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Method for constructing hybrid catalyst and cascade degradation of organophosphorus nerve poison by fixing palladium and organophosphorus hydrolase by using COFs

A nerve agent and organophosphorus technology, applied in the field of nanomaterials, can solve the problems of inconsistent catalytic conditions, unstable recovery of ultrafine Pd nanoparticles and organophosphorus hydrolase, etc., and achieve the effect of complete degradation and reduced loss.

Active Publication Date: 2021-06-01
HEBEI UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] Therefore, a highly stable and modifiable COFs was selected as the carrier for the co-immobilization of ultrafine Pd nanoparticles and organophosphate hydrolase, which overcomes the inconsistency between the catalytic conditions of Pd and organophosphate hydrolase, and realizes the cascade degradation of organophosphate nerve agents. , At the same time, it solves the problems of instability and difficult recovery of ultrafine Pd nanoparticles and organophosphate hydrolase

Method used

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  • Method for constructing hybrid catalyst and cascade degradation of organophosphorus nerve poison by fixing palladium and organophosphorus hydrolase by using COFs
  • Method for constructing hybrid catalyst and cascade degradation of organophosphorus nerve poison by fixing palladium and organophosphorus hydrolase by using COFs
  • Method for constructing hybrid catalyst and cascade degradation of organophosphorus nerve poison by fixing palladium and organophosphorus hydrolase by using COFs

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0042] Example 1: Using COFs to immobilize palladium and organophosphate hydrolase to construct a hybrid catalyst, the preparation process is as follows:

[0043]

[0044] 1) Using a monomer with a triazine group and a monomer with a hydroxyl group, a covalent organic framework material COFs-OH containing a hydroxyl group is prepared by a hot solvent method; the specific process is:

[0045] 0.26mmol of 2,4,6-tris(4-aminophenyl)-1,3,5-triazine, 0.39mmol of 2,5-dihydroxyterephthalaldehyde, 5.1mL of mesitylene, 0.9 Add mL of dioxane and 0.6 mL (6mol / L) of acetic acid into the pressure-resistant tube, sonicate for 15 minutes to fully disperse the mixture, then vacuumize to remove the air, and then react in an oil pan at 120°C for 3 days. After completion, a reddish-brown precipitate is obtained; the reddish-brown solid is separated and purified, that is, first washed with dioxane three times, then washed with N,N-dimethylformamide until there is no turbidity, and finally washe...

Embodiment 2

[0056] Embodiment 2: Effect of reaction temperature and sodium borohydride addition on the activity of cascade degradation methyl parathion

[0057] Add 5 mg of the hybrid catalyst prepared in Example 1 (fixed for 8 h), 1.44 μmol of methyl parathion and a certain amount of sodium borohydride to 1.5 mL of Tris-HCl buffer (50 mM, pH=9) In the reaction at a certain temperature, the reaction temperature and the addition of sodium borohydride in the system were optimized by measuring the amount of 4-AP generated per unit time. When the sodium borohydride addition amount is 22.5 mg, the cascade degradation activity when the reaction temperature is 20 ° C, 30 ° C, 40 ° C, 50 ° C, 60 ° C, 70 ° C, 80 ° C and 90 ° C is as follows Figure 9 As shown, when the reaction temperature is 70°C, the highest degradation activity is 8.372μM / min / g. Taking the preferred reaction temperature of 70°C, the cascade degradation activity is as Figure 10 As shown, the degradation rate is the largest wh...

Embodiment 3

[0058] Example 3: 5 mg of the hybrid catalyst prepared in Example 1 (fixed time of 8 h), 1.44 μmol of methyl parathion and 18.75 mg of sodium borohydride were put into 1.5 mL of pH=9, and the concentration was 50 mM In Tris-HCl buffer, react at 70°C. By monitoring the content of 4-AP in the reaction system at different times of degradation to observe the degradation of organophosphorus nerve agents, from Figure 11 It can be observed that methyl parathion can be completely degraded to 4-AP in 50min.

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Abstract

The invention discloses a method for constructing a hybrid catalyst and cascade degradation of an organophosphorus nerve poison by fixing palladium and organophosphorus hydrolase by using COFs (Covalent Organic Frameworks), and the method comprises the following steps of: preparing a hydroxyl-containing covalent organic framework material from a monomer with triazinyl and a monomer with hydroxyl by using a hot solvent method; fixing palladium in situ into holes of the covalent organic framework material by using a two-phase method, and then carrying out carboxylation modification and activation; and finally, performing mixing with an OPH solution for enzyme immobilization to obtain the hybrid catalyst. The palladium nanoparticles and the organophosphorus hydrolase are co-immobilized on the covalent organic framework, so that the stability of the palladium nanoparticles and the organophosphorus hydrolase in the use process is improved. Specifically, the palladium nanoparticles are located in the pores, the enzyme is located on the surface, and the structure can ensure the accessibility of each chemical component and avoid mutual inhibition of different catalysts. The constructed hybrid catalyst is used for cascade degradation of the organophosphorus nerve poison, the degradation efficiency is high, degradation is more thorough, and the hybrid catalyst can be repeatedly used.

Description

technical field [0001] The invention belongs to the technical field of nanometer materials, and in particular relates to a method for using COFs to immobilize palladium and organophosphate hydrolase to construct a hybrid catalyst and to cascade degrade organophosphate nerve agents. Background technique [0002] Organophosphorus nerve agents are widely used as pesticides to kill agricultural pests. Organophosphate nerve agents can chemically bond with acetylcholinesterase in organisms to inactivate acetylcholinesterase, thereby destroying the nervous system to achieve the purpose of killing insects. Although organophosphorus nerve agents can be used as insecticides to serve human beings, their pollution to the environment is also a potential threat to human beings. At present, a variety of technologies have been developed for the degradation of organophosphate nerve agents. Among them, organophosphate hydrolase, as a biocatalyst, can hydrolyze organophosphate nerve agents suc...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/06A62D3/35A62D3/02C12N11/02A62D101/04A62D101/26
CPCB01J31/069B01J31/003A62D3/02A62D3/35C12N11/02C12N9/16A62D2101/04A62D2101/26Y02P20/584
Inventor 姜艳军赵浩王涵熙刘冠华孟瑞袁野郝凯娜周丽亚
Owner HEBEI UNIV OF TECH
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