CN108862483B - Electrode for electrocatalytic degradation of organic pollutants, preparation method and application thereof - Google Patents

Electrode for electrocatalytic degradation of organic pollutants, preparation method and application thereof Download PDF

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CN108862483B
CN108862483B CN201810693691.6A CN201810693691A CN108862483B CN 108862483 B CN108862483 B CN 108862483B CN 201810693691 A CN201810693691 A CN 201810693691A CN 108862483 B CN108862483 B CN 108862483B
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electrode
organic pollutants
electrocatalytic degradation
degradation
electrochemical oxidation
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CN108862483A (en
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李子亨
孙明旭
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Jilin University
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Jilin University
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    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/46Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/467Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
    • C02F1/4672Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds

Abstract

An electrode for electrocatalytic degradation of organic pollutants, a preparation method and application thereof, belonging to the technical field of thin film materials. Fixing graphite paper with the thickness of 50-300 mu M on a glass sheet as an anode, fixing a platinum electrode as a cathode, using a mixed aqueous solution of 0.1-0.5M sodium nitrate, 1-10 mM potassium permanganate and 0.5-1.0M sulfuric acid as an electrolyte, regulating and controlling the electrochemical oxidation potential by a direct current stabilized voltage power supply, wherein the potential is 1-3V, the oxidation time is 10-30 min, and electrochemically oxidizing the graphite paper on the glass sheet to obtain a target electrode. The electrode pair has a pH of 3-11 and a concentration of 20-40 mg L‑1The rhodamine B has obvious catalytic degradation effect. The graphite oxide electrode prepared based on the electrochemical oxidation method has good stability and high degradation efficiency, and the preparation process is simple, easy to operate, low in preparation and sewage treatment cost and easy to popularize.

Description

Electrode for electrocatalytic degradation of organic pollutants, preparation method and application thereof
Technical Field
The invention belongs to the technical field of thin film materials, and particularly relates to an electrode for electrocatalytic degradation of organic pollutants, a preparation method and application thereof.
Background
With the increasing discharge amount of industrial wastewater, domestic sewage and agricultural wastewater, the natural environment on which people live is seriously polluted, so that the exploration of an effective water pollution treatment method becomes a research hotspot in recent years. At present, the harm brought by the mass application of the dye is more and more obvious. In the case of rhodamine B, research shows that the rhodamine B can directly harm the health of human bodies and has potential carcinogenicity, mutagenicity and cardiotoxicity. In 2008, China clearly stipulates that it is prohibited to be used as a food additive. Rose Bengal B is permeable to the skin and toxic at high concentrations.
Among the numerous treatment methods, the electrocatalytic degradation method has the advantages of low cost, high efficiency, easy operation and the like, and is concerned. The graphite oxide film electrode prepared by electrochemical oxidation can provide good electrocatalytic activity and degrade organic pollutants.
Disclosure of Invention
The invention provides an electrode for electrocatalytic degradation of organic pollutants, which has high efficiency, low cost and easy operation, a preparation method and application thereof.
The invention relates to a preparation method of an electrode for electrocatalytic degradation of organic pollutants, which is characterized by comprising the following steps: graphite paper fixed on a glass sheet is used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate, potassium permanganate and sulfuric acid is used as an electrolyte, a target electrode for electrocatalytic degradation of organic pollutants is obtained by electrochemically oxidizing the graphite paper, and the electrochemical oxidation potential is obtained by regulating and controlling a direct-current stabilized voltage power supply.
In the method, the thickness of the graphite paper is 50-300 μm.
In the method, the concentration of the sodium nitrate is 0.1-0.5M.
In the method, the concentration of potassium permanganate is 1-10 mM.
In the method, the concentration of the sulfuric acid is 0.5-1.0M.
In the method, the electrochemical oxidation potential is 1-3V.
In the method, the electrochemical oxidation time is 10-30 min.
The electrode prepared by the invention can be applied to electrocatalytic degradation of organic pollutants.
The application and the method are as follows: the area is 1cm2The target electrode of the electrochemical graphite oxide paper is used as an anode, the platinum electrode is used as a cathode, and Na2SO4And the NaCl mixed aqueous solution is used as electrolyte, a constant-current stabilized voltage power supply is used for carrying out electrocatalytic degradation on the organic pollutants under the condition of constant current, and then an ultraviolet spectrophotometer is used for monitoring the condition that the absorbance changes along with the concentration of the organic pollutants at the position of 554nm of the maximum absorption wavelength of the organic pollutants.
The above application, the electrolyte Na2SO4And NaCl concentrations were 0.1M and 0.01M, respectively.
The above applications, theThe current density for electrocatalytic degradation is 10-50 mAcm-2
In the application, the concentration of the organic pollutants for electrocatalytic degradation is 20-40 mg L-1
In the application, the pH value of the organic pollutant for electrocatalytic degradation is 3-11.
The principle of the electrode prepared by the invention used for electrocatalytic degradation of organic pollutants is as follows: the oxidized graphite electrode surface forms a large number of hydrophilic groups to which organic matter dissolved in the solution can be transported. Under a range of voltages and in a dielectric environment, H2O (in acidic medium) or OH-The discharge (in alkaline medium) forms hydroxyl radicals with oxidation activity on the surface of the graphite oxide electrode, and organic matters are oxidized and degraded.
The invention has the beneficial effects that: the graphite oxide electrode prepared based on the electrochemical oxidation method has good stability and high degradation efficiency. The preparation process is simple, easy to operate, low in preparation and sewage treatment cost and easy to popularize.
Drawings
In order to more clearly illustrate the technical solution of the present invention and the properties of the material prepared by the same, a diagram related to example 1 is given below.
FIG. 1 is an X-ray electron diffraction pattern of a target electrode.
FIG. 2 is a scanning electron microscope atlas of a target electrode.
FIG. 3 shows the current density of the target electrode is 10-50 mAcm-2And (3) obtaining a relation map of the electrocatalytic degradation rate of rhodamine B and time.
FIG. 4 shows the concentration of the target electrode pair is 20-40 mg L-1The relationship map of the electrocatalytic degradation rate of rhodamine B and time.
FIG. 5 is a graph of a relationship between an electrocatalytic degradation rate of a target electrode to rhodamine B with a pH of 3-11 and time.
As can be seen from the X-ray electron diffraction pattern of the target electrode in FIG. 1, the graphite is partially oxidized, and the strong diffraction peak appearing at 26.4 degrees 2 theta is the diffraction peak of graphite; the weaker diffraction peak appearing at 12 ° at 2 θ is that of graphite oxide.
As can be seen from the scanning electron microscopy pattern of the target electrode of fig. 2, the graphite layers of the target electrode had previously expanded and delaminated.
The current density of the target electrode in the figure 3 is 10-50 mAcm-2The relationship graph of the electrocatalytic degradation rate of rhodamine B and time shows that the electrocatalytic degradation rate is increased along with the increase of the current density, but when the current density is increased to 30mA cm-2In the above case, the electrocatalytic degradation rate hardly increases any more.
The concentration of the target electrode pair is 20-40 mg L from FIG. 4-1The relationship graph of the electrocatalytic degradation rate of rhodamine B and time shows that the electrocatalytic degradation efficiency is reduced along with the increase of the concentration.
As can be seen from the graph of the relationship between the electrocatalytic degradation rate of the target electrode with the pH value of 3-11 and the time in FIG. 5, the electrode in the pH value range has a remarkable catalytic degradation effect on organic matters, and the electrocatalytic degradation rate under an acidic condition is obviously higher than that under an alkaline condition.
Detailed Description
The present invention will be further described with reference to the following examples, but the present invention is not limited to these examples.
Example 1:
fixing graphite paper with the thickness of 50 mu M on a glass sheet to serve as an anode, a platinum electrode as a cathode, and a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) as an electrolyte, wherein the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.
Example 2:
fixing graphite paper with the thickness of 50 mu M on a glass sheet to serve as an anode, a platinum electrode as a cathode, and a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) as an electrolyte, wherein the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 2V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.
Example 3:
graphite paper with the thickness of 50 mu M is fixed on a glass sheet to be used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) is used as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 1V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.
Example 4:
graphite paper with the thickness of 50 mu M is fixed on a glass sheet to be used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) is used as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 20min, and the target electrode is obtained through electrochemical oxidation.
Example 5:
graphite paper with the thickness of 50 mu M is fixed on a glass sheet to be used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) is used as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 30min, and the target electrode is obtained through electrochemical oxidation.
Example 6:
graphite paper with the thickness of 100 mu M is fixed on a glass sheet to be used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) is used as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.
Example 7:
graphite paper with the thickness of 200 mu M is fixed on a glass sheet to be used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) is used as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.
Example 8:
graphite paper with the thickness of 300 mu M is fixed on a glass sheet to serve as an anode, a platinum electrode serves as a cathode, a mixed aqueous solution of sodium nitrate (0.1M), potassium permanganate (0.4mM) and sulfuric acid (0.7M) serves as an electrolyte, the electrochemical oxidation potential is regulated and controlled by a direct-current stabilized voltage power supply, the potential is 3V, the oxidation time is 10min, and the target electrode is obtained through electrochemical oxidation.

Claims (6)

1. A preparation method of an electrode for electrocatalytic degradation of organic pollutants is characterized by comprising the following steps: graphite paper is used as an anode, a platinum electrode is used as a cathode, a mixed aqueous solution of sodium nitrate, potassium permanganate and sulfuric acid is used as an electrolyte, a target electrode for electrocatalytic degradation of organic pollutants is obtained by electrochemically oxidizing the graphite paper, and the electrochemical oxidation potential is obtained by regulating and controlling a direct-current stabilized voltage supply; wherein the thickness of the graphite paper is 50-300 mu m; the concentration of sodium nitrate is 0.1-0.5M, the concentration of potassium permanganate is 1-10 mM, and the concentration of sulfuric acid is 0.5-1.0M; the electrochemical oxidation potential is 1-3V, and the electrochemical oxidation time is 10-30 min.
2. The method of claim 1 for preparing an electrode for electrocatalytic degradation of organic contaminants, wherein: the organic pollutant is rhodamine B.
3. An electrode for electrocatalytic degradation of organic contaminants, comprising: is prepared by the method of claim 1 or 2.
4. Use of an electrode for the electrocatalytic degradation of organic pollutants as claimed in claim 3 in the electrocatalytic degradation of organic pollutants.
5. Use of an electrode for electrocatalytic degradation of organic pollutants as claimed in claim 4, wherein: the current density for electrocatalytic degradation is 10-50 mAcm-2The concentration of the organic pollutants is 20-40 mg L-1The pH of the organic pollutants is 3-11.
6. Use of an electrode for electrocatalytic degradation of organic pollutants as claimed in claim 4 or 5, wherein: the organic pollutant is rhodamine B.
CN201810693691.6A 2018-06-29 2018-06-29 Electrode for electrocatalytic degradation of organic pollutants, preparation method and application thereof Active CN108862483B (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
TW201326035A (en) * 2011-12-23 2013-07-01 Academia Sinica Large-scale production apparatus for preparing graphene and graphene oxide and the method thereof
CN105899457A (en) * 2013-11-20 2016-08-24 曼彻斯特大学 Production of graphene oxide
CN106938845A (en) * 2017-03-10 2017-07-11 华南理工大学 A kind of graphite oxide positive electrode and preparation method for lithium ion battery, the preparation method of lithium ion cell positive

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
TW201326035A (en) * 2011-12-23 2013-07-01 Academia Sinica Large-scale production apparatus for preparing graphene and graphene oxide and the method thereof
CN105899457A (en) * 2013-11-20 2016-08-24 曼彻斯特大学 Production of graphene oxide
CN106938845A (en) * 2017-03-10 2017-07-11 华南理工大学 A kind of graphite oxide positive electrode and preparation method for lithium ion battery, the preparation method of lithium ion cell positive

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