Three-phase gas diffusion electrode, hydrogen peroxide generating device and application
By using a three-phase gas diffusion electrode and a hydrogen peroxide generator in the washing machine, hydrogen peroxide is generated to replace or reduce detergents, the problem of environmental pollution of existing washing machines is solved and a low-carbon and environmentally friendly clothing cleaning effect is achieved.
Patent Information
- Application Number
- CN202410993036.8
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Priority Date
- 2023-08-17
- Filing Date
- 2024-07-23
- Publication Date
- 2025-02-21
- Estimated Expiration
- Not applicable · inactive patent
AI Technical Summary
The fabric washing method of existing washing machines relies on the frequent addition of detergents, which leads to inconvenience of users and causes pollution to the environment.
A three-phase gas diffusion electrode and hydrogen peroxide generator are used to generate hydrogen peroxide in the electrolyte through the electrode to replace or reduce the use of detergents.
Without using or reducing detergents, efficient cleaning of clothes can be achieved, environmental pollution can be reduced, and the requirements of low-carbon and environmental protection can be met.
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Figure CN119491251A_ABST
Abstract
Description
Technical Field
[0001] The present disclosure relates to the technical field of clothing cleaning, and in particular to a three-phase gas diffusion electrode, a hydrogen peroxide generating device and applications. Background Art
[0002] The current method of washing fabrics in washing machines is still to add detergent and wash with the washing machine program. This method is widely used, but frequent addition of detergent brings inconvenience to users. At the same time, with the development of low-carbon and environmentally friendly lifestyles, the discharge of wastewater containing detergents will cause harm to the environment.
[0003] As an important oxidant, bleaching agent, and disinfectant, hydrogen peroxide has important applications in water treatment, textiles, sanitary food, and other fields. Therefore, introducing hydrogen peroxide into the washing process of fabrics will reduce or even replace the use of detergents. At the same time, as a green molecule, hydrogen peroxide decomposes into oxygen and water, which will not pollute the environment. Summary of the invention
[0004] In order to solve the above technical problems, the present disclosure provides a three-phase gas diffusion electrode, a hydrogen peroxide generating device and applications.
[0005] In a first aspect, the present disclosure provides a three-phase gas diffusion electrode, the three-phase gas diffusion electrode comprising a gas diffusion layer, an intermediate layer and a catalyst layer;
[0006] Wherein, the gas diffusion layer and the catalyst layer are both conductive carbon-based material layers.
[0007] As a preferred technical solution of the present disclosure, the gas diffusion layer comprises a carbon material, and preferably the carbon material is carbon black.
[0008] As a preferred technical solution of the present disclosure, the components of the catalytic layer include carbon material, and preferably the carbon material is carbon black or doped carbon material.
[0009] As a preferred technical solution of the present disclosure, the doping element of the doped carbon material is selected from any one of N, Pt, Co or Ru, or a combination of at least two of them.
[0010] As a preferred technical solution of the present disclosure, in the doped carbon material, the doping amount of the doping element is 0.1-10wt%.
[0011] As a preferred technical solution of the present disclosure, the thickness of the gas diffusion layer and the catalyst layer are independently selected from 0.2-5 mm.
[0012] As a preferred technical solution of the present disclosure, the thickness of the intermediate layer is 0.1-3 mm.
[0013] As a preferred technical solution of the present disclosure, the porosity of the three-phase gas diffusion electrode is 72.1-90%.
[0014] As a preferred technical solution of the present disclosure, the intermediate layer is selected from any one of a metal platinum mesh, a metal nickel mesh or a stainless steel mesh, or a combination of at least two of them.
[0015] In a second aspect, the present disclosure provides a method for preparing the three-phase gas diffusion electrode according to the first aspect, the preparation method comprising the following steps:
[0016] preparing a slurry of a gas diffusion layer and pressing the slurry to obtain the gas diffusion layer;
[0017] Preparing a slurry of a catalyst layer and pressing it to obtain the catalyst layer;
[0018] The gas catalyst layer, the intermediate layer and the catalytic layer are stacked, pressed and sintered to obtain the three-phase gas diffusion electrode.
[0019] As a preferred technical solution of the present disclosure, the components of the slurry of the gas diffusion layer and the slurry of the catalyst layer independently include carbon material and a binder.
[0020] As a preferred technical solution of the present disclosure, in the slurry of the gas diffusion layer, the mass ratio of the carbon material to the binder is 7:3 to 4:6.
[0021] As a preferred technical solution of the present disclosure, in the slurry of the catalytic layer, the mass ratio of the carbon material to the binder is 7:3 to 4:6.
[0022] As a preferred technical solution of the present disclosure, the pressing pressure is independently selected from 10-30 MPa, preferably 20 MPa.
[0023] As a preferred technical solution of the present disclosure, the pressing time is independently selected from 1-3 minutes.
[0024] As a preferred technical solution of the present disclosure, the sintering temperature is 320-350°C, preferably 340°C.
[0025] As a preferred technical solution of the present disclosure, the sintering time is 1-3 hours, preferably 1 hour.
[0026] In a third aspect, the present disclosure provides a hydrogen peroxide generating device, wherein the hydrogen peroxide generating device comprises the three-phase gas diffusion electrode described in the first aspect.
[0027] As a preferred technical solution of the present disclosure, the cathode of the hydrogen peroxide generating device is the three-phase gas diffusion electrode described in the first aspect.
[0028] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes an anode, and the anode includes a metal base layer and a catalyst layer.
[0029] As a preferred technical solution of the present disclosure, the material of the metal base layer includes any one of titanium, nickel or platinum, or a combination of at least two of them.
[0030] As a preferred technical solution of the present disclosure, the catalyst layer is a transition metal coating, and the components of the transition metal coating are selected from any one of ruthenium, iridium, tantalum, palladium or their oxides, or a combination of at least two thereof.
[0031] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes a power supply, preferably a DC power supply, and the power supply is connected to the anode and the cathode.
[0032] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes an ion exchange layer disposed between the cathode and the anode.
[0033] In a fourth aspect, the present disclosure provides the use of the three-phase gas diffusion electrode described in the first aspect or the hydrogen peroxide generating device described in the third aspect in a washing device, a disinfecting device or a cleaning device, preferably in a laundry device, a dishwashing device or an air purification device.
[0034] In a fifth aspect, the present disclosure provides the use of the three-phase gas diffusion electrode described in the first aspect or the hydrogen peroxide generating device described in the third aspect in removing stains or odors, sterilizing and disinfecting, and color bleaching.
[0035] As a preferred technical solution of the present disclosure, the stains include protein stains and / or pigment stains.
[0036] Compared with the prior art, the technical solution provided by the embodiments of the present disclosure has the following advantages:
[0037] The hydrogen peroxide generating device provided by the present disclosure can be applied to devices such as clothing washing. When applied to clothing washing, clothing can be washed while reducing the use of detergent or even without using detergent, thereby enhancing the washing effect of fabrics, reducing the amount of detergent used, and achieving low-carbon and environmental protection. BRIEF DESCRIPTION OF THE DRAWINGS
[0038] The accompanying drawings, which are incorporated in and constitute a part of this specification, illustrate embodiments consistent with the present disclosure and, together with the description, serve to explain the principles of the present disclosure.
[0039] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings required for use in the embodiments or the description of the prior art will be briefly introduced below. Obviously, for ordinary technicians in this field, other drawings can be obtained based on these drawings without paying any creative labor.
[0040] Figure 1 It is a schematic structural diagram of the three-phase gas diffusion electrode according to an embodiment of the present disclosure;
[0041] Among them, 1-gas diffusion layer; 2-intermediate layer; 3-catalytic layer. DETAILED DESCRIPTION
[0042] In order to more clearly understand the above-mentioned objectives, features and advantages of the present disclosure, the scheme of the present disclosure will be further described below. It should be noted that the embodiments of the present disclosure and the features in the embodiments can be combined with each other without conflict.
[0043] In the following description, many specific details are set forth to facilitate a full understanding of the present disclosure, but the present disclosure may also be implemented in other ways different from those described herein; it is obvious that the embodiments in the specification are only part of the embodiments of the present disclosure, rather than all of the embodiments.
[0044] As for stain treatment of clothes, the current conventional method is to provide different kinds of detergents to remove the stains, but the large-scale use of detergents may cause problems such as environmental pollution.
[0045] The present disclosure provides a three-phase gas diffusion electrode, such as Figure 1 As shown, the three-phase gas diffusion electrode includes a gas diffusion layer 1, an intermediate layer 2 and a catalyst layer 3;
[0046] Wherein, the gas diffusion layer and the catalyst layer are both conductive carbon-based material layers.
[0047] The three-phase gas diffusion electrode provided by the present invention contacts air on one side and electrolyte on the other side. Oxygen molecules in the air pass through the electrode sheet and obtain electrons on the other side of the electrode sheet to produce hydrogen peroxide. The produced hydrogen peroxide can be used for disinfection, sterilization, clothing cleaning, etc.
[0048] As a preferred technical solution of the present disclosure, the gas diffusion layer comprises a carbon material, and preferably the carbon material is carbon black.
[0049] As a preferred technical solution of the present disclosure, the components of the catalytic layer include carbon material, and preferably the carbon material is carbon black or doped carbon material.
[0050] As a preferred technical solution of the present disclosure, the doping element of the doped carbon material is selected from any one of N, Pt, Co or Ru, or a combination of at least two of them.
[0051] As a preferred technical solution of the present disclosure, in the doped carbon material, the doping amount of the doping element is 0.1-10wt%, for example, 0.2wt%, 0.5wt%, 1wt%, 2wt%, 3wt%, 4wt%, 5wt%, 6wt%, 7wt%, 8wt%, 9wt% and the like.
[0052] In the present disclosure, the doped carbon material may be selected from conventional doped carbon materials in the art, and may also be prepared. The present disclosure does not impose too many limitations on this, and any doped carbon material that can achieve the purpose of the present disclosure may be applied to the present disclosure.
[0053] As a preferred technical solution of the present disclosure, the thickness of the gas diffusion layer and the catalyst layer are independently selected from 0.2-5 mm, for example, 0.5 mm, 1 mm, 1.5 mm, 2 mm, 2.5 mm, 3 mm, 3.5 mm, 4 mm, 4.5 mm, etc.
[0054] As a preferred technical solution of the present disclosure, the thickness of the intermediate layer is 0.1-3 mm, for example, 0.5 mm, 1 mm, 1.5 mm, 2 mm, 2.5 mm, etc.
[0055] As a preferred technical solution of the present disclosure, the porosity of the three-phase gas diffusion electrode is 72.1-90%, for example, 75%, 78%, 80%, 82%, 85%, 88%, etc.
[0056] When the porosity of the three-phase gas diffusion electrode is within the preferred range defined in the present disclosure, the electrode with a reasonable pore size distribution is conducive to the rapid transfer of oxygen in the air, thereby ensuring the production efficiency of hydrogen peroxide in subsequent applications.
[0057] In the three-phase gas diffusion electrode, in order to improve the conductivity, the intermediate layer (support layer or substrate layer) is selected from a metal mesh structure, and the conductive carbon-based material layers (gas diffusion layer and catalyst layer) are respectively pressed on both sides of the substrate layer to obtain the three-phase gas diffusion electrode.
[0058] As a preferred technical solution of the present disclosure, the intermediate layer is selected from any one of a metal platinum mesh, a metal nickel mesh or a stainless steel mesh, or a combination of at least two of them.
[0059] The density of the three-phase gas diffusion electrode provided by the present disclosure is 1-2 g / cm 3 The conductivity is above 300S / m. The excellent conductivity can ensure the ion exchange rate in the electrolyte, and then ensure the efficiency of hydrogen peroxide production in subsequent applications.
[0060] The contact angle between the three-phase gas diffusion electrode provided by the present invention and water is between 100-160°. Within this range, it can ensure that the electrolyte is in full contact with the electrode, providing sufficient reaction sites for the electrolysis reaction, thereby facilitating the smooth progress of the electrolysis process, and can also ensure that the gas passage works normally and is not submerged by the electrolyte.
[0061] The three-phase gas diffusion electrode provided by the present disclosure has a high efficiency in producing hydrogen peroxide, wherein when the current is maintained at 5A and the current density is 50mA / cm 2 The electrode was operated for 30 minutes. The hydrogen peroxide concentration was tested by the potassium titanium oxalate method, which was 3-4.85 g / L. The hydrogen peroxide yield was 1.32 g, and the current efficiency reached 88%. When the current was maintained at 2 A, the current density was 20 mA / cm 2 The electrode was run for 30 minutes, and the hydrogen peroxide concentration was tested by the potassium titanium oxalate method, which was 1.2-2.095 g / L, the hydrogen peroxide production was 0.61 g, and the current efficiency reached 97%.
[0062] The three-phase gas diffusion electrode provided by the present invention maintains a current of 5A and a current density of 50mA / cm 2 The electrode was run for more than 200 times under the condition of 30min operation, and it still had excellent application effect. The concentration of hydrogen peroxide was 2.85-4.61g / L.
[0063] In a second aspect, the present disclosure provides a method for preparing the three-phase gas diffusion electrode according to the first aspect, the preparation method comprising the following steps:
[0064] preparing a slurry of a gas diffusion layer and pressing the slurry to obtain the gas diffusion layer;
[0065] Preparing a slurry of a catalyst layer and pressing it to obtain the catalyst layer;
[0066] The gas catalyst layer, the intermediate layer and the catalytic layer are stacked, pressed and sintered to obtain the three-phase gas diffusion electrode.
[0067] As a preferred technical solution of the present disclosure, the components of the slurry of the gas diffusion layer and the slurry of the catalyst layer independently include carbon material and a binder.
[0068] As a preferred technical solution of the present disclosure, in the slurry of the gas diffusion layer, the mass ratio of the carbon material to the binder is 7:3 to 4:6, for example, 4.5:5.5, 5:5, 5.5:4.5, 6:4, 6.5:3.5, etc.
[0069] As a preferred technical solution of the present disclosure, in the slurry of the catalytic layer, the mass ratio of the carbon material to the binder is 7:3 to 4:6, for example, 4.5:5.5, 5:5, 5.5:4.5, 6:4, 6.5:3.5, etc.
[0070] In the gas diffusion layer and the catalyst layer described in the present disclosure, the binder will decompose during the sintering process, and the components of the gas diffusion layer and the catalyst layer finally obtained basically do not include solvents and binders.
[0071] As a preferred technical solution of the present disclosure, the pressing pressure is independently selected from 10-30 MPa, such as 12 MPa, 15 MPa, 18 MPa, 20 MPa, 22 MPa, 25 MPa, 28 MPa, etc., preferably 20 MPa.
[0072] As a preferred technical solution of the present disclosure, the pressing time is independently selected from 1-3 min, such as 1.5 min, 2 min, 2.5 min, etc.
[0073] As a preferred technical solution of the present disclosure, the sintering temperature is 320-350°C, for example, 325°C, 330°C, 335°C, 340°C, 345°C, etc., preferably 340°C.
[0074] As a preferred technical solution of the present disclosure, the sintering time is 1-3 hours, such as 1.5 hours, 2 hours, 2.5 hours, etc., preferably 1 hour.
[0075] As a specific embodiment of the present disclosure, the method for preparing the three-phase gas diffusion electrode comprises the following steps:
[0076] (1) preparing a slurry of a gas diffusion layer containing a carbon material and a binder, wherein the mass ratio of the carbon material to the binder is 7:3 to 4:6, and the slurry further contains a solvent, and the present disclosure does not specifically limit the solvent used;
[0077] (2) preparing a slurry of a catalyst layer containing a carbon material and a binder, wherein the mass ratio of the carbon material to the binder is 7:3 to 4:6, and the slurry also contains a solvent, and the present disclosure does not specifically limit the solvent used;
[0078] (3) pressing the slurry of the gas diffusion layer and the slurry of the catalyst layer at 10-30 MPa, preferably 20 MPa, for 1-3 min to obtain the gas diffusion layer sheet and the catalyst layer sheet;
[0079] (4) placing the gas diffusion layer and the catalyst layer on both sides of the intermediate layer (metal mesh structure), and continuing to press at 10-30 MPa, preferably 20 MPa for 1-3 minutes to obtain a sheet electrode;
[0080] (5) The sheet electrode is placed in a sintering device such as a muffle furnace and calcined at 320-350° C., preferably 340° C. for 1 hour to obtain the three-phase gas diffusion electrode.
[0081] In a third aspect, the present disclosure provides a hydrogen peroxide generating device, wherein the hydrogen peroxide generating device comprises the three-phase gas diffusion electrode described in the first aspect.
[0082] As a preferred technical solution of the present disclosure, the cathode of the hydrogen peroxide generating device is the three-phase gas diffusion electrode described in the first aspect.
[0083] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes an anode, and the anode includes a metal base layer and a catalyst layer.
[0084] The anode and cathode in the hydrogen peroxide generating device disclosed in the present invention can undergo oxidation-reduction reaction to continuously generate hydrogen peroxide.
[0085] In the present disclosure, the anode may be completely immersed in the electrolyte or may be in contact with the electrolyte on one side.
[0086] In the present disclosure, in order to be applicable to different overall structures and use environments, and at the same time, to ensure the working stability and safety of the anode, the material of the metal base layer is preferably a metal material with high stability and strong corrosion resistance.
[0087] As a preferred technical solution of the present disclosure, the material of the metal base layer includes any one of titanium, nickel or platinum, or a combination of at least two of them.
[0088] As a preferred technical solution of the present disclosure, the catalyst layer is a transition metal coating, and the components of the transition metal coating are selected from any one of ruthenium, iridium, tantalum, palladium or their oxides, or a combination of at least two thereof.
[0089] As a preferred technical solution of the present disclosure, the thickness of the anode is ≥0.5 mm, for example, 0.6 mm, 0.7 mm, 0.8 mm, 0.9 mm, 1.0 mm, etc.
[0090] In the hydrogen peroxide generating device provided by the present disclosure, the anode plate may be a flat plate structure, or a two-dimensional structure such as a mesh or porous structure.
[0091] The chemical reaction occurring at the anode is:
[0092] 2H2O→O2+4H + +4e -
[0093] The cathode is a three-phase gas diffusion electrode, which has an efficient gas molecule transmission channel and abundant hydrogen peroxide reaction sites. When used, the chemical reaction formula occurring at the cathode is:
[0094] O2+2H2O+4e - →2H2O2
[0095] In the present disclosure, the production rate of hydrogen peroxide on the cathode is 0-60 mg / min, such as 10 mg / min, 20 mg / min, 30 mg / min, 40 mg / min, 50 mg / min, etc., and the current efficiency is not less than 70%, which is sufficient to meet application requirements.
[0096] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes a power supply, preferably a DC power supply, and the power supply is connected to the anode and the cathode.
[0097] As a preferred technical solution of the present disclosure, the hydrogen peroxide generating device further includes an ion exchange layer disposed between the cathode and the anode.
[0098] In the hydrogen peroxide generating device disclosed in the present invention, the anode and cathode not only serve as electrolytic generating devices, but also as structural supporting devices. Therefore, in order to ensure safety, the hydrogen peroxide generating device preferably includes a supporting structure to prevent deformation of the electrodes. At the same time, the supporting device needs to ensure that the cathode can fully contact with the air and is not airtight.
[0099] In a fourth aspect, the present disclosure provides the use of the three-phase gas diffusion electrode described in the first aspect or the hydrogen peroxide generating device described in the third aspect in a washing device, a disinfecting device or a cleaning device, preferably in a laundry device, a dishwashing device or an air purification device.
[0100] In the present disclosure, when the hydrogen peroxide device is used, a water inlet pipeline can be set, and then an external or direct current power supply can be directly connected. The hydrogen peroxide generating device includes cathode and anode plates, as well as related support structures and sealing components.
[0101] In the present disclosure, the overall structure of the hydrogen peroxide generating device is small in volume, has no moving components, and is safe in structure, and hydrogen peroxide can be produced and used immediately.
[0102] In the present disclosure, when the hydrogen peroxide device is applied to a clothing washing device, a water inlet flow rate of 0-10 L / min (for example, 1 L / min, 2 L / min, 3 L / min, 4 L / min, 5 L / min, 6 L / min, 7 L / min, 8 L / min, 9 L / min, etc.) can be selected to match the water inlet program of the washing device.
[0103] In the present disclosure, when the electrolyte solution (water) completely fills the hydrogen peroxide generating device, the DC power supply can provide electron supply to the electrode sheet, and the current is preferably 0-10A, such as 1A, 2A, 3A, 4A, 5A, 6A, 7A, 8A, 9A, etc.
[0104] In a fifth aspect, the present disclosure provides the use of the three-phase gas diffusion electrode described in the first aspect or the hydrogen peroxide generating device described in the third aspect in removing stains or odors, sterilizing and disinfecting, and color bleaching.
[0105] As a preferred technical solution of the present disclosure, the stains include protein stains and / or pigment stains.
[0106] The hydrogen peroxide generated by the hydrogen peroxide generator provided by the present disclosure can be used to remove stains, especially some special stains, such as blood stains or pigments, and can be cleaned without adding any detergents, so as to achieve detergent-free washing. For other stains, such as oil stains, detergents can also be used to assist in washing, which can effectively reduce the amount of detergents used, reduce environmental pollution and carbon emissions.
[0107] As a preferred technical solution of the present disclosure, the peculiar smell includes smoke smell and / or hot pot smell, etc.
[0108] In the following description, many specific details are set forth to facilitate a full understanding of the present disclosure, but the present disclosure may also be implemented in other ways different from those described herein; it is obvious that the embodiments in the specification are only part of the embodiments of the present disclosure, rather than all of the embodiments.
[0109] Example 1
[0110] This embodiment provides a three-phase gas diffusion electrode, comprising a gas diffusion layer, an intermediate layer and a catalyst layer stacked in sequence, wherein:
[0111] The gas diffusion layer is composed of carbon black and has a layer thickness of 1 mm;
[0112] The middle layer is a metal nickel mesh with a thickness of 1 mm;
[0113] The catalyst layer consists of carbon black doped with N and has a layer thickness of 1 mm.
[0114] The preparation method is as follows:
[0115] (1) mixing carbon black, a binder PTFE, and a solvent anhydrous ethanol in a mass ratio of 1:1:100, and heating the ethanol to volatilize it to obtain a slurry of a gas diffusion layer;
[0116] (2) mixing carbon black, a binder PTFE, pyridine, and a solvent anhydrous ethanol in a mass ratio of 1:1:0.001:100, and heating the ethanol to volatilize it to obtain a slurry of a catalyst layer;
[0117] (3) pressing the slurry of the gas diffusion layer and the slurry of the catalyst layer at 20 MPa for 1 min respectively to obtain the gas diffusion layer sheet and the catalyst layer sheet;
[0118] (4) Placing the gas diffusion layer and the catalyst layer on both sides of the metal nickel mesh respectively, and continuing to press at 20 MPa for 1 min to obtain a sheet electrode;
[0119] (5) The sheet electrode is placed in a sintering device such as a muffle furnace and calcined at 340° C. for 1 hour, and then cooled naturally to obtain the three-phase gas diffusion electrode.
[0120] Example 2-3
[0121] This embodiment provides a three-phase gas diffusion electrode.
[0122] The difference from Example 1 is that in this example, the thickness of the gas diffusion layer is 0.2 mm (Example 2) or 5 mm (Example 3).
[0123] Embodiment 4-5
[0124] This embodiment provides a three-phase gas diffusion electrode.
[0125] The difference from Example 1 is that in this example, the thickness of the catalytic layer is 0.2 mm (Example 4) or 5 mm (Example 5).
[0126] Embodiment 6-7
[0127] This embodiment provides a three-phase gas diffusion electrode.
[0128] The difference from Example 1 is that in this example, in the slurry of the gas diffusion layer, the mass ratio of the carbon material to the binder is 7:3 (Example 6) and 4:6 (Example 7).
[0129] Embodiment 8-9
[0130] This embodiment provides a three-phase gas diffusion electrode.
[0131] The difference from Example 1 is that in this example, in the slurry of the catalytic layer, the mass ratio of the carbon material to the binder is 7:3 (Example 8) and 4:6 (Example 9).
[0132] Comparative Example 1
[0133] This comparative example provides an electrode.
[0134] The difference from Example 1 is that this comparative example provides a graphite felt hydrogen peroxide electrode (Shandong Mingsibei Special Materials Co., Ltd.).
[0135] Performance Testing
[0136] The electrodes provided in Examples 1-9 and Comparative Example 1 were subjected to performance tests in the following manner:
[0137] (1) Conductivity: Tested using the four-probe resistivity test method.
[0138] (2) Porosity: The test was conducted using the mercury intrusion method, where the test sample was 4×4 cm 2 .
[0139] (3) Contact angle: The hydrophilicity and hydrophobicity of the electrode were characterized using a contact angle meter. Distilled water was used as the test solution. The solution volume for each contact angle test was 4 μL. The contact angle was calculated based on the collected photos.
[0140] (4-1) Current efficiency (distance between cathode and anode 1 cm):
[0141] Electrode effective area: 10×10cm 2 , the distance between the anode and cathode of the electrode is 1 cm, 300 mL of circulating water, the pH is adjusted to 11, the circulating water is pumped into the electrode device using a circulating pump, the water flow rate is 100 mL / min, the power is turned on, the anode is a metal titanium electrode coated with ruthenium and iridium, and the cathode is a three-phase gas diffusion electrode provided in the embodiment;
[0142] When the current is maintained at 5A, the current density is 50mA / cm 2 , the electrode was operated for 30 min, the hydrogen peroxide concentration was tested by the potassium titanium oxalate method, and the current efficiency was calculated;
[0143] When the current is maintained at 2A, the current density is 20mA / cm 2 , the electrode was operated for 30 min, the hydrogen peroxide concentration was tested by the potassium titanium oxalate method, and the current efficiency was calculated;
[0144] Current efficiency = actual hydrogen peroxide concentration / theoretical hydrogen peroxide concentration;
[0145] Among them, when the current is maintained at 5A and the current density is 50mA / cm 2 , when the electrode is running for 30 min, the theoretical hydrogen peroxide concentration is 5.29 g / L;
[0146] When the current is maintained at 2A, the current density is 20mA / cm 2 When the electrode runs for 30 minutes, the theoretical hydrogen peroxide concentration is 2.12g / L.
[0147] (4-2) Current efficiency (distance between cathode and anode 3 mm):
[0148] Electrode effective area: 10×10cm 2 , the distance between the anode and cathode of the electrode is 1 cm, tap water is pumped into the electrode device using a peristaltic pump, the water flow rate is 100 mL / min, the power is turned on, the anode is a metal titanium electrode coated with ruthenium and iridium, and the cathode is a three-phase gas diffusion electrode provided in the embodiment;
[0149] When the current is maintained at 2A, the current density is 20mA / cm 2 , the electrode was operated for 30 min, the hydrogen peroxide concentration was tested by the potassium titanium oxalate method, and the current efficiency was calculated;
[0150] Current efficiency = actual hydrogen peroxide concentration / theoretical hydrogen peroxide concentration;
[0151] The theoretical hydrogen peroxide concentration is 0.21 g / L.
[0152] (5-1) Electrode life (distance between cathode and anode 1 cm):
[0153] According to the current efficiency test method (4-1), at a current density of 50 mA / cm 2 The test is run under the conditions of . The operation is continued until the current efficiency is lower than 80% of the initial current efficiency. The operation time is the electrode life.
[0154] (5-2) Electrode life (distance between cathode and anode: 3 mm):
[0155] According to the current efficiency test method (4-2), at a current density of 20 mA / cm 2 The test is run under the conditions of . The operation is continued until the current efficiency is lower than 80% of the initial current efficiency. The operation time is the electrode life.
[0156] The test results are shown in Table 1 and Table 2:
[0157] Table 1
[0158]
[0159] Table 2
[0160]
[0161]
[0162] Application Example 1
[0163] This application example provides a hydrogen peroxide generating device, wherein:
[0164] The cathode is a three-phase gas diffusion electrode provided in the embodiment;
[0165] The anode is a titanium plate with a transition metal catalyst coating.
[0166] It should be noted that, in this article, relational terms such as "first" and "second" are only used to distinguish one entity or operation from another entity or operation, and do not necessarily require or imply any such actual relationship or order between these entities or operations. Moreover, the terms "include", "comprise" or any other variants thereof are intended to cover non-exclusive inclusion, so that a process, method, article or device including a series of elements includes not only those elements, but also other elements not explicitly listed, or also includes elements inherent to such process, method, article or device. In the absence of further restrictions, the elements defined by the sentence "comprise a ..." do not exclude the existence of other identical elements in the process, method, article or device including the elements.
[0167] The above description is only a specific embodiment of the present disclosure, so that those skilled in the art can understand or implement the present disclosure. Various modifications to these embodiments will be apparent to those skilled in the art, and the general principles defined herein may be implemented in other embodiments without departing from the spirit or scope of the present disclosure. Therefore, the present disclosure will not be limited to the embodiments described herein, but will conform to the widest scope consistent with the principles and novel features disclosed herein.
Claims
1. A three-phase gas diffusion electrode, characterized in that: The three-phase gas diffusion electrode comprises a gas diffusion layer, an intermediate layer and a catalyst layer; Wherein, the gas diffusion layer and the catalyst layer are both conductive carbon-based material layers.
2. The three-phase gas diffusion electrode according to claim 1, characterized in that: The gas diffusion layer comprises a carbon material, and preferably the carbon material is carbon black.
3. The three-phase gas diffusion electrode according to claim 1 or 2, characterized in that: The catalyst layer comprises a carbon material, and preferably the carbon material is carbon black or a doped carbon material; Preferably, the doping element of the doped carbon material is selected from any one or a combination of at least two of N, Pt, Co or Ru; Preferably, in the doped carbon material, the doping amount of the doping element is 0.1-10 wt %.
4. The three-phase gas diffusion electrode according to any one of claims 1 to 3, characterized in that: The thickness of the gas diffusion layer and the catalyst layer are each independently selected from 0.2-5 mm; And / or, the thickness of the intermediate layer is 0.1-3 mm.
5. The three-phase gas diffusion electrode according to any one of claims 1 to 4, characterized in that: The porosity of the three-phase gas diffusion electrode is 72.1-90%.
6. The three-phase gas diffusion electrode according to any one of claims 1 to 5, characterized in that: The intermediate layer is selected from any one of a metal platinum mesh, a metal nickel mesh or a stainless steel mesh, or a combination of at least two of them.
7. The method for preparing a three-phase gas diffusion electrode according to any one of claims 1 to 6, characterized in that: The preparation method comprises the following steps: preparing a slurry of a gas diffusion layer and pressing the slurry to obtain the gas diffusion layer; Preparing a slurry of a catalyst layer and pressing it to obtain the catalyst layer; The gas catalyst layer, the intermediate layer and the catalytic layer are stacked, pressed and sintered to obtain the three-phase gas diffusion electrode.
8. The preparation method according to claim 7, characterized in that: The components of the slurry of the gas diffusion layer and the slurry of the catalyst layer independently include a carbon material and a binder; Preferably, in the slurry of the gas diffusion layer, the mass ratio of the carbon material to the binder is 7:3 to 4:6; Preferably, in the slurry of the catalytic layer, the mass ratio of the carbon material to the binder is 7:3 to 4:
6.
9. The preparation method according to claim 7 or 8, characterized in that: The pressing pressure is independently selected from 10-30 MPa, preferably 20 MPa; And / or, the sintering temperature is 320-350°C, preferably 340°C; And / or, the sintering time is 1-3 hours, preferably 1 hour.
10. A hydrogen peroxide generating device, characterized in that: The hydrogen peroxide generating device comprises a three-phase gas diffusion electrode as claimed in any one of claims 1 to 6; Preferably, the cathode of the hydrogen peroxide generating device is a three-phase gas diffusion electrode as claimed in any one of claims 1 to 6.
11. The hydrogen peroxide generating device according to claim 10, characterized in that: The hydrogen peroxide generating device further comprises an anode, wherein the anode comprises a metal substrate and a catalyst layer; Preferably, the material of the metal base layer includes any one of titanium, nickel or platinum, or a combination of at least two thereof; Preferably, the catalyst layer is a transition metal coating, and the components of the transition metal coating are selected from any one of ruthenium, iridium, tantalum, palladium or their oxides, or a combination of at least two thereof.
12. The hydrogen peroxide generating device according to claim 10 or 11, characterized in that: The hydrogen peroxide generating device further comprises a power supply, preferably a DC power supply, the power supply being connected to the anode and the cathode; And / or, the hydrogen peroxide generating device further comprises an ion exchange layer disposed between the cathode and the anode.
13. Use of the three-phase gas diffusion electrode according to any one of claims 1 to 6 or the hydrogen peroxide generating device according to any one of claims 10 to 12 in a washing device, a disinfecting device or a cleaning device, preferably in a laundry device, a dishwashing device or an air purification device.
14. Use of the three-phase gas diffusion electrode according to any one of claims 1 to 6 or the hydrogen peroxide generator according to any one of claims 10 to 12 in removing stains or odors, sterilizing and disinfecting, and color bleaching; Preferably, the stains include protein stains and / or pigment stains.
Citation Information
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