[go: up one dir, main page]

CN116199315B - An electro-Fenton reaction device and method for wastewater treatment - Google Patents

An electro-Fenton reaction device and method for wastewater treatment Download PDF

Info

Publication number
CN116199315B
CN116199315B CN202310112381.1A CN202310112381A CN116199315B CN 116199315 B CN116199315 B CN 116199315B CN 202310112381 A CN202310112381 A CN 202310112381A CN 116199315 B CN116199315 B CN 116199315B
Authority
CN
China
Prior art keywords
fenton
catalyst
electro
carbon
gas diffusion
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Active
Application number
CN202310112381.1A
Other languages
Chinese (zh)
Other versions
CN116199315A (en
Inventor
全燮
王凯旋
秦欣
曹佩珂
陈硕
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Dalian University of Technology
Original Assignee
Dalian University of Technology
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Dalian University of Technology filed Critical Dalian University of Technology
Priority to CN202310112381.1A priority Critical patent/CN116199315B/en
Publication of CN116199315A publication Critical patent/CN116199315A/en
Priority to PCT/CN2024/081330 priority patent/WO2024169997A1/en
Application granted granted Critical
Publication of CN116199315B publication Critical patent/CN116199315B/en
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • 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
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01FMIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F33/00Other mixers; Mixing plants; Combinations of mixers
    • B01F33/40Mixers using gas or liquid agitation, e.g. with air supply tubes
    • 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
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2305/00Use of specific compounds during water treatment
    • C02F2305/02Specific form of oxidant
    • C02F2305/023Reactive oxygen species, singlet oxygen, OH radical
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2305/00Use of specific compounds during water treatment
    • C02F2305/02Specific form of oxidant
    • C02F2305/026Fenton's reagent

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Water Supply & Treatment (AREA)
  • Organic Chemistry (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)

Abstract

The invention discloses an electro-Fenton reaction device for wastewater treatment, which comprises a plurality of gas diffusion chambers (5) which are arranged in parallel in a reaction tank (3), wherein cathodes (1) are respectively arranged outside corresponding side walls on the gas diffusion chambers (5), and anodes (2) are correspondingly arranged in parallel and equidistant with each cathode (1); the cathodes (1) and the anodes (2) are respectively connected with a power supply (4); a coil pipe structure is arranged in the gas diffusion chamber (5), one end of the coil pipe structure is communicated with the gas inlet (6), and the other end of the coil pipe structure is communicated with the gas outlet (7); a plurality of water inlets (9) and water outlets (10) are arranged on the reaction tank (3). The invention adopts the oxygen supply mode of the gas diffusion electrode, can enhance the mass transfer efficiency of oxygen, can supply gas to the cathode at both sides of the gas diffusion chamber, and can efficiently utilize the space of the reaction device; good effect of treating wastewater, high current efficiency, low energy consumption and low operation and maintenance cost.

Description

electro-Fenton reaction device and method for wastewater treatment
Technical Field
The invention belongs to the field of wastewater treatment, and particularly relates to an electro-Fenton reaction device and method for wastewater treatment.
Background
The industrial wastewater has wide sources and complex components, and contains a large amount of refractory substances such as emulsified oil, heavy metals, cyanide and refractory organic pollutants. Wherein, the organic pollutant difficult to degrade is difficult to be effectively degraded by the traditional biological method and chemical oxidation method due to the characteristics of durability, high toxicity and difficult biodegradation. Advanced oxidation techniques, represented by Fenton technology, are effective methods for removing refractory organic contaminants from wastewater. By H in the conventional Fenton process 2 O 2 With Fe 2+ The reaction generates active oxygen free radical (such as OH, O) 2 · -1 O 2 ) Is used for degrading and mineralizing pollutants. The Fenton reaction process needs to be maintainedContinuously adding H 2 O 2 High concentration H 2 O 2 There is an explosion risk during storage, transportation and use. In recent years, the electro-Fenton technology is considered as a promising technology for wastewater treatment. The electro-Fenton technology only takes green oxygen and water as raw materials, and the oxygen generates a di-electron oxygen reduction reaction on the surface of a cathode to generate H in situ 2 O 2 Solves the problem of additional addition of H in the traditional Fenton reaction 2 O 2 Potential safety hazard caused by the method effectively avoids H 2 O 2 Explosion risks in storage, transportation and use. In the electro-Fenton reaction process, the mass transfer efficiency of oxygen is critical, and H can be directly influenced 2 O 2 Is effective in treating wastewater. The current reported electro-Fenton reaction device is as Chinese patent invention: CN113401981B discloses a device and method for treating organic wastewater by electro-Fenton without adding medicament; chinese invention patent: CN102674505B discloses a special device for treating organic sewage by utilizing an electro-Fenton reaction, which is characterized in that oxygen or air is directly exposed into a reaction solution, the exposed oxygen or air needs to be dissolved in the reaction solution to form dissolved oxygen, the dissolved oxygen is naturally diffused to the surface of a cathode and then subjected to an oxygen reduction reaction, and the mass transfer efficiency and the utilization rate of the oxygen in the dissolution and diffusion process are lower, so that H in the electro-Fenton process is caused 2 O 2 Low yield and low current efficiency.
Therefore, it is necessary to effectively improve the mass transfer efficiency of oxygen and the utilization efficiency of current in the electro-Fenton technology for the industrial application of the technology.
Disclosure of Invention
The invention aims to provide an electro-Fenton reaction device for wastewater treatment, wherein an electrode with a gas diffusion oxygen supply mode is adopted at a cathode and combined with the oxidation action of an anode, so that the problem of low oxygen mass transfer efficiency in the prior art is solved, the current efficiency is improved, the wastewater treatment effect is enhanced, and the running cost is reduced.
The invention provides an electro-Fenton reaction device for achieving the purpose, which is characterized by comprising a plurality of gas diffusion chambers which are arranged in parallel in a reaction tank, wherein cathodes are respectively arranged outside corresponding side walls on the gas diffusion chambers, anodes are correspondingly arranged in parallel and equidistant with each cathode, and a cathode electrode group and an anode electrode group which are mutually and parallelly arranged in an interpenetration way are formed; the cathodes and the anodes are respectively connected with a power supply;
a coil pipe structure is arranged in the gas diffusion chamber, one end of the coil pipe structure is communicated with the gas inlet, and the other end of the coil pipe structure is communicated with the gas outlet;
the reaction tank is provided with a plurality of water inlets and water outlets.
Preferably, the cathode and the gas diffusion chamber are separated and fixed by a waterproof insulating pad.
Preferably, the water inlet and the water outlet are correspondingly arranged on the reaction tank between each cathode and each anode; the water inlet is also provided with a water pump.
Preferably, the side wall of the gas diffusion chamber is a hollowed-out plate, and the thickness is 0.1-10 cm.
Preferably, the coil structure comprises a partition dividing the interior of the gas diffusion chamber into a plurality of tortuous passages; an air pump is arranged at an air inlet communicated with the coil pipe structure.
The invention provides a method for treating wastewater by an electro-Fenton reaction device, which is characterized by comprising the following steps of:
s1, adding wastewater to be treated into a reaction tank;
s2, connecting the anode with the positive electrode of the power supply, and connecting the cathode with the negative electrode of the power supply;
s3, introducing oxygen-containing gas into the gas diffusion chamber, and generating H in situ through oxygen reduction reaction 2 O 2 Will H 2 O 2 Generating active oxygen free radicals under the action of Fenton catalyst or catalytic active site, and carrying out electro-Fenton degradation reaction on the wastewater.
Preferably, the cathode adopts an electrode with a gas diffusion oxygen supply mode and is composed of an internal gas diffusion layer and an external catalytic layer; the gas diffusion layer comprises a metal net, carbon paper, carbon cloth and carbon felt which are wrapped by conductive materials; the catalytic layer is a catalyst coating of two catalytic active sites or a catalyst coating for loading hydrogen peroxide; will beThe catalyst is coated, adhered to the gas diffusion layer, or the gas diffusion layer and the catalytic layer are pressed together. The two catalytically active site catalysts have two different catalytically active sites, i.e. "bifunctional" catalysts, one of which can electrocatalytic oxygen reduction to H 2 O 2 Subsequently electrospynthesized H 2 O 2 Is decomposed in situ on another catalytic active site to generate active oxygen free radicals (such as OH and O) 2 · -1 O 2 ) Is used for treating wastewater.
The anode adopts a carbon electrode, a titanium-based tin antimony oxide coating electrode, a titanium-based ruthenium iridium oxide coating electrode, a titanium-based lead dioxide electrode or a platinum electrode and a boron-doped diamond electrode; the carbon electrode comprises graphite, carbon paper, carbon cloth and carbon felt.
Preferably, the two catalysts of the catalytic active sites comprise a heteroatom doped carbon catalyst, a metal nanoparticle supported porous carbon catalyst, a metal oxide nanoparticle supported porous carbon catalyst, a metal monatomic supported carbon catalyst, and a metal cluster supported carbon catalyst; the catalyst for loading hydrogen peroxide comprises a heteroatom doped carbon catalyst, layered porous carbon, carbon nanospheres, a metal nanoparticle loaded porous carbon catalyst, a metal oxide nanoparticle loaded porous carbon catalyst, a metal single atom loaded carbon catalyst and a metal cluster loaded carbon catalyst.
Preferably, when the catalytic layer is a catalyst coating for loading hydrogen peroxide, the hydrogen peroxide is synthesized by a catalyst for producing hydrogen peroxide, and active free radicals are generated by the reaction of the Fenton catalyst and the hydrogen peroxide; the electro-Fenton degradation reaction is a fluidized bed Fenton reaction or a fixed bed Fenton reaction; the Fenton catalyst in the fluidized bed Fenton reaction process is added into the reaction solution in the form of a homogeneous Fenton catalyst or a powdery heterogeneous Fenton catalyst; the recovery method of the powdery heterogeneous Fenton catalyst comprises natural sedimentation or membrane filtration; the homogeneous Fenton catalyst comprises Fe 2+ 、Fe 3+ The method comprises the steps of carrying out a first treatment on the surface of the The powdery heterogeneous Fenton catalyst comprises FeOCl and Fe 3 O 4 、Fe 2 O 3 FeOOH; the fixed bed Fenton reaction is characterized in that a granular heterogeneous Fenton catalyst with the size of 0.5-20 mm is piled in a reaction zone, and an insulating screen is arranged between the granular heterogeneous Fenton catalyst and an electrode; the granular heterogeneous Fenton catalyst comprises FeOCl and Fe 3 O 4 、Fe 2 O 3 FeOOH and loading the powdery heterogeneous Fenton catalyst on a particle carrier; the particle carrier comprises alumina, titanium dioxide, zirconium dioxide, silicon dioxide and ceramic particles.
Preferably, the electro-Fenton degradation reaction is powered by a power supply, the power supply mode comprises a constant voltage mode or a constant current mode, and when the constant voltage mode is set, the voltage applied to the cathode is between-0.1 and-10V; when the constant current mode is set, the applied current density is 0.1-200 mAcm -2
Compared with the prior art, the invention has the beneficial effects that:
the electro-Fenton reaction device has the advantages of low cost, easy operation, small occupied area and long service life; can generate a sufficient amount of H in situ 2 O 2 Avoiding H 2 O 2 Explosion risk in storage and transportation, fe 2+ /Fe II Is high; the oxygen supply mode of the gas diffusion electrode is adopted, so that the mass transfer efficiency of oxygen can be enhanced, and sufficient O is provided for the electro-Fenton reaction 2 But also plays a role of stirring, and enhances the diffusion and mass transfer of pollutants; the device for treating wastewater has the advantages of good treatment effect, high current efficiency, low energy consumption and low operation and maintenance cost.
Drawings
FIG. 1 is a front cross-sectional view of an electro-Fenton reaction device of the present invention;
FIG. 2 is a top cross-sectional view of the electro-Fenton reaction device of the present invention;
FIG. 3 is a schematic view showing the internal structure of a gas diffusion chamber in the electro-Fenton reaction device of the present invention;
FIG. 4 is an overall construction diagram of the electro-Fenton reaction device of the present invention;
wherein: 1. a cathode; 2. an anode; 3. a reaction tank; 4. a power supply; 5. a gas diffusion chamber; 6. an air inlet; 7. an air outlet; 8. a reaction zone; 9. a water inlet; 10. and a water outlet.
Detailed Description
The invention is further illustrated below in connection with specific examples, but is not limited in any way.
The invention provides an electro-Fenton reaction device for wastewater treatment, which is shown in figures 1-4, and comprises a plurality of gas diffusion chambers 5 which are arranged in parallel in a reaction tank 3, wherein cathodes 1 are respectively arranged outside corresponding side walls on the gas diffusion chambers 5, anodes 2 are correspondingly arranged in parallel and equidistant with each cathode 1, and a cathode electrode group and an anode electrode group which are mutually and parallelly inserted are formed; the cathodes 1 and the anodes 2 are respectively connected with a power supply 4.
Oxygen gas can directly permeate the cathode 1, the anode is connected with the power supply anode, the cathode is connected with the power supply cathode, and the anode is electrified and then passes through the anode-cathode separator 2e - In situ formation of H by oxygen reduction 2 O 2 H generated in situ 2 O 2 Generating active oxygen free radical (such as OH, O) under the action of Fenton catalyst or catalytic active site 2 · -1 O 2 ) The device is used for degrading pollutants, the edge connection part of the cathode 1 and the gas diffusion chamber 5 is separated and fixed by a waterproof insulating pad, the gas diffusion chamber 5 is provided with an air inlet 6 and an air outlet 7, the air inlet 6 is externally connected with an air pump to control the flow of gas, the inner space of the reaction tank 3 is a reaction zone 8, the reaction zone 8 is used for carrying out electro-Fenton degradation reaction on wastewater, the reaction tank 3 is provided with a water inlet 9 and a water outlet 10, and specifically, the reaction tank 3 is correspondingly arranged between each cathode 1 and each anode 2, and the water inlet 9 is externally connected with a water pump to control the flow of wastewater.
The cathode 1 adopts an electrode with a gas diffusion oxygen supply mode and consists of a gas diffusion layer and a catalytic layer; the gas diffusion layer comprises, but is not limited to, a metal mesh, carbon paper, carbon cloth, carbon felt and the like which are wrapped by conductive materials; the catalytic layer may be a coating material supporting a catalyst having a "bifunctional" function, or a coating material supporting a catalyst having a high selectivity and a high activity for hydrogen peroxide production. Wherein the conductive material comprises one or more of carbon black, activated carbon, graphite, carbon nano tube and the like.
A "bifunctional" catalyst has two different catalytically active sites, one of which can electrocatalytic oxygen reduction to H 2 O 2 Subsequently electrospynthesized H 2 O 2 Is decomposed in situ on another catalytic active site to generate active oxygen free radicals (such as OH and O) 2 · -1 O 2 ) The method is used for treating wastewater; the "bifunctional" catalyst includes heteroatom doped carbon catalysts, metal nanoparticle supported porous carbon catalysts, metal oxide nanoparticle supported porous carbon catalysts, metal single atom supported carbon catalysts, metal cluster supported carbon catalysts, and the like.
When the catalytic layer is a catalytic coating of two catalytically active sites, no Fenton catalyst is required to be added or used in any form, and the pollutant is catalytically degraded by virtue of a 'bifunctional' catalyst.
When the catalytic layer is a catalyst coating for loading hydrogen peroxide, the Fenton reaction needs to use a Fenton catalyst, the hydrogen peroxide is synthesized by the catalyst for producing hydrogen peroxide, and the Fenton catalyst and the hydrogen peroxide react to generate active free radicals to degrade pollutants, so that the Fenton reaction mode can be set as a fluidized bed Fenton reaction mode or a fixed bed Fenton reaction mode according to requirements.
Catalysts for hydrogen peroxide production include, but are not limited to, heteroatom doped carbon catalysts, layered porous carbon, carbon nanospheres, metal nanoparticle supported porous carbon catalysts, metal oxide nanoparticle supported porous carbon catalysts, metal single atom supported carbon catalysts, metal cluster supported carbon catalysts, and the like;
fenton catalyst in fluidized bed Fenton reaction process with homogeneous Fenton catalyst (such as Fe 2+ 、Fe 3+ Etc.) or heterogeneous Fenton catalysts in powder form (e.g. FeOCl, fe 3 O 4 、Fe 2 O 3 FeOOH, etc.) is added into the reaction solution, and the powdery heterogeneous Fenton catalyst is recovered and reused through natural sedimentation or membrane filtration, etc.;
the method comprises the steps of accumulating and fixing a granular heterogeneous Fenton catalyst in a reaction zone in a fixed bed Fenton reaction mode; the size range of the granular heterogeneous Fenton catalyst is 0.5-20 mm, so that the diffusion and the transmission of the reaction solution are facilitated; an insulating screen is arranged between the piled granular heterogeneous Fenton catalyst and the electrode, so that the Fenton catalyst is prevented from being in direct contact with the electrode, and the conductivity between the cathode and the anode is not influenced;
the species of the granular heterogeneous Fenton catalyst comprise FeOCl and Fe 3 O 4 、Fe 2 O 3 FeOOH, etc.; the catalyst can be granular catalyst or powder heterogeneous Fenton catalyst supported on a granular carrier (such as alumina, titania, zirconia, silica, ceramic particles and the like).
The anode 2 comprises carbon electrode (such as graphite, carbon paper, carbon cloth, carbon felt, etc.), titanium-based tin-antimony oxide coated electrode, titanium-based ruthenium-iridium oxide coated electrode, titanium-based lead dioxide electrode, platinum electrode, and boron-doped diamond electrode.
The spacing between the cathode 1 and the anode 2 is fixed and consistent, and the spacing range of the polar plates is 0.1-10 cm.
The side wall of the gas diffusion chamber 5 is a hollowed-out plate, a coil pipe structure is arranged in the hollow-out plate, the inside of the gas diffusion chamber 5 is partitioned into a plurality of coiled multi-tortuous channels by using partition plates, particularly, a plurality of partition plates are arranged in the gas diffusion chamber 5, one side of each partition plate is provided with a notch, wherein the notches of two adjacent partition plates are positioned on opposite sides, for example, the notch of a first partition plate is arranged on the right side, the notch of a second partition plate is arranged on the left side, the notch of a third partition plate is arranged on the right side, and the like, so that the gas diffusion chamber 5 forms the multi-tortuous channels. The coil pipe structure can increase the air supply pressure, prolong the residence time of the air, support the cathode, avoid the deformation of the cathode electrode plate, prolong the service life of the electrode, enable the gas diffusion chamber 5 to be filled with oxygen, air or the mixed gas of the oxygen and the air according to the requirements, enable one end of the coil pipe structure to be communicated with the air inlet 6, and enable the other end to be communicated with the air outlet 7, enable two sides of the gas diffusion chamber 5 to be supplied with air to the cathode 1, and enable the thickness of the hollow plate on the side wall of the gas diffusion chamber 5 to be 0.1-10 cm.
The number of units of the gas diffusion chamber 5 and the electrode group can be set according to the requirement, and the optimized number of units is 1-20 groups.
The power is supplied by a power supply 4 in the electro-Fenton reaction process, the power supply mode can be set to be a constant voltage mode or a constant current mode, the voltage applied to the cathode 1 in the constant voltage mode is between-0.1 and-10V, preferably between-0.2 and-2V, and the current density applied in the constant current mode is between 0.1 and 200mAcm -2 Preferably 0.5 to 50mAcm -2
Example 1:
an oxygen doped carbon black/carbon paper electrode with the size of 10cm multiplied by 10cm is used as a cathode 1, a titanium-based tin antimony oxide coated electrode with the same size is used as an anode 2, the electrode spacing is fixed to be 2cm, the electrode is placed into an electro-Fenton reaction tank 3 with the slightly larger size, the number of units of an electro-Fenton reaction zone 8 is 4, the cathode 1 and the anode 2 are respectively externally connected with a power supply 4 through copper wires, and the thickness of a gas diffusion chamber 5 is 2cm. For a concentration of 50mgL -1 And (2) organic wastewater such as levofloxacin, phenol, 2, 4-dichlorophenol, neonomine and 2, 4-dichlorophenoxyacetic acid is subjected to electro-Fenton treatment. 50mM sodium sulfate electrolyte and 0.2gL were added -1 The powder heterogeneous Fenton catalyst FeOCl is introduced into the gas diffusion chamber 5 in the reaction process, and the electro-Fenton treatment is carried out on the organic wastewater under the constant voltage mode of-0.6V of the voltage applied by the cathode 1 through the power supply 4.
The test analysis of the organic sewage before and after treatment shows that: after 0.5 hour of electro-Fenton treatment, the degradation rates of the levofloxacin, the phenol, the 2, 4-dichlorophenol, the neonomine and the 2, 4-dichlorophenoxyacetic acid are respectively 99%, 97% and 98%; after 2 hours of electro-Fenton treatment, the initial Total Organic Carbon (TOC) removal was 78%, 76%, 75%, 68% and 69%, respectively.
Example 2:
the electro-Fenton reaction device in this example was identical to the device in example 1, and the treated industrial wastewater was secondary effluent of coking wastewater with an initial Chemical Oxygen Demand (COD) of 312mgL -1 TOC value of 69mgL -1 The initial pH was 7.2. Operating conditions and example 1 SecurityAnd keeping the same.
Analysis and test are carried out on secondary effluent of the coking wastewater after being treated by electro-Fenton for 3 hours, and the result shows that the COD value of the secondary effluent of the coking wastewater is 312mgL -1 To 43mgL -1 TOC value is 69mgL -1 To 13mgL -1
Many possible variations and modifications of the disclosed technology can be made by anyone skilled in the art without departing from the scope of the technology, or the technology can be modified to be equivalent. Therefore, any simple modification, equivalent variation and modification of the above embodiments according to the technical substance of the present invention shall still fall within the scope of the technical solution of the present invention.

Claims (8)

1. The electro-Fenton reaction device is characterized by comprising a plurality of gas diffusion chambers (5) which are arranged in parallel in a reaction tank (3), wherein cathodes (1) are respectively arranged outside corresponding side walls on the gas diffusion chambers (5), anodes (2) are correspondingly arranged in parallel and equidistant with each cathode (1), and a cathode electrode group and an anode electrode group which are mutually and parallelly inserted are formed; the cathodes (1) and the anodes (2) are respectively connected with a power supply (4);
a coil pipe structure is arranged in the gas diffusion chamber (5), one end of the coil pipe structure is communicated with the gas inlet (6), and the other end of the coil pipe structure is communicated with the gas outlet (7);
a plurality of water inlets (9) and water outlets (10) are arranged on the reaction tank (3);
the side wall of the gas diffusion chamber (5) is a hollowed-out plate;
the coil structure comprises a multi-tortuous channel which is formed by dividing the inside of a gas diffusion chamber (5) into a plurality of tortuous channels by a baffle plate; an air pump is arranged at an air inlet (6) communicated with the coil pipe structure.
2. An electro-Fenton reaction device according to claim 1, characterized in that the cathode (1) is separated from the gas diffusion chamber (5) by a waterproof insulating pad and fixed.
3. An electro-Fenton reaction device according to claim 1, characterized in that the water inlet (9) and the water outlet (10) are correspondingly arranged on the reaction tank (3) between each cathode (1) and the anode (2); the water inlet (9) is also provided with a water pump.
4. A method of treating wastewater in an electro-Fenton reaction device according to any of claims 1-3, comprising the steps of:
s1, adding wastewater to be treated into a reaction tank;
s2, connecting the anode with the positive electrode of the power supply, and connecting the cathode with the negative electrode of the power supply;
s3, introducing oxygen-containing gas into the gas diffusion chamber, and generating H in situ through oxygen reduction reaction 2 O 2 Will H 2 O 2 Generating active oxygen free radicals under the action of Fenton catalyst or catalytic active site, and carrying out electro-Fenton degradation reaction on the wastewater.
5. The method for treating wastewater by using an electro-Fenton reaction device according to claim 4, wherein the cathode adopts an electrode with a gas diffusion oxygen supply mode and consists of a gas diffusion layer and a catalytic layer; the gas diffusion layer comprises a metal net, carbon paper, carbon cloth and carbon felt which are wrapped by conductive materials; the catalytic layer is a catalyst coating of two catalytic active sites or a catalyst coating for loading hydrogen peroxide;
the anode adopts a carbon electrode, a titanium-based tin antimony oxide coating electrode, a titanium-based ruthenium iridium oxide coating electrode, a titanium-based lead dioxide electrode or a platinum electrode and a boron-doped diamond electrode; the carbon electrode comprises graphite, carbon paper, carbon cloth and carbon felt.
6. The method for treating wastewater by an electro-Fenton reaction device according to claim 5, wherein the catalysts of the two catalytic active sites comprise heteroatom doped carbon catalysts, metal nanoparticle supported porous carbon catalysts, metal oxide nanoparticle supported porous carbon catalysts, metal single atom supported carbon catalysts and metal cluster supported carbon catalysts; the catalyst for loading hydrogen peroxide comprises a heteroatom doped carbon catalyst, layered porous carbon, carbon nanospheres, a metal nanoparticle loaded porous carbon catalyst, a metal oxide nanoparticle loaded porous carbon catalyst, a metal single atom loaded carbon catalyst and a metal cluster loaded carbon catalyst.
7. The method for treating wastewater by using an electro-Fenton reaction device according to claim 5, wherein when the catalytic layer is a catalyst coating for producing hydrogen peroxide, hydrogen peroxide is synthesized by a catalyst for producing hydrogen peroxide, and active free radicals are generated by the reaction of the Fenton catalyst and the hydrogen peroxide; the electro-Fenton degradation reaction is a fluidized bed Fenton reaction or a fixed bed Fenton reaction; the Fenton catalyst in the fluidized bed Fenton reaction process is added into the reaction solution in the form of a homogeneous Fenton catalyst or a powdery heterogeneous Fenton catalyst; the recovery method of the powdery heterogeneous Fenton catalyst comprises natural sedimentation or membrane filtration; the homogeneous Fenton catalyst comprises Fe 2+ 、Fe 3+ The method comprises the steps of carrying out a first treatment on the surface of the The powdery heterogeneous Fenton catalyst comprises FeOCl and Fe 3 O 4 、Fe 2 O 3 FeOOH; the granular heterogeneous Fenton catalyst with the size of 0.5-20 and mm is piled in the reaction zone in the fixed bed Fenton reaction, and an insulating screen is arranged between the granular heterogeneous Fenton catalyst and the electrode; the granular heterogeneous Fenton catalyst comprises FeOCl and Fe 3 O 4 、Fe 2 O 3 FeOOH and loading the powdery heterogeneous Fenton catalyst on a particle carrier; the particle carrier comprises alumina, titanium dioxide, zirconium dioxide, silicon dioxide and ceramic particles.
8. The method for treating wastewater by using an electro-Fenton reaction device according to claim 4, wherein the electro-Fenton degradation reaction is powered by a power supply, and the power supply mode comprises a constant voltage mode or a constant current mode, and when the constant voltage mode is set, the voltage applied to the cathode is-0.1 to-10V; when the constant current mode is set, the applied current density is 0.1-200 mA cm -2
CN202310112381.1A 2023-02-14 2023-02-14 An electro-Fenton reaction device and method for wastewater treatment Active CN116199315B (en)

Priority Applications (2)

Application Number Priority Date Filing Date Title
CN202310112381.1A CN116199315B (en) 2023-02-14 2023-02-14 An electro-Fenton reaction device and method for wastewater treatment
PCT/CN2024/081330 WO2024169997A1 (en) 2023-02-14 2024-03-13 Electro-fenton reaction apparatus and method used for wastewater treatment

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202310112381.1A CN116199315B (en) 2023-02-14 2023-02-14 An electro-Fenton reaction device and method for wastewater treatment

Publications (2)

Publication Number Publication Date
CN116199315A CN116199315A (en) 2023-06-02
CN116199315B true CN116199315B (en) 2024-04-12

Family

ID=86518584

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202310112381.1A Active CN116199315B (en) 2023-02-14 2023-02-14 An electro-Fenton reaction device and method for wastewater treatment

Country Status (2)

Country Link
CN (1) CN116199315B (en)
WO (1) WO2024169997A1 (en)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116199315B (en) * 2023-02-14 2024-04-12 大连理工大学 An electro-Fenton reaction device and method for wastewater treatment

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20050202290A1 (en) * 2004-03-10 2005-09-15 Belabbes Merzougui Integrated hybrid electrochemical device
CN209383458U (en) * 2018-11-28 2019-09-13 江苏南资环保科技有限公司 A kind of electricity Fenton oxidation reaction unit
CN111153471A (en) * 2020-01-12 2020-05-15 大连理工大学 A monolithic multichannel electrode for sequential reduction and oxidation of halogenated organics
CN112047438A (en) * 2020-09-08 2020-12-08 湖南大学 A method for treating organic wastewater by using double-cathode electro-Fenton continuous flow

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ITMI20012379A1 (en) * 2001-11-12 2003-05-12 Uhdenora Technologies Srl ELECTROLYSIS CELL WITH GAS DIFFUSION ELECTRODES
CN202499740U (en) * 2012-03-26 2012-10-24 北京化工大学 Photoelectric Fenton reaction device utilizing gas diffusion electrodes
KR102209270B1 (en) * 2018-12-14 2021-01-29 한국과학기술연구원 Sulfated transition metal oxide catalysts for electro-fenton reaction system, electrode comprising the same and electro-fenton reaction system using the same
CN114074971B (en) * 2020-08-20 2023-05-23 中国石油化工股份有限公司 electro-Fenton composite oxidation device and method for degrading organic pollutants in high-chlorine-content sewage
CN113943943B (en) * 2021-11-26 2022-12-09 浙江工业大学 Gas diffusion electrode for preparing p-aminophenol by nitrobenzene electrolytic reduction method and preparation and application thereof
CN116199315B (en) * 2023-02-14 2024-04-12 大连理工大学 An electro-Fenton reaction device and method for wastewater treatment

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20050202290A1 (en) * 2004-03-10 2005-09-15 Belabbes Merzougui Integrated hybrid electrochemical device
CN209383458U (en) * 2018-11-28 2019-09-13 江苏南资环保科技有限公司 A kind of electricity Fenton oxidation reaction unit
CN111153471A (en) * 2020-01-12 2020-05-15 大连理工大学 A monolithic multichannel electrode for sequential reduction and oxidation of halogenated organics
CN112047438A (en) * 2020-09-08 2020-12-08 湖南大学 A method for treating organic wastewater by using double-cathode electro-Fenton continuous flow

Also Published As

Publication number Publication date
WO2024169997A1 (en) 2024-08-22
CN116199315A (en) 2023-06-02

Similar Documents

Publication Publication Date Title
CN107473337B (en) Device and method for treating refractory wastewater by coupling electro-catalytic membrane and three-dimensional electrode
Reis et al. Use of gas diffusion electrode for the in situ generation of hydrogen peroxide in an electrochemical flow-by reactor
CN102381753B (en) A bioelectrochemical membrane reactor device
CN107117690B (en) Device and method for treating refractory pollutants through electrocatalytic oxidation
CN107162118B (en) Cathode-anode built-in ceramic microfiltration membrane reactor suitable for removing water pollutants of water source
US20230129237A1 (en) Water-processing electrochemical reactor
CN104710063B (en) High salt contains photoelectrocatalysis/Fenton coupled processing system and the processing method of poly-waste water
CN102092820A (en) Method and device for removing organic matters from water by using double-pool double-effect visible light in response to photo-electro-Fenton reaction
CN101723533B (en) Method for treating concentrated water produced by coking wastewater recycling process
CN1562795A (en) Photoelectrocatalysis and oxidation device for treating organic substance in water
CN201325897Y (en) Waste water treatment equipment of multi-dimensional electrode electrical catalytic reactor of horizontal electrode plate
US3788967A (en) Wastewater treatment using electrolysis with activated carbon cathode
CN100334006C (en) Three-phase activated carbon fluidized bed electrochemical treatment installation and method for organic wastewater
CN116199315B (en) An electro-Fenton reaction device and method for wastewater treatment
CN110869323A (en) Method of operating a wastewater treatment system
CN201043148Y (en) Photocatalytic and electrocatalytic co-processing device for organic wastewater
CN117023731A (en) Endogenous micro-nano O 2 Bubble-reinforced filtering type heterogeneous electro-Fenton sewage treatment system
WO2024119637A1 (en) Anode and cathode synergistic electrocatalytic system for wastewater treatment and application
CN116874043A (en) Electrochemical double-membrane reactor and wastewater treatment method based on electrochemical double-membrane reactor
CN113896313A (en) A kind of process method for electrochemical treatment of wastewater and co-production of hydrogen
CN115849522B (en) Flow anode electrochemical sewage treatment device and process based on screening type current collector
CN217264974U (en) Electrochemical-ozone oxidation treatment coking wastewater device
CN116199386B (en) High-concentration organic wastewater degradation equipment and degradation method
CN218231992U (en) Sewage treatment system with fixed bed heterogeneous catalysis and bipolar electrocatalysis
CN114873695A (en) Novel three-dimensional particle electrode electrocatalytic oxidation device

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination
GR01 Patent grant
GR01 Patent grant