CN109279691A - A kind of electrochemical appliance preparing hydrogen peroxide and application - Google Patents
A kind of electrochemical appliance preparing hydrogen peroxide and application Download PDFInfo
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- CN109279691A CN109279691A CN201811216055.0A CN201811216055A CN109279691A CN 109279691 A CN109279691 A CN 109279691A CN 201811216055 A CN201811216055 A CN 201811216055A CN 109279691 A CN109279691 A CN 109279691A
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- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 title claims abstract description 176
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 71
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 45
- 239000007789 gas Substances 0.000 claims abstract description 37
- 239000004744 fabric Substances 0.000 claims abstract description 29
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 26
- 238000004065 wastewater treatment Methods 0.000 claims abstract description 19
- 238000002360 preparation method Methods 0.000 claims abstract description 15
- 239000000463 material Substances 0.000 claims abstract description 8
- 241000894006 Bacteria Species 0.000 claims abstract description 7
- 230000002779 inactivation Effects 0.000 claims abstract description 7
- 229960002163 hydrogen peroxide Drugs 0.000 claims description 78
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 60
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 30
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 28
- 239000001301 oxygen Substances 0.000 claims description 28
- 229910052760 oxygen Inorganic materials 0.000 claims description 28
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 18
- 244000005700 microbiome Species 0.000 claims description 15
- 230000000415 inactivating effect Effects 0.000 claims description 13
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 12
- 229910017604 nitric acid Inorganic materials 0.000 claims description 12
- 239000007800 oxidant agent Substances 0.000 claims description 10
- 230000001590 oxidative effect Effects 0.000 claims description 10
- 238000000034 method Methods 0.000 claims description 9
- 239000007787 solid Substances 0.000 claims description 9
- 239000000843 powder Substances 0.000 claims description 8
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 6
- 229910003460 diamond Inorganic materials 0.000 claims description 5
- 239000010432 diamond Substances 0.000 claims description 5
- 238000002156 mixing Methods 0.000 claims description 4
- 230000008569 process Effects 0.000 claims description 4
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 3
- 239000004202 carbamide Substances 0.000 claims description 3
- 238000005119 centrifugation Methods 0.000 claims description 3
- 239000000919 ceramic Substances 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 230000005611 electricity Effects 0.000 claims description 3
- 239000007788 liquid Substances 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 238000005406 washing Methods 0.000 claims description 3
- 239000006185 dispersion Substances 0.000 claims description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 5
- 239000001257 hydrogen Substances 0.000 abstract description 5
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 5
- 150000002978 peroxides Chemical class 0.000 abstract description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 12
- WQYVRQLZKVEZGA-UHFFFAOYSA-N hypochlorite Chemical compound Cl[O-] WQYVRQLZKVEZGA-UHFFFAOYSA-N 0.000 description 8
- 230000003197 catalytic effect Effects 0.000 description 6
- 229910052757 nitrogen Inorganic materials 0.000 description 6
- 239000013535 sea water Substances 0.000 description 6
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 4
- 238000005273 aeration Methods 0.000 description 4
- 238000006555 catalytic reaction Methods 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 239000000460 chlorine Substances 0.000 description 4
- 229910052801 chlorine Inorganic materials 0.000 description 4
- 239000003792 electrolyte Substances 0.000 description 4
- 230000009467 reduction Effects 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 239000006260 foam Substances 0.000 description 3
- 238000011065 in-situ storage Methods 0.000 description 3
- 230000000087 stabilizing effect Effects 0.000 description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 230000005518 electrochemistry Effects 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 230000001699 photocatalysis Effects 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 238000001354 calcination Methods 0.000 description 1
- 238000001311 chemical methods and process Methods 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 238000012795 verification Methods 0.000 description 1
Classifications
-
- 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
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/722—Oxidation by peroxides
-
- 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
- C02F1/50—Treatment of water, waste water, or sewage by addition or application of a germicide or by oligodynamic treatment
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/24—Halogens or compounds thereof
- C25B1/26—Chlorine; Compounds thereof
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/28—Per-compounds
- C25B1/30—Peroxides
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
Abstract
A kind of electrochemical appliance preparing hydrogen peroxide and application are related to a kind of electrochemical appliance for preparing hydrogen peroxide and application.Purpose is to solve the problems, such as that hydrogen peroxide preparation facilities is that can not persistently provide hydrogen peroxide caused by intermittent flow device or settling vessel and be difficult to widely carry out engineer application.Device is made of cathode chamber, anode chamber, cathode and anode；Cathode chamber side is connected to anode chamber side；Cloth gas chamber is provided with below cathode chamber inner cathode, gas distribution ceiling face is porous plate；The bottom surface of cathode is arranged towards gas distribution ceiling face middle line；The material of cathode is the foamy carbon of graphene doping or the foamy carbon of carbonitride doping.The present invention improves the efficiency of hydrogen peroxide preparation using graphene or the doping of carbonitride and foamy carbon and is conducive to the concentration of stable peroxide hydrogen；Apparatus of the present invention can generate hydrogen peroxide in steady and continuous under low current density.Apparatus of the present invention are applied in wastewater treatment and bacteria inactivation rate.The present invention is suitable for preparing hydrogen peroxide.
Description
Technical field
The present invention relates to a kind of electrochemical appliance for preparing hydrogen peroxide and applications.
Background technique
Hydrogen peroxide is widely used in wastewater treatment and microorganism inactivating device as oxidant, in ultraviolet radiation and
In the research of photocatalysis bacteria inactivation rate, the presence for adding hydrogen peroxide can greatly improve bacteria inactivation rate efficiency, therefore, in recent years
Strengthen the deactivation to microorganism in such a way that electrochemical in-situ produces hydrogen peroxide successively.The preparation method of hydrogen peroxide
It commonly include photocatalytic method, electrochemical synthesis etc..The problem of electrochemical synthesis, is: existing hydrogen peroxide preparation
Device is intermittent flow device or settling vessel, and intermittent flow device is only capable of generating the hydrogenperoxide steam generator of intermittent flow, can not persistently mention
For hydrogen peroxide；It is difficult to widely carry out engineer application using settling vessel when preparing hydrogen peroxide.
Summary of the invention
The present invention in order to solve existing hydrogen peroxide preparation facilities be intermittent flow device or settling vessel, it is caused to hold
It is continuous that hydrogen peroxide is provided and is difficult to the problem of widely carrying out engineer application, propose a kind of electrochemistry dress for preparing hydrogen peroxide
It sets and applies.
The electrochemical appliance that the present invention prepares hydrogen peroxide is made of cathode chamber, anode chamber, cathode and anode；The cathode
Room and anode chamber are set side by side, and cathode chamber side is connected to anode chamber side by pipeline；Cathode and anode are tabular, cathode
It is vertically provided in cathode chamber, anode is vertically provided in anode chamber；Cathode chamber bottom is provided with cathode chamber water inlet pipe and oxygen
Inlet pipe；Cloth gas chamber is provided with below cathode chamber inner cathode, gas distribution ceiling face is porous plate；The bottom surface of cathode is towards gas distribution ceiling face
Middle line setting；Cloth gas chamber is connected to the outlet side of oxygen inlet pipe；Cathode chamber row is provided on the side wall of cathode chamber above cathode
Water pipe；Anode chamber bottom is provided with anode chamber's water inlet pipe, is provided with anode chamber's drainpipe on anode chamber's side wall above anode；Institute
The material for stating cathode is the foamy carbon of graphene doping or the foamy carbon of carbonitride doping；The anode is boron-doped diamond electricity
Pole.
It the principle of the invention and has the beneficial effect that
1, when apparatus of the present invention are run, startup power supply first, the cathode chamber water inlet pipe being arranged respectively to cathode chamber bottom and
Anode chamber's water inlet pipe of anode chamber bottom setting is continuously passed through seawater as electrolyte；Cathode chamber drainpipe and anode chamber row simultaneously
Water pipe draining；After being passed through oxygen by cloth gas chamber of the oxygen inlet pipe into cathode chamber, oxygen evenly distributes in cloth gas chamber and from cloth
The porous plate of gas chamber top surface enters cathode chamber with aeration mode, and the top at cloth gas chamber center, therefore cloth gas chamber energy is arranged in cathode
Enough realize that anticathode two surfaces carry out uniform aeration；By electro-catalysis process, oxygen passes through oxygen reduction in cathode surface
Two electron systems generate hydrogen peroxide in situ, and the hydrogen peroxide that cathode surface generates is dissolved in water to form hydrogenperoxide steam generator,
Finally it is discharged from pole room drainpipe；Chlorine is precipitated in anode by electrochemical process in a large amount of chloride ion in the seawater of anode chamber,
Chlorine is dissolved in water outlet water flow and generates hypochlorite, ultimately forms hypochlorite solution, is discharged from anode chamber's drainpipe；
2, apparatus of the present invention can be stablized under low current density generates hydrogen peroxide, what present invention anode applied with cathode
Minimum current density is 10mA/cm2；
3, in apparatus of the present invention cathode chamber bottom be arranged cathode chamber water inlet pipe and anode chamber bottom setting anode chamber into
Water pipe is continuously passed through seawater as electrolyte, and the hydrogen peroxide that cathode surface generates is dissolved in water to form hydrogenperoxide steam generator,
Finally it is discharged from pole room drainpipe；I.e. apparatus of the present invention are continuous stream mode operation, can continue to generate hydrogenperoxide steam generator,
In the case of continuous flow, the concentration highest stabilizing for the hydrogenperoxide steam generator that the present invention generates is in 26mg/L.
4, foamy carbon itself has electro-catalysis function, can utilize oxygen, by two-electron reduction system and then prepare
Hydrogen oxide, the present invention are adulterated using graphene or carbonitride and foamy carbon, can be improved the catalytic activity of electrode, further increase
The efficiency of hydrogen peroxide preparation and the concentration for being conducive to stable peroxide hydrogen；
Due to the structure that graphene has π-pi-conjugated, graphene is introduced to enhance in the foamy carbon of graphene doping
The distribution capability and transfer ability of electrodic electron, while oxygen vacancies is introduced, hydrogen peroxide is enhanced in the life of the active site
At, therefore can be improved catalytic activity；Similar is that the foamy carbon that carbonitride adulterates introduces more nitrogen holes, nitrogen
The active site that the hydrogen peroxide that hole is used as generates, simultaneously because the electronegativity of nitrogen is stronger, therefore after carbonitride doping
Electrodic electron transfer ability and distribution capability are improved, therefore can be improved catalytic activity；Foamy carbon has tolerance good and the longevity
Long advantage is ordered, foamy carbon makes gained doping type foam carbon cathode be resistant to complicated water quality and have as electrode basement
There is longer service life.
Application of the above-mentioned electrochemical appliance for preparing hydrogen peroxide in wastewater treatment equipment and microorganism inactivating device；
Application of the electrochemical appliance for preparing hydrogen peroxide in wastewater treatment and bacteria inactivation rate is specifically by following
Step carries out: the oxidant inlet of the cathode chamber drainpipe and wastewater treatment equipment that will prepare the electrochemical appliance of hydrogen peroxide connects
It is logical, or the cathode chamber drainpipe of the electrochemical appliance of hydrogen peroxide and the oxidant inlet company of microorganism inactivating device will be prepared
It is logical；Hydrogenperoxide steam generator is inputted into wastewater treatment equipment or microorganism inactivating device using cathode chamber drainpipe as oxidation
Agent is completed.
The electrochemical appliance that the present invention prepares hydrogen peroxide can generate the hydrogenperoxide steam generator of continuous flow, by this peroxidating
It, can be continuously to wastewater treatment equipment after the electrochemical appliance of hydrogen preparation is connect with wastewater treatment equipment or microorganism inactivating device
Or microorganism inactivating device supply hydrogenperoxide steam generator can be improved existing wastewater treatment equipment or microorganism gone out as oxidant
The powder feeding efficiency that removable mounting is set can also improve treatment effeciency at the same time.
Detailed description of the invention
Fig. 1 is the structural schematic diagram for the electrochemical appliance that the present invention prepares hydrogen peroxide；
Fig. 2 is that the hydrogenperoxide steam generator concentration that generates under different hydraulic detention times of device is at any time in embodiment 1
Change curve；
Fig. 3 is that the hydrogenperoxide steam generator concentration that generates under different hydraulic detention times of device is at any time in embodiment 3
Change curve.
Specific embodiment:
The technical solution of the present invention is not limited to the following list, further includes between each specific embodiment
Any reasonable combination.
Specific embodiment 1: embodiment is described with reference to Fig. 1, present embodiment prepares the electrochemistry dress of hydrogen peroxide
It sets and is made of cathode chamber 1, anode chamber 2, cathode 3 and anode 4；
The cathode chamber 1 and anode chamber 2 are set side by side, and 1 side of cathode chamber is connected to 2 side of anode chamber by pipeline；Yin
Pole 3 and anode 4 are tabular, and cathode 3 is vertically provided in cathode chamber 1, and anode 4 is vertically provided in anode chamber 2；Cathode chamber 1
Bottom is provided with cathode chamber water inlet pipe 5 and oxygen inlet pipe 7；Cloth gas chamber 8 is provided with below 1 inner cathode 3 of cathode chamber, cloth gas chamber 8 pushes up
Face is porous plate；The bottom surface of cathode 3 is arranged towards 8 top surface middle line of cloth gas chamber；The outlet side of cloth gas chamber 8 and oxygen inlet pipe 7 connects
It is logical；Cathode chamber drainpipe 9 is provided on the side wall of the cathode chamber 1 of 3 top of cathode；2 bottom of anode chamber is provided with anode chamber's water inlet
Pipe 6 is provided with anode chamber's drainpipe 10 on 2 side wall of anode chamber of the top of anode 4；The material of the cathode 3 is graphene doping
Foamy carbon or carbonitride doping foamy carbon；The anode 4 is boron-doped diamond electrode.
It present embodiment principle and has the beneficial effect that
1, when present embodiment device is run, startup power supply, the cathode chamber being arranged respectively to 1 bottom of cathode chamber are intake first
Pipe 5 and anode chamber's water inlet pipe 6 of 2 bottom of anode chamber setting are continuously passed through seawater as electrolyte；Cathode chamber drainpipe 9 simultaneously
It is drained with anode chamber's drainpipe 10；After being passed through oxygen by cloth gas chamber 8 of the oxygen inlet pipe 7 into cathode chamber 1, oxygen is in cloth gas chamber
8 evenly distribute and enter cathode chamber 1 from the porous plate of 8 top surface of cloth gas chamber with aeration mode, and cathode 3 is arranged at 8 center of cloth gas chamber
Top, therefore cloth gas chamber 8 can be realized and carry out uniform aeration to two surfaces of cathode 3；By electro-catalysis process, oxygen exists
3 surface of cathode generates hydrogen peroxide by two electron system of oxygen reduction in situ, and the hydrogen peroxide that 3 surface of cathode generates is dissolved in
Hydrogenperoxide steam generator is formed in water, is finally discharged from pole room drainpipe 9；A large amount of chloride ion is by electricity in the seawater of anode chamber 2
Chlorine is precipitated in anode in chemical process, and chlorine is dissolved in water outlet water flow and generates hypochlorite, hypochlorite solution is ultimately formed, from anode
Room drainpipe 10 is discharged；
2, present embodiment device can be stablized under low current density generates hydrogen peroxide, present embodiment anode and negative
The minimum current density that pole applies is 10mA/cm2；
3, the sun of 1 bottom of cathode chamber is arranged in present embodiment device cathode chamber water inlet pipe 5 and the setting of 2 bottom of anode chamber
Pole room water inlet pipe 6 is continuously passed through seawater as electrolyte, and the hydrogen peroxide that 3 surface of cathode generates is dissolved in water to form peroxidating
Hydrogen solution is finally discharged from pole room drainpipe 9；I.e. present embodiment device is continuous stream mode operation, can continue to generate
Hydrogen peroxide solution, in continuous flow, the concentration highest stabilizing for the hydrogenperoxide steam generator that the present invention generates is in 26mg/L.
4, foamy carbon itself has electro-catalysis function, can utilize oxygen, by two-electron reduction system and then prepare
Hydrogen oxide, present embodiment are adulterated using graphene or carbonitride and foamy carbon, can be improved the catalytic activity of electrode, further
It improves the efficiency of hydrogen peroxide preparation and is conducive to the concentration of stable peroxide hydrogen；
Due to the structure that graphene has π-pi-conjugated, graphene is introduced to enhance in the foamy carbon of graphene doping
The distribution capability and transfer ability of electrodic electron, while oxygen vacancies is introduced, hydrogen peroxide is enhanced in the life of the active site
At, therefore can be improved catalytic activity；Similar is that the foamy carbon that carbonitride adulterates introduces more nitrogen holes, nitrogen
The active site that the hydrogen peroxide that hole is used as generates, simultaneously because the electronegativity of nitrogen is stronger, therefore after carbonitride doping
Electrodic electron transfer ability and distribution capability are improved, therefore can be improved catalytic activity；Foamy carbon has tolerance good and the longevity
Long advantage is ordered, foamy carbon makes gained doping type foam carbon cathode be resistant to complicated water quality and have as electrode basement
There is longer service life.
Specific embodiment 2: the present embodiment is different from the first embodiment in that: the air inlet of the oxygen inlet pipe 7
End is connected to the gas outlet of oxygenerator.Other steps and parameter are same as the specific embodiment one.
Specific embodiment 3: the present embodiment is different from the first and the second embodiment in that: the cathode 3 and power supply
Cathode is connected by conducting wire；Anode 4 is connect with positive pole by conducting wire；The current density that positive pole applies to anode 4 is most
Low is 10mA/cm2；The minimum 10mA/cm of current density applied to anode 42.Other steps and parameter and specific embodiment
One or two is identical.
Specific embodiment 4: unlike one of present embodiment and specific embodiment one to three: the cathode chamber 1
It is identical with the hydraulic detention time of anode chamber 2.Other steps and parameter are identical as one of specific embodiment one to three.
Specific embodiment 5: present embodiment is unlike specific embodiment four: the cathode chamber 1 and anode chamber
2 hydraulic detention time is 70s~280s.Other steps and parameter are identical as specific embodiment four.
Specific embodiment 6: unlike one of present embodiment and specific embodiment one to five: the graphene
The foamy carbon of doping the preparation method comprises the following steps: using hummers method graphene, by graphene dispersion second alcohol and water mixing
In liquid, mixed liquor is transferred in hydrothermal reaction kettle, is put into block-like foamy carbon, is heated under the conditions of 175~185 DEG C of oil bath
It 5.6~6.5 hours, that is, completes；The quality of graphene is 60~100mg in the mixed liquor of the second alcohol and water, second alcohol and water
The volume of mixed liquor is 295~305ml, and the mixed liquor of second alcohol and water is (1.9~2.1) by second alcohol and water by volume: 1 mixing
It forms；Foamy carbon is cube block, and specification is (49~51) mm × 25mm × 3mm.Other steps and parameter and specific embodiment party
One of formula one to five is identical.
Specific embodiment 7: unlike one of present embodiment and specific embodiment one to six: the carbonitride
The foamy carbon of doping the preparation method comprises the following steps: taking urea to be placed in ceramic crucible, by crucible and in Muffle furnace, at 545~555 DEG C
Lower calcining 1.9~2.1 hours, obtains calcined powder；2.3~2.5g calcined powder is taken to be added to 495~505mL sulfuric acid and nitric acid
Mixed liquor in stir 1.9~2.1 hours, then filter out the solid in mixed liquor, solid be centrifuged and is washed, finally
Solid after centrifugation and washing is placed in drying 47~49 hours in 79~81 DEG C of vacuum oven, obtains g-C3N4；By g-
Mixed liquor is transferred in hydrothermal reaction kettle by C3N4 ultrasonic disperse in the mixed liquor of second alcohol and water, is put into block-like foam
Carbon is heated 5.6~6.5 hours under the conditions of 175~185 DEG C of oil bath, that is, is completed；G- in the mixed liquor of the second alcohol and water
The quality of C3N4 is 60~100mg, and the volume of the mixed liquor of second alcohol and water is 295~305ml, and the mixed liquor of second alcohol and water is by second
Alcohol and water is (1.9~2.1) by volume: 1 mixes；Foamy carbon is cube block, and specification is (49~51) mm × 25mm
×3mm；The mixed liquor of the sulfuric acid and nitric acid is that the 1:1 concentrated sulfuric acid and nitric acid mix by volume ratio；The quality of the concentrated sulfuric acid point
Number is 98%；The mass fraction of concentrated nitric acid is 68%.Other steps and parameter are identical as one of specific embodiment one to six.
Specific embodiment 8: the electrochemical appliance that present embodiment prepares hydrogen peroxide goes out in wastewater treatment and microorganism
Application in work.
The electrochemical appliance that present embodiment prepares hydrogen peroxide can generate the hydrogenperoxide steam generator of continuous flow, by this mistake
It, can be continuously to wastewater treatment after the electrochemical appliance of hydrogen oxide preparation is connect with wastewater treatment equipment or microorganism inactivating device
Device or microorganism inactivating device supply hydrogenperoxide steam generator can be improved existing wastewater treatment equipment or micro- life as oxidant
The powder feeding efficiency of object inactivating device can also improve treatment effeciency at the same time.
Specific embodiment 9: present embodiment is unlike specific embodiment eight: described prepares hydrogen peroxide
Electrochemical appliance in wastewater treatment and bacteria inactivation rate application specifically sequentially include the following steps:
The oxidant inlet of cathode chamber drainpipe 9 and wastewater treatment equipment that the electrochemical appliance of hydrogen peroxide will be prepared connects
It is logical, or the cathode chamber drainpipe 9 of the electrochemical appliance of hydrogen peroxide and the oxidant inlet company of microorganism inactivating device will be prepared
It is logical；Hydrogenperoxide steam generator is inputted into wastewater treatment equipment or microorganism inactivating device using cathode chamber drainpipe 9 as oxidation
Agent is completed.Other steps and parameter are identical as specific embodiment eight.
Using following experimental verification beneficial effects of the present invention:
Embodiment 1:
The electrochemical appliance that the present invention prepares hydrogen peroxide is made of cathode chamber 1, anode chamber 2, cathode 3 and anode 4；It is described
Cathode chamber 1 and anode chamber 2 are set side by side, and 1 side of cathode chamber is connected to 2 side of anode chamber by pipeline；Cathode 3 and anode 4 are
Tabular, cathode 3 are vertically provided in cathode chamber 1, and anode 4 is vertically provided in anode chamber 2；1 bottom of cathode chamber is provided with yin
Pole room water inlet pipe 5 and oxygen inlet pipe 7；Cloth gas chamber 8 is provided with below 1 inner cathode 3 of cathode chamber, 8 top surface of cloth gas chamber is porous plate；
The bottom surface of cathode 3 is arranged towards 8 top surface middle line of cloth gas chamber；Cloth gas chamber 8 is connected to the outlet side of oxygen inlet pipe 7；3 top of cathode
Cathode chamber drainpipe 9 is provided on the side wall of cathode chamber 1；2 bottom of anode chamber is provided with anode chamber's water inlet pipe 6,4 top of anode
Anode chamber's drainpipe 10 is provided on 2 side wall of anode chamber；
The material of the cathode 3 is the foamy carbon of graphene doping；The anode 4 is boron-doped diamond electrode；It is described
The inlet end of oxygen inlet pipe 7 is connected to the gas outlet of oxygenerator；The cathode 3 is connect with power cathode by conducting wire；Anode 4
It is connect with positive pole by conducting wire；The cathode chamber 1 is identical with the hydraulic detention time of anode chamber 2；Positive pole is to anode 4
The current density of application is 10mA/cm2；The current density applied to anode 4 is 10mA/cm2；The cathode chamber 1 and anode chamber 2
Hydraulic detention time it is identical；
The foamy carbon of graphene doping the preparation method comprises the following steps: using hummers method graphene, by graphene point
It is dispersed in the mixed liquor of second alcohol and water, mixed liquor is transferred in hydrothermal reaction kettle, be put into block-like foamy carbon, at 180 DEG C
It heats 6 hours, that is, completes under the conditions of oil bath；The quality of graphene is 80mg, second alcohol and water in the mixed liquor of the second alcohol and water
The volume of mixed liquor be 300ml, the mixed liquor of second alcohol and water mixes by volume for 2:1 by second alcohol and water；Foamy carbon
For cube block, specification is 50mm × 25mm × 3mm；
Fig. 2 is that the hydrogenperoxide steam generator concentration that generates under different hydraulic detention times of device is at any time in embodiment 1
Change curve；The corresponding hydraulic detention time of curve 1~3 is 70s, 140s and 280s in Fig. 2；Fig. 2, it can be seen that
After 10min, concentration of hydrogen peroxide value caused by device starts the value that tends towards stability in embodiment 1；And when with hydraulic retention
Between increase, concentration of hydrogen peroxide caused by device increases in embodiment 1.When hydraulic detention time is 70s, what device generated
Concentration of hydrogen peroxide is stablized in 10mg/L.
Embodiment 2:
The present embodiment is unlike the first embodiment: the material of the cathode 3 is foamy carbon；Hydraulic detention time is 70s.
When hydraulic detention time is 70s in embodiment 2, the concentration of hydrogen peroxide that device generates is less than 1mg/L.
Embodiment 3:
The electrochemical appliance that the present invention prepares hydrogen peroxide is made of cathode chamber 1, anode chamber 2, cathode 3 and anode 4；It is described
Cathode chamber 1 and anode chamber 2 are set side by side, and 1 side of cathode chamber is connected to 2 side of anode chamber by pipeline；Cathode 3 and anode 4 are
Tabular, cathode 3 are vertically provided in cathode chamber 1, and anode 4 is vertically provided in anode chamber 2；1 bottom of cathode chamber is provided with yin
Pole room water inlet pipe 5 and oxygen inlet pipe 7；Cloth gas chamber 8 is provided with below 1 inner cathode 3 of cathode chamber, 8 top surface of cloth gas chamber is porous plate；
The bottom surface of cathode 3 is arranged towards 8 top surface middle line of cloth gas chamber；Cloth gas chamber 8 is connected to the outlet side of oxygen inlet pipe 7；3 top of cathode
Cathode chamber drainpipe 9 is provided on the side wall of cathode chamber 1；2 bottom of anode chamber is provided with anode chamber's water inlet pipe 6,4 top of anode
Anode chamber's drainpipe 10 is provided on 2 side wall of anode chamber；The material of the cathode 3 is the foamy carbon of carbonitride doping；The sun
Pole 4 is boron-doped diamond electrode.
The inlet end of the oxygen inlet pipe 7 is connected to the gas outlet of oxygenerator；The cathode 3 passes through conducting wire with power cathode
Connection；Anode 4 is connect with positive pole by conducting wire；The current density that positive pole applies to anode 4 is 10mA/cm2；On the sunny side
The current density that pole 4 applies is 10mA/cm2；The cathode chamber 1 is identical with the hydraulic detention time of anode chamber 2；
The foamy carbon of carbonitride doping the preparation method comprises the following steps: taking urea to be placed in ceramic crucible, by crucible and in horse
Not in furnace, is calcined 2 hours at 550 DEG C, obtain calcined powder；2.4g calcined powder is taken to be added to 500mL sulfuric acid and nitric acid
Stirred 2 hours in mixed liquor, then filter out the solid in mixed liquor, solid is centrifuged and is washed, finally will centrifugation and
Solid after washing is placed in drying 48 hours in 80 DEG C of vacuum oven, obtains g-C3N4；By g-C3N4 ultrasonic disperse in second
In the mixed liquor of alcohol and water, mixed liquor is transferred in hydrothermal reaction kettle, is put into block-like foamy carbon, in 180 DEG C of oil bath item
It heats 6 hours, that is, completes under part；The quality of g-C3N4 is 80mg, the mixing of second alcohol and water in the mixed liquor of the second alcohol and water
The volume of liquid is 300ml, and the mixed liquor of second alcohol and water is mixed by volume for 2:1 by second alcohol and water；Foamy carbon is cube
Body block, specification are 50mm × 25mm × 3mm；The mixed liquor of the sulfuric acid and nitric acid is that the 1:1 concentrated sulfuric acid and nitric acid mix by volume ratio
It closes；The mass fraction of the concentrated sulfuric acid is 98%；The mass fraction of concentrated nitric acid is 68%.
Fig. 3 is that the hydrogenperoxide steam generator concentration that generates under different hydraulic detention times of device is at any time in embodiment 3
Change curve；The corresponding hydraulic detention time of curve 1~3 is 70s, 140s and 280s in Fig. 3；Fig. 3, it can be seen that
After 5min, concentration of hydrogen peroxide value caused by device starts the value that tends towards stability in embodiment 3；And with hydraulic detention time
Increase, concentration of hydrogen peroxide caused by device increases in embodiment 3.When hydraulic detention time is 280s, what device generated
The concentration highest stabilizing of hydrogenperoxide steam generator is in 26mg/L.
Embodiment 4:
The present embodiment is as different from Example 3: the material of the cathode 3 is foamy carbon；Hydraulic detention time is 70s.
When hydraulic detention time is 70s in embodiment 4, the concentration of hydrogen peroxide highest 1.1mg/L of device generation.
Claims (9)
1. a kind of electrochemical appliance for preparing hydrogen peroxide, it is characterised in that: the device is by cathode chamber (1), anode chamber (2), yin
Pole (3) and anode (4) are constituted；
The cathode chamber (1) and anode chamber (2) are set side by side, and cathode chamber (1) side and anode chamber (2) side are connected by pipeline
It is logical；Cathode (3) and anode (4) are tabular, and cathode (3) is vertically provided in cathode chamber (1), and anode (4) is vertically provided at sun
In pole room (2)；Cathode chamber (1) bottom is provided with cathode chamber water inlet pipe (5) and oxygen inlet pipe (7)；Cathode chamber (1) inner cathode (3)
Lower section is provided with cloth gas chamber (8), and cloth gas chamber (8) top surface is porous plate；The bottom surface of cathode (3) is towards cloth gas chamber (8) top surface middle line
Setting；Cloth gas chamber (8) is connected to the outlet side of oxygen inlet pipe (7)；It is provided on the side wall of cathode chamber (1) above cathode (3)
Cathode chamber drainpipe (9)；Anode chamber (2) bottom is provided with anode chamber's water inlet pipe (6), anode chamber (2) side wall above anode (4)
On be provided with anode chamber's drainpipe (10)；
The material of the cathode (3) is the foamy carbon of graphene doping or the foamy carbon of carbonitride doping；
The anode (4) is boron-doped diamond electrode.
2. the electrochemical appliance according to claim 1 for preparing hydrogen peroxide, it is characterised in that: the oxygen inlet pipe (7)
Inlet end be connected to the gas outlet of oxygenerator.
3. the electrochemical appliance according to claim 1 for preparing hydrogen peroxide, it is characterised in that: the cathode (3) and electricity
Source cathode is connected by conducting wire；Anode (4) is connect with positive pole by conducting wire；The electric current that positive pole applies to anode (4)
The minimum 10mA/cm of density2；The minimum 10mA/cm of current density applied to anode (4)2。
4. the electrochemical appliance according to claim 1 for preparing hydrogen peroxide, it is characterised in that: the cathode chamber (1) and
The hydraulic detention time of anode chamber (2) is identical.
5. the electrochemical appliance according to claim 4 for preparing hydrogen peroxide, it is characterised in that: the cathode chamber (1) and
The hydraulic detention time of anode chamber (2) is 70s~280s.
6. the electrochemical appliance according to claim 1 for preparing hydrogen peroxide, it is characterised in that: the graphene doping
Foamy carbon the preparation method comprises the following steps: using hummers method graphene, by graphene dispersion in the mixed liquor of second alcohol and water,
Mixed liquor is transferred in hydrothermal reaction kettle, block-like foamy carbon is put into, under the conditions of 175~185 DEG C of oil bath heat 5.6~
It 6.5 hours, that is, completes；The quality of graphene is 60~100mg, the mixed liquor of second alcohol and water in the mixed liquor of the second alcohol and water
Volume be 295~305ml, the mixed liquor of second alcohol and water is (1.9~2.1) by second alcohol and water by volume: 1 mixes；
Foamy carbon is cube block, and specification is (49~51) mm × 25mm × 3mm.
7. the electrochemical appliance according to claim 1 for preparing hydrogen peroxide, it is characterised in that: the carbonitride doping
Foamy carbon the preparation method comprises the following steps: urea is taken to be placed in ceramic crucible, by crucible and in Muffle furnace, calcined at 545~555 DEG C
1.9~2.1 hours, obtain calcined powder；2.3~2.5g calcined powder is taken to be added to the mixing of 495~505mL sulfuric acid and nitric acid
It is stirred 1.9~2.1 hours in liquid, then filters out the solid in mixed liquor, solid is centrifuged and is washed, it finally will centrifugation
It is placed in drying 47~49 hours in 79~81 DEG C of vacuum oven with the solid after washing, obtains g-C3N4；G-C3N4 is surpassed
Sound is scattered in the mixed liquor of second alcohol and water, and mixed liquor is transferred in hydrothermal reaction kettle, block-like foamy carbon is put into, 175
It heats 5.6~6.5 hours, that is, completes under the conditions of~185 DEG C of oil bath；The quality of g-C3N4 in the mixed liquor of the second alcohol and water
Volume for 60~100mg, the mixed liquor of second alcohol and water is 295~305ml, and the mixed liquor of second alcohol and water presses body by second alcohol and water
Product is than being (1.9~2.1): 1 mixes；Foamy carbon is cube block, and specification is (49~51) mm × 25mm × 3mm；It is described
The mixed liquor of sulfuric acid and nitric acid is that the 1:1 concentrated sulfuric acid and nitric acid mix by volume ratio；The mass fraction of the concentrated sulfuric acid is 98%；It is dense
The mass fraction of nitric acid is 68%.
8. preparing the electrochemical appliance of hydrogen peroxide answering in wastewater treatment and bacteria inactivation rate as described in claim 1
With.
9. application according to claim 8, it is characterised in that: the electrochemical appliance for preparing hydrogen peroxide is useless
Application in water process and bacteria inactivation rate specifically sequentially includes the following steps:
The oxidant inlet of cathode chamber drainpipe (9) and wastewater treatment equipment that the electrochemical appliance of hydrogen peroxide will be prepared connects
It is logical, or the oxidant inlet of cathode chamber drainpipe (9) and microorganism inactivating device of the electrochemical appliance of hydrogen peroxide will be prepared
Connection；Inputted using cathode chamber drainpipe (9) into wastewater treatment equipment or microorganism inactivating device hydrogenperoxide steam generator as
Oxidant is completed.
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| CN112030182A (en) * | 2020-09-18 | 2020-12-04 | 安徽大学 | Electrochemical device, method for synthesizing hydrogen peroxide by electrochemically decomposing urea and application |
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