CN112376072A - Membrane electrode for producing ozone water by using tap water and preparation method thereof - Google Patents
Membrane electrode for producing ozone water by using tap water and preparation method thereof Download PDFInfo
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- CN112376072A CN112376072A CN202011257518.5A CN202011257518A CN112376072A CN 112376072 A CN112376072 A CN 112376072A CN 202011257518 A CN202011257518 A CN 202011257518A CN 112376072 A CN112376072 A CN 112376072A
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- 239000012528 membrane Substances 0.000 title claims abstract description 167
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 title claims abstract description 56
- 238000002360 preparation method Methods 0.000 title claims abstract description 49
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 32
- 239000008399 tap water Substances 0.000 title claims abstract description 23
- 235000020679 tap water Nutrition 0.000 title claims abstract description 23
- 239000003054 catalyst Substances 0.000 claims abstract description 100
- 238000005341 cation exchange Methods 0.000 claims abstract description 68
- 239000000919 ceramic Substances 0.000 claims abstract description 34
- 239000002131 composite material Substances 0.000 claims abstract description 34
- 239000003014 ion exchange membrane Substances 0.000 claims abstract description 31
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 25
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 16
- 239000001301 oxygen Substances 0.000 claims abstract description 16
- 239000002994 raw material Substances 0.000 claims abstract description 14
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 8
- 239000007787 solid Substances 0.000 claims abstract description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 73
- 229910003460 diamond Inorganic materials 0.000 claims description 57
- 239000010432 diamond Substances 0.000 claims description 57
- 239000000463 material Substances 0.000 claims description 44
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 36
- 229910052799 carbon Inorganic materials 0.000 claims description 36
- 239000004642 Polyimide Substances 0.000 claims description 31
- 238000000034 method Methods 0.000 claims description 31
- 229920001721 polyimide Polymers 0.000 claims description 31
- 229910002804 graphite Inorganic materials 0.000 claims description 28
- 239000010439 graphite Substances 0.000 claims description 28
- 239000007789 gas Substances 0.000 claims description 23
- 230000003197 catalytic effect Effects 0.000 claims description 20
- PPWPWBNSKBDSPK-UHFFFAOYSA-N [B].[C] Chemical compound [B].[C] PPWPWBNSKBDSPK-UHFFFAOYSA-N 0.000 claims description 19
- 125000005842 heteroatom Chemical group 0.000 claims description 18
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 18
- 150000003058 platinum compounds Chemical class 0.000 claims description 18
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- 238000006243 chemical reaction Methods 0.000 claims description 13
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- 229920005989 resin Polymers 0.000 claims description 13
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 12
- 239000011153 ceramic matrix composite Substances 0.000 claims description 12
- USIUVYZYUHIAEV-UHFFFAOYSA-N diphenyl ether Chemical compound C=1C=CC=CC=1OC1=CC=CC=C1 USIUVYZYUHIAEV-UHFFFAOYSA-N 0.000 claims description 12
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 12
- 238000001035 drying Methods 0.000 claims description 11
- 238000001125 extrusion Methods 0.000 claims description 11
- UGKDIUIOSMUOAW-UHFFFAOYSA-N iron nickel Chemical compound [Fe].[Ni] UGKDIUIOSMUOAW-UHFFFAOYSA-N 0.000 claims description 11
- 125000004432 carbon atom Chemical group C* 0.000 claims description 9
- 239000003153 chemical reaction reagent Substances 0.000 claims description 9
- 229910021389 graphene Inorganic materials 0.000 claims description 9
- 238000000227 grinding Methods 0.000 claims description 9
- 229910052704 radon Inorganic materials 0.000 claims description 9
- SYUHGPGVQRZVTB-UHFFFAOYSA-N radon atom Chemical compound [Rn] SYUHGPGVQRZVTB-UHFFFAOYSA-N 0.000 claims description 9
- 238000010992 reflux Methods 0.000 claims description 9
- 238000003756 stirring Methods 0.000 claims description 9
- 230000008595 infiltration Effects 0.000 claims description 8
- 238000001764 infiltration Methods 0.000 claims description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 7
- WSMYVTOQOOLQHP-UHFFFAOYSA-N Malondialdehyde Chemical compound O=CCC=O WSMYVTOQOOLQHP-UHFFFAOYSA-N 0.000 claims description 6
- DSVGQVZAZSZEEX-UHFFFAOYSA-N [C].[Pt] Chemical compound [C].[Pt] DSVGQVZAZSZEEX-UHFFFAOYSA-N 0.000 claims description 6
- GTDPSWPPOUPBNX-UHFFFAOYSA-N ac1mqpva Chemical compound CC12C(=O)OC(=O)C1(C)C1(C)C2(C)C(=O)OC1=O GTDPSWPPOUPBNX-UHFFFAOYSA-N 0.000 claims description 6
- 238000010438 heat treatment Methods 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 125000006158 tetracarboxylic acid group Chemical group 0.000 claims description 6
- 230000003993 interaction Effects 0.000 claims description 5
- 229910052697 platinum Inorganic materials 0.000 claims description 5
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 4
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical compound OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 claims description 4
- 239000011159 matrix material Substances 0.000 claims description 4
- 229910052757 nitrogen Inorganic materials 0.000 claims description 4
- 238000002390 rotary evaporation Methods 0.000 claims description 4
- 229910052710 silicon Inorganic materials 0.000 claims description 4
- 239000010703 silicon Substances 0.000 claims description 4
- 239000011593 sulfur Substances 0.000 claims description 4
- 229910052717 sulfur Inorganic materials 0.000 claims description 4
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims description 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 3
- 229910052736 halogen Inorganic materials 0.000 claims description 3
- 150000002367 halogens Chemical class 0.000 claims description 3
- 229910052698 phosphorus Inorganic materials 0.000 claims description 3
- 239000011574 phosphorus Substances 0.000 claims description 3
- JOKPITBUODAHEN-UHFFFAOYSA-N sulfanylideneplatinum Chemical class [Pt]=S JOKPITBUODAHEN-UHFFFAOYSA-N 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims 1
- 229940045985 antineoplastic platinum compound Drugs 0.000 claims 1
- 125000002091 cationic group Chemical group 0.000 claims 1
- 229910052739 hydrogen Inorganic materials 0.000 claims 1
- 239000001257 hydrogen Substances 0.000 claims 1
- 229910052742 iron Inorganic materials 0.000 claims 1
- 238000010030 laminating Methods 0.000 claims 1
- 229940118019 malondialdehyde Drugs 0.000 claims 1
- 239000002184 metal Substances 0.000 claims 1
- 229910052759 nickel Inorganic materials 0.000 claims 1
- 230000003204 osmotic effect Effects 0.000 claims 1
- 150000002927 oxygen compounds Chemical class 0.000 claims 1
- CLSUSRZJUQMOHH-UHFFFAOYSA-L platinum dichloride Chemical class Cl[Pt]Cl CLSUSRZJUQMOHH-UHFFFAOYSA-L 0.000 claims 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 18
- 239000006227 byproduct Substances 0.000 abstract description 6
- 239000003792 electrolyte Substances 0.000 abstract description 6
- 238000005265 energy consumption Methods 0.000 abstract description 5
- 238000005868 electrolysis reaction Methods 0.000 abstract description 4
- 238000004659 sterilization and disinfection Methods 0.000 abstract description 4
- 235000020188 drinking water Nutrition 0.000 abstract description 3
- 239000003651 drinking water Substances 0.000 abstract description 3
- 230000005518 electrochemistry Effects 0.000 abstract description 2
- 230000007613 environmental effect Effects 0.000 abstract description 2
- 239000010865 sewage Substances 0.000 abstract description 2
- 239000013078 crystal Substances 0.000 description 17
- 229910052755 nonmetal Inorganic materials 0.000 description 14
- 238000003825 pressing Methods 0.000 description 9
- 239000000047 product Substances 0.000 description 9
- 238000000151 deposition Methods 0.000 description 8
- 150000003460 sulfonic acids Chemical class 0.000 description 8
- 239000006185 dispersion Substances 0.000 description 5
- ZSBDPRIWBYHIAF-UHFFFAOYSA-N n-acetylacetamide Chemical compound CC(=O)NC(C)=O ZSBDPRIWBYHIAF-UHFFFAOYSA-N 0.000 description 5
- 239000002245 particle Substances 0.000 description 5
- 238000002791 soaking Methods 0.000 description 5
- 238000010025 steaming Methods 0.000 description 5
- 239000000758 substrate Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 3
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- 238000005260 corrosion Methods 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- QYSYEILYXGRUOM-UHFFFAOYSA-N [Cl].[Pt] Chemical compound [Cl].[Pt] QYSYEILYXGRUOM-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- -1 platinum hydroxide compound Chemical class 0.000 description 2
- 238000005728 strengthening Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910019032 PtCl2 Inorganic materials 0.000 description 1
- 229910019029 PtCl4 Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000004061 bleaching Methods 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 239000013081 microcrystal Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- BDHFUVZGWQCTTF-UHFFFAOYSA-M sulfonate Chemical compound [O-]S(=O)=O BDHFUVZGWQCTTF-UHFFFAOYSA-M 0.000 description 1
- 125000001273 sulfonato group Chemical group [O-]S(*)(=O)=O 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- FBEIPJNQGITEBL-UHFFFAOYSA-J tetrachloroplatinum Chemical compound Cl[Pt](Cl)(Cl)Cl FBEIPJNQGITEBL-UHFFFAOYSA-J 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 238000009423 ventilation Methods 0.000 description 1
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- 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
- C25B1/13—Ozone
-
- 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
- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
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- 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
- C25B13/00—Diaphragms; Spacing elements
- C25B13/02—Diaphragms; Spacing elements characterised by shape or form
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
Abstract
The invention relates to the technical field of environmental electrochemistry, in particular to a membrane electrode for generating ozone water by using tap water and a preparation method thereof. The membrane electrode comprises an ion exchange membrane, an anode catalyst layer arranged on one side of the ion exchange membrane and a cathode catalyst layer arranged on the other side of the ion exchange membrane, wherein the cation exchange membrane is a porous ceramic-based solid polymer electrolyte membrane or a graphite-phase C3N4/PFSA solid electrolyte composite membrane. The invention has wide application, such as drinking water disinfection, municipal sewage treatment, medical disinfection and the like. The membrane electrode of the invention only needs water as the raw material for producing ozone water by using tap water, thus the energy consumption is low; the invention does not need an air pump, and the noise generated by use is low; high-purity ozone is generated, no other by-product is generated, no nitrogen oxide is generated, and no secondary pollution is generated to the environment; can work for a long time, has stable electrolysis efficiency and does not need to additionally add oxygen-containing electrolyte.
Description
Technical Field
The invention relates to the technical field of environmental electrochemistry, in particular to a membrane electrode for generating ozone water by using tap water and a preparation method thereof.
Background
Ozone can be used for purifying air, bleaching drinking water, sterilizing, treating industrial waste and the like. In practical application, ozone is mainly prepared by a dielectric barrier discharge method, an electrolytic method, an ultraviolet method and the like. The widely applied ozone generation technology at present is a high-voltage discharge ozone generation technology, noise generated by an air pump is large, toxic nitrogen oxides are easily generated in the process of preparing ozone, and the concentration of the prepared ozone is low. The electrolytic water type ozone preparation device is high in current efficiency, the prepared ozone is high in concentration, nitrogen oxide cannot be generated in the electrolytic process, secondary pollution to the environment cannot be generated, however, in the prior art, acid electrolyte is generally required to be utilized, the generated ozone is output as gas, and the ozone is required to be introduced into water through a pipeline to prepare ozone water.
Disclosure of Invention
In order to overcome the defects and shortcomings in the prior art, the invention aims to provide a membrane electrode for producing ozone water by using tap water, wherein the membrane electrode only needs water as a raw material for preparing ozone, has low energy consumption, can generate high-purity ozone, and does not contain any other by-product.
Another object of the present invention is to provide a method for preparing a membrane electrode for producing ozone water using tap water, which is simple in operation, low in production cost, and high in product quality.
The purpose of the invention is realized by the following technical scheme: a membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane, an anode catalyst layer arranged on one side of the ion exchange membrane and a cathode catalyst layer arranged on the other side of the ion exchange membrane, wherein the cation exchange membrane is a porous ceramic-based solid polymer electrolyte membrane or a graphite-phase C3N4/PFSA solid electrolyte composite membrane.
The porous ceramic-based solid polymer electrolyte membrane is used as a cation exchange membrane, electrolyte does not need to be added, and the generation of byproducts is reduced; the conductive coating has good conductivity and high current efficiency; has good chemical stability and thermal stability.
The graphite phase C3N4/PFSA solid electrolyte composite membrane is used as a cation exchange membrane, so that the conductivity is remarkably improved, and the proton conductivity is remarkably improved.
The raw material for producing ozone only needs water, so that the energy consumption is low, the electrolysis efficiency is not influenced by the air quality, drying is not needed, and nitrogen oxides NOx are not generated; the electrolytic tank can work for a long time, has stable electrolytic efficiency, and does not need to additionally add any oxygen-containing electrolyte; high purity ozone and oxygen can be generated without any other by-products.
Further, the anode catalyst layer is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer is made of a graphene composite material.
The boron-carbon diamond heterojunction material has high mechanical property, good corrosion resistance, good thermal stability and simultaneously extremely high electrochemical stability; the membrane electrode formed by the structure is corrosion resistant, and the problem of falling off of an electrolytic catalyst coating is solved; no hot spot damage risk, strengthening unique structural design, far exceeding the common PEM electrolytic ozone device; the service life of the membrane electrode can continuously work for more than 3 years; the ozone is generated by using low-voltage direct current, the voltage is not higher than 36V, the safety is high, more ozone gas is generated by less energy, the purity of the generated ozone gas is far higher than that of a corona method and an ultraviolet light method, the purity of the generated ozone gas is more than 400% of that of the corona method, and the purity of the generated ozone gas is more than 900% of that of the ultraviolet light method; the ozone generator has the advantages of low power consumption, no maintenance, low frequency, no need of circulating cooling, high purity ozone durability, ozone generation instantaneity and the like.
The other purpose of the invention is realized by the following technical scheme: a preparation method of a membrane electrode for producing ozone water by using tap water comprises the following steps:
(1) preparing an anode catalyst layer by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane;
(3) preparing a cathode catalyst layer;
(4) pressing the anode catalyst layer, the cation exchange membrane and the cathode catalyst layer to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
The preparation method is simple, the process is mature, and the membrane electrode prepared by pressing occupies small space, is highly integrated and portable; the structure is stable and the durability is good; the membrane electrode has good ventilation performance, and the cation exchange membrane is not easy to deform in the preparation process.
Further, in the step (1), the preparation method of the anode catalyst layer includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at the temperature of 1300-1700 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon matrix to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into diamond microcrystal under the pressure of 5-7Gpa, and then grows into a diamond film.
The anode catalyst layer prepared by the method has simple instrument and equipment and convenient operation; the manufacturing cost of the diamond is low, and the film forming process is easy to control; the diamond crystal nucleus grows under the pressure of 5-7Gpa, and the speed and the quality of the deposited film can be effectively improved.
Further, in the step (2), the cation exchange membrane is a porous ceramic-based solid electrolyte composite membrane, and the preparation method of the cation exchange membrane includes the following steps:
a1, preparation of the ceramic-based sulfonated polyimide material: taking 2.8-3.2 parts of diphenyl ether tetracarboxylic dianhydride monoatomic dispersion platinum carbon, 0.8-1.2 parts of diacetyl amide and 2.8-3.2 parts of malonaldehyde according to parts by weight to obtain sulfonated polyimide;
a2, adding sulfonated polyimide into propylene glycol to prepare a sulfonated polyimide solution, wherein the weight ratio of the sulfonated polyimide to the propylene glycol is (7.5-8.5): 0.28 to 0.32, and pressurizing the porous nickel-iron ceramic plate to perform a permeation reaction to prepare the ceramic matrix composite heterogeneous membrane;
a3, soaking the ceramic matrix composite heterogeneous membrane obtained in the step A2 in a hydrochloric acid solution to obtain the cation exchange membrane.
The porous ceramic-based solid electrolyte composite membrane is prepared by the method, and the method is simple to operate; the porous ceramic-based solid electrolyte composite membrane prepared by the method has good conductivity and high current efficiency; the chemical stability and the thermal stability are good; can conduct current and selectively permeate ions to couple reaction and separation.
Further, in the step A2, the pressure for the infiltration reaction is 18-22MPa on the porous nickel-iron ceramic plate.
Further, the cation exchange membrane is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane comprises the following steps: mixing the graphite phase and the perfluorinated sulfonic acid resin according to the weight ratio of 3.8-4.2:0.9-1.1, heating, and performing extrusion molding to form a film, thus obtaining the cation exchange membrane.
The graphite phase C3N4/PFSA solid electrolyte composite membrane prepared by the method has obviously increased conductivity and proton conductivity, probably because acid-base conjugate ion pairs are formed by abundant base groups on the graphite phase C3N4 and sulfonate groups on the PFSA resin, and the proton selectivity and the proton transmission speed are increased.
Further, in the step (2), after the graphite phase and the perfluorosulfonic acid resin are mixed, the mixture is heated to 190 ℃ and 210 ℃ to perform extrusion molding to form the film.
Further, in the step (3), the preparation method of the cathode catalytic material for preparing the cathode catalyst layer includes the following steps: taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying for 7-9h at the temperature of 380-420 ℃ after stirring, refluxing and rotary evaporation, grinding to below 50nm, and treating and interacting at the temperature of 950-1050 ℃ to obtain the cathode catalytic material.
The cathode catalyst layer is prepared by adopting the method, and test results show that the platinum element in the catalyst exists in the form of single-atom platinum, the catalytic activity is high, and in acid and alkaline systems, the initial potential and half-wave potential of oxygen reduction are equivalent to those of a commercial carbon-supported platinum catalyst with the platinum content of 20%; and other metal elements are not introduced in the preparation process, so that the stability is better.
Further, the non-metal heteroatom is at least one of nitrogen, oxygen, sulfur, phosphorus, silicon and halogen, and the platinum compound is at least one of platinum hydroxide compound, platinum sulfur compound and platinum chlorine compound.
The invention has the beneficial effects that: the membrane electrode for producing ozone water by using tap water has wide application, such as drinking water disinfection, municipal sewage treatment, medical disinfection and the like. The membrane electrode of the invention only needs water as the raw material for producing ozone water by using tap water, thus the energy consumption is low; the invention does not need an air pump, and the noise generated by use is low; high-purity ozone is generated, no other by-product is generated, no nitrogen oxide is generated, and no secondary pollution is generated to the environment; can work for a long time, has stable electrolysis efficiency and does not need to additionally add oxygen-containing electrolyte.
The preparation method of the membrane electrode for producing ozone water by using tap water has the advantages of simple operation, low production cost and high product quality.
Drawings
FIG. 1 is a schematic structural view of the present invention;
the reference signs are: 1-anode catalyst layer; 2-ion exchange membrane; 3-cathode catalyst layer.
Detailed Description
The present invention will be further described below to facilitate understanding of those skilled in the art, and the embodiments are not to be construed as limiting the present invention.
In a typical embodiment of the present invention, the object of the present invention is achieved by the following technical solutions: a membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane, an anode catalyst layer arranged on one side of the ion exchange membrane and a cathode catalyst layer arranged on the other side of the ion exchange membrane, wherein the cation exchange membrane is a porous ceramic-based solid polymer electrolyte membrane or a graphite-phase C3N4/PFSA solid electrolyte composite membrane.
Further, the anode catalyst layer is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer is made of a graphene composite material.
A preparation method of a membrane electrode for producing ozone water by using tap water comprises the following steps:
(1) preparing an anode catalyst layer by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane;
(3) preparing a cathode catalyst layer;
(4) pressing the anode catalyst layer, the cation exchange membrane and the cathode catalyst layer to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
Further, in the step (1), the preparation method of the anode catalyst layer includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at the temperature of 1300-1700 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon matrix to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into diamond micro-products under the pressure of 5-7Gpa, and then grows into a diamond film.
Further, in the step (2), the cation exchange membrane is a porous ceramic-based solid electrolyte composite membrane, and the preparation method of the cation exchange membrane includes the following steps:
a1, preparation of the ceramic-based sulfonated polyimide material: taking 2.8-3.2 parts of diphenyl ether tetracarboxylic dianhydride monoatomic dispersion platinum carbon, 0.8-1.2 parts of diacetyl amide and 2.8-3.2 parts of malonaldehyde according to parts by weight to obtain sulfonated polyimide;
a2, adding sulfonated polyimide into propylene glycol to prepare a sulfonated polyimide solution, wherein the weight ratio of the sulfonated polyimide to the propylene glycol is (7.5-8.5): 0.28 to 0.32, and pressurizing the porous nickel-iron ceramic plate to perform a permeation reaction to prepare the ceramic matrix composite heterogeneous membrane;
a3, soaking the ceramic matrix composite heterogeneous membrane obtained in the step A2 in a hydrochloric acid solution to obtain the cation exchange membrane.
Further, in the step A2, the pressure for the infiltration reaction is 18-22MPa on the porous nickel-iron ceramic plate.
Further, the cation exchange membrane is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane comprises the following steps: mixing the graphite phase and the perfluorinated sulfonic acid resin according to the weight ratio of 3.8-4.2:0.9-1.1, heating, and performing extrusion molding to form a film, thus obtaining the cation exchange membrane.
Further, in the step (2), after the graphite phase and the perfluorosulfonic acid resin are mixed, the mixture is heated to 190 ℃ and 210 ℃ to perform extrusion molding to form the film.
Further, in the step (3), the preparation method of the cathode catalytic material for preparing the cathode catalyst layer includes the following steps: taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying for 7-9h at the temperature of 380-420 ℃ after stirring, refluxing and rotary evaporation, grinding to below 50nm, and treating and interacting at the temperature of 950-1050 ℃ to obtain the cathode catalytic material.
Further, the non-metal heteroatom is at least one of nitrogen, oxygen, sulfur, phosphorus, silicon and halogen, and the platinum compound is at least one of platinum hydroxide compound, platinum sulfur compound and platinum chlorine compound.
Example 1
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a porous ceramic-based solid polymer electrolyte membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1500 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon substrate to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 6Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a porous ceramic-based solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps:
a1, preparation of the ceramic-based sulfonated polyimide material: taking 3 parts of diphenyl ether tetracarboxylic dianhydride monoatomic dispersion platinum carbon, 1 part of diacetyl amide and 3 parts of malonaldehyde according to parts by weight to obtain sulfonated polyimide;
a2, adding sulfonated polyimide into propylene glycol to prepare a sulfonated polyimide solution, wherein the weight ratio of the sulfonated polyimide to the propylene glycol is (8): 0.3, pressurizing the porous nickel-iron ceramic plate for carrying out a permeation reaction to prepare the ceramic matrix composite heterogeneous membrane;
a3, soaking the ceramic matrix composite heterogeneous membrane obtained in the step A2 in a hydrochloric acid solution to obtain the cation exchange membrane 2.
In the step A2, the pressure for the infiltration reaction is 20Mpa on the porous nickel-iron ceramic plate.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying at the temperature of 400 ℃ for 8 hours after stirring, refluxing and rotary steaming, grinding to the particle size of less than 50nm, and treating at the temperature of 1000 ℃ for interaction.
The nonmetallic heteroatom is nitrogen, and the platinum compound is Pt (OH)2。
The membrane electrode of the embodiment only needs water as a raw material for producing ozone water by using tap water, so that the energy consumption is low, the electrolysis efficiency is not influenced by air quality, drying is not needed, and nitrogen oxide NOx is not generated; the corrosion is avoided, and the problem that the electrolytic catalyst coating falls off is solved; when the electrolytic tank is used, the conductivity of water is obviously increased from 0.0891S/cm to 0.2280S/cm, the proton conductivity is increased by 220%, the electrolytic tank can work for a long time, the electrolytic efficiency is stable, and no oxygen-containing electrolyte is required to be additionally added; generating 28% high-purity ozone and 72% oxygen without any other by-products; no hot spot damage risk, strengthening unique structural design, far exceeding the common PEM electrolytic ozone device; the service life of the membrane electrode can continuously work for more than 3 years.
Example 2
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1500 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon substrate to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 6Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps:
in the step (2), the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps: and mixing the graphite phase and the perfluorinated sulfonic acid resin according to the weight ratio of 4:1, heating, and performing extrusion molding to form a film, thereby obtaining the cation exchange membrane 2.
In the step (2), the graphite phase and the perfluorinated sulfonic acid resin are mixed and heated to 200 ℃ for extrusion molding to form a film.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying at the temperature of 400 ℃ for 8 hours after stirring, refluxing and rotary steaming, grinding to the particle size of less than 50nm, and treating at the temperature of 1000 ℃ for interaction.
The nonmetallic heteroatom is oxygen, and the platinum compound is Pt (OH)2。
In the embodiment, the graphite phase C3N4/PFSA solid electrolyte composite membrane is used as the cathode, the electrical conductivity of the membrane electrode is significantly increased, and the proton conductivity is increased by 220%, presumably because the acid-base conjugated ion pair is formed by the abundant base group on the graphite phase C3N4 and the sulfonate on the PFSA, and the proton selectivity and the proton transmission speed are increased. This example is capable of producing 29% high purity ozone and 71% oxygen.
Example 3
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a porous ceramic-based solid polymer electrolyte membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1300 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon substrate to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 5Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a porous ceramic-based solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps:
a1, preparation of the ceramic-based sulfonated polyimide material: taking 2.8 parts of diphenyl ether tetracarboxylic dianhydride monoatomic dispersion platinum carbon, 0.8 part of diacetyl amide and 2.8 parts of malonaldehyde according to parts by weight to obtain sulfonated polyimide;
a2, adding sulfonated polyimide into propylene glycol to prepare a sulfonated polyimide solution, wherein the weight ratio of the sulfonated polyimide to the propylene glycol is (7.5): 0.28, pressurizing the porous nickel-iron ceramic plate for carrying out infiltration reaction to prepare the ceramic matrix composite heterogeneous membrane;
a3, soaking the ceramic matrix composite heterogeneous membrane obtained in the step A2 in a hydrochloric acid solution to obtain the cation exchange membrane 2.
In the step A2, the pressure for the infiltration reaction is 18Mpa on the porous nickel-iron ceramic plate.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying at 380 ℃ for 9 hours after stirring, refluxing and rotary evaporation, grinding to below 50nm, and treating and interacting at 950 ℃.
The non-metal heteroatom is sulfur, and the platinum compound is PtS.
This example was able to generate 27% high purity ozone and 73% oxygen.
Example 4
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a porous ceramic-based solid polymer electrolyte membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1700 ℃, and combining the hydrogen atoms and the active free radicals with the carbon matrix to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 7Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a porous ceramic-based solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps:
a1, preparation of the ceramic-based sulfonated polyimide material: according to the parts by weight, 3.2 parts of diphenyl ether tetracarboxylic dianhydride monoatomic dispersion platinum carbon, 1.2 parts of diacetyl amide and 3.2 parts of malonaldehyde are taken to obtain sulfonated polyimide;
a2, adding sulfonated polyimide into propylene glycol to prepare a sulfonated polyimide solution, wherein the weight ratio of the sulfonated polyimide to the propylene glycol is (8.5): 0.32, pressurizing the porous nickel-iron ceramic plate for carrying out infiltration reaction to prepare the ceramic matrix composite heterogeneous membrane;
a3, soaking the ceramic matrix composite heterogeneous membrane obtained in the step A2 in a hydrochloric acid solution to obtain the cation exchange membrane 2.
In the step A2, the pressure for the infiltration reaction is 22MPa on the porous nickel-iron ceramic plate.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying for 7 hours at the temperature of 420 ℃ after stirring, refluxing and rotary steaming, grinding to the particle size of less than 50nm, and treating and interacting at the temperature of 1050 ℃ to obtain the cathode catalytic material.
The nonmetal heteroatom is silicon, and the platinum compound is PtS2。
This example is capable of generating 26% high purity ozone and 74% oxygen.
Example 5
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1500 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon substrate to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 6Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps: and mixing the graphite phase and the perfluorinated sulfonic acid resin according to the weight ratio of 3.8:0.9, heating, and performing extrusion molding to form a film, thereby obtaining the cation exchange membrane 2.
In the step (2), the graphite phase and the perfluorinated sulfonic acid resin are mixed and heated to 190 ℃ for extrusion molding to form the film.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying at the temperature of 400 ℃ for 8 hours after stirring, refluxing and rotary steaming, grinding to the particle size of less than 50nm, and treating at the temperature of 1000 ℃ for interaction.
The nonmetal heteroatom is fluorine, and the platinum compound is PtCl4。
This example is capable of generating 28% high purity ozone and 72% oxygen.
Example 6
A membrane electrode for producing ozone water by using tap water comprises an ion exchange membrane 2, an anode catalyst layer 1 arranged on one side of the ion exchange membrane 2 and a cathode catalyst layer 3 arranged on the other side of the ion exchange membrane 2, wherein the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane.
The anode catalyst layer 1 is made of a boron-carbon diamond heterojunction material, and the cathode catalyst layer 3 is made of a graphene composite material.
A method for preparing the membrane electrode as described above, comprising the steps of:
(1) preparing an anode catalyst layer 1 by adopting a boron-carbon diamond heterojunction material;
(2) preparing a cation exchange membrane 2;
(3) preparing a cathode catalyst layer 3;
(4) pressing the anode catalyst layer 1, the cation exchange membrane 2 and the cathode catalyst layer 3 to prepare a membrane electrode;
wherein, the steps (1) to (3) can be carried out simultaneously or the sequence can be changed.
In the step (1), the preparation method of the anode catalyst layer 1 includes the steps of: decomposing carbon gas and radon gas into carbon and hydrogen atoms and active free radicals at 1500 ℃, wherein the hydrogen atoms and the active free radicals are combined with the carbon substrate to form a carbide transition layer; depositing diamond crystal nucleus on the carbide transition layer by carbon atoms; the formed diamond crystal nucleus grows into a diamond micro product under the pressure of 6Gpa, and then grows into a diamond film. The proper pressure in the growth stage can increase the growth speed of the film and improve the quality of the film.
In the step (2), the cation exchange membrane 2 is a graphite phase C3N4/PFSA solid electrolyte composite membrane, and the preparation method of the cation exchange membrane 2 comprises the following steps: and mixing the graphite phase and the perfluorinated sulfonic acid resin according to the weight ratio of 4.2:1.1, heating, and performing extrusion molding to form a film, thereby obtaining the cation exchange membrane 2.
In the step (2), the graphite phase and the perfluorinated sulfonic acid resin are mixed and heated to 210 ℃ for extrusion molding to form a film.
In the step (3), the preparation method of the cathode catalytic material used for preparing the cathode catalyst layer 3 includes the following steps: the cathode catalytic material is prepared by taking a carbon carrier, a non-metal heteroatom reagent and a platinum compound as raw materials, drying at the temperature of 400 ℃ for 8 hours after stirring, refluxing and rotary steaming, grinding to the particle size of less than 50nm, and treating at the temperature of 1000 ℃ for interaction.
The non-metal heteroatom is chlorine, and the platinum compound is PtCl2。
This example was able to generate 27% high purity ozone and 73% oxygen.
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention, and not for limiting the protection scope of the present invention, although the present invention is described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions can be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention.
Claims (10)
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