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Method for removing PPCPs in water by catalyzing H2O2 with MIL-100 (Fe/Mn) derivative

A technology of H2O2 and derivatives, applied in the field of water treatment, can solve the problems of iron sludge precipitation, activated carbon failure, narrow applicable pH range, etc., and achieve the effect of low preparation cost and high efficiency

Active Publication Date: 2021-01-15
HUAQIAO UNIVERSITY +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

For example, activated carbon adsorbs PPCPs. With the increase of adsorption and use time, activated carbon will gradually lose its effectiveness; it is difficult to cultivate a large number of microorganisms that can stably produce specific enzymes in traditional sewage treatment processes, so the effect of microbial treatment of PPCPs in sewage is not ideal; Chemical oxidation technology is often used as the most commonly used method to remove PPCPs in water due to its advantages of fast reaction rate, high removal rate and stable effect.
Among them, catalytic H 2 o 2 Oxidative removal of PPCPs is widely used, but traditional catalysts have a narrow applicable pH range, iron sludge precipitation, H 2 o 2 Disadvantages such as low utilization rate need to be addressed. 2 o 2 Catalysts for further development and optimization

Method used

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  • Method for removing PPCPs in water by catalyzing H2O2 with MIL-100 (Fe/Mn) derivative
  • Method for removing PPCPs in water by catalyzing H2O2 with MIL-100 (Fe/Mn) derivative
  • Method for removing PPCPs in water by catalyzing H2O2 with MIL-100 (Fe/Mn) derivative

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0033] Embodiment 1: Explore the preparation and characterization of MIL-100 (Fe / Mn) derivative catalyst material, the steps are as follows:

[0034] (1) Add 2.50 g of ferrous sulfate heptahydrate, 0.50 g of manganese sulfate monohydrate and 2.52 g of trimesic acid into 35 ml of N,N-dimethylformamide (DMF), and magnetically stir and mix for 24 hours;

[0035] (2) Put the mixed solution of step (1) into a 50ml polytetrafluoroethylene-lined stainless steel autoclave, place in a muffle furnace, heat at 180°C for 12h, and cool to room temperature after the reaction is complete;

[0036] (3) The product obtained in step (2) was first washed with DMF for 3 times, then washed with ethanol for 3 times, and dried at 60° C. for 12 hours to obtain a brown powder;

[0037] (4) The brown powder prepared in (3) was calcined at 350° C. for 3 h in an air atmosphere in a muffle furnace to prepare a MIL-100 (Fe / Mn) derivative catalyst.

[0038] (5) Field emission scanning electron microscopy (...

Embodiment 2

[0039] Embodiment 2: explore catalyst material dosage to MIL-100 (Fe / Mn) derivative catalytic H 2 o 2 The impact of degrading PPCPs, the details are as follows:

[0040] (1) In this implementation case, under normal temperature and pressure, the typical representatives of PPCPs MNZ and BPB aqueous solutions with a concentration of 5 mg / L were prepared respectively, and H was added with a concentration of 30 mM and 1 mM 2 o 2The mixed solution in two groups of reactors, each group is added with 0.02g / L, 0.05g / L, 0.1g / L, 0.15g / L, 0.20g / L MIL-100 (Fe / Mn) derivative catalyst, use 0.2 mol / L phosphate buffer to adjust the pH of the mixture to 7.0, and react for 10 min. The liquid samples were taken out from the reactor periodically, and the remaining MNZ and BPB concentrations of the samples were determined by high performance liquid chromatography (HPLC). Please refer to the sampling time figure 2 and image 3 . Among them, the dosage concentration of MIL-100(Fe / Mn) deriva...

Embodiment 3

[0042] Embodiment 3: Exploring initial pH to MIL-100 (Fe / Mn) derivative catalytic H 2 o 2 The impact of degrading typical PPCPs (MNZ and BPB), the details are as follows:

[0043] (1) In this implementation case, under normal temperature and pressure, MNZ and BPB, the typical representatives of PPCPs with a concentration of 5mg / L, were prepared respectively, and the concentrations of 30mM and 1mM H 2 o 2 The mixed solution of the mixed solution is placed in two groups of reactors, and each group is added the MIL-100 (Fe / Mn) derivative catalyst prepared by 0.15mg / L embodiment, and the pH of each group mixed solution is adjusted with 0.2mol / L phosphate buffer The values ​​are 3, 5, 7, 9, 11, and the reaction takes 10 minutes. The liquid samples were taken out from the reactor periodically, and the remaining MNZ and BPB concentrations of the samples were determined by high performance liquid chromatography (HPLC). Among them, the dosage concentration of MIL-100(Fe / Mn) derivat...

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Abstract

The invention discloses a method for removing drugs and personal care products (PPCPs) in water by catalyzing H2O2 with an MIL100 (Fe / Mn) derivative. The method comprises the following steps of: (1) preparing MIL-100 (Fe / Mn) by using a hydrothermal method; (2) calcining the MIL-100 (Fe / Mn) prepared in the step (1) to prepare an MIL-100 (Fe / Mn) derivative; (3) separately preparing a metronidazole target solution of which the concentration is 0.5-5mg / L and a butylparaben target solution of which the concentration is 0.5-5mg / L, and adjusting the pH values to 3-9; and (4) respectively adding a certain amount of MIL-100 (Fe / Mn) derivative catalyst and H2O2 into the two PPCPs solutions, and performing reactions at the temperature of between 10 and 40 DEG C. It is found for the first time that the effect of the MIL-100 (Fe / Mn) derivative for catalyzing H2O2 to degrade PPCPs is superior to that of other catalysts, and the high removal rate can be maintained under the acidic to neutral condition. The method is easy to operate, simple in process and low in equipment requirement, can be widely used for removing emerging pollutants in a water environment, and has a wide market application prospect.

Description

technical field [0001] The invention relates to the technical field of water treatment, in particular to a method of utilizing MIL-100 (Fe / Mn) derivatives to catalyze H 2 o 2 Methods for removing PPCPs from water. Background technique [0002] Pharmaceuticals and personal care products (PPCPs) are an emerging class of environmental pollutants, which include antibiotics, preservatives, hormones, synthetic musk and other product categories. Due to the health care and preventive effects of PPCPs and the needs of human beings to cure diseases, the production scale of PPCPs can reach two million tons per year, and it is still increasing. However, PPCPs are chemically persistent and resistant to biodegradation. Due to their widespread use, they can flow into water bodies through industry, agriculture, hospitals, households, and sewage treatment plants, making them continuously accumulate in the environment. Excessive accumulation of PPCPs in the body may affect the endocrine sy...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C02F1/72B01J23/889C02F101/34C02F101/38C02F101/30
CPCC02F1/722C02F1/725B01J23/8892B01J23/002C02F2101/38C02F2101/34C02F2103/002C02F2101/30
Inventor 苑宝玲汲玉玺付明来方明泽张志勇艾慧颖
Owner HUAQIAO UNIVERSITY
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