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Ferrous-base metal organic framework material, normal-pressure synthesis method thereof and method of catalytically activating persulfate to treat organic pollutants

A technology of organic pollutants and organic skeletons, applied in the direction of organic compound/hydride/coordination complex catalysts, water pollutants, oxidized water/sewage treatment, etc., can solve the problem of unstable activation effect, harsh synthesis conditions, pH value Large impact and other issues, to achieve broad practical application prospects, low requirements for synthesis equipment, and good durability

Active Publication Date: 2019-03-19
广东仁安生态有限公司
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] The purpose of the present invention is to solve the problems of harsh synthesis conditions of metal organic framework materials, low activation efficiency of traditional catalysts in the activated PS system, great influence of pH value, easy to cause secondary pollution, unstable activation effect of existing metal organic framework materials, etc. , successfully achieved good results in the experiment of activating persulfate to degrade POPs pollutants under a wide range of pH conditions using a heterogeneous catalyst synthesized at atmospheric pressure with a high proportion of ferrous-based metal-organic framework materials (Fe(II)-MOFs). solution effect

Method used

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  • Ferrous-base metal organic framework material, normal-pressure synthesis method thereof and method of catalytically activating persulfate to treat organic pollutants
  • Ferrous-base metal organic framework material, normal-pressure synthesis method thereof and method of catalytically activating persulfate to treat organic pollutants
  • Ferrous-base metal organic framework material, normal-pressure synthesis method thereof and method of catalytically activating persulfate to treat organic pollutants

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0038] In this example, the effects of different pH values ​​on the catalytic activation of PS to degrade DBP by Fe(II)-MOFs were compared.

[0039] (1) Preparation of Fe(Ⅱ)-MOFs: Take terephthalic acid (1.065g) and FeCl respectively 2 4H 2 O (2.65g) was placed in a 500ml three-necked flask, and 250ml of N,N-dimethylformamide was added to dissolve it, then 30ml of methanol was added, and 8ml of hydrofluoric acid was added dropwise to make the solution light green, and then dried with The nitrogen gas removes dissolved oxygen from the mixture. The synthesis conditions were controlled to the following five types: 140°C&24h, 140°C&18h, 140°C&12h, 120°C&24h and 100°C&24h, respectively named as Fe(Ⅱ)-MOFs-1 / 2 / 3 / 4 / 5, in Cool to room temperature under a dry nitrogen atmosphere. After the three-necked flask is cooled, transfer the reacted mixture to a centrifuge tube, and centrifuge at 10,000rpm for 10 minutes to separate the solid; then pour the solid into a beaker, wash with meth...

Embodiment 2

[0047] In this example, the effects of different pH values ​​on the catalytic activation of PS to degrade DBP by Fe(II)-MOFs were compared.

[0048] (1) Preparation of Fe(Ⅱ)-MOFs: Take terephthalic acid (1.065g) and FeCl respectively 2 4H 2 O (2.65g) was placed in a 500ml three-necked flask, and 250ml of N,N-dimethylformamide was added to dissolve it, then 30ml of methanol was added, and 8ml of hydrofluoric acid was added dropwise to make the solution light green, and then dried with The nitrogen gas removes dissolved oxygen from the mixture. The mixture was heated to 140° C., stirred under a dry nitrogen atmosphere for 24 h, then stopped heating, and cooled to room temperature under a dry nitrogen atmosphere. After the three-necked flask is cooled, transfer the reacted mixture to a centrifuge tube, and centrifuge at 10,000rpm for 10 minutes to separate the solid; then pour the solid into a beaker, wash with methanol for 1 hour, and centrifuge for 3 times. Put them into a v...

Embodiment 3

[0056] The present embodiment compares the different mol ratios of PS and DBP (n Na 2 S 2 o 8 / n DBP=30, 50, 150, 200, 250, 300, 350) on the catalytic activation of Fe(Ⅱ)-MOFs.

[0057] (1) The preparation method of Fe(II)-MOFs is the same as step (1) in Example 2;

[0058] (2) The DBP solution of 0.018mmol / L is standby;

[0059] (3) Using conical flask as reactor, add 0.054, 0.090, 0.180, 0.270, 0.360, 0.450, 0.540mmol Na to the reactor 2 S 2 o 8 and 0.018mmol / L DBP 100mL, add 0.03g metal organic framework material to the reactor at the same time, place the Erlenmeyer flask in a shaker at 180rpm, react at normal temperature (25°C), and take samples for analysis at fixed points;

[0060] (4) Add 0.090mmol Na to the reactor 2 S 2 o 8 , other conditions are the same as (3);

[0061] (5) Add 0.180mmol Na to the reactor 2 S 2 o 8 , other conditions are the same as (3);

[0062] (6) Add 0.270mmol Na to the reactor 2 S 2 o 8 , other conditions are the same as (3); ...

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Abstract

The invention discloses a ferrous-base metal organic framework material, a normal-pressure synthesis method thereof and a method of catalytically activating persulfate to treat organic pollutants. Themethod includes: successfully synthesizing a heterogeneous catalyst high-proportion ferrous-base metal organic framework material (Fe(II)-MOFs); utilizing the characteristic that the metal organic framework is high in active site and catalytic activity to catalytically activate sulfate at normal temperature to generate sulfate radical to degrade persistent organic pollutants. The catalyst is easyto be recycled, still has good activating effect after being reutilized for several times and is an environment-friendly material. The method is suitable for various persistent organic pollutants, high in durability, short in catalysis time, convenient in operation, capable of having good degradation effect within a wide pH value range and great in application prospect of degrading the persistentorganic pollutants.

Description

technical field [0001] The invention belongs to the technical field of water pollution control, and in particular relates to a ferrous-based metal-organic framework material, a normal-pressure synthesis method thereof, and a method for treating organic pollutants by catalytically activating persulfate. Background technique [0002] Based on sulfate radical (SO4 - ·) advanced oxidation technology, due to its high efficiency in degrading pollutants, has received more and more attention and attention from researchers in the field of degrading persistent organic pollutants. In existing reports, photoactivation, heat activation, ultrasound, and metal ion activation are generally used to generate sulfate radicals for PS. However, traditional catalytic activation methods have low efficiency, are greatly affected by pH, and easily cause secondary pollution. However, it is difficult to be widely used in practical industry. The use of metal-organic frameworks as heterogeneous cataly...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/16B01J35/02C02F1/72C02F101/30B01J35/00
CPCC02F1/725B01J31/1691C02F2101/30B01J35/00B01J35/30
Inventor 万金泉池海远马邕文王艳
Owner 广东仁安生态有限公司
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