CN109603844A - FeMnC aeroge Fenton cathode and preparation method thereof and application in degrading perfluorinated compound - Google Patents
FeMnC aeroge Fenton cathode and preparation method thereof and application in degrading perfluorinated compound Download PDFInfo
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Abstract
The present invention relates to FeMnC aeroge Fenton cathode and preparation method thereof and in the application of degrading perfluorinated compound.By Fe, Mn bimetallic, growth in situ obtains the FeMnC aeroge Fenton cathode material into the carbon aerogels skeleton of 3D damascene structures simultaneously.CO is passed sequentially through later2And N2Activation, in the anode and cathode synergistic oxidation system with BDD anode, degrading perfluorinated compound.Compared with prior art, the present invention by base metal Fe and Mn, construct in the network structure of CA simultaneously by original position, not only increases the catalytic activity of electrode, while the stability of electrode and reusable property also greatly improve.Meanwhile Fe10MnC electricity Fenton cathode and boron-doped diamond (BDD) anode can realize efficient Synergistic degradation PFCs.PFCs for environmental protection under mild reaction conditions, efficient process high toxicity, high chemical stability provides a kind of new way, has very extensive application prospect in actual water treatment field.
Description
Technical field
The invention belongs to water-treatment technology field, be related to a kind of preparation of " iron-manganese-carbon " aeroge Fenton cathode with
And the degrading perfluorinated compound of efficient oxidation is cooperateed with BDD anode with it.
Background technique
Perfluorochemical (perfluorinated compounds, PFCs) is a kind of artificial synthesized novel lasting ring
Border pollutant, since PFCs is largely used for a long time, and C-F key has highly polar, is difficult to degrade in nature, and in the environment
Accumulation and bioconcentration are very strong, generally existing in water environment, it has also become one of environment and the chief threat of human health.
Perfluoro caprylic acid (Perfluorooctanoic acid, PFOA) therein and perfluorooctane sulfonate
(perfluorosulfonic acid, PFOS) is present in water body by frequent report in recent years, in animal and human body.Due to
PFOA is highly stable, the high bond energy (127kcalmol of C-F-1) and F-High reduction potential (F+e-→F-, E0=3.6V) and
Carbochain lack can attack site, traditional bioremediation is difficult to be effectively removed PFCs pollutant in water, in addition by
The concentration of the PFCs in individual sewage disposal plant effluents is caused to be higher than water inlet the degradation of PFCs presoma in microorganism.At present
The research of removal technology about PFCs is concentrated mainly on separation removal and chemical degradation, and economic cost is high, and is also easy to produce secondary
Pollution.Traditional high-level oxidation technology can not directly degrade, such as most of research shows that the OH of strong oxidizing property does not have C-F
There is effect, is unable to direct oxidation degradation PFOA.Current absorption, microfiltration, chemical degradation (including oxidative degradation and deoxidization, degradation),
Light degradation and air-atomizing waterpower vortex (ASH) the methods of technology and pyrolysis are widely used in removing PFCs in industrial wastewater
Research.Electrochemical advanced oxidation (EAOPs) is that one kind is degraded using highly effective reaction group OH as oxidant at normal temperature
The technology of organic pollutants in water body.Out-phase electricity Fenton (E-Fenton) technology in EAOPs passes through the surface Fe of catalystIIAnd its
Its modified Fenton reaction and electrochemical in-situ generate H2O2The catalysis reaction of Fenton/ Fenton-like occurs and generates OH.Due to its nothing
Need to additionally add oxidant, without secondary pollution, reaction condition is mild, easy to operate, easy realization automation the advantages that and by pass
Note, and it is widely used in the wastewater treatment containing organic pollutant.Out-phase E-Fenton overcomes the shortcomings that conventional homogeneous Fenton technology,
The Fe in homogeneous Fenton catalysis is replaced with solid fenton catalyst2+, pH response range is wide, catalyst recoverable, secondary iron
Sludge-polluted phenomenon is greatly alleviated, to be widely used in organic matter degradation.But also exist simultaneously H2O2Yield compared with
It is low, the problems such as catalyst is easy to fall off, easy in inactivation.Based on this, the present invention utilizes a step by preparing novel dual metal cathode material
Synthetic method constructs Fenton catalyst in situ, to improve the oxidability and service life of out-phase E-Fenton catalyst system.
Diamond has the characteristics that high rigidity, easily thermally conductive, high stability, extremely wide potential energy window, pure diamond are a kind of
Good insulating materials, it is difficult to be applied to electrochemical field.Boron doping imparts the good electric conductivity of diamond, maintains
The original excellent electrochemical property of diamond electrode, referred to as boron-doped diamond thin-film electrode (boron doped diamond,
BDD).BDD electrode has wider work potential window, high chemical stability and high OEP (2.7V vs SHE).PFCs is to straight
The traditional high-level oxidation technology connect has inertia, though OH has strong oxidizing property, it is unable to direct oxidation PFCs substantially,
The removal rate of Fenton degradation PFOA can be neglected substantially.Later period is the study found that PFCs is easy to lose on the surface anode BDD
An electronics is removed, the perfluoroalkyl radical of generation is easy to by some Strong oxdiative active material (such as OH) mineralizing and degradings.Cause
This is mentioned while reducing operating cost for the New Method for Processing for exploring more quick, efficient, environmental protection organic pollutants in water body
High disposal effect, the present invention combine out-phase E-Fenton technology with anode BDD, i.e., by the novel out-phase E-Fenton yin of preparation
Pole and BDD anode are formed by anode and cathode collaboration system, efficiently remove PFCs.
Summary of the invention
It is unstable the purpose of the present invention is being constructed for existing out-phase E-Fenton catalyst, it is easy to fall off, repeat benefit
With H in property difference and system2O2The problem of low yield, at the same also for solving PFCs difficult to degrade to effectively remove needs a large amount of
The problem of OH, provides a kind of FeMnC aeroge Fenton cathode and preparation method thereof and the application in degrading perfluorinated compound,
Improve 2 electronic selections and H of electrode stability and cathodic oxygen reduction2O2Yield, and establish a kind of anodic-cathodic collaboration oxygen
FeMnC out-phase E-Fenton cathode and BDD anode are carried out high toxicity in Synergistic degradation water body by the electrochemistry collaboration system of change, high
The PFCs of chemical stability realizes quick, environment-friendly high-efficiency removal.
The purpose of the present invention can be achieved through the following technical solutions: a kind of FeMnC aeroge Fenton cathode,
It is characterized in that, is that growth in situ obtains described into the carbon aerogels skeleton of 3D damascene structures simultaneously by Fe, Mn bimetallic
FeMnC aeroge Fenton cathode material.
The preparation method of above-mentioned FeMnC aeroge Fenton cathode, which is characterized in that specifically includes the following steps:
Step (1): weighing suitable resorcinol, formaldehyde and sodium carbonate, be added to the water, be uniformly mixed, and is made
Precursor solution；
Step (2): molysite and manganese salt being added into precursor solution made from step (1), is uniformly mixed, and injection is held
In device, sealing；
Step (3): by the container of step (2) sealing under the conditions of 20~30 DEG C, isothermal reaction 24~30 hours, in 40~
Under the conditions of 50 DEG C, isothermal reaction 24~30 hours, under the conditions of 85~90 DEG C, isothermal reaction 70~75 hours, " iron-is generated
Manganese-carbon " wet gel, by " iron-manganese-carbon " wet gel in being impregnated in acetone under room temperature 3~5 days, replacement one time third daily
Ketone after the completion of to be impregnated, in drying 2~3 days under room temperature, is tied to replace the water in " iron-manganese-carbon " wet gel
Complete " iron-manganese-carbon " xerogel of structure；
Step (4): " iron-manganese-carbon " xerogel made from step (3) is placed in tube furnace, in N2Under atmosphere, forged
It burns, is then cooled to room temperature, obtains " iron-manganese-carbon " aeroge Fenton cathode.
Gained " iron-manganese-carbon " aeroge Fenton cathode is using preceding passing sequentially through CO2And N2Activation, specific activation method
It is as follows:
Step (5): " iron-manganese-carbon " aeroge Fenton cathode made from step (4) is placed in tube furnace, in CO2
Under atmosphere, CO is carried out2Activation heat treatment is then cooled to room temperature, and CO is made2" iron-manganese-carbon " silica aerogel electrode of activation；
Step (6): again by CO made from step (5)2Activation " iron-manganese-carbon " silica aerogel electrode is placed in tube furnace, in N2
Under atmosphere, N is carried out2Activation heat treatment is then cooled to room temperature, obtains CO2/N2" iron-manganese-carbon " aeroge after activation
(FeMnC) Fenton cathode.
CO in step (5)2The condition of activation heat treatment are as follows: in CO2Flow velocity is 30~60mLmin-1CO2Under atmosphere, with
3-5℃·min-1Rate be warming up to 830~850 DEG C, constant temperature 1~2 hour, then with 3-5 DEG C of min-1Rate be down to room
Temperature.
N in step (6)2The condition of activation heat treatment are as follows: in N2Flow velocity is 100~150mLmin-1N2Under atmosphere, with 4
~5 DEG C of min-1Rate be warming up to 830~870 DEG C, constant temperature 1~2 hour, then with 4~5 DEG C of min-1Rate be down to
Room temperature.
Resorcinol in step (1), formaldehyde, water and sodium carbonate molar ratio be 1:2:16-18:0.0008.
Molysite described in step (2) is ferric acetyl acetonade (C15H21FeO6), the manganese salt is four acetate hydrate manganese
(C4H6MnO4·4H2O)；
Mass fraction ratio m is added in precursor solutionFe/m(Fe+C)=1~4% ferric acetyl acetonade and mMn/m(Mn+C)=20
~40% four acetate hydrate manganese.Fe, Mn bimetallic compared to only doping metals Fe or metal Mn and other ratios is co-doped with
Miscellaneous CA, the FeMnC electrode for optimizing Fe, Mn mass ratio have higher catalytic activity and higher H2O2Yield and more
Big OH concentration, and then it is more advantageous to the catalytic degradation of PFCs.
Application of the above-mentioned FeMnC aeroge Fenton cathode in degrading perfluorinated compound, which is characterized in that
FeMnC aeroge Fenton cathode after activation is used in the anode and cathode synergistic oxidation system with BDD anode,
Using two electrode DC power supplys, with 10~30mAcm-2Constant current density, Na of the perfluorochemical in 0.05M2SO4For
Degradation reaction is carried out in supporting electrolyte, solution is in oxygen with 50~100mLmin before reaction-1Rate be first aerated 20~
30 minutes, reaction temperature was 25-30 DEG C, and pH range is 2~5, and oxygen aeration rate is kept constant during degradation reaction.Its
In, PFCs is easy to lose an electronics, the perfluoroalkyl radical (C of generation on the surface anode BDDnF2n+1), CnF2n+1·
The great amount of hydroxy group free radical (OH) easily generated with Fenton cathode combines, and generates unstable intermediate, gradually takes off later
Fluorine, until being degraded by permineralization.
The concentration of the fluorine compounds is 50mgL-1。
The present invention for existing out-phase E-Fenton catalyst construct it is unstable, it is easy to fall off, reusable property difference with
And H in system2O2The problem of low yield, while being also to solve the problems, such as that effectively removing for PFCs difficult to degrade needs a large amount of OH.It will
Fe, Mn bimetallic growth in situ prepare " iron-manganese-carbon " aeroge (FeMnC) out-phase into the CA matrix of 3D damascene structures
E-Fenton cathode.And combine the electrode with BDD anode, establish a kind of electrochemistry synergic agent of anodic-cathodic synergistic oxidation
System, high toxicity in water body of degrading, the PFCs of high chemical stability is, it can be achieved that environmental protection, quickly and efficiently remove.Meanwhile FeMnC
Electrode repeatedly uses, and is still able to maintain excellent catalytic activity.
Compared with prior art, the invention has the characteristics that:
(1) compared with existing Fenton cathode material, FeMnC out-phase E-Fenton cathode collection constructed by the present invention
The advantages of multiple material, is in one: being substrate, its electro-chemical activity and height with higher using carbon aerogels (CA) on the one hand
Specific surface area, be also O22 electronic reduction reactions (ORR) occurs in situ in cathode and generates H2O2Provide good condition；It is another
Aspect, the FeMnC of the codope of metal Fe and Mn have the advantage that (i) has high machine than the electrode that single Fe or list Mn is adulterated
Tool intensity increases the practical usability of electrode；(ii) there is biggish reference area (713m2·g-1), be conducive to active O2
Absorption, and reduce resistance to mass tranfer；(iii) have moderate hydrophilic and hydrophobic (contact angle, 123 °~145 °), both guaranteed electrode with
Waste water comes into full contact with, and prevents solution from immersing electrode duct, can extend electrode life；(iv) be conducive to the graphitization of CA,
A large amount of network-like highly crystallized graphitic carbons are distributed in electrode, greatly improves the electron transfer rate in catalytic process, adds
Fast ferromanganese ore；(v) there are 2 high electronics oxygen reduction activities, greatly improve H2O2Yield；(vi) there is high catalysis H2O2It decomposes
Generate OH efficiency, OH concentration in raising system；(vii) there is excellent catalytic activity and stability, in the drop of highly acid
It solves in solution almost without digestion of metallic ion, it can be achieved that biphase interface catalysis completely；(viii) electrode, which is used repeatedly, still has
Standby excellent catalytic degradation performance.
(2) with the method for traditional degradation PFCs, such as photochemical method, photocatalytic method, electrochemical oxidation process and ultrasonic method
It compares, the synergistic oxidation system of FeMnC out-phase E-Fenton cathode of the invention and BDD anode has low energy consumption, and it is environmentally friendly, efficiently
And treatment process it is easy the features such as.Wherein, PFCs is easy to lose an electronics on the surface anode BDD, generates perfluoroalkyl
Free radical, perfluoroalkyl radical in conjunction with the OH for a large amount of strong oxidizing properties that FeMnC out-phase E-Fenton cathode generates, are given birth to again
At unstable intermediate, gradually defluorinate, circulation, until permineralization.
(3) in the present invention, on the basis of many experiments, regulate and control out the metal Fe in FeMnC out-phase E-Fenton cathode
It is moderate with the content of metal Mn, that is, ensure the mechanical strength of electrode, there is certifiable electrode H with higher2O2Yield and decomposition life
At the efficiency of OH.
(4) preparation process of the present invention is simple, easy control of reaction conditions, and operation is easy, and the prices of raw materials are cheap, system
Standby at low cost, efficient stable, preparing resulting FeMnC out-phase E-Fenton cathode can realize in acid condition to difficult to degrade,
The rapidly and efficiently removal of high toxicity pollutant PFCs is suitable for extension industrial production, is with a wide range of applications.
Detailed description of the invention
The TOC removal rate curve for the degradation PFOA that Fig. 1 is FeMnC out-phase E-Fenton produced by the present invention；
Fig. 2 is the removal of Fe10MnC out-phase E-Fenton cathode produced by the present invention and different anode Synergistic degradation PFOA
Rate curve.
Specific embodiment
The present invention is described in detail with specific embodiment below in conjunction with the accompanying drawings.
Embodiment 1:
It is unstable to be constructed for existing out-phase E-Fenton catalyst, easy to fall off, reusable property difference and body
H in system2O2The problem of low yield, while being also to solve the problems, such as that effectively removing for PFCs difficult to degrade needs a large amount of OH.By Fe,
Mn bimetallic growth in situ prepares " iron-manganese-carbon " aeroge out-phase E-Fenton yin into the CA matrix of 3D damascene structures
Pole.And combine the electrode with BDD anode, a kind of electrochemistry collaboration system of anodic-cathodic synergistic oxidation is established, water of degrading
High toxicity in body, the PFCs of high chemical stability.
" iron-manganese-carbon " or " iron-carbon " and " manganese-carbon " aeroge out-phase E-Fenton cathode material in the present embodiment
Specific preparation process is as follows:
(1) suitable resorcinol, formaldehyde, water, sodium carbonate are weighed, then with resorcinol: formaldehyde: water: sodium carbonate
Precursor solution is divided into quarter after forming uniform solution for 1:2:17.5:0.0008 mixing by molar ratio, point
Not Jia Ru: (i) mFe/m(Fe+C)=1~5% ferric acetyl acetonade；(ii)mFe/m(Fe+C)The ferric acetyl acetonade and m of=5-13%Mn/
m(Mn+C)=5~10% 4 acetate hydrate manganese；(iii)mFe/m(Fe+C)The ferric acetyl acetonade and m of=1-4%Mn/m(Mn+C)=20~
40% 4 acetate hydrate manganese；(iv)mMn/m(Mn+C)=1~5% 4 acetate hydrate manganese.It is injected separately into after stirring evenly rectangular
Sealing after among body glass container.
(2) container is placed in 20~30 DEG C of constant temperature 24~30 hours, 40~50 DEG C constant temperature 24~30 hours, 85~90 DEG C
" iron-manganese-carbon " or " iron-carbon " and " manganese-carbon " wet gel is formed so that polymerization occurs within constant temperature 70~75 hours.Then will
The gel prepared impregnates 3~5 days in acetone at room temperature, an acetone is replaced daily, for replacing in gel
Water after dipping terminates, is dried 2~3 days at room temperature, obtains the xerogel of a large amount of structural integrities.Then these are done
Gel is placed in temperature programming in tube furnace, in the case where nitrogen flow rate is the nitrogen atmosphere of 300~400mLmin, with 1~2 DEG C every point
The heating rate of clock rises to 930~970 DEG C, and is kept for 4~5 hours at such a temperature, is then down to room temperature with phase same rate, i.e.,
Respectively correspond non-activated blocky " iron-manganese-carbon " or " iron-carbon " and " manganese-carbon " aeroge of obtained structural integrity.
(3) by prepared above-mentioned serial carbon aerogels CO2Activation, the activation method are as follows: electrode is placed in tubular type
Temperature programming in furnace, in the case where carbon dioxide flow rate is the carbon dioxide atmosphere of 30~50mLmin, with 3~5 DEG C of speed per minute
Rate rises to 830~850 DEG C, is kept for 1~2 hour at such a temperature, after being then down to room temperature with phase same rate, has obtained structure
Complete bulk CO2" iron-manganese-carbon " silica aerogel electrode of activation.Again by CO2Electrode after activation is placed in program liter in tube furnace
Temperature rises to 830~870 DEG C under the nitrogen atmosphere of 100~150mLmin of nitrogen flow rate with 4~5 DEG C of rates per minute,
It is kept for 1~2 hour at such a temperature, room temperature is then down to phase same rate, has obtained structure completely bulk CO2And N2Activation
" iron-manganese-carbon " aeroge (FeC, Fe0.8MnC, Fe10MnC, MnC).
Embodiment 2
It is assessment " iron-manganese-carbon " or " iron-carbon " and " manganese-carbon " aeroge to the degradation capability of PFCs, the series is different
Phase E-Fenton cathode be used for in the anode and cathode synergistic oxidation system of BDD anode, for PFCs most representativeization of degrading
Close one of object, i.e. perfluoro caprylic acid (PFOA).Degradation condition are as follows: electrode area is 8.5cm2, using two electrode DC power supplys, with
10~30mAcm-2Constant current density, voltage~2.2V.PFOA (100ml, 50mgL-1) in the Na of 0.05M2SO4For
Degradation reaction is carried out in supporting electrolyte, solution is in oxygen with 50~100mLmin before reaction-1Rate be first aerated 20~
30 minutes, reaction temperature was 25-30 DEG C, and pH range is 2~5, and oxygen aeration rate is kept constant during degradation reaction.By
Fig. 1 it is found that when FeC, Fe0.8MnC, Fe10MnC and MnC are as out-phase E-Fenton cathode, degrade 240min when to PFOA's
TOC removal rate is respectively~52% ,~68% ,~96% and 86%.Wherein, the catalysis of Fe10MnC out-phase E-Fenton cathode
The ability of degradation PFOA is most strong.For stability of the assessment Fe10MnC electrode in water process, Fe10MnC electrodes are carried out
Repeat degradation experiment.Experiment condition is as described above.The experimental results showed that Fe10MnC electrode reuses it in 1200min
Afterwards ,~7.6% is only reduced to the TOC removal rate of PFOA.
Embodiment 3
It is assessment " iron-manganese-carbon " or " iron-carbon " and " manganese-carbon " aeroge to the degradation capability of PFCs, the series is different
Phase E-Fenton cathode be used for in the anode and cathode synergistic oxidation system of BDD anode, for PFCs most representativeization of degrading
Close one of object, i.e. perfluorooctane sulfonate (PFOS).Degradation condition are as follows: electrode area is 8.5cm2, using two electrode DCs electricity
Source, with 10~30mAcm-2Constant current density, voltage~2.2V.PFOS (100ml, 50mgL-1) 0.05M's
Na2SO4To carry out degradation reaction in supporting electrolyte, solution is in oxygen with 50~100mLmin before reaction-1Rate it is first
Aeration 20~30 minutes, reaction temperature are 25-30 DEG C, and pH range is 2~5, and oxygen aeration rate is protected during degradation reaction
It holds constant.When FeC, Fe0.8MnC, Fe10MnC and MnC are as out-phase E-Fenton cathode, degrade 240min when to the drop of PFOS
Solution rate is respectively~71% ,~74% ,~92% and 83%.Wherein, the catalytic degradation of Fe10MnC out-phase E-Fenton cathode
The ability of PFOS is most strong.
Embodiment 4
It is evaluation BDD electrode to the synergistic effect of AFe10MnC out-phase E-Fenton cathode, using carbon-point, Pt piece and BDD
Three kinds of anodes carry out degradation experiment to PFOA, and electrode area is 8.5cm2, using two electrode DC power supplys, with 10~30mA
cm-2Constant current density, voltage~2.2V.PFOA (100ml, 50mgL-1) in the Na of 0.05M2SO4For supporting electrolyte
Middle carry out degradation reaction, solution is in oxygen with 50~100mLmin before reaction-1Rate be first aerated 20~30 minutes, react
Temperature is 25-30 DEG C, and pH range is 2~5, and oxygen aeration rate is kept constant during degradation reaction.Fig. 2 is different anodes
To PFOA as the removal rate of the variation of time compares in 240min.It can be seen from the figure that BDD is in 240min to PFOA
Removal rate~97%, be Pt piece and carbon-point~1.2 and~2.1 times respectively.That is PFOA can be effectively formed on the surface anode BDD
Perfluorocarboxylic acid free radical, and then decarboxylation, form perfluoroalkyl radical, which generates unstable with hydroxyl radical reaction
Perfluoroalkyl alcohol, and quickly carry out the rearrangement and hydrolysis of intramolecular, defluorinate, circulation, until by permineralization.
The above description of the embodiments is intended to facilitate ordinary skill in the art to understand and use the invention.
Person skilled in the art obviously easily can make various modifications to these case study on implementation, and described herein one
As principle be applied in other embodiments without having to go through creative labor.Therefore, the present invention is not limited to the above embodiments, this
Field technical staff announcement according to the present invention, improvement and modification made without departing from the scope of the present invention all should be in the present invention
Protection scope within.
Claims (9)
1. a kind of FeMnC aeroge Fenton cathode, which is characterized in that be by Fe, Mn bimetallic simultaneously growth in situ to 3D
In the carbon aerogels skeleton of damascene structures, the FeMnC aeroge Fenton cathode material is obtained.
2. a kind of preparation method of FeMnC aeroge Fenton cathode described in claim 1, which is characterized in that specific packet
Include following steps:
Step (1): weighing suitable resorcinol, formaldehyde and sodium carbonate, be added to the water, be uniformly mixed, and forerunner is made
Liquid solution；
Step (2): molysite and manganese salt being added into precursor solution made from step (1), is uniformly mixed, and inject container
In, sealing；
Step (3): by the container of step (2) sealing under the conditions of 20~30 DEG C, isothermal reaction 24~30 hours, in 40~50 DEG C
Under the conditions of, isothermal reaction 24~30 hours, under the conditions of 85~90 DEG C, isothermal reaction 70~75 hours, generate " iron-manganese-
Carbon " wet gel replaces an acetone by " iron-manganese-carbon " wet gel in being impregnated in acetone under room temperature 3~5 days daily,
To replace the water in " iron-manganese-carbon " wet gel, after the completion of to be impregnated, in drying 2~3 days under room temperature, it is complete to obtain structure
Whole " iron-manganese-carbon " xerogel；
Step (4): " iron-manganese-carbon " xerogel made from step (3) is placed in tube furnace, in N2Under atmosphere, calcined, with
After be cooled to room temperature, obtain " iron-manganese-carbon " aeroge Fenton cathode.
3. the preparation method of FeMnC aeroge Fenton cathode according to claim 2, which is characterized in that gained
" iron-manganese-carbon " aeroge Fenton cathode is using preceding passing sequentially through CO2And N2Activation, specific activation method are as follows:
Step (5): " iron-manganese-carbon " aeroge Fenton cathode made from step (4) is placed in tube furnace, in CO2Atmosphere
Under, carry out CO2Activation heat treatment is then cooled to room temperature, and CO is made2" iron-manganese-carbon " silica aerogel electrode of activation；
Step (6): again by CO made from step (5)2Activation " iron-manganese-carbon " silica aerogel electrode is placed in tube furnace, in N2Atmosphere
Under, carry out N2Activation heat treatment is then cooled to room temperature, obtains CO2/N2" iron-manganese-carbon " aeroge (FeMnC) after activation
Fenton cathode.
4. the preparation method of FeMnC aeroge Fenton cathode according to claim 3, which is characterized in that step (5)
Middle CO2The condition of activation heat treatment are as follows: in CO2Flow velocity is 30~60mLmin-1CO2Under atmosphere, with 3-5 DEG C of min-1's
Rate is warming up to 830~850 DEG C, and constant temperature 1~2 hour, then with 3-5 DEG C of min-1Rate be down to room temperature.
5. the preparation method of FeMnC aeroge Fenton cathode according to claim 3, which is characterized in that step (6)
Middle N2The condition of activation heat treatment are as follows: in N2Flow velocity is 100~150mLmin-1N2Under atmosphere, with 4~5 DEG C of min-1's
Rate is warming up to 830~870 DEG C, and constant temperature 1~2 hour, then with 4~5 DEG C of min-1Rate be down to room temperature.
6. the preparation method of FeMnC aeroge Fenton cathode according to claim 2, which is characterized in that step (1)
Middle resorcinol, formaldehyde, water and sodium carbonate molar ratio be 1:2:16-18:0.0008.
7. the preparation method of FeMnC aeroge Fenton cathode according to claim 2, which is characterized in that step (2)
The molysite is ferric acetyl acetonade (C15H21FeO6), the manganese salt is four acetate hydrate manganese (C4H6MnO4·4H2O)；
Mass fraction ratio m is added in precursor solutionFe/m(Fe+C)=1~4% ferric acetyl acetonade and mMn/m(Mn+C)=20~
40% four acetate hydrate manganese.
8. a kind of FeMnC aeroge Fenton cathode as described in claim 1 is in the application of degrading perfluorinated compound, spy
Sign is,
FeMnC aeroge Fenton cathode after activation is used in the anode and cathode synergistic oxidation system with BDD anode, is used
Two electrode DC power supplys, with 10~30mAcm-2Constant current density, Na of the perfluorochemical in 0.05M2SO4To support
Degradation reaction is carried out in electrolyte, solution is in oxygen with 50~100mLmin before reaction-1Rate be first aerated 20~30 points
Clock, reaction temperature are 25-30 DEG C, and pH range is 2~5, and oxygen aeration rate is kept constant during degradation reaction.
9. FeMnC aeroge Fenton cathode according to claim 8 is in the application of degrading perfluorinated compound, described
The concentration of fluorine compounds is 50mgL-1。
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