CN115676891B - Electrochemical separation and fixation of UO in radioactive wastewater 22+ And ReO 4- Is a method of (2) - Google Patents
Electrochemical separation and fixation of UO in radioactive wastewater 22+ And ReO 4- Is a method of (2) Download PDFInfo
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- 238000000926 separation method Methods 0.000 title claims abstract description 46
- 238000000034 method Methods 0.000 title claims abstract description 31
- 239000002354 radioactive wastewater Substances 0.000 title claims abstract description 17
- 230000009467 reduction Effects 0.000 claims abstract description 29
- 239000003792 electrolyte Substances 0.000 claims abstract description 20
- 239000010411 electrocatalyst Substances 0.000 claims abstract description 5
- 238000002360 preparation method Methods 0.000 claims abstract description 5
- 239000003054 catalyst Substances 0.000 claims description 73
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 54
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 50
- 229910052799 carbon Inorganic materials 0.000 claims description 39
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 23
- 229910017604 nitric acid Inorganic materials 0.000 claims description 23
- 229910002804 graphite Inorganic materials 0.000 claims description 16
- 239000010439 graphite Substances 0.000 claims description 16
- 239000000463 material Substances 0.000 claims description 10
- 239000000956 alloy Substances 0.000 claims description 3
- 229910045601 alloy Inorganic materials 0.000 claims description 3
- 239000002923 metal particle Substances 0.000 claims description 3
- 239000002105 nanoparticle Substances 0.000 claims description 3
- 229920000557 Nafion® Polymers 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
- 238000002791 soaking Methods 0.000 claims description 2
- 239000000758 substrate Substances 0.000 claims description 2
- 238000009210 therapy by ultrasound Methods 0.000 claims description 2
- 230000005611 electricity Effects 0.000 claims 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 abstract description 10
- 229910052770 Uranium Inorganic materials 0.000 abstract description 9
- 229910052702 rhenium Inorganic materials 0.000 abstract description 8
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 abstract description 8
- 230000000694 effects Effects 0.000 abstract description 7
- 230000002378 acidificating effect Effects 0.000 abstract description 6
- YSZJKUDBYALHQE-UHFFFAOYSA-N rhenium trioxide Chemical compound O=[Re](=O)=O YSZJKUDBYALHQE-UHFFFAOYSA-N 0.000 abstract description 5
- 239000002245 particle Substances 0.000 abstract description 3
- 230000005684 electric field Effects 0.000 abstract description 2
- 230000005518 electrochemistry Effects 0.000 abstract description 2
- 230000009931 harmful effect Effects 0.000 abstract description 2
- 230000008569 process Effects 0.000 abstract description 2
- 239000000126 substance Substances 0.000 abstract description 2
- 239000004094 surface-active agent Substances 0.000 abstract description 2
- 231100000331 toxic Toxicity 0.000 abstract description 2
- 230000002588 toxic effect Effects 0.000 abstract description 2
- 229910002007 uranyl nitrate Inorganic materials 0.000 abstract description 2
- 238000002474 experimental method Methods 0.000 description 20
- 238000001179 sorption measurement Methods 0.000 description 14
- 238000001000 micrograph Methods 0.000 description 6
- 239000000047 product Substances 0.000 description 6
- 239000002915 spent fuel radioactive waste Substances 0.000 description 6
- 229910052778 Plutonium Inorganic materials 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 3
- 230000001788 irregular Effects 0.000 description 3
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 description 3
- 230000006978 adaptation Effects 0.000 description 2
- 150000001450 anions Chemical class 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 229910052713 technetium Inorganic materials 0.000 description 2
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- GKLVYJBZJHMRIY-OUBTZVSYSA-N Technetium-99 Chemical compound [99Tc] GKLVYJBZJHMRIY-OUBTZVSYSA-N 0.000 description 1
- 229910052776 Thorium Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
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- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000002285 radioactive effect Effects 0.000 description 1
- 238000003904 radioactive pollution Methods 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
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Abstract
Separation and fixation of UO in radioactive wastewater 2 2+ And ReO 4 ‑ A method of radionuclides comprising (i) preparing an electrocatalyst; (ii) preparation of an electrolyte; (iii) electrical separation conditions; (iv) an electrical separation operation; (v) electrically isolating the product. The method mainly adopts an electrochemical separation method, realizes reduction of rhenium and removal of uranium by utilizing an electric field and an electron reduction effect in electrochemistry, has the advantages of high efficiency, convenience, simplicity in operation, low cost and the like, does not need to add any surfactant in the whole process, can not generate toxic and harmful substances, and successfully solves the problem that uranium and rhenium in acidic radioactive wastewater are difficult to separate, and the final products obtained by the electrochemical separation method are blocky rhenium trioxide particles and electro-adsorbed uranyl nitrate.
Description
Technical Field
The invention belongs to a wastewater treatment technology containing radionuclides, and in particular relates to a method for electrochemically separating and fixing UO in radioactive wastewater from acidic radioactive wastewater 2 2+ And ReO 4 - Is a method of (2).
Background
Nuclear energy is taken as a low-carbon emission technology and is expected to play an important role in meeting the energy demand of the future society. During the development and utilization of nuclear energy, a lot of spent fuel is produced, of which 95% of uranium (mainly U 238 ) And 1% plutonium, and other nuclides such as plutonium, technetium, strontium, thorium, and the like. At present, there are two ideas for the international treatment of spent fuel, one is to recycle usable nuclides, such as uranium and plutonium nuclides, which can be recycled to produce mixed fuel; the other is to solidify and landfill the spent fuel as waste. However, if these radionuclides are accidentally leaked into the environment during the treatment, they can cause long-term, irreparable harm to the environment, and can further enter the human body through the food chain to be enriched in the human body, seriously jeopardizing the health of the human body. For example, the radionuclide technetium-99 is a long-lived fission product with a long half-life (2.13×10 5 years) in spent fuel to be mainly water-solubleExtremely strong, extremely stable pertechnetate anion TcO 4 - Exists in the form of (2) and TcO 4 - Has extremely strong migration capability in the environment. Meanwhile, the spent fuel has extremely strong acidity (3M HNO) 3 ) But also contains a large excess of a variety of common anions such as nitrate, chloride, etc. Because all technetium isotope species are radioactive, rhenium (Re) is often used as 99 Non-radiochemical analogs of Tc were studied. In addition, uranium leaked into the environment can also cause significant environmental and human health concerns.
The current common treatment methods for radioactive wastewater comprise a chemical precipitation method, an evaporation concentration method, a membrane treatment method, a biological treatment method, an adsorption method and the like. However, no method has been developed to achieve simultaneous separation of UO from stationary radioactive wastewater 2 2+ And ReO 4 - . Thus, a strain capable of simultaneously separating and fixing ReO under an acidic condition is developed 4 - And UO 2 2+ The method has important significance for the treatment of radioactive pollution in the environment.
Disclosure of Invention
The invention aims to overcome the defects existing in the prior art and aims to provide a method for electrochemically separating and fixing the ReO in radioactive wastewater 4 - And UO 2 2+ Is a method of (2).
The technical scheme of the invention is as follows: electrochemical separation of UO in radioactive wastewater 2 2+ And ReO 4 - A method of radionuclide comprising the steps of:
(i) Preparation of electrocatalyst: dissolving a catalyst in ethanol, adding a proper amount of Nafion117 solution, uniformly ultrasonically and dropwise adding the solution onto a carbon felt, and baking the solution in an infrared oven;
(ii) Preparation of electrolyte: according to the acidity of radioactive wastewater, preparing various wastes containing various UOs with different acidity 2 2 + and ReO 4 - Is a solution of (a) and (b);
(iii) Conditions for electrical separation: the electrical separation condition is pulse voltage;
(iv) Electrical separation operation: immersing the electrocatalyst prepared in step (i) in the electrolyte prepared in step (ii), and performing an electroseparation operation under the conditions of step (iii);
(v) Electroseparation of the product: and (3) taking out the substrate material subjected to the electroseparation in the step (iv) to obtain an electroseparation reduction product subjected to post-treatment.
Preferably, in the step (i), the catalyst, alcohol and Nafion117 solution are added according to the following amounts: catalyst: alcohol: nafion 117=3 to 6mg,800 to 1200uL,80 to 120uL. .
Preferably, the catalyst in step (i) comprises: monoatomic catalysts, metal particle catalysts, alloy catalysts, nonmetallic catalysts, or carbon-based catalysts.
Preferably, the electrolyte in the step (ii) has an acidity of 3M nitric acid to 1M nitric acid, a pH of 0 to 1, and UO 2 2+ And ReO 4 - The concentrations of (2) were 100ppm, respectively.
Preferably, in the step (iii) of the electrical separation condition, the difference between the high voltage and the low voltage of the pulse voltage is 0 to 5V, and the duty ratio is 1 to 100%.
Preferably, the electrode in step (iv) is a graphite rod electrode or a catalyst material electrode.
Preferably, the time of the electric separation operation in the step (iv) is 5min to 1000min.
Preferably, the post-treatment of the electrically separated product of step (v) is: soaking the reacted carbon felt in ethanol, carrying out ultrasonic treatment until the catalyst material loaded on the carbon felt is dissolved in ethanol solution, and then drying the ethanol solution with the dissolved catalyst material in an infrared oven.
The beneficial effects of the invention are as follows:
aiming at the problem that extracting and separating uranium and rhenium from acidic spent fuel radioactive wastewater is difficult at present, the invention provides an electrochemical separation method for extracting rhenium from radioactive wastewater, thereby separating uranium and rhenium. The method mainly adopts an electrochemical separation method, and realizes the reduction of rhenium and the removal of uranium by utilizing an electric field and electron reduction in electrochemistry. The electrochemical separation method has the advantages of high efficiency, convenience, simple operation, low cost and the like, any surfactant is not needed to be added in the whole process, toxic and harmful substances are not generated, the problem that uranium and rhenium in acidic radioactive wastewater are difficult to separate is successfully solved, and the final product obtained by the electrochemical separation method is blocky rhenium trioxide particles and electrosorbed uranyl nitrate, and the blocky rhenium trioxide particles can be generated under different acidic conditions.
Drawings
FIG. 1 is a graph of UO at pH=1 in the present invention 2 2+ And ReO 4 - Is a graph of the effect of electrical separation.
FIG. 2 is a diagram of UO under 1M nitric acid in the present invention 2 2+ And ReO 4 - Is a graph of the effect of electrical separation.
FIG. 3 is a diagram of UO under 3M nitric acid in the present invention 2 2+ And ReO 4 - Is a graph of the effect of electrical separation.
FIG. 4 is a ReO produced by electroreduction immobilization in example 5 of the present invention 3 Scanning electron microscope images.
FIG. 5 is a ReO produced by electroreduction immobilization in example 10 of the present invention 3 Scanning electron microscope images.
FIG. 6 is a ReO produced by electroreduction immobilization in example 15 according to the present invention 3 Scanning electron microscope images.
FIG. 7 is a ReO obtained in example 5 of the present invention 3 Is an X-ray diffraction pattern of (2).
Detailed Description
The invention is described below with reference to the drawings and examples for electrochemical separation of UO from radioactive wastewater 2 2+ And ReO 4 - The method of radionuclide is described in detail.
Samples (trade name and place of origin) used in the examples:
1. the catalyst adopts: a single atom catalyst, a metal particle catalyst, or an alloy catalyst;
2. the ethanol adopts industrial pure ethanol;
3. the Nafion117 solution adopts an industrial pure product;
4. the carbon felt is an industrial pure product;
5. the electrode adopts an industrial pure graphite rod electrode, and the catalyst material electrode adopts a hollow carbon supported Ru nano particle catalyst;
6. nitric acid is industrially pure, and the concentration is 16M nitric acid;
7. containing UO 2 2+ And ReO 4 - Respectively adopts analytically pure UO as electrolyte 2 (NO 3 ) 2 ·6H 2 O and NaReO 4 And (5) preparing.
Example 1
Preparing an electrolyte, wherein UO 2 2 And ReO 4 - The solution was adjusted to ph=1 with nitric acid at a concentration of 100ppm, respectively. 5mg of hollow carbon supported Ru nanoparticle catalyst was weighed into a 10mL beaker, and 1mL of ethanol solution and 100. Mu.L of Nafion117 solution were added and sonicated for 10min until the solution was uniform. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electroseparation reduction experiment for 30min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electrosorption amount of (C) is 188.4mg/g, for ReO 4 - The amount of electro-adsorption was 177.5mg/g.
Example 2
Preparing an electrolyte, wherein UO 2 2+ And ReO 4 - The solution was adjusted to ph=1 with nitric acid at a concentration of 100ppm, respectively. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electroseparation reduction experiment for 60min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electro-adsorption amount of the catalyst is 299.0mg/g, and the catalyst is used for ReO 4 - The electrosorption amount of (C) was 319.9mg/g.
Example 3
Preparing an electrolyte, wherein UO 2 2+ And ReO 4 - The solution was adjusted to ph=1 with nitric acid at a concentration of 100ppm, respectively. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electric separation reduction experiment for 120min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO (ultra-low) reduction experiment 2 2+ The electro-adsorption amount of (C) is 312.2mg/g, for ReO 4 - The amount of electric adsorption of (C) was 536.5mg/g.
Example 4
Preparing an electrolyte, wherein UO 2 2+ And ReO 4 - The solution was adjusted to ph=1 with nitric acid at a concentration of 100ppm, respectively. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electric separation reduction experiment for 420min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electric adsorption quantity of (C) is 416.8mg/g, for ReO 4 - The electrosorption amount of (C) was 705.6mg/g.
Example 5
Preparing an electrolyte, wherein UO 2 2+ And ReO 4 - The solution was adjusted to ph=1 with nitric acid at a concentration of 100ppm, respectively. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing 1440min electroseparation reduction experiment under the condition of pulse voltage of-5V and duty ratio of 50%, and performing UO 2 2+ The electrosorption amount of (C) is 455.9mg/g, for ReO 4 - The electrosorption amount of (C) was 859.6mg/g.
Example 6
FIG. 1 shows the electrical separation of UO under pH=1 in the present invention 2 2+ And ReO 4 - From the graph, it can be seen that the electrical separation method of the present invention can achieve the separation of UO 2 2+ And ReO 4 - And a good removal effect is achieved.
Example 7
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 1M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electroseparation reduction experiment for 5min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electro-adsorption amount of (C) is 68.2mg/g, for ReO 4 - The amount of electric adsorption was 122.7mg/g.
Example 8
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 1M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Under the condition of pulse voltage of-5V and duty ratio of 50%, performing an electric separation reduction experiment for 240min to UO 2 2+ The electric adsorption quantity of (C) is 141.6mg/g, for ReO 4 - The electrosorption amount of (C) was 267.2mg/g.
Example 9
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 1M. Weigh 5mg of catalyst in a 10mL beaker and add 1mL of ethanol solution and 100 mu L Nafion117 solution was sonicated for 10min until the solution was homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Under the condition of pulse voltage of-5V and duty ratio of 50%, performing 1080min electroseparation reduction experiment to UO 2 2+ The electric adsorption quantity of (C) is 356.9mg/g, for ReO 4 - The electrosorption amount of (C) was 559.2mg/g.
Example 10
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 1M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing 1440min electroseparation reduction experiment under the condition of pulse voltage of-5V and duty ratio of 50%, and performing UO 2 2+ The electro-adsorption amount of (C) is 359.1mg/g, and the catalyst is used for ReO 4 - The electrosorption amount of (C) was 585.1mg/g.
Example 11
FIG. 2 shows the electrical separation of UO under 1M nitric acid in the present invention 2 2+ And ReO 4 - From the graph, it can be seen that the electrical separation method of the present invention can achieve the separation of UO 2 2+ And ReO 4 - And a good removal effect is achieved.
Example 12
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 3M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. At a pulse voltage of-5V and a duty cycle of 50%Run 15min of electroseparation reduction experiments on UO 2 2+ The electroadsorption amount of (C) is 102.7mg/g, for ReO 4 - The electrosorption amount of (C) was 173.0mg/g.
Example 13
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 3M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electroseparation reduction experiment for 60min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electrosorption amount of (C) is 253.5mg/g, for ReO 4 - The amount of electric adsorption of (C) was 243.1mg/g.
Example 14
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 3M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. Performing an electric separation reduction experiment for 420min under the condition of pulse voltage of-5V and duty ratio of 50 percent, and performing a UO reduction experiment 2 2+ The electric adsorption quantity of (C) is 285.1mg/g, for ReO 4 - The electrosorption amount of (C) was 365.6mg/g.
Example 15
Preparing 100mL of electrolyte, wherein UO 2 2+ And ReO 4 - The concentration of (2) was 100ppm and the concentration of nitric acid was 3M. Weigh 5mg of catalyst in a 10mL beaker, add 1mL ethanol solution and 100. Mu.L Nafion117 solution and sonicate for 10min until the solution is homogeneous. The catalyst solution was dropped on a 1 x 1 carbon felt and baked in an infrared oven. And then taking the carbon felt loaded with the catalyst as a working electrode and taking a graphite rod as a counter electrode. At the position ofPerforming 1440min electroseparation reduction experiment under the condition of pulse voltage of-5V and duty ratio of 50%, and performing UO 2 2+ The electric adsorption quantity of (C) is 303.7mg/g, for ReO 4 - The electrosorption amount of (C) was 373.6mg/g.
Example 16
FIG. 3 shows the electrical separation of UO under 3M nitric acid in the present invention 2 2+ And ReO 4 - From the graph, it can be seen that the electrical separation method of the present invention can achieve the separation of UO 2 2+ And ReO 4 - And a good removal effect is achieved.
Example 17
The morphology of the electrode sample obtained after the electrical separation for 24 hours at ph=1 was characterized, and fig. 4 is a scanning electron microscope image. From the figure it can be seen that the samples after electroseparation reduction appear as irregular lumps.
Example 18
The morphology of the electrode sample obtained after electrical separation for 24 hours under the condition of 1M is characterized, and FIG. 5 is a scanning electron microscope image. From the figure, it can be seen that the samples after electroseparation reduction exhibit an irregular block or bar shape.
Example 19
The morphology of the electrode sample obtained after electrical separation for 24 hours under the condition of 3M is characterized, and FIG. 6 is a scanning electron microscope image. From the figure it can be seen that the samples after electroseparation reduction exhibit irregular clumps.
Example 20
Fig. 7 is an XRD pattern of the resulting electrode sample after electrical separation at ph=1 for 24 hours, from which diffraction peaks of typical rhenium trioxide can be seen, as compared to a standard XRD pattern. Peaks at 2θ= 16.566 ° and 25.457 ° are attributed to the (110) and (210) crystal planes of rhenium trioxide, while the crystal forms are intact.
Other embodiments of the disclosure will be apparent to those skilled in the art from consideration of the specification and practice of the disclosure disclosed herein. This application is intended to cover any adaptations, uses, or adaptations of the disclosure following, in general, the principles of the disclosure and including such departures from the present disclosure as come within known or customary practice within the art to which the disclosure pertains. It is intended that the specification and examples be considered as exemplary only, with a true scope and spirit of the disclosure being indicated by the following claims.
Claims (9)
1. Electrochemical separation and fixation of UO in radioactive wastewater 2 2+ And ReO 4 - A method of radionuclides characterized by: the method comprises the following steps: (i) preparation of electrocatalyst: dissolving a catalyst in ethanol, adding a proper amount of Nafion117 solution, uniformly ultrasonically, dripping the solution onto a carbon felt, and baking the solution in an infrared oven; (ii) preparation of an electrolyte: preparing UO containing different acidity according to the acidity of radioactive wastewater 2 2+ And ReO 4 - Is a solution of (a) and (b); (iii) conditions for electrical separation: the electrical separation condition is pulse voltage; (iv) an electrical separation operation: immersing the electrocatalyst prepared in step (i) in the electrolyte prepared in step (ii), and performing an electroseparation operation under the conditions of step (iii); (v) electrically isolating the product: taking out the substrate material subjected to the electroseparation in the step (iv) to obtain an electroseparated reduction product subjected to post-treatment;
the catalyst in step (i) comprises: single atom catalysts, metal particle catalysts, alloy catalysts, or carbon-based catalysts.
2. The method according to claim 1, characterized in that: in the step (i), the catalyst, alcohol and Nafion117 solution are added according to the following amounts: catalyst: alcohol: nafion 117=3 to 6mg,800 to 1200ul,
80~120uL。
3. the method according to claim 1, characterized in that: in the step (i), the hollow carbon supported Ru nanoparticle catalyst is adopted as the catalyst material electrode.
4. The method according to claim 1, characterized in that: the electricity in the step (ii)The acidity of the solution is 3M nitric acid to 1M nitric acid, the pH value is 0 to 1, and the UO is 2 2+ And ReO 4 - The concentration of (2) was 100ppm.
5. The method according to claim 1, characterized in that: in the step (iii) of the electrical separation condition, the difference between the high voltage and the low voltage of the pulse voltage is 0-5V, and the duty ratio is 1-100%.
6. A method according to claim 1 or 3, characterized in that: the electrode in the step (iv) is a graphite rod electrode or a catalyst material electrode.
7. The method according to claim 1, characterized in that: the time of the electrical separation operation in the step (iv) is 1 min-1440 min.
8. The method according to claim 7, wherein: the separation operation in the step (iv) is 5 min-1000 min.
9. The method according to claim 1, characterized in that: the post-treatment of the electrically separated product of step (v) is: soaking the reacted carbon felt in ethanol, carrying out ultrasonic treatment until the catalyst material loaded on the carbon felt is dissolved in ethanol solution, and then drying the ethanol solution with the dissolved catalyst material in an infrared oven.
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| CN202211376155.6A CN115676891B (en) | 2022-11-04 | 2022-11-04 | Electrochemical separation and fixation of UO in radioactive wastewater 22+ And ReO 4- Is a method of (2) |
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| CN110575830A (en) * | 2019-09-12 | 2019-12-17 | 中国原子能科学研究院 | platinum-containing catalyst and preparation method and application thereof |
| CN112342385A (en) * | 2020-09-28 | 2021-02-09 | 西北工业大学 | Device and method for extracting uranium from uranium-containing wastewater or seawater and application of device and method |
| CN114395764A (en) * | 2021-12-16 | 2022-04-26 | 西南科技大学 | Application of molybdenum disulfide with sulfur boundary defect in electrochemical extraction of uranium from seawater |
| CN114507874A (en) * | 2022-01-12 | 2022-05-17 | 西南科技大学 | Application of uranium-loaded molybdenum disulfide nanosheet in electrocatalytic alkaline hydrogen evolution reaction |
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| CN110575830A (en) * | 2019-09-12 | 2019-12-17 | 中国原子能科学研究院 | platinum-containing catalyst and preparation method and application thereof |
| CN112342385A (en) * | 2020-09-28 | 2021-02-09 | 西北工业大学 | Device and method for extracting uranium from uranium-containing wastewater or seawater and application of device and method |
| CN114395764A (en) * | 2021-12-16 | 2022-04-26 | 西南科技大学 | Application of molybdenum disulfide with sulfur boundary defect in electrochemical extraction of uranium from seawater |
| CN114507874A (en) * | 2022-01-12 | 2022-05-17 | 西南科技大学 | Application of uranium-loaded molybdenum disulfide nanosheet in electrocatalytic alkaline hydrogen evolution reaction |
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