WO2019192043A1 - 放射性废液处理方法及装置 - Google Patents

放射性废液处理方法及装置 Download PDF

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WO2019192043A1
WO2019192043A1 PCT/CN2018/085070 CN2018085070W WO2019192043A1 WO 2019192043 A1 WO2019192043 A1 WO 2019192043A1 CN 2018085070 W CN2018085070 W CN 2018085070W WO 2019192043 A1 WO2019192043 A1 WO 2019192043A1
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reverse osmosis
stage
liquid
radioactive waste
continuous electric
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English (en)
French (fr)
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赵璇
李福志
张猛
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Tsinghua University
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Tsinghua University
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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
    • G21F9/06—Processing
    • G21F9/12—Processing by absorption; by adsorption; by ion-exchange

Definitions

  • the present application relates to the technical field of radioactive waste liquid treatment, and in particular, to a method and a device for treating radioactive waste liquid.
  • the reverse osmosis treatment has the characteristics of good effluent quality, low energy consumption and strong adaptability.
  • the ion exchange has a good removal effect on the radionuclide in the form of ions in the waste liquid. , are common processing techniques.
  • the conventional reverse osmosis treatment and ion exchange combination process is: a reverse osmosis membrane device and an ion exchanger are combined in series, and the reverse osmosis membrane device separates the radioactive waste liquid into a purification liquid and a concentrated liquid, and the activity of the purification liquid is lower than that of the radioactive liquid.
  • the waste liquid and the concentrate have higher radioactivity than the radioactive waste liquid, and the purified liquid enters the ion exchanger for further purification treatment.
  • the concentrated liquid produced by the separation of the radioactive waste liquid needs to be solidified by the solidification process for treatment, and the volumetric capacity of the radioactive waste liquid in the solidified body is only about 20%, resulting in a large amount of secondary radioactive solid waste, and the treatment process is complicated; Since the concentration of the radionuclide in the purification liquid is lowered to a lower level, the utilization rate of the ion exchange resin is also lower, resulting in a larger amount of secondary radioactive solid waste.
  • a radioactive waste liquid processing method and apparatus which have a higher level of radioactive waste liquid purification, and can significantly reduce the amount of radioactive waste generated, thereby achieving a small quantification of radioactive waste.
  • a method for treating a radioactive waste liquid comprising: separating a radioactive waste liquid to obtain a first purification liquid and a concentrated liquid; and performing ion exchange treatment on the concentrated liquid to obtain a first a second purification liquid; wherein, the first purification liquid and the second purification liquid are discharged; or the second purification liquid is returned to the separation treatment process to discharge the first purification liquid; or, the second purification liquid is returned to the separation treatment In the process, the first purification liquid is discharged to the remaining second purification liquid.
  • the first purification liquid that meets or even exceeds the discharge standard is obtained by separating the radioactive waste liquid, and the radionuclide is substantially retained in the concentrated liquid, and the concentrated liquid has a higher concentration.
  • the concentration of the radionuclide, which is ion-exchanged can significantly improve the utilization efficiency of the ion exchange resin, thereby significantly reducing the amount of radioactive waste ion exchange resin. Since the method does not produce a radioactive concentrate, the curing process is eliminated, thereby further reducing the amount of radioactive waste generated.
  • a radioactive waste liquid processing apparatus comprising: a separation unit, an ion exchange unit, and a drainage unit, wherein a concentrate outlet of the separation unit is connected to an inlet of the ion exchange unit; The purification liquid outlet of the separation unit is connected to the drainage unit; the purification liquid outlet of the ion exchange unit is connected to the inlet of the drainage unit and/or the separation unit.
  • FIG. 1 is a schematic view showing a process flow of a method for treating a radioactive waste liquid provided by an embodiment of the present application.
  • Fig. 2 is a graph showing the relationship between the equilibrium adsorption amount Q of the ion exchange resin to the radionuclide oxime and the equilibrium concentration Ce of the radionuclide ruthenium in the solution.
  • FIG. 3 is a schematic diagram showing the process flow of a radioactive waste liquid processing apparatus provided by an embodiment of the present application.
  • FIG. 4 is a schematic view showing the process flow of a radioactive waste liquid processing apparatus according to another embodiment of the present application.
  • FIG. 5 is a schematic diagram showing the process flow of a radioactive waste liquid processing apparatus according to another embodiment of the present application.
  • FIG. 6 is a flow chart showing the process of a radioactive waste liquid processing apparatus provided by another embodiment of the present application.
  • FIG. 7 is a flow chart showing the process of a radioactive waste liquid processing apparatus provided by another embodiment of the present application.
  • 101 activated carbon filter
  • 102 inorganic adsorption column
  • 103 oil water separator
  • 104 security filter
  • 105 buffer water tank
  • 106 paper core filter
  • 107 self-cleaning filter
  • 108 ultrafilter
  • 201 buffer water tank
  • 202 security filter
  • 203 high pressure pump
  • 204 circulating pump
  • first-stage continuous electric desalination equipment 221, first-stage continuous electric desalination equipment; 222, second-stage continuous electric desalination equipment; 223, intermediate water tank; 224, activator tank;
  • Radioactive wastewater treatment is different from conventional wastewater treatment because: 1) the mass concentration of radionuclide ions in radioactive wastewater is extremely low, and the mass concentration of radionuclide ions is further reduced to achieve the environmental emission requirement of 10Bq. /L, which far exceeds the capacity of conventional wastewater treatment technology; 2) An important principle of radioactive wastewater treatment is the small quantification of radioactive waste; 3) the operability and maintainability of equipment under radioactive conditions need to be considered.
  • the embodiments of the present application provide a radioactive waste liquid treatment method and device, which have higher radioactive waste liquid purification level, and can significantly reduce the amount of radioactive waste generated, and realize small radioactive waste. Quantify.
  • concentration factor is calculated as (influent volume) / (volume of concentrate);
  • reverse osmosis recovery is calculated as (reverse osmosis total purified liquid production) / (reverse osmosis total water intake).
  • FIG. 1 is a schematic view showing a process flow of a method for treating a radioactive waste liquid provided by an embodiment of the present application, according to which:
  • the radioactive waste water is first separated and treated to obtain a first purified liquid and a concentrated liquid.
  • the concentration factor is more than 2 times, preferably 2 to 3 times, and the majority of the radioactive nuclides in the radioactive waste water are retained in the concentrate, so that the mass concentration of the radionuclide in the concentrate can reach the radioactivity in the radioactive waste liquid.
  • the mass concentration of radionuclides in the first purification liquid is less than twice the mass concentration of radionuclides, which is lower than the mass concentration of radionuclides in the radioactive waste water, which is even better than the emission standard (radioactivity is less than 10Bq/ L), discharge treatment.
  • the concentrate is subjected to ion exchange treatment to obtain a second purification liquid.
  • the radioactive concentrated waste liquid is not generated, the curing process is eliminated, and the amount of radioactive waste generated is reduced.
  • Fig. 2 the relationship between the equilibrium adsorption amount Q of the ion exchange resin to the radionuclide iridium and the equilibrium concentration Ce of the radionuclide iridium in the solution is shown, and it can be seen that the radionuclide is in solution.
  • the higher the equilibrium concentration Ce in the ion the higher the equilibrium adsorption amount Q of the ion exchange resin to the radionuclide.
  • the mass concentration of the radionuclide in the concentrated liquid can be more than twice the mass concentration of the radionuclide in the radioactive waste liquid, and the concentrated liquid has a high concentration of radionuclides, and ion exchange is performed.
  • the treatment can significantly improve the utilization efficiency of the ion exchange resin, thereby significantly reducing the amount of generation of the radioactive waste ion exchange resin, and achieving a small amount of radioactive waste.
  • the discharge treatment is performed.
  • the first purification liquid and the second purification liquid may be directly discharged, or the two may be mixed and discharged.
  • the second purification liquid is mixed with the first purification liquid and then discharged.
  • the separation treatment may adopt one or more of a nanofiltration process, a reverse osmosis process, and a continuous electric desalination process according to actual conditions such as the composition, content, and processing requirements of the radioactive waste water. Combination process.
  • the nanofiltration process has certain selectivity for ion separation, and has the advantages of low process osmotic pressure, low operating pressure, and energy saving, so that it is desirable to select a purification liquid.
  • Some ions are retained in nature, and the nanofiltration process can be used as a preferred process for the separation of radioactive wastewater.
  • the first-stage or two-stage reverse osmosis process may be used, but it is not limited thereto, and the three-stage, four-stage or more reverse osmosis process may be adopted according to actual conditions.
  • the radioactive waste liquid is subjected to a first-stage reverse osmosis process to obtain a first-stage reverse osmosis purification liquid and a first-stage reverse osmosis concentrate as the first purification liquid and the concentrated liquid, respectively.
  • the first-stage reverse osmosis process may employ one or two or more stages of reverse osmosis treatment.
  • the upper stage reverse osmosis treated intermediate concentrate is used as the next stage of reverse osmosis treatment. That is, the radioactive waste liquid is subjected to reverse osmosis treatment of two or more stages in sequence to obtain a concentrated liquid, and at the same time, the purified liquid is sent out from each section, and the purified liquid sent from all the sections is combined into a first-stage reverse osmosis concentrate.
  • the radioactive waste liquid is first sent to the first-stage reverse osmosis process to obtain the first-stage reverse osmosis purification liquid and the first-stage reverse osmosis concentrate, and then the first-stage reverse osmosis purification liquid is sent to the second stage.
  • the reverse osmosis process is processed to obtain a second-stage reverse osmosis purification liquid and a second-stage reverse osmosis concentrate.
  • the second-stage reverse osmosis concentrate is returned to the first-stage reverse osmosis process, and the first-stage reverse osmosis concentrate is used as the concentrate to be sent to the ion exchange treatment process;
  • the second-stage reverse osmosis purification liquid is less than 10 Bq/ L, in line with the requirements of the discharge standard, as the first purification liquid for discharge treatment.
  • the first-stage reverse osmosis process may adopt one or two or more stages of reverse osmosis treatment.
  • the intermediate concentrate produced by the reverse osmosis treatment of the previous stage is used as the next stage of reverse osmosis treatment.
  • the influent water, that is, the radioactive waste liquid is subjected to reverse osmosis treatment of two or more stages in sequence to obtain a concentrated liquid, and the purified liquid is sent out from each section, and the purified liquid sent from all the sections is merged into the first-stage reverse osmosis purification liquid.
  • the second-stage reverse osmosis process may employ one or two or more stages of reverse osmosis treatment.
  • the intermediate concentrate produced by the reverse osmosis treatment as the next stage is reversed.
  • the infiltrated influent, that is, the radioactive waste liquid is subjected to reverse osmosis treatment of two or more stages in sequence to obtain a second-stage reverse osmosis concentrate, and the purified liquid is sent from each section, and the purified liquid sent from all the sections is merged into the second stage.
  • Reverse osmosis purification solution may be reversed.
  • the first-stage reverse osmosis process and the second-stage reverse osmosis process all adopt three-stage reverse osmosis treatment to form a “two-stage three-stage” reverse osmosis process for separation of radioactive wastewater pairs, which has high purification. Capacity and concentration factor reduce the load on the ion exchange treatment process while increasing the reverse osmosis recovery rate.
  • the first-stage reverse osmosis purification liquid produced by the first-stage reverse osmosis process or the second-stage reverse osmosis purification liquid produced by the two-stage reverse osmosis process has a radioactivity of more than 10 Bq/L, or when pursuing the discharged purification liquid
  • the first-stage reverse osmosis purification liquid produced by the first-stage reverse osmosis process or the second-stage reverse osmosis purification liquid produced by the two-stage reverse osmosis process can be sent to the continuous electric desalination process. Further fine processing is performed.
  • the fine treatment may be a one-stage or two-stage continuous electric desalination process, but is not limited thereto, and a three-stage, four-stage or higher continuous electric desalination process may be adopted according to actual conditions.
  • the first-stage reverse osmosis purification liquid produced by the first-stage reverse osmosis process or the second-stage reverse osmosis purification liquid produced by the two-stage reverse osmosis process is subjected to a first-stage continuous electric desalination process for fine treatment to obtain the first Purification liquids often meet the requirements of emission standards, even reach the natural background level, and discharge treatment, resulting in the return of the first-stage continuous electric desalting concentrate to the first-stage reverse osmosis process or the first-stage reverse osmosis process. Infiltration process.
  • the activator may be added to the second-stage reverse osmosis purification liquid produced by the first-stage reverse osmosis process or the second-stage reverse osmosis purification liquid produced by the two-stage reverse osmosis process, and then sent.
  • the activator can be prepared from pure water having a resistivity of more than 0.5 M ⁇ cm and different kinds of inorganic salts, and the activator contains ions Ca 2+ , Na + , Sr 2+ , Zn 2+ , Mg 2+ , Fe 2 .
  • the type of anion is not limited, the concentration of the activator stock solution is related to the dosage, ensuring that the ion concentration in the radioactive waste water is as follows after the activator is added to the radioactive waste water and mixed uniformly: Ca 2+ 0.1 mg / L ⁇ 0.2 mg/L, Na + 0.2 mg/L to 0.3 mg/L, Sr 2+ 8 mg/L to 9 mg/L, Zn 2+ 18 mg/L to 20 mg/L, Mg 2+ 0.2 mg/L to 0.25 mg/ L, Fe 2+ 0.04 mg/L to 0.05 mg/L and K + 100 mg/L to 150 mg/L.
  • the first-stage reverse osmosis purification liquid produced by the first-stage reverse osmosis process or the second-stage reverse osmosis purification liquid produced by the two-stage reverse osmosis process is firstly sent to the first-stage continuous electric desalination process to obtain The first-stage continuous electric desalination purification liquid and the first-stage continuous electric demineralization concentrate, and then the first-stage continuous electric desalination purification liquid is sent to the second-stage continuous electric desalination process to obtain the second-stage continuous electric elimination
  • the first-stage continuous electric desalting concentrate and the second-stage continuous electric desalting concentrate return to the first-stage reverse osmosis process in the first-stage reverse osmosis process or the two-stage reverse
  • an activator may be added to the first-stage continuous electric desalination purification liquid, and then sent to a second-stage continuous electric desalination process for purification treatment.
  • the activator may be selected from an activator as described above.
  • the separation treatment process is not limited to adopting the above process, for example, it may be a continuous electric desalination process of more than one level; a nanofiltration-reverse osmosis combination process; a nanofiltration-continuous electric desalination combination process; The reverse osmosis-continuous electric desalination combination process and the like can be determined by those skilled in the art according to actual conditions.
  • the radioactive waste water is optionally pretreated before the radioactive waste water is separated, but this is not an essential process.
  • the selective adsorption characteristics of the inorganic adsorption are used to specifically adsorb the radionuclide which is easy to penetrate the ion exchange bed, thereby prolonging the use of the ion exchange resin.
  • the cycle further reduces the amount of radioactive waste ion exchange resin produced.
  • the activity of the specific radionuclide targeted by the inorganic adsorbent exceeds a preset threshold, such as the radioactivity of rhodium in the radioactive waste liquid, the radioactivity of rhodium or the total radioactivity of rhodium and ruthenium is higher than 10 4 Bq/L, at this time, the inorganic adsorbent needs to be replaced.
  • a preset threshold such as the radioactivity of rhodium in the radioactive waste liquid
  • the radioactivity of rhodium or the total radioactivity of rhodium and ruthenium is higher than 10 4 Bq/L
  • radioactive waste water may also contain impurities such as oils, organic matter, colloids and particulate matter. Most of these impurities are non-radioactive, but will be produced by processes such as inorganic adsorption, reverse osmosis and ion exchange. Influence, pretreatment to remove these impurities, can extend the life cycle of inorganic adsorbents, reverse osmosis membranes, ion exchange resins, reduce the replacement of inorganic adsorbents and ion exchange resins, and further reduce the amount of radioactive waste ion exchange resin and radioactive waste inorganic The amount of adsorbent produced.
  • impurities such as oils, organic matter, colloids and particulate matter. Most of these impurities are non-radioactive, but will be produced by processes such as inorganic adsorption, reverse osmosis and ion exchange. Influence, pretreatment to remove these impurities, can extend the life cycle of inorganic adsorbents, reverse o
  • activated carbon Due to its unique surface properties, activated carbon has good adsorption capacity for oils, organic matter, colloids, particulate matter and other impurities. Therefore, activated carbon can be used to remove these impurities, simplifying the pretreatment process equipment and processes. When the resistance of the activated carbon bed is too large or the filtrate does not meet the subsequent water inflow requirements (contamination index SDI ⁇ 2), the activated carbon needs to be replaced.
  • the embodiment of the present application further provides a radioactive waste liquid processing apparatus, which will be described in detail below with reference to FIGS. 3 to 7.
  • FIG. 3 is a schematic diagram showing the process flow of a radioactive waste liquid processing apparatus provided by an embodiment of the present application.
  • the apparatus includes a separation unit 200, an ion exchange unit 300, and a drainage unit 400, wherein the radioactive waste water supply is connected to the inlet of the separation unit 200, the concentrate outlet of the separation unit 200 is connected to the inlet of the ion exchange unit 300; and the separation unit 200 is purified.
  • the liquid outlet is connected to the drain unit 400; the purge liquid outlet of the ion exchange unit 300 is connected to the drain unit 400 and/or the inlet of the separation unit 200.
  • the drain unit 400 includes a first drain subunit and a second drain subunit (not shown), the purge liquid outlet of the separation unit 200 is connected to the first drain subunit, and the purge outlet of the ion exchange unit 300 Connected to the second drainage subunit, the first drainage subunit and the second drainage subunit may be in communication.
  • the first purification liquid and the second purification liquid may be directly discharged according to different requirements, or may be discharged after mixing the two;
  • the second purification liquid is mixed with the first purification liquid and meets the requirements of the discharge standard, the second purification liquid is mixed with the first purification liquid and discharged.
  • the drainage unit 400 may be only a drainage pipe, or may be connected to the production water tank 401 (shown in FIG. 6 and FIG. 7) on the drainage pipe, or other forms for discharging the purification liquid, which is not limited in the application.
  • the purification liquid outlet of the ion exchange unit 300 may also be connected to the inlet of the separation unit 200, and the second purification liquid may be returned in whole or in part as a part of the water entering the separation unit 200, which can reduce the concentration of the radionuclide in the water entering the separation unit 200. , thereby improving the decontamination effect of the whole device on the radionuclide.
  • the separation unit 200 includes one or a combination of two or more of a nanofiltration unit, a reverse osmosis subunit, a continuous electric desalting subunit.
  • the separation unit 200 includes a reverse osmosis subunit 210 (shown in FIG. 5), and the reverse osmosis subunit 210 employs a one-stage or two-stage reverse osmosis device, but is not limited thereto, and may also adopt three according to actual conditions. Grade, quadruple or more reverse osmosis equipment.
  • the reverse osmosis subunit 210 adopts a first stage reverse osmosis apparatus, and the concentrated liquid outlet of the reverse osmosis apparatus 213 It is connected to the inlet of the ion exchange unit 300.
  • the purification liquid sent from the reverse osmosis apparatus 213 has been lower than 10 Bq/L, which meets the requirements of the discharge standard, and can be discharged. At this time, the purification liquid outlet of the reverse osmosis apparatus 213 is connected to the drainage unit 400.
  • the concentrate outlet of the reverse osmosis apparatus 213 is divided into two branches via a pipe, one branch is connected to the inlet of the reverse osmosis apparatus 213, and the other branch is connected to the inlet of the ion exchange unit 300. This also reduces the discharge amount of the concentrate, reduces the load of the ion exchange unit 300, further improves the utilization of the ion exchange resin, and avoids energy waste and saves energy.
  • the reverse osmosis device 213 may employ one reverse osmosis membrane module or two or more reverse osmosis membrane modules in series.
  • the concentrate outlet of the previous reverse osmosis membrane module is next to the next
  • the inlet of the reverse osmosis membrane module is connected, that is, the intermediate concentrate produced by the last reverse osmosis membrane module is used as the inlet water of the next reverse osmosis membrane module, and the purification liquids sent from all the reverse osmosis membrane modules are merged into the purification liquid of the reverse osmosis apparatus 213.
  • the reverse osmosis subunit 210 employs a two-stage reverse osmosis apparatus, wherein the first stage reverse osmosis apparatus 211 and The second reverse osmosis device 212 is connected in two stages.
  • the purified liquid outlet of the first-stage reverse osmosis device 211 is connected to the inlet of the second-stage reverse osmosis device 212, and the concentrated liquid outlet of the second-stage reverse osmosis device 212 is
  • the inlet of the primary reverse osmosis apparatus 211 is connected, and the concentrate outlet of the first stage reverse osmosis apparatus 211 is connected to the inlet of the ion exchange unit 300.
  • the purified liquid sent from the second-stage reverse osmosis device 212 is often lower than 10 Bq/L, and meets the requirements of the discharge standard, and can be discharged.
  • the purified liquid outlet of the first-stage reverse osmosis device 212 is connected to the drain unit 400. .
  • the concentrate outlet of the first stage reverse osmosis apparatus 211 is divided into two branches via a pipeline, one branch is connected to the inlet of the first stage reverse osmosis apparatus 211, and the other branch is connected to the ion exchange unit.
  • the import of 300 is connected. This also reduces the discharge amount of the concentrate, reduces the load of the ion exchange unit 300, further improves the utilization of the ion exchange resin, and avoids energy waste and saves energy.
  • the first-stage reverse osmosis device 211 may adopt a reverse osmosis membrane module or two or more reverse osmosis membrane modules connected in series, and when more than two reverse osmosis membrane modules are used, the concentrate outlet of the previous reverse osmosis membrane module Connected to the inlet of the next reverse osmosis membrane module, the intermediate concentrate produced by the previous reverse osmosis membrane module is used as the inlet water of the next reverse osmosis membrane module, and the purification liquid sent from all the reverse osmosis membrane modules is merged into the first stage reverse osmosis. The cleaning liquid of the device 211.
  • the second stage reverse osmosis apparatus 212 may also employ a reverse osmosis membrane module or two or more reverse osmosis membrane modules in series, and similarly, when more than two reverse osmosis membrane modules are employed, the concentrate of the previous reverse osmosis membrane module
  • the outlet is connected to the inlet of the next reverse osmosis membrane module, that is, the intermediate concentrate produced by the previous reverse osmosis membrane module is used as the inlet water of the next reverse osmosis membrane module, and the purification liquids sent from all the reverse osmosis membrane modules are merged into the second stage.
  • the cleaning fluid of the infiltration device 212 may also employ a reverse osmosis membrane module or two or more reverse osmosis membrane modules in series, and similarly, when more than two reverse osmosis membrane modules are employed, the concentrate of the previous reverse osmosis membrane module The outlet is connected to the inlet of the next reverse osmosis membrane module, that is, the intermediate concentrate produced
  • the first-stage reverse osmosis device 211 and the second-stage reverse osmosis device 212 are all connected in series by a three-stage reverse osmosis membrane module to form a "two-stage three-stage" reverse osmosis unit for separation and treatment of radioactive waste water.
  • the high purification capacity and concentration factor reduce the load of the ion exchange unit 300 while increasing the reverse osmosis recovery rate.
  • a continuous electric desalting unit can be arranged downstream of the reverse osmosis subunit, and the first stage reverse osmosis purification liquid produced by the first stage reverse osmosis apparatus or the two-stage reverse osmosis process can be produced.
  • the second stage reverse osmosis purification liquid is sent to the continuous electric desalting subunit for further fine processing.
  • the fine treatment may be a one-stage or two-stage continuous electric desalination apparatus, but it is not limited thereto, and three-stage, four-stage or more-stage continuous electric desalination equipment may be used according to actual conditions.
  • the continuous electric desalination unit uses a two-stage continuous electric desalination apparatus
  • the first-stage continuous electric desalination apparatus 221 is connected in series with the second-stage continuous electric desalination apparatus 222, specifically , the purification liquid outlet of the reverse osmosis subunit, that is, the purification liquid outlet of the first-stage reverse osmosis equipment or the purification liquid outlet of the second-stage reverse osmosis equipment of the two-stage reverse osmosis equipment, and the inlet of the first-stage continuous electric desalination equipment 221 Connected, the purified liquid outlet of the first-stage continuous electric desalination device 221 is connected to the inlet of the second-stage continuous electric desalination device 222, and the purified liquid outlet of the second-stage continuous electric desalination device 222 is connected to the drain unit 400, first The concentrate outlet of the stage continuous electric desalination apparatus 221 and the concentrate outlet of the second stage continuous electric desal
  • the inlet of the reverse osmosis subunit 210 refers to the inlet of the reverse osmosis apparatus 213, and when the reverse osmosis subunit 210 employs a two-stage reverse osmosis apparatus, Referring to FIG. 7, the inlet of the reverse osmosis subunit 210 refers to the inlet of the first stage reverse osmosis apparatus 211.
  • an intermediate water tank may be connected between the reverse osmosis subunit and the continuous electric desalination unit.
  • the intermediate tank is connected to the activator tank.
  • an intermediate water tank can be connected between the first-stage continuous electric desalination device 221 and the second-stage continuous electric desalination device 222. 223, the intermediate water tank 223 is connected to the activator tank 224, and a dosing pump is provided to control the amount of the activator to be added, so that the purified liquid produced by the continuous electric desalting subunit treatment reaches the natural background level.
  • the ion exchange unit 300 includes a primary ion exchanger 301.
  • the ion exchangers 301 of two or more stages may be connected in series.
  • the pre-processing unit 100 may be provided upstream of the separation unit 200, but is not essential. If necessary, the pre-processing unit 100 may be one of a water separator, an activated carbon filter, an inorganic membrane filter, a security filter, a paper core filter, a self-cleaning filter, an ultrafilter, an inorganic adsorption column, or Several combinations.
  • the selective adsorption characteristics of the inorganic adsorption are used to specifically adsorb the radionuclide which is easy to penetrate the ion exchange bed, thereby prolonging the use of the ion exchange resin.
  • the cycle further reduces the amount of radioactive waste ion exchange resin produced.
  • any one of the radioactivity in the radioactive waste liquid, the radioactivity of the thorium, and the total radioactivity of the plutonium and thorium is 10 5 Bq/L or more, it is preferably passed through the inorganic adsorption column 102 (as shown in the figure). 5 to FIG. 7)
  • Pretreatment for removing ruthenium and/or ruthenium may be carried out using an inorganic adsorption column for ruthenium, an inorganic adsorption column for ruthenium or an inorganic adsorption column for ruthenium and osmium.
  • radioactive waste water may also contain impurities such as oils, organic matter, colloids, and particulate matter. Most of these impurities are non-radioactive, but will be inorganic adsorbents, reverse osmosis membranes, and ion exchange resins. When it is affected, pretreatment removes these impurities, which can extend the life cycle of inorganic adsorbents, reverse osmosis membranes, and ion exchange resins, reduce the replacement of inorganic adsorbents and ion exchange resins, and further reduce the amount and radioactivity of radioactive waste ion exchange resins. The amount of waste inorganic adsorbent produced.
  • activated carbon filter 101 Due to its unique surface properties, activated carbon has good adsorption capacity for oils, organic matter, colloids, particulate matter and other impurities. Therefore, activated carbon filter 101 (shown in Figures 5 and 6) can be used to remove these impurities and simplify pretreatment. Process equipment and processes.
  • the pretreatment unit 100 may employ an oil-water separator 103 and an inorganic adsorption column. 102.
  • the paper core filter 106, the self-cleaning filter 107, and the ultrafilter 108 are sequentially connected.
  • the oil-water separator 103 is used for removing oil impurities in the radioactive waste water, and reducing the influence of the oil impurities on the subsequent process;
  • the inorganic adsorption column 102 is for removing the radionuclide which is easy to penetrate the ion exchange bed, and prolonging the ion exchange resin. The use period reduces the amount of generation of the radioactive waste ion exchange resin;
  • a security filter 104 is disposed between the oil water separator 103 and the inorganic adsorption column 102 to remove particulate matter, and protect the inorganic adsorption column 102 from being blocked by adsorption.
  • the paper core filter 106 is used for removing particulate matter in the radioactive waste water, and the filter element containing the particulate matter is convenient for subsequent treatment and disposal; the self-cleaning filter 107 directly intercepts impurities in the radioactive waste water by using the filter screen, and further removes suspended matter and particulate matter.
  • the self-cleaning filter 107 is capable of automatically discharging sewage, improving intelligence, and making the process more efficient; the ultrafilter 108 is capable of deeply removing impurities, proteins, microorganisms, and macromolecular organic substances in a colloidal form in the radioactive waste water.
  • the pretreatment unit 100 can deeply remove impurities in the radioactive waste water, conform to the water inflow requirement of the subsequent process, greatly reduce the influence of impurities on the separation treatment process and the ion exchange process, and improve the separation unit 200 and the ion exchange unit 300. Operation cycle.
  • a buffer water tank 105 may be connected between the inorganic adsorption column 102 and the paper core filter 106 to buffer the radioactive waste water after the inorganic adsorption treatment.
  • the separation unit 200 may further include a buffer water tank 201 to buffer the radioactive waste water from the pretreatment unit 100.
  • a security filter 202 may be further coupled between the buffer tank 201 and the reverse osmosis subunit 210 for protecting the reverse osmosis apparatus of the subsequent process.
  • the apparatus also includes a suitable water supply pump 10, a circulation pump 204, and a high pressure pump 203, which may be various pumps commonly used in the art, such as a plunger pump, a centrifugal pump, and the like.
  • the above-mentioned radioactive waste water method can be implemented to achieve a high level of radioactive waste liquid purification, and at the same time, the amount of radioactive waste generated can be significantly reduced, and the radioactive waste can be quantified.
  • the concentrations of Cs + , Sr 2+ , and Co 2+ were measured by Thermocouple Thermo Scientific ICAP Q-type inductively coupled plasma-mass spectrometry (ICP-MS).
  • the concentration of oil was determined by Shimadzu OCT-1. Characterization was performed using a total organic carbon TOC analyzer.
  • the "decontamination factor” is calculated as (the activity of the influent water) / (the activity of the purified liquid).
  • the radioactive waste water treatment apparatus used in this embodiment employs the apparatus shown in Fig. 6.
  • the reverse osmosis apparatus 213 is a series of three reverse osmosis membrane modules, and each reverse osmosis membrane module is provided with a reverse osmosis membrane element Dow BW30-4040.
  • the equipment, components and materials used in the device are shown in the following table:
  • the radioactive waste water treated in this example is simulated radioactive waste water, which contains Cs+2000 ⁇ g/L, Co 2+ 875 ⁇ g/L, Sr 2+ 1230 ⁇ g/L, and surfactant 10 mg/L.
  • the designed treatment capacity of the radioactive waste water treatment device is 1 m 3 /h, and the ion exchange bed treatment rate is about 10 BV/h.
  • the above simulated radioactive wastewater was pretreated by activated carbon adsorption bed.
  • the concentration of surfactant in water was reduced to 0.98 mg/L, and the concentration of radionuclide ions was unchanged.
  • the concentration of Cs + in water was reduced to 0.08 ⁇ g/ L, substantially completely removes Cs + from the wastewater.
  • the operating pressure of the high pressure pump 203 is 1.5 MPa, the reverse osmosis recovery rate is 60%, the 3 m 3 /h concentrated water is returned to the reverse osmosis circulation treatment, and the 0.67 m 3 /h concentrated water enters the ion exchange bed for ion exchange treatment, and the ion exchange purification liquid is produced.
  • the water was 0.67 m 3 /h, and the ion exchange production water was all returned as a part of the reverse osmosis water, and the production of the reverse osmosis purification liquid reached 1 m 3 /h.
  • the rejection rates of the reverse osmosis device 213 for Cs + , Sr 2+ , and Co 2+ were 95%, 98%, and 98%, respectively.
  • the ion exchange bed has higher decontamination factors for the three radionuclide ions Cs + , Sr 2+ and Co 2+ , which are about 10 3 respectively, and Cs + and Sr 2+ in the ion exchange production water.
  • the Co 2+ concentrations were 0.71 ⁇ g/L, 1.30 ⁇ g/L, and 1.80 ⁇ g/L, respectively.
  • the ion exchange water is mixed with the simulated radioactive waste water and used as reverse osmosis water.
  • the concentrations of Cs + , Sr 2+ and Co 2+ are 299 ⁇ g/L, 525 ⁇ g/L and 739 ⁇ g/L, respectively.
  • the reverse osmosis purification liquid is the device.
  • the concentrations of Cs + , Sr 2+ and Co 2+ in the produced water were 28.5 ⁇ g/L, 20.6 ⁇ g/L and 28.9 ⁇ g/L, respectively.
  • the decontamination factors for Cs + , Sr 2+ and Co 2+ were installed. Reached 17, 42, 43 respectively.
  • the decontamination factors of Cs + , Sr 2+ and Co 2+ are continuously reduced in the ion exchange bed.
  • the ion exchange bed decontaminates Cs + , Sr 2+ and Co 2+ .
  • the factors were 1.8, 2.1 and 2.0, respectively.
  • the concentrations of Cs + , Sr 2+ and Co 2+ in ion exchange water were 821 ⁇ g/L, 1252 ⁇ g/L and 1604 ⁇ g/L, respectively.
  • the 2+ concentrations were 59.8 ⁇ g/L, 40.2 ⁇ g/L and 54.1 ⁇ g/L, respectively.
  • the decontamination factors of Cs + , Sr 2+ and Co 2+ were 8, 22 and 23 respectively.
  • the simulated radioactive waste water is directly purified by the ion exchange bed after being pretreated by the activated carbon adsorption bed and the ruthenium adsorption bed. After 400 hours of operation, the device goes to the total of Cs + , Sr 2+ and Co 2+ .
  • the pollution factor is only about 2, respectively. It can be seen that, after the separation treatment is used to concentrate the radioactive waste water, the ion exchange treatment of the concentrated liquid can greatly improve the decontamination factor of the radionuclide, prolong the service life of the ion exchange bed, and greatly reduce the amount of radioactive solid waste. .
  • the activated carbon adsorption process may not be provided.
  • the helium adsorption process may not be provided.

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Abstract

一种放射性废液处理方法,该方法包括：将放射性废液进行分离处理，得到第一净化液和浓缩液；将所述浓缩液进行离子交换处理，得到第二净化液；其中，将所述第一净化液与所述第二净化液排放处理；或者，将所述第二净化液返回所述分离处理工序，将所述第一净化液排放处理；或者，将部分所述第二净化液返回所述分离处理工序，将所述第一净化液与其余部分所述第二净化液排放处理。一种利用上述方法处理放射性废液的装置。所述放射性废液处理方法及装置，具有更高的放射性废液净化水平，同时能够显著降低放射性废物的产生量，实现放射性废物的小量化。

Description

放射性废液处理方法及装置
相关申请的交叉引用
本申请要求享有于2018年04月03日提交的名称为“放射性废液处理方法及装置”的中国专利申请201810290186.7的优先权，该申请的全部内容通过引用并入本文中。
技术领域
本申请涉及放射性废液处理技术领域，尤其涉及一种放射性废液处理方法及装置。
背景技术
对于核工业领域产生的放射性废液，反渗透处理因具有出水水质好、能耗低、适应性强等特点，离子交换因对废液中以离子形态存在的放射性核素具有很好的去除效果，均为常用的处理工艺。
因放射性废液中放射性成分复杂且含量很低，为了适应对核工业建设中环境辐射防护提出的越来越高的要求，目前对放射性废液多采用组合式处理工艺。常规的反渗透处理和离子交换的组合工艺形式是：反渗透膜设备和离子交换器串联组合，反渗透膜设备将放射性废液分离为净化液和浓缩液，净化液的放射性活度低于放射性废液，浓缩液的放射性活度高于放射性废液，净化液进入离子交换器进行进一步的净化处理。其中，放射性废液分离产生的浓缩液需要利用固化工艺形成固化体进行处理，固化体中放射性废液的体积包容量仅为20％左右，导致产生大量二次放射性固体废物，且处理工艺复杂；而由于净化液中放射性核素的浓度降为更低水平，使得离子交换树脂的利用率也更低，从而导致二次放射性固体废物的产生量更大。
因此，需要一种新的放射性废液处理方法及装置，使放射性废物小量 化。
发明内容
根据本申请的实施例，提供了一种放射性废液处理方法及装置，具有更高的放射性废液净化水平，同时能够显著降低放射性废物的产生量，实现放射性废物的小量化。
根据本申请实施例的一个方面，提供了一种放射性废液处理方法，该方法包括：将放射性废液进行分离处理，得到第一净化液和浓缩液；将浓缩液进行离子交换处理，得到第二净化液；其中，将第一净化液与第二净化液排放处理；或者，将第二净化液返回分离处理工序，将第一净化液排放处理；或者，将部分第二净化液返回分离处理工序，将第一净化液与其余部分第二净化液排放处理。
根据本申请实施例的放射性废液处理方法，通过对放射性废液进行分离处理，得到符合甚至优于排放标准的第一净化液，将放射性核素基本保留在浓缩液中，浓缩液具有较高的放射性核素浓度，将其进行离子交换处理，能够明显提高离子交换树脂的利用效率，从而显著减少放射性废离子交换树脂的产生量。因为该方法不产生放射性浓缩液，省去了固化工艺，从而进一步降低放射性废物的产生量。
根据本申请实施例的另一个方面，还提供了一种放射性废液处理装置，该装置包括分离单元、离子交换单元和排水单元，其中，分离单元的浓缩液出口与离子交换单元的进口相连；分离单元的净化液出口连接至排水单元；离子交换单元的净化液出口连接至排水单元和/或分离单元的进口。
附图说明
为了更清楚地说明本申请实施例的技术方案，下面将对本申请实施例中所需要使用的附图作简单地介绍，对于本领域普通技术人员来讲，在不付出创造性劳动的前提下，还可以根据这些附图获得其他的附图。
图1示出了本申请一个实施例提供的放射性废液处理方法工艺流程示意图。
图2示出了离子交换树脂对放射性核素铯的平衡吸附量Q与放射性核素铯在溶液中的平衡浓度Ce之间的关系图。
图3示出了本申请一个实施例提供的放射性废液处理装置工艺流程示意图。
图4示出了本申请另一个实施例提供的放射性废液处理装置工艺流程示意图。
图5示出了本申请另一个实施例提供的放射性废液处理装置工艺流程示意图。
图6示出了本申请另一个实施例提供的放射性废液处理装置工艺流程图。
图7示出了本申请另一个实施例提供的放射性废液处理装置工艺流程图。
标号说明：
10，供水泵；
100，预处理单元；
101，活性炭过滤器；102，无机吸附柱；103，油水分离器；104，保安过滤器；105，缓存水箱；106，纸芯过滤器；107，自清洗过滤器；108，超滤器；
200，分离单元；
201，缓冲水箱；202，保安过滤器；203，高压泵；204，循环泵；
210，反渗透子单元；
211，第一级反渗透设备；212，第二级反渗透设备；213，反渗透设备；
221，第一级连续电除盐设备；222，第二级连续电除盐设备；223，中间水箱；224，活化剂箱；
300，离子交换单元；
301，离子交换器；
400，排水单元；
401，产水箱。
具体实施方式
下面将详细描述本申请的各个方面的特征和示例性实施例，为了使本申请的目的、技术方案及优点更加清楚明白，以下结合附图及实施例，对本申请进行进一步详细描述。应理解，此处所描述的具体实施例仅被配置为解释本申请，并不被配置为限定本申请。对于本领域技术人员来说，本申请可以在不需要这些具体细节中的一些细节的情况下实施。下面对实施例的描述仅仅是为了通过示出本申请的示例来提供对本申请更好的理解。
需要说明的是，在本文中，诸如第一和第二等之类的关系术语仅仅用来将一个实体或者操作与另一个实体或操作区分开来，而不一定要求或者暗示这些实体或操作之间存在任何这种实际的关系或者顺序。而且，术语“包括”、“包含”或者其任何其他变体意在涵盖非排他性的包含，从而使得包括一系列要素的过程、方法、物品或者设备不仅包括那些要素，而且还包括没有明确列出的其他要素，或者是还包括为这种过程、方法、物品或者设备所固有的要素。在没有更多限制的情况下，由语句“包括……”限定的要素，并不排除在包括所述要素的过程、方法、物品或者设备中还存在另外的相同要素。
放射性废水处理不同于常规的废水处理，这是因为：1)放射性废水中放射性核素离子的质量浓度极低，而进一步降低放射性核素离子的质量浓度，以达到环境排放要求的放射性活度10Bq/L，这远远超出了常规废水处理技术的能力；2)放射性废水处理的一个重要原则就是，放射性废物小量化；3)需要考虑放射性条件下设备的可操作性和可维护性。
基于放射性废水处理的以上特殊要求，本申请实施例提供了一种放射性废液处理方法及装置，具有更高的放射性废液净化水平，同时能够显著降低放射性废物的产生量，实现放射性废物的小量化。
在本文中，“浓缩倍数”按(进水体积)/(浓缩液的体积)计算；“反渗透回收率”按(反渗透的总净化液产量)/(反渗透的总进水量)计 算。
图1示出了本申请一个实施例提供的放射性废液处理方法工艺流程示意图，根据该方法：
首先将放射性废水进行分离处理，得到第一净化液和浓缩液。其中，浓缩倍数为2倍以上，优选为2～3倍，放射性废水中的放射性核素绝大多数被保留在浓缩液中，可以使浓缩液中放射性核素的质量浓度达到放射性废液中放射性核素的质量浓度的2倍以上，第一净化液中放射性核素的质量浓度则低于放射性废水中放射性核素的质量浓度，达到甚至优于排放标准的要求(放射性活度低于10Bq/L)，进行排放处理。
进一步地，将浓缩液进行离子交换处理，得到第二净化液。这样一方面由于不会产生放射性浓缩废液，从而省去了固化工艺，降低放射性废物的产生量。另一方面，如图2示出了离子交换树脂对放射性核素铯的平衡吸附量Q与放射性核素铯在溶液中的平衡浓度Ce之间的关系图，可以看出，放射性核素在溶液中的平衡浓度Ce越高，离子交换树脂对放射性核素的平衡吸附量Q越高。由于在上述分离处理工序中，浓缩液中放射性核素的质量浓度可以达到放射性废液中放射性核素的质量浓度的2倍以上，浓缩液具有较高的放射性核素浓度，将其进行离子交换处理，能够明显提高离子交换树脂的利用效率，从而显著减少放射性废离子交换树脂的产生量，实现放射性废物的小量化。
经检测第二净化液的放射性活度符合排放标准的要求，则进行排放处理，此时，可以将第一净化液和第二净化液分别直接排放，也可以是将两者混合后排放。经检测第二净化液与第一净化液混合后符合排放标准的要求，则将第二净化液与第一净化液混合后进行排放处理。
还可以将第二净化液全部或部分返回作为分离处理工序进水的一部分，这样能够降低分离处理工序进水的放射性核素浓度，进而提高整套工艺方法对放射性核素的去污效果。
根据本申请的一些实施例，分离处理可以根据放射性废水的组分、含量、及处理要求等实际情况，采用纳滤工艺、反渗透工艺、连续电除盐工艺中的一种或两种以上的组合工艺。
尽管纳滤工艺的分离性能低于反渗透工艺，但是纳滤工艺对离子的分离具有一定的选择性，还具有过程渗透压低、操作压力低、省能等优点，因此当希望净化液中能够选择性地保留一些离子，纳滤工艺可以作为优选工艺进行放射性废水的分离处理。
当分离处理工序采用反渗透工艺时，可以采用一级或两级反渗透工艺处理，但并不限于此，还可以根据实际情况采用三级、四级或更多级反渗透工艺。
作为一个示例，将放射性废液经过一级反渗透工艺处理，得到一级反渗透净化液和一级反渗透浓缩液分别作为第一净化液和浓缩液。
可选地，一级反渗透工艺可以采用一段或两段以上的反渗透处理，当采用两段以上的反渗透处理时，上一段反渗透处理的中间浓缩液作为下一段反渗透处理的进水，即放射性废液依次经过两段以上的反渗透处理，得到浓缩液，同时从每一段送出该段净化液，所有段送出的净化液汇合为一级反渗透浓缩液。
作为另一个示例，先将放射性废液送入第一级反渗透工艺处理，得到第一级反渗透净化液和第一级反渗透浓缩液，再将第一级反渗透净化液送入第二级反渗透工艺处理，得到第二级反渗透净化液和第二级反渗透浓缩液。其中，第二级反渗透浓缩液返回送入第一级反渗透工艺，第一级反渗透浓缩液即作为上述浓缩液，送入离子交换处理工序；第二级反渗透净化液低于10Bq/L，符合排放标准的要求，作为第一净化液进行排放处理。
可选地，第一级反渗透工艺可以采用一段或两段以上的反渗透处理，当采用两段以上的反渗透处理时，上一段反渗透处理产生的中间浓缩液作为下一段反渗透处理的进水，即放射性废液依次经过两段以上的反渗透处理，得到浓缩液，同时从每一段送出该段净化液，所有段送出的净化液汇合为第一级反渗透净化液。
可选地，第二级反渗透工艺可以采用一段或两段以上的反渗透处理，同样地，当采用两段以上的反渗透处理时，上一段反渗透处理产生的中间浓缩液作为下一段反渗透处理的进水，即放射性废液依次经过两段以上的反渗透处理，得到第二级反渗透浓缩液，同时从每一段送出该段净化液， 所有段送出的净化液汇合为第二级反渗透净化液。
作为一个可选方案，第一级反渗透工艺和第二级反渗透工艺均采用三段反渗透处理，组成“两级三段”反渗透工艺进行放射性废水对的分离处理，具有较高的净化能力和浓缩倍数，减小离子交换处理工序的负荷，同时提高反渗透回收率。
当一级反渗透工艺产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液，放射性活度大于10Bq/L时，或者，当追求所排放的净化液能够达到更低的放射性活度时，还可以将一级反渗透工艺产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液送入连续电除盐工艺进行进一步地精细处理。精细处理可以是采用一级或两级连续电除盐工艺，但并不限于此，还可以根据实际情况采用三级、四级或更高级连续电除盐工艺。
作为一个示例，将一级反渗透工艺产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液经过一级连续电除盐工艺进行精细处理，得到第一净化液，往往已经达到排放标准的要求，甚至达到天然本底水平，进行排放处理，产生的一级连续电除盐浓缩液返回一级反渗透工艺或两级反渗透工艺中的第一级反渗透工艺。
为了提高连续电除盐工艺的净化水平，还可以在一级反渗透工艺产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液中加入活化剂，再送入一级连续电除盐工艺进行深度净化处理。活化剂可以由电阻率大于0.5MΩ·cm的纯水和不同种类的无机盐配制而成，活化剂中含有离子Ca 2+、Na +、Sr 2+、Zn 2+、Mg 2+、Fe 2+和K +，阴离子种类不限，活化剂原液浓度与投加剂量相关，保证在活化剂加入放射性废水中并混合均匀后，放射性废水中含有的离子浓度如下：Ca 2+0.1mg/L～0.2mg/L、Na +0.2mg/L～0.3mg/L、Sr 2+8mg/L～9mg/L、Zn 2+18mg/L～20mg/L、Mg 2+0.2mg/L～0.25mg/L、Fe 2+0.04mg/L～0.05mg/L和K +100mg/L～150mg/L。
作为另一个示例，先将一级反渗透工艺产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液送入第一级连续电除盐工艺处理，得到第一级连续电除盐净化液和第一级连续电除盐浓缩液，再将第一 级连续电除盐净化液送入第二级连续电除盐工艺处理，得到第二级连续电除盐净化液和第二级连续电除盐浓缩液，其中，第二级连续电除盐净化液即为第一净化液，往往已经达到排放标准的要求，甚至达到天然本底水平，进行排放处理，第一级连续电除盐浓缩液和第二级连续电除盐浓缩液则返回一级反渗透工艺或两级反渗透工艺中的第一级反渗透工艺。
同样地，为了提高连续电除盐工艺的净化水平，还可以在第一级连续电除盐净化液中加入活化剂，再送入第二级连续电除盐工艺进行净化处理。活化剂可以选用如前文所述的活化剂。
可以理解的是，分离处理工序并不限于采用上述工艺，如还可以是一级以上的连续电除盐工艺；纳滤一反渗透组合工艺；纳滤一连续电除盐组合工艺；纳滤一反渗透一连续电除盐组合工艺等，本领域技术人员可以根据实际情况进行确定。
在放射性废水进行分离处理之前，可选择地对放射性废水进行预处理，但这并不是必须的工序。
考虑到放射性废水中锶、铯(尤其是铯)最容易穿透离子交换床，利用无机吸附的选择性特点对易穿透离子交换床的放射性核素进行特定吸附，从而延长离子交换树脂的使用周期，进一步减少放射性废离子交换树脂的产生量。基于上述考虑，放射性废液中锶的放射性活度、铯的放射性活度、锶与铯的总放射性活度中任一者为10 5Bq/L以上时，优选进行去除锶和/或铯的预处理。当无机吸附剂针对的特定放射性核素的放射性活度超过预设的临界值，如放射性废液中锶的放射性活度、铯的放射性活度或锶与铯的总放射性活度高于10 4Bq/L，此时，需要更换无机吸附剂。
放射性废水中除放射性核素和无机盐之外，还可能存在的油类、有机物、胶体、颗粒物等杂质，这些杂质大部分是非放射性的，但会对无机吸附、反渗透、离子交换等工艺产生影响，预处理去除这些杂质，能够延长无机吸附剂、反渗透膜、离子交换树脂的使用周期，减少无机吸附剂和离子交换树脂的更换，进一步减少放射性废离子交换树脂的产生量和放射性废无机吸附剂的产生量。活性炭因其独特的表面性能，对油类、有机物、胶体、颗粒物等杂质都有良好的吸附能力，因此可以采用活性炭吸附去除 这些杂质，简化预处理工艺设备和流程。当活性炭床层的阻力过大或者滤过液不满足后续的进水要求(污染指数SDI＜2)时，需要更换活性炭。
还可以预先对放射性废水调节pH值至6～8，可以使反渗透工艺的处理效果更好，并使反渗透膜具有较长的使用寿命。
为了实现上述放射性废液处理方法，本申请实施例进一步提供了一种放射性废液处理装置，以下结合图3至图7进行详细说明。
图3示出了本申请一个实施例提供的放射性废液处理装置工艺流程示意图。该装置包括分离单元200、离子交换单元300和排水单元400，其中，放射性废水供水与分离单元200的进口相连，分离单元200的浓缩液出口与离子交换单元300的进口相连；分离单元200的净化液出口连接至排水单元400；离子交换单元300的净化液出口连接至排水单元400和/或分离单元200的进口。
作为一个示例，排水单元400包括第一排水子单元和第二排水子单元(图中未示出)，分离单元200的净化液出口连接至第一排水子单元，离子交换单元300的净化液出口连接至第二排水子单元，第一排水子单元和第二排水子单元之间可以是连通的。这样，经检测第二净化液的放射性活度符合排放标准的要求时，可以根据不同需求将第一净化液和第二净化液分别直接排放，也可以是将两者混合后排放；经检测第二净化液与第一净化液混合后符合排放标准的要求时，则将第二净化液与第一净化液混合后进行排放。
可以理解的是，排水单元400可以仅仅是排水管道，也可以是在排水管道上连接产水箱401(如图6和图7所示)，或者其他将净化液排出的形式，本申请不作限制。
离子交换单元300的净化液出口还可以连接至分离单元200的进口，可以将第二净化液全部或部分返回作为分离单元200进水的一部分，这样能够降低分离单元200进水的放射性核素浓度，进而提高整套装置对放射性核素的去污效果。
根据本申请的一些实施例，分离单元200包括纳滤子单元、反渗透子单元、连续电除盐子单元中的一种或两种以上的组合。
作为一个示例，分离单元200包括反渗透子单元210(如图5所示)，反渗透子单元210中采用一级或两级反渗透设备，但并不限于此，还可以根据实际情况采用三级、四级或更多级反渗透设备。
在一些实施例中，请参照图6示出的本申请一个实施例提供的放射性废液处理装置工艺流程图，反渗透子单元210中采用一级反渗透设备，反渗透设备213的浓缩液出口与离子交换单元300的进口相连。从反渗透设备213送出的净化液已经低于10Bq/L，符合排放标准的要求，可以进行排放处理，此时，反渗透设备213的净化液出口连接至排水单元400。
为了提高反渗透回收率，反渗透设备213的浓缩液出口经管道分为两个支路，一个支路与反渗透设备213的进口相连，另一个支路与离子交换单元300的进口相连。这样还减少了浓缩液的排出量，降低离子交换单元300的负荷，进一步提高离子交换树脂的利用率，以及避免了能量浪费，节约能耗。
进一步地，反渗透设备213可以采用一个反渗透膜组件或两个以上的反渗透膜组件串联，当采用两个以上的反渗透膜组件时，上一个反渗透膜组件的浓缩液出口与下一个反渗透膜组件的进口相连，即将上一个反渗透膜组件产生的中间浓缩液作为下一个反渗透膜组件的进水，所有反渗透膜组件送出的净化液汇合为反渗透设备213的净化液。
在一些实施例中，请参照图7示出的本申请一个实施例提供的放射性废液处理装置工艺流程图，反渗透子单元210采用两级反渗透设备，其中第一级反渗透设备211和第二反渗透设备212串联为两级，具体地，第一级反渗透设备211的净化液出口与第二级反渗透设备212的进口相连，第二级反渗透设备212的浓缩液出口与第一级反渗透设备211的进口相连，第一级反渗透设备211的浓缩液出口与离子交换单元300的进口相连。从第二级反渗透设备212送出的净化液往往已经低于10Bq/L，符合排放标准的要求，可以进行排放处理，此时，第一级反渗透设备212的净化液出口连接至排水单元400。
为了提高反渗透回收率，第一级反渗透设备211的浓缩液出口经管道分为两个支路，一个支路与第一级反渗透设备211的进口相连，另一个支 路与离子交换单元300的进口相连。这样还减少了浓缩液的排出量，降低离子交换单元300的负荷，进一步提高离子交换树脂的利用率，以及避免了能量浪费，节约能耗。
进一步地，第一级反渗透设备211可以采用一个反渗透膜组件或两个以上的反渗透膜组件串联，当采用两个以上的反渗透膜组件时，上一个反渗透膜组件的浓缩液出口与下一个反渗透膜组件的进口相连，即将上一个反渗透膜组件产生的中间浓缩液作为下一个反渗透膜组件的进水，所有反渗透膜组件送出的净化液汇合为第一级反渗透设备211的净化液。
第二级反渗透设备212也可以采用一个反渗透膜组件或两个以上的反渗透膜组件串联，同样地，当采用两个以上的反渗透膜组件时，上一个反渗透膜组件的浓缩液出口与下一个反渗透膜组件的进口相连，即将上一个反渗透膜组件产生的中间浓缩液作为下一个反渗透膜组件的进水，所有反渗透膜组件送出的净化液汇合为第二级反渗透设备212的净化液。
作为一个可选方案，第一级反渗透设备211和第二级反渗透设备212均采用三段反渗透膜组件串联，组成“两级三段”反渗透单元进行放射性废水的分离处理，具有较高的净化能力和浓缩倍数，减小离子交换单元300的负荷，同时提高反渗透回收率。
当一级反渗透设备产出的一级反渗透净化液或两级反渗透设备产出的第二级反渗透净化液，放射性活度大于10Bq/L时，或者，当追求所排放的净化液能够达到更低的放射性活度时，还可以在反渗透子单元的下游设置连续电除盐子单元，将一级反渗透设备产出的一级反渗透净化液或两级反渗透工艺产出的第二级反渗透净化液送入连续电除盐子单元进行进一步地精细处理。精细处理可以是采用一级或两级连续电除盐设备，但并不限于此，还可以根据实际情况采用三级、四级或更多级连续电除盐设备。
作为一个示例，当连续电除盐子单元采用两级连续电除盐设备时，请参照图7，其中第一级连续电除盐设备221与第二级连续电除盐设备222串联，具体地，反渗透子单元的净化液出口，即一级反渗透设备的净化液出口或两级反渗透设备中第二级反渗透设备的净化液出口，与第一级连续电除盐设备221的进口相连，第一级连续电除盐设备221的净化液出口与 第二级连续电除盐设备222的进口相连，第二级连续电除盐设备222的净化液出口连接至排水单元400，第一级连续电除盐设备221的浓缩液出口和第二级连续电除盐设备222的浓缩液出口分别与反渗透子单元210的进口相连。当反渗透子单元210采用一级反渗透设备时，请参照图6，反渗透子单元210的进口指的是反渗透设备213的进口，当反渗透子单元210采用两级反渗透设备时，请参照图7，反渗透子单元210的进口指的是第一级反渗透设备211的进口。
为了提高连续电除盐子单元的净化水平，当连续电除盐子单元采用一级连续电除盐设备时，可以在反渗透子单元与连续电除盐子单元之间连接一中间水箱，该中间水箱与活化剂箱相连。这样，在反渗透子单元送出的净化液中，如一级反渗透设备产出的一级反渗透净化液或两级反渗透设备产出的第二级反渗透净化液中，加入活化剂，再送入一级连续电除盐设备进行深度净化处理。当连续电除盐子单元采用两级连续电除盐设备串联时，请参照图7，可以在第一级连续电除盐设备221与第二级连续电除盐设备222之间连接一中间水箱223，该中间水箱223与活化剂箱224相连，并设置加药泵以控制活化剂的加入量，使经连续电除盐子单元处理后产出的净化液达到天然本底水平。
根据本申请的一些实施例，请参照图6、图7，离子交换单元300包括一级离子交换器301，当然，也可以是两级以上的离子交换器301串联。
如图4所示，在分离单元200的上游还可以设置预处理单元100，但并不是必须的。如需设置，预处理单元100可以是包括油水分离器、活性炭过滤器、无机膜过滤器、保安过滤器、纸芯过滤器、自清洗过滤器、超滤器、无机吸附柱中的一种或几种的组合。
考虑到放射性废水中锶、铯(尤其是铯)最容易穿透离子交换床，利用无机吸附的选择性特点对易穿透离子交换床的放射性核素进行特定吸附，从而延长离子交换树脂的使用周期，进一步减少放射性废离子交换树脂的产生量。基于上述考虑，放射性废液中锶的放射性活度、铯的放射性活度、锶与铯的总放射性活度中任一者为10 5Bq/L以上时，优选通过无机 吸附柱102(如图5至图7所示)进行去除锶和/或铯的预处理，可以采用针对锶的无机吸附柱、针对铯的无机吸附柱或针对锶和铯的无机吸附柱。
放射性废水中除放射性核素和无机盐之外，还可能存在的油类、有机物、胶体、颗粒物等杂质，这些杂质大部分是非放射性的，但会对无机吸附剂、反渗透膜、离子交换树脂等产生影响，预处理去除这些杂质，能够延长无机吸附剂、反渗透膜、离子交换树脂的使用周期，减少无机吸附剂和离子交换树脂的更换，进一步减少放射性废离子交换树脂的产生量和放射性废无机吸附剂的产生量。活性炭因其独特的表面性能，对油类、有机物、胶体、颗粒物等杂质都有良好的吸附能力，因此可以采用活性炭过滤器101(如图5和图6所示)去除这些杂质，简化预处理工艺设备和流程。
有些放射性废水中杂质含量较多，对活性炭过滤器101负荷较大，采用活性炭过滤器101不能达到满意的杂质去除效果，请参照图6，预处理单元100可以采用油水分离器103、无机吸附柱102、纸芯过滤器106、自清洗过滤器107和超滤器108依次连接。其中，油水分离器103用于去除放射性废水中的油类杂质，降低油类杂质对后续工艺的影响；无机吸附柱102用于去除易穿透离子交换床的放射性核素，延长离子交换树脂的使用周期，减少放射性废离子交换树脂的产生量；可选地在油水分离器103与无机吸附柱102之间设置保安过滤器104，去除颗粒物，对无机吸附柱102起保护作用，防止颗粒物堵塞吸附柱；纸芯过滤器106用于去除放射性废水中的颗粒物，容纳了颗粒物的滤芯便于后续的处理处置；自清洗过滤器107利用滤网直接拦截放射性废水中的杂质，进一步去除悬浮物和颗粒物，自清洗过滤器107能够自动排污，提高智能化，使工艺更高效；超滤器108能够深度去除放射性废水中以胶体形态存在的杂质、蛋白质、微生物和大分子有机物。采用该预处理单元100，能够深度去除放射性废水中的杂质，使水质符合后续工艺的进水要求，大大减少杂质对分离处理工序、离子交换工序的影响，提高分离单元200、离子交换单元300的运行周期。在无机吸附柱102与纸芯过滤器106之间可以连接缓存水箱105，以缓存无机吸附处理后的放射性废水。
分离单元200还可以包括缓冲水箱201，以缓存来自预处理单元100的放射性废水。在缓冲水箱201与反渗透子单元210之间可以进一步连接保安过滤器202，用于保护后续工艺的反渗透设备。
该装置还包括适当的供水泵10、循环泵204和高压泵203，可以是本领域常用的各种泵，例如柱塞泵、离心泵等。
采用本申请实施例提供的放射性废水处理装置，能够实施上述放射性废水方法，以实现高的放射性废液净化水平，同时能够显著降低放射性废物的产生量，实现放射性废物的小量化。
下面借助实施例来举例说明本申请，但这些实施例绝不构成对本申请的限制。
以下实施例中Cs +、Sr 2+、Co 2+的浓度采用美国热电赛默飞ICAP Q型电感耦合等离子体-质谱ICP-MS仪进行测定，油类的浓度采用日本岛津OCT-1型总有机碳TOC分析仪进行表征。
“去污因子”按(进水的放射性活度)/(净化液的放射性活度)计算。
实施例1
本实施例所用放射性废水处理装置采用如图6所示的装置，反渗透设备213为三个反渗透膜组件串联，每个反渗透膜组件中设置有一支反渗透膜元件陶氏BW30-4040。装置采用的设备、元件、材料如下表所示：
Figure PCTCN2018085070-appb-000001
本实施例处理的放射性废水为模拟放射性废水，其中含有Cs+2000 μg/L，Co 2+875μg/L，Sr 2+1230μg/L，表面活性剂10mg/L。
放射性废水处理装置的设计处理量为1m 3/h，离子交换床处理速率约为10BV/h。
上述模拟放射性废水先经过活性炭吸附床预处理，水中的表面活性剂浓度降低至0.98mg/L，放射性核素离子浓度不变，进一步经铯吸附床预处理，水中Cs +浓度降低至0.08μg/L，基本上完全去除了废水中的Cs +。
高压泵203操作压力为1.5MPa，反渗透回收率为60％，3m 3/h浓水返回反渗透循环处理，0.67m 3/h浓水进入离子交换床进行离子交换处理，离子交换净化液产水0.67m 3/h，离子交换产水全部返回作为反渗透进水的一部分，反渗透的净化液产量达到1m 3/h。
反渗透设备213对Cs +、Sr 2+、Co 2+的截留率分别为95％、98％和98％。在装置开始运行时，离子交换床对三种放射性核素离子Cs +、Sr 2+、Co 2+的去污因子较高，分别约为10 3，离子交换产水中Cs +、Sr 2+、Co 2+浓度分别为0.71μg/L、1.30μg/L和1.80μg/L。离子交换产水与模拟放射性废水混合后作为反渗透进水，其中Cs +、Sr 2+、Co 2+浓度分别为299μg/L、525μg/L和739μg/L，反渗透的净化液，即装置产水中Cs +、Sr 2+、Co 2+的浓度分别为28.5μg/L、20.6μg/L和28.9μg/L，此时，装置对Cs +、Sr 2+、Co 2+的去污因子分别达到17、42、43。
随着装置运行时间增长，离子交换床对Cs +、Sr 2+、Co 2+的去污因子不断降低，在运行400h后，离子交换床对Cs +、Sr 2+、Co 2+的去污因子分别为1.8、2.1和2.0，离子交换产水中Cs +、Sr 2+、Co 2+的浓度分别为821μg/L、1252μg/L和1604μg/L，装置产水中Cs +、Sr 2+、Co 2+浓度分别为59.8μg/L、40.2μg/L和54.1μg/L，此时，装置对Cs +、Sr 2+、Co 2+的去污因子分别达到8、22、23。
如果不进行分离处理，经活性炭吸附床和铯吸附床预处理后直接采用离子交换床对上述模拟放射性废水进行净化处理，运行400h后，装置对Cs +、Sr 2+、Co 2+的总去污因子分别仅为2左右。可见，本申请采用分离处理将放射性废水进行浓缩后，对浓缩液进行离子交换处理，可以大幅度提高装置对放射性核素的去污因子，延长离子交换床使用寿命，大幅度降低 放射性固体废物量。
如果放射性废水中污染指数SDI低于2，可以不设置活性炭吸附工序。
如果放射性废水中Cs +离子含量低于10 5Bq/L，可以不设置铯吸附工序。
以上所述，仅为本申请的具体实施方式，应理解，本申请的保护范围并不局限于此，任何熟悉本技术领域的技术人员在本申请揭露的技术范围内，可轻易想到各种等效的修改或替换，这些修改或替换都应涵盖在本申请的保护范围之内。

Claims (22)

  1. 一种放射性废液处理方法，其中，所述方法包括：
    将放射性废液进行分离处理，得到第一净化液和浓缩液；
    将所述浓缩液进行离子交换处理，得到第二净化液；
    其中，将所述第一净化液与所述第二净化液排放处理；或者，将所述第二净化液返回所述分离处理工序，将所述第一净化液排放处理；或者，将部分所述第二净化液返回所述分离处理工序，将所述第一净化液与其余部分所述第二净化液排放处理。
  2. 根据权利要求1所述的方法，其中，所述分离处理采用纳滤工艺、反渗透工艺、连续电除盐工艺中的一种或两种以上的组合工艺。
  3. 根据权利要求1所述的方法，其中，所述将放射性废液进行分离处理，得到第一净化液和浓缩液包括：将放射性废液经过一级或两级反渗透工艺处理。
  4. 根据权利要求3所述的方法，其中，每级所述反渗透工艺采用一段或两段以上的反渗透处理，当采用两段以上的反渗透处理时，上一段反渗透处理的中间浓缩液作为下一段反渗透处理的进水，从各段送出净化液汇合为所述反渗透工艺的净化液。
  5. 根据权利要求3所述的方法，其中，所述两级反渗透工艺处理包括：
    将放射性废液依次经过第一级反渗透工艺和第二级反渗透工艺处理，将所述第二级反渗透工艺送出的第二级反渗透浓缩液返回所述第一级反渗透工艺，从所述第一级反渗透工艺送出所述浓缩液。
  6. 根据权利要求3所述的方法，其中，所述将放射性废液经过一级或两级反渗透工艺处理之后，还包括：将所述一级或两级反渗透工艺处理得到的净化液经过一级或两级连续电除盐工艺处理。
  7. 根据权利要求6所述的方法，其中，所述两级连续电除盐工艺处理包括：
    将所述一级或两级反渗透工艺处理得到的净化液依次经过第一级连续 电除盐工艺和第二级连续电除盐工艺处理，得到所述第一净化液；所述第一级连续电除盐工艺送出的第一级连续电除盐浓缩液和所述第二级连续电除盐工艺送出的第二级连续电除盐浓缩液返回所述一级或两级反渗透工艺。
  8. 根据权利要求7所述的方法，其中，在所述第一级连续电除盐工艺送出的中间净化液中加入活化剂，再送入所述第二级连续电除盐工艺。
  9. 根据权利要求1所述的方法，其中，所述放射性废液的体积为所述浓缩液的体积的2倍以上，所述浓缩液中放射性核素的浓度为所述放射性废液中放射性核素的浓度的2倍以上。
  10. 根据权利要求1所述的方法，其中，所述放射性废液进行所述分离处理之前，经过预处理，以去除油类、胶体、颗粒物、锶、铯中的一种以上，和/或，调节pH值。
  11. 根据权利要求10所述的方法，其中，所述放射性废液中，锶的放射性活度、铯的放射性活度、锶与铯的总放射性活度中任一者为10 5Bq/L以上时，需要进行去除锶和/或铯的预处理。
  12. 一种放射性废液处理装置，其中，该装置包括分离单元、离子交换单元和排水单元，其中，
    所述分离单元的浓缩液出口与所述离子交换单元的进口相连；
    所述分离单元的净化液出口连接至所述排水单元；
    所述离子交换单元的净化液出口连接至所述排水单元和/或所述分离单元的进口。
  13. 根据权利要求12所述的装置，其中，所述分离单元包括纳滤子单元、反渗透子单元、连续电除盐子单元中的一种或两种以上的组合。
  14. 根据权利要求13所述的装置，其中，所述分离单元包括反渗透子单元，其中，所述反渗透子单元包括一级或两级反渗透设备。
  15. 根据权利要求14所述的装置，其中，所述分离单元进一步包括连续电除盐子单元，所述反渗透子单元和所述连续电除盐子单元依次连接；其中，所述连续电除盐子单元包括一级或两级连续电除盐设备。
  16. 根据权利要求14或15所述的装置，其中，所述反渗透设备采用 一个反渗透膜组件或两个以上的反渗透膜组件串联，当采用两个以上的反渗透膜组件时，上一个反渗透膜组件的浓缩液出口与下一个反渗透膜组件的进口相连。
  17. 根据权利要求14或15所述的装置，其中，所述反渗透子单元包括一级反渗透设备，所述反渗透设备的浓缩液出口经管道分为两个支路，一个支路与所述反渗透设备的进口相连，另一个支路与所述离子交换单元的进口相连；或者，
    所述反渗透子单元包括两级反渗透设备，其中第一级反渗透设备的浓缩液出口经管道分为两个支路，一个支路与第一级反渗透设备的进口相连，另一个支路与所述离子交换单元的进口相连。
  18. 根据权利要求14或15所述的装置，其中，所述反渗透子单元包括两级反渗透设备，其中，第一级反渗透设备的净化液出口与第二级反渗透设备的进口相连，第二级反渗透设备的浓缩液出口与所述第一级反渗透设备的进口相连，第一级反渗透设备的浓缩液出口与所述离子交换单元的进口相连。
  19. 根据权利要求15所述的装置，其中，所述连续电除盐子单元包括两级连续电除盐设备，其中，所述反渗透子单元的净化液出口与所述第一级连续电除盐设备的进口相连，所述第一级连续电除盐设备的净化液出口与所述第二级连续电除盐设备的进口相连，所述第二级连续电除盐设备的净化液出口连接至所述排水单元，所述第一级连续电除盐设备的浓缩液出口和所述第二级连续电除盐设备的浓缩液出口分别与所述反渗透子单元的进口相连。
  20. 根据权利要求19所述的装置，其中，所述第一级连续电除盐设备的净化液出口经中间水箱与所述第二级连续电除盐设备的进口相连，所述中间水箱与活化剂箱相连。
  21. 根据权利要求12所述的装置，其中，所述离子交换单元包括一级或两级以上的离子交换器。
  22. 根据权利要求12所述的装置，其中，该装置还包括预处理单元，所述预处理单元与所述分离单元的进口相连，用于去除放射性废液中 的油类、胶体、颗粒物、锶、铯中的一种以上，和/或，调节pH值。
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