CN116459790B - Preparation method of flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material - Google Patents
Preparation method of flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material Download PDFInfo
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- CN116459790B CN116459790B CN202310448234.1A CN202310448234A CN116459790B CN 116459790 B CN116459790 B CN 116459790B CN 202310448234 A CN202310448234 A CN 202310448234A CN 116459790 B CN116459790 B CN 116459790B
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- 239000000835 fiber Substances 0.000 title claims abstract description 113
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 title claims abstract description 93
- 229910052740 iodine Inorganic materials 0.000 title claims abstract description 93
- 239000011630 iodine Substances 0.000 title claims abstract description 93
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 title claims abstract description 80
- 239000000463 material Substances 0.000 title claims abstract description 80
- 238000002360 preparation method Methods 0.000 title claims abstract description 20
- 229920000742 Cotton Polymers 0.000 claims abstract description 56
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims abstract description 50
- 238000001035 drying Methods 0.000 claims abstract description 48
- 238000001914 filtration Methods 0.000 claims abstract description 32
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 30
- 239000008367 deionised water Substances 0.000 claims abstract description 28
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 28
- 229910001961 silver nitrate Inorganic materials 0.000 claims abstract description 25
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 21
- 229910000033 sodium borohydride Inorganic materials 0.000 claims abstract description 21
- 239000012279 sodium borohydride Substances 0.000 claims abstract description 21
- 238000000967 suction filtration Methods 0.000 claims abstract description 16
- -1 polytetrafluoroethylene Polymers 0.000 claims abstract description 15
- 238000004140 cleaning Methods 0.000 claims abstract description 12
- 238000002156 mixing Methods 0.000 claims abstract description 7
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims abstract description 6
- 239000004810 polytetrafluoroethylene Substances 0.000 claims abstract description 6
- 238000003763 carbonization Methods 0.000 claims abstract description 5
- 230000009467 reduction Effects 0.000 claims abstract description 5
- 239000005539 carbonized material Substances 0.000 claims abstract description 3
- 241000219000 Populus Species 0.000 claims description 35
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 claims description 30
- 239000011812 mixed powder Substances 0.000 claims description 29
- YKTSYUJCYHOUJP-UHFFFAOYSA-N [O--].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-] Chemical compound [O--].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-] YKTSYUJCYHOUJP-UHFFFAOYSA-N 0.000 claims description 27
- 238000000137 annealing Methods 0.000 claims description 26
- 239000000725 suspension Substances 0.000 claims description 21
- 238000001291 vacuum drying Methods 0.000 claims description 20
- 238000000034 method Methods 0.000 claims description 17
- 238000003756 stirring Methods 0.000 claims description 15
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 12
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 11
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 10
- 238000004062 sedimentation Methods 0.000 claims description 10
- 239000011858 nanopowder Substances 0.000 claims description 9
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 claims description 7
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims description 7
- KWIUHFFTVRNATP-UHFFFAOYSA-N Betaine Natural products C[N+](C)(C)CC([O-])=O KWIUHFFTVRNATP-UHFFFAOYSA-N 0.000 claims description 7
- 239000002202 Polyethylene glycol Substances 0.000 claims description 7
- 229960003237 betaine Drugs 0.000 claims description 7
- 230000004048 modification Effects 0.000 claims description 7
- 238000012986 modification Methods 0.000 claims description 7
- 229920001223 polyethylene glycol Polymers 0.000 claims description 7
- 238000007711 solidification Methods 0.000 claims description 6
- 230000008023 solidification Effects 0.000 claims description 6
- 239000002270 dispersing agent Substances 0.000 claims description 5
- 238000003760 magnetic stirring Methods 0.000 claims description 5
- 229910052757 nitrogen Inorganic materials 0.000 claims description 5
- 238000003825 pressing Methods 0.000 claims description 5
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 5
- 238000005406 washing Methods 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 4
- 238000004506 ultrasonic cleaning Methods 0.000 claims description 4
- 238000005189 flocculation Methods 0.000 claims description 2
- 230000002285 radioactive effect Effects 0.000 abstract description 6
- 239000000126 substance Substances 0.000 abstract description 6
- 239000011148 porous material Substances 0.000 abstract description 3
- 150000001875 compounds Chemical class 0.000 abstract 1
- 229910052709 silver Inorganic materials 0.000 description 10
- 239000004332 silver Substances 0.000 description 10
- JKFYKCYQEWQPTM-UHFFFAOYSA-N 2-azaniumyl-2-(4-fluorophenyl)acetate Chemical compound OC(=O)C(N)C1=CC=C(F)C=C1 JKFYKCYQEWQPTM-UHFFFAOYSA-N 0.000 description 6
- 229910021612 Silver iodide Inorganic materials 0.000 description 6
- 229940045105 silver iodide Drugs 0.000 description 6
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 description 5
- 238000001179 sorption measurement Methods 0.000 description 5
- 239000013078 crystal Substances 0.000 description 4
- 239000007789 gas Substances 0.000 description 3
- 238000002173 high-resolution transmission electron microscopy Methods 0.000 description 3
- 238000001878 scanning electron micrograph Methods 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000002105 nanoparticle Substances 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- 210000001685 thyroid gland Anatomy 0.000 description 2
- 230000004580 weight loss Effects 0.000 description 2
- 239000002028 Biomass Substances 0.000 description 1
- 206010006458 Bronchitis chronic Diseases 0.000 description 1
- 229910014033 C-OH Inorganic materials 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910014570 C—OH Inorganic materials 0.000 description 1
- 201000004624 Dermatitis Diseases 0.000 description 1
- 241000124033 Salix Species 0.000 description 1
- 238000003917 TEM image Methods 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000004964 aerogel Substances 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 206010006451 bronchitis Diseases 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229920002678 cellulose Polymers 0.000 description 1
- 235000010980 cellulose Nutrition 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 208000007451 chronic bronchitis Diseases 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000007334 copolymerization reaction Methods 0.000 description 1
- 239000013310 covalent-organic framework Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 238000006073 displacement reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000032050 esterification Effects 0.000 description 1
- 238000005886 esterification reaction Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 238000006266 etherification reaction Methods 0.000 description 1
- 244000144992 flock Species 0.000 description 1
- 125000002485 formyl group Chemical class [H]C(*)=O 0.000 description 1
- 238000000024 high-resolution transmission electron micrograph Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 125000000468 ketone group Chemical group 0.000 description 1
- 230000003902 lesion Effects 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000012621 metal-organic framework Substances 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 239000002915 spent fuel radioactive waste Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 238000003911 water pollution Methods 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
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- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/0203—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising compounds of metals not provided for in B01J20/04
- B01J20/0233—Compounds of Cu, Ag, Au
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/16—Alumino-silicates
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28054—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their surface properties or porosity
- B01J20/28057—Surface area, e.g. B.E.T specific surface area
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- B01J20/28054—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their surface properties or porosity
- B01J20/28095—Shape or type of pores, voids, channels, ducts
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- G—PHYSICS
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- 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
- G21F9/02—Treating gases
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- B01D2257/00—Components to be removed
- B01D2257/20—Halogens or halogen compounds
- B01D2257/202—Single element halogens
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J2220/00—Aspects relating to sorbent materials
- B01J2220/40—Aspects relating to the composition of sorbent or filter aid materials
- B01J2220/48—Sorbents characterised by the starting material used for their preparation
- B01J2220/4812—Sorbents characterised by the starting material used for their preparation the starting material being of organic character
- B01J2220/4825—Polysaccharides or cellulose materials, e.g. starch, chitin, sawdust, wood, straw, cotton
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Abstract
The invention discloses a preparation method of a flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material, which comprises the following steps: putting the fly wadding fibers into deionized water, ultrasonically cleaning, removing seeds, filtering, and drying in an oven; immersing the fly wadding fiber into silver nitrate solution, and uniformly mixing by ultrasonic; transferring the obtained solution into a hydrothermal reaction kettle with a polytetrafluoroethylene lining, carrying out hydrothermal carbonization, carrying out suction filtration on carbonized materials, and drying for later use; and (3) reducing the obtained carbonized flying cotton fiber in sodium borohydride solution, and performing suction filtration and drying after reduction to obtain the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material. The invention loads zero-valent nano silver in the interface and pores of the fly wadding fiber base material, and nano silver granular substances are generated. The prepared material has stable property, the gaseous iodine is captured and then is fixed with zero-valent nano silver to generate an AgI compound, and the material has excellent gaseous iodine fixing capability. Successful preparation of this material facilitates efficient capture and curing of radioactive gaseous iodine.
Description
Technical Field
The invention belongs to the technical field of radioactive gaseous iodine solidification of biomass waste resources in the environment, and particularly relates to a preparation method of a flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Background
The fly wadding is the seed of poplar willow, is white villus, is easy to cause skin allergy, chronic bronchitis and other diseases to human body, has a wax layer on the surface, can float on the water surface for a long time and cause water pollution, and is inflammable, and fire disaster is easy to cause. The fly wadding fiber cannot be spun due to the short, soft and low strength, and has not been widely used until now. However, compared with other celluloses, the fly wadding fiber has a unique hollow pipeline structure, and after the fiber is modified into a curing agent, the fiber can be cured in an inner layer and an outer layer, and active sites can be fully utilized. The flyball contains aldehyde, ester and ketone groups which have potential capturing capability on gaseous iodine, and in addition, the flyball fiber surface is rich in hydroxyl groups, can be complexed with silver ions through ion dipole interaction, is a stable point passivation site of zero-valent nano silver after the silver ions are reduced, and is a good material for preparing the zero-valent nano silver. The fly wadding fiber can be functionally modified by using hydroxyl as an activation center through means of esterification, etherification, graft copolymerization and the like, and has wide application environment.
Along with the rapid development of nuclear energy, the academy is increasingly concerned about the treatment of radioactive nuclear spent fuel, 129 i and 131 i is iodine isotope which generates great harm in nuclear reaction. 129 I half-life is long (T) 1/2 ＝1.52×10 7 y), organic iodine and inorganic iodine are easily and widely distributed in water, atmosphere, soil and other mediums, and continuously exist and accumulate in the environment, so that serious harm is caused to the area; 131 i although the half-life is short (T 1/2 =8.02d), but has high activity and high environmental and human hazard. In addition, iodine is easily concentrated in human thyroid glands, causing thyroid lesions, so that they are all required to be solidified immediately after release and reliably stored in the ground. The existing curing materials of gaseous iodine mainly comprise active carbon, silver-based zeolite, nano aerogel, metal organic framework, covalent organic framework and the like, but due to the fact that stability is poor, the preparation process is complex, the preparation cost is high, the later-stage processing is difficult, the environment adaptability is poor and other limiting factors, a new alternative material is urgently needed.
Disclosure of Invention
It is an object of the present invention to address at least the above problems and/or disadvantages and to provide at least the advantages described below.
To achieve these objects and other advantages and in accordance with the purpose of the invention, there is provided a method for preparing a high-efficiency fixed gaseous iodine material of flying flock fiber liability zero-valent nano silver, comprising the steps of:
step one, putting the fly wadding fibers into deionized water, ultrasonically cleaning, removing seeds, filtering, and drying in an oven;
step two, immersing the fly wadding fiber in the step one into silver nitrate solution with a certain concentration, and uniformly mixing by ultrasonic;
transferring the solution obtained in the step two into a hydrothermal reaction kettle with a polytetrafluoroethylene lining, carrying out hydrothermal carbonization, carrying out suction filtration on the carbonized material, and drying for later use;
and step four, reducing the carbonized flying cotton fiber obtained in the step three in sodium borohydride solution with a certain concentration, and performing suction filtration and drying after the reduction to obtain the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material.
Preferably, the fly wadding fiber in the first step is one or more of non-pretreated poplar wadding fiber and catkin fiber, and is dried in an oven at 25-85 ℃ after ultrasonic cleaning and seed removal for 5 hours, wherein the ultrasonic cleaning temperature is not higher than 60 ℃; the mass volume ratio of the fly wadding fiber to the deionized water is 1g to 1000mL.
Preferably, in the second step, the concentration of the silver nitrate solution is 0.01-50.0 g/L, the mass ratio of the fly-flocculation fiber to the silver nitrate is 1:0.01-1, the ultrasonic mixing time is 0.1-96 h, and the ultrasonic mixing temperature is 50 ℃.
Preferably, the hydrothermal temperature in the step three is controlled at 45-200 ℃, the hydrothermal carbonization time is 2 hours, and the mass-volume ratio of the fly wadding fiber to the polytetrafluoroethylene lining is 1 g/500 mL.
Preferably, in the fourth step, the concentration of sodium borohydride is 0.01-15 mol/L, the mass ratio of the fly wadding fiber to the sodium borohydride is 10:57, the reduction temperature is 20-90 ℃, and the drying temperature in a vacuum drying oven after suction filtration is 75 ℃.
Preferably, in the fourth step, after the reduced carbonized fly-wadding fiber is filtered and dried, the carbonized fly-wadding fiber is subjected to aluminum silicate modification treatment, and the specific method comprises the following steps:
s1, preparing modified layered aluminum silicate, and doping aluminum oxide nano powder into the modified layered aluminum silicate to obtain silicate mixed powder;
s2, carrying out thermal annealing treatment on the silicate mixed powder;
s3, adding the carbonized flying cotton fiber loaded with the zero-valent nano silver into absolute ethyl alcohol, magnetically stirring to obtain a suspension, adding silicate mixed powder after thermal annealing into the suspension, adding polyethylene glycol as a dispersing agent, stirring, dispersing, filtering and drying to obtain the carbonized flying cotton fiber mixed with aluminum silicate, pressing into a sheet, and then crushing to obtain the flying cotton fiber loaded with the zero-valent nano silver high-efficiency fixed gaseous iodine material.
Preferably, in S1, the specific method for preparing the modified layered aluminum silicate and incorporating the aluminum oxide nano powder into the modified layered aluminum silicate includes: adding layered aluminum silicate into absolute ethyl alcohol, and stirring to obtain a suspension, wherein the mass volume ratio of the layered aluminum silicate to the absolute ethyl alcohol is 1 g:30-100 mL; adding acrylic acid and cocoamidopropyl dimethyl betaine into the suspension, reacting for 2-24 hours at 70-80 ℃, adding aluminum oxide nano powder into the suspension, performing ultrasonic dispersion, wherein the ultrasonic frequency is 40-80 kHz, the ultrasonic time is 20-40 min, standing, filtering a sedimentation product, washing the sedimentation product with deionized water for multiple times, and drying to obtain silicate mixed powder; wherein the mass ratio of the aluminum silicate, the acrylic acid, the cocoamidopropyl dimethyl betaine and the aluminum oxide is 100:2-30:5-35:40-80.
Preferably, in S2, the method for performing thermal annealing treatment on the silicate mixed powder includes: the silicate mixed powder is put into a high-temperature annealing furnace, nitrogen is introduced, the annealing temperature is 400-800 ℃, and the annealing time is 2-24 hours.
Preferably, in the step S3, the magnetic stirring speed is 1200-3000 r/min, and the mass ratio of the carbonized fly-wadding fiber to the silicate mixed powder to the polyethylene glycol is 30:1-3:5.
The flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is applied to the field of solidification of gaseous iodine.
The invention at least comprises the following beneficial effects:
(1) Silver is loaded on the fly-wadding fiber in a nano simple substance form, zero-valent nano silver is loaded on the surface of the fly-wadding fiber base material and in fiber pores, a film-shaped metal coating is formed, granular substances are attached, and the property is stable. The curing capacity of the gaseous iodine is higher, the cured iodine is mainly stored in the form of silver iodide, and the cured iodine is not easy to volatilize, thereby being beneficial to the storage and curing treatment of radioactive iodine.
(2) The raw materials used in the invention are fly wadding fibers, especially the current abandoned poplar and catkin fibers, which avoid the pollution to the environment, and the fly wadding fibers have wide sources and low cost.
(3) The preparation method is simple in preparation process, does not involve any toxic or harmful reagent, and does not cause secondary pollution in the preparation process.
(4) The invention fully utilizes the unique hollow structure of poplar/catkin fiber, ensures that the poplar/catkin fiber is solidified into an inner layer and an outer layer, and fully utilizes the material space and the active site.
(5) According to the invention, silicate mixed powder is added into the carbonized fly-wadding fiber for silicate modification, so that the specific surface area of the carbonized fly-wadding fiber is remarkably increased, the porosity of the carbonized fly-wadding fiber is increased, and the adsorption capacity of the fly-wadding fiber loaded with zero-valent nano silver to gaseous iodine by the high-efficiency fixed gaseous iodine material is further improved. Wherein, the silicate mixed powder is subjected to thermal annealing treatment, so that the compactness of the gaps of the silicate mixed powder is improved.
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.
Drawings
FIG. 1 is an XRD pattern of a flying wadding fiber loaded with zero-valent nano silver prepared in example 2 of the invention before and after curing of a gaseous iodine material with high-efficiency fixation;
fig. 2 is an SEM image of the fly wadding fiber prepared in example 2 of the present invention before adsorbing gaseous iodine by the zero-valent nano silver-loaded high-efficiency fixed gaseous iodine material;
fig. 3 is an SEM image of the fly wadding fiber prepared in example 2 of the present invention loaded with zero-valent nano silver after gaseous iodine is adsorbed by the high-efficiency fixed gaseous iodine material.
Fig. 4 is a physical diagram of the fly wadding fiber prepared in the embodiment 2 of the invention before and after curing the zero-valent nano silver-loaded high-efficiency fixed gaseous iodine material;
FIG. 5 is a TEM and HRTEM chart of the flying wadding fiber loaded with zero-valent nano silver prepared in example 2 of the invention before and after curing the gaseous iodine material;
FIG. 6 is an iodine solidification graph of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in the embodiment 2 of the invention;
FIG. 7 is an XPS chart of the fly wadding fiber prepared in the embodiment 2 of the invention before and after solidification of the zero-valent nano silver-loaded high-efficiency fixed gaseous iodine material;
FIG. 8 is a graph of thermal weight loss of the zero-valent nano silver loaded high-efficiency fixed gaseous iodine material of the fly wadding fiber prepared in example 2 of the present invention;
fig. 9 is an iodine solidification graph of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in the embodiment 2 and the embodiment 7 of the invention.
Detailed Description
The present invention is described in further detail below with reference to the drawings to enable those skilled in the art to practice the invention by referring to the description.
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:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of catkin fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.015g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the catkin fiber in the first step into 0.5g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated catkin fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying at 45 ℃ in a vacuum drying oven for later use.
And step four, reducing the catkin fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, wherein the mass of sodium borohydride is 0.57g, filtering the solution, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the catkin fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 2:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.015g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.5g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a hydrothermal reaction kettle lined with 50mL polytetrafluoroethylene, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, and drying in a vacuum drying oven at 45 ℃ for standby after suction filtration.
And step four, reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, filtering the solution with the mass of 0.57g, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 3:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of catkin fiber into deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.006g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the catkin fiber in the first step into 0.2g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated catkin fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying at 45 ℃ in a vacuum drying oven for later use.
And step four, reducing the catkin fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, wherein the mass of sodium borohydride is 0.57g, filtering the solution, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the catkin fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 4:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.006g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.2g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying at 45 ℃ in a vacuum drying oven for later use.
And step four, reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution for 12 hours at normal temperature, wherein the mass of sodium borohydride is 0.57g, filtering the solution, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 5:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.006g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.2g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 4 hours at 160 ℃ in an oven, carrying out suction filtration, and drying at 45 ℃ in a vacuum drying oven for later use.
And step four, reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution for 12 hours at normal temperature, wherein the mass of sodium borohydride is 0.57g, filtering the solution, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 6:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.006g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.2g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 200 ℃ in an oven, carrying out suction filtration, and drying at 45 ℃ in a vacuum drying oven for later use.
And step four, reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution for 12 hours at normal temperature, wherein the mass of sodium borohydride is 0.57g, filtering the solution, and drying the solution in a vacuum drying oven at 75 ℃ to obtain the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 7:
the preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.015g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.5g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying in a 45 ℃ vacuum drying oven for later use.
Reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, filtering the solution with the mass of 0.57g, drying the solution in a vacuum drying oven at 75 ℃, and carrying out aluminum silicate modification treatment on the carbonized fly-cotton fiber, wherein the specific method comprises the following steps:
s1, 10g of layered aluminum silicate is put into 300mL of absolute ethyl alcohol, and suspension is obtained after stirring; adding 0.2g of acrylic acid and 0.5g of cocoamidopropyl dimethyl betaine into the suspension, reacting for 3 hours at 70 ℃, adding 4g of aluminum oxide nano powder into the mixture, performing ultrasonic dispersion, wherein the ultrasonic frequency is 40kHz, the ultrasonic time is 20min, standing, filtering a sedimentation product, washing the sedimentation product with deionized water for multiple times, and drying to obtain silicate mixed powder;
s2, putting silicate mixed powder into a high-temperature annealing furnace, and introducing nitrogen, wherein the annealing temperature is 400 ℃, and the annealing time is 2 hours;
s3, adding 0.03g of carbonized flying cotton fiber loaded with zero-valent nano silver into absolute ethyl alcohol, magnetically stirring to obtain a suspension, adding 0.001g of silicate mixed powder after thermal annealing into the suspension at the magnetic stirring speed of 1200r/min, adding 0.005g of polyethylene glycol as a dispersing agent, stirring, dispersing, filtering and drying to obtain carbonized flying cotton fiber mixed with aluminum silicate, pressing into a sheet, and then crushing to obtain the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 8
The preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.015g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.5g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying in a 45 ℃ vacuum drying oven for later use.
Reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, filtering the solution with the mass of 0.57g, drying the solution in a vacuum drying oven at 75 ℃, and carrying out aluminum silicate modification treatment on the carbonized fly-cotton fiber, wherein the specific method comprises the following steps:
s1, 10g of layered aluminum silicate is put into 300mL of absolute ethyl alcohol, and suspension is obtained after stirring; adding 1.6g of acrylic acid and 2g of cocoamidopropyl dimethyl betaine into the suspension, reacting for 3 hours at 70 ℃, adding 6g of aluminum oxide nano powder into the mixture, performing ultrasonic dispersion, wherein the ultrasonic frequency is 60kHz, the ultrasonic time is 30min, standing, filtering a sedimentation product, washing the sedimentation product with deionized water for multiple times, and drying to obtain silicate mixed powder;
s2, putting silicate mixed powder into a high-temperature annealing furnace, and introducing nitrogen, wherein the annealing temperature is 600 ℃, and the annealing time is 2 hours;
s3, adding 0.03g of carbonized flying cotton fiber loaded with zero-valent nano silver into absolute ethyl alcohol, magnetically stirring to obtain a suspension, adding 0.002g of silicate mixed powder after thermal annealing into the suspension at a magnetic stirring speed of 2100r/min, adding 0.005g of polyethylene glycol as a dispersing agent, stirring, dispersing, filtering and drying to obtain carbonized flying cotton fiber mixed with aluminum silicate, pressing into a sheet, and then crushing to obtain the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material.
Example 9
The preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting 0.1g of poplar fiber into 100mL of deionized water, ultrasonically cleaning for 5 hours, removing seeds, filtering, and drying in an oven at 45 ℃;
adding 0.015g of silver nitrate into 30mL of deionized water, ultrasonically dissolving for 5min, and placing the poplar fiber in the first step into 0.5g/L of silver nitrate solution, and ultrasonically treating at 50 ℃ for 48h, wherein the treated poplar fiber turns black;
transferring the solution obtained in the step two into a 50mL polytetrafluoroethylene-lined hydrothermal reaction kettle, carrying out hydrothermal reaction for 2h at 160 ℃ in an oven, carrying out suction filtration, and drying in a 45 ℃ vacuum drying oven for later use.
Reducing the poplar fiber obtained in the step three in 11.349g/L sodium borohydride solution at 25 ℃ for 12 hours, filtering the solution with the mass of 0.57g, drying the solution in a vacuum drying oven at 75 ℃, and carrying out aluminum silicate modification treatment on the carbonized fly-cotton fiber, wherein the specific method comprises the following steps:
s1, 10g of layered aluminum silicate is put into 300mL of absolute ethyl alcohol, and suspension is obtained after stirring; adding 3g of acrylic acid and 3g of cocoamidopropyl dimethyl betaine into the suspension, reacting for 24 hours at 80 ℃, adding 8g of aluminum oxide nano powder into the mixture, performing ultrasonic dispersion, wherein the ultrasonic frequency is 40kHz, the ultrasonic time is 20 minutes, standing, filtering a sedimentation product, washing the sedimentation product with deionized water for multiple times, and drying to obtain silicate mixed powder;
s2, putting silicate mixed powder into a high-temperature annealing furnace, and introducing nitrogen, wherein the annealing temperature is 400 ℃, and the annealing time is 2 hours;
s3, adding 0.03g of carbonized flying cotton fiber loaded with zero-valent nano silver into absolute ethyl alcohol, magnetically stirring to obtain a suspension, adding 0.003g of silicate mixed powder after thermal annealing into the suspension at a magnetic stirring speed of 3000r/min, adding 0.005g of polyethylene glycol as a dispersing agent, stirring, dispersing, filtering and drying to obtain carbonized flying cotton fiber mixed with aluminum silicate, pressing into a sheet, and then crushing to obtain the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material.
Fig. 1 is an XRD pattern of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in example 2 of the present invention before and after curing, wherein ycf@ag is before curing, ycf@ag-I is after curing, and before curing gaseous iodine, the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material shows clear carbon fiber structure peaks at 2θ=15.8°, 22.5 ° and zero-valent silver peaks at 2θ=38.2 °, 44.5 °, 64.8 ° and 77.5 ° respectively corresponding to (111), (200), (220) and (311) crystal faces thereof, indicating that the zero-valent silver is better loaded on poplar cotton fiber. After iodine absorption, the peak of the carbon fiber structure in the material disappears, the fiber structure of the surface is damaged to a certain extent, and simultaneously, characteristic peaks of silver iodide are shown at 2 theta = 22.5 degrees, 23.9 degrees, 25.8 degrees, 39.6 degrees, 42.8 degrees, 46.7 degrees, 71.1 degrees and the like, and the characteristic peaks respectively correspond to (100), (002), (101), (110), (103), (112) and (300) crystal faces of the characteristic peaks, so that the iodine is solidified in the curing agent in the form of silver iodide.
Fig. 2 and 3 are SEM images of the flying cotton fiber prepared in example 2 before the flying cotton fiber loaded with zero-valent nano silver efficiently fixes the gaseous iodine material to adsorb gaseous iodine, and as shown in the figure, the zero-valent nano silver is loaded on the surface of the flying cotton fiber substrate and in the fiber pores in the form of nano particles. Fig. 4 is a physical diagram of the fly wadding fiber loaded with zero-valent nano silver prepared in the embodiment 2 before and after curing, the appearance of the material is loose brown fiber before curing, and the material is changed into purple black after curing the gaseous iodine.
Fig. 5 is TEM and HRTEM images before and after curing of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in example 2 of the present invention, the first three images being the material before curing, and before curing, the zero-valent nano silver is loaded in nano particle form on the surface of the flying cotton fiber substrate and in the fiber gaps. In HRTEM, the interplanar spacing is 0.237nm, corresponding to the (111) crystal plane in elemental silver. The three figures are cured materials, silver iodide is distributed on the surfaces of the materials in a granular form, the inter-plane distance is 0.372nm in HRTEM, and the inter-plane distance corresponds to the (002) crystal plane of the silver iodide materials. It is confirmed that the silver iodide is produced by the reaction of silver and iodine in the material for curing the iodine.
Carrying out a gaseous iodine curing experiment on the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in the embodiments 1-9; the method comprises the following steps: the invention adopts the radioactive iodine simple substance instead of the radioactive iodine simple substance; firstly, placing excessive iodine simple substance at the bottom of a 500mL gas collection bottle, taking 20mg flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material (examples 1-9) to be placed in a 25mL crucible, placing the crucible in the gas collection bottle, covering a bottle cap, placing the gas collection bottle in a baking oven at 75-200 ℃, solidifying for 48h at maximum in different time intervals, taking out from the baking oven, cooling to room temperature, and measuring the content of solidified gaseous iodine of the modified cotton fiber according to a weight method. The calculation formula is as follows: q= (m 2 -m 1 )/m 1 X 100wt%, where Q (wt%) is the curing amount of iodine, m 1 (mg) and m 2 (mg) the weight of the flying cotton fiber loaded with zero-valent nano silver before and after curing the iodine of the gaseous iodine material is effectively fixed, and each curing material is subjected to three steps in parallelPerforming secondary curing experiments, and taking an average value; .
Fig. 6 is a curing graph of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in the embodiment 2 of the invention, and it can be seen that the material has extremely high adsorption efficiency to gaseous iodine, the curing amount of iodine is gradually increased along with the increase of the contact time, the adsorption balance can be basically reached within 4 hours, and the maximum adsorption amount is 1093mg/g. Fig. 9 is a curing graph of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in examples 2 and 7 of the present invention, and as can be seen from comparison of fig. 6 and 9, the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in example 7 has more excellent iodine curing effect than example 2, because silicate mixed powder is added into carbonized flying cotton fiber in example 7 to modify the flying cotton fiber, the specific surface area of carbonized flying cotton fiber is remarkably increased, the porosity of carbonized flying cotton fiber is increased, and the adsorption capacity of the flying cotton fiber loaded with zero-valent nano silver high-efficiency fixed gaseous iodine material to gaseous iodine is further improved. Wherein, the silicate mixed powder is subjected to thermal annealing treatment, so that the compactness of the gaps of the silicate mixed powder is improved.
FIG. 7 shows XPS patterns before and after the flying cotton fiber loaded with zero-valent nano silver and prepared in the embodiment 2 of the invention is cured, peaks of C1s, ag3d, O1s and I3d mainly appear in the material, successful loading of Ag and successful curing of I are again demonstrated, and electron displacement of Ag3d from 374.3eV,368.3eV to 374.0eV and 368.0eV is demonstrated from Ag 0 To Ag + An electron shift of O1s from 533.2eV,532.0eV to 532.8eV,531.6eV, and an increase in 532.8eV area, representing an increase in c=o bonds, presumably because Ag reacts with I to expose the binding sites for C-OH and Ag, and finally, the peak of I3d at 630.4eV,618.9eV indicates iodine as I after curing 3 The morphology of the silver-loaded fly wadding fiber is fixed in a solidified gaseous iodine material under the high-temperature condition of the silver-loaded fly wadding fiber.
Fig. 8 is a thermal weight loss graph of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material prepared in the embodiment 2 of the invention, and the material has a mass loss of less than 3% before 200 ℃ and excellent thermal stability, and can meet the operation requirement under the high-temperature condition as shown in the graph.
The number of equipment and the scale of processing described herein are intended to simplify the description of the present invention. Applications, modifications and variations of the present invention will be readily apparent to those skilled in the art.
Although embodiments of the present invention have been disclosed above, it is not limited to the details and embodiments shown and described, it is well suited to various fields of use for which the invention would be readily apparent to those skilled in the art, and accordingly, the invention is not limited to the specific details and illustrations shown and described herein, without departing from the general concepts defined in the claims and their equivalents.
Claims (6)
1. The preparation method of the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is characterized by comprising the following steps of:
step one, putting the fly wadding fibers into deionized water, ultrasonically cleaning, removing seeds, filtering, and drying in an oven;
step two, immersing the fly wadding fiber in the step one into silver nitrate solution with a certain concentration, and uniformly mixing by ultrasonic;
transferring the solution obtained in the step two into a hydrothermal reaction kettle with a polytetrafluoroethylene lining, carrying out hydrothermal carbonization, carrying out suction filtration on the carbonized material, and drying for later use;
reducing the carbonized fly-wadding fiber obtained in the step three in sodium borohydride solution with a certain concentration, filtering and drying after the reduction, and carrying out aluminum silicate modification treatment on the carbonized fly-wadding fiber, wherein the specific method comprises the following steps of:
s1, preparing modified layered aluminum silicate, and doping aluminum oxide nano powder into the modified layered aluminum silicate to obtain silicate mixed powder;
s2, carrying out thermal annealing treatment on the silicate mixed powder;
s3, adding the carbonized flying cotton fiber loaded with the zero-valent nano silver into absolute ethyl alcohol, magnetically stirring to obtain a suspension, adding silicate mixed powder after thermal annealing into the suspension, adding polyethylene glycol as a dispersing agent, stirring, dispersing, filtering and drying to obtain the carbonized flying cotton fiber mixed with aluminum silicate, pressing into a sheet, and then crushing to obtain the flying cotton fiber loaded with the zero-valent nano silver high-efficiency fixed gaseous iodine material;
in the step S1, the specific method for preparing the modified layered aluminum silicate and doping the aluminum oxide nano powder into the modified layered aluminum silicate comprises the following steps: adding layered aluminum silicate into absolute ethyl alcohol, and stirring to obtain a suspension, wherein the mass volume ratio of the layered aluminum silicate to the absolute ethyl alcohol is 1 g:30-100 mL; adding acrylic acid and cocoamidopropyl dimethyl betaine into the suspension, reacting for 2-24 hours at 70-80 ℃, adding aluminum oxide nano powder into the mixture, performing ultrasonic dispersion, wherein the ultrasonic frequency is 40-80 kHz, the ultrasonic time is 20-40 min, standing, filtering a sedimentation product, washing the sedimentation product with deionized water for multiple times, and drying to obtain silicate mixed powder; wherein the mass ratio of aluminum silicate to acrylic acid to cocoamidopropyl dimethyl betaine to aluminum oxide is 100:2-30:5-35:40-80;
in S2, the method for performing thermal annealing treatment on the silicate mixed powder includes: the silicate mixed powder is put into a high-temperature annealing furnace, nitrogen is introduced, the annealing temperature is 400-800 ℃, and the annealing time is 2-24 hours;
in the step S3, the magnetic stirring speed is 1200-3000 r/min, and the mass ratio of the carbonized fly-flocculation fiber to the silicate mixed powder to the polyethylene glycol is 30:1-3:5.
2. The method for preparing the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material according to claim 1, wherein the flying cotton fiber in the first step is one or more of non-pretreated poplar fiber and catkin fiber, and is dried in an oven at 25-85 ℃ after ultrasonic cleaning and seed removal for 5 hours, wherein the ultrasonic cleaning temperature is not higher than 60 ℃; the mass volume ratio of the fly wadding fiber to the deionized water is 1g to 1000mL.
3. The method for preparing the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material, which is characterized in that the concentration of silver nitrate solution in the second step is 0.01-50.0 g/L, the mass ratio of the flying wadding fiber to the silver nitrate is 1:0.01-1, the ultrasonic mixing time is 0.1-96 h, and the ultrasonic mixing temperature is 50 ℃.
4. The method for preparing the flying wadding fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material, which is disclosed in claim 1, is characterized in that the hydrothermal temperature in the step three is controlled to be 45-200 ℃, the hydrothermal carbonization time is 2h, and the mass-volume ratio of the flying wadding fiber to the polytetrafluoroethylene lining is 1g:500mL.
5. The method for preparing the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material, which is characterized in that in the fourth step, the sodium borohydride concentration is 0.01-15 mol/L, the mass ratio of the flying cotton fiber to the sodium borohydride is 10:57, the reduction temperature is 20-90 ℃, and the drying temperature in a vacuum drying oven after suction filtration is 75 ℃.
6. The application of the material prepared by the method for preparing the flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material according to any one of claims 1-5, wherein the prepared flying cotton fiber loaded zero-valent nano silver high-efficiency fixed gaseous iodine material is applied to the field of solidification of gaseous iodine.
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