CN105006263B - A kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste - Google Patents
A kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste Download PDFInfo
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- CN105006263B CN105006263B CN201510347259.8A CN201510347259A CN105006263B CN 105006263 B CN105006263 B CN 105006263B CN 201510347259 A CN201510347259 A CN 201510347259A CN 105006263 B CN105006263 B CN 105006263B
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- 230000002285 radioactive effect Effects 0.000 title claims abstract description 86
- 239000010808 liquid waste Substances 0.000 title claims abstract description 52
- 238000000034 method Methods 0.000 title claims abstract description 41
- AMWRITDGCCNYAT-UHFFFAOYSA-L manganese oxide Inorganic materials [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 title claims abstract description 34
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 27
- 238000002360 preparation method Methods 0.000 title claims abstract description 22
- WAEMQWOKJMHJLA-UHFFFAOYSA-N Manganese(2+) Chemical compound [Mn+2] WAEMQWOKJMHJLA-UHFFFAOYSA-N 0.000 claims abstract description 44
- 150000002696 manganese Chemical class 0.000 claims abstract description 16
- 239000007788 liquid Substances 0.000 claims abstract description 15
- 238000000926 separation method Methods 0.000 claims abstract description 10
- 239000007787 solid Substances 0.000 claims abstract description 9
- 238000001914 filtration Methods 0.000 claims abstract description 8
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 110
- 238000005273 aeration Methods 0.000 claims description 68
- 239000011572 manganese Substances 0.000 claims description 39
- 238000006243 chemical reaction Methods 0.000 claims description 13
- 239000012528 membrane Substances 0.000 claims description 9
- 238000003828 vacuum filtration Methods 0.000 claims description 8
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 7
- 239000011565 manganese chloride Substances 0.000 claims description 7
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 5
- 229910000357 manganese(II) sulfate Inorganic materials 0.000 claims description 5
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(II) nitrate Inorganic materials [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 2
- 150000002500 ions Chemical class 0.000 abstract description 16
- 238000010521 absorption reaction Methods 0.000 abstract description 6
- 239000003513 alkali Substances 0.000 abstract description 5
- 238000000975 co-precipitation Methods 0.000 abstract description 3
- 229910052596 spinel Inorganic materials 0.000 abstract description 3
- 239000011029 spinel Substances 0.000 abstract description 3
- 239000000243 solution Substances 0.000 description 71
- XLJKHNWPARRRJB-UHFFFAOYSA-N cobalt(2+) Chemical compound [Co+2] XLJKHNWPARRRJB-UHFFFAOYSA-N 0.000 description 60
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 34
- 238000002474 experimental method Methods 0.000 description 28
- 229910001385 heavy metal Inorganic materials 0.000 description 4
- 239000000463 material Substances 0.000 description 3
- 229910001429 cobalt ion Inorganic materials 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000003672 processing method Methods 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 239000013049 sediment Substances 0.000 description 2
- 238000004062 sedimentation Methods 0.000 description 2
- 238000004088 simulation Methods 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- NWUYHJFMYQTDRP-UHFFFAOYSA-N 1,2-bis(ethenyl)benzene;1-ethenyl-2-ethylbenzene;styrene Chemical compound C=CC1=CC=CC=C1.CCC1=CC=CC=C1C=C.C=CC1=CC=CC=C1C=C NWUYHJFMYQTDRP-UHFFFAOYSA-N 0.000 description 1
- 229910021580 Cobalt(II) chloride Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 description 1
- 238000009388 chemical precipitation Methods 0.000 description 1
- 239000000701 coagulant Substances 0.000 description 1
- 238000009831 deintercalation Methods 0.000 description 1
- 235000013399 edible fruits Nutrition 0.000 description 1
- 238000005485 electric heating Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- -1 for example Substances 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 239000003456 ion exchange resin Substances 0.000 description 1
- 229920003303 ion-exchange polymer Polymers 0.000 description 1
- 229910001437 manganese ion Inorganic materials 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 230000005226 mechanical processes and functions Effects 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000010802 sludge Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
-
- 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
- G21F9/06—Processing
- G21F9/12—Processing by absorption; by adsorption; by ion-exchange
-
- 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
- G21F9/06—Processing
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- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Treatment Of Water By Oxidation Or Reduction (AREA)
Abstract
The present invention relates to a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, this method specifically includes following steps：(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；(2) aqueous slkali is added into mixed liquor, the pH of mixed liquor is adjusted to 8 13, then carries out constant temperature Air Exposure；(3) mixed liquor after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid.Compared with prior art, the present invention uses fabricated in situ mangano-manganic oxide method, plus during alkali, pending radioactive element ion and Mn2+Co-precipitation is formed, meanwhile, generated in-situ mangano-manganic oxide has strong absorption property, and pending radioactive element ion can replace Mn2+Into in the spinel structure lattice of mangano-manganic oxide, under the synergy for being co-precipitated and adsorbing, the radioactive element ion in nuclear power plant's radioactive liquid waste, non-secondary pollution can be efficiently removed.
Description
Technical field
The invention belongs to environmental technology field, it is related to a kind of method for handling nuclear power plant's radioactive liquid waste, more particularly, to
A kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste.
Background technology
With developing rapidly for nuclear industry, increasing radwaste is produced, and the processing of nuclear waste is also increasingly subject to
Concern.Therefore, system research simulation nuclear power plant radioactive liquid waste is very meaningful.
At present, processing contains Co both at home and abroad2+The method of radioactive liquid waste is commonly absorption method, ion-exchange, membrane separation process
Deng.However, the above method still suffers from many weak points, so as to influence Co2+The treatment effect of radioactive liquid waste, for example, chemical
The precipitation method are to remove impurities in water with coagulant sedimentation mostly, and the sludge quantity that this method is produced is big, and water outlet mostly can not be direct
Qualified discharge；Ion exchange resin price is higher, acid, alkali or salt etc. is needed during resin regeneration, operating cost is higher, regenerated liquid
Need further processing；And adsorb that requirement of the rule to sorbing material is higher, the surface area and adsorption capacity of sorbing material are big,
It is a difficult point to find a kind of suitable adsorbent；Evaporation process and membrane processing method power consumption are larger, but also need subsequent treatment.By
This is visible, and traditional single method has its limitation, cost-effective radioactive liquid waste in terms of radioactive liquid waste is handled
Processing method still need to further research.
In-situ preparation mangano-manganic oxide method be it is a kind of collect the method that is combined with absorption method of chemical precipitation, it be characterized in
Heavy metal co-precipitation occurs during in-situ preparation and the suction-operated of mangano-manganic oxide is generated through aerating oxidation.In-situ preparation four
Mn 3 O heavy metal ion has very strong affinity, and contents of many kinds of heavy metal ion can be removed simultaneously, with strong absorption property, treats
Heavy-metal ion removal can enter in mangano-manganic oxide lattice and be difficult to leach, and secondary pollution not resulted in, to reduce radioactivity
Material harm provides reference value.However, relevant in-situ preparation mangano-manganic oxide method is used to handle nuclear power plant's Spent Radioactive at present
The technical information of liquid is rarely reported.
The content of the invention
It is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide a kind of ion remaval efficiency
The method of the simple in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste of high and technique.
The purpose of the present invention can be achieved through the following technical solutions：
A kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, this method specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 8-13, then carry out perseverance
Warm Air Exposure；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
The radioactive element in pending nuclear power plant's radioactive liquid waste described in step (1) includes58Co、60Co、55Fe、59Fe、65Zn、51Cr or54One or more in Mn.
The concentration of the radioactive element in pending nuclear power plant's radioactive liquid waste described in step (1) is 0.01-20mg/L,
B3+Concentration is 0-3000mg/L.
Manganese salt described in step (1) includes MnCl2、Mn(NO3)2Or MnSO4In one kind.
In mixed liquor described in step (1), Mn2+Mol ratio with radioactive element is (1-40):1.
Aqueous slkali described in step (2) is NaOH solution, KOH solution or Ca (OH)2One kind in solution.
The molar concentration of described aqueous slkali is 1-2mol/L.
The condition of constant temperature Air Exposure described in step (2) is：Controlling reaction temperature is 20-70 DEG C, controls aeration time
For 30-300min, it is 0.2-5L/min to control air mass flow.
The condition of constant temperature Air Exposure described in step (2) is：Controlling reaction temperature is 60 DEG C, controls the aeration time to be
105min, it is 0.7L/min to control air mass flow.
The vacuum filtration being filtered into using 0.45 μm of filter membrane described in step (3).
In the present invention, described pending nuclear power plant's radioactive liquid waste contains the easy by mangano-manganic oxide knot of similar cobalt ions
The radioactive element of conjunction.
The inventive method is in actual mechanical process, and the optimal experiment condition of ion remaval efficiency is：Reaction time
105min, Mn2+/Co2+=25:1, the air mass flow 0.7L/min of aeration, 65 DEG C of reaction temperature, pH10.5.But consider sedimentation effect
Fruit and financial cost, it is determined that optimum condition is：Reaction time 105min, Mn2+/Co2+=15:1, the air mass flow of aeration
0.7L/min, 60 DEG C of reaction temperature, pH10.5, and Co in water outlet on this condition2+Concentration is 9.63ng/L, total Mn2+Concentration
47.06μg/L。
The in-situ preparation mangano-manganic oxide method that the present invention is used is fabricated in situ mangano-manganic oxide method, and its essence is exactly
By Mn2+Plus alkali generation Mn (OH)2, radioactive element and Mn occur for this process2+Co-precipitation, remove part radioactive element
Ion, then by aeration air oxidation, that is, generate mangano-manganic oxide.Mangano-manganic oxide has strong absorption property, Er Qiesi in itself
Mn 3 O structure is spinel structure, when the radius size and Mn of the radioactive element ion in nuclear power plant's radioactive liquid waste2+
When close, for example, cobalt ions etc., these radioactive element ions just can replace Mn2+And enter the spinelle knot of mangano-manganic oxide
In structure lattice, and the crystalline phase stablized, so as to remove a variety of radioactive elements in nuclear power plant's radioactive liquid waste.
Compared with prior art, the invention has the characteristics that：
Due to using fabricated in situ mangano-manganic oxide method, plus ion to be removed is co-precipitated with manganese ion formation during alkali.
In addition, generated in-situ mangano-manganic oxide has strong absorption property in itself, and pending radioactive element ion can be replaced
Mn2+Into in the spinel structure lattice of mangano-manganic oxide, it is difficult that radioactive element ion occurs again from mangano-manganic oxide lattice
Middle deintercalation and the phenomenon leached.Under the synergy for being co-precipitated and adsorbing, can efficiently it remove in nuclear power plant's radioactive liquid waste
Radioactive element ion, technique is simple, easy to operate, the advantages of not easily causing secondary pollution.
Embodiment
With reference to specific embodiment, the present invention is described in detail.
Embodiment 1：
Simulated waste volume of water sample is 500mL, and reaction temperature is by constant temperature water bath control, by electronic during dropwise addition alkali lye
Stirring carrys out mixed solution, and oxidation-adsorption process acts on agitating solution by aeration.
Experimental procedure is：By CoCL2 6H2O (CoCl2·6H2O) it is made into Co2+Concentration is 500mg/L solution, takes 10ml
It is added in 500ml volumetric flask, to configure Co2+Concentration is 10mg/L or so the simulation aqueous solution；Add boric acid (H3BO3)
2.8182g, makes B in solution3+Concentration is 1000mg/L；Then, by metered manganese salt MnCl2, stirring, it is molten to be made into raw water
Liquid；Retransfer in 1000mL four-hole boiling flasks, it is molten with 2mol/L NaOH regulations in the electric heating constant temperature water temperature groove of certain temperature
Liquid pH value (rate of addition about 30 drops/minute), then carries out period of aeration with certain air mass flow.It is quiet after reaction terminates
Put, then separation of solid and liquid is made by vacuum filtration, determine Co in liquid2+Ion and total Mn2+Concentration.
Wherein, the temperature that constant temperature water bath is set is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2 +Mol ratio is 20:1, the time of aeration is 30min, and the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 56.10, total Mn2+The μ g/L of concentration 271.01, sediment color is that brown is partially yellow.
Embodiment 2：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 60min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 44.73, total Mn2+The μ g/L of concentration 159.57, sediment color is brown.
Embodiment 3：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 90min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 29.10, total Mn2+The μ g/L of concentration 144.83, color is that brown is partially black.
Embodiment 4：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 14.21, total Mn2+The μ g/L of concentration 59.96, color is that brown is partially black.
Embodiment 5：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 150min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 14.18, total Mn2+The μ g/L of concentration 47.20, color is that brown is partially black.
Embodiment 6：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20：1, aeration when
Between be 300min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 11.46, total Mn2+The μ g/L of concentration 43.47, color is that brown is partially black.
Embodiment 7：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 1:1, the time of aeration
For 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 270.9, total Mn2+The μ g/L of concentration 128.05, color is that brown is partially yellow.
Embodiment 8：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 10:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 21.10, total Mn2+The μ g/L of concentration 61.08, color is brown.
Embodiment 9：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 30:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 13.41, total Mn2+The μ g/L of concentration 61.45, color is that brown is partially black.
Embodiment 10：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 40:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 12.79, total Mn2+The μ g/L of concentration 63.69, color is that brown is partially black
Embodiment 11：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 0.2L/min.
Experimental result is：Co2+The μ g/L of concentration 25.31, total Mn2+The μ g/L of concentration 309.20, color is brown.
Embodiment 12：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 0.4L/min.
Experimental result is：Co2+The μ g/L of concentration 15.05, total Mn2+The μ g/L of concentration 29.18, color is that brown is partially black.
Embodiment 13：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 0.7L/min.
Experimental result is：Co2+The μ g/L of concentration 14.07, total Mn2+The μ g/L of concentration 50.34, color is that brown is partially black.
Embodiment 14：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 2.1L/min.
Experimental result is：Co2+The μ g/L of concentration 14.98, total Mn2+The μ g/L of concentration 70.34, color is that brown is partially black.
Embodiment 15：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 2.5L/min.
Experimental result is：Co2+The μ g/L of concentration 28.66, total Mn2+The μ g/L of concentration 150.14, color is that brown is partially black.
Embodiment 16：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 20 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 382.50, total Mn2+The μ g/L of concentration 315.68, color is that brown is partially yellow.
Embodiment 17：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 30 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 258.20, total Mn2+The μ g/L of concentration 288.72, color is that brown is partially yellow.
Embodiment 18：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 40 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 27.73, total Mn2+The μ g/L of concentration 163.14, color is brown.
Embodiment 19：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 60 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 8.869, total Mn2+The μ g/L of concentration 58.06, color is that brown is partially black.
Embodiment 20：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 70 DEG C, and the pH through the NaOH solution adjusted is Mn in 9, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 6.507, total Mn2+The μ g/L of concentration 52.15, color is that brown is partially black.
Embodiment 21：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 8, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 68.53, total Mn2+The μ g/L of concentration 198.67, color is that brown is partially yellow.
Embodiment 22：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 10, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 2.669, total Mn2+The μ g/L of concentration 8.53, color is black.
Embodiment 23：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 11, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 33.22, total Mn2+The μ g/L of concentration 75.76, color is that black is partially brown.
Embodiment 24：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 50 DEG C, and the pH through the NaOH solution adjusted is Mn in 12, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 120min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+The μ g/L of concentration 48.99, total Mn2+The μ g/L of concentration 125.67, color is that black is partially yellow.
Embodiment 25：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 60 DEG C, and the pH through the NaOH solution adjusted is Mn in 10, solution2+/Co2+Mol ratio is 20:1, aeration when
Between be 90min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+Concentration 20.94ng/L, total Mn2+The μ g/L of concentration 21.99, color is black.
Embodiment 26：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 60 DEG C, and the pH through the NaOH solution adjusted is Mn in 10.5, solution2+/Co2+Mol ratio is 15:1, aeration
Time is 105min, and the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+Concentration 9.63ng/L, total Mn2+The μ g/L of concentration 47.16, color is black.
Embodiment 27：
Experimental procedure is same as Example 1, and the technological parameter of use is different from embodiment 1, specific as follows：Constant temperature water bath
The temperature of setting is 55 DEG C, and the pH through the NaOH solution adjusted is Mn in 10, solution2+/Co2+Mol ratio is 25:1, aeration when
Between be 105min, the air mass flow of aeration is 1.4L/min.
Experimental result is：Co2+Concentration 17.03ng/L, total Mn2+The μ g/L of concentration 36.89, color is black.
Embodiment 28：
The method of the present embodiment in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 13, then carry out constant temperature
Air Exposure；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
Wherein, in step (1), the radioactive element in pending nuclear power plant's radioactive liquid waste includes58Co、60Co、55Fe
And65Zn；The concentration of radioactive element is 20mg/L, B3+Concentration is 3000mg/L.
The manganese salt used is Mn (NO3)2, by Mn2+Mol ratio with radioactive element is 40:1, by Mn (NO3)2It is added to
In mixed liquor.
In step (2), aqueous slkali is KOH solution, and the molar concentration of the KOH solution is 1.5mol/L.
The condition of constant temperature Air Exposure is：Controlling reaction temperature is 70 DEG C, and it is 30min to control aeration time, controls air
Flow is 5L/min.
The vacuum filtration being filtered into using 0.45 μm of filter membrane in step (3).
Embodiment 29：
The method of the present embodiment in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 8, then carry out constant temperature exposure
Gas disposal；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
Wherein, in step (1), the radioactive element in pending nuclear power plant's radioactive liquid waste includes60Co、59Fe、65Zn
And54Mn；The concentration of radioactive element is 0.1mg/L, B3+Concentration is 0mg/L.
The manganese salt used is MnCl2, by Mn2+Mol ratio with radioactive element is 1:1, by MnCl2It is added to mixed liquor
In.
In step (2), aqueous slkali is Ca (OH)2Solution, the Ca (OH)2The molar concentration of solution is 1mol/L.
The condition of constant temperature Air Exposure is：Controlling reaction temperature is 20 DEG C, and it is 300min to control aeration time, controls air
Flow is 0.2L/min.
The vacuum filtration being filtered into using 0.45 μm of filter membrane in step (3).
Embodiment 30：
The method of the present embodiment in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 10.5, then carry out perseverance
Warm Air Exposure；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
Wherein, in step (1), the radioactive element in pending nuclear power plant's radioactive liquid waste includes58Co、65Zn and54Mn；
The concentration of radioactive element is 10mg/L, B3+Concentration is 1500mg/L.
The manganese salt used is MnSO4, by Mn2+Mol ratio with radioactive element is 15:1, by MnSO4It is added to mixed liquor
In.
In step (2), aqueous slkali is NaOH solution, and the molar concentration of the NaOH solution is 2mol/L.
The condition of constant temperature Air Exposure is：Controlling reaction temperature is 65 DEG C, and it is 120min to control aeration time, controls air
Flow is 0.6L/min.
The vacuum filtration being filtered into using 0.45 μm of filter membrane in step (3).
Embodiment 31：
The method of the present embodiment in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 10, then carry out constant temperature
Air Exposure；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
Wherein, in step (1), the radioactive element in pending nuclear power plant's radioactive liquid waste includes58Co、60Co and55Fe；
The concentration of radioactive element is 14mg/L, B3+Concentration is 1800mg/L.
The manganese salt used is MnCl2, by Mn2+Mol ratio with radioactive element is 25:1, by MnCl2It is added to mixed liquor
In.
In step (2), aqueous slkali is NaOH solution, and the molar concentration of the NaOH solution is 1.8mol/L.
The condition of constant temperature Air Exposure is：Controlling reaction temperature is 65 DEG C, and it is 105min to control aeration time, controls air
Flow is 0.7L/min.
The vacuum filtration being filtered into using 0.45 μm of filter membrane in step (3).
Embodiment 32：
The method of the present embodiment in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, specifically includes following step
Suddenly：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 10, then carry out constant temperature
Air Exposure；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completes to treat
Handle the purified treatment of nuclear power plant's radioactive liquid waste.
Wherein, in step (1), the radioactive element in pending nuclear power plant's radioactive liquid waste includes58Co、65Zn and51Cr；
The concentration of radioactive element is 0.01mg/L, B3+Concentration is 10mg/L.
The manganese salt used is Mn (NO3)2, by Mn2+Mol ratio with radioactive element is 20:1, by MnSO4It is added to mixing
In liquid.
In step (2), aqueous slkali is NaOH solution, and the molar concentration of the NaOH solution is 2mol/L.
The condition of constant temperature Air Exposure is：Controlling reaction temperature is 55 DEG C, and it is 240min to control aeration time, controls air
Flow is 1L/min.
The vacuum filtration being filtered into using 0.45 μm of filter membrane in step (3).
Claims (6)
1. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste, it is characterised in that this method is specific
Comprise the following steps：
(1) manganese salt is added in pending nuclear power plant's radioactive liquid waste, and stirred, be configured to mixed liquor；
(2) aqueous slkali is added into mixed liquor made from step (1), the pH of mixed liquor is adjusted to 8-13, then carry out constant temperature exposure
Gas disposal；
(3) mixed liquor of the step (2) after constant temperature Air Exposure is stood, filtering carries out separation of solid and liquid, that is, completed to pending
The purified treatment of nuclear power plant's radioactive liquid waste；
The radioactive element in pending nuclear power plant's radioactive liquid waste described in step (1) includes58Co、60Co、55Fe、59Fe、65Zn、51Cr or54One or more in Mn；
In mixed liquor described in step (1), Mn2+Mol ratio with radioactive element is (1-40):1；
Manganese salt described in step (1) includes MnCl2、Mn(NO3)2Or MnSO4In one kind；
The condition of constant temperature Air Exposure described in step (2) is：Controlling reaction temperature is 20-70 DEG C, and it is 30- to control aeration time
300min, it is 0.2-5L/min to control air mass flow.
2. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste according to claim 1, its
It is characterised by, the concentration of the radioactive element in pending nuclear power plant's radioactive liquid waste described in step (1) is 0.01-20mg/
L, B3+Concentration is 0-3000mg/L.
3. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste according to claim 1, its
It is characterised by, the aqueous slkali described in step (2) is NaOH solution, KOH solution or Ca (OH)2One kind in solution.
4. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste according to claim 3, its
It is characterised by, the molar concentration of described aqueous slkali is 1-2mol/L.
5. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste according to claim 1, its
It is characterised by, the condition of the constant temperature Air Exposure described in step (2) is：Controlling reaction temperature is 60 DEG C, controls the aeration time to be
105min, it is 0.7L/min to control air mass flow.
6. a kind of method of in-situ preparation mangano-manganic oxide processing nuclear power plant radioactive liquid waste according to claim 1, its
It is characterised by, the vacuum filtration being filtered into using 0.45 μm of filter membrane described in step (3).
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