CN106966465A - A kind of method that three-diemsnional electrode constructs electrochemical treatments high concentrated organic wastewater - Google Patents
A kind of method that three-diemsnional electrode constructs electrochemical treatments high concentrated organic wastewater Download PDFInfo
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- CN106966465A CN106966465A CN201710093840.0A CN201710093840A CN106966465A CN 106966465 A CN106966465 A CN 106966465A CN 201710093840 A CN201710093840 A CN 201710093840A CN 106966465 A CN106966465 A CN 106966465A
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- concentrated organic
- organic wastewater
- high concentrated
- electrochemical treatments
- complex mineral
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Classifications
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F2001/46133—Electrodes characterised by the material
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
- C02F2101/322—Volatile compounds, e.g. benzene
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
- C02F2101/327—Polyaromatic Hydrocarbons [PAH's]
Abstract
The present invention relates to a kind of method that three-diemsnional electrode constructs electrochemical treatments high concentrated organic wastewater, including：Complex mineral is added in the electrolysis reactor for filling high concentrated organic wastewater, pH to 5~10 is adjusted, cell reaction is carried out under conditions of Aerated stirring fluidisation, clear water is then discharged by non-woven fabrics self-forming dynamic membrane.The method of the present invention has good degradation effect to the phenyl ring class of difficult degradation, heterocyclic, polycyclic class, macromolecular, persistent organism, has good adaptability to all kinds of high concentrated organic wastewaters；With power consumption is low, applicable pH mild condition, it is not required to add chemical agent, does not produce the remarkable advantages such as iron containing sludge, treatment effeciency are high, controllability is good.
Description
Technical field
The invention belongs to field of waste water treatment, more particularly to a kind of three-diemsnional electrode constructs electrochemical treatments high concentration organic waste
The method of water.
Background technology
High concentrated organic wastewater is generally referred to by petrochemical industry, organic chemical industry are synthesized, leather is produced, pharmacy, coking, spinning
Knit, print and dye and the COD of the industry such as food discharge is more than 2000mg/L, B/C is less than 0.3 organic wastewater.This waste water it is organic
Thing content height, complicated component, strong toxicity, are difficult to light degradation and biodegradation in natural environment, and biological and environment is caused
Very big harm, if directly discharged, it will directly result in serious water environment pollution and ecological disruption, and then threaten the mankind to be good for
Health.Therefore the processing to high concentrated organic wastewater has obtained extensive attention.
High-concentration organic wastewater treatment method typically has Physical, chemical method, bioanalysis and membrane separation process and combinations thereof
Method, such as biochemical-physical are combined, biochemistry-chemical oxidation joint etc..In recent years, high-level oxidation technology is widely used
And popularization, its processing method more traditional in the application of high-concentration difficult-degradation organic sewage advanced treating has better
Prospect.
Electrochemical oxidation technology is a kind of high-level oxidation technology, and its dominant mechanism is the reaction system during electrolysis
Produce Strong oxdiative material (OH, O2、H2O2、Cl2、OCl-、ClO3 -), occur direct oxidation with the organic pollution in waste water
Reaction and indirect oxidation reaction, the larger molecular organicses of the difficult degradation in waste water are decomposed into the small molecule of easily biological-degradable,
Improve waste water biodegradability, or even directly by its permineralization be CO2And H2The inorganic matters such as O.
Electrochemical Reactor with Three-dimensional Electrode oxidizing process is to fill granular or other clastics electricity in traditional two-dimentional electrolyzer electric interpolar
Pole material, makes filling electrode material surface powered, as a new pole, by extra electric field put on reactor inner anode plate with
Three dimensional particles electrode between minus plate, particle granules surface has the material degraded to catalytic organism, in electric field and catalytic materials
The many oxide matter based on hydroxyl radical free radical (OH) is produced in the presence of matter, in system, OH is very strong oxidant,
And there is wide applicability to the oxidation of organic matter, by most of organic matter permineralization or easy biochemistry can be degraded to
Small organic molecule.Compared with traditional two-dimensional electrode electrochemical oxidation process, the specific surface area increase of three-diemsnional electrode, applicable pH
Mild condition, the mass transfer effect of material is greatly improved because interparticle distance diminishes, and improves current efficiency and treatment effect.
The content of the invention
The technical problems to be solved by the invention are to provide a kind of three-diemsnional electrode and construct electrochemical treatments high concentration organic waste
The method of water, this method has low power consumption, applicable pH mild condition, is not required to add chemical agent, does not produce iron containing sludge, processing
Efficiency high, controllability are good and the remarkable advantage such as can be recycled.
The technical advantages of the present invention are that having for the phenyl ring class of difficult degradation, heterocyclic, polycyclic class, macromolecular, persistence
Machine thing has good degradation effect, has good adaptability to all kinds of high concentrated organic wastewaters.
The method that a kind of three-diemsnional electrode of the present invention constructs electrochemical treatments high concentrated organic wastewater, including：
Complex mineral is added in the electrolysis reactor for filling high concentrated organic wastewater, pH to 5~10 (preferably 9 is adjusted
~10), cell reaction is carried out under conditions of Aerated stirring fluidisation, clear water is then discharged by non-woven fabrics self-forming dynamic membrane；Its
In, Ti/Sb-SnO prepared by the electrolysis reactor middle-jiao yang, function of the spleen and stomach extremely thermal decomposition method2Electrode, negative electrode is graphite electrode；What is added answers
Mineral are closed as the 3rd electrode of flowing.
The three-diemsnional electrode includes positive plate, minus plate, the 3rd electrode provided with flowing between two-plate, the described 3rd
Electrode is chalcopyrite, the pyrite particle of the different quality ratio mixing of screened obtained certain grade.
Element mass content in the complex mineral includes：Sulphur 40~44%, iron 35~38%, copper 15~18%.
The addition of the complex mineral is 4g/L~20g/L；Particle size range is 40~100 mesh.
The complex mineral is the mixture of chalcopyrite and pyrite.
The mass ratio of the chalcopyrite and pyrite is 1：1.
The electrolysis reactor is that basal diameter is 9cm, a height of 8cm hydrostatic column.
The Ti/Sb-SnO2The preparation of electrode includes step：
(1) Titanium base is pre-processed：Ti nets are cleaned by ultrasonic in absolute ethyl alcohol, certain volume than HF, HNO3、H2O is mixed
Close in acid and etch 2min, be finally cleaned by ultrasonic 15min with deionized water, dry standby.
(2)Ti/Sb-SnO2The preparation of electrode：By SnCl4·5H2O and SbCl3·3H2O presses 8:2 (the amount ratios of material) are made into
Hydrochloric acid aqueous isopropanol, is imported in culture dish, and Ti matrixes are immersed in culture dish, slow lifting, every time by Ti matrixes after lifting
In 80 DEG C of baking ovens dry, after drying continue lift, repeatedly 3~8 times lifting after 450~500 DEG C calcining 15~25min, it is above-mentioned
Step is repeated several times (preferably 4 times), obtains Ti/Sb-SnO2Electrode.
The Aerated stirring is conducive to complex mineral electrode particle to be well mixed in reactive tank with high concentrated organic wastewater.
The condition of the cell reaction is：Electrode voltage is 7~12V (preferably 8V)；Electrolysis time is 3.5~4.5h.
The pore diameter range of the non-woven fabrics self-forming dynamic membrane is 150~200 mesh.
The non-woven fabrics self-forming dynamic membrane is prepared from using non-woven wraps backing material.
After the clear water discharge, complex mineral is reused in electrolysis reactor.
The principle of the present invention is as follows：
Complex mineral Electrochemical Reactor with Three-dimensional Electrode oxidizing process be added between electrolysis reactor electrode it is screened obtain it is certain
The different types of metalliferous mineral of grade, the composition metal ore deposit that the present invention is added is chalcopyrite and the mixed-powder of pyrite.It is yellow
Copper mine is a kind of copper and iron fluidisation thing mineral, is existed more with irregular granular and compact massive aggregated form；Pyrite is flowing molten iron
Compound, is a kind of semiconductor mineral.Chalcopyrite and pyrite are 1 in mass ratio:1 it is well mixed after be put into electrolysis reactor, it is yellow
Copper mine and pyrite composite particles constitute countless small microelectrodes in electrolysis reactor, and adding electrolytic cell, (electrolysis is anti-
Answer device) face body ratio, effective electrode area greatly increases, the treating capacity increase of unit cell body, and because interparticle distance is small and shortens
The migration distance of reactant, increases material mass transfer velocity.In addition, pyrite is semiconductor mineral, reaction can be prevented effectively from
In groove due to pole plate spacing it is small caused by short circuit phenomenon, improve current efficiency and treatment effect.In electrolytic process, it is combined
The organic matter that metalliferous mineral is formed in countless micro-current reactors, waste water is oxidized also in the presence of mosaic electrode micro-current
It is former.In addition, the Fe on complex mineral surface2+The H produced with cell reaction process2O2Combination forms Fenton reagent, ferrous ion
(Fe2+) and H2O2Between chain reaction catalysis generation OH, utilize the pollutant in OH oxidation Decomposition water.In complex mineral
The copper contained and some metal impurities contribute to Fe2+/Fe3+Circulation, improve the catalytic activity of complex mineral.Except this it
Outside, the removal of the direct oxidation of anode and indirect oxidation to organic matter also plays good treatment effect, pollutant is entered one
Step degraded.Clear water is discharged by 40 mesh or so non-woven fabrics self-forming dynamic membrane after cell reaction, complex mineral particle entrapment is in electrolysis
Reused in reactor
Beneficial effect
(1) present invention, without adding chemical agent, reacts bar using complex mineral as the three-diemsnional electrode of electrochemical reactor
Part is gentle, it is easy to control, and substantially increases the treatment effect to high concentrated organic wastewater, reduces processing cost；
(2) traditional advanced oxidation two-dimensional electrode electrochemical oxidation system water outlet residual iron ion, colourity is high, and of the invention
Complex mineral make the Electrochemical Reactor with Three-dimensional Electrode oxidation processes of catalyst, due to Fe2+、Cu2+Stripping quantity controlled, colourity
Removal effect is good, and avoids the secondary pollutions such as iron containing sludge, high treating effect；
(3) excessive Fe will not be produced in method of the invention2+With organic matter competition consumption hydroxyl radical free radical OH and
H2O2, and the copper contained in grandidierite and some metal impurities are conducive to Fe2+/Fe3+Circulation, therefore complex mineral catalytic activity
Preferably, the utilization ratio of oxidant is significantly improved；
(4) complex mineral is not consumed substantially as catalyst during the course of the reaction in method of the invention, easily reclaims profit
With, and be used repeatedly and still have higher catalytic activity, processing cost is further saved, the level of resources utilization is improved.
Brief description of the drawings
Fig. 1 constructs the process chart of electrochemical treatments high concentrated organic wastewater for three-diemsnional electrode in the present invention；Wherein, 1
It is aerator for reactive tank, 2,3 be positive plate, 4 be the complex mineral of suspended state, 5 be minus plate, 6 is that non-woven fabrics is spontaneous
Dynamic Membrane, 7 be adjustable stabilized voltage supply, 8 be centrifugal pump.
Embodiment
With reference to specific embodiment, the present invention is expanded on further.It should be understood that these embodiments are merely to illustrate the present invention
Rather than limitation the scope of the present invention.In addition, it is to be understood that after the content of the invention lectured has been read, people in the art
Member can make various changes or modifications to the present invention, and these equivalent form of values equally fall within the application appended claims and limited
Scope.
Embodiment 1
It is the chalcopyrites of 40~100 mesh by screened obtained particle diameter, pyrite complex mineral is by quality proportioning 1:1 mixing
Uniformly, add and fill the basal diameter of the percolate (COD value 2320mg/L) after Anaerobic Treatment for 9cm, a height of 8cm's
(anode is Ti/Sb-SnO prepared by thermal decomposition method in cylindrical reactive tank2Electrode, negative electrode is graphite electrode), complex mineral
Dosage is 5g/L, and regulation pH value of sewage water makes complex mineral particle to 9~10 under Aerated stirring fluidization conditions after being well mixed
Suspended state is in reactive tank.It is spontaneous by non-woven fabrics after cell reaction 240min under conditions of electrode voltage is 10V
Dynamic Membrane (150~200 mesh) discharges clear water, determines water outlet COD value, and calculate COD clearances.As a result show, complex mineral three
Dimension electrode construct and non-woven fabrics self-forming dynamic membrane electrochemical treatments Anaerobic Treatment after percolate, COD clearance highests can
Up to 88.67%.Complex mineral particle is reused 5 times, and it is respectively 88.67%, 86.12%, 87.73% to measure COD clearances,
88.34%th, 86.15%.COD clearances are maintained at more than 86%, illustrate that complex mineral three-diemsnional electrode particle can as catalyst
To reclaim and repeatedly recycle, and catalytic activity is still very high.
Embodiment 2
It is the chalcopyrites of 40~100 mesh by screened obtained particle diameter, pyrite complex mineral is by quality proportioning 1:1 mixing
Uniformly, add and fill the basal diameter of dyeing waste water (COD value 3846mg/L) for 9cm, in a height of 8cm cylindrical reactive tank
(anode is Ti/Sb-SnO prepared by thermal decomposition method2Electrode, negative electrode is graphite electrode), the dosage of complex mineral is 8g/L, is mixed
Uniform rear regulation pH value of sewage water is closed to 9~10, complex mineral particle is in reactive tank under Aerated stirring fluidization conditions
Suspended state.Pass through non-woven fabrics self-forming dynamic membrane (150~200 after cell reaction 240min under conditions of electrode voltage is 8V
Mesh) discharge clear water, water outlet COD value is determined, and calculate COD clearances.As a result show, complex mineral three-diemsnional electrode is constructed and nonwoven
Cloth self-forming dynamic membrane electrochemical treatments dyeing waste water, COD clearances reach as high as 83.56%.Complex mineral particle recycling 5
Secondary, it is respectively 83.56%, 80.23%, 82.15%, 83.34%, 82.77% to measure COD clearances.COD clearances are maintained at
More than 80%, illustrate that complex mineral three-diemsnional electrode particle can be reclaimed as catalyst and repeatedly recycled, and catalytic activity according to
It is so very high.
Embodiment 3
It is the chalcopyrites of 40~100 mesh by screened obtained particle diameter, pyrite complex mineral is by quality proportioning 1:1 mixing
Uniformly, add and fill the basal diameter of coking chemical waste water (COD value 4560mg/L) for 9cm, in a height of 8cm cylindrical reactive tank
(anode is Ti/Sb-SnO prepared by thermal decomposition method2Electrode, negative electrode is graphite electrode), the dosage of complex mineral is 10g/L,
Regulation pH value of sewage water makes complex mineral particle locate in reactive tank to 9~10 under Aerated stirring fluidization conditions after well mixed
In suspended state.Under conditions of electrode voltage is 9V after cell reaction 240min by non-woven fabrics self-forming dynamic membrane (150~
200 mesh) discharge clear water, water outlet COD value is determined, and calculate COD clearances.As a result show, complex mineral three-diemsnional electrode construct and
Non-woven fabrics self-forming dynamic membrane electrochemical treatments coking chemical waste water, COD clearances reach as high as 88.89%.Complex mineral particle is repeated
Using 5 times, it is respectively 88.89%, 87.47%, 88.56%, 86.73%, 88.04% to measure COD clearances.COD clearances
More than 86% is maintained at, illustrates that complex mineral three-diemsnional electrode particle can be reclaimed as catalyst and repeatedly recycled, and catalysis
Activity is still very high.
Embodiment 4
It is the chalcopyrites of 40~100 mesh by screened obtained particle diameter, pyrite complex mineral is by quality proportioning 1:1 mixing
Uniformly, add and fill the basal diameter of paper waste (COD value 2650mg/L) for 9cm, in a height of 8cm cylindrical reactive tank
(anode is Ti/Sb-SnO prepared by thermal decomposition method2Electrode, negative electrode is graphite electrode), the dosage of complex mineral is 6g/L, is mixed
Uniform rear regulation pH value of sewage water is closed to 9~10, complex mineral particle is in reactive tank under Aerated stirring fluidization conditions
Suspended state.Clear water is discharged by non-woven fabrics self-forming dynamic membrane after cell reaction 240min under conditions of electrode voltage is 10V,
Water outlet COD value is determined, and calculates COD clearances.As a result show, complex mineral three-diemsnional electrode is constructed and non-woven fabrics self-forming dynamic membrane
(150~200 mesh) electrochemical treatments paper waste, COD clearances reach as high as 93.26%.Complex mineral particle recycling 5
Secondary, it is respectively 93.26%, 90.08%, 92.15%, 93.14%, 91.87% to measure COD clearances.COD clearances are maintained at
More than 90%, illustrate that complex mineral three-diemsnional electrode particle can be reclaimed as catalyst and repeatedly recycled, and catalytic activity according to
It is so very high.
Claims (8)
1. a kind of method that three-diemsnional electrode constructs electrochemical treatments high concentrated organic wastewater, including：
Complex mineral is added in the electrolysis reactor for filling high concentrated organic wastewater, pH to 5~10 is adjusted, in Aerated stirring
Cell reaction is carried out under conditions of fluidisation, clear water is then discharged by non-woven fabrics self-forming dynamic membrane；Wherein, electrolysis reactor middle-jiao yang, function of the spleen and stomach
The Ti/Sb-SnO that extremely prepared by thermal decomposition method2Electrode, negative electrode is graphite electrode；The complex mineral of addition is used as the 3rd of flowing
Electrode.
2. the method that a kind of three-diemsnional electrode according to claim 1 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, the element mass content in the complex mineral includes：Sulphur 40~44%, iron 35~38%, copper 15~18%, remaining
For impurity.
3. the method that a kind of three-diemsnional electrode according to claim 1 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, the addition of the complex mineral is 4g/L~20g/L；Particle size range is 40~100 mesh.
4. the method that a kind of three-diemsnional electrode according to Claims 2 or 3 constructs electrochemical treatments high concentrated organic wastewater, its
It is characterised by, the complex mineral is the mixture of chalcopyrite and pyrite.
5. the method that a kind of three-diemsnional electrode according to claim 4 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, the mass ratio of the chalcopyrite and pyrite is 1：1.
6. the method that a kind of three-diemsnional electrode according to claim 1 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, the condition of the cell reaction is：Electrode voltage is 7~12V；Electrolysis time is 3.5~4.5h.
7. the method that a kind of three-diemsnional electrode according to claim 1 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, the pore diameter range of the non-woven fabrics self-forming dynamic membrane is 150~200 mesh.
8. the method that a kind of three-diemsnional electrode according to claim 1 constructs electrochemical treatments high concentrated organic wastewater, it is special
Levy and be, after the clear water discharge, complex mineral is reused in electrolysis reactor.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113413882A (en) * | 2021-06-23 | 2021-09-21 | 兰州大学 | Preparation method and application of sodium alginate @ natural mineral/biochar composite gel beads |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101838074A (en) * | 2010-05-18 | 2010-09-22 | 华南理工大学 | Method for degrading nitrobenzene waste water by polyphase electrocatalytic oxidation-Fenton coupling process and reactor thereof |
| CN102234166A (en) * | 2010-05-05 | 2011-11-09 | 上海东硕环保科技有限公司 | Three-dimensional electrolytic oxidation and membrane separation integrated industrial waste water recycling process |
| CN106379964A (en) * | 2016-11-08 | 2017-02-08 | 江苏蓝必盛化工环保股份有限公司 | Electrocatalysis-catalytic oxidation device for deeply treating chemical wastewater and wastewater treatment method |
-
2017
- 2017-02-21 CN CN201710093840.0A patent/CN106966465A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102234166A (en) * | 2010-05-05 | 2011-11-09 | 上海东硕环保科技有限公司 | Three-dimensional electrolytic oxidation and membrane separation integrated industrial waste water recycling process |
| CN101838074A (en) * | 2010-05-18 | 2010-09-22 | 华南理工大学 | Method for degrading nitrobenzene waste water by polyphase electrocatalytic oxidation-Fenton coupling process and reactor thereof |
| CN106379964A (en) * | 2016-11-08 | 2017-02-08 | 江苏蓝必盛化工环保股份有限公司 | Electrocatalysis-catalytic oxidation device for deeply treating chemical wastewater and wastewater treatment method |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113413882A (en) * | 2021-06-23 | 2021-09-21 | 兰州大学 | Preparation method and application of sodium alginate @ natural mineral/biochar composite gel beads |
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