CN108573762B - Method for in-situ treatment of strontium-containing radioactive waste liquid of nuclear power plant by using hydrotalcite prepared by electrochemistry - Google Patents
Method for in-situ treatment of strontium-containing radioactive waste liquid of nuclear power plant by using hydrotalcite prepared by electrochemistry Download PDFInfo
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- 239000007788 liquid Substances 0.000 title claims abstract description 56
- 238000000034 method Methods 0.000 title claims abstract description 45
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 title claims abstract description 38
- 229910001701 hydrotalcite Inorganic materials 0.000 title claims abstract description 38
- 229960001545 hydrotalcite Drugs 0.000 title claims abstract description 38
- 239000002901 radioactive waste Substances 0.000 title claims abstract description 26
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 18
- 229910052712 strontium Inorganic materials 0.000 title claims abstract description 17
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 title claims abstract description 17
- 230000005518 electrochemistry Effects 0.000 title description 5
- 239000000243 solution Substances 0.000 claims abstract description 29
- 238000006243 chemical reaction Methods 0.000 claims abstract description 25
- 239000011701 zinc Substances 0.000 claims abstract description 24
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 16
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 16
- 239000002699 waste material Substances 0.000 claims abstract description 15
- 238000000926 separation method Methods 0.000 claims abstract description 12
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 11
- 239000003792 electrolyte Substances 0.000 claims abstract description 11
- 230000002285 radioactive effect Effects 0.000 claims abstract description 10
- 239000002253 acid Substances 0.000 claims abstract description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 4
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 4
- 239000010439 graphite Substances 0.000 claims abstract description 4
- 238000000746 purification Methods 0.000 claims abstract description 3
- 239000012670 alkaline solution Substances 0.000 claims abstract 3
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 30
- 238000001556 precipitation Methods 0.000 claims description 19
- 239000011780 sodium chloride Substances 0.000 claims description 15
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- 239000011259 mixed solution Substances 0.000 claims description 6
- 239000002244 precipitate Substances 0.000 claims description 6
- 238000003756 stirring Methods 0.000 claims description 6
- 238000001914 filtration Methods 0.000 claims description 5
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 claims description 4
- 239000004327 boric acid Substances 0.000 claims description 4
- 238000004088 simulation Methods 0.000 claims description 4
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 3
- 230000035484 reaction time Effects 0.000 claims description 3
- 159000000008 strontium salts Chemical class 0.000 claims description 3
- 230000001105 regulatory effect Effects 0.000 claims description 2
- 125000002091 cationic group Chemical group 0.000 claims 1
- 230000009977 dual effect Effects 0.000 claims 1
- 238000002360 preparation method Methods 0.000 claims 1
- 230000003068 static effect Effects 0.000 claims 1
- 230000008569 process Effects 0.000 abstract description 16
- 229910021645 metal ion Inorganic materials 0.000 abstract description 8
- 229910001427 strontium ion Inorganic materials 0.000 abstract description 8
- 230000015572 biosynthetic process Effects 0.000 abstract description 5
- 239000002354 radioactive wastewater Substances 0.000 abstract description 5
- 238000003786 synthesis reaction Methods 0.000 abstract description 5
- 239000003463 adsorbent Substances 0.000 abstract description 2
- 239000000126 substance Substances 0.000 abstract description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 abstract 1
- 229910002651 NO3 Inorganic materials 0.000 abstract 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 abstract 1
- 239000000463 material Substances 0.000 abstract 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 22
- 230000000694 effects Effects 0.000 description 21
- 229910001868 water Inorganic materials 0.000 description 21
- 238000001179 sorption measurement Methods 0.000 description 15
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Inorganic materials [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 14
- 239000013049 sediment Substances 0.000 description 12
- 238000002474 experimental method Methods 0.000 description 9
- 239000002585 base Substances 0.000 description 7
- 229910052751 metal Inorganic materials 0.000 description 7
- 239000002184 metal Substances 0.000 description 7
- PWYYWQHXAPXYMF-UHFFFAOYSA-N strontium(2+) Chemical compound [Sr+2] PWYYWQHXAPXYMF-UHFFFAOYSA-N 0.000 description 7
- 238000002848 electrochemical method Methods 0.000 description 6
- 150000002500 ions Chemical class 0.000 description 6
- 239000002351 wastewater Substances 0.000 description 6
- 239000003513 alkali Substances 0.000 description 5
- 150000001875 compounds Chemical class 0.000 description 5
- 239000002925 low-level radioactive waste Substances 0.000 description 4
- 229910021502 aluminium hydroxide Inorganic materials 0.000 description 3
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 238000000975 co-precipitation Methods 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 230000018109 developmental process Effects 0.000 description 3
- 229910001679 gibbsite Inorganic materials 0.000 description 3
- 229910001385 heavy metal Inorganic materials 0.000 description 3
- 230000032683 aging Effects 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 238000009388 chemical precipitation Methods 0.000 description 2
- 238000009833 condensation Methods 0.000 description 2
- 230000005494 condensation Effects 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000013401 experimental design Methods 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 239000000941 radioactive substance Substances 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000004317 sodium nitrate Substances 0.000 description 2
- 235000010344 sodium nitrate Nutrition 0.000 description 2
- 229910001631 strontium chloride Inorganic materials 0.000 description 2
- AHBGXTDRMVNFER-UHFFFAOYSA-L strontium dichloride Chemical compound [Cl-].[Cl-].[Sr+2] AHBGXTDRMVNFER-UHFFFAOYSA-L 0.000 description 2
- 239000006228 supernatant Substances 0.000 description 2
- 230000002194 synthesizing effect Effects 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 229910021511 zinc hydroxide Inorganic materials 0.000 description 2
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 101100496858 Mus musculus Colec12 gene Proteins 0.000 description 1
- 229910052776 Thorium Inorganic materials 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- 229910052770 Uranium Inorganic materials 0.000 description 1
- 229910007570 Zn-Al Inorganic materials 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 238000005119 centrifugation Methods 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005485 electric heating Methods 0.000 description 1
- 238000003411 electrode reaction Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 238000005189 flocculation Methods 0.000 description 1
- 230000016615 flocculation Effects 0.000 description 1
- 238000005187 foaming Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- XLYOFNOQVPJJNP-ZSJDYOACSA-N heavy water Substances [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 description 1
- 239000002927 high level radioactive waste Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 230000006698 induction Effects 0.000 description 1
- 239000010857 liquid radioactive waste Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229910001426 radium ion Inorganic materials 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- UUCCCPNEFXQJEL-UHFFFAOYSA-L strontium dihydroxide Chemical compound [OH-].[OH-].[Sr+2] UUCCCPNEFXQJEL-UHFFFAOYSA-L 0.000 description 1
- 229910001866 strontium hydroxide Inorganic materials 0.000 description 1
- 239000011135 tin Substances 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- DNYWZCXLKNTFFI-UHFFFAOYSA-N uranium Chemical compound [U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U] DNYWZCXLKNTFFI-UHFFFAOYSA-N 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
- G21F9/20—Disposal of liquid waste
-
- 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
- G21F9/10—Processing by flocculation
-
- 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
Landscapes
- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Environmental & Geological Engineering (AREA)
- Electrolytic Production Of Metals (AREA)
- Water Treatment By Electricity Or Magnetism (AREA)
Abstract
本发明涉及电化学制备水滑石原位处理核电厂含锶放射性废液的方法，配制含有Sr2+的模拟放射性废水作为电解液，滴加碱溶液、酸溶液，调节pH至5～11，使用双电源进行电解，一组以铝片作为阳极，石墨作为阴极，直流稳压电源作为电源；一组以两片锌片分别作为阴阳两极，脉冲电源作为电源，并利用倒极变换阴阳极，在恒温条件下进行电解合成，反应结束后将电解液静置，过滤，进行固液分离，即完成对模拟废液的净化处理。本发明无需投加大量药剂或者吸附剂，只需控制废液中一定浓度的硝酸根与氯离子即可，无二次污染，且达到多种二价放射性金属离子的高效去除，本发明仅阐述对锶离子的去除，并实现固液高效分离，所需材料来源广泛，工艺简单且操作方便。The invention relates to a method for electrochemically preparing hydrotalcite for in-situ treatment of radioactive waste liquid containing strontium in a nuclear power plant. The simulated radioactive waste water containing Sr 2+ is prepared as an electrolyte, an alkaline solution and an acid solution are added dropwise, the pH is adjusted to 5-11, and the pH value is adjusted to 5-11. Double power supply for electrolysis, one group uses aluminum sheet as anode, graphite as cathode, DC stabilized power supply as power supply; one group uses two zinc sheets as cathode and anode, pulse power supply as power supply, and uses reverse pole to convert cathode and anode, Electrolytic synthesis is carried out under constant temperature conditions. After the reaction is completed, the electrolyte is allowed to stand, filtered, and solid-liquid separation is carried out, that is, the purification treatment of the simulated waste liquid is completed. The present invention does not need to add a large amount of chemicals or adsorbents, only needs to control a certain concentration of nitrate and chloride ions in the waste liquid, no secondary pollution, and achieves efficient removal of various divalent radioactive metal ions, the present invention only describes The removal of strontium ions and the realization of high-efficiency solid-liquid separation require a wide range of material sources, simple process and convenient operation.
Description
Technical Field
The invention belongs to the technical field of environmental protection, relates to a method for treating radioactive waste liquid of a nuclear power plant, and particularly relates to a method for in-situ treatment of strontium-containing radioactive waste liquid of the nuclear power plant by using hydrotalcite prepared by electrochemistry.
Background
The development of nuclear energy in the 50 th of the 20 th century turns to peaceful purpose, and with the continuous development of the utilization of nuclear energy technology, radioactive waste water continuously enters the environment and seriously threatens the environmental safety and human health, so that the research on how to safely, economically and effectively treat and treat nuclear waste has important significance.
In China, radioactive waste liquid is generally divided into three types according to the level of radioactivity, namely high-level radioactive waste liquid, medium-level radioactive waste liquid and low-level radioactive waste liquid, the harmfulness of the medium-low level radioactive waste liquid is relatively small, the medium-low level radioactive waste liquid can be attenuated to a safe level within hundreds of years, but the production amount is huge, and the treatment workload is heavy. From the development of nuclear energy technology to the present, the treatment method applied to medium and low-level radioactive waste liquid at the present stage generally comprises the following steps: chemical precipitation, ion exchange, evaporative concentration, adsorption, membrane separation, and the like. The chemical precipitation method has a common treatment effect, is not beneficial to solid-liquid separation of the strong radioactive wastewater, and has excessive factors influencing the final flocculation precipitation effect and solid-liquid separation in the reaction process; when the ion content in the waste liquid is high, the resin bed is easy to penetrate and lose efficacy, and needs to be replaced immediately; evaporative concentration methods are not suitable for treating waste water with volatile substances and foaming tendency; the heat energy consumption is large, and the operation cost is high; meanwhile, the problems of scaling, corrosion, explosion and the like need to be considered in the design and operation processes; the adsorption method utilizes porous adsorbent, so that the adsorption capacity is strong, and the price is low, so that the adsorption method is generally applied to the adsorption treatment of radioactive wastewater; the membrane separation method has high requirement on water quality and needs pretreatment. Therefore, the traditional single method has limitations in the aspect of radioactive waste liquid treatment, and more economic and effective treatment methods still need to be further researched.
Chinese patent CN102336461A discloses a method for removing heavy metal ions from an aqueous solution by using hydrotalcite. The method for removing metal ions from an aqueous solution using hydrotalcite according to the present invention includes the steps of removing metal ions from an aqueous solution using hydrotalcite; the metal ions are heavy metal ions or radioactive substance ions; the metal ions comprise one or more of mercury, chromium, lead, arsenic, cadmium, tin, copper and zinc heavy metal ions; the radioactive substance ions comprise uranium, thorium and radium ions. The method is characterized in that the hydrotalcite is synthesized in situ in the wastewater to be treated, and is not required to be separated and dried after synthesis and then added, and the operation can influence the adsorption activity of the hydrotalcite, thereby influencing the adsorption effect of the hydrotalcite on metal ions. Compared with a coprecipitation method, the electrochemical method for synthesizing the hydrotalcite has the advantages that the hydrotalcite is convenient, rapid and easy to synthesize, the electrochemical method does not need to be synthesized under the conditions of high temperature and high pressure, even can be synthesized under normal temperature and normal pressure, a metal salt solution with a certain proportion does not need to be prepared, metals needed by hydrotalcite synthesis all enter the solution through metal electrode electrolysis, a long-time ageing process is omitted, radioactive strontium elements in radioactive waste liquid of a nuclear power plant can be efficiently removed, the efficient solid-liquid separation of sediments can be realized, the process is simple, the operation is convenient, and secondary pollution is not easily caused.
Disclosure of Invention
The invention aims to overcome the defects in the prior art and provide a method for in-situ treatment of strontium-containing radioactive waste liquid in a nuclear power plant by using hydrotalcite prepared by electrochemistry.
The purpose of the invention can be realized by the following technical scheme:
the method for in-situ treatment of the strontium-containing radioactive waste liquid of the nuclear power plant by using the hydrotalcite prepared by the electrochemistry adopts the following steps:
(1) preparing radioactive simulation waste liquid of a nuclear power plant, adding electrolyte, boric acid and strontium salt, and uniformly stirring to prepare mixed liquid;
(2) adding an alkali solution or an acid solution into the mixed solution prepared in the step (1), adjusting the pH of the mixed solution to 5-11, and performing constant-temperature electrolysis by using double power supplies, wherein one of the double power supplies is aluminum sheet as an anode, graphite as a cathode and a direct-current stabilized power supply as a power supply; one zinc sheet is respectively used as a cathode and an anode, a pulse power supply is used as a power supply, the cathode and the anode are switched to electrolyze and synthesize hydrotalcite by utilizing the inverse pole, and after the reaction is finished, constant-temperature stirring treatment is carried out;
(3) and (3) standing, filtering and carrying out solid-liquid separation on the mixed solution electrolyzed in the step (2), so as to finish the purification treatment of the radioactive waste liquid of the nuclear power plant to be treated, and removing the obtained precipitate through standing and precipitation.
The radioactive element Sr in the radioactive simulation waste liquid of the nuclear power plant2+The concentration is 0-20 mg/L, B3+The concentration is 0 to 3000mg/L, and as a preferred embodiment, Sr is used2+The concentration is 5mg/L, B3+The concentration was 1000 mg/L.
The electrolyte in the step (1) comprises NaCl/or NaNO3The electrolyte is added into a nuclear power plant to be treatedThe concentration of the radioactive waste liquid is 0.05-0.2 mol/L, the preferable concentration is 0.05-0.1 mol/L, and the strontium salt used for preparing the radioactive simulation waste liquid is SrCl2。
The alkali solution in the step (2) is NaOH solution with the concentration of 1-5 mol/L, and the acid solution is HNO with the concentration of 1-2 mol/L3And (3) solution. The ratio of the current density of the zinc electrode to that of the aluminum electrode is 1:1 to 1:4, and the current density is controlled to be 30 to 135mA/cm2The reaction temperature is 30-70 ℃, the reaction time is 60-240 min, and the rotation speed is controlled to be 400-700 r/min.
In a preferred embodiment, sodium nitrate and sodium chloride are used as electrolytes, the concentration of the sodium nitrate is 0.1mol/L, the concentration of the sodium chloride is 0.05mol/L, and the current density is 45mA/cm in the aluminum electrode electrolysis current density in the constant-temperature electrolysis synthesis process2The reaction time is 240min, the reaction temperature is 40 ℃, the rotating speed is 500r/min, the initial pH is 11, and the electrode distance is 2cm (the distance between a zinc electrode and an aluminum electrode and a graphite electrode is 2 cm). When Sr is2+When the concentration of the inlet water is 5mg/L, Sr is in the outlet water2+The concentration was 43. mu.g/L.
And (3) adopting natural filtration of qualitative filter paper.
The invention adopts an electrochemical method to prepare Zn-Al hydrotalcite, and the essence of the method is to obtain Zn through electrolysis2+，Al3+And continuously generating OH at the cathode-Keeping the solution in a stable alkaline environment to form a good coprecipitation environment for Hydrotalcite, and dividing the coprecipitation process of Hydrotalcite Like Compounds (HTLCs) into reaction stages of precipitation, induced precipitation, recombination and crystallization condensation, wherein Al (OH) is added into the solution3Has smaller solubility product, the trivalent metal ions precipitate firstly, namely Al (OH) is generated firstly3The gel-like sediment is formed in the reaction kettle,
Al(H2O)6 3++3OH-→Al(OH)3↓+6H2O
due to its pair OH-Adsorption, enrichment, induction of divalent metal ions (Zn)2+) The precipitation of (a) is carried out,
Al(OH)3+Zn(H2O)6 2++2OH-→Al(OH)3·Zn(OH)2↓+6H2O
the pH value is higher than that of the single system Zn2+The pH value of the precipitate is greatly reduced, and when the pH value of the solution is increased to Zn2+In the case of precipitation of the desired basicity alone, a large amount of Zn (OH)2The precipitate is separated out,
Zn(H2O)6 2++2OH-→Zn(OH)2↓+6H2O
and for Sr that needs to be removed2+When the pH value is raised to the alkalinity required for the separate precipitation,
Sr(H2O)6 2++2OH-→Sr(OH)2↓+6H2O
the adjacent hydroxyl groups in the obtained composite product (mixed hydroxide) are further subjected to dehydration condensation,
Zn2+(OH)3·Al3+(OH)2→(HO)Zn2+-O-Al3+(OH)2+H2O
(HO)Zn2+-O-Al3+(OH)2+2Zn2+(OH)2→(HO)Zn2+-O-Al3+[-O-Zn2+(OH)]2+2H2O
(HO)Zn2+-O-Al3+[-O-Zn2+(OH)]2+3H2O→{(HO)Zn2+-OH-Al3+[-OH-Zn2+(OH)]2}3++3OH-
until all cation octahedral coordination groups form a tightly packed network structure by using common bridge type hydroxyl, and the cation octahedral coordination groups are added into radionuclide Sr2+Simultaneously electrolyze and feed Zn into the simulated waste liquid2+And Al3+With a radionuclide Sr2+Form a network structure to obtain Sr2+Embedded between hydrotalcite-like plates.
The hydrotalcite-like compound synthesized in situ by the electrochemical method has strong adsorption activity, can adjust reaction conditions, control the particle size of the hydrotalcite and other environment beneficial to adsorption, increase the specific surface area and improve the activity of the hydrotalcite-like compound on radionuclide Sr2+The adsorption reaction rate of (2). In addition, the synthesized hydrotalcite-like compound has the functions of ion exchange and adsorption at the same time, and can be used for treating Sr in radioactive wastewater2+The adsorption effect of the hydrotalcite has an enhancement effect, and after the reaction is finished, the hydrotalcite can be simply, quickly and effectively subjected to solid-liquid separation without centrifugation, filtration and other steps due to the very obvious self-precipitation effect, and the hydrotalcite after the adsorption is separated from a solution system and then is solidified or reused. The adsorption effect of the hydrotalcite can be completely applied to emergency treatment of high-level wastewater, medium-level wastewater and low-level wastewater, and the treated water quality basically reaches the level of direct discharge.
Meanwhile, the electrochemical method adopted by the invention generates the needed Zn by electrolyzing the metal anode2+，Al3+Controlling electrolysis conditions, completely meeting the metal proportion required by synthesizing the hydrotalcite, avoiding secondary pollution without adding metal salt, and obtaining the hydrotalcite with stronger activity for Sr in radioactive waste liquid2+And (4) removing.
Compared with the prior art, the method adopts the electrochemical method to synthesize the hydrotalcite-like compound in situ, does not need to add metal salt and strict addition steps in the traditional hydrotalcite synthesis process, omits a high-temperature long-time aging process, can even synthesize the hydrotalcite at normal temperature, can adsorb the strontium-containing waste liquid of the nuclear power plant to be treated in situ, has good precipitation effect, is extremely easy to separate solid from liquid, and can efficiently remove radioactive strontium elements in the radioactive waste liquid of the nuclear power plant. The invention can solve the problem of treatment of a large amount of medium-low level wastewater at present, can realize high-efficiency solid-liquid separation of sediments, and has the advantages of simple process, convenient operation and less possibility of causing secondary pollution.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the invention, but are not intended to limit the invention in any way. It should be noted that variations and modifications can be made by persons skilled in the art without departing from the spirit of the invention. All falling within the scope of the present invention.
Example 1:
the volume of the simulated waste liquid water sample is 500mL, the reaction temperature is controlled by a constant-temperature water bath, and the solution is mixed by electric stirring when dilute acid and alkali liquor are dripped to adjust the pH value.
The experimental steps are as follows:
1) mixing strontium chloride (SrCl)2) To prepare Sr2+Adding 50ml of solution with the concentration of 50mg/L into a 500ml volumetric flask to prepare Sr2+The simulated waste liquid with the concentration of about 5 mg/L;
2) weighing boric acid (H) in a metered amount3BO3) NaNO as electrolyte3Adding NaCl into a 500ml volumetric flask to ensure that the concentration of boric acid in the solution is 1000 mg/L; so that NaNO is present3The concentration is 0.05mol/L, and the NaCl concentration is 0.1 mol/L;
3) transferring 500ml of simulated waste liquid into a 600ml container, and adding 60g/L NaOH and 4mol/L HNO into an electric heating constant-temperature water tank at a certain temperature3Adjusting the pH value of the solution to an experimental design value;
4) selecting electrodes required by an experiment, weighing the mass, current density, electrode spacing and a power supply before electrode reaction, fixing the electrodes and connecting the power supply; adjusting the stirring speed to an experimental design value;
5) cooling and standing at room temperature after the reaction is finished until the supernatant is completely clear, filtering, performing solid-liquid separation, and taking the supernatant to determine Sr2+The concentration is weighed, the weight of the anode after the reaction is obtained, the dissolution amount of the anode is obtained, and the utilization rate is calculated;
6) the resulting precipitate was washed with deionized water and weighed after drying at 60 ℃ for 24 h.
Wherein the temperature of the constant temperature water bath is 40 deg.C, the initial pH of the solution adjusted by acid and alkali is 9, and the current density of the aluminum electrode DC power supply is 62.5mA/cm2The current density of the zinc electrode pulse power supply is 125mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 237 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 2:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base adjusted solution is 9, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode direct current power supply is 135mA/cm2Reaction time 120min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 669 μ g/L, the color of the sediment is white, and the precipitation effect is good.
Example 3:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base adjusted solution is 9, and the current density of the aluminum electrode direct current power supply is 135mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 120min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 344 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 4:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base regulated solution is 3, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 483 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 5:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: arranged in a thermostatic water bathThe temperature is 40 deg.C, the initial pH of the acid-base adjusted solution is 5, and the current density of the aluminum electrode DC power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 278 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 6:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base adjusted solution is 7, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 222 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 7:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base adjusted solution is 9, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 68 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 8:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 40 ℃, the initial pH of the acid-base adjusted solution is 11, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 43 mug/L, the color of the sediment is white, and the precipitation effect is good.
Example 9:
the experimental procedure is the same as that of example 1, and the adopted process parameters are different from those of example 1, specifically as follows: the temperature of the constant temperature water bath is 50 ℃, the initial pH of the solution adjusted by acid and alkali is 11, and the current density of the aluminum electrode direct current power supply is 45mA/cm2The current density of the zinc electrode pulse power supply is 135mA/cm2Reaction time 240min, NaNO3The concentration is 0.05mol/L, the NaCl concentration is 0.1mol/L, the rotating speed is 500r/min, and the electrode spacing is 2 cm.
The experimental results are as follows: sr2+The concentration is 115 mug/L, the color of the sediment is white, and the precipitation effect is good.
The foregoing description of specific embodiments of the present invention has been presented. It is to be understood that the present invention is not limited to the specific embodiments described above, and that various changes and modifications may be made by one skilled in the art within the scope of the appended claims without departing from the spirit of the invention.
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| CN110184636B (en) * | 2019-05-06 | 2021-04-16 | 浙江大学 | Method for preparing hydrotalcite film on aluminum surface in situ by multi-potential step method |
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