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DNA hybrid catalyst/MOFs composite material and preparation and application thereof

A composite material and catalyst technology, which is applied in the preparation of carbon-based compounds, organic compound/hydride/coordination complex catalysts, organic compound preparation, etc. It can solve the problems of deactivation, variability, and complicated preparation of immobilized materials. , to achieve good high temperature resistance, good resistance to organic solvents, and increase the value of recycling and reuse

Inactive Publication Date: 2020-05-08
EAST CHINA NORMAL UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] Aiming at the deficiencies of natural enzymes and prior art, the purpose of the present invention is to solve the problem of complicated preparation of immobilized materials of DNA hybrid catalysts, and overcome the deficiencies of variability and inactivation of DNA hybrid catalysts in the process of immobilization; Metal-organic frameworks (MOFs) synthesized in aqueous phase with good biocompatibility as immobilization materials for DNA hybrid catalysts

Method used

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  • DNA hybrid catalyst/MOFs composite material and preparation and application thereof
  • DNA hybrid catalyst/MOFs composite material and preparation and application thereof
  • DNA hybrid catalyst/MOFs composite material and preparation and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1G4

[0073] Preparation of Example 1G4DNA / MOFs composite material (G4DNA@ZIF-90)

[0074] (1) Mix the buffer of single-stranded DNA rich in guanine G with potassium chloride KCl buffer and hemin Hemin buffer to obtain the DNA hybrid catalyst G4DNA;

[0075] (2) the aqueous solution of the G4DNA that step (1) obtains, imidazole-2-formaldehyde is mixed with the aqueous solution of zinc nitrate (synthetic method reaction mechanism diagram is as follows figure 1 shown), to obtain the DNA hybrid catalyst / MOFs composite material, the SEM image of the G4DNA / MOFs composite material is shown in figure 2 shown.

Embodiment 2

[0076] Example 2G4DNA / MOFs Composite Material Size Selective Catalysis of Pyrogallol and Guaiacol

[0077] Detect the catalytic activity of the G4DNA / MOFs composite material (G4DNA@ZIF-90) prepared in Example 1 of the present invention in aqueous solution:

[0078] H 2 o 2 (1.9 mM) was added to 1 mL Tris-HCl buffer (10 mM, pH=7) containing about 4 mg G4DNA@ZIF-90 and 10 mM pyrogallol (THB) or 10 mM guaiacol to initiate the reaction. Measure the absorbance value of the supernatant product at various time points of the reaction using a UV-Vis spectrophotometer, as image 3 The initial rate diagram of the product shown in b shows that the molecular sizes of pyrogallol and guaiacol are relatively small and similar. Using pyrogallol as a substrate, the initial rate of pyrogallol to catalyzed red bisphenols by G4DNA@ZIF-90 is about It is 68% of free G4DNA catalysis; and use guaiacol as substrate and no product is observed, this is because the molecular size of the catalyzed produ...

Embodiment 3

[0079] Example 3G4 The activity of DNA / MOFs composite materials in different catalytic cycles, and the recovery of activity after soaking in different solutions

[0080]Detect the catalytic activity recovery ability of the G4DNA / MOFs composite material (G4DNA@ZIF-90) prepared in Example 1 of the present invention in aqueous solution: as Figure 4 a shows the comparison of the relative activities of G4DNA / MOFs composites for catalyzing pyrogallol (I represents the first catalytic cycle; II represents the second catalytic cycle; III represents the third catalytic cycle); after three catalytic cycles , the catalytic activity of G4DNA@ZIF-90 dropped to about 20% of the initial activity. The G4DNA@ZIF-90 particles with reduced activity were immersed in Tris-HCl buffer solution at 88 °C, and after cooling, the solids were sequentially soaked to K + and Hemin buffer solution, the activity recovery step is the same as the synthesis process of G4DNA. After treatment, G4DNA@ZIF-90 rec...

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Abstract

The invention discloses a preparation method of a DNA hybrid catalyst (G4DNA) / MOFs composite material. The preparation method comprises the following steps: sequentially mixing a guanine (G)-rich single-stranded DNA buffer solution with a potassium chloride (KCl) buffer solution and a hemin buffer solution to obtain a DNA hybrid catalyst (G4DNA); and mixing a certain amount of G4DNA with an aqueous imidazole-2-formaldehyde solution (having a concentration of 200 mM and containing 2 wt% of a stabilizer polyvinylpyrrolidone (PVP)) at room temperature, adding an aqueous solution (with a concentration of 416 mM) of zinc nitrate, and carrying out stirring to obtain the DNA hybrid catalyst / MOFs composite material, namely G4DNA@ZIF-90. The preparation method has the advantages of simple reactionconditions, few synthesis steps, short time consumption and low production cost. The preparation method of the DNA hybrid catalyst / MOFs composite material is used for applying artificial enzyme to thefield of industrial catalysis, and has potential application value.

Description

technical field [0001] The invention belongs to the field of industrial catalysis of biocatalysts, and relates to a DNA hybrid catalyst / MOFs composite material and its preparation and application. Background technique [0002] DNA-based hybrid catalysts are biocatalysts formed by the covalent or supramolecular combination of DNA (double-stranded DNA, G-quadruplex DNA and mirror DNA) and transition metal complexes. DNA hybrid catalysts are currently used in a variety of applications in the field of organic synthesis, such as Diels-Alder reaction, Friedel-Crafts reaction, Michael addition and so on. Compared with natural enzymes, DNA hybrid catalysts have advantages such as biodegradability, small size, low cost, easy in situ synthesis, higher stability, and compatibility with existing immobilization techniques. Therefore, the use of DNA hybrid catalysts as a substitute for natural enzymes for industrial catalysis is of great significance for expanding the practicability of D...

Claims

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Application Information

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IPC IPC(8): B01J31/22C07C45/52C07C49/747
CPCB01J31/1691B01J31/2217B01J31/0244C07C45/52C07C2602/12B01J2531/0213B01J2531/26C07C49/747
Inventor 裴昊李丽钟慧业
Owner EAST CHINA NORMAL UNIVERSITY
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