In-situ hydrogen peroxide production-catalytic reaction device
By designing an in-situ hydrogen peroxide production-catalytic reaction device and adopting specific electrode materials and structures, the problem of high manufacturing costs was solved, and efficient pollutant degradation effects were achieved, making it suitable for deep sewage treatment.
Patent Information
- Application Number
- CN202422649488.2
- Authority / Receiving Office
- CN · China
- Patent Type
- Utility models(China)
- Current Assignee / Owner
- Filing Date
- 2024-10-31
- Publication Date
- 2025-09-23
- Estimated Expiration
- 2034-10-31
AI Technical Summary
The high manufacturing cost of existing in-situ hydrogen peroxide electrode reactors and their difficulty in adapting to the ozone catalytic oxidation system in actual production have limited their industrial application in the field of deep wastewater treatment.
An in-situ hydrogen peroxide production-catalytic reaction device was designed. Glass sand core plates, g-C3N4/PVP/GF cathodes, and SnO2-RuO2/Ti anodes were evenly spaced inside a box. Combined with an aeration head and a peristaltic pump, an electrochemical catalytic reaction was realized, which reduced the manufacturing cost and improved the catalytic efficiency.
It achieves efficient pollutant degradation, with a COD removal rate of over 91% in 60 minutes. It has a simple structure, easy operation, and low cost, and has broad market application prospects.
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Figure CN223372858U_ABST
Abstract
Description
Technical Field
[0001] The present application relates to the field of deep water treatment in environmental engineering and chemical production technology, and in particular to an in-situ hydrogen peroxide production-catalytic reaction device. Background Art
[0002] When exploring ways to enhance ozone catalytic oxidation systems, the introduction of electrocatalytic systems has undoubtedly brought revolutionary progress to this field. This innovative approach cleverly combines ozone catalytic oxidation with the in-situ generation of H2O2, greatly improving the efficiency of the system. Its core mechanism lies in the cathode O2 reduction reaction occurring within the electrocatalytic reaction device, which follows a four-electron pathway and a two-electron pathway. When the rate at which H2O2 generated by the two-electron pathway is released from the electrode surface exceeds the rate at which it regains electrons, H2O2 accumulates in the solution and becomes the dominant product. It is worth noting that H2O2 plays a vital role in this system. It can effectively promote the decomposition of O3 into highly reactive HO· radicals, which not only accelerates the conversion of pollutants but also significantly improves the utilization efficiency of ozone. At the same time, the electrochemical oxidation at the anode also provides strong support for the direct mineralization of some pollutants.
[0003] A series of landmark research results have emerged in scientific research. Hou et al., through detailed comparative experiments, demonstrated the effectiveness of various carbon-based cathode materials (e.g., carbon-polytetrafluoroethylene, carbon felt, and reticulated glassy carbon) for the removal of diethyl phthalate (DEP) in an electro-perozonation system (i.e., electro-peroxone system). The carbon-polytetrafluoroethylene cathode, thanks to its excellent H₂O₂ yield, achieved a TOC removal rate of 91.8% within 60 minutes. This remarkable performance was positively correlated with the electrode H₂O₂ yield, further confirming the catalytic role of H₂O₂ in O₃ decomposition and HO₀ radical generation. Although the undivided reaction apparatus somewhat reduced the apparent current efficiency (approximately 86%-80%), the system maintained high DEP removal rates over six consecutive reaction cycles. Zhang et al., using a template method, fabricated a Ni-Ce / OMC (ordered mesoporous carbon) particle electrode and successfully applied it to the treatment of high-salinity organic wastewater. The presence of salt provided a sufficient electrolyte environment for the system. Using HR-TEM and SEM characterization techniques, they found that the incorporation of Ce and Ni did not alter the microporous structure of OMCs, but rather promoted the dispersion of tiny oxide crystals. The incorporation of the two metals resulted in lower charge transfer resistance (Rct) compared to single metal incorporation. With increased metal oxide dispersion, more oxygen vacancies and active sites were exposed, accelerating electron transfer and reducing surface resistance. CV curve analysis further demonstrated that Ni0.2-Ce0.2 / OMC exhibited the highest O2 reduction peak current (0.287 mA) at -0.419 V and achieved a 93.7% COD removal rate within 60 minutes in the treatment of coal chemical reverse osmosis wastewater. Wu et al. prepared Mn- and Fe-modified carbon nanotubes as cathode catalysts and constructed a carbon-PTFE gas diffusion electrode. This electrode performed well in an electro-ozone hybrid system, degrading 71.9% of diatrizoate (DTZ) in just 10 minutes. XRD and SEM characterization results showed that the catalyst surface was covered with MnFe2O4 crystal particles. The addition of Fe and Mn oxides not only promoted the decomposition of O3, but also accelerated the decomposition process of H2O2. Ghalebizade and Ayati designed a cylindrical array electro-ozonation reactor with circulating flow and conducted degradation experiments on the dye Acid Orange 7 (AO7). By optimizing operating conditions such as current density, pollutant concentration, oxygen flow rate, and pH, the system successfully degraded 99% of the high-concentration AO7 (500 mg / L) within 40 minutes, while achieving significant reductions in COD and TOC (72% and 52%, respectively).However, despite significant laboratory success, these research findings remain limited in industrial application due to the high manufacturing costs of in-situ hydrogen peroxide electrode reactors and their incompatibility with ozone catalytic oxidation systems used in production. In practice, H₂O₂ is often added externally, which increases the risks and costs of transportation and storage and limits the widespread application of ozonation technology in advanced wastewater treatment. Utility Model Content
[0004] In order to make up for the above deficiencies, the present application provides an in-situ hydrogen peroxide generation-catalytic reaction device to solve the problems raised in the above background technology.
[0005] In order to achieve the above-mentioned purpose, the technical solution adopted by the present invention to solve the technical problem is as follows:
[0006] A catalytic reaction device for in-situ hydrogen peroxide production comprises a box body and a top cover installed on the top of the box body. A plurality of glass sand core plates are arranged at equal intervals inside the box body. Four g-C3N4 / PVP / GF cathodes and three SnO2-RuO2 / Ti anodes are sequentially installed between the plurality of glass sand core plates and the box body. Four air inlets are opened at equal intervals on the side wall of the box body, and four aeration heads are arranged at equal intervals on the inner bottom. The four air inlets are respectively interconnected with the air inlet ends of the four aeration heads. The four aeration heads are respectively located at the bottom of the four g-C3N4 / PVP / GF cathodes.
[0007] Furthermore, four cathode power connections are provided at equal intervals on the side wall of the box, and the four cathode power connections are electrically connected to the four g-C3N4 / PVP / GF cathodes respectively.
[0008] Furthermore, three anode power connections are provided at equal intervals on the other side of the box, and the three anode power connections are respectively connected to the three SnO2-RuO2 / Ti anode batteries.
[0009] Furthermore, a plurality of water inlets are provided at equal intervals on the bottom of the box side, and a plurality of the water inlets are provided with connecting pipes.
[0010] Furthermore, an air outlet is provided at the top of the top cover, and the air outlet is provided with an exhaust valve.
[0011] Furthermore, a water outlet is provided on the side wall of the top cover, and a peristaltic pump is installed at the water outlet.
[0012] Furthermore, a sealing ring is provided between the box body and the top cover, and the edge has a connecting plate and is connected by bolts.
[0013] The utility model has the following beneficial effects:
[0014] 1. This utility model can be used with various ozone oxidation devices and can be equipped with different numbers of cathodes and anodes according to actual production needs to meet actual production needs. At the same time, the reactor cavity is made of organic glass, and the electrode tank can be equipped with different types and numbers of cathodes and anodes according to actual needs. It is universally applicable to various ozone catalytic oxidation systems, greatly reducing manufacturing costs.
[0015] 2. Comparative experiments using the dye cationic red as the target pollutant revealed that the ozone catalytic oxidation system equipped with an electrochemical catalytic reactor achieved a COD removal rate exceeding 91% in 60 minutes, compared to approximately 60% for a conventional ozone catalytic oxidation process using activated carbon as a catalyst. This significantly improved catalytic efficiency. Furthermore, the electrochemical-catalytic reactor of this utility model boasts advantages such as simple structure, easy operation, and low cost, and has broad market application prospects and commercial value. BRIEF DESCRIPTION OF THE DRAWINGS
[0016] In order to more clearly illustrate the technical solutions of the implementation methods of the present application, the following is a brief introduction to the drawings required for use in the implementation methods. It should be understood that the following drawings only show certain embodiments of the present application and therefore should not be regarded as limiting the scope. For ordinary technicians in this field, other relevant drawings can be obtained based on these drawings without paying any creative work.
[0017] Figure 1 This is a schematic structural diagram of an in-situ hydrogen peroxide production-catalytic reaction device provided in an embodiment of the present application;
[0018] Figure 2 A schematic diagram of the internal structure of the in-situ hydrogen peroxide generation-catalytic reaction device provided in an embodiment of the present application;
[0019] Figure 3 A schematic side view of the structure of an in-situ hydrogen peroxide generation-catalytic reaction device provided in an embodiment of the present application;
[0020] Figure 4 A schematic structural diagram of the hydrogen peroxide-catalytic reaction data provided in the embodiment of the present application.
[0021] In the figure: 1-box; 2-top cover; 3-glass sand core board; 4-g-C3N4 / PVP / GF cathode; 5-SnO2-RuO2 / Ti anode; 6-air inlet; 7-aeration head; 8-cathode power connection; 9-anode power connection; 10-water inlet; 11-air outlet; 12-water outlet. DETAILED DESCRIPTION
[0022] The technical solutions in the embodiments of the present application will be clearly and completely described below in conjunction with the drawings in the embodiments of the present application. Obviously, the described embodiments are only part of the embodiments of the present application, rather than all the embodiments.
[0023] Example:
[0024] See also Figure 1 、 Figure 2 、 Figure 3 , an in-situ hydrogen peroxide generation-catalytic reaction device, including a box body 1 and a top cover 2 installed on the top of the box body 1.
[0025] The housing 1 is made of corrosion-resistant, high-strength materials, ensuring the stability and durability of the device during long-term operation. Its interior provides convenient installation for other components. The top cover 2 is tightly fitted to the housing 1 via a sealing ring and secured with connecting plates and bolts, ensuring a tight seal within the device to prevent gas and liquid leakage. Furthermore, the top cover 2 is easily removable for maintenance and cleaning of the interior of the housing 1.
[0026] See also Figure 1 、 Figure 2 、 Figure 3 、 Figure 4 A catalytic reaction device for in-situ production of hydrogen peroxide, comprising a plurality of glass sand core plates 3 arranged at equal intervals inside a box body 1, four g-C3N4 / PVP / GF cathodes 4 and three SnO2-RuO2 / Ti anodes 5 being sequentially installed between the plurality of glass sand core plates 3 and the box body 1, four air inlets 6 being arranged at equal intervals on the side wall of the box body 1, and four aeration heads 7 being arranged at equal intervals on the inner bottom, the four air inlets 6 being respectively interconnected with the air inlet ends of the four aeration heads 7, and the four aeration heads 7 being respectively located at the bottom of the four g-C3N4 / PVP / GF cathodes 4; four cathode power connection points 8 being arranged at equal intervals on the side wall of the box body 1; three anode power connection points 9 being arranged at equal intervals on the other side of the box body 1; a plurality of water inlets 10 being arranged at equal intervals on the bottom side of the box body 1; an air outlet 11 being arranged on the top of the top cover 2; and a water outlet 12 being arranged on the side wall of the top cover 2.
[0027] A number of glass sand core plates 3 are arranged at equal intervals inside the box 1 to serve as support and separation layers for the reaction medium and to promote uniform distribution of gas and liquid.
[0028] Four g-C3N4 / PVP / GF cathodes 4 and three SnO2-RuO2 / Ti anodes 5 are sequentially installed between the glass sand core plate 3 and the housing 1. The materials and arrangement of these electrodes are optimized to improve the efficiency of hydrogen peroxide production and the effectiveness of the catalytic reaction. The cathodes primarily function to electrochemically reduce O2 to H2O2, while the anodes primarily function to electrochemically oxidize and degrade pollutants.
[0029] Four air inlets 6 are evenly spaced on the sidewall of the box 1 for introducing gases required for the reaction, such as oxygen. Four aeration heads 7 are evenly spaced on the bottom of the box 1. The air inlet end of each aeration head 7 is interconnected with the corresponding air inlet 6 to ensure that the gas can be evenly and effectively dispersed into the reaction medium, especially near the cathode located below it.
[0030] Four cathode connections 8 are evenly spaced on the sidewall of the box 1, electrically connected to the four g-C3N4 / PVP / GF cathodes 4 to provide the current required for the electrochemical reaction. Three anode connections 9 are evenly spaced on the other side of the box 1, connected to the three SnO2-RuO2 / Ti anodes 5, also to provide the current required for the electrochemical reaction.
[0031] A plurality of water inlets 10 are provided at equal intervals on the bottom of the box body 1 , and each water inlet 10 is provided with a connecting pipe for introducing wastewater to be treated.
[0032] A gas outlet 11 is provided on the top of the top cover 2 and is provided with an exhaust valve for exhausting gases generated during the reaction, such as unreacted oxygen and generated hydrogen peroxide vapor.
[0033] A water outlet 12 is provided on the side wall of the top cover 2 and a peristaltic pump is installed to control the outflow speed and flow rate of the liquid after the reaction.
[0034] Among them, the electrochemical-catalytic reactor of this utility model includes components such as a reactor cavity, an electrode area, an aeration head and a peristaltic pump. The reactor cavity is made of organic glass, and multiple electrode slots are set on both sides of the inner wall of the reactor in the electrode area, which can be used to install anode electrodes and cathode electrodes of different sizes and quantities. The main function of the cathode is to electrochemically reduce O2 to generate H2O2, and the main function of the anode is to electrochemically oxidize and degrade pollutants. The oxygen in the air introduced by the aeration head produces hydrogen peroxide through electrochemical action between the anode and the cathode. Under the action of the peristaltic pump, wastewater from the external water storage tank enters the electrochemical-catalytic reactor from the water inlet, and flows out from the water outlet carrying the H2O2 generated by the electrode.
[0035] It should be noted that the specific model and specifications of the aeration head 7 need to be selected and determined according to the actual specifications of the device, and the specific selection calculation method adopts the existing technology in this field, so it will not be described in detail.
[0036] The power supply and principle of the cathode power connection point 8 and the anode power connection point 9 are clear to those skilled in the art and will not be described in detail here.
[0037] It will be apparent to those skilled in the art that the present application is not limited to the details of the exemplary embodiments described above, and that the present application can be implemented in other specific forms without departing from the spirit or essential characteristics of the present application. Therefore, the embodiments should be considered in all respects as illustrative and non-restrictive, and the scope of the present application is defined by the appended claims, not the foregoing description, and all variations within the meaning and range of equivalents of the claims are intended to be included therein. Any reference sign in a claim should not be construed as limiting the claim to which it relates.
Claims
1. An in-situ hydrogen peroxide generation-catalytic reaction device, comprising a housing (1) and a top cover (2) mounted on the top of the housing (1), characterized in that: A plurality of glass sand core plates (3) are arranged at equal intervals inside the box (1), and four g-C3N4 / PVP / GF cathodes (4) and three SnO2-RuO2 / Ti anodes (5) are sequentially installed between the plurality of glass sand core plates (3) and the box (1). Four air inlets (6) are opened at equal intervals on the side wall of the box (1), and four aeration heads (7) are arranged at equal intervals on the inner bottom. The four air inlets (6) are respectively connected to the air inlet ends of the four aeration heads (7), and the four aeration heads (7) are respectively located at the bottom of the four g-C3N4 / PVP / GF cathodes (4).
2. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 1, characterized in that: Four cathode power connection points (8) are provided at equal intervals on the side wall of the box (1), and the four cathode power connection points (8) are electrically connected to the four g-C3N4 / PVP / GF cathodes (4) respectively.
3. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 2, characterized in that: Three anode power connection points (9) are provided at equal intervals on the other side of the box (1), and the three anode power connection points (9) are respectively connected to the three SnO2-RuO2 / Ti anode (5) batteries.
4. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 3, characterized in that: A plurality of water inlets (10) are provided at equal intervals on the bottom side of the box body (1), and a plurality of the water inlets (10) are provided with connecting pipes.
5. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 4, characterized in that: An air outlet (11) is provided at the top of the top cover (2), and an exhaust valve is provided at the air outlet (11).
6. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 5, characterized in that: A water outlet (12) is provided on the side wall of the top cover (2), and a peristaltic pump is installed at the water outlet (12).
7. The in-situ hydrogen peroxide generation-catalytic reaction device according to claim 6, characterized in that: A sealing ring is provided between the box body (1) and the top cover (2), and the edges are provided with connecting plates and are connected by bolts.