Electrocatalytic ammonia synthesis device

Abstract

The electrocatalytic ammonia synthesis device comprises a plurality of polar plates and electrolyte plates which are sequentially stacked, each polar plate is provided with an anode side and a cathode side which are oppositely arranged, a proton exchange membrane is arranged between the electrolyte plates and the anode sides of the polar plates, and gas diffusion electrodes are arranged between the electrolyte plates and the cathode sides of the polar plates. Wherein each polar plate comprises a first cavity opening area and a first flow field area which are communicated with each other, each electrolyte plate comprises a second cavity opening area and a second flow field area which are independent from each other, and the first cavity opening area is communicated with the second cavity opening area, so that the second cavity opening area of any electrolyte plate can be used as a transmission channel between the first cavity opening areas of two adjacent polar plates; the distribution uniformity of reaction gas in the electrocatalytic ammonia synthesis device is improved, and the reaction stability in each reaction area is improved, so that the reliability and the reaction efficiency of the electrocatalytic ammonia synthesis device in the working process are improved, and the total yield of ammonia gas can be improved; and the electrocatalytic ammonia synthesis device can meet the industrialization requirement.

Description

Technical Field

[0001] This application relates to the field of electrochemistry technology, in particular to an electrocatalytic ammonia synthesis device. Background Art

[0002] Electrocatalytic ammonia synthesis is a technology that converts hydrogen (H 2 ) and nitrogen (N 2 ) into ammonia (NH 3 ) through an electrochemical method. It can be carried out under normal temperature and pressure conditions and is used to replace the traditional Haber-Bosch ammonia synthesis process, thereby solving the problems of high energy consumption and large carbon emissions in the traditional process.

[0003] In the prior art, electrocatalytic ammonia synthesis devices mainly work in an intermittent ammonia synthesis mode. Although they can meet the research needs of laboratories, they cannot achieve continuous production of ammonia, resulting in the inability of existing electrocatalytic ammonia synthesis devices to meet industrial requirements. Summary of the Utility Model

[0004] In view of this, this application provides an electrocatalytic ammonia synthesis device to solve the technical problem that the electrocatalytic ammonia synthesis device in the prior art cannot meet industrial requirements.

[0005] This application provides an electrocatalytic ammonia synthesis device, which includes a plurality of electrode plates and a plurality of electrolyte plates. The plurality of electrode plates and the plurality of electrolyte plates are stacked in sequence along a first direction. Each of the electrode plates has an anode side and a cathode side arranged oppositely. A proton exchange membrane is further arranged between each of the electrolyte plates and the anode side of each of the electrode plates, and a gas diffusion electrode is further arranged between each of the electrolyte plates and the cathode side of each of the electrode plates.

[0006] Wherein, the electrode plate includes a first cavity area and a first flow field area that are communicated with each other, the electrolyte plate includes a second cavity area and a second flow field area that are independent of each other, and the first cavity area is communicated with the second cavity area.

[0007] In the embodiments of the present application, the first cavity regions of each electrode plate are communicated with the first flow field regions and are also communicated with the second cavity regions of the adjacent electrolyte plates, so that the second cavity regions of each electrolyte plate can serve as a transmission channel between the first cavity regions of the adjacent electrode plates. This ensures that after the reaction gas flows into the electrocatalytic ammonia synthesis device, it can flow into the first cavity regions of each electrode plate along the first direction and then into the first flow field regions of each electrode plate for reaction, which is conducive to improving the uniformity of the distribution of the reaction gas in the electrocatalytic ammonia synthesis device, enabling the reaction to occur simultaneously in each reaction region during the operation of the electrocatalytic ammonia synthesis device, and facilitating the improvement of the overall working efficiency of the electrocatalytic ammonia synthesis device and the production of ammonia.

[0008] Meanwhile, the second cavity regions of each electrolyte plate are set to be independent of the second flow field regions, which can reduce the possibility of the reaction gas leaking into the second flow field regions during the flow process, improve the stability and safety of the reaction in the third reaction region, and contribute to enhancing the reliability of the electrocatalytic ammonia synthesis device during operation.

[0009] Therefore, in this embodiment, multiple electrode plates and multiple electrolyte plates are stacked in sequence along the first direction to form an electrocatalytic ammonia synthesis device, which is conducive to improving the integration degree of the electrocatalytic ammonia synthesis device. By setting the first cavity regions and the first flow field regions of each electrode plate to be communicated with each other, the second cavity regions and the second flow field regions of each electrolyte plate to be independent of each other, and the first cavity regions and the second cavity regions of the adjacent electrode plates and electrolyte plates to be communicated with each other, the second cavity region of any electrolyte plate can serve as a transmission channel between the first cavity regions of the adjacent two electrode plates, which is conducive to improving the uniformity of the distribution of the reaction gas in the electrocatalytic ammonia synthesis device and enhancing the stability of the reaction in each reaction region. Thus, it is beneficial to improve the reliability and reaction efficiency of the electrocatalytic ammonia synthesis device during operation, and further increase the total output of ammonia, enabling the electrocatalytic ammonia synthesis device to meet the industrial requirements.

[0010] In a possible implementation manner, both the first cavity region and the second cavity region include a hydrogen inlet, a hydrogen outlet, a nitrogen inlet, and a nitrogen outlet. Along the second direction, the hydrogen inlet and the hydrogen outlet are diagonally distributed with respect to each flow field region, the nitrogen inlet and the nitrogen outlet are diagonally distributed with respect to each flow field region, and the hydrogen inlet is adjacent to the nitrogen outlet, and the nitrogen inlet is adjacent to the hydrogen outlet.

[0011] In a possible implementation manner, in each of the electrode plates, the first flow field region on the anode side of the electrode plate is communicated with the hydrogen inlet and the hydrogen outlet for flowing hydrogen, and the first flow field region on the cathode side of the electrode plate is communicated with the nitrogen inlet and the nitrogen outlet for flowing nitrogen.

[0012] When the plurality of the electrode plates and the plurality of the electrolyte plates are stacked in sequence along the first direction, the gas pressures on both sides of the electrolyte plate are the same.

[0013] In a possible implementation manner, the gas pressure on the anode side of the electrode plate is P1, and P1 satisfies 50 kPa ≤ P1 ≤ 1000 kPa. The gas pressure on the cathode side of the electrode plate is P2, and P2 satisfies 50 kPa ≤ P2 ≤ 1000 kPa.

[0014] In a possible implementation manner, the flow rate of the hydrogen is V1, the flow rate of the nitrogen is V2, and V1 and V2 satisfy V1 ≥ 2×V2, where V1 satisfies 2 m / s ≤ V1 ≤ 20 m / s, and V2 satisfies 1 m / s ≤ V2 ≤ 10 m / s.

[0015] In a possible implementation manner, the electrolyte plate further includes a third cavity area communicating with the second flow field area. The third cavity area includes at least one electrolyte inlet and at least one electrolyte outlet. The electrolyte inlet and the electrolyte outlet are distributed on both sides of the second flow field area along the third direction.

[0016] In the electrocatalytic ammonia synthesis device, the electrolyte inlets of the electrolyte plates are located on the same side of the electrocatalytic ammonia synthesis device, and the electrolyte outlets of the electrolyte plates are located on the same side of the electrocatalytic ammonia synthesis device.

[0017] In a possible implementation manner, the electrocatalytic ammonia synthesis device further includes a flow splitting device and a flow converging device. The flow splitting device and the flow converging device are distributed on both sides of the electrocatalytic ammonia synthesis device along the third direction. The flow splitting device is communicated with the electrolyte inlets of the electrolyte plates, and the flow converging device is communicated with the electrolyte outlets of the electrolyte plates.

[0018] In a possible implementation manner, the second flow field area includes a plurality of electrolyte flow channels for circulating the electrolyte. The plurality of electrolyte flow channels are spaced apart along the second direction and extend along the third direction. Each of the electrolyte flow channels is a hollow structure, and adjacent electrolyte flow channels are independent of each other.

[0019] In a possible implementation manner, along the first direction, the projection of each of the electrolyte flow channels is linear or curved.

[0020] In a possible implementation manner, along the third direction, the liquid inlet of each of the electrolyte flow channels is communicated with the electrolyte inlet, the liquid outlet of each of the electrolyte flow channels is communicated with the electrolyte outlet, and the flow cross-sectional area of each of the liquid outlets is greater than or equal to the flow cross-sectional area of each of the liquid inlets.

[0021] In a possible implementation, the area of the second flow field region is S1, and S1 satisfies 200 cm 2 ≤ S1 ≤ 500 cm 2 ; the length of each electrolyte flow channel is L, and L satisfies 50 mm ≤ L ≤ 200 mm; the flow cross-sectional area of each electrolyte flow channel is S2, and S2 satisfies 10 mm 2 ≤ S2 ≤ 100 mm 2 ; the distance between adjacent electrolyte flow channels is H, and H satisfies 1 mm ≤ H ≤ 10 mm; the flow velocity of the electrolyte is V3, and V3 satisfies 0.1 m / s ≤ V3 ≤ 5 m / s.

[0022] In a possible implementation, the electrocatalytic ammonia synthesis device includes a plurality of the electrode plates and a plurality of reaction units. The plurality of electrode plates and the plurality of reaction units are stacked in sequence along a first direction. Each reaction unit includes the electrolyte plate, the proton exchange membrane, and the gas diffusion electrode.

[0023] The electrocatalytic ammonia synthesis device further includes two end plates. The two end plates are spaced apart along the first direction. The plurality of electrode plates and the plurality of reaction units are all located between the two end plates. The electrode plates between adjacent reaction units are bipolar plates, and the electrode plates between the end plates and their adjacent reaction units are all monopolar plates.

[0024] In a possible implementation, the electrocatalytic ammonia synthesis device further includes two insulating plates and two current collector plates. The two insulating plates and the two current collector plates are all spaced apart along the first direction. The plurality of electrode plates and the plurality of reaction units are all located between the two current collector plates. The two insulating plates are respectively located between the two current collector plates and the two end plates.

[0025] Along the first direction, the end plates, the insulating plates, and the current collector plates at the same end of the electrocatalytic ammonia synthesis device are all provided with fourth cavity regions. The fourth cavity regions communicate with each other, and the fourth cavity region of the current collector plate communicates with the first cavity region of its adjacent electrode plate.

[0026] It should be understood that the above general description and the following detailed description are only exemplary and do not limit the present application. BRIEF DESCRIPTION OF THE DRAWINGS

[0027] In order to more clearly illustrate the technical solutions of the embodiments of the present application, the drawings required for use in the embodiments will be briefly introduced below. Obviously, the drawings in the following description are only some embodiments of the present application. For those of ordinary skill in the art, other drawings can be obtained based on these drawings without creative efforts.

[0028] Figure 1 is the exploded view of the electrocatalytic ammonia synthesis device provided by this application;

[0029] Figure 2 is Figure 1 the enlarged view of the reaction unit in

[0030] Figure 3 is Figure 2 the structural schematic diagram of the electrolyte plate in an embodiment of

[0031] Explanation of reference numerals:

[0032] 1 - end plate;

[0033] 11 - top plate;

[0034] 12 - bottom plate;

[0035] 2 - insulating plate;

[0036] 21 - first insulating plate;

[0037] 22 - second insulating plate;

[0038] 3 - current collector plate;

[0039] 31 - first current collector plate;

[0040] 32 - second current collector plate;

[0041] 4 - electrode plate;

[0042] 41 - first cavity area;

[0043] 42 - first flow field area;

[0044] 5 - reaction unit;

[0045] 51 - electrolyte plate;

[0046] 511 - second cavity area;

[0047] 511a - hydrogen inlet;

[0048] 511b - hydrogen outlet;

[0049] 511c - nitrogen inlet;

[0050] 511d - nitrogen outlet;

[0051] 512 - second flow field area;

[0052] 512a - electrolyte flow channel;

[0053] 512a1 - liquid inlet;

[0054] 512a2 - liquid outlet;

[0055] 513 - Third cavity area;

[0056] 513a - Electrolyte inlet;

[0057] 513b - Electrolyte outlet;

[0058] 52 - Proton exchange membrane;

[0059] 53 - Gas diffusion electrode;

[0060] 54 - Seal;

[0061] 6 - Fourth cavity area.

[0062] The accompanying drawings here are incorporated into the specification and form a part of this specification, showing embodiments consistent with this application, and are used together with the specification to explain the principles of this application. Detailed implementation manners

[0063] For a better understanding of the technical solutions of this application, the embodiments of this application will be described in detail below with reference to the accompanying drawings.

[0064] It should be clear that the described embodiments are only a part of the embodiments of this application, rather than all of the embodiments. All other embodiments obtained by those of ordinary skill in the art based on the embodiments in this application without creative efforts belong to the scope of protection of this application.

[0065] The terms used in the embodiments of this application are only for the purpose of describing specific embodiments and are not intended to limit this application. The singular forms "a", "the", and "said" 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.

[0066] It should be understood that the term " / and / " used herein is only a relational expression describing associated objects, indicating that there can be three relationships. For example, A and / or B can represent: A alone, both A and B exist simultaneously, and B alone. In addition, the character " / " herein generally represents an "or" relationship between the associated objects before and after.

[0067] The embodiments of this application provide an electrocatalytic ammonia synthesis device, such as Figure 1 , Figure 2 and Figure 3As shown in the figure, the electrocatalytic ammonia synthesis device includes a plurality of electrode plates 4 and a plurality of electrolyte plates 51. The plurality of electrode plates 4 and the plurality of electrolyte plates 51 are stacked in sequence along the first direction x. Each electrode plate 4 has an anode side (not marked in the figure) and a cathode side (not marked in the figure) arranged oppositely. A proton exchange membrane 52 is further provided between each electrolyte plate 51 and the anode side of each electrode plate 4, and a gas diffusion electrode 53 is further provided between each electrolyte plate 51 and the cathode side of each electrode plate 4.

[0068] Among them, the electrode plate 4 includes a first cavity area 41 and a first flow field area 42 that communicate with each other. The electrolyte plate 51 includes a second cavity area 511 and a second flow field area 512 that are independent of each other, and the first cavity area 41 communicates with the second cavity area 511.

[0069] It should be noted that in this application, the thickness direction of the electrolyte plate 51 is set as the first direction x, the length direction of the electrolyte plate 51 is set as the second direction y, and the width direction of the electrolyte plate 51 is set as the third direction z.

[0070] In the embodiment of this application, by stacking a plurality of electrode plates 4 and a plurality of electrolyte plates 51 in sequence along the first direction x, there are two reaction zones between any electrolyte plate 51 and its adjacent two electrode plates 4, that is, the first reaction zone between the electrolyte plate 51 and the anode side of its adjacent electrode plate 4, and the second reaction zone between the electrolyte plate 51 and the cathode side of its other adjacent electrode plate 4. And the inside of the electrolyte plate 51 is used for flowing the electrolyte, so that there is also a third reaction zone inside it. Thus, a structure of one plate and three reaction zones can be formed between any electrolyte plate 51 and its adjacent two electrode plates 4, which is beneficial to improving the integration degree of the electrocatalytic ammonia synthesis device, reducing the overall size of the electrocatalytic ammonia synthesis device, and reducing the production cost of the catalytic ammonia synthesis device.

[0071] Among them, the first cavity area 41 of each electrode plate 4 is set to communicate with the first flow field area 42 and communicate with the second cavity area 511 of its adjacent electrolyte plate 51, so that the second cavity area 511 of each electrolyte plate 51 can be used as a transmission channel between the first cavity areas 41 of the adjacent electrode plates 4, to ensure that after the reaction gas flows into the electrocatalytic ammonia synthesis device, it can flow into the first cavity area 41 of each electrode plate 4 along the first direction x, and then flow into the first flow field area 42 of each electrode plate 4 for reaction. This is beneficial to improving the uniformity of the distribution of the reaction gas in the electrocatalytic ammonia synthesis device, enabling each reaction zone to react simultaneously during the operation of the electrocatalytic ammonia synthesis device, which is beneficial to improving the overall working efficiency of the electrocatalytic ammonia synthesis device and increasing the ammonia production.

[0072] Meanwhile, the second cavity area 511 and the second flow field area 512 of each electrolyte plate 51 are set to be independent of each other, which can reduce the possibility of reaction gas leaking into the second flow field area 512 during the flow process, improve the stability and safety of the reaction in the third reaction area, and is beneficial to improving the reliability of the electrocatalytic ammonia synthesis device during operation.

[0073] Specifically, taking the electrolyte in the electrolyte as lithium mediation and the reaction gases as hydrogen and nitrogen as examples. Hydrogen is used to flow between the electrolyte plate 51 and the anode side of its adjacent plate 4, nitrogen is used to flow between the electrolyte plate 51 and the cathode side of its adjacent plate 4, and the electrolyte mediated by lithium is used to flow in the second flow field area 512. During the operation of the electrocatalytic ammonia synthesis device, hydrogen reacts in the first reaction area to generate protons, and moves towards the second reaction area through the proton exchange membrane 52. The electrolyte reacts in the third reaction area to generate lithium ions, and moves towards the second reaction area, and is reduced to metallic lithium at the gas diffusion electrode 53. Nitrogen reacts with metallic lithium in the second reaction area to generate nitrides and / or nitrogen atoms, and then the nitrides and / or nitrogen atoms react with protons to generate ammonia and lithium ions. Finally, the lithium ions are incorporated into the electrolyte and flow out of the electrocatalytic ammonia synthesis device, and the ammonia and the unreacted nitrogen flow out of the electrocatalytic ammonia synthesis device together.

[0074] Therefore, in this embodiment, the multiple plates 4 and the multiple electrolyte plates 51 are stacked in sequence along the first direction x to form the electrocatalytic ammonia synthesis device, which is beneficial to improving the integration degree of the electrocatalytic ammonia synthesis device. By setting the first cavity area 41 and the first flow field area 42 of each plate 4 to be interconnected, the second cavity area 511 and the second flow field area 512 of each electrolyte plate 51 to be independent of each other, and the first cavity area 41 of the adjacent plate 4 and the second cavity area 511 of the electrolyte plate 51 to be interconnected, the second cavity area 511 of any electrolyte plate 51 can serve as a transmission channel between the first cavity areas 41 of the adjacent two plates 4, which is beneficial to improving the uniformity of the distribution of the reaction gas in the electrocatalytic ammonia synthesis device and improving the stability of the reaction in each reaction area, thereby being beneficial to improving the reliability and reaction efficiency of the electrocatalytic ammonia synthesis device during operation, and further being able to increase the total output of ammonia, so that the electrocatalytic ammonia synthesis device can meet the industrial demand.

[0075] In a possible implementation manner, the electrolyte of the electrolyte can also be calcium mediation.

[0076] In a possible implementation manner, the material of the substrate of the plate 4 is graphite, stainless steel or titanium.

[0077] In a possible implementation manner, the material of the gas diffusion electrode 53 can be stainless steel, titanium, platinum or gold.

[0078] In a specific implementation manner, such asFigure 3 As shown, the electrolyte plate 51 further includes a third cavity area 513 communicating with the second flow field area 512. The third cavity area 513 includes at least one electrolyte inlet 513a and at least one electrolyte outlet 513b. The electrolyte inlet 513a and the electrolyte outlet 513b are distributed on both sides of the second flow field area 512 along the third direction z.

[0079] When a plurality of electrode plates 4 and a plurality of electrolyte plates 51 are sequentially stacked along the first direction x to form an electrocatalytic ammonia synthesis device, the electrolyte inlets 513a of each electrolyte plate 51 are located on the same side of the electrocatalytic ammonia synthesis device, and the electrolyte outlets 513b of each electrolyte plate 51 are located on the same side of the electrocatalytic ammonia synthesis device.

[0080] In the embodiment of the present application, the electrolyte plate 51 further includes a third cavity area 513 communicating with the second flow field area 512. The third cavity area 513 is arranged on both sides of the second flow field area 512 along the third direction z for communicating with a liquid supply device that provides electrolyte.

[0081] Specifically, the third cavity area 513 includes at least one electrolyte inlet 513a and at least one electrolyte outlet 513b, and the electrolyte inlet 513a and the electrolyte outlet 513b are distributed on both sides of the second flow field area 512 along the third direction z, so that the electrolyte can flow into the second flow field area 512 through the electrolyte inlet 513a on one side of the electrolyte plate 51 for reaction and flow out of the second flow field area 512 through the electrolyte outlet 513b on the other side of the electrolyte plate 51. Through such a design, the electrolyte can continuously flow in the second flow field area 512 to ensure the stability of the reaction in each reaction area, so that the electrocatalytic ammonia synthesis device can continuously and stably produce ammonia, which is beneficial to improving the reliability of the electrocatalytic ammonia synthesis device during operation, and further ensuring the working efficiency of the electrocatalytic ammonia synthesis device in industrial applications.

[0082] More specifically, when a plurality of electrode plates 4 and a plurality of electrolyte plates 51 are sequentially stacked along the first direction x to form an electrocatalytic ammonia synthesis device, the electrolyte inlets 513a of each electrolyte plate 51 can be located on the same side of the electrocatalytic ammonia synthesis device, and the electrolyte outlets 513b of each electrolyte plate 51 can be located on the same side of the electrocatalytic ammonia synthesis device, which is beneficial to reducing the complexity of the pipeline connection between the liquid supply device and each electrolyte plate 51, making the overall layout more concise, so as to optimize the space utilization rate of installing the electrocatalytic ammonia synthesis device, and is also beneficial to installing components such as valves, flow meters, and pressure gauges, facilitating the staff to centrally control and monitor the electrocatalytic ammonia synthesis device, so as to improve the stability and reliability of the electrocatalytic ammonia synthesis device during operation.

[0083] In a possible implementation manner, the third cavity region 513 includes a plurality of electrolyte inlets 513a and a plurality of electrolyte outlets 513b. The plurality of electrolyte inlets 513a and the plurality of electrolyte outlets 513b are both distributed at intervals along the second direction y to improve the flow efficiency of the electrolyte, thereby facilitating the promotion of the reaction efficiency in each reaction region, so as to further increase the ammonia production.

[0084] In a specific implementation manner, the electrocatalytic ammonia synthesis device further includes a flow splitting device (not marked in the figure) and a flow converging device (not marked in the figure). The flow splitting device and the flow converging device are distributed on both sides of the electrocatalytic ammonia synthesis device along the third direction z. The flow splitting device is communicated with the electrolyte inlets 513a of each electrolyte plate 51, and the flow converging device is communicated with the electrolyte outlets 513b of each electrolyte plate 51.

[0085] In the embodiment of the present application, by arranging a flow splitting device and a flow converging device on both sides of the electrocatalytic ammonia synthesis device along the third direction z, along the flow direction of the electrolyte, one end of the flow splitting device is communicated with the liquid supply device, and the other end is communicated with the electrolyte inlets 513a of each electrolyte plate 51. One end of the flow converging device is communicated with the electrolyte outlets 513b of each electrolyte plate 51, and the other end is communicated with the liquid supply device.

[0086] Specifically, the flow splitting device can evenly distribute the electrolyte flowing into the electrocatalytic ammonia synthesis device into each electrolyte plate 51, reducing the possibility of local reaction or uneven reaction in the electrocatalytic ammonia synthesis device to ensure the stable production of ammonia. At the same time, the uniform distribution of the electrolyte can improve the uniformity of the electrolyte concentration and temperature in each reaction region to ensure the uniformity of the reaction in each reaction region and reduce the possibility of local overheating of the electrocatalytic ammonia synthesis device, which is beneficial to improving the safety of the electrocatalytic ammonia synthesis device during operation and prolonging the service life of the electrocatalytic ammonia synthesis device.

[0087] Specifically, the flow converging device can collect the electrolyte flowing out of each electrolyte plate 51 for unified detection and replenishment of the electrolyte, and after replenishment, it is uniformly transmitted back to the liquid supply device to realize the recycling of the electrolyte.

[0088] In addition, by arranging the flow splitting device and the flow converging device, the adjustment of the electrolyte in any electrolyte plate 51 can also be realized. For example, components such as valves are arranged on the pipeline between the flow splitting device and each electrolyte plate 51 to control the flow rate, flow velocity, etc. of the electrolyte in the electrolyte plate 51, which is beneficial to further improving the control degree of the reaction in the electrocatalytic ammonia synthesis device by the staff. And when there are a plurality of independent flow channels in the second flow field region 512 of each electrolyte plate 51, the adjustment of the electrolyte in any flow channel can also be realized.

[0089] In a possible implementation manner, at least one of the shunt device and the confluence device can be detachably connected to the electrocatalytic ammonia synthesis device, so as to facilitate the maintenance and transportation of the electrocatalytic ammonia synthesis device.

[0090] In a specific implementation manner, as Figure 3 shown, the second flow field area 512 includes a plurality of electrolyte flow channels 512a for circulating the electrolyte. The plurality of electrolyte flow channels 512a are spaced apart along the second direction y and extend along the third direction z. Each electrolyte flow channel 512a is a hollow structure, and adjacent electrolyte flow channels 512a are independent of each other.

[0091] In the embodiments of the present application, by setting each electrolyte flow channel 512a in the second flow field area 512 as a hollow structure, the first reaction area, the second reaction area and the third reaction area are communicated, so as to facilitate the transmission of reactants such as protons and lithium ions. At the same time, to ensure the stability and reliability of each reaction area during the operation of the electrocatalytic ammonia synthesis device, the electrocatalytic ammonia synthesis device is usually placed along the second direction y. And by setting adjacent electrolyte flow channels 512a to be independent of each other, it can ensure that the electrolyte flowing into the second flow field area 512 flows stably in each electrolyte flow channel 512a, reducing the possibility of cross-flow between adjacent electrolyte flow channels 512a, so as to avoid the electrolyte concentrating under the second flow field area 512 under the action of gravity, thereby further improving the uniformity of the electrolyte distribution in the second flow field area 512 and the uniformity of the reaction between each reaction area. In addition, by setting independent electrolyte flow channels 512a, the overall structural strength of the second flow field area 512 can also be improved, so as to extend the service life of the electrocatalytic ammonia synthesis device.

[0092] In a specific implementation manner, as Figure 3 shown, along the first direction x, the projection of each electrolyte flow channel 512a is linear or curved.

[0093] In the embodiments of the present application, by setting each electrolyte flow channel 512a as a linear structure, it is convenient for processing, which is beneficial to reducing the processing difficulty of each electrolyte flow channel 512a and improving the production efficiency of the electrolyte plate 51. At the same time, the linear electrolyte flow channel 512a can reduce eddy current and friction loss during the flow of the electrolyte, so as to be beneficial to reducing the flow resistance of the electrolyte during the flow process and improving the efficiency of the electrolyte circulating flow. In addition, the curved electrolyte flow channel 512a can extend the flow time of the electrolyte in the second flow field area 512 to promote the full participation of the electrolyte in the reaction, which is beneficial to further improving the reaction efficiency.

[0094] In a specific embodiment, along the third direction z, the liquid inlet 512a1 of each electrolyte flow channel 512a is communicated with the electrolyte inlet 513a, the liquid outlet 512a2 of each electrolyte flow channel 512a is communicated with the electrolyte outlet 513b, and the flow cross-sectional area of each liquid outlet 512a2 is greater than or equal to that of each liquid inlet 512a1.

[0095] In the embodiment of the present application, along the first direction x, the projection of each electrolyte flow channel 512a may also be a gradient structure, that is, along the flow direction of the electrolyte, the flow cross-sectional area of each electrolyte flow channel 512a gradually increases, or the flow cross-sectional area of each electrolytic flow channel 512a first gradually increases and then gradually decreases. When the flow cross-sectional area of each electrolyte flow channel 512a gradually increases along the flow direction of the electrolyte, the flow resistance of the electrolyte during the flow process can be reduced, thereby reducing the pressure drop and further reducing the energy consumption during the circulating flow of the electrolyte. When the flow cross-sectional area of each electrolyte flow channel 512a first gradually increases and then gradually decreases along the flow direction of the electrolyte, the electrolyte can stay in the region where the flow cross-sectional area gradually increases for a longer time to enable the electrolyte to fully participate in the reaction, and then accelerate the flow in the region where the flow cross-sectional area gradually decreases to quickly discharge the electrolyte participating in the reaction, which is beneficial to improving the ammonia production efficiency and the circulation efficiency of the electrolyte.

[0096] In a specific embodiment, the area of the second flow field region 512 is S1, and S1 satisfies 200 cm 2 ≤S1≤500 cm 2 , and S1 may specifically be 200 cm 2 , 210 cm 2 , 220 cm 2 , 230 cm 2 , 240 cm 2 , 250 cm 2 , 260 cm 2 , 270 cm 2 , 280 cm 2 , 290 cm 2 , 300 cm 2 , 310 cm 2 , 320 cm 2 , 330 cm 2 , 340 cm 2 , 350 cm 2 , 360 cm 2 , 370 cm 2 , 380 cm 2 , 390 cm 2 , 400 cm 2 , 410 cm 2 , 420 cm 2, 430 cm 2 , 440 cm 2 , 450 cm 2 , 460 cm 2 , 470 cm 2 , 480 cm 2 , 490 cm 2 , 500 cm 2 etc.

[0097] When the area S1 of the second flow field region 512 satisfies 200 cm 2 ≤ S1 ≤ 500 cm 2 At this time, the area of the second flow field region 512 is moderate, so that the hydrogen, nitrogen and electrolyte flowing into the electrocatalytic ammonia synthesis device can fully react, so as to ensure that while generating more ammonia, the electrocatalytic ammonia synthesis device as a whole has good heat dissipation performance, so as to extend the service life of the electrocatalytic ammonia synthesis device.

[0098] In a specific embodiment, the length of each electrolyte flow channel 512a is L, and L satisfies 50 mm ≤ L ≤ 200 mm. Specifically, L can be 50 mm, 60 mm, 70 mm, 80 mm, 90 mm, 100 mm, 110 mm, 120 mm, 130 mm, 140 mm, 150 mm, 160 mm, 170 mm, 180 mm, 190 mm, 200 mm, etc.

[0099] When the length L of each electrolyte flow channel 512a satisfies 50 mm ≤ L ≤ 200 mm, the length of each electrolyte flow channel 512a is moderate, so that while the electrolyte fully participates in the reaction to generate ammonia, the production cost of the electrolyte plate 51 is reduced, thereby reducing the production cost of the electrocatalytic ammonia synthesis device.

[0100] In a specific embodiment, the cross-sectional flow area of each electrolyte flow channel 512a is S2, and S2 satisfies 10 mm 2 ≤ S2 ≤ 100 mm 2 , S2 can specifically be 10 mm 2 , 11 mm 2 , 13 mm 2 , 15 mm 2 , 17 mm 2 , 19 mm 2 , 20 mm 2 , 21 mm 2 , 23 mm 2 , 25 mm 2 , 27 mm 2 , 29 mm 2 , 30 mm 2 , 31 mm 2 , 33 mm2 , 35 mm 2 , 37 mm 2 , 39 mm 2 , 40 mm 2 , 41 mm 2 , 43 mm 2 , 45 mm 2 , 47 mm 2 , 49 mm 2 , 50 mm 2 , 51 mm 2 , 53 mm 2 , 55 mm 2 , 57 mm 2 , 59 mm 2 , 60 mm 2 , 61 mm 2 , 63 mm 2 , 65 mm 2 , 67 mm 2 , 69 mm 2 , 70 mm 2 , 71 mm 2 , 73 mm 2 , 75 mm 2 , 77 mm 2 , 79 mm 2 , 80 mm 2 , 81 mm 2 , 83 mm 2 , 85 mm 2 , 87 mm 2 , 89 mm 2 , 90 mm 2 , 91 mm 2 , 93 mm 2 , 95 mm 2 , 97 mm 2 , 99 mm 2 , 100 mm 2 etc.

[0101] When the cross-sectional flow area S2 of each electrolyte flow channel 512a satisfies 10 mm 2 ≤ S2 ≤ 100 mm 2 the cross-sectional flow area of each electrolyte flow channel 512a is appropriate, so that the flow velocity of the electrolyte in each electrolyte flow channel 512a is appropriate, so as to improve the generation efficiency of ammonia while the electrolyte fully participates in the reaction.

[0102] In a specific embodiment, the distance between adjacent electrolyte flow channels 512a is H, and H satisfies 1 mm ≤ H ≤ 10 mm. Specifically, H can be 1 mm, 1.2 mm, 1.4 mm, 1.6 mm, 1.8 mm, 2 mm, 2.2 mm, 2.4 mm, 2.6 mm, 2.8 mm, 3 mm, 3.2 mm, 3.4 mm, 3.6 mm, 3.8 mm, 4 mm, 4.2 mm, 4.4 mm, 4.6 mm, 4.8 mm, 5 mm, 5.2 mm, 5.4 mm, 5.6 mm, 5.8 mm, 6 mm, 6.2 mm, 6.4 mm, 6.6 mm, 6.8 mm, 7 mm, 7.2 mm, 7.4 mm, 7.6 mm, 7.8 mm, 8 mm, 8.2 mm, 8.4 mm, 8.6 mm, 8.8 mm, 9 mm, 9.2 mm, 9.4 mm, 9.6 mm, 9.8 mm, 10 mm, etc.

[0103] When the distance H between adjacent electrolyte flow channels 512a satisfies 1 mm ≤ H ≤ 10 mm, the distance between adjacent electrolyte flow channels 512a is appropriate, so as to ensure the overall structural stability of the second flow field area 512 while enabling there to be more and independent electrolyte flow channels 512a in the second flow field area 512, thereby improving the distribution uniformity of the electrolyte and the generation efficiency of ammonia.

[0104] In a specific embodiment, the flow rate of the electrolyte is V3, and V3 satisfies 0.1 m / s ≤ V3 ≤ 5 m / s. Specifically, V3 can be 0.1 m / s, 0.3 m / s, 0.5 m / s, 0.7 m / s, 0.9 m / s, 1 m / s, 1.1 m / s, 1.3 m / s, 1.5 m / s, 1.7 m / s, 1.9 m / s, 2 m / s, 2.1 m / s, 2.3 m / s, 2.5 m / s, 2.7 m / s, 2.9 m / s, 3 m / s, 3.1 m / s, 3.3 m / s, 3.5 m / s, 3.7 m / s, 3.9 m / s, 4 m / s, 4.1 m / s, 4.3 m / s, 4.5 m / s, 4.7 m / s, 4.9 m / s, 5 m / s, etc.

[0105] When the flow rate V3 of the electrolyte satisfies 0.1 m / s ≤ V3 ≤ 5 m / s, the flow rate of the electrolyte flowing in each electrolyte plate 51 is appropriate, so as to carry away more heat during the flow process to reduce the working temperature of each electrolyte plate 51, improve the stability and reliability of each electrolyte plate 51 during the working process, and thus contribute to extending the service life of the electrocatalytic ammonia synthesis device. At the same time, when the electrolyte flows in each electrolyte flow channel 512a at this flow rate, the electrolyte at the end of each electrolyte flow channel 512a still has a high electrolyte concentration, so that the end of each electrolyte flow channel 512a can still participate in the reaction to generate ammonia, which is beneficial to further improving the ammonia generation efficiency.

[0106] In a specific embodiment, the current density in the second flow field region 512 is J, and J satisfies 100 mA / cm 2 ≤ J ≤ 2000 mA / cm 2 , and J can specifically be 100 mA / cm 2 , 200 mA / cm 2 , 300 mA / cm 2 , 400 mA / cm 2 , 500 mA / cm 2 , 600 mA / cm 2 , 700 mA / cm 2 , 800 mA / cm 2 , 900 mA / cm 2 , 1000 mA / cm 2 , 1100 mA / cm 2 , 1200 mA / cm 2 , 1300 mA / cm 2 , 1400 mA / cm 2 , 1500 mA / cm 2 , 1600 mA / cm 2 , 1700 mA / cm 2 , 1800 mA / cm 2 , 1900 mA / cm 2 , 2000 mA / cm 2 etc.

[0107] When the current density J in the second flow field region 512 satisfies 100 mA / cm 2 ≤ J ≤ 2000 mA / cm 2 , it can enable the electrocatalytic ammonia synthesis device to be in a high-power working state, so as to promote the reaction efficiency in each reaction zone and improve the ammonia generation efficiency, while avoiding the possibility of damage to the electrocatalytic ammonia synthesis device due to excessive working temperature.

[0108] In a specific embodiment, as shown in Figure 2 and Figure 3 , the first cavity region 41 and the second cavity region 511 both include a hydrogen inlet 511a, a hydrogen outlet 511b, a nitrogen inlet 511c, and a nitrogen outlet 511d. Along the second direction y, the hydrogen inlet 511a and the hydrogen outlet 511b are distributed diagonally with respect to each flow field region, the nitrogen inlet 511c and the nitrogen outlet 511d are distributed diagonally with respect to each flow field region, and the hydrogen inlet 511a is adjacent to the nitrogen outlet 511d, and the nitrogen inlet 511c is adjacent to the hydrogen outlet 511b.

[0109] In the embodiments of the present application, the cavity areas of the electrode plate 4 and the electrolyte plate 51 both include a hydrogen inlet 511a, a hydrogen outlet 511b, a nitrogen inlet 511c, and a nitrogen outlet 511d, and the projections of each inlet and outlet along the first direction x can overlap, so as to improve the stability of hydrogen, nitrogen, and ammonia during the flow process and reduce the risk of leakage of each gas during the flow process.

[0110] Specifically, on the electrode plate 4, along the second direction y, the hydrogen inlet 511a and the hydrogen outlet 511b are diagonally distributed with respect to the first flow field area 42, the nitrogen inlet 511c and the nitrogen outlet 511d are diagonally distributed with respect to the first flow field area 42, and the hydrogen inlet 511a is adjacent to the nitrogen outlet 511d, and the nitrogen inlet 511c is adjacent to the hydrogen outlet 511b. Taking the hydrogen inlet and outlet as an example, through such a design method, it is beneficial to increase the hydrogen flow rate while extending the flow path of hydrogen, so that hydrogen can be fully diffused to each position in the first flow field area 42, so as to improve the uniformity of the distribution of hydrogen in the first flow field area 42, thereby increasing the proportion of hydrogen participating in the reaction, improving the proton generation efficiency in the first reaction area, and further improving the working efficiency of the electrocatalytic ammonia synthesis device.

[0111] At the same time, during the operation of the electrocatalytic ammonia synthesis device, by setting the flow directions of hydrogen and nitrogen to be opposite, it is beneficial to further promote the reaction efficiency of each reaction area and improve the ammonia generation efficiency.

[0112] In a possible implementation manner, in each electrode plate 4, the first flow field area 42 on the anode side of the electrode plate 4 is communicated with the hydrogen inlet 511a and the hydrogen outlet 511b for flowing hydrogen, and the first flow field area 42 on the cathode side of the electrode plate 4 is communicated with the nitrogen inlet 511c and the nitrogen outlet 511d for flowing nitrogen.

[0113] When a plurality of electrode plates 4 and a plurality of electrolyte plates 51 are stacked in sequence along the first direction x to form an electrocatalytic ammonia synthesis device, the gas pressures on both sides of the electrolyte plate 51 are the same.

[0114] In the embodiments of the present application, since the electrolyte flow channel 512a of the electrolyte plate 51 is a hollow structure, when hydrogen flows on the anode side of the adjacent electrode plate 4 and nitrogen flows on the cathode side of the adjacent electrode plate 4, the possibility of the electrolyte diffusing toward the two side electrode plates 4 along the first direction x during the flow process can be blocked by controlling the gas pressures on both sides of the electrolyte plate 51, so that the electrolyte can be restricted within each electrolyte flow channel 512a, so as to ensure that the reactions in each reaction area can proceed stably.

[0115] Specifically, during the operation of the electrocatalytic ammonia synthesis device, the electrolyte can be restricted within each electrolyte flow channel 512a by controlling the gas pressures on both sides of the electrolyte plate 51 along the first direction x to be the same, so as to improve the stability and reliability of the electrolyte during the flowing process, thereby ensuring the safety of the electrocatalytic ammonia synthesis device during the operation process.

[0116] Meanwhile, a proton exchange membrane 52 is further provided between the electrolyte plate 51 and the anode side of the adjacent plate 4, and a gas diffusion electrode 53 is further provided between the electrolyte plate 51 and the cathode side of the adjacent plate 4. During the operation of the electrocatalytic ammonia synthesis device, the proton exchange membrane 52 and the gas diffusion electrode 53 can also play a role in blocking the diffusion of the electrolyte along the first direction x, which is beneficial to further improving the safety of the electrocatalytic ammonia synthesis device during the operation process.

[0117] In a specific embodiment, the gas pressure on the anode side of the plate 4 is P1, and P1 satisfies 50 kPa ≤ P1 ≤ 1000 kPa.

[0118] In the embodiments of the present application, the gas pressure P1 on the anode side of the plate 4 can specifically be 50 kPa, 70 kPa, 90 kPa, 110 kPa, 130 kPa, 150 kPa, 170 kPa, 190 kPa, 210 kPa, 230 kPa, 250 kPa, 270 kPa, 290 kPa, 310 kPa, 330 kPa, 350 kPa, 370 kPa, 390 kPa, 410 kPa, 430 kPa, 450 kPa, 470 kPa, 490 kPa, 510 kPa, 530 kPa, 550 kPa, 570 kPa, 590 kPa, 610 kPa, 630 kPa, 650 kPa, 670 kPa, 690 kPa, 710 kPa, 730 kPa, 750 kPa, 770 kPa, 790 kPa, 810 kPa, 830 kPa, 850 kPa, 870 kPa, 890 kPa, 910 kPa, 930 kPa, 950 kPa, 970 kPa, 990 kPa, etc.

[0119] When the gas pressure P1 on the anode side of the plate 4 (i.e., the gas pressure of hydrogen) satisfies 50 kPa ≤ P1 ≤ 1000 kPa, the gas pressure on the anode side of the plate 4 is appropriate, which can ensure the concentration of hydrogen in the electrocatalytic ammonia synthesis device, can also limit the diffusion of the electrolyte in the adjacent electrolyte plate 51 along the first direction x towards the direction of the plate 4, and can also avoid excessive air pressure from damaging the sealing effect between the adjacent plates 4 and between the adjacent plates 4 and the electrolyte plate 51. Therefore, while ensuring the stable flow of the electrolyte, the safety and reliability of the electrocatalytic ammonia synthesis device during the operation process can be improved.

[0120] In a specific embodiment, the gas pressure on the cathode side of the electrode plate 4 is P2, and P2 satisfies 50 kPa ≤ P2 ≤ 1000 kPa.

[0121] In the embodiment of the present application, the gas pressure P2 on the cathode side of the electrode plate 4 can specifically be 60 kPa, 80 kPa, 100 kPa, 120 kPa, 140 kPa, 160 kPa, 180 kPa, 200 kPa, 220 kPa, 240 kPa, 260 kPa, 280 kPa, 300 kPa, 320 kPa, 340 kPa, 360 kPa, 380 kPa, 400 kPa, 420 kPa, 440 Pa, 460 kPa, 480 kPa, 500 kPa, 520 kPa, 540 kPa, 560 kPa, 580 kPa, 600 kPa, 620 kPa, 640 kPa, 680 kPa, 700 kPa, 720 kPa, 740 kPa, 760 kPa, 780 kPa, 800 kPa, 820 kPa, 840 kPa, 860 kPa, 880 kPa, 900 kPa, 920 kPa, 940 kPa, 960 kPa, 980 kPa, 1000 kPa, etc.

[0122] When the gas pressure P2 (i.e., the gas pressure of nitrogen) on the cathode side of the electrode plate 4 satisfies 50 kPa ≤ P2 ≤ 1000 kPa, the gas pressure on the cathode side of the electrode plate 4 is moderate, which can ensure the concentration of nitrogen in the electrocatalytic ammonia synthesis device, and can also limit the diffusion of the electrolyte in the adjacent electrolyte plate 51 along the first direction x towards the direction of the electrode plate 4, and can also avoid excessive air pressure from damaging the sealing effect between adjacent electrode plates 4 and between adjacent electrode plates 4 and the electrolyte plate 51, so as to ensure the stable flow of the electrolyte while improving the safety and reliability of the electrocatalytic ammonia synthesis device during operation.

[0123] In a specific embodiment, the flow rate of hydrogen is V1, the flow rate of nitrogen is V2, and V1 and V2 satisfy V1 ≥ 2 × V2, where V1 satisfies 2 m / s ≤ V1 ≤ 20 m / s and V2 satisfies 1 m / s ≤ V2 ≤ 10 m / s.

[0124] In the embodiment of the present application, during the operation of the electrocatalytic ammonia synthesis device, due to the large consumption of hydrogen, by setting the hydrogen flow rate to be at least twice the nitrogen flow rate, it can ensure a relatively high reaction degree in each reaction zone, thereby ensuring the stable and continuous production of ammonia, which is beneficial to improving the stability and reliability of the electrocatalytic ammonia synthesis device during operation.

[0125] Among them, the flow rate V1 of hydrogen can specifically be 2 m / s, 2.5 m / s, 3 m / s, 3.5 m / s, 4 m / s, 4.5 m / s, 5 m / s, 5.5 m / s, 6 m / s, 6.5 m / s, 7 m / s, 7.5 m / s, 8 m / s, 8.5 m / s, 9 m / s, 9.5 m / s, 10 m / s, 10.5 m / s, 11 m / s, 11.5 m / s, 12 m / s, 12.5 m / s, 13 m / s, 13.5 m / s, 14 m / s, 14.5 m / s, 15 m / s, 15.5 m / s, 16 m / s, 16.5 m / s, 17 m / s, 17.5 m / s, 18 m / s, 18.5 m / s, 19 m / s, 19.5 m / s, 20 m / s, etc.

[0126] When the flow rate V1 of hydrogen satisfies 2 m / s ≤ V1 ≤ 20 m / s, the concentration at the hydrogen inlet 511a of each plate 4 can be ensured to be relatively high, so that the reaction on the anode side of each plate 4 can proceed stably, and has a relatively high reaction efficiency, and further the production efficiency of ammonia can be ensured.

[0127] Meanwhile, the flow rate V2 of nitrogen can specifically be 1 m / s, 1.2 m / s, 1.4 m / s, 1.6 m / s, 1.8 m / s, 2 m / s, 3 m / s, 3.2 m / s, 3.4 m / s, 3.6 m / s, 3.8 m / s, 4 m / s, 4.2 m / s, 4.4 m / s, 4.6 m / s, 4.8 m / s, 5 m / s, 5.2 m / s, 5.4 m / s, 5.6 m / s, 5.8 m / s, 6 m / s, 6.2 m / s, 6.4 m / s, 6.6 m / s, 6.8 m / s, 7 m / s, 7.2 m / s, 7.4 m / s, 7.6 m / s, 7.8 m / s, 8 m / s, 8.2 m / s, 8.4 m / s, 8.6 m / s, 8.8 m / s, 9 m / s, 9.2 m / s, 9.4 m / s, 9.6 m / s, 9.8 m / s, 10 m / s, etc.

[0128] When the flow rate V2 of nitrogen satisfies 1 m / s ≤ V2 ≤ 10 m / s, the concentration at the nitrogen inlet 511c of each plate 4 can be ensured to be relatively high, so that the reaction on the cathode side of each plate 4 can proceed stably, and has a relatively high reaction efficiency, and further the production efficiency of ammonia can be ensured.

[0129] In a specific embodiment, as Figure 1 shown, the electrocatalytic ammonia synthesis device includes a plurality of plates 4 and a plurality of reaction units 5. The plurality of plates 4 and the plurality of reaction units 5 are stacked in sequence along the first direction x. Each reaction unit 5 includes an electrolyte plate 51, a proton exchange membrane 52, and a gas diffusion electrode 53.

[0130] The electrocatalytic ammonia synthesis device further includes two end plates 1, which are spaced apart along the first direction x. A plurality of electrode plates 4 and a plurality of reaction units 5 are both located between the two end plates 1, and the electrode plates 4 between adjacent reaction units 5 are bipolar plates, while the electrode plates 4 between the end plate 1 and its adjacent reaction unit 5 are both monopolar plates.

[0131] In the embodiment of the present application, the two end plates 1 can be a top plate 11 and a bottom plate 12 respectively.

[0132] When the plurality of electrode plates 4 and the plurality of reaction units 5 are stacked in sequence along the first direction x to form the electrocatalytic ammonia synthesis device, the electrode plates 4 between adjacent reaction units 5 are bipolar plates, so that the anode side of the bipolar plate abuts against the proton exchange membrane 52 of one reaction unit 5, and the cathode side of the bipolar plate abuts against the gas diffusion electrode 53 of another reaction unit 5, thereby enabling a first reaction zone and a second reaction zone to be formed on both sides of any reaction unit 5 for the circulation of hydrogen and nitrogen.

[0133] Meanwhile, the electrode plate 4 between the top plate 11 and its adjacent reaction unit 5 is a monopolar plate, so that the anode side of the monopolar plate abuts against the proton exchange membrane 52 of the adjacent reaction unit 5, and the cathode side of the monopolar plate abuts against the top plate 11, or the cathode side of the monopolar plate abuts against the gas diffusion electrode 53 of the adjacent reaction unit 5, and the anode side of the monopolar plate abuts against the top plate 11, thereby eliminating the need for the reaction gas to flow between the top plate 11 and its adjacent electrode plate 4, which is beneficial to improving the effective utilization rate of the reaction gas in the electrocatalytic ammonia synthesis device, and further improving the production efficiency and output of ammonia.

[0134] In addition, the electrode plate 4 between the bottom plate 12 and its adjacent reaction unit 5 is a monopolar plate, so that the anode side of the monopolar plate abuts against the proton exchange membrane 52 of the adjacent reaction unit 5, and the cathode side of the monopolar plate abuts against the bottom plate 12, or the cathode side of the monopolar plate abuts against the gas diffusion electrode 53 of the adjacent reaction unit 5, and the anode side of the monopolar plate abuts against the bottom plate 12, thereby eliminating the need for the reaction gas to flow between the bottom plate 12 and its adjacent electrode plate 4, which is beneficial to improving the effective utilization rate of the reaction gas in the electrocatalytic ammonia synthesis device, and further improving the production efficiency and output of ammonia.

[0135] In a possible implementation manner, such as Figure 2As shown in the figure, the electrocatalytic ammonia synthesis device further includes a seal 54. Along the first direction x, seals 54 are provided on both the anode side and the cathode side of the bipolar plate, so that during the process of stacking multiple plates 4 and multiple reaction units 5 in sequence along the first direction x to form the electrocatalytic ammonia synthesis device, the anode side of the bipolar plate is hermetically connected to the electrolyte plate 51 of one reaction unit 5, and the cathode side of the bipolar plate is hermetically connected to the electrolyte plate 51 of another reaction unit 5, so as to improve the sealing performance between the bipolar plate and its adjacent electrolyte plate 51, thereby reducing the possibility of reaction gas leakage during the flow process, and further facilitating the improvement of the stability and reliability of the electrocatalytic ammonia synthesis device during operation.

[0136] Meanwhile, along the first direction x, a seal 54 can also be provided between the top plate 11 and its adjacent single plate, so as to hermetically connect the top plate 11 and the single plate, which is conducive to further reducing the possibility of reaction gas flowing into the space between them.

[0137] In addition, along the first direction x, a seal 54 can also be provided between the bottom plate 12 and its adjacent single plate, so as to hermetically connect the bottom plate 12 and the single plate, which is conducive to further reducing the possibility of reaction gas flowing into the space between them.

[0138] In a specific embodiment, as Figure 1 shown in the figure, the electrocatalytic ammonia synthesis device further includes two insulating plates 2 and two current collector plates 3. The two insulating plates 2 and the two current collector plates 3 are spaced apart along the first direction x. Multiple plates 4 and multiple reaction units 5 are both located between the two current collector plates 3, and the two insulating plates 2 are respectively located between the two current collector plates 3 and the two end plates 1.

[0139] Along the first direction x, the end plate 1, the insulating plate 2 and the current collector plate 3 located at the same end of the electrocatalytic ammonia synthesis device are all provided with fourth cavity areas 6. The fourth cavity areas 6 communicate with each other, and the fourth cavity area 6 of the current collector plate 3 communicates with the first cavity area 41 of its adjacent plate 4.

[0140] In the embodiments of the present application, the two insulating plates 2 can be respectively a first insulating plate 21 and a second insulating plate 22, and the two current collector plates 3 can be respectively a first current collector plate 31 and a second current collector plate 32.

[0141] When multiple plates 4 and multiple reaction units 5 are stacked in sequence along the first direction x to form the electrocatalytic ammonia synthesis device, there is a first insulating plate 21 and a first current collector plate 31 between the top plate 11 and its adjacent single plate, and the first insulating plate 21 is located between the first current collector plate 31 and the top plate 11. There is a second insulating plate 22 and a second current collector plate 32 between the bottom plate 12 and its adjacent single plate, and the second insulating plate 22 is located between the second current collector plate 32 and the bottom plate 12.

[0142] Among them, the first current collector plate 31 and the second current collector plate 32 are used to communicate with an external circuit so as to transmit current to each electrode plate 4 and each reaction unit 5, thereby ensuring the stability and reliability of the electrocatalytic ammonia synthesis device during operation. The first insulating plate 21 and the second insulating plate 22 are respectively used to isolate the first current collector plate 31 from the top plate 11 and the second current collector plate 32 from the bottom plate 12 to avoid the risk of short circuit, thereby ensuring the safety of the electrocatalytic ammonia synthesis device during operation.

[0143] Meanwhile, along the first direction x, fourth cavity areas 6 are provided on the end plate 1, the insulating plate 2, and the current collector plate 3 at the same end of the electrocatalytic ammonia synthesis device. The fourth cavity areas 6 communicate with each other, and the fourth cavity area 6 of the current collector plate 3 communicates with the first cavity area 41 of its adjacent electrode plate 4.

[0144] Taking the top plate 11, the first insulating plate 21, and the first current collector plate 31 as an example, hydrogen inlets 511a, hydrogen outlets 511b, nitrogen inlets 511c, and nitrogen outlets 511d are provided in the fourth cavity area 6 of the top plate 11, the fourth cavity area 6 of the first insulating plate 21, and the fourth cavity area 6 of the first current collector plate 31. Along the first direction x, the hydrogen inlets 511a communicate with each other, the hydrogen outlets 511b communicate with each other, the nitrogen inlets 511c communicate with each other, and the nitrogen outlets 511d communicate with each other.

[0145] During the process of hydrogen flowing into the electrocatalytic ammonia synthesis device for reaction, along the first direction x, hydrogen first flows into the electrocatalytic ammonia synthesis device from the hydrogen inlet 511a of the top plate 11, then sequentially passes through the hydrogen inlets 511a of the first insulating plate 21 and the first current collector plate 31, and flows into the hydrogen inlet 511a of the single electrode plate adjacent to the first current collector plate 31. At this time, the hydrogen is split, so that a part of the hydrogen flows into the anode side of this single electrode plate for reaction, and the other part of the hydrogen continues to flow towards the bottom plate 12 and is split multiple times during the flow process, so that the hydrogen can flow into the anode sides of the remaining bipolar plates for reaction. After the hydrogen flows into the bottom of the electrocatalytic ammonia synthesis device (i.e., the hydrogen inlet 511a of the single electrode plate adjacent to the second current collector plate 32), the hydrogen is no longer split at this time and all flows into the anode side of the single electrode plate adjacent to the second current collector plate 32 for reaction. Meanwhile, the unreacted hydrogen can flow into the hydrogen outlets 511b of each cavity area after flowing out of each reaction area and flow towards the top plate 11, so that the unreacted hydrogen in each reaction area converges and uniformly flows out of the electrocatalytic ammonia synthesis device through the hydrogen outlet 511b of the top plate 11 for recycling.

[0146] During the process of nitrogen flowing into the electrocatalytic ammonia synthesis device for reaction, along the first direction x, nitrogen first flows into the electrocatalytic ammonia synthesis device from the nitrogen inlet 511c of the top plate 11, then successively passes through the nitrogen inlets 511c of the first insulating plate 21 and the first current collector plate 31, and flows into the nitrogen inlet 511c of the monopolar plate adjacent to the first current collector plate 31. At this time, the nitrogen is split, so that part of the nitrogen flows into the cathode side of this monopolar plate for reaction, and the other part of the nitrogen continues to flow towards the bottom plate 12 and is split multiple times during the flow process, so that the nitrogen can flow into the cathode sides of the remaining bipolar plates for reaction. After the nitrogen flows into the bottom of the electrocatalytic ammonia synthesis device (i.e., the nitrogen inlet 511c of the monopolar plate adjacent to the second current collector plate 32), the nitrogen is no longer split at this time and all flows into the cathode side of the monopolar plate adjacent to the second current collector plate 32 for reaction. At the same time, the unreacted nitrogen and the ammonia generated by the reaction flow out from each reaction zone, can flow into the nitrogen outlet 511d of each cavity area, and flow towards the top plate 11, so that the unreacted hydrogen and the ammonia generated by the reaction in each reaction zone are converged and then uniformly flow out of the electrocatalytic ammonia synthesis device through the nitrogen outlet 511d of the top plate 11, so as to collect ammonia and recycle the unreacted nitrogen.

[0147] In a possible implementation manner, along the first direction x, each fourth cavity area 6 not only overlaps with the projection of the first cavity area 41 of each plate 4, but also overlaps with the projection of the second cavity area 511 of each electrolyte plate 51, that is, the projections of each hydrogen inlet 511a, each hydrogen outlet 511b, each nitrogen inlet 511c and each nitrogen outlet 511d of the electrocatalytic ammonia synthesis device all overlap. By such a design method, the flow effect of the gas can be optimized, the assembly difficulty during the stacking process of the electrocatalytic ammonia synthesis device can be reduced, and the stacking efficiency can be improved.

[0148] In a possible implementation manner, the electrocatalytic ammonia synthesis device further includes two backpressure valves (not marked in the figure) respectively connected to the hydrogen outlet 511b and the nitrogen outlet 511d, which are used to adjust the gas pressure inside the electrocatalytic ammonia synthesis device to ensure that the gas pressures on both sides of the electrolyte plate 51 along the first direction x are equal.

[0149] The structure, characteristics and function effects of the present application have been described in detail based on the embodiments shown in the drawings. The above is only the preferred embodiment of the present application, but the present application is not limited to the implementation scope shown in the drawings. Any changes made according to the concept of the present application, or modified into equivalent embodiments with equivalent changes, still within the spirit covered by the specification and the drawings, should be within the protection scope of the present application.

Claims

1. An electrocatalytic ammonia synthesis device, characterized in that: The electrocatalytic ammonia synthesis device comprises a plurality of electrode plates and a plurality of electrolyte plates, wherein the plurality of electrode plates and the plurality of electrolyte plates are sequentially stacked along a first direction, each electrode plate having an anode side and a cathode side arranged opposite to each other, a proton exchange membrane is further arranged between each electrolyte plate and the anode side of each electrode plate, and a gas diffusion electrode is further arranged between each electrolyte plate and the cathode side of each electrode plate; The electrode plate includes a first cavity area and a first flow field area which are interconnected, and the electrolyte plate includes a second cavity area and a second flow field area which are independent of each other, and the first cavity area is connected with the second cavity area.

2. The electrocatalytic ammonia synthesis device according to claim 1, characterized in that: The first cavity port area and the second cavity port area both include a hydrogen inlet, a hydrogen outlet, a nitrogen inlet and a nitrogen outlet. Along the second direction, the hydrogen inlet and the hydrogen outlet are distributed diagonally relative to each flow field area, the nitrogen inlet and the nitrogen outlet are distributed diagonally relative to each flow field area, and the hydrogen inlet is adjacent to the nitrogen outlet, and the nitrogen inlet is adjacent to the hydrogen outlet.

3. The electrocatalytic ammonia synthesis device according to claim 2, characterized in that: In each of the electrode plates, the first flow field area located on the anode side of the electrode plate is connected to the hydrogen inlet and the hydrogen outlet for circulating hydrogen, and the first flow field area located on the cathode side of the electrode plate is connected to the nitrogen inlet and the nitrogen outlet for circulating nitrogen; When the plurality of electrode plates and the plurality of electrolyte plates are stacked in sequence along the first direction, the gas pressures on both sides of the electrolyte plates are the same.

4. The electrocatalytic ammonia synthesis device according to claim 3, characterized in that: The gas pressure on the anode side of the electrode plate is P1, and P1 satisfies 50kpa≤P1≤1000kpa, and the gas pressure on the cathode side of the electrode plate is P2, and P2 satisfies 50kpa≤P2≤1000kpa.

5. The electrocatalytic ammonia synthesis device according to claim 3, characterized in that: The flow rate of the hydrogen is V1, the flow rate of the nitrogen is V2, and V1 and V2 satisfy V1≥2×V2, wherein V1 satisfies 2m / s≤V1≤20m / s, and V2 satisfies 1m / s≤V2≤10m / s.

6. The electrocatalytic ammonia synthesis device according to claim 1, characterized in that: The electrolyte plate further includes a third cavity region connected to the second flow field region, the third cavity region includes at least one electrolyte inlet and at least one electrolyte outlet, the electrolyte inlet and the electrolyte outlet are distributed on both sides of the second flow field region along a third direction; In the electrocatalytic ammonia synthesis device, the electrolyte inlet of each electrolyte plate is located at the same side of the electrocatalytic ammonia synthesis device, and the electrolyte outlet of each electrolyte plate is located at the same side of the electrocatalytic ammonia synthesis device.

7. The electrocatalytic ammonia synthesis device according to claim 6, characterized in that: The electrocatalytic ammonia synthesis device also includes a diverter and a converging device, which are distributed on both sides of the electrocatalytic ammonia synthesis device along a third direction, the diverter is connected to the electrolyte inlet of each electrolyte plate, and the converging device is connected to the electrolyte outlet of each electrolyte plate.

8. The electrocatalytic ammonia synthesis device according to claim 6, characterized in that: The second flow field area includes a plurality of electrolyte flow channels for circulating electrolyte. The plurality of electrolyte flow channels are spaced apart along the second direction and extend along the third direction. Each of the electrolyte flow channels is a hollow structure, and adjacent electrolyte flow channels are independent of each other.

9. The electrocatalytic ammonia synthesis device according to claim 8, characterized in that: Along the first direction, the projection of each electrolyte flow channel is a straight line or a curve.

10. The electrocatalytic ammonia synthesis device according to claim 8, characterized in that: Along the third direction, the liquid inlet of each electrolyte flow channel is connected to the electrolyte inlet, the liquid outlet of each electrolyte flow channel is connected to the electrolyte outlet, and the flow cross-sectional area of ​​each liquid outlet is greater than or equal to the flow cross-sectional area of ​​each liquid inlet.

11. The electrocatalytic ammonia synthesis device according to claim 8, characterized in that: The area of ​​the second flow field is S1, and S1 satisfies 200cm 2 ≤S1≤500cm 2 ; The length of each electrolyte flow channel is L, and L satisfies 50mm≤L≤200mm; The flow cross-sectional area of ​​each electrolyte flow channel is S2, and S2 satisfies 10mm 2 ≤S2≤100mm 2 ; The distance between adjacent electrolyte flow channels is H, and H satisfies 1mm≤H≤10mm; the flow rate of the electrolyte is V3, and V3 satisfies 0.1m / s≤V3≤5m / s.

12. The electrocatalytic ammonia synthesis device according to any one of claims 1 to 11, characterized in that: The electrocatalytic ammonia synthesis device comprises a plurality of electrode plates and a plurality of reaction units, wherein the plurality of electrode plates and the plurality of reaction units are stacked in sequence along a first direction, and each reaction unit comprises the electrolyte plate, the proton exchange membrane and the gas diffusion electrode; The electrocatalytic ammonia synthesis device also includes two end plates, which are spaced apart along a first direction, and the plurality of electrode plates and the plurality of reaction units are located between the two end plates, and the electrode plates between adjacent reaction units are bipolar plates, and the electrode plates between the end plates and the adjacent reaction units are monopolar plates.

13. The electrocatalytic ammonia synthesis device according to claim 12, characterized in that: The electrocatalytic ammonia synthesis device further comprises two insulating plates and two current collecting plates, the two insulating plates and the two current collecting plates are spaced apart and distributed along the first direction, the plurality of electrode plates and the plurality of reaction units are located between the two current collecting plates, and the two insulating plates are respectively located between the two current collecting plates and the two end plates; Along the first direction, the end plate, the insulating plate and the current collecting plate located at the same end of the electrocatalytic ammonia synthesis device are all provided with a fourth cavity area, each of the fourth cavity areas is interconnected, and the fourth cavity area of ​​the current collecting plate is interconnected with the first cavity area of ​​the adjacent electrode plate.

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