washing removal, and TBP could be multiplexed.TBP+ diluent is after being repeatedly multiplexed, finally
Organic liquid waste is put in becoming.This waste liquid is mainly polluted by uranium, plutonium and fission product.The TBP+ that spentnuclear fuel last handling process generates
Diluent is the higher organic liquid waste of radioactive activity.The wet metallurgy course of uranium can also generate radioactive useless TBP+ diluent, but
The weak many of radioactivity.In addition to this, Radioactive myocardial damage further comprises lubricating oil in one loop of nuclear power station system, vacuum
Pump oil etc. can generate liquid scintillation solution in nuclear science research and other mix waste liquid.
The inflammability of Radioactive myocardial damage is allowed to be suitable for being handled using incineration method, and obtains very high volume reduction
Than.It is the oxide of various elements, carbon dioxide and water on the product theory of organic liquid waste completely burned.Burning disposal is extensive
For the mature technology of debirs processing, applied in many countries.Product carbon dioxide, water and ash content (phosphorus, sulphur and gold
Belong to oxide) it is all easy to incorporation immobilized base (such as cement) and the waste shape for being suitable for long term storage or disposition is made
State.The shortcomings that incineration method is equipment design processing difficulties, and maintenance cost is high, and safety and public reception are low.
In addition to burning, there are also acid digestion, wet oxidation method, electrochemical oxidation process, photochemical oxidation method, alkaline water solutions
Radioactive myocardial damage is handled with the methods of biodegrade.
For from the strict sense, SCWO is also one kind of wet oxidation, due to the special physico-chemical property of supercritical water, is
Organic matter and oxide provide homogeneous, fast reaction environment, so as to rapid, thorough oxidizable radioactive organic waste
Liquid, efficiency are very high.
Summary of the invention
It is organic that the present invention mainly emphasis handles used oil with radionuclide etc. using the method for supercritical water oxidation
Waste, for various defects existing for low-activity debirs in processing in the prior art, it is an object of the invention to use
New-type method handles these wastes, and to improve treatment effeciency (handling debirs template organic matter treatment effeciency at this stage can
To reach 99% or more), it prepares for its large scale processing debirs with radionuclide.
The technical solution adopted by the present invention are as follows: a kind of device of supercritical water oxidation processing Radioactive myocardial damage, including
Oxygen cylinder, glove box, the first high-pressure pump, tube furnace, heat exchanger, counterbalance valve, water storage container, the second high-pressure pump, gives up at high-pressure pump
Flow container and organic liquid waste container, wherein
Oxygen cylinder provides enough oxidation sources for entire supercritical water oxidation reduction process, and oxygen is injected whole by high-pressure pump
A system；
High-pressure pump is used for injection oxygen or air in entire stills for air blowing body；
Glove box provides closed environment, guarantees not to be leaked in environment when operator handles radioactive liquid waste；
First high-pressure pump is used to inject organic liquid waste into oxidation autoclave body；
Tube furnace provides heating and the temperature-controlling system of stills for air blowing, guarantees that stills for air blowing are run within the scope of set temperature；
Entire reaction system is discharged to reach predetermined temperature in treatment liquid after the cooling stills for air blowing of heat exchanger have reacted；
Counterbalance valve controls this reacting system pressure；
Water storage container is supplied to the second high-pressure pump abundance water source so that heat exchanger section exchanges heat and injects the water of reaction system
Source；
Water phase needed for second high-pressure pump is used in stills for air blowing body inject；
It is to be analyzed that waste liquid tank collects the liquid that is disposed；
Organic liquid waste container holds Radioactive myocardial damage using proprietary material.
Wherein, entire treatment process is entirely to complete in the glove box being relatively isolated from, and does not have any radioactive material
Matter leaks during the reaction.
Wherein, the second high-pressure pump takes full advantage of stills for air blowing oxidation processes during injecting water phase and comes out more than substance
Heat.
Wherein, counterbalance valve can control the high pressure that entire reaction system gets 25MPa, and the super of supercritical oxidation kettle is maintained to face
The normal operation of boundary's reaction.
Wherein, tube furnace heat supply can be up to 600 degrees Celsius, provide reliable guarantee for the temperature of supercritical reaction.
The present invention also provides a kind of methods of supercritical water oxidation processing Radioactive myocardial damage, using above-mentioned device,
The method steps are as follows:
Step 1. water phase is pumped into heat exchanger by the second high-pressure pump, enters in stills for air blowing after preheating, first
Organic liquid waste to be processed is pumped into stills for air blowing by high-pressure pump, and oxygen is pumped into stills for air blowing by high-pressure pump；
The reaction primary condition (being higher than super critical point) of the related oxidized kettle of experiment needed for step 2. is set；
Step 3. organic liquid waste carries out SCWO reaction in stills for air blowing；
The step 4. exhaust gas (CO of generation2) it is discharged into glove box, it filters, is discharged into factory owner's chimney after qualified；
The waste water that step 5. whole flow process generates is low-activity waste liquid, disposition or recycling.
The advantages of the present invention over the prior art are that:
(1), the present invention is compared compared to traditional process equipment, and apparatus structure is simple, and land occupation face is small, compact-sized, is conveniently answered
For mutually concerning core treatment plant；
(2), the final product for the debirs production that the present invention is handled is water and carbon dioxide, and it is useless not generate secondary pollution
Object；
(3), the present invention processing processing debirs ultrahigh in efficiency, many organic matter decomposition efficiencies can be up to 99% with
On.
Detailed description of the invention
Fig. 1 is SCWO equipment and its flow diagram in the prior art；
Fig. 2 is the schematic device that a kind of supercritical water oxidation of the present invention handles Radioactive myocardial damage, wherein 1 is oxygen
Gas cylinder, 2 be high-pressure pump, and 3 be glove box, and 4 be the first high-pressure pump, and 5 be tube furnace, and 6 be heat exchanger, and 7 be counterbalance valve, and 8 be storage
Water container, 9 be the second high-pressure pump, and 10 be waste liquid tank, and 11 be organic liquid waste container；
Fig. 3 is heat exchanger appearance schematic diagram.
Specific embodiment
With reference to the accompanying drawing and specific embodiment further illustrates the present invention.
It is as follows that radioactivity debirs key step is handled using supercritical water oxidation method:
Step (1) configures required oxygen source (hydrogen peroxide, high pure oxygen or O3Deng), meet corresponding oxidation of organic compounds process
In required oxygen quality fraction scale；
Step (2), to debirs carry out relevant treatment (meet high-pressure pump and normally inject situation), this step with specific reference to
The Different treatments meeting different from of processed material, but its final purpose is provided to that organic matter is allowed normally to inject；
Step (3), residence time t and relevant reactor volume according to needed for each reaction and oxygen quality point
Number ratio, calculates pump speed v under corresponding conditions；
Step (4) starts to adjust high pressure pump speed, is injected separately into oxygen and organic matter, and preheated device is preheating to specified temperature
Degree enters reaction response device (temperature T is at 400-600 degrees Celsius), and reactor core pressure is between 24-30Mpa；
Step (5), every kind of reactant have optimization treatment conditions, after being disposed, first cool down, and then pass through back
Pressure valve (counterbalance valve) decompression, finally reaches normal pressure；
Step (6) collects liquid and gas product analysis ingredient and removal efficiency respectively, is carried out with this to reaction further
Optimization processing.
The invention proposes a kind of by the way of supercritical oxidation, with radiation protection design, continuous operation, is suitable for
Carry out the radioactivity organic waste treatment device of the processing of Radioactive myocardial damage.Schematic diagram is equipped as shown in Fig. 2, the present invention one
The device of kind supercritical water oxidation processing Radioactive myocardial damage, including oxygen cylinder 1, high-pressure pump 2, glove box 3, the first high pressure
Pump 4, tube furnace 5, heat exchanger 6, counterbalance valve 7, water storage container 8, the second high-pressure pump 9, waste liquid tank 10 and organic liquid waste container 11,
In,
1. oxygen cylinder 1 connects 2 injection end of high-pressure pump by pipeline, the outlet of high-pressure pump 2 is connected to oxidation by pipeline
At kettle mixing mouth；
2. water storage container 8 connects 9 injection end of the second high-pressure pump by pipeline, the second high pressure pump outlet end is connected by pipeline
Heat exchanger 6 is taken away to have reacted liquid waste heat while having passed through pipeline and is connected at stills for air blowing mixing mouth；
3. oxygen cylinder 1, high-pressure pump 2, water storage container 8, the second high-pressure pump 9, waste liquid tank 10 are placed in outside glove box 3, and first
High-pressure pump 4, tube furnace 5, heat exchanger 6, counterbalance valve 7, organic liquid waste container 11 are placed in glove box 3；
4. organic liquid waste container 11 connects 4 inlet of the first high-pressure pump by pipeline, 4 outlet end of the first high-pressure pump is equally logical
Piping connection reaches at stills for air blowing mixing mouth；
5. being reacted completely under 5 heat effect of tube furnace after at stills for air blowing mixing mouth and connecting heat exchanger by pipeline again
Cooling facilitates discharge at 6, is then connected to liquid after counterbalance valve 7 depressurizes by pipeline and is collected into waste liquid tank 10, gas CO2
Self-discharged.
In addition, organic liquid waste container 11: being made of the dedicated material for holding radioactive substance, dedicated for holding radiation
Property substance.
Wherein, a) the first high-pressure pump 4, for organic liquid waste to be added into stills for air blowing.B) the second high-pressure pump 9, for past oxygen
Change kettle and the aqueous phase substances such as water or hydrogen peroxide are added.C) high-pressure pump 2, for air or oxygen to be added toward stills for air blowing.D) it aoxidizes
Kettle, organic liquid waste, water, the oxygen of addition are reacted wherein.It is processed into using corrosion resistant titanium or monel metal, it is resistance to
50MPa or more is pressed, pressure container standard is deferred in design, processing.E) electrically heated rod being conveniently replaceable or heat are assembled in tube furnace 5
Resistance can be heated to 500 DEG C or more, outsourcing thermal insulation material.F) counterbalance valve 7 control the pressure of oxidation system.G) liquid channel system,
Using corrosion resisting alloy pipe (pressure container standard is deferred in design, processing).H) radiation protecting systems, mainly sealing chamber, will
Stills for air blowing, the first high-pressure pump 4, counterbalance valve 7 are installed on glove box.
The characteristics of device of supercritical water oxidation processing Radioactive myocardial damage, also resides in:
1) the first high-pressure pump 4: for organic liquid waste to be added into stills for air blowing；
2) the second high-pressure pump 9: for the aqueous phase substances such as water or hydrogen peroxide to be added toward stills for air blowing；
3) high-pressure pump 2；For air or oxygen to be added toward stills for air blowing；
4) stills for air blowing: organic liquid waste, water, the oxygen of addition react wherein.Using corrosion resistant titanium or monel metal
It is processed into, pressure-resistant 50MPa or more；
5) counterbalance valve 7: the pressure of oxidation system is controlled；
6) liquid channel system: corrosion resisting alloy pipe is used；
7) radiation protecting systems: stills for air blowing, the first high-pressure pump 4, counterbalance valve 7 are installed on glove box by mainly glove box
It is interior；
8) tube furnace 5: heating rod is had, can be heated to 500 DEG C or more, outsourcing thermal insulation material.
The device application method that the supercritical water oxidation handles Radioactive myocardial damage is as follows:
1. heat exchanger is added in water by the second high-pressure pump 9, it is added in stills for air blowing after preheating, the first high-pressure pump 4 is by organic waste
Liquid is added in stills for air blowing, and oxygen is added in stills for air blowing high-pressure pump 2；
2. the condition of stills for air blowing is adjusted to the critical point of water or more, temperature is higher than 647.3K, and pressure is greater than 30MPa；
The reaction of 3.SCWO oxidizable radioactive organic liquid waste can occur in stills for air blowing；
4. exhaust gas (the CO of generation2) it is discharged into glove box, it filters, is discharged into factory owner's chimney after qualified；
5. the waste water that whole flow process generates is low-activity waste liquid, disposition or recycling.
Embodiment is described below:
A kind of device of supercritical water oxidation processing Radioactive myocardial damage, comprising:
1. stills for air blowing are processed into using Hastelloy, long 60cm, internal diameter Φ 5cm, outer diameter Φ 9cm.
2. 4 every power of outside weld are the electrical bar of 500W, outsourcing 2cm heat-insulated asbestos, then be made into thickness 1mm stainless steel
Sleeve seal.
3. liquid pump is high pressure liquid chromatograph pump, maximum stream flow 20mL/min, oxygen pump is hyperbaric oxygen air pump,
100mL/min, influidic pipe are Φ 8mm Hastelloy pipe.Fluid path between pump and stills for air blowing connects check valve.
4. heat exchanger is process for stainless steel, shape is as shown in figure 3, outer tube is Φ 16mm, inner tube Φ 8mm Hastelloy
Pipe, overall length 50cm, outer tube water pump, inner tube connect stills for air blowing.
5. pressure limiting valve is stainless steel digital display pressure limiting valve, range 50MPa.
6. glove box is standard glove box, check valve, organic phase feed pump, stills for air blowing, heat exchanger and the reasonable cloth of pressure limiting valve
It is placed in glove box.
7. water phase is added pump, oxygen pump, oxygen cylinder and is placed in outside glove box.
The supercritical water oxidation handles the device application method of Radioactive myocardial damage, includes the following steps:
1. the TBP/ kerosene that Radioactive myocardial damage is 30%, 99% industrial oxygen is oxidant, and deionized water is water
Phase.
2. stills for air blowing temperature setting is 750K, digital display pressure limiting valve pressure value is set in advance as 30MPa.
Deionized water, charging rate 5mL/min is added 3. starting water phase and pump being added.
4. after kettle temperature degree to be oxidized is reached for 750K, pump, oxygen 40mL/min (30MPa) is added in starting oxygen.Then open
It moves and organic is added to pump, charging rate 5mL/min.
After 5. reaction stops, with 500mL, 0.1mol/L dust technology flushing pipeline.
Experimental result
1. the TBP/ kerosene 2.7L of coprocessing 30%.
2. organic carbon presence is not detected in waste water using TOC analyzer, TBP- diluent destroys following to detection limit
(10-5mol/L)。
3. generating waste water about 5.2L.
4. can sufficiently prove that organic matter is completely decomposed into waste water and carbon dioxide by measurement TOC content.
Claims (1)
1. using the method for supercritical water oxidation processing Radioactive myocardial damage, it is characterised in that: this method comprises:
By the way of supercritical oxidation, with radiation protection design and continuous operation, this method utilizes overcritical this method
The device of water oxidation processes Radioactive myocardial damage includes oxygen cylinder (1), high-pressure pump (2), glove box (3), the first high-pressure pump
(4), tube furnace (5), heat exchanger (6), counterbalance valve (7), water storage container (8), the second high-pressure pump (9), waste liquid tank (10) and organic
Waste fluid container (11), wherein
Oxygen cylinder (1) connects high-pressure pump (2) injection end by pipeline, and high-pressure pump (2) outlet is connected to tubular type by pipeline
Furnace (5) mixes at mouth；
Water storage container (8) connects the second high-pressure pump (9) injection end by pipeline, and the second high pressure pump outlet end is changed by pipeline connection
Hot device (6) is taken away to have reacted liquid waste heat while having passed through pipeline and is connected at tube furnace (5) mixing mouth；
Oxygen cylinder (1), high-pressure pump (2), water storage container (8), the second high-pressure pump (9) and waste liquid tank (10) are placed in glove box (3)
Outside, the first high-pressure pump (4), tube furnace (5), heat exchanger (6), counterbalance valve (7) and organic liquid waste container (11) are placed in glove box (3)
It is interior；
Organic liquid waste container (11) connects the first high-pressure pump (4) inlet by pipeline, and the first high-pressure pump (4) outlet end is equally logical
Piping connection reaches at tube furnace (5) mixing mouth；
Oxygen gas and water and organic liquid waste react again logical under tube furnace (5) heat effect after at tube furnace (5) mixing mouth completely
Cooling facilitates discharge at piping connection heat exchanger (6), and liquid is collected after being then connected to counterbalance valve (7) decompression by pipeline
In to waste liquid tank (10), gas CO2Self-discharged；
The method and step that the supercritical water oxidation handles Radioactive myocardial damage is as follows:
1. heat exchanger is added in water by the second high-pressure pump (9), it is added in tube furnace (5) after preheating, the first high-pressure pump (4) is by organic waste
Liquid is added in tube furnace (5), and oxygen is added in tube furnace (5) high-pressure pump (2)；
2. the condition of tube furnace (5) is adjusted to the critical point of water or more, temperature is higher than 647.3K, and pressure is greater than 30MPa；
The reaction of 3.SCWO oxidizable radioactive organic liquid waste can occur in tube furnace (5)；
4. exhaust gas is discharged into glove box, filtering is discharged into factory owner's chimney after qualified；
5. the waste liquid that whole flow process generates is low-activity waste liquid, disposition or recycling.
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| CN107958716A (en) * | 2017-11-17 | 2018-04-24 | 深圳中广核工程设计有限公司 | Nuclear power plant's radioactivity organic waste treatment device and method |
| CN108511099B (en) * | 2018-03-23 | 2020-10-27 | 岭东核电有限公司 | Treatment method of radioactive waste oil of million kilowatt nuclear power plant |
| CN108447581A (en) * | 2018-04-23 | 2018-08-24 | 何辉 | A kind of Radioactive myocardial damage processing unit and its method |
| CN109036611B (en) * | 2018-06-30 | 2022-03-01 | 天津市德信成环保科技有限公司 | Method for treating nuclear power steam generator cleaning waste liquid and radioactive waste organic solvent |
| CN110272762B (en) * | 2019-07-11 | 2020-07-24 | 深圳大学 | CO (carbon monoxide)2Method for gasifying sludge by synergistic action with subcritical/supercritical water |
| CN113643837B (en) * | 2021-07-30 | 2024-07-23 | 四川固力铁环保工程有限责任公司 | Mineralization-oxidation treatment process for radioactive TBP/OK organic waste liquid |
| CN114596977B (en) * | 2022-03-15 | 2024-09-27 | 中国原子能科学研究院 | Pretreatment method for supercritical water oxidation TBP-kerosene organic solvent |
| CN114842995B (en) * | 2022-04-29 | 2024-09-10 | 西安交通大学 | Supercritical water oxidation treatment reactor for refractory radioactive organic waste |
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| JPH0470600A (en) * | 1990-07-11 | 1992-03-05 | Ngk Insulators Ltd | Extraction device for radioactive waste liquid including depositable solid and its washing method |
| CN100344386C (en) * | 1997-08-20 | 2007-10-24 | 株式会社东芝 | Waste processing method and waste processing apparatus |
| CN101182065A (en) * | 2007-11-09 | 2008-05-21 | 东华大学 | Method for treating high-concentration organic waste water in acroleic acid production |
| CN101830554B (en) * | 2010-05-18 | 2012-03-07 | 山东大学 | Method for improving oxygen utilization rate of supercritical water oxidation system |
| CN102849888A (en) * | 2012-10-11 | 2013-01-02 | 南京师范大学 | Zero-release organic wastewater treating device and zero-release organic wastewater treating method |
| JP2014228469A (en) * | 2013-05-24 | 2014-12-08 | 栗田工業株式会社 | Method for storing radioactive waste water and underground water storage tank |
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| CN106251924B (en) * | 2016-01-21 | 2019-01-11 | 青岛天和清原科技有限公司 | The method of supercritical water oxidation processing PVA polymeric material |
| CN106082426B (en) * | 2016-08-10 | 2019-03-22 | 广州中国科学院先进技术研究所 | With H2O2Supercritical water oxidation system and technique as oxidant |
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