Electrochemical method, electrode and system for synthesizing hydrogen peroxide without aeration

Abstract

The invention provides an electrochemical method, an electrode and a system for synthesizing hydrogen peroxide without aeration, and relates to the technical field of electrochemical preparation of hydrogen peroxide. The multistage hole penetrating type cathode with a specific multistage hole channel structure is adopted, the oxygen-containing electrolyte penetrates through the multistage hole penetrating type cathode for electrochemical reaction under the non-aeration condition, dissolved oxygen in fluid is forced to make efficient contact with catalytic active sites through the multistage hole channel structure, the mass transfer process is greatly enhanced, and the catalytic activity of the catalyst is improved. And the diffusion limitation of the traditional flow-through electrode is overcome. And meanwhile, the structure required for synthesizing hydrogen peroxide is simplified by an aeration-free operation mode, and the energy consumption and the cost are reduced. Finally, through the synergistic effect of the technical characteristics, the high-yield and high-flux synchronous output of hydrogen peroxide can be realized under the condition that an expensive catalyst and external gas aeration are not needed.

Description

Technical Field

[0001] This invention relates to the field of electrochemical preparation of hydrogen peroxide, and in particular to an electrochemical method, electrode, and system for the synthesis of hydrogen peroxide without aeration. Background Technology

[0002] Hydrogen peroxide is an important green oxidant and disinfectant, widely used in chemical, environmental protection, electronics, and medical fields. Traditional large-scale centralized production via the anthraquinone process suffers from high energy consumption and significant storage and transportation risks, making it difficult to meet the needs of distributed, on-demand production. In recent years, the in-situ preparation of hydrogen peroxide via the electrochemical two-electron oxygen reduction pathway has become a research hotspot due to its flexibility.

[0003] Existing electrochemical synthesis technologies for hydrogen peroxide typically face several key challenges: First, high-performance catalysts often rely on precious metals (such as platinum and palladium) or complexly synthesized non-metallic carbon materials (such as nitrogen-doped carbon nanotubes), resulting in high material costs and complex preparation. Second, the reaction system is highly dependent on external aeration (introducing pure oxygen or air) to replenish oxygen reactants, increasing system complexity and operating costs. Furthermore, the low solubility and slow mass transfer of oxygen in the electrolyte limit the reaction rate. Finally, the common flow-through electrode structure has limited mass transfer efficiency, making it difficult to simultaneously achieve high hydrogen peroxide yield and high throughput, thus failing to meet the demand for high-throughput production in practical applications.

[0004] Therefore, there is an urgent need to develop an electrochemical method and apparatus that can achieve efficient, high-throughput hydrogen peroxide synthesis using low-cost materials without relying on external aeration. Summary of the Invention

[0005] In view of this, the technical problem to be solved by the present invention is: how to provide an electrochemical method and apparatus that is low-cost, low-energy-consumption, simple in structure, and can simultaneously achieve high-yield and high-throughput synthesis of hydrogen peroxide.

[0006] On one hand, the present invention provides an electrochemical method for synthesizing hydrogen peroxide without aeration, comprising the following steps: S100, providing an electrochemical cell, the electrochemical cell comprising a porous anode and a multi-level porous through-hole cathode; S200, introducing an oxygen-containing electrolyte into the electrochemical cell, wherein the oxygen-containing electrolyte, under the action of a driving force, penetrates and flows through the multi-level porous through-hole cathode without external gas aeration; S300, applying a voltage between the multi-level porous through-hole cathode and the porous anode, causing oxygen dissolved in the electrolyte to undergo a two-electron oxygen reduction reaction inside the multi-level porous through-hole cathode to generate hydrogen peroxide; S400, collecting the electrolyte effluent containing hydrogen peroxide.

[0007] Optionally, the flow rate of the oxygen-containing electrolyte is 0.5 mL / min to 8 mL / min.

[0008] Optionally, in step S300, the voltage applied between the multi-level through-hole cathode and the multi-hole anode is 2 V to 8 V.

[0009] Alternatively, the porous anode may be made of any one of titanium, stainless steel, or conductive metal oxide.

[0010] Optionally, the porous anode is a titanium metal mesh with a pore size of 40 mesh to 400 mesh.

[0011] Optionally, the distance between the multi-level through-hole cathode and the porous anode is 0.1 cm to 1 cm.

[0012] Optionally, the oxygen-containing electrolyte includes an electrolyte and oxygen; the electrolyte is one of sodium sulfate, potassium sulfate, sodium hydroxide, or potassium hydroxide solution.

[0013] Optionally, the electrochemical cell operates in dead-end filtration mode.

[0014] On the other hand, the present invention provides a hierarchical porous through-hole electrode for aeration-free hydrogen peroxide synthesis, comprising: a biomass substrate; and a laser-induced graphene layer located on at least one surface of the biomass substrate; wherein, the hierarchical porous through-hole electrode has a through-hole hierarchical channel structure, the hierarchical channel structure including micron-sized channels naturally formed by the biomass substrate and nano-sized pores generated by the laser-induced process; the laser-induced graphene layer is integrally connected to the biomass substrate through an in-situ formed mechanical anchoring interface.

[0015] Optionally, the pore size of the micron-sized channels ranges from 1 μm to 100 μm.

[0016] Optionally, the pore size of the nanoscale pores ranges from 10 nm to 1000 nm.

[0017] Optionally, the thickness of the laser-induced graphene layer is greater than 10 μm.

[0018] Alternatively, the biomass substrate may be made of wood, bamboo, plant leaves, or biomass fiber membrane.

[0019] On the other hand, the present invention also provides an aeration-free hydrogen peroxide synthesis system, comprising: an electrochemical cell, which includes: Such as the multi-stage through-hole cathode described above; A porous anode is spaced apart from a multi-level through-hole cathode. A power supply for applying voltage between a multi-stage through-hole cathode and a multi-stage anode; A fluid-driven device is used to pump oxygen-containing electrolyte into an electrochemical cell in a through-flow manner and to make the oxygen-containing electrolyte flow through a multi-hole through-cathode.

[0020] The implementation of this invention offers the following advantages: By employing a multi-level porous through-hole cathode with a specific multi-level channel structure, and allowing oxygen-containing electrolyte to flow through the cathode for electrochemical reaction under aeration-free conditions, this multi-level channel structure forces dissolved oxygen in the fluid to achieve efficient contact with the catalytically active sites, greatly enhancing the mass transfer process and overcoming the diffusion limitations of traditional flow-through electrodes. Simultaneously, the aeration-free operation mode simplifies the structure required for hydrogen peroxide synthesis, reducing energy consumption and cost. Ultimately, these technical features work synergistically, enabling this invention to achieve high yield and high throughput of hydrogen peroxide simultaneously without expensive catalysts or external gas aeration, significantly reducing the operational complexity and overall cost of hydrogen peroxide electrochemical synthesis.

[0021] Furthermore, this invention also provides a hierarchical through-hole electrode for aeration-free hydrogen peroxide synthesis. This electrode utilizes the natural micron-sized channels of biomass materials and laser-induced nano-sized pores. The micron-sized channels, acting as the main fluid pathways, significantly reduce fluid resistance, ensuring that the electrolyte can pass smoothly through the electrode at a high flux. Meanwhile, the nano-sized pores greatly increase the specific surface area of ​​the electrode, providing abundant two-electron oxygen reduction reaction active sites. Attached Figure Description

[0022] Figure 1 This is a cross-sectional scanning electron microscope image of a multi-level through-hole electrode in one embodiment; Figure 2 This is a top-view scanning electron microscope image of a multi-level through-hole electrode at different micro- and nano-scales, as shown in one embodiment. Figure 3 This is a diagram showing the aperture distribution at different scales of a multi-level through-hole electrode in one embodiment; Figure 4 This is a diagram illustrating the performance of a multi-level perforated electrode in producing hydrogen peroxide at different flow rates, as shown in one embodiment. Figure 5 This is a diagram illustrating the performance of a multi-level through-hole electrode in producing hydrogen peroxide at different voltages, as shown in one embodiment. Detailed Implementation

[0023] The present invention will now be described in further detail with reference to the accompanying drawings and specific embodiments. The step numbers in the following embodiments are only for ease of explanation and do not limit the order of the steps. The execution order of each step in the embodiments can be adapted according to the understanding of those skilled in the art.

[0024] The terminology used in the embodiments of this application is for the purpose of describing particular embodiments only and is not intended to limit the embodiments of this application. The singular forms “a,” “the,” and “the” used in the embodiments of this application and the appended claims are also intended to include the plural forms unless the context clearly indicates otherwise. It should also be understood that the term “and / or” as used herein refers to and includes any or all possible combinations of one or more of the associated listed items.

[0025] In the following description, when referring to the accompanying drawings, unless otherwise indicated, the same numbers in different drawings represent the same or similar elements. The embodiments described in the following exemplary embodiments do not represent all embodiments consistent with this application. Rather, they are merely examples of apparatuses and methods consistent with some aspects of this application as detailed in the appended claims. In the description of this application, it should be understood that the terms "first," "second," "third," etc., are used only to distinguish similar objects and are not necessarily used to describe a specific order or sequence, nor should they be construed as indicating or implying relative importance. Those skilled in the art can understand the specific meaning of the above terms in this application according to the specific circumstances.

[0026] Furthermore, in the description of this application, unless otherwise stated, "multiple" means two or more. "And / or" describes the relationship between related objects, indicating that three relationships can exist. For example, A and / or B can represent: A alone, A and B simultaneously, or B alone. The character " / " generally indicates that the preceding and following related objects have an "or" relationship.

[0027] Example 1 In this embodiment, as Figure 1 An electrochemical method for synthesizing hydrogen peroxide without aeration, as shown, includes the following steps: S100, provides an electrochemical cell, which includes a porous anode and a multi-level porous through-hole cathode; S200. An oxygen-containing electrolyte is introduced into the electrochemical cell, wherein the oxygen-containing electrolyte, under the action of driving force, penetrates and flows through the multi-stage perforated cathode without the addition of external gas aeration. S300: A voltage is applied between the multi-level porous through-hole cathode and the porous anode, causing the oxygen dissolved in the electrolyte to undergo a two-electron oxygen reduction reaction inside the multi-level porous through-hole cathode to generate hydrogen peroxide. S400, Collect the electrolyte effluent containing hydrogen peroxide.

[0028] In this embodiment, the porous anode is made of any one of titanium, stainless steel or conductive metal oxide. The porous anode mainly undergoes an oxygen evolution reaction during electrolysis, which is used to mix with the electrolyte to form an oxygen-containing electrolyte. The oxygen generated by the oxygen evolution reaction can move with the electrolyte into the interior of the multi-level porous through-hole cathode to react.

[0029] In this embodiment, the oxygen generated inside the multi-level porous through-hole cathode mainly utilizes oxygen dissolved directly in the electrolyte from the air (i.e., dissolved oxygen). The oxygen generated by the porous anode is to replenish the dissolved oxygen, and the oxygen that cannot be dissolved in the electrolyte is released to the outside as it passes through the multi-level porous through-hole cathode.

[0030] Specifically, the porous anode is a titanium metal mesh structure with a pore size of 40 mesh to 400 mesh.

[0031] In this embodiment, in step S300, the voltage applied between the multi-level through-hole cathode and the porous anode is 2 V to 8 V, which can ensure that the oxygen evolution reaction occurs, and also avoid side reactions (such as hydrogen evolution reaction, further reduction or decomposition of hydrogen peroxide), heat generation runaway and sharp increase in energy consumption caused by excessive voltage.

[0032] In this embodiment, the oxygen-containing electrolyte comprises two parts: oxygen and electrolyte. The electrolyte can be selected from sodium sulfate, potassium sulfate, sodium hydroxide, or potassium hydroxide solution. Oxygen is generated through the oxygen evolution reaction described above and moves along with the electrolyte to form the oxygen-containing electrolyte.

[0033] In this embodiment, when fixing the porous anode and the multi-level through-hole cathode, the multi-level through-hole cathode is placed 0.1 cm to 1 cm directly below the porous anode. Specifically, setting 0.1 cm as the lower limit of the spacing is mainly to reserve necessary physical insulation space. In this device, by embedding an insulating gasket between the porous anode and the multi-level through-hole cathode or using a high-precision fine-tuning bracket to fix the electrode plates, it is ensured that under the impact of high-pressure fluid in dead-end filtration, neither the flexible nor rigid electrode plates will physically contact each other, leading to a short circuit. Setting 0.1 cm as the lower limit of the spacing can effectively prevent the hydrogen peroxide generated by the cathode from being directly oxidized by the porous anode. According to the definition of resistance, an excessively large spacing will significantly increase the ion transport resistance of the electrolyte, especially for low-concentration solutions with poor conductivity. An excessively large spacing leads to a sharp increase in energy consumption. Setting 1 cm as the upper limit of the spacing can effectively prevent the accumulation of oxygen bubbles generated by the porous anode between the electrodes, which would cause a sharp increase in local resistance when the spacing is too large. In addition, maintaining a spacing of less than 1 cm allows the trace oxygen generated at the anode to quickly reach the cathode interface through diffusion or fluid shearing, serving as a supplement to dissolved oxygen. This mitigates oxygen loss caused by excessive spacing and ensures high-flux hydrogen peroxide generation efficiency.

[0034] In this embodiment, the flow rate of the oxygen-containing electrolyte is 0.5 mL / min to 8 mL / min. This flow rate range can ensure a certain hydrogen peroxide yield and prevent the oxygen conversion rate from being too low due to too short a residence time.

[0035] In this embodiment, the electrochemical cell operates in dead-end filtration mode. Dead-end filtration mode means that all incoming electrolyte flows out through the multi-perforated perforated cathode, with no bypass discharge. Dead-end filtration mode helps maintain a stable liquid flow through the cathode, ensuring oxygen flows to the multi-perforated perforated cathode, thereby guaranteeing the continuous progress of the reaction.

[0036] Example 2 Based on Example 1, this embodiment provides a multi-level porous through-hole electrode for the synthesis of hydrogen peroxide without aeration.

[0037] In this embodiment, the multi-level through-hole electrode includes: Biomass substrate; And a laser-induced graphene layer located on at least one surface of the biomass substrate; The multi-level perforated electrode has a through-hole multi-level pore structure, which includes micron-level pores naturally formed by the biomass substrate and nano-level pores generated by the laser-induced process. The laser-induced graphene layer and the biomass substrate are integrated and connected through an in-situ mechanical anchoring interface.

[0038] In this embodiment, the pore size of the micron-sized channels ranges from 1 μm to 100 μm.

[0039] In this embodiment, the pore size of the nanoscale pores ranges from 10 nm to 1000 nm.

[0040] In this embodiment, the thickness of the laser-induced graphene layer is greater than 10 μm.

[0041] In this embodiment, the biomass substrate is made of any one of wood, bamboo, plant leaves, or biomass fiber membrane.

[0042] In one possible embodiment, the fabrication of a multi-level through-hole electrode includes the following steps: S1. Select biomass materials with natural microchannels (such as wood, bamboo, leaves, or biomass fiber membranes) as the biomass substrate. Cut them into thin sheets of a certain thickness (e.g., 0.5-5 mm) perpendicular to the natural grain or parallel to the fiber direction. Then, perform washing, drying, and other steps to remove impurities and obtain a dried biomass precursor.

[0043] Specifically, this invention directly utilizes natural biomass (such as wood, bamboo, and leaves) as biomass precursors, eliminating reliance on expensive metals (such as platinum and palladium) or complex artificial carbon nanomaterials. Biomass substrates are widely available, extremely low-cost, and possess natural micron-scale channels, enabling the value-added utilization of waste resources and demonstrating excellent environmental friendliness. Simultaneously, this invention significantly enhances the transport and resupply of oxygen to the catalytic interface within the hierarchical channels by utilizing an oxygen-containing electrolyte forced through a multi-level porous permeable electrode, overcoming the diffusion limitations of traditional flow-through electrodes.

[0044] In this embodiment, OSB boards are selected as the biomass base.

[0045] S2. A carbon dioxide laser is used to scan the surface of the biomass precursor, causing the lignin, cellulose and other components of the OPS board to undergo instantaneous high-temperature photothermal conversion, which in situ transforms them into highly conductive graphene carbon material, forming a graphene layer.

[0046] Specifically, laser-induced technology was used to further convert biomass precursors into highly conductive graphene-based carbon materials. Compared to pyrolysis methods, the laser-induced process can be completed instantaneously at room temperature and pressure, eliminating the need for prolonged high-temperature carbonization, thus significantly reducing energy consumption and time costs. Furthermore, the laser-induced process allows for graphical customization, and through computer-aided design, the geometry of the electrodes can be precisely controlled, facilitating industrial scale-up and integration.

[0047] Furthermore, the hierarchical through-hole electrode combines the natural micron-sized channels of biomass with laser-induced nanopores. The micron-sized channels, acting as pathways for high-speed fluid transport, significantly reduce flow resistance and ensure high-throughput transport; the nanopores provide a vast number of active sites, enhancing microscopic mass transfer and catalysis. The synergistic effect of these two technologies breaks through the mass transfer limit, enabling high-throughput, highly efficient synthesis of hydrogen peroxide in an aeration-free mode.

[0048] S3. The laser-induced graphene based on Ossun board is precisely cut to a size close to that of the multi-level hole through-electrode, then fixed onto the multi-level hole through-electrode, and the non-reactive area is insulated and sealed to ensure the stability of the effective reaction area.

[0049] In this embodiment, in step S1, the OSB board is a fiberboard with uniform density made from radiata pine as raw material through steps such as peeling, slicing, and drying.

[0050] In this embodiment, to facilitate installation during the laser-induced generation of multi-level hole structures, the thickness of the OSB plate is set to 1 mm, and the length and width are both set to 10 cm.

[0051] Specifically, in step S2, computer-aided design software is used to plan the electrode geometry, and a carbon dioxide laser is used to scan the dried biomass precursor. By precisely controlling the laser energy density distribution (including laser power, scanning speed, line spacing, and pulse frequency), the lignin, cellulose, and other components in the biomass undergo instantaneous high-temperature photothermal conversion. The laser-induced process utilizes the instantaneous high energy of the laser to trigger a nonlinear thermal effect, inducing the breaking and recombination of chemical bonds in biomass macromolecules. This causes the carbon-containing biomass precursor to undergo rapid dehydrogenation, deoxygenation, and aromatic ring reconstruction, thereby transforming it in situ into a highly conductive graphene-based carbon material. In the actual preparation process, the laser parameters are matched differently according to the physicochemical properties of different biomass substrates (such as fiber density, porosity and component ratio): for low-density wood, a higher scanning speed and moderate power are used to prevent excessive ablation; for medium and high-density wood or OSB, the scanning speed is appropriately reduced or the pulse frequency is increased to ensure that the heat energy can effectively penetrate and form a continuous and deep graphene network, so that graphene layers with uniform conductivity and excellent catalytic activity can be obtained on biomass from different sources.

[0052] Specifically, the high energy density of the laser drives the carbonization reaction while simultaneously causing the instantaneous pyrolysis of the components inside the biomass precursor, generating a large amount of gaseous products (such as water and carbon dioxide). During the overflow process, the gaseous products, through a micro-region pressure release effect, induce abundant nanoscale wrinkles and pores in situ while maintaining the original micron-scale longitudinal channels of the biomass precursor, ultimately constructing a hierarchical pore structure with a high specific surface area. This hierarchical pore structure forms a stable mechanical anchoring interface through the in-situ integrated connection between the graphene layer and the uncarbonized substrate. This cross-linked rigid three-dimensional carbon network not only provides a large number of electrocatalytic active sites but also possesses extremely high structural strength, effectively resisting the scouring force of high-velocity fluids. This prevents structural collapse, carbon layer peeling, or pore blockage under high-speed penetrating flow fields, ensuring the performance stability of the hierarchical permeable electrode in the aeration-free hydrogen peroxide synthesis process.

[0053] In one specific embodiment, a carbon dioxide laser with a wavelength of 10.6 μm, an output power of 40 W, and a spot diameter of 1.8 ± 0.2 mm was used to laser-induce laser treatment on the surface of the MDF board in an air atmosphere. The laser power was set to 35% of its maximum power (i.e., 14 W), the scanning speed to 1000 mm / s, the line spacing to 0.01 mm, and the pulse frequency to 8 kHz. The results of the laser-induced treatment are as follows: Figure 1 As shown, the lignin, cellulose, and other components of the OPS board undergo instantaneous high-temperature photothermal conversion, transforming them in situ into highly conductive graphene-based carbon materials, forming a material with properties such as... Figure 1 The graphene layer shown in segment ab. Figure 1Section bc is Osmanthus board that has not undergone laser induction.

[0054] It should be noted that in the actual preparation process, the laser parameters are differentiated according to the physicochemical properties of different biomass substrates (such as fiber density, porosity, and component ratio): for low-density wood, a higher scanning speed and moderate power are used to prevent excessive ablation; for medium- and high-density wood or OSB, the scanning speed is appropriately reduced or the pulse frequency is increased to ensure effective heat penetration and the formation of a continuous and deep graphene network, thereby obtaining a graphitized layer with uniform conductivity and excellent catalytic activity on biomass from different sources. The laser-induced OSB-based graphene material has a multi-level porous structure ranging from micrometers to nanometers (e.g., ... Figure 2 ).

[0055] Specifically, such as Figure 3 As shown, in the 100nm to 100μm scale, the average pore size (296.6nm, 3.3μm and 31.8μm) of each order of magnitude (100nm to 1μm, 1μm to 10μm, 10μm to 100μm) is close to the geometric mean of that order of magnitude (316.2nm, 3.2μm and 31.6μm), reflecting the uniformity of pore distribution. Although the average pore size in the 20nm to 200nm scale is relatively large (90.5nm), the minimum pore size can still reach 20nm to 40nm, further demonstrating the wide range of pore sizes of the laser-induced Ossun board-based graphene material.

[0056] In this embodiment, a multi-level perforated electrode (laser-induced graphene electrode based on Ossun board) is used as the cathode, with an effective reaction area of ​​1 cm * 1 cm, which is used to reduce dissolved oxygen and generate hydrogen peroxide solution.

[0057] In this embodiment, the porous anode is a 40-mesh, 0.4 mm thick titanium mesh fixed to a titanium plate current collector, which mainly undergoes oxygen evolution reaction during electrolysis. When fixing the multi-level porous through-electrode cathode and anode, the laser-induced Ossun board-based graphene electrode is placed 0.5 cm directly below the titanium mesh anode.

[0058] In this embodiment, a 0.01 M sodium sulfate solution is selected as the electrolyte, and no additional gas is introduced into the electrolyte during the electrolysis process.

[0059] In this embodiment, the electrochemical reaction of the multi-level perforated electrode is carried out in dead-end filtration mode, and the concentration of the filtered hydrogen peroxide is determined by titration with standard potassium permanganate solution (4 mM).

[0060] In this embodiment, the performance of hydrogen peroxide production was measured at a voltage of 5 V and at different electrolyte flow rates of 0.5 mL / min, 1 mL / min, 2 mL / min, 4 mL / min, and 8 mL / min. Figure 4 As shown by the blue lines, it can be seen that the hierarchical permeable electrode can effectively produce hydrogen peroxide under electrochemical reaction when the flow rate is between 0.5 mL / min and 8 mL / min. Furthermore, as the electrolyte flow rate increases, the average hydraulic residence time of the electrolyte in the hierarchical permeable electrode gradually decreases, such as... Figure 4 The yellow line in the figure shows that the production of hydrogen peroxide gradually increases when the electrolyte flow rate is 0.5 mL / min to 2 mL / min, and reaches its maximum when the electrolyte flow rate is 2 mL / min, and gradually decreases when the electrolyte flow rate is 2 mL / min to 8 mL / min.

[0061] Therefore, in this embodiment, the flow rate of the electrolyte is controlled at 2 mL / min.

[0062] In this embodiment, as Figure 5 As shown, at a flow rate of 2 mL / min, with external voltages of 2 V, 3 V, 4 V, 5 V, 6 V, 7 V, and 8 V, the hydrogen peroxide yield and Faraday current efficiency distribution were measured as follows: Figure 5 The blue and pink lines indicate that the multi-level porous through-electrode of this invention exhibits excellent hydrogen peroxide production performance, achieving a high hydrogen peroxide yield (up to 6000 mg / L). -1 h -1 ) and Faraday current efficiency (up to nearly 90%).

[0063] In summary, under non-aeration conditions, this multi-level permeable electrode can produce hydrogen peroxide at flow rates of 0.5 mL / min to 8 mL / min and voltages of 2 V to 8 V. Furthermore, at a flow rate of 2 mL / min and a voltage of 5 V, the yield can exceed 6000 mg / L. -1 h -1 It also has a capacity of 1200Lm -2 h -1 (i.e., 1cm) 2 High water flux (flow rate of 2 ml / min under fixed electrode area).

[0064] Example 3 This embodiment provides an aeration-free hydrogen peroxide synthesis system based on any of the above embodiments.

[0065] The aeration-free hydrogen peroxide synthesis system of this embodiment includes an electrochemical cell and a fluid drive device.

[0066] In this embodiment, the electrochemical cell includes: a power source, a porous anode, and a multi-level porous through-hole cathode as described above.

[0067] The porous anode and the multi-level through-hole cathode are arranged alternately; the power supply is used to apply voltage between the multi-level through-hole cathode and the porous anode, thereby providing energy for electrolysis.

[0068] A fluid-driven device is used to pump oxygen-containing electrolyte into an electrochemical cell in a through-flow manner and to make the oxygen-containing electrolyte flow through a multi-hole through-cathode.

[0069] In one possible embodiment, the fluid drive device is a peristaltic pump.

[0070] The above is a detailed description of the preferred embodiments of the present invention. However, the present invention is not limited to the embodiments described. Those skilled in the art can make various equivalent modifications or substitutions without departing from the spirit of the present invention. All such equivalent modifications or substitutions are included within the scope defined by the claims of this application.

Claims

1. An electrochemical method for synthesizing hydrogen peroxide without aeration, characterized in that, Includes the following steps: S100. An electrochemical cell is provided, the electrochemical cell comprising a porous anode and a multi-level porous through-hole cathode; S200. An oxygen-containing electrolyte is introduced into the electrochemical cell, wherein the oxygen-containing electrolyte, under the action of a driving force, penetrates and flows through the multi-level porous through-hole cathode without the addition of external gas aeration. S300, Apply a voltage between the multi-level porous through-hole cathode and the porous anode, so that the oxygen dissolved in the oxygen-containing electrolyte undergoes a two-electron oxygen reduction reaction inside the multi-level porous through-hole cathode to generate hydrogen peroxide; S400, Collect the electrolyte effluent containing the hydrogen peroxide.

2. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, The flow rate of the oxygen-containing electrolyte is 0.5 mL / min to 8 mL / min.

3. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, In step S300, the voltage applied between the multi-level through-hole cathode and the multi-hole anode is 2 V to 8 V.

4. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, The porous anode is made of any one of titanium, stainless steel, or conductive metal oxide.

5. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1 or 4, characterized in that, The porous anode is a titanium metal mesh with a pore size of 40 mesh to 400 mesh.

6. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, The distance between the multi-level through-hole cathode and the multi-hole anode is 0.1 cm to 1 cm.

7. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, The oxygen-containing electrolyte includes an electrolyte and oxygen; the electrolyte is one of sodium sulfate, potassium sulfate, sodium hydroxide, or potassium hydroxide solution.

8. The electrochemical method for synthesizing hydrogen peroxide without aeration according to claim 1, characterized in that, The electrochemical cell operates in dead-end filtration mode.

9. A multi-level porous through-hole electrode for aeration-free hydrogen peroxide synthesis, characterized in that, include: Biomass substrate; And a laser-induced graphene layer located on at least one surface of the biomass substrate; The multi-level perforated electrode has a through-hole multi-level channel structure, which includes micron-level channels naturally formed by the biomass substrate and nano-level pores generated by the laser-induced process; the laser-induced graphene layer is integrally connected to the biomass substrate through an in-situ formed mechanical anchoring interface.

10. The multi-level through-hole electrode according to claim 9, characterized in that, The pore size of the micron-sized channels ranges from 1 μm to 100 μm.

11. The multi-level through-hole electrode according to claim 9, characterized in that, The pore size of the nanoscale pores ranges from 10 nm to 1000 nm.

12. The multi-level through-hole electrode according to claim 9, characterized in that, The thickness of the laser-induced graphene layer is greater than 10 μm.

13. The multi-level through-hole electrode according to claim 9, characterized in that, The biomass substrate is made of wood, bamboo, plant leaves, or biomass fiber membrane.

14. A non-aeration hydrogen peroxide synthesis system, characterized in that, include: Electrochemical cells, comprising: The multi-stage through-hole cathode according to any one of claims 9 to 13; A porous anode is spaced apart from the multi-level porous through-hole cathode; A power source for applying voltage between the multi-stage through-hole cathode and the multi-hole anode; A fluid drive device is used to pump an oxygen-containing electrolyte into an electrochemical cell in a penetrating flow manner, and to make the oxygen-containing electrolyte flow through the multi-stage perforated cathode.

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