CN117431566A - Catalyst for producing hydrogen by water electrolysis, preparation method thereof and water electrolysis hydrogen production tank - Google Patents
Catalyst for producing hydrogen by water electrolysis, preparation method thereof and water electrolysis hydrogen production tank Download PDFInfo
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- CN117431566A CN117431566A CN202210816554.3A CN202210816554A CN117431566A CN 117431566 A CN117431566 A CN 117431566A CN 202210816554 A CN202210816554 A CN 202210816554A CN 117431566 A CN117431566 A CN 117431566A
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- hydrogen
- water
- conductive diamond
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- 239000003054 catalyst Substances 0.000 title claims abstract description 53
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 239000001257 hydrogen Substances 0.000 title claims abstract description 47
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 47
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 37
- 238000005868 electrolysis reaction Methods 0.000 title claims abstract description 30
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 29
- 238000002360 preparation method Methods 0.000 title abstract description 13
- 239000000758 substrate Substances 0.000 claims abstract description 78
- 239000010432 diamond Substances 0.000 claims abstract description 46
- 229910003460 diamond Inorganic materials 0.000 claims abstract description 33
- 239000000463 material Substances 0.000 claims abstract description 25
- 239000002245 particle Substances 0.000 claims abstract description 23
- 238000000034 method Methods 0.000 claims abstract description 16
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 15
- 229910052721 tungsten Inorganic materials 0.000 claims abstract description 14
- 238000000137 annealing Methods 0.000 claims abstract description 11
- 229910021477 seaborgium Inorganic materials 0.000 claims abstract description 10
- 239000000126 substance Substances 0.000 claims abstract description 7
- 238000005229 chemical vapour deposition Methods 0.000 claims abstract description 6
- 150000001247 metal acetylides Chemical class 0.000 claims abstract description 4
- 230000000149 penetrating effect Effects 0.000 claims description 2
- 239000011651 chromium Substances 0.000 description 19
- 239000012528 membrane Substances 0.000 description 10
- 229910039444 MoC Inorganic materials 0.000 description 7
- UORVGPXVDQYIDP-UHFFFAOYSA-N borane Chemical compound B UORVGPXVDQYIDP-UHFFFAOYSA-N 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 229910052750 molybdenum Inorganic materials 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- QIJNJJZPYXGIQM-UHFFFAOYSA-N 1lambda4,2lambda4-dimolybdacyclopropa-1,2,3-triene Chemical compound [Mo]=C=[Mo] QIJNJJZPYXGIQM-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 239000013543 active substance Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 229910000085 borane Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000004050 hot filament vapor deposition Methods 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229910001260 Pt alloy Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- DSVGQVZAZSZEEX-UHFFFAOYSA-N [C].[Pt] Chemical compound [C].[Pt] DSVGQVZAZSZEEX-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- UFGZSIPAQKLCGR-UHFFFAOYSA-N chromium carbide Chemical compound [Cr]#C[Cr]C#[Cr] UFGZSIPAQKLCGR-UHFFFAOYSA-N 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 229910003470 tongbaite Inorganic materials 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
-
- 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
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- 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
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/054—Electrodes comprising electrocatalysts supported on a carrier
-
- 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
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
Landscapes
- 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)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
Abstract
The invention provides a preparation method of a catalyst for hydrogen production by water electrolysis, which is characterized by comprising the following steps of: s1: providing a substrate, and assembling conductive diamond particles on the surface of the substrate by a chemical vapor deposition method to obtain nano blue diamond particles; s2: annealing the nano blue diamond particles to form cracks, wherein the cracks penetrate through the conductive diamond layer to expose the substrate locally, so as to obtain a catalyst; wherein the material of the substrate is one or more of simple substances and/or carbides of Cr, mo, W and Sg.
Description
Technical Field
The invention relates to the field of materials for producing hydrogen by water electrolysis, in particular to a hydrogen production catalyst material of a proton exchange membrane electrolytic cell.
Background
Hydrogen energy is the clean energy source with the most development potential, and simultaneously, the hydrogen energy society is also the strategic development direction for realizing energy safety in China. The proton exchange membrane electrolytic tank (Proton Exchange Membrane Water Electrolyzer) is an electrolytic water device for efficiently producing hydrogen, and is an important tool for realizing green hydrogen production in a hydrogen energy society. The characteristics of quick start response, low working temperature and capability of modular pile installation are considered as the earliest commercialized device for producing hydrogen by water electrolysis.
The energy conversion component of the proton exchange membrane electrolyzer is a membrane electrode assembly (Membrane Electrode Assembly), wherein the core energy conversion material is a catalyst material that reduces the activation energy of water that is respectively oxidized and reduced at both poles. The existing cathode hydrogen evolution catalyst close to large-scale commercialization is a catalyst composed of nano platinum or platinum alloy active substances supported by a carbon-based carrier, has extremely fast electrocatalytic activity on water reduction hydrogen evolution (Hydrogen Evolution Reaction) of a cathode, and has the following defects: the carbon-based carrier carrying the active substances has poor chemical corrosion resistance, the platinum noble metal is very rare, the durability of other transition metal-based catalysts is insufficient under the acidic condition, and the iridium and ruthenium catalysts for water oxidation oxygen evolution (Oxygen Evolution Reaction) used for the membrane electrode anode are more rare, so that the cost of the whole membrane electrode assembly is very high, and large-scale commercialization is seriously hindered.
Disclosure of Invention
Based on the above-mentioned problems, there is a need to provide a catalyst for water electrolysis for hydrogen production by proton exchange membrane without noble metal, a method for preparing the same, and a water electrolysis hydrogen production tank using the catalyst for water electrolysis for hydrogen production by proton exchange membrane.
A method for preparing a catalyst for producing hydrogen by electrolyzing water, comprising the following steps:
S1：
providing a substrate, and assembling conductive diamond particles on the surface of the substrate by a chemical vapor deposition method to obtain nano blue diamond particles;
S2：
annealing the nano blue diamond particles to form cracks, wherein the cracks penetrate through the conductive diamond layer to be formed on the substrate and expose part of the substrate, so that a catalyst is obtained;
wherein the material of the substrate is one or more of simple substances and/or carbides of Cr, mo, W and Sg.
In one embodiment, the temperature of the annealing process is 100-800 ℃.
A catalyst for hydrogen production by water electrolysis, which is prepared by the preparation method of the catalyst for hydrogen production by water electrolysis.
A catalyst for producing hydrogen by electrolysis of water comprises a substrate and a conductive diamond particle layer formed on the surface of the substrate, wherein the conductive diamond layer is arranged to form a structure which enables the substrate to be locally exposed on the surface of the substrate.
In one embodiment, the catalyst is formed with fissures through the conductive diamond layer, and the fissures are formed on the substrate through the conductive diamond layer, leaving the substrate partially exposed.
A water electrolysis hydrogen production cell comprising an anode and a cathode, the catalyst layer of the anode and/or cathode using the catalyst of any one of the above.
The catalyst preparation method of the invention utilizes the difference of thermal expansion coefficients of the conductive diamond and the substrate material to form cracks on the nano blue diamond particles through annealing, and provides a catalyst, wherein the structure is that a conductive diamond layer is arranged to enable the substrate to be formed on the surface of the substrate in a locally exposed structure, the structure can be obtained through the preparation method or can be prepared through other preparation methods, and the catalyst has the beneficial effects that:
1. the specific surface area of the conductive diamond layer increases.
2. The catalyst taking the simple substance or carbide of the VI B group element Cr, mo, W, sg as a substrate has hydrogen evolution property, and hydrogen is rapidly separated out under lower overpotential by locally exposing the substrate.
Drawings
In order to more clearly illustrate the embodiments of the invention or the technical solutions of the prior art, the drawings which are used in the description of the embodiments or the prior art will be briefly described, it being obvious that the drawings in the description below are only some embodiments of the invention, and that other drawings can be obtained from these drawings without inventive faculty for a person skilled in the art.
FIG. 1 is a flow chart of a method for preparing a catalyst for hydrogen production by water electrolysis in accordance with an embodiment of the present invention.
Fig. 2 is a schematic structural view of a catalyst for hydrogen production by water electrolysis according to an embodiment of the present invention.
Fig. 3 is a diagram of a method of preparing a catalyst for hydrogen production by electrolysis of water in accordance with an embodiment of the present invention.
FIG. 4 is a SEM image of a catalyst for hydrogen production by electrolysis of water according to an embodiment of the present invention.
FIG. 5 is a graph showing the hydrogen evolution effect of a water electrolysis hydrogen production catalyst according to an embodiment of the present invention in comparison with a platinum carbon catalyst.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The invention provides a catalyst for hydrogen production by water electrolysis, which is prepared by a preparation method of the catalyst for hydrogen production by water electrolysis, and comprises the following steps:
step S1:
providing a substrate, and assembling conductive diamond particles on the surface of the substrate by a chemical vapor deposition method to obtain the nano blue diamond particles.
Wherein the substrate is made of Cr (chromium), mo (molybdenum), W (tungsten) and Sg%) And/or one or more of the elements and/or carbides of (a) and (b).
For example, the material of the substrate is one or more of simple substances of Cr, mo, W and Sg. For example, the material of the substrate is Cr, for example, the material of the substrate is Mo, for example, the material of the substrate is W, for example, the material of the substrate is Sg, for example, the material of the substrate is Cr and Mo, for example, the material of the substrate is Cr and W, for example, the material of the substrate is Cr and Sg, for example, the material of the substrate is Mo and Sg, for example, the material of the substrate is W and Sg, for example, the material of the substrate is Cr, mo and W, for example, the material of the substrate is Cr, W and Sg, for example, the material of the substrate is Mo, W and Sg, for example, the material of the substrate is Cr, mo, W and Sg.
For example, the substrate is made of Cr 3 C 2 (chromium carbide), moC (molybdenum carbide), WC (tungsten carbide). For example, the material of the substrate is Cr 3 C 2 For example, the substrate is MoC, for example, WC, for example, cr 3 C 2 And MoC, for example, the substrate is made of Cr 3 C 2 And WC, for example, the substrate is made of MoC and WC, for example, the substrate is made of Cr 3 C 2 MoC and WC.
For example, the substrate may also be made of one or more of the elements Cr, mo, W, sg and Cr 3 C 2 A mixture of one or more of MoC, WC. In this embodiment, descriptions are not unnecessarily omitted.
In one embodiment, in the step S1, the conductive diamond particles are assembled on the surface of the substrate by a hot wire chemical vapor deposition method, wherein parameters of the hot wire chemical vapor deposition method are that the temperature of a base station is 500-800 ℃, the temperature of a hot wire is 180-2400 ℃, the air pressure is 1-5kPa, 100-1000sccm of hydrogen gas is introduced, 1-20sccm of methane and 1-20sccm of borane are introduced, and the substrate is grown for more than 10 minutes.
In one embodiment, in the step S1, the conductive diamond particles are assembled on the surface of the substrate by a microwave plasma chemical vapor deposition method, and parameters of the microwave plasma chemical vapor deposition method are as follows: the microwave power is 500-3000W, the hydrogen is 100-1000sccm, the methane is 1-20sccm, the borane is 1-10sccm, the temperature of the base station is 500-700 ℃, the air pressure is 4-6kPa, and the growth time is 3-10h.
Step S2:
and annealing the nano blue diamond particles to form cracks, wherein the cracks penetrate through the conductive diamond layer to expose part of the substrate, so as to obtain the catalyst.
In a preferred embodiment, in step S2, the formed fissures extend through the conductive diamond layer and then onto the substrate to expose the substrate locally.
The conductive diamond layer formed by the invention wraps the nano blue diamond particles of the substrate, and the particle size is 10-1000 mu m.
By utilizing the difference of the thermal expansion coefficients of the conductive diamond and the substrate material, cracks are formed on the nano blue diamond particles through an annealing process, and extend inwards from the surface of the nano blue diamond particles, namely, the cracks penetrate through the conductive diamond layer and extend towards the substrate, so that the substrate is locally exposed to the outside.
In one embodiment, in step S2 of the present invention, the temperature of the annealing treatment is 100-800 ℃. Further, the annealing treatment may be multiple times.
The invention provides a catalyst for hydrogen production by water electrolysis, which comprises a substrate and a conductive diamond particle layer formed on the surface of the substrate, wherein the conductive diamond layer is arranged to form a structure with the substrate partially exposed on the surface of the substrate.
The catalyst can be prepared by the preparation method of the invention, and the catalyst prepared by the preparation method is formed with cracks penetrating through the conductive diamond layer, preferably, the cracks penetrate through the conductive diamond layer to be formed on the substrate, so that the substrate is partially exposed to the outside, and in the embodiment, the description is not unnecessarily repeated.
The catalyst preparation method provided by the invention utilizes the difference of thermal expansion coefficients of the conductive diamond and the substrate material to form cracks on the nano blue diamond particles through annealing, preferably, the cracks penetrate through the conductive diamond layer to form on the substrate, or provides a catalyst, wherein the structure is that the conductive diamond layer is arranged to enable the substrate to be formed on the surface of the substrate in a locally exposed structure, the structure can be obtained through the preparation method and can also be prepared through other preparation methods, and the catalyst has the beneficial effects that:
1. the specific surface area of the conductive diamond layer increases.
2. The catalyst taking the simple substance or carbide of the VI B group element Cr, mo, W, sg as a substrate has hydrogen evolution property, and hydrogen is rapidly separated out under lower overpotential by locally exposing the substrate.
A water electrolysis hydrogen production tank comprising an anode and a cathode, wherein the catalyst layer of the anode and/or the cathode uses the catalyst.
The technical features of the above-described embodiments may be arbitrarily combined, and all possible combinations of the technical features in the above-described embodiments are not described for brevity of description, however, as long as there is no contradiction between the combinations of the technical features, they should be considered as the scope of the description.
The above examples illustrate only a few embodiments of the invention, which are described in detail and are not to be construed as limiting the scope of the invention. It should be noted that it will be apparent to those skilled in the art that several variations and modifications can be made without departing from the spirit of the invention, which are all within the scope of the invention. Accordingly, the scope of protection of the present invention is to be determined by the appended claims.
Claims (7)
1. A method for preparing a catalyst for producing hydrogen by electrolyzing water, which is characterized by comprising the following steps:
S1：
providing a substrate, and assembling conductive diamond particles on the surface of the substrate by a chemical vapor deposition method to obtain nano blue diamond particles;
S2：
annealing the nano blue diamond particles to form cracks, wherein the cracks penetrate through the conductive diamond layer to expose the substrate locally, so that the catalyst is obtained;
wherein the material of the substrate is one or more of simple substances and/or carbides of Cr, mo, W and Sg.
2. The method for preparing a catalyst for hydrogen production by water electrolysis according to claim 1, wherein in the step S2, the formed slit extends to the substrate to partially expose the substrate after penetrating the conductive diamond layer.
3. The method for producing a catalyst for hydrogen production by electrolysis of water according to claim 1, wherein the temperature of the annealing treatment is 100 to 800 ℃.
4. A catalyst for the production of hydrogen by electrolysis of water, characterized by being produced by the method for producing a catalyst for the production of hydrogen by electrolysis of water according to any one of claims 1 to 3.
5. A catalyst for hydrogen production by electrolysis of water, comprising a substrate and a layer of conductive diamond particles formed on the surface of the substrate, the conductive diamond layer being arranged such that structures which leave the substrate partially exposed are formed on the surface of the substrate.
6. The catalyst for the production of hydrogen by electrolysis of water of claim 5 wherein the catalyst is formed with fissures and the fissures are formed through the conductive diamond layer on the substrate leaving the substrate partially exposed.
7. A water electrolysis hydrogen production tank, characterized by comprising an anode and a cathode, wherein the catalyst layer of the anode and/or the cathode uses the catalyst of any one of claims 1 to 6.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210816554.3A CN117431566A (en) | 2022-07-12 | 2022-07-12 | Catalyst for producing hydrogen by water electrolysis, preparation method thereof and water electrolysis hydrogen production tank |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210816554.3A CN117431566A (en) | 2022-07-12 | 2022-07-12 | Catalyst for producing hydrogen by water electrolysis, preparation method thereof and water electrolysis hydrogen production tank |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN117431566A true CN117431566A (en) | 2024-01-23 |
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Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202210816554.3A Pending CN117431566A (en) | 2022-07-12 | 2022-07-12 | Catalyst for producing hydrogen by water electrolysis, preparation method thereof and water electrolysis hydrogen production tank |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN117431566A (en) |
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2022
- 2022-07-12 CN CN202210816554.3A patent/CN117431566A/en active Pending
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