Large multi-layer plate frame type electrocatalytic nitrogen synthesis ammonia electrolytic cell and application thereof
The design of a large-scale multi-layer plate-and-frame electrocatalytic nitrogen-to-ammonia electrolyzer solves the problems of insufficient nitrogen diffusion and uneven electrode contact, achieving efficient nitrogen conversion and low-carbon ammonia synthesis, which is suitable for green chemical plants and carbon neutrality projects.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- HUANENG POWER INT INC YINGKOU POWER PLANT
- Filing Date
- 2026-03-06
- Publication Date
- 2026-05-29
AI Technical Summary
The existing electrolyzer has poor structural design, resulting in insufficient diffusion of nitrogen on the electrode surface, inability of reactants to effectively contact the active sites of the catalyst, unreasonable flow channel design, lack of turbulence enhancement mechanism, uneven contact between the electrode surface and the electrolyte, mixing of ammonia generated by the reaction with unreacted gases, high separation and purification costs, poor sealing of the electrolyzer, easy leakage or cross-contamination of gases, and uneven current density.
It adopts a large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer, including anode and cathode components, using hollow stainless steel metal plates and transparent acrylic plates, with built-in serpentine flow channels and gas channels, optimized flow channel design, transparent acrylic plates allowing real-time observation of bubble behavior, multi-layer sealing gaskets to ensure sealing, snap-fit fixed electrodes, and modular component design for easy assembly and maintenance.
It improves the diffusion rate of nitrogen on the electrode surface, ensures that the reactants are in full contact with the catalyst, reduces bubble accumulation, improves catalyst utilization, prevents leakage and cross-contamination of gases, improves Faraday efficiency and system stability, and reduces carbon emissions in the ammonia synthesis process.
Smart Images
Figure CN122105434A_ABST
Abstract
Description
Technical Field
[0001] This invention relates to the field of electrolytic cell technology, specifically to a large-scale multilayer plate-and-frame electrocatalytic nitrogen-to-ammonia electrolytic cell and its application. Background Technology
[0002] Ammonia synthesis is an indispensable chemical raw material in agriculture and industry, widely used in fertilizer production, energy storage, and chemical manufacturing. Traditionally, ammonia synthesis has primarily relied on the Haber-Bosch process, which has been the mainstream industrial method since its invention in the early 20th century. The Haber-Bosch process produces ammonia by reacting nitrogen and hydrogen on an iron-based catalyst under high temperature (400-500℃) and high pressure (15-30MPa) conditions. While this method is highly efficient, it has significant drawbacks: the reaction requires maintaining high temperature and pressure, consuming 1-2% of global energy consumption, and relying on fossil fuels as a hydrogen source; the production process also generates large amounts of greenhouse gases (such as carbon dioxide), exacerbating climate change.
[0003] With the increasing global demand for sustainable development and clean energy, the development of technologies for efficient ammonia synthesis under mild conditions has become a research hotspot. Electrocatalytic nitrogen-to-ammonia (eNRR) technology has emerged, utilizing electrical energy (such as from solar or wind power) to directly reduce nitrogen to ammonia at ambient temperature and pressure. However, eNRR technology is still in the laboratory stage, and its industrial application faces a core challenge—poor electrolyzer structural design, with specific defects as follows:
[0004] First, existing electrolyzers often employ simple flat plate or single-chamber designs, resulting in insufficient diffusion of nitrogen on the electrode surface, which prevents reactants from effectively contacting the active sites of the catalyst. The flow channel design is unreasonable, lacking a turbulence enhancement mechanism, and the gas has low solubility in the electrolyte, easily forming a concentration gradient.
[0005] Second, the interface between the electrode surface and the electrolyte is uneven, with some areas over-reacting and others idle, resulting in low catalyst utilization, unstable electrode fixing, and easy displacement or deformation; the electrolyte distribution is uneven, with dead zones.
[0006] Third, the ammonia gas produced by the reaction mixes with unreacted nitrogen gas and byproducts (such as hydrogen gas), making separation and purification costly; at the same time, bubbles accumulate on the electrode surface, blocking the reaction interface and causing "gas blockage".
[0007] Fourth, the assembly method is simple (such as single bolt fixing) and lacks multi-layer sealing design, which makes the electrolytic cell poorly sealed, resulting in leakage or cross-contamination of gas. The concentration of charging points causes uneven current density.
[0008] In view of this, the present invention proposes a large-scale multilayer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer and its application. Summary of the Invention
[0009] This invention proposes a large-scale multilayer plate-and-frame electrocatalytic nitrogen ammonia synthesis electrolyzer and its application, which solves the problem in the prior art where insufficient diffusion of nitrogen on the electrode surface leads to the inability of reactants to effectively contact the active sites of the catalyst.
[0010] The technical solution of the present invention is as follows: a large multilayer plate and frame electrocatalytic nitrogen synthesis ammonia electrolyzer, comprising an anode assembly, a proton exchange membrane and a cathode assembly, wherein the proton exchange membrane is disposed between the anode assembly and the cathode assembly;
[0011] The anode assembly includes a first stainless steel plate, a first sealing gasket is bonded to one side of the first stainless steel plate, a first acrylic plate is fixedly connected to one side of the first sealing gasket, an anode counter electrode is fixedly connected to the inner side of the first acrylic plate, a second sealing gasket is fixedly connected to the outer side of the first acrylic plate, and one side of the second sealing gasket is bonded to a proton exchange membrane.
[0012] The cathode assembly includes a second stainless steel metal plate, a third sealing gasket is bonded to one side of the second stainless steel metal plate, a second acrylic plate is fixedly connected to one side of the third sealing gasket, a cathode working electrode is fixedly connected to the inner side of the second acrylic plate, a fourth sealing gasket is bonded to the outer side of the second acrylic plate, and one side of the fourth sealing gasket is bonded to the proton exchange membrane.
[0013] Preferably, both the first stainless steel plate and the second stainless steel plate have hollow internal structures, and their internal structures are identical.
[0014] Preferably, the first stainless steel metal plate has a first liquid inlet at its top and a first liquid outlet at its bottom.
[0015] Preferably, a side plate is fixedly connected to one side of the first stainless steel metal plate, and the side plate has a plurality of through grooves evenly distributed along the vertical direction.
[0016] Preferably, the top of the first acrylic plate is provided with an anode outlet for discharging oxygen, and the inner side of the first acrylic plate is provided with a first channel communicating with the anode outlet.
[0017] Preferably, a first retainer is fixedly connected to the inner side of the first channel, and the anode electrode is snapped into the inner side of the first retainer.
[0018] Preferably, the second stainless steel metal plate has a second liquid inlet at its top and a second liquid outlet at its bottom.
[0019] Preferably, the top of the second acrylic plate is provided with a cathode inlet for introducing nitrogen gas, the bottom of the second acrylic plate is provided with a cathode outlet for discharging nitrogen gas, and a second channel is provided on the inner side of the second acrylic plate, wherein the cathode inlet and the cathode outlet are both connected to the second channel.
[0020] Preferably, a second retainer is fixedly connected to the inner side of the second channel, and the cathode working electrode is snapped into the inner side of the second retainer.
[0021] The present invention also provides an application of a large-scale multilayer plate-and-frame electrocatalytic nitrogen ammonia synthesis electrolyzer, which replaces the traditional Haber-Bosch process, is driven by renewable energy, and makes the carbon emissions of the ammonia synthesis process zero; the application scenarios include green plants or carbon neutrality projects that meet the ISO 14000 standard.
[0022] The working principle and beneficial effects of this invention are as follows:
[0023] 1. The first and second stainless steel metal plates have hollow internal structures, forming built-in serpentine flow channels, which, combined with sealing gaskets (such as the first sealing gasket), enhance turbulence. The second channel on the cathode side is directly connected to the cathode inlet, allowing nitrogen to diffuse linearly. By optimizing the flow channel design and gas-liquid flow path, the diffusion rate of nitrogen on the electrode surface is significantly improved, ensuring that the reactants fully contact the active sites of the catalyst. This reduces nitrogen mass transfer resistance, increases the ammonia synthesis reaction rate, and greatly improves the Faraday efficiency (electron utilization efficiency).
[0024] 2. The first and second acrylic plates are made of transparent material and have built-in gas channels (such as the first and second channels). The gas outlets at the anode and cathode have optimized the gas discharge path. The transparent acrylic plate design allows operators to observe the bubble behavior and reaction interface in real time and adjust the airflow or electrolyte flow in a timely manner to prevent "gas blockage" caused by bubble accumulation. This design reduces reaction interruption and downtime and improves the stability of continuous operation.
[0025] 3. The anode counter electrode and the cathode working electrode are fixed by the first and second clamps respectively to prevent displacement; the hollow metal plate and hollow structure ensure uniform distribution of electrolyte, and the optimized electrode fixing method and fluid distribution make the electrode surface in uniform contact with the electrolyte, avoiding excessive local reaction or idleness, and improving catalyst utilization.
[0026] 4. The first, second, third, and fourth sealing gaskets form a multi-layer sealing barrier. The proton exchange membrane isolates the anode and cathode electrolytes. The multi-layer sealing gasket design effectively prevents liquid and gas leakage, ensures anode and cathode isolation, and improves system safety.
[0027] 5. The through slots on the side plates simplify the bolt fixing and alignment process; the components are quickly assembled by snap-fit and adhesive; the multi-layer plate frame design can be stacked horizontally or vertically; the modular stacking structure and standardized components make the electrolytic cell easy to scale up to industrial scale while simplifying the maintenance process. Attached Figure Description
[0028] The present invention will now be described in further detail with reference to the accompanying drawings and specific embodiments.
[0029] Figure 1 This is a schematic diagram of the structure of a large multilayer plate-and-frame electrocatalytic nitrogen-to-ammonia electrolyzer according to the present invention.
[0030] Figure 2 This is an exploded view of a large multilayer plate-and-frame electrocatalytic nitrogen-to-ammonia electrolyzer according to the present invention.
[0031] Figure 3 This is a schematic diagram of the anode assembly of the present invention;
[0032] Figure 4 This is a schematic diagram of the structure of the first stainless steel metal plate of the present invention;
[0033] Figure 5 This is a schematic diagram of the internal structure of the first acrylic plate of the present invention;
[0034] Figure 6 This is a schematic diagram of the cathode assembly of the present invention;
[0035] Figure 7 This is a schematic diagram of the internal structure of the second acrylic plate of the present invention.
[0036] In the diagram: 10, Anode assembly; 101, First stainless steel plate; 102, First liquid inlet; 103, First liquid outlet; 104, First sealing gasket; 105, First acrylic plate; 106, Anode counter electrode; 107, Second sealing gasket; 108, First channel; 109, First mounting bracket; 100, Anode outlet; 10a, Side plate; 10b, Through groove; 20, Proton exchange membrane; 30, Cathode assembly; 301, Second stainless steel plate; 302, Second liquid inlet; 303, Second liquid outlet; 304, Third sealing gasket; 305, Cathode working electrode; 306, Second acrylic plate; 307, Fourth sealing gasket; 308, Second channel; 309, Second mounting bracket; 300, Cathode inlet; 30a, Cathode outlet. Detailed Implementation
[0037] The technical solutions of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those of ordinary skill in the art without creative effort are within the scope of protection of the present invention.
[0038] like Figures 1 to 7 As shown, this embodiment proposes a large-scale multilayer plate and frame electrocatalytic nitrogen synthesis ammonia electrolyzer, including an anode assembly 10, a proton exchange membrane 20 and a cathode assembly 30, with the proton exchange membrane 20 disposed between the anode assembly 10 and the cathode assembly 30.
[0039] The anode assembly 10 includes a first stainless steel plate 101, a first liquid inlet 102 at the top of the first stainless steel plate 101, a first liquid outlet 103 at the bottom of the first stainless steel plate 101, a first sealing gasket 104 bonded to one side of the first stainless steel plate 101, a first acrylic plate 105 fixedly connected to one side of the first sealing gasket 104, an anode counter electrode 106 fixedly connected to the inner side of the first acrylic plate 105, an anode outlet 100 for oxygen extraction at the top of the first acrylic plate 105, a first channel 108 communicating with the anode outlet 100 on the inner side of the first acrylic plate 105, a first retainer 109 fixedly connected to the inner side of the first channel 108, the anode counter electrode 106 being snapped into the inner side of the first retainer 109, and a second sealing gasket 107 fixedly connected to the outer side of the first acrylic plate 105, with one side of the second sealing gasket 107 bonded to the proton exchange membrane 20.
[0040] The cathode assembly 30 includes a second stainless steel plate 301. A second liquid inlet 302 is provided at the top of the second stainless steel plate 301, and a second liquid outlet 303 is provided at the bottom of the second stainless steel plate 301. A third sealing gasket 304 is adhered to one side of the second stainless steel plate 301, and a second acrylic plate 306 is fixedly connected to one side of the third sealing gasket 304. A cathode working electrode 305 is fixedly connected to the inner side of the second acrylic plate 306, and a cathode gas inlet for introducing nitrogen is provided at the top of the second acrylic plate 306. 300. The bottom end of the second acrylic plate 306 is provided with a cathode outlet 30a for discharging nitrogen gas. The inner side of the second acrylic plate 306 is provided with a second channel 308. The cathode inlet 300 and the cathode outlet 30a are both connected to the second channel 308. The inner side of the second channel 308 is fixedly connected with a second bracket 309. The cathode working electrode 305 is clipped into the inner side of the second bracket 309. The outer side of the second acrylic plate 306 is bonded with a fourth sealing gasket 307. One side of the fourth sealing gasket 307 is bonded to the proton exchange membrane 20.
[0041] In this embodiment, the assembly process is as follows:
[0042] First, the anode assembly 10 and the cathode assembly 30 are assembled separately, with the proton exchange membrane 20 placed in the middle. The anode assembly 10 includes a first stainless steel plate 101, a first sealing gasket 104, a first acrylic plate 105, an anode counter electrode 106, and a second sealing gasket 107; the cathode assembly 30 includes a second stainless steel plate 301, a third sealing gasket 304, a second acrylic plate 306, a cathode working electrode 305, and a fourth sealing gasket 307. The assemblies are fixed by adhesive and snap-fit, and finally fastened with bolts to form a sealed structure.
[0043] The operation process is as follows:
[0044] Nitrogen gas is introduced through the cathode inlet 300 and diffuses to the surface of the cathode working electrode 305 through the second channel 308 within the second acrylic plate 306. Under energized conditions, current is introduced through the first stainless steel plate 101 and the second stainless steel plate 301. Nitrogen gas undergoes an electrocatalytic reduction reaction (eNRR) at the cathode to generate ammonia gas (NH3). The remaining nitrogen and ammonia gas are discharged from the cathode outlet 30a. The electrolyte enters through the first inlet 102 and the second inlet 302, flows through the anode and cathode regions respectively, carrying away reaction products and heat, and is then discharged from the first outlet 103 and the second outlet 303, achieving continuous circulation. The proton exchange membrane 20 allows protons (H⁺) to migrate from the anode side to the cathode side, maintaining charge balance. On the anode electrode 106, water undergoes an oxidation reaction to generate oxygen O2. The oxygen is discharged from the anode outlet 100 through the first channel 108 in the first acrylic plate 105. The transparent acrylic plate, the first acrylic plate 105, and the second acrylic plate 306 allow for real-time observation of bubble behavior, enabling timely adjustment of airflow or electrolyte flow to avoid gas blockage. The multi-layer plate frame structure is compact, the sealing gasket enhances gas-liquid turbulence, improves nitrogen diffusion efficiency, and the proton exchange membrane 20 isolates the anode and cathode electrolytes to prevent cross-contamination. The transparent acrylic plate design enables real-time monitoring and reduces downtime.
[0045] The anode counter electrode 106 and the cathode working electrode 305 are respectively engaged by the first retainer 109 and the second retainer 309 to ensure that the electrode positions are fixed and to avoid uneven reaction caused by displacement. The retainer design allows for quick electrode replacement and adaptation to different catalysts. The first channel 108 and the second channel 308 optimize the gas flow path and reduce resistance. For example, the cathode inlet 300 is directly connected to the second channel 308, which enables linear diffusion of nitrogen and improves utilization.
[0046] In a further preferred embodiment of the present invention, both the first stainless steel metal plate 101 and the second stainless steel metal plate 301 have hollow internal structures, and their internal structures are the same.
[0047] In this embodiment, a built-in flow channel is formed inside the hollow metal plate. When the electrolyte flows in from the inlet (such as the first inlet 102), eddies and turbulence are generated in the hollow cavity, prolonging the residence time and ensuring sufficient contact between the electrolyte and the electrode surface. The hollow structure, together with the first sealing gasket 104, ensures that the fluid is evenly distributed throughout the entire electrode area, avoiding excessively high or low local concentrations. For example, with the assistance of the hollow plate, nitrogen gas on the cathode side can diffuse more easily to the active sites of the cathode working electrode 305. The hollow cavity serves as a heat dissipation channel, dissipating the heat of reaction, maintaining temperature stability, preventing overheating that could lead to catalyst deactivation, and ensuring uniform fluid distribution to maintain consistent current density, improve catalyst utilization, and extend electrode life.
[0048] In a further preferred embodiment of the present invention, a side plate 10a is fixedly connected to one side of the first stainless steel metal plate 101, and a plurality of through grooves 10b are provided on the side plate 10a that are equidistantly distributed in the vertical direction.
[0049] In this embodiment, the through-slot 10b serves as a channel for bolts or fasteners, simplifying the alignment and fastening process when multiple layers are stacked, and ensuring the precise positioning of each component (such as acrylic plates and gaskets). The through-slot 10b can guide the bypass flow of electrolyte or gas, preventing the formation of dead zones. For example, under high pressure conditions, the through-slot allows for partial fluid diversion, reducing the pressure in the main channel and enhancing system stability.
[0050] This invention also provides an application of a large-scale multilayer plate-and-frame electrocatalytic nitrogen ammonia synthesis electrolyzer, which replaces the traditional Haber-Bosch process and is driven by renewable energy, making the carbon emissions of the ammonia synthesis process zero; application scenarios include green plants or carbon neutrality projects that meet ISO 14000 standards.
[0051] The above are merely preferred embodiments of the present invention and are not intended to limit the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the protection scope of the present invention.
Claims
1. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen-to-ammonia electrolyzer, characterized in that, It includes an anode assembly (10), a proton exchange membrane (20), and a cathode assembly (30), wherein the proton exchange membrane (20) is disposed between the anode assembly (10) and the cathode assembly (30); The anode assembly (10) includes a first stainless steel metal plate (101), a first sealing gasket (104) is bonded to one side of the first stainless steel metal plate (101), a first acrylic plate (105) is fixedly connected to one side of the first sealing gasket (104), an anode counter electrode (106) is fixedly connected to the inner side of the first acrylic plate (105), a second sealing gasket (107) is fixedly connected to the outer side of the first acrylic plate (105), and one side of the second sealing gasket (107) is bonded to the proton exchange membrane (20). The cathode assembly (30) includes a second stainless steel metal plate (301), a third sealing gasket (304) is bonded to one side of the second stainless steel metal plate (301), a second acrylic plate (306) is fixedly connected to one side of the third sealing gasket (304), a cathode working electrode (305) is fixedly connected to the inner side of the second acrylic plate (306), a fourth sealing gasket (307) is bonded to the outer side of the second acrylic plate (306), and one side of the fourth sealing gasket (307) is bonded to the proton exchange membrane (20).
2. The large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 1, characterized in that, Both the first stainless steel metal plate (101) and the second stainless steel metal plate (301) have hollow internal structures, and their internal structures are the same.
3. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 2, characterized in that, The first stainless steel metal plate (101) has a first liquid inlet (102) at its top end and a first liquid outlet (103) at its bottom end.
4. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 3, characterized in that, A side plate (10a) is fixedly connected to one side of the first stainless steel metal plate (101), and a plurality of through slots (10b) are provided on the side plate (10a) and distributed at equal intervals along the vertical direction.
5. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 3, characterized in that, The top of the first acrylic plate (105) is provided with an anode outlet (100) for discharging oxygen, and the inner side of the first acrylic plate (105) is provided with a first channel (108) communicating with the anode outlet (100).
6. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 5, characterized in that, A first card holder (109) is fixedly connected to the inner side of the first channel (108), and the anode electrode (106) is snapped into the inner side of the first card holder (109).
7. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 2, characterized in that, The second stainless steel metal plate (301) has a second liquid inlet (302) at its top end and a second liquid outlet (303) at its bottom end.
8. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 7, characterized in that, The second acrylic plate (306) has a cathode inlet (300) for introducing nitrogen gas at its top end and a cathode outlet (30a) for discharging nitrogen gas at its bottom end. A second channel (308) is provided on the inner side of the second acrylic plate (306). The cathode inlet (300) and cathode outlet (30a) are both connected to the second channel (308).
9. A large-scale multi-layer plate-and-frame electrocatalytic nitrogen synthesis ammonia electrolyzer according to claim 8, characterized in that, The inner side of the second channel (308) is fixedly connected to a second card holder (309), and the cathode working electrode (305) is snapped into the inner side of the second card holder (309).
10. An application of the large-scale multilayer plate-and-frame electrocatalytic nitrogen ammonia synthesis electrolyzer according to claim 9, wherein the electrolyzer replaces the traditional Haber-Bosch process, is driven by renewable energy, and achieves zero carbon emissions in the ammonia synthesis process; application scenarios include green plants or carbon neutrality projects that comply with ISO 14000 standards.