Over-current electrochemical hydrogen peroxide generation device and application thereof

Abstract

The invention belongs to the technical field of electrochemistry, and particularly relates to an over-current type device for electrochemically generating hydrogen peroxide and application of the over-current type device. Comprising an electrolysis module, a power supply, a water pump, a water tank and an electric connection device, the electrolysis module comprises an electrolyte cavity with an opening in one side, and a first flow guide grid, a metal support, a cathode electrode, an insulation grid, an anode electrode and a second flow guide grid are arranged in the electrolyte cavity; a spacing baffle is arranged at the position, close to the opening, of the electrolyte cavity, a fixing clamping groove is formed in the spacing baffle, and the metal support and a connector of the anode electrode penetrate through the fixing clamping groove and then are connected with a power source through an electric connecting device. The device does not need a diaphragm, is simple in structure, is easy to operate, is controllable in cost, meets the use requirements of hydrogen peroxide solutions with different concentrations in different scenes, and can be conveniently integrated into various household appliance purification equipment.

Description

Technical Field

[0001] This invention belongs to the field of electrochemical technology, specifically relating to a device for generating hydrogen peroxide by flow electrochemistry and its application. Background Technology

[0002] Hydrogen peroxide (H2O2) is a naturally occurring chemical substance found in water and air. It possesses strong oxidizing properties, with water and oxygen as its only reaction byproducts. It is an environmentally friendly green oxidant widely used in medical disinfection, fine chemicals, wastewater treatment, pulp bleaching, cleaning, and etching. Industrial production of hydrogen peroxide primarily relies on the cumbersome anthraquinone cycle process, requiring large-scale, energy-intensive equipment. Furthermore, the photodegradability of hydrogen peroxide solutions increases the cost and risk associated with its storage and transportation. Electrochemical preparation of hydrogen peroxide enables "on-demand" production of hydrogen peroxide, meeting the needs for different concentrations of hydrogen peroxide solution in various scenarios. However, traditional electrochemical devices are limited by low catalyst efficiency, poor equipment stability, high reactor design requirements, and difficulties in large-scale application. Summary of the Invention

[0003] The purpose of this invention is to provide a small, diaphragm-free, highly efficient, energy-saving, stable, simple, easy-to-operate, cost-controllable, small-scale, dispersed, flow-through electrochemical hydrogen peroxide generation device and its applications. This device uses tap water or natural water as the electrolyte. When the electrolyte flows through the electrochemical reaction device, a two-electron oxygen reduction reaction generates hydrogen peroxide at the cathode. The generated hydrogen peroxide is then thoroughly mixed in the electrolyte through the reactor, forming a hydrogen peroxide solution rich in micro-nano bubbles, achieving "on-demand production" of hydrogen peroxide. This modular electrolysis device can be used independently or integrated into household air purification equipment. The electrode reaction area can be adjusted according to usage requirements to improve the hydrogen peroxide synthesis efficiency, thereby meeting the needs for different concentrations of hydrogen peroxide solution in different scenarios.

[0004] Specifically, the present invention provides the following technical solution: An apparatus for generating hydrogen peroxide by flow electrochemistry includes an electrolysis module (1), a power supply (2), a water pump (3), a water tank (4), and an electrical connection device (5). The electrolysis module (1) includes an electrolyte chamber with an opening on one side. The electrolyte chamber is provided with a first flow guide grid (121), a metal support (13), a cathode electrode (14), an insulating grid (15), an anode electrode (16), and a second flow guide grid (122) from bottom to top. The electrolyte chamber is provided with a spacer baffle for sealing the electrolyte chamber near the opening. The spacer baffle is provided with a lower fixing slot (113) and an upper fixing slot (114). The connector of the metal bracket (13) passes through the lower fixing slot (113) and is connected to the negative terminal of the power supply (2) through an electrical connection device (5). The connector of the anode electrode (16) passes through the upper fixing slot (114) and is connected to the positive terminal of the power supply (2) through another electrical connection device (5).

[0005] Preferably, the anode electrode (16) comprises a titanium substrate, and a catalytic layer with a thickness of 2-5 μm is disposed on the surface of the titanium substrate; The titanium substrate is a titanium mesh, a porous titanium plate, or a sintered titanium felt; the catalyst layer comprises one or more metal oxides selected from the oxides of platinum, ruthenium, iridium, palladium, titanium, and cobalt.

[0006] Preferably, the method for preparing the anode electrode (16) includes the following steps: A) Prepare an ethanol solution of the metal salt; B) The ethanol solution of the metal salt is uniformly coated onto the titanium substrate, then dried, transferred to a muffle furnace for calcination, and the coating-drying-calcination process is repeated 10-30 times to obtain the final product.

[0007] Preferably, in step B), the ethanol solution of the metal salt is applied in batches of 1m each time. 2 The coating amount on the substrate is 4-8 mL; And / or, in step B), the drying temperature is 80-150℃ and the time is 5-20 min; the calcination temperature is 300-500℃ and the time is 1-3 hours.

[0008] Preferably, the cathode electrode (14) includes a carbon substrate, and an active layer is disposed on the surface of the carbon substrate; The carbon substrate is PAN-based carbon fiber felt, porous graphite plate, graphite carbon felt, or activated carbon felt (all carbon materials with a three-dimensional porous structure); the active layer comprises one or more active substances selected from graphite, polytetrafluoroethylene, and carbon powder with high specific surface area (such as Cabot XC-72R, BP2000, Ketjen Black ECP, etc.), and the loading of the active substance is 1-4 mg / cm³. 2 .

[0009] Preferably, an opening is provided at one corner of the first guide grille (121) and the second guide grille (122); The opening of the first flow guide grille (121) is provided with an inlet (111) on the side of the electrolyte cavity, and the inlet (111) is connected to the water tank (4) through a conduit; the water pump (3) is provided on the conduit connecting the inlet (111) and the water tank (4); The second flow guide grille (122) has an outlet (112) on the side of the electrolyte chamber corresponding to the opening. The outlet (112) is connected to the water tank (4) through a conduit.

[0010] Preferably, the first flow guide grille (121) and the second flow guide grille (122) are respectively provided with U-shaped flow guide grooves on the side that is in contact with the inner wall of the electrolyte cavity, which can prevent the formation of eddies.

[0011] Preferably, each of the electrical connection devices (5) includes a fastening bolt (51) and a wire (52). The opening of the electrolyte chamber is provided with two mounting holes, one above and one below. The connector of the metal bracket (13) and a wire (52) are locked in the lower mounting hole by a fastening bolt (51). The wire is connected to the negative terminal of the power supply (2). The connector of the anode electrode (16) and another wire (52) are locked in the upper mounting hole by another fastening bolt (51), and the wire is connected to the positive terminal of the power supply (2). More preferably, the fastening bolt is sealed with sealant to protect the electrolyte inside the cavity from leakage and the oxidation of the metal components at the connection.

[0012] Preferably, the electrolysis module (1) includes an upper electrolyte chamber (17) and a lower electrolyte chamber (11). The upper electrolyte cavity (17) and the lower electrolyte cavity (11) are respectively provided with T-shaped protrusions and U-shaped grooves to achieve the snap-fit ​​of the upper electrolyte cavity (17) and the lower electrolyte cavity (11) to seal the entire internal components of the electrolyte cavity.

[0013] The present invention also provides the application of the above-mentioned flow-through electrochemical hydrogen peroxide generating device, which is integrated into a household cleaning appliance used for sterilization, disinfection or removal of organic matter. By electrolyzing the water flowing through the device, a hydrogen peroxide solution with nano-microbubbles is synthesized, which has strong oxidizing properties and can quickly kill bacteria and viruses and remove organic pollutants, thereby having the functions of sterilization, deodorization and degradation of organic matter.

[0014] The beneficial effects achieved by this invention are as follows: (1) The present invention provides a flow electrochemical hydrogen peroxide generation device that can use natural water as raw material to generate hydrogen peroxide through a two-electron oxygen reduction reaction, thereby realizing the "on-demand use" of hydrogen peroxide, solving the cost and risk problems caused by hydrogen peroxide storage and transportation, and making it easy to integrate into various cleaning appliances that require sterilization and purification, and meeting the usage needs of different concentrations of hydrogen peroxide solution in different scenarios. (2) The present invention provides a flow electrochemical device for generating hydrogen peroxide. The entire device is a diaphragm-free design and a modular electrolysis device. It can be used alone or integrated into household appliance purification equipment. The electrode reaction area and device volume can be changed according to the usage requirements. (3) The present invention provides a device for generating hydrogen peroxide by flow-through electrochemical process. The U-shaped structure design on the flow guide grid increases the residence time of water inside the electrolyzer, prolongs the electrolysis time, increases the concentration of hydrogen peroxide, and avoids the formation of eddies. (4) The present invention provides a flow electrochemical hydrogen peroxide generation device, which improves the hydrogen peroxide synthesis efficiency by optimizing the material composition of the anode electrode and the cathode electrode. (5) The device for generating hydrogen peroxide by flow electrochemical process provided by the present invention has the advantages of high efficiency and energy saving, good stability, simple preparation process, rapid mass production and controllable cost. Attached Figure Description

[0015] Figure 1 This is a schematic diagram showing the connection relationship of a flow-through electrochemical hydrogen peroxide generating device according to a specific embodiment; Figure 2 This is a schematic diagram showing the exploded structure of the electrolysis module in a flow-through electrochemical hydrogen peroxide generating device as described in a specific embodiment. Figure 3 This is a schematic cross-sectional view of the electrolysis module in a flow-through electrochemical hydrogen peroxide generating device as described in a specific embodiment. Figure 4 This is a top view of the second flow guide grid in a flow-through electrochemical hydrogen peroxide generating device according to a specific embodiment; Figure 5 A cross-sectional view of the second flow guide grid in a flow-through electrochemical hydrogen peroxide generating device according to a specific embodiment; Figure 6 This is a graph showing the change in hydrogen peroxide concentration in the water tank during the circulating water test of the device for generating hydrogen peroxide using a flow-through electrochemical method as described in Specific Embodiment 1. Figure 7 This is a graph showing the change in hydrogen peroxide concentration in the water tank during the circulating water test of the device for generating hydrogen peroxide by a flow-through electrochemical process described in Specific Embodiment 2. Figure 8 The concentration change of hydrogen peroxide generated by a single flow through the device in a specific embodiment 3 is shown in the flow electrochemical hydrogen peroxide generation device. Figure 9 This is a stability test of hydrogen peroxide generated by a single flow through the device described in Specific Embodiment 4. Figure 10 For the specific comparative example 1, the concentration change of hydrogen peroxide generated by a single flow through the device in an electrochemical flow-through process is shown. In the attached diagram with reference to the label: 1. Electrolysis module; 2. Power supply; 3. Water pump; 4. Water tank; 5. Electrical connection device; 11. Lower electrolyte chamber; 121. First flow guide grid; 122. Second flow guide grid; 13. Metal support; 14. Cathode electrode; 15. Insulating grid; 16. Anode electrode; 17. Upper electrolyte chamber; 51. Fastening bolt; 52. Wire; 111. Inlet; 112. Outlet; 113. Lower fixing slot; 114. Upper fixing slot. Detailed Implementation

[0016] This invention provides a device for generating hydrogen peroxide by flow electrochemistry. The anode electrode and cathode electrode adopt a plate-shaped curved surface (such as a sawtooth) structure and a three-dimensional porous structure, respectively, which can effectively increase the reaction area and improve the generation rate of hydrogen peroxide.

[0017] The anode electrode is an inert material such as a porous titanium plate, titanium mesh, or sintered titanium felt. The surface of the anode electrode is coated or electroplated with a catalyst layer, which includes one or more metal oxides selected from the oxides of platinum, ruthenium, iridium, palladium, titanium, and cobalt.

[0018] The cathode electrode is a carbon material with a three-dimensional porous structure, such as PAN-based carbon fiber felt, porous graphite plate, graphite carbon felt, or activated carbon felt. An active layer is provided on the surface of the cathode electrode. This active layer includes one or more of graphite, polytetrafluoroethylene composites, and commercially available toners with high specific surface area (such as Cabot XC-72R, BP2000, and Ketjen Black ECP). The active material loading is 1-4 mg / cm³. 2 The thickness of the cathode electrode is 1-4 mm.

[0019] This invention provides an apparatus for the generation of hydrogen peroxide via a flow-through electrochemical process, such as... Figure 1-5As shown, the system includes an electrolysis module 1, a power supply 2, a water pump 3, an electrolyte tank 4, and an electrical connection device 5. The electrolysis module 1 includes a lower electrolyte chamber 11 and an upper electrolyte chamber 17, which are detachable components fixed within the chamber. The lower electrolyte chamber 11 and the upper electrolyte chamber 17 are respectively provided with an inlet 111 and an outlet 112. The inlet 111 and the outlet 112 are connected to the water tank 4 via conduits. The water pump 3 is mounted on the conduit connecting the inlet 111 and the water tank 4. Water flows into the electrolyte chamber through the inlet 111, passes sequentially through the first flow guide grille 121, the metal support 13, the cathode electrode 14, the insulating grille 15, the anode electrode 16, and the second flow guide grille 122, and flows out of the electrolyte chamber through the outlet 112. Both the inlet 111 and the outlet 112 are equipped with quick-connect plugs for easy connection to the water circuit.

[0020] In a preferred embodiment, the upper electrolyte cavity 17 and the lower electrolyte cavity 11 are respectively provided with a T-shaped protrusion and a U-shaped groove at the connection point. The upper electrolyte cavity 17 and the lower electrolyte cavity 11 are interlocked to seal the entire internal components of the electrolyte cavity. Preferably, the upper electrolyte cavity 17 and the lower electrolyte cavity 11 are made of polyphenylene oxide (PPO), which has good flame retardancy and heat resistance, high heat resistance, high rigidity, and good dimensional stability. The upper electrolyte cavity 17 and the lower electrolyte cavity 11 can be fixedly connected by hot plate welding. This connection method has strong structural strength and can withstand pressure of more than 2.5 MPa.

[0021] In a preferred embodiment, the first and second flow guide grilles 121 and 122 are provided with U-shaped flow guide grooves, with one side of the U-shaped flow guide grooves adhering to the inner wall of the electrolyte chamber. This changes the flow direction of the electrolyte, prolongs the residence time of the electrolyte in the electrolyte chamber, increases the electrolysis time and the concentration of hydrogen peroxide generated, and effectively prevents the formation of eddies. The insulating grille 15 is used to separate the cathode electrode 14 and the anode electrode 16, and presses the cathode electrode 14 onto the metal support 13 to conduct electricity through the metal support 13. The first and second flow guide grilles 121 and 122 are respectively provided with openings at one corner, facing the inlet 111 and outlet 112 respectively, facilitating the inflow and outflow of electrolyte. The first flow guide grille 121, the second flow guide grille 122, and the insulating grille 15 are made of plastic, ceramic, or three-dimensional polymer materials.

[0022] In a preferred embodiment, the metal bracket 13 is made of stainless steel, titanium, nickel, or copper, and the thickness of the metal bracket is 0.2-1.5 mm.

[0023] In a preferred embodiment, the connector of the anode electrode 16 and the connector of the metal bracket 13 that is attached to the cathode electrode 14 are respectively set in the upper fixing slot 114 and the lower fixing slot 113 on the partition plate of the electrolyte chamber, and are connected to the positive and negative terminals of the power supply 2 through fastening bolts 51 and wires 52. The opening of the electrolyte chamber is provided with two mounting holes for inserting fastening bolts 51. The fastening bolts 51 are threaded self-tapping screws, and the screws are made of 304 stainless steel, titanium, copper or stainless steel plated with nickel.

[0024] In a preferred embodiment, the device for generating hydrogen peroxide via a flow-through electrochemical process is placed in the electrolyte within the water purification device. The electrolyte can be mineral water, tap water, or natural water. The anode electrode 16 and cathode electrode 12 are in direct contact with the electrolyte. When the power is turned on, the electrolyte flows through the electrolysis device (anode electrode: H2O → 1 / 2 O2 + 2H2O). + +2e - and cathode electrode O2+2H + +2e - →2H2O2) can be used to synthesize hydrogen peroxide solution.

[0025] Furthermore, in addition to the above reactions, hydrogen peroxide also undergoes a decomposition reaction at the anode: (H₂O₂ → HO₂· + H₂O) + +e - ;HO2·→O2+H + +e - ).

[0026] Based on the above-mentioned electrolysis device, the present invention also provides an application in household appliance purification equipment, in which the device is used to electrolyze tap water or mineral water flowing through the electrolysis device to synthesize a hydrogen peroxide solution with nano-microbubbles. This solution has strong oxidizing properties and can quickly kill bacteria, viruses and organic pollutants, thereby having the functions of sterilization, deodorization and degradation of organic matter.

[0027] Assembly of the hydrogen peroxide electrolysis unit: The first flow guide grille 121 and the second flow guide grille (122) are respectively set in the lower electrolyte cavity 11 and the upper electrolyte cavity 17. The connector of the metal bracket 13 is set in the lower fixing slot 113 of the lower electrolyte cavity 11. The cathode electrode 14 is pressed to fit onto the metal bracket 13. The metal bracket 13 is fixed with fastening bolts 51. The anode electrode 16 is set below the second flow guide grille 121 in the upper electrolyte cavity 17. The connector of the anode electrode 16 passes through the upper fixing slot 114 and is fixed with fixing bolts 51. The insulating grille 15 is set between the cathode electrode 14 and the anode electrode 16. The upper electrolyte cavity 17 and the lower electrolyte cavity 11 are interlocked by T-shaped protrusions and U-shaped grooves to seal the entire internal components of the electrolyte cavity. The electrolysis module is connected to the positive and negative terminals of the power supply 2 through wires 52.

[0028] The technical effects of the present invention will be explained in detail below through specific implementation examples: Example 1 The hydrogen peroxide electrolysis device electrolyzes tap water to produce hydrogen peroxide solution: Anode electrode preparation: A sandblasted titanium mesh plate of suitable size (4*4mm aperture, 0.7mm thickness) was cut and immersed in a 10wt% NaOH solution at 80℃ for 1 hour to remove oil. It was then ultrasonically cleaned in distilled water for 3 minutes, followed by heating in a 10% oxalic acid solution at a constant temperature of 80℃ for 90 minutes to remove the surface oxide film and perform etching, facilitating coating adhesion. The treated titanium mesh plate was then ultrasonically cleaned in distilled water for 3 minutes and dried for use as the electrode substrate.

[0029] Weigh 4.78 g of chloroplatinic acid (H2PtCl6·xH2O, Pt>35%) solid and add it to 50 ml of ethanol solution. Stir until completely dissolved to obtain a metal salt solution. The metal salt solution was uniformly coated onto the titanium substrate with a brush. The titanium substrate was then dried in an oven at 80°C for 10 minutes, removed and cooled to room temperature, and then transferred to a muffle furnace and calcined at 300°C for 1 hour. The coating-drying-calcining process was repeated 10 times. The final calcination temperature was 500°C and the calcination time was 3 hours. The substrate was then removed and cooled to room temperature to obtain an anode electrode with a coating thickness of 2 μm.

[0030] Preparation of the cathode electrode: Graphite carbon felt (Inner Mongolia Wanxing Carbon Co., Ltd., 3mm thick, specific surface area 150-300g / m²) was used. 2 The working electrode was cut into 4x4mm sheet shapes, and the carbon catalyst (Cabot XC-72R) was deposited on the surface of the graphite carbon felt by electrophoretic adsorption process to obtain a cathode electrode with a catalyst loading of 2.5mg / cm².

[0031] The anode and cathode electrodes prepared in the above process are respectively... Figure 2 The device, as shown, is installed in an electrolysis unit. The anode electrode and the metal support pressed against the cathode electrode of the hydrogen peroxide electrolysis unit are connected to the negative and positive terminals of the power supply respectively via electrical connection devices. Figure 1 As shown. Then, 1L of tap water (TDS value 130) was added to the water tank for a performance test of circulating electrolytic synthesis of hydrogen peroxide. The water tank was placed in a constant temperature water bath stirrer at 25℃, and a small magnetic stirrer was used to continuously stir the water. The working dimensions of the anode electrode were 40x40mm and 0.7mm thick, and the working dimensions of the cathode electrode were 40x40mm and 2.0mm thick. The water pump was turned on (12V, 0.6W, flow rate 70ml / min), and the electrolysis module performed hydrogen peroxide electrochemical synthesis for 60 minutes under a constant voltage of 12V. The concentration of hydrogen peroxide in the water tank was measured every 5 minutes. (The text repeats itself here.) Figure 6 As shown, the final results indicate that the highest hydrogen peroxide content in the solution was measured after 20 minutes of electrolysis under constant voltage of 12V, with a concentration of 4.1 mg / L.

[0032] In Example 1, the hydrogen peroxide concentration increased linearly with time within 20 minutes. After electrolysis for more than 20 minutes, the concentration of hydrogen peroxide in the solution remained stable. The highest concentration of hydrogen peroxide was measured at 4.1 mg / L after 20 minutes of electrolysis. This is because, without aeration, the hydrogen peroxide produced by electrolysis relies on dissolved oxygen in the water and oxygen produced by anodic electrolysis. After 20 minutes of electrolysis, the oxygen adsorbed at the cathode and the dissolved oxygen in the water reach saturation, and the production of hydrogen peroxide and the side reactions reach equilibrium, at which point the concentration of hydrogen peroxide in the tank remains stable.

[0033] Example 2 Compared with Example 1, the only difference is that a 4 cm diameter air plate was placed in the water tank, and hydrogen peroxide was electrochemically synthesized for 60 minutes under constant voltage (12V) conditions using an oxygenation air pump (gas flow rate: 300 ml / min). The concentration of hydrogen peroxide in the water tank was tested every 5 minutes. Figure 7 As shown, the final results indicate that the highest hydrogen peroxide content in the solution was measured after electrolysis for 15 minutes under constant voltage (12V) conditions, with a concentration of 8.4 mg / L.

[0034] Compared to Example 1, the hydrogen peroxide concentration was twice that when air was introduced. This indicates that sufficient oxygen is beneficial for hydrogen peroxide formation, but the hydrogen peroxide concentration does not increase linearly with the amount of oxygen. Increasing the aeration rate has two effects on the online hydrogen peroxide concentration: it increases the concentration dissolved in the aqueous solution and it increases the oxygen transfer rate in the solution. At ambient pressure and room temperature, once the dissolved oxygen concentration in the water and the oxygen adsorbed on the cathode reach their maximum values, further increasing the aeration rate will not increase the hydrogen peroxide concentration. The time to oxygen saturation is shortened under aeration conditions, and the rate of hydrogen peroxide synthesis increases.

[0035] Example 3 The preparation process of the electrode assembly and the electrolysis device are the same as in Example 1, except that the water pump's inlet and outlet pipes are placed in two separate water tanks. Tap water (TDS130) is added to the tank containing the inlet pipe, and the concentration of hydrogen peroxide in the outlet solution is tested every 5 minutes. Figure 8 As shown, the final results indicate that a hydrogen peroxide solution with a concentration of approximately 4.2 mg / L can be stably produced during the 60-minute electrolysis experiment.

[0036] like Figure 8 As described above, the concentration of hydrogen peroxide stabilizes after 20 minutes of electrolysis. During the first 20 minutes of electrolysis, the concentration of hydrogen peroxide increases because the oxygen adsorbed at the cathode and the dissolved oxygen in the water are not yet saturated (i.e., the amount of oxygen has not yet stabilized). After more than 20 minutes of electrolysis, the concentration of hydrogen peroxide reaches its maximum and then remains stable. This phenomenon is caused by side reactions: while the electroreduction of oxygen to produce hydrogen peroxide occurs, the 4e- of oxygen is also reduced to OH-, leading to the further reduction of hydrogen peroxide; hydrogen peroxide is oxidized at the anode to intermediate free radicals and oxygen. (H₂O₂ → HO₂·+H₂O) + +e - ;HO2·→O2+H + +e - H2O- 2e - →O2+2H + Under constant voltage of 12V, the electrochemical synthesis of hydrogen peroxide using flowing water can maintain an equilibrium state, meaning that the generation of hydrogen peroxide and the side reactions that occur are in equilibrium. In Example 2, since the tap water flows through the electrolysis device only once, after 20 minutes of electrolysis, the electrolysis system for synthesizing hydrogen peroxide stabilizes, and the concentration of the generated hydrogen peroxide also stabilizes.

[0037] Example 4 Figure 9Example 2 is a stability test of the synthesis of hydrogen peroxide by electrolyzing tap water through an electrolysis device under constant voltage of 12V. The experimental results show that the device of the present invention operated stably for 330 hours without any degradation. Example 4 proves the stability of the flow-through electrochemical hydrogen peroxide generation device of the present invention.

[0038] Comparative Example 1 The preparation process of the electrode assembly and the electrolysis device are the same as in Example 1, except that untreated graphite carbon felt (Inner Mongolia Wanxing Carbon Co., Ltd., 3mm thick, specific surface area 150-300g / m²) is used. 2 Cut the material into 4x4mm sheets and use them directly as the cathode electrode. Test the concentration of hydrogen peroxide in the outlet solution every 5 minutes. Figure 10 As shown, the final results indicate that the highest hydrogen peroxide content in the solution was measured under constant pressure of 12V, with a concentration of 0.7 mg / L. When untreated graphite carbon felt was used directly as the reaction cathode, the generation rate and amount of hydrogen peroxide were significantly lower than in Example 1. This is because the untreated graphite carbon felt surface has fewer active sites, which is unfavorable for oxygen adsorption and transfer.

[0039] In summary, this invention provides a flow-through electrochemical hydrogen peroxide generator that can stably produce a hydrogen peroxide solution of a certain concentration using tap water as raw material, achieving "on-demand production" of hydrogen peroxide and solving the cost and risk problems associated with hydrogen peroxide storage and transportation. Furthermore, depending on the application scenario, the yield and synthesis rate of hydrogen peroxide can be improved by increasing the electrode area or introducing air, facilitating integration into various cleaning appliances requiring sterilization and purification, and meeting the needs for different concentrations of hydrogen peroxide solution in different scenarios, thus demonstrating broad application prospects.

[0040] Although the present invention has been described in detail above with general descriptions, specific embodiments, and experiments, modifications or improvements can be made to it, which will be obvious to those skilled in the art. Therefore, all such modifications or improvements made without departing from the spirit of the present invention fall within the scope of protection claimed by the present invention.

Claims

1. A device for generating hydrogen peroxide via a flow-through electrochemical process, characterized in that, It includes an electrolysis module (1), a power supply (2), a water pump (3), a water tank (4), and an electrical connection device (5); The electrolysis module (1) includes an electrolyte chamber with an opening on one side. The electrolyte chamber is provided with a first flow guide grid (121), a metal support (13), a cathode electrode (14), an insulating grid (15), an anode electrode (16), and a second flow guide grid (122) from bottom to top. The electrolyte chamber is provided with a spacer baffle for sealing the electrolyte chamber near the opening. The spacer baffle is provided with a lower fixing slot (113) and an upper fixing slot (114). The connector of the metal bracket (13) passes through the lower fixing slot (113) and is connected to the negative terminal of the power supply (2) through an electrical connection device (5). The connector of the anode electrode (16) passes through the upper fixing slot (114) and is connected to the positive terminal of the power supply (2) through another electrical connection device (5).

2. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to claim 1, characterized in that, The anode electrode (16) includes a titanium substrate, and a catalytic layer with a thickness of 2-5 μm is disposed on the surface of the titanium substrate; The titanium substrate is a titanium mesh, a porous titanium plate, or a sintered titanium felt; the catalyst layer comprises one or more metal oxides selected from the oxides of platinum, ruthenium, iridium, palladium, titanium, and cobalt.

3. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to claim 2, characterized in that, The method for preparing the anode electrode (16) includes the following steps: A) Prepare an ethanol solution of the metal salt; B) The ethanol solution of the metal salt is uniformly coated onto the titanium substrate, then dried, transferred to a muffle furnace for calcination, and the coating-drying-calcination process is repeated 10-30 times to obtain the final product.

4. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to claim 3, characterized in that, In step B), the ethanol solution of the metal salt is applied in batches of 1m each time. 2 The coating amount on the substrate is 4-8 mL; And / or, in step B), the drying temperature is 80-150℃ and the time is 5-20 min; the calcination temperature is 300-500℃ and the time is 1-3 hours.

5. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-4, characterized in that, The cathode electrode (14) includes a carbon substrate, and an active layer is disposed on the surface of the carbon substrate; The carbon substrate is PAN-based carbon fiber felt, porous graphite plate, graphite carbon felt, or activated carbon felt; the active layer comprises one or more active materials selected from graphite, polytetrafluoroethylene, and carbon powder with high specific surface area, wherein the loading of the active material is 1-4 mg / cm³. 2 .

6. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-4, characterized in that, An opening is provided at one corner of the first guide grille (121) and the second guide grille (122); The opening of the first flow guide grille (121) is provided with an inlet (111) on the side of the electrolyte cavity, and the inlet (111) is connected to the water tank (4) through a conduit; the water pump (3) is provided on the conduit connecting the inlet (111) and the water tank (4); The second flow guide grille (122) has an outlet (112) on the side of the electrolyte chamber corresponding to the opening. The outlet (112) is connected to the water tank (4) through a conduit.

7. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-4, characterized in that, The first flow guide grille (121) and the second flow guide grille (122) are respectively provided with U-shaped flow guide grooves on the side that is in contact with the inner wall of the electrolyte cavity.

8. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-4, characterized in that, Each of the electrical connection devices (5) includes a fastening bolt (51) and a wire (52); The opening of the electrolyte chamber is provided with two mounting holes, one above and one below. The connector of the metal bracket (13) and a wire (52) are locked in the lower mounting hole by a fastening bolt (51). The wire is connected to the negative terminal of the power supply (2). The connector of the anode electrode (16) and another wire (52) are locked in the upper fixed mounting hole by another fastening bolt (51), and the wire is connected to the positive terminal of the power supply (2).

9. The apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-4, characterized in that, The electrolysis module (1) includes an upper electrolyte chamber (17) and a lower electrolyte chamber (11). The upper electrolyte cavity (17) and the lower electrolyte cavity (11) are respectively provided with a T-shaped protrusion and a U-shaped groove at the connection point to realize the snap-fit ​​between the upper electrolyte cavity (17) and the lower electrolyte cavity (11).

10. The application of the apparatus for generating hydrogen peroxide by flow-through electrochemical means according to any one of claims 1-9, characterized in that, The device is integrated into a household cleaning appliance used for sterilization, disinfection, or removal of organic matter.

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