Carbon-based supramolecular recognition material and preparation method thereof and application of carbon-based supramolecular recognition material in adsorption and separation of Cs

A supramolecular and carbon-based technology, applied in chemical instruments and methods, other chemical processes, alkali metal oxides/hydroxides, etc., can solve the problem of low selectivity and adsorption capacity, small particle size of supramolecular materials, organic reagents Problems such as large amount of use, to achieve the effect of high partition coefficient and selectivity, simple synthesis method, and high practical value

Pending Publication Date: 2018-10-09
EAST CHINA UNIV OF TECH
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Problems solved by technology

The above solvent extraction process has high extraction capacity and strong selectivity for Cs(I), but has the following disadvantages: (1) the extraction agent, diluent and phase modifier are easily hydrolyzed and radiolyzed in a high-acid, strong-irradiated environment, which affects the extraction A large amount of secondary high-level radioactive waste liquid is produced; (2) in order to improve the separation coefficient of cesium, multi-step extraction, washing and stripping are required, the scale of equipment is large, and the amount of organic reagents used is large
Another example is to use the same method to load HexylCalix[4], CalixBNapC6 and BiPCalix[4]C6 to SiO 2 -P, the preparation of silicon-based supramolecular recognition materials, and proposed PCEC ( P artition of C esium by E xtraction C chromatography) extraction chromatographic separation process, the optimal adsorption acidity for Cs(I) is 3.0M, and the distribution coefficient reaches 41.37cm 3 g -1 、18.01cm 3 g -1 and 59.43cm 3 g -1 (Sep.Purif.Technol.,2016,171:17-25,Chem.Eng.J.,2010,159:58-66,Solvent Extr.Ion Exc.,2010,28:526-542), there are following defici

Method used

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  • Carbon-based supramolecular recognition material and preparation method thereof and application of carbon-based supramolecular recognition material in adsorption and separation of Cs
  • Carbon-based supramolecular recognition material and preparation method thereof and application of carbon-based supramolecular recognition material in adsorption and separation of Cs
  • Carbon-based supramolecular recognition material and preparation method thereof and application of carbon-based supramolecular recognition material in adsorption and separation of Cs

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preparation example Construction

[0035] Such as figure 1 As shown, the preparation method of the carbon-based supramolecular recognition material provided by the embodiment of the present invention includes the following steps:

[0036] S101: Polymerize the polymer in millimeter-scale macroporous-mesoporous carbon spheres to form a carbon-based carrier, and the mass percentage of the polymer in the carbon-based carrier is 0-10%;

[0037] S102: Using carbon-based carrier and calix[4]arene double crown-6 as raw materials, a carbon-based supramolecular recognition material was prepared by vacuum solvent evaporation-induced self-assembly method.

[0038] The preparation method of the carbon-based carrier of the present invention is:

[0039] (1) Concentrated nitric acid was added to millimeter-scale macroporous-mesoporous carbon spheres, reacted at 120°C for 4h, cooled to room temperature, washed until neutral, and dried at 80°C for 4h.

[0040] (2) Under vacuum conditions, add polymer monomers and correspondi...

Embodiment 1

[0053] Embodiment 1 carbon-based supramolecular recognition material

[0054] Add 5g of millimeter-sized macroporous-mesoporous carbon spheres to 4mL of concentrated nitric acid, react at 120°C for 4h, cool to room temperature, wash until neutral, and dry at 80°C for 4h;

[0055] 0.212 g m / p-formylstyrene, 0.0376 g m / p-divinylbenzene, 0.675 g methyl Sodium benzoate, 0.426g dioctyl phthalate, 0.035g 1,1-dicyclohexylamine-1-carbonitrile mixture and 0.035g a,a-azobisisobutyronitrile, and spin at room temperature Steam for 90 minutes, then raise the temperature to 50°C for 120 minutes. and in N 2 Under protective conditions, move to a three-necked flask, continue to react at 90°C for 24h, and then cool to room temperature.

[0056] Wash and filter the above product with acetone and methanol, repeat three times, put it into a vacuum oven and dry at 50°C for 24 hours to obtain the MMCs-P carbon-based material, weigh 2.0g of MMCs-P and add 80mL of methanol, shake at constant tempe...

Embodiment 2

[0057] The preparation of embodiment 2 carbon-based carrier

[0058] Add 5g of millimeter-sized macroporous-mesoporous carbon spheres to 4mL of concentrated nitric acid, react at 120°C for 4h, cool to room temperature, wash until neutral, and dry at 80°C for 4h;

[0059] Under vacuum conditions, with 1,2,3-trichloropropane and m-xylene as solvents, m / p-formylstyrene, m / p-divinylbenzene, sodium methylbenzoate, Dioctyl phthalate, 1,1-dicyclohexylamine-1-carbonitrile mixture and a,a-azobisisobutyronitrile, and rotate at room temperature for 90min, then raise the temperature to 50°C to continue 120min. and in N 2 Under protective conditions, move to a three-necked flask, continue to react at 90°C for 24h, and then cool to room temperature.

[0060] Wash and filter the above product with acetone and methanol, repeat three times, put it in a vacuum oven and dry it at 50°C for 24 hours to obtain MMCs-P-x carbon-based material, where x represents the mass of styrene-divinylbenzene ...

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Abstract

The invention belongs to the technical field of nuclear fuel post-treatment and discloses a carbon-based supramolecular recognition material and a preparation method thereof and application of the carbon-based supramolecular recognition material in adsorption and separation of Cs. A polymer is polymerized to millimeter-level macroporous-mesoporous carbon spheres to form a carbon-based carrier; thepolymer in a carbon-based carrier has mass percentage of 0-10%; the carbon-based carrier and calix[4]-arene-biscrown-6 are used as raw materials subjected to vacuum solvent evaporation induced self-assembly to prepare the carbon-based supramolecular recognition material; the mass of the carbon-based carrier in the carbon-based supramolecular recognition material is 0.5-40 times that of calix[4]-arene-biscrown-6; the calix[4]-arene-biscrown-6 has a structural formula shown as in (1). The carbon-based supramolecular recognition material disclosed herein has the structure well retained in a strong acid solution, has excellent adsorption selectivity for cesium ions, and is applicable to high-selectivity adsorption separation of cesium from strong-acidity high-emission waste liquid.

Description

technical field [0001] The invention belongs to the technical field of nuclear fuel post-processing, and in particular relates to a carbon-based supramolecular recognition material, a preparation method thereof and an application of adsorption and separation of Cs. Background technique [0002] The treatment and disposal of high level liquid waste (HLLW) is one of the key links in nuclear fuel reprocessing engineering, and it is also a worldwide problem, which is of great significance to the sustainable development of nuclear power. HLLW contains a large number of strong radionuclides, among which, 135 Cs has a long half-life, is easy to migrate, and has great potential harm to the environment; 137 Although Cs has a short half-life, it will release a lot of heat during the decay process, which is one of the most dangerous elements that affect the safe disposal of solidified bodies. If it can be separated, it can not only reduce the volume of the solidified body, shorten th...

Claims

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Application Information

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IPC IPC(8): B01J20/26B01J20/28B01J20/30G21F9/12
CPCB01J20/20B01J20/26B01J20/28004B01J20/28019G21F9/12
Inventor 张志宾董志敏刘云海曹小红戴荧王有群花榕柳和生
Owner EAST CHINA UNIV OF TECH
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