CN113877517A - Bismuth sulfide aerogel adsorbent for removing radioactive iodine and preparation method and application thereof - Google Patents
Bismuth sulfide aerogel adsorbent for removing radioactive iodine and preparation method and application thereof Download PDFInfo
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Abstract
The invention discloses a bismuth sulfide aerogel adsorbent for removing radioactive iodine and a preparation method and application thereof, wherein the bismuth sulfide aerogel adsorbent has a three-dimensional net-shaped porous structure, the average pore diameter of the three-dimensional net-shaped porous structure is 8-10nm, and the preparation method comprises the following steps: adding bismuth nitrate pentahydrate, thiourea, polyvinylpyrrolidone and chitosan into water, mixing to obtain a mixed solution, adding the mixed solution into a reaction kettle, carrying out heat preservation reaction at 180-220 ℃ for 180-220 min, and cooling to room temperature after the reaction is finished; uniformly shaking the reacted feed liquid, quickly freezing the feed liquid by using liquid nitrogen, putting the feed liquid into a freeze dryer, and freeze-drying the feed liquid for 3 to 5 days to obtain bismuth sulfide/chitosan aerogel; calcining the bismuth sulfide/chitosan aerogel at 200-300 ℃, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent, wherein the adsorbent has good acid and alkali resistance chemical stability, so that the bismuth sulfide aerogel adsorbent has excellent selectivity and efficient removal capacity for gaseous radioactive iodide ions.
Description
Technical Field
The invention relates to an adsorption material for treating radioactive waste gas in a spent fuel post-treatment process, in particular to a bismuth sulfide aerogel adsorbent for removing radioactive iodine and a preparation method thereof.
Background
As a key nuclide in fission products, radionuclide iodine: (129I and131I) the biological agent has strong migration capability, is easy to volatilize and is easy to enrich biologically, thus having potential threat to the environment and human body.131The half-life of I is only 8.02 days, and the radioactivity is extremely strong, and is a main contributor of the irradiation dose outside the nuclear accident.129The half-life of I is 1.57X 107A long-lived nuclear species can cause nearly permanent radioactive contamination of the environment if leaked into the environment. A review report on radioactive iodine pollution remediation issued by the national laboratory of oak ridge in the united states (ORNL/TM-6350) shows that 99.5% of the radioactive iodine enters the exhaust treatment system in gaseous form. When a nuclear accident occurs, radioactive iodine is ingested by the human body in the form of iodine vapor, organic iodine (methyl iodide) vapor and aerosol, resulting in metabolic disorders, mental retardation and increased thyroid cancer of the human body, and therefore, how to selectively enrich and separate radionuclide iodine from a complex environmental system and achieve safe disposal thereof is a difficult problem in the field of environmental radiochemistry.
Disclosure of Invention
In view of the above technical problems, the present invention needs to provide a bismuth sulfide aerogel adsorbent for removing radioactive iodine with high adsorption performance and good acid-base stability, and a preparation method thereof.
An object of the present invention is to solve at least the above problems and/or disadvantages and to provide at least the advantages described hereinafter.
To achieve these objects and other advantages in accordance with the present invention, there is provided a bismuth sulfide aerogel adsorbent for radioactive iodine removal, having a three-dimensional network porous structure, and an average pore size of the three-dimensional network porous structure being 8 to 10 nm.
The invention also provides a preparation method of the bismuth sulfide aerogel adsorbent for removing radioactive iodine, which comprises the following steps:
adding bismuth nitrate pentahydrate, thiourea, polyvinylpyrrolidone and chitosan into water, mixing to obtain a mixed solution, adding the mixed solution into a reaction kettle, carrying out heat preservation reaction at 180-220 ℃ for 180-220 min, and cooling to room temperature after the reaction is finished;
step two, uniformly shaking the material liquid reacted in the step one, quickly freezing the material liquid by using liquid nitrogen, and then putting the material liquid into a freeze dryer for freeze drying for 3-5 days to obtain the bismuth sulfide/chitosan aerogel;
and step three, calcining the bismuth sulfide/chitosan aerogel at 200-300 ℃, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent.
Preferably, the mass ratio of the bismuth nitrate pentahydrate to the thiourea to the polyvinylpyrrolidone to the chitosan is 3-3.5: 3.5-4.5: 1-1.5: 1; the mass volume ratio of the chitosan to the water is 1g: 180-250 mL; the water is deionized water.
Preferably, the polyvinylpyrrolidone has a K value of 98.
Preferably, in the third step, the calcining time is 180-220 min.
Preferably, the process of the first step is replaced by: adding chitosan into supercritical CO2In the reaction kettle, then introducing CO2At a temperature of 40-60 ℃ and a pressure ofThe supercritical CO is utilized under the pressure of 15-20 MPa2Swelling chitosan for 45-60 min, releasing pressure, adding the chitosan obtained after pressure release, bismuth nitrate pentahydrate, thiourea and polyvinylpyrrolidone into water, mixing to obtain a mixed solution, adding the mixed solution into a microwave and ultrasonic integrated reactor, simultaneously starting microwaves and ultrasonic waves for synergistic treatment for 15-30 min, then adding the mixed solution into a reaction kettle, carrying out heat preservation reaction at 180-220 ℃ for 120-150 min, and cooling to room temperature after the reaction is finished.
Preferably, the power of the microwave is 200-350W, the power of the ultrasonic is 300-400W, and the ultrasonic frequency is 35-60 KHz; the treatment temperature is 50-60 ℃.
The invention also provides application of the bismuth sulfide aerogel adsorbent prepared by the preparation method in radioactive iodine removal.
The invention at least comprises the following beneficial effects: according to the invention, the bismuth sulfide aerogel material with the three-dimensional network structure and high specific surface area and porosity is synthesized by a sol-gel method, due to the synergistic effect of physical adsorption of the surface and pores of the three-dimensional network structure and chemical adsorption of bismuth ions, and the bismuth ions have high affinity to iodine according to the HASB soft-hard acid-base theory, so that the bismuth sulfide aerogel adsorbent has excellent selectivity and high-efficiency removal capability to radioactive iodine in gas, and meanwhile, the preparation process is simple and the efficiency is high.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention.
Description of the drawings:
fig. 1 is an SEM image of a bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention;
fig. 2 is an XRD image of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention;
fig. 3 is an infrared absorption spectrum of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention;
fig. 4 is a nitrogen adsorption-desorption isotherm of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention;
fig. 5 is a pore size distribution curve of the bismuth sulfide aerogel adsorbent for radioactive iodine removal prepared in example 1 of the present invention;
fig. 6 is an XRD chart before and after adsorption of iodine by the bismuth sulfide aerogel adsorbent for removal of radioactive iodine prepared in example 1 of the present invention;
fig. 7 is an adsorption power line diagram of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention;
fig. 8 is a graph showing the adsorption effect of the bismuth sulfide aerogel adsorbents for radioactive iodine removal prepared in examples 1 and 3 of the present invention;
fig. 9 is an adsorption isotherm diagram of a bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1 of the present invention;
fig. 10 is an XRD chart of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 of the present invention after soaking in solutions with different pH.
The specific implementation mode is as follows:
the present invention is further described in detail below with reference to the attached drawings so that those skilled in the art can implement the invention by referring to the description text.
It will be understood that terms such as "having," "including," and "comprising," as used herein, do not preclude the presence or addition of one or more other elements or groups thereof.
Example 1:
a preparation method of a bismuth sulfide aerogel adsorbent for removing radioactive iodine comprises the following steps:
step one, adding 0.485g of pentahydrate bismuth nitrate, 0.6g of thiourea, 0.2g of polyvinylpyrrolidone and 0.15g of chitosan into 30mL of deionized water, fully dissolving to obtain a mixed solution, adding the mixed solution into a 50mL reaction kettle, keeping the temperature at 200 ℃ for reaction for 200min, and cooling to room temperature after the reaction is finished; the K value of the polyvinylpyrrolidone is 98;
step two, uniformly shaking the material liquid reacted in the step one, quickly freezing the material liquid by using liquid nitrogen, putting the material liquid into a freeze dryer, and freeze-drying the material liquid for 3 days to obtain the bismuth sulfide/chitosan aerogel;
step three, calcining the bismuth sulfide/chitosan aerogel at 200 ℃ for 200min, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent (Bi) for removing radioactive iodine2S3@I2)。
Example 2:
a preparation method of a bismuth sulfide aerogel adsorbent for removing radioactive iodine comprises the following steps:
step one, adding 0.485g of pentahydrate bismuth nitrate, 0.6g of thiourea, 0.2g of polyvinylpyrrolidone and 0.15g of chitosan into 30mL of deionized water, fully dissolving to obtain a mixed solution, adding the mixed solution into a 50mL reaction kettle, keeping the temperature at 200 ℃ for reaction for 200min, and cooling to room temperature after the reaction is finished; the K value of the polyvinylpyrrolidone is 98;
step two, uniformly shaking the material liquid reacted in the step one, quickly freezing the material liquid by using liquid nitrogen, putting the material liquid into a freeze dryer, and freeze-drying the material liquid for 5 days to obtain the bismuth sulfide/chitosan aerogel;
and step three, calcining the bismuth sulfide/chitosan aerogel at 250 ℃ for 200min, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent for removing radioactive iodine.
Example 3:
a preparation method of a bismuth sulfide aerogel adsorbent for removing radioactive iodine comprises the following steps:
step one, adding chitosan into supercritical CO2In the reaction kettle, then introducing CO2Using supercritical CO at 55 deg.C and 20MPa2Swelling chitosan for 45min, relieving pressure, adding 0.15g of chitosan obtained after pressure relief, 0.485g of bismuth nitrate pentahydrate, 0.6g of thiourea and 0.2g of polyvinylpyrrolidone into 30mL of deionized water, fully dissolving to obtain a mixed solution, adding the mixed solution into a microwave and ultrasonic integrated reactor, simultaneously starting microwaves and ultrasonic waves for synergistic treatment for 25min, adding the mixed solution into a reaction kettle, carrying out heat preservation reaction at 200 ℃ for 140min, and cooling after the reaction is finishedCooling to room temperature; the K value of the polyvinylpyrrolidone is 98; the power of the microwave is 200-350W, the power of the ultrasonic is 300-400W, and the ultrasonic frequency is 35-60 KHz; the treatment temperature is 50-60 ℃.
Step two, uniformly shaking the material liquid reacted in the step one, quickly freezing the material liquid by using liquid nitrogen, putting the material liquid into a freeze dryer, and freeze-drying the material liquid for 3 days to obtain the bismuth sulfide/chitosan aerogel;
step three, calcining the bismuth sulfide/chitosan aerogel at 200 ℃ for 200min, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent (Bi) for removing radioactive iodine2S3@I2-1)。
Fig. 1 is a Scanning Electron Microscope (SEM) image of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1, and it can be seen from fig. 1 that the calcined bismuth sulfide aerogel has a three-dimensional network porous structure.
Fig. 2 is an XRD spectrum of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1, and it can be seen from fig. 2 that the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 has sharp diffraction peaks at 2 θ 25 °, 28.455 °, 31.805 ° and 46.562 °, corresponding to Bi2S3The characteristic peak of the adsorbent indicates that the main phase of the prepared bismuth sulfide aerogel adsorbent for removing radioactive iodine is bismuth sulfide.
Fig. 3 is an infrared absorption spectrum of the bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1. As can be seen from fig. 3, the bismuth sulfide aerogel for removing radioactive iodine prepared in example 1 is 718, 1372, 1623, 3429cm-1A clear characteristic peak appears, wherein, 3429cm-1The absorption peaks at the left and right are the absorption peaks of the O-H bond, which are generated by the small amount of water adsorbed in the sample. And at 718, 1372 and 1623cm-1The absorption peak generated here is a Bi — S bond vibration absorption peak, indicating that a large amount of Bi — S bonds are present in the prepared bismuth sulfide aerogel adsorbent for removing radioactive iodine.
Fig. 4 is a nitrogen adsorption-desorption isotherm of the bismuth sulfide aerogel adsorbent for radioactive iodine removal prepared in example 1. As shown in fig. 4, when the relative pressure is 0.3-0.8, the adsorption amount of the bismuth sulfide aerogel to nitrogen gas is slowly increased, and the bismuth sulfide aerogel is mainly adsorbed on the inner surface of the aerogel structure in a monomolecular layer adsorption manner at this stage; when the relative pressure is increased to 0.8-0.95, the adsorption capacity of the bismuth sulfide aerogel on nitrogen is obviously increased, and gas molecules are mainly adsorbed on the inner surface of the aerogel structure in a polymolecular layer; when the relative pressure reaches 0.95-1.0, the adsorption capacity of nitrogen is remarkably increased, which indicates that the adsorption of gas molecules is mainly capillary condensation of a pore structure and the variation range of the section is narrow, and indicates that the pore size distribution of the bismuth sulfide aerogel is more concentrated.
Fig. 5 is a pore size distribution curve of the bismuth sulfide aerogel adsorbent for radioactive iodine removal prepared in example 1. As shown in FIG. 5, the BET surface area of the prepared bismuth sulfide aerogel material for removing radioactive iodine was found to be 4.69m by testing2Per g, pore volume of 0.01cm3(iv)/g, average pore diameter 9.3 nm.
FIG. 6 is an XRD spectrum of the bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1 after adsorption of iodine, and as shown in FIG. 6, Bi in the bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1 after adsorption of iodine2S3The characteristic peak of (a) disappears, and new diffraction peaks appear at 2 θ of 226.860 °, 35.235 ° and 41.616 °, corresponding to BiI3The characteristic peak shows that the bismuth sulfide aerogel adsorbent effectively adsorbs radioactive iodine and generates a stable product BiI3。
Fig. 7 is a graph showing adsorption kinetics of the bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1. As shown in fig. 7, the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 adsorbs iodine (specifically, a certain amount of I is added)2Placing into a 30mL glass bottle, placing 50mg of bismuth sulfide aerogel synthesized in example 1 into conical filter paper at the top of the bottle, sealing the glass bottle with a cover, heating to 75 ℃ under ambient pressure to evaporate iodine), gradually increasing the adsorption capacity of the sample to iodine with the increase of contact time, wherein the adsorption capacity is rapidly increased to 450mg/g in a period of 0-200min, and then the adsorption capacity is leveledThe adsorption is slowly increased to reach the balance in about 900min and the maximum adsorption capacity is 1200 mg/g.
Fig. 8 is a graph showing the adsorption effect of the bismuth sulfide aerogel adsorbents for radioactive iodine removal prepared in example 1 and example 3; (the specific implementation process is to add a certain amount of I2Putting the bismuth sulfide aerogel into a 30mL glass bottle, putting 50mg of the bismuth sulfide aerogel synthesized in the example 1 or the example 3 into conical filter paper at the top of the bottle, covering the conical filter paper to seal the glass bottle, heating the bismuth sulfide aerogel to 75 ℃ under the ambient pressure to evaporate iodine), gradually increasing with the increase of contact time, gradually increasing the adsorption capacity until the adsorption is balanced, and the adsorption effect of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in the example 3 is better than that of the example 1.
Fig. 9 is an adsorption isotherm diagram of the bismuth sulfide aerogel adsorbent for removing radioiodine prepared in example 1. As shown in fig. 9, the experiment shows that the equilibrium adsorption capacity (qe) is significantly increased with the increase of the equilibrium concentration (Ce) of iodine in the aqueous solution according to the experiment, when the equilibrium concentration (Ce) of iodine is increased, the adsorption isotherm of the bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 in the cyclohexane solution of iodine is taken (the specific implementation process is that 100mg of iodine is taken, 100mL of cyclohexane is used to prepare 100mL of cyclohexane solution of 1000ppm of iodine, then 50, 100, 200, 400, 600, 800ppm of iodine is prepared, 10mL of the above iodine solution with different concentrations is taken and added into a 20mL scintillation vial, 10mg of bismuth sulfide aerogel material sample is added thereto, stirring is carried out for 24 hours at normal temperature, after reaching the adsorption equilibrium, the supernatant is taken and filtered by a 0.22 μm organic phase filter membrane, and the concentration of residual iodine in the filtrate is measured by ultraviolet spectrophotometry). The adsorption data are analyzed according to Freundlich and Langmuir fitting models, which shows that the prepared bismuth sulfide aerogel adsorbent for removing radioactive iodine mostly belongs to chemical adsorption and nonlinear adsorption, the adsorption process is easy to carry out, and the affinity of the bismuth sulfide aerogel and iodine is strong.
Fig. 10 is XRD patterns of bismuth sulfide aerogel adsorbent for removing radioactive iodine prepared in example 1 after soaking in solutions with different pH. The specific implementation process is that 100mg of bismuth sulfide synthesized in the example 1 is aerogelAnd (3) soaking the glue into 10mL of aqueous solution with the pH values of 2, 4, 6, 8, 10 and 12 respectively, then placing the glue into a shaking table to shake for 24 hours, taking out a powder sample obtained after suction filtration and drying, and carrying out XRD test. Bi in XRD pattern2S3The characteristic peak of the bismuth sulfide aerogel adsorbent for removing radioactive iodine is not changed, and the prepared bismuth sulfide aerogel adsorbent for removing radioactive iodine has better acid and alkali chemical stability.
According to the bismuth sulfide aerogel adsorbent for removing radioactive iodine and the preparation method thereof, the bismuth sulfide aerogel material with the three-dimensional network structure is constructed, on the premise that the high adsorption performance of the bismuth-based material on radioactive iodine is kept, the physical adsorption enrichment function of the three-dimensional network structure of the aerogel is cooperatively utilized, and the bismuth sulfide aerogel adsorbent has good acid-base chemical stability and excellent selectivity and efficient removal capability on gaseous radioactive iodine ions. Meanwhile, the preparation process is simple and the efficiency is high.
While embodiments of the invention have been described above, it is not limited to the applications set forth in the description and the embodiments, which are fully applicable in various fields of endeavor to which the invention pertains, and further modifications may readily be made by those skilled in the art, it being understood that the invention is not limited to the details shown and described herein without departing from the general concept defined by the appended claims and their equivalents.
Claims (8)
1. The bismuth sulfide aerogel adsorbent for removing radioactive iodine is characterized by having a three-dimensional net-shaped porous structure, wherein the average pore diameter of the three-dimensional net-shaped porous structure is 8-10 nm.
2. A method for preparing the bismuth sulfide aerogel adsorbent for removing radioactive iodine according to claim 1, comprising the following steps:
adding bismuth nitrate pentahydrate, thiourea, polyvinylpyrrolidone and chitosan into water, mixing to obtain a mixed solution, adding the mixed solution into a reaction kettle, carrying out heat preservation reaction at 180-220 ℃ for 180-220 min, and cooling to room temperature after the reaction is finished;
step two, uniformly shaking the material liquid reacted in the step one, quickly freezing the material liquid by using liquid nitrogen, and then putting the material liquid into a freeze dryer for freeze drying for 3-5 days to obtain the bismuth sulfide/chitosan aerogel;
and step three, calcining the bismuth sulfide/chitosan aerogel at 200-300 ℃, and then cooling to room temperature to obtain the bismuth sulfide aerogel adsorbent.
3. The preparation method of the bismuth sulfide aerogel adsorbent for removing radioactive iodine according to claim 2, wherein the mass ratio of the bismuth nitrate pentahydrate to the thiourea to the polyvinylpyrrolidone to the chitosan is 3-3.5: 3.5-4.5: 1-1.5: 1; the mass volume ratio of the chitosan to the water is 1g: 180-250 mL; the water is deionized water.
4. The method of preparing a bismuth sulfide aerogel adsorbent for the removal of radioactive iodine according to claim 2, wherein said polyvinylpyrrolidone has a K value of 98.
5. The preparation method of the bismuth sulfide aerogel adsorbent for removing radioactive iodine according to claim 2, wherein in the third step, the calcination time is 180-220 min.
6. The method for preparing the bismuth sulfide aerogel adsorbent for removing radioactive iodine according to claim 2, wherein the process of the first step is replaced by: adding chitosan into supercritical CO2In the reaction kettle, then introducing CO2Supercritical CO is utilized at the temperature of 40-60 ℃ and the pressure of 15-20 MPa2Swelling chitosan for 45-60 min, releasing pressure, adding the chitosan obtained after pressure release, bismuth nitrate pentahydrate, thiourea and polyvinylpyrrolidone into water, mixing to obtain a mixed solution, adding the mixed solution into a microwave and ultrasonic integrated reactor, simultaneously starting microwaves and ultrasonic waves for synergistic treatment for 15-30 min, adding the mixed solution into a reaction kettle, and carrying out heat preservation reaction at 180-220 ℃ for 12 minAnd (3) 0-150 min, and cooling to room temperature after the reaction is finished.
7. The preparation method of the bismuth sulfide aerogel adsorbent for removing radioactive iodine according to claim 6, wherein the microwave power is 200-350W, the ultrasonic power is 300-400W, and the ultrasonic frequency is 35-60 KHz; the treatment temperature is 50-60 ℃.
8. Use of the bismuth sulfide aerogel adsorbent prepared by the preparation method according to any one of claims 1 to 7 in radioactive iodine removal.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114505047A (en) * | 2022-03-08 | 2022-05-17 | 西南科技大学 | Sulfydryl modified SBA-15 and preparation method thereof, bismuth-based adsorbent and preparation method and application thereof |
| CN114653334A (en) * | 2022-03-15 | 2022-06-24 | 广西大学 | Bi synthesized by hydrothermal method2S3@SiO2Nanofiber membrane and preparation method and application thereof |
| CN114653334B (en) * | 2022-03-15 | 2023-08-04 | 广西大学 | Bi synthesized by hydrothermal method 2 S 3 @SiO 2 Nanofiber membrane and preparation method and application thereof |
| CN114669279A (en) * | 2022-04-12 | 2022-06-28 | 西南科技大学 | Preparation and application of bismuth-based plant tannin @ collagen fiber hydrothermal carbon high-efficiency iodine-immobilized vapor material |
| CN114669279B (en) * | 2022-04-12 | 2023-09-15 | 西南科技大学 | Preparation and application of bismuth-based vegetable tannin@collagen fiber hydrothermal carbon efficient immobilized iodine vapor material |
| CN115178230A (en) * | 2022-05-20 | 2022-10-14 | 西南科技大学 | Preparation method and application of all-silica zeolite confinement copper nanoparticle adsorbent |
| CN116251566A (en) * | 2023-03-01 | 2023-06-13 | 西华师范大学 | Preparation method and application of bismuth-doped polyvinylpyrrolidone porous carbon material |
| CN116251566B (en) * | 2023-03-01 | 2024-04-30 | 西华师范大学 | Preparation method and application of bismuth-doped polyvinylpyrrolidone porous carbon material |
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