Free radical controllable-release defect coordination metal-organic framework, and preparation method and application thereof

A technology of coordinating metals and organic frameworks, applied in water treatment parameter control, chemical instruments and methods, organic compounds/hydrides/coordination complex catalysts, etc. , Unable to achieve controllable release of free radicals, single content of catalytic active sites, etc., to achieve the effects of easy process production, efficient treatment, and simple preparation process

Active Publication Date: 2020-04-07
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003] The MOFs-based advanced oxidation system can provide a stable and single catalytic active site for generating free radicals, which cannot achieve the controlled release of free radicals, and cannot effectively play the role of free radicals in oxidative degradation of organic wastewater.
The research on the catalytic degradation of organic wastewater by MOFs advanced oxidation system found that the content of defect-co

Method used

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  • Free radical controllable-release defect coordination metal-organic framework, and preparation method and application thereof
  • Free radical controllable-release defect coordination metal-organic framework, and preparation method and application thereof
  • Free radical controllable-release defect coordination metal-organic framework, and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0033] This example provides a method for preparing a defect-coordinated metal-organic framework with controlled release of free radicals, which includes the following steps:

[0034] (1) Dissolve 0.5 mmol of ferrous chloride tetrahydrate and 0.5 mmol of terephthalic acid in 130 mmol of N,N-dimethylformamide and stir for 20 minutes to obtain a mixed solution;

[0035] (2) Add 10 mmol acetic acid to the mixed solution in step (1) and continue stirring under N 2 Deoxygenate in the atmosphere for 30 minutes to obtain a reaction mixture, transfer the reaction mixture to a 25 mL lined polytetrafluoroethylene autoclave reactor and react at 150°C for 12 hours to obtain a post-reaction mixture;

[0036] (3) After the reaction is finished, wait for the reaction kettle to cool down to room temperature and use a high-speed centrifuge to analyze the product, and use 120mL N,N-dimethylformamide to wash the solid product twice, each washing time is 45min, and continue to use methanol to was...

Embodiment 2

[0041] This example provides a method for preparing a defect-coordinated metal-organic framework with controlled release of free radicals, which includes the following steps:

[0042] (1) Dissolve 0.5 mmol of ferrous chloride tetrahydrate and 0.5 mmol of terephthalic acid in 260 mmol of N,N-dimethylformamide and stir for 20 minutes to obtain a mixed solution;

[0043] (2) Add 15 mmol n-butyric acid to the mixed solution in step (1) and continue to stir for 20 min and 2 Deoxygenate in the atmosphere for 30 minutes to obtain a reaction mixture, transfer the reaction mixture to a 25 mL lined polytetrafluoroethylene autoclave reactor and react at 150°C for 12 hours to obtain a post-reaction mixture;

[0044](3) After the reaction is finished, wait for the reaction kettle to cool down to room temperature and use a high-speed centrifuge to analyze the product, and use 120mL N,N-dimethylformamide to wash the solid product twice, each washing time is 45min, and continue to use methano...

Embodiment 3

[0049] This example provides a method for preparing a defect-coordinated metal-organic framework with controlled release of free radicals, which includes the following steps:

[0050] (1) Dissolve 0.5 mmol ferrous chloride tetrahydrate and 0.5 mmol terephthalic acid in 320 mmol N,N-dimethylformamide and stir for 20 minutes to obtain a mixed solution;

[0051] (2) Add 20 mmol n-octanoic acid to the mixed solution in step (1) and continue stirring for 20 min and 2 Deoxygenate in the atmosphere for 30 minutes to obtain a reaction mixture, transfer the reaction mixture to a 25 mL lined polytetrafluoroethylene autoclave reactor and react at 150°C for 12 hours to obtain a post-reaction mixture;

[0052] (3) After the reaction is finished, wait for the reaction kettle to cool down to room temperature and use a high-speed centrifuge to analyze the product, and use 120mL N,N-dimethylformamide to wash the solid product twice, each washing time is 45min, and continue to use methanol to w...

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Abstract

The invention discloses a free radical controllable-release defect coordination metal-organic framework, and a preparation method and an application thereof. The preparation method comprises the following steps: introducing monocarboxylic acid to partially replace a polybasic carboxylic acid organic ligand to participate in synthesis of a skeleton structure when ferrous ions are coordinated with the polybasic carboxylic acid organic ligand, carrying out washing and vacuum thermal activation to remove the monocarboxylic acid in order to obtain a metal-organic framework material with adjustabledefect coordination catalytic activity iron center content, and adjusting the exposure degree of defect coordination active sites to realize controllable release of free radicals during catalytic activation of persulfate. The high-proportion defect coordination metal-organic framework material is prepared by the method, and the content of the defect coordination iron catalytic activity center of the product can be regulated. The synthesized metal-organic framework material can be used for efficiently treating various non-degradation organic wastewater as a catalyst of heterogeneous activated persulfate, and has the advantages of simple synthesis steps, controllable release of free radicals, high catalytic activity, good stability, good recyclability and the like.

Description

technical field [0001] The invention belongs to the technical field of functional materials, and in particular relates to a defect-coordinated metal-organic framework with controllable release of free radicals, a preparation method and application thereof. Background technique [0002] Metal Organic Frameworks (MOFs) are new porous materials with specific periodic network structures formed by the self-assembly of metal center ions and organic bridging ligands. The material has the characteristics of high specific surface area, tunable channel structure and diversity of metal centers and organic bridging ligands, and has wide application potential in the field of catalysis. [0003] The advanced oxidation system based on MOFs can provide a stable and single content of catalytic active sites for generating free radicals, which cannot realize the controlled release of free radicals, and cannot effectively play the role of free radicals in oxidative degradation of organic wastew...

Claims

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Application Information

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IPC IPC(8): C08G83/00B01J31/22B01J35/10C02F1/72C02F101/34C02F101/36C02F103/30
CPCB01J31/2208B01J35/1052B01J35/1061C02F1/725C02F2101/34C02F2101/36C02F2103/30C02F2209/08C08G83/008
Inventor 王艳黄梅万金泉马邕文闫志成
Owner SOUTH CHINA UNIV OF TECH
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