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Cationic organic polymer as well as preparation method and application thereof

A cationic, polymer technology, applied in the field of chemistry, which can solve problems such as poor selectivity, large impact, and limited application

Active Publication Date: 2018-06-01
SUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Inorganic materials such as layered double hydroxide (LDH) (Kang, M.J.; Rhee, S.W.; Moon, H.Radiochim Acta, 1996.75 (3), 169-174), although the cost of this type of material is low, but its effect on TcO 4 - / ReO 4 - The adsorption capacity is low, the selectivity is poor, and the competing ions especially CO 3 2- The impact is large, and it is not acid-resistant
MOFs such as SCU-100 (Sheng, D.; Zhu, L., Xu, C.; Xiao, C.; Wang, Y.; Wang, Y.; Wang, Y,; Chen, L,; Diwu, J, ; Chen, J,; Chai, Z,; Albrecht-Schmitt, T.E.Environ.Sci.Technol.2017.51(6), 3471-3479), can efficiently adsorb TcO 4 - / ReO 4 - , but due to the instability of the Ag-N coordination bond, the material is prone to crystal structure collapse under high acidity conditions
Ion exchange resins, such as Purolite A530E and A532E, are cationic materials containing two types of quaternary ammonium salt functional groups, which can remove TcO with high selectivity 4 - / ReO 4 - , but the removal kinetics of this type of material is slow, and under irradiation conditions, the functional groups will be broken, and the removal capacity will decrease, which limits its application in high-level waste liquid

Method used

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  • Cationic organic polymer as well as preparation method and application thereof
  • Cationic organic polymer as well as preparation method and application thereof
  • Cationic organic polymer as well as preparation method and application thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0041] With tetrakis (1-imidazolylphenyl) ethylene and α, α-dibromo-p-xylene as raw materials, the reaction is carried out according to the following reaction scheme, and the specific method is as follows:

[0042]

[0043] Take a 30 mL microwave tube, add 0.134 g (0.225 mmol) of substance A (tetrakis(1-imidazolylphenyl)ethylene) and 16 mL of N,N'-dimethylformamide (DMF), stir until uniformly dispersed , then 0.119 g (0.45 mmol) of substance B (α,α-dibromo-p-xylene) was added and stirred until dissolved. Put the microwave tube containing the above mixture into a microwave reactor, and react at 100° C. for 4 hours. After centrifugation, a yellow solid product was obtained (yield: 61%).

[0044] The above yellow solid was washed 3 times with 20 ml of DMF, 2-3 times with ethanol, and 3 times with water. The washed solid was freeze-dried to obtain a yellow powder, which was named SCU-POP-1-Br.

[0045] Soak SCU-POP-1-Br in a saturated sodium chloride solution, the chloride i...

Embodiment 2

[0048] Take a 30 mL microwave tube, add 0.134 g (0.225 mmol) of tetrakis(1-imidazolylphenyl)ethylene and 16 mL of N,N-dimethylformamide (DMF), stir until uniformly dispersed, then add 0.1071 g (0.3 mmol) of 1,3,5-tris(bromomethyl)benzene was stirred until dissolved, the microwave tube containing the above mixture was put into a microwave reactor, and reacted at 100° C. for 4 hours. After centrifugation, a yellow solid product was obtained (yield: 75%).

[0049] The above yellow solid was washed 3 times with 20 ml of DMF, 2-3 times with ethanol, and 3 times with water. The obtained solid was freeze-dried to obtain a yellow powder, which was named SCU-POP-2-Br.

[0050] Soak SCU-POP-2-Br in a saturated sodium chloride solution, the chloride ions in the solution undergo an ion exchange reaction with the bromide ions in SCU-POP-2-Br, centrifuge, wash 3 times with water and freeze-dry to obtain Obtain cationic organic polymer, it is named as SCU-POP-2-Cl, hereinafter referred to ...

Embodiment 3

[0052] Take a 30 mL microwave tube, add 0.134 g (0.225 mmol) of tetrakis(1-imidazolylphenyl)ethylene and 16 mL of N,N-dimethylformamide (DMF), stir until uniformly dispersed, then add 0.1026 g (0.225 mmol) of 1,2,4,5-tetrakis(bromomethyl)benzene was stirred until dissolved, the microwave tube containing the above mixture was put into a microwave reactor, and reacted at 100° C. for 4 hours. After centrifugation, a yellow solid product was obtained (yield: 88%).

[0053] The above yellow solid was washed 3 times with 20 ml of DMF, 2-3 times with ethanol, and 3 times with water. The yellow powder obtained after freeze-drying the obtained solid was named SCU-POP-3-Br.

[0054] Soak SCU-POP-3-Br in saturated sodium chloride solution, centrifuge, wash 3 times with water and then freeze-dry to obtain a cationic organic polymer, which is named SCU-POP-3-Cl, hereinafter referred to as SCU-POP -3, its NMR spectrum is as follows Figure 10 shown.

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Abstract

The invention relates to a cationic organic polymer which is obtained by performing a polymerization reaction on a compound containing imidazole groups or pyridine groups and halohydrocarbon in an organic solvent at the temperature of 0-300 DEG C for 0-24h, wherein the ratio of the imidazole or pyridine groups to halogens is 1: 1; the compound containing the imidazole groups or pyridine groups isselected from the following chemical formulas; R1 is an imidazole group or pyridine group, and m, n, p and r are independently selected from integers that are greater than 0; the halohydrocarbon is selected from the following chemical formulas; X is independently selected from F, Cl, Br or I, and m is any integer which is 0 or greater. The invention also discloses application of the cationic organic polymer prepared by the preparation method, which serves as an HTcO4 radical and / or a perrhenic acid radical, in an adsorbent.

Description

technical field [0001] The invention relates to the field of chemistry, in particular to a cationic organic polymer and its preparation method and application. Background technique [0002] 99 Tc is a long half-life (2.13×10 5 Year) can produce fission products of beta rays. About 1 ton of spent fuel contains 600 grams to 1 kilogram of 99 Tc. During the long-term storage of high-level radioactive waste, 99 Tc will have a great impact on the environment: it is usually expressed as pertechnetate (TcO) in aqueous solution 4 - ) form, and has high water solubility and mobility. Due to its negative charge, it is difficult to be adsorbed by general minerals or rocks, and it is easy to enter the biosphere with the migration of groundwater, thereby causing pollution to the environment. At present, vitrification is the main form of solidification of nuclear waste, but during the high-temperature curing process, technetium forms volatile oxides Tc with oxygen at high temperatur...

Claims

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Application Information

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IPC IPC(8): C08G73/06B01J20/26B01J20/30B01D15/08
CPCB01D15/08B01J20/262B01J20/265C08G73/0616C08G73/0627
Inventor 王殳凹李杰肖成梁
Owner SUZHOU UNIV
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