Integrated continuous magnesium-nitrogen hydrolysis ammonia supply system and method

Abstract

This invention discloses an integrated continuous magnesium nitridation hydrolysis ammonia supply system and method, relating to the fields of new energy and ammonia energy. The system includes a high-temperature reaction unit, a continuous hydrolysis reaction unit, and a waste recovery unit. The high-temperature reaction unit is used for the nitridation reaction of magnesium powder and nitrogen gas, and unreacted nitrogen gas is condensed and refluxed to participate in the nitridation reaction again. The continuous hydrolysis reaction unit is used to receive the magnesium nitride generated by the nitridation reaction, drive the magnesium nitride to flow and contact the sprayed reaction liquid to undergo a hydrolysis reaction, generating ammonia gas and reaction byproducts. The waste recovery unit is used to clean and collect the reaction byproducts flowing within the hydrolysis reaction unit. This invention has a reasonable structure; the reaction process in the metal nitridation and hydrolysis ammonia production system is controllable, the reaction is continuous, the products are easy to recover, the ammonia is easy to store, and maintenance time is short.

Description

Technical Field

[0001] This invention relates to the fields of new energy and ammonia energy, specifically to an integrated continuous magnesium nitride hydrolysis ammonia supply system and method. Background Technology

[0002] Ammonia is considered a reliable alternative to hydrogen energy. It exists as a gas at room temperature and is easily liquefied and stored. Ammonia is a zero-carbon compound with high energy density and is also a hydrogen storage medium. As a hydrogen-rich fuel, its combustion products are water and nitrogen, which is environmentally friendly and widely used in energy storage, chemical raw materials, power generation, and agriculture.

[0003] The traditional Haber-Bosch process for ammonia synthesis in the ammonia chemical industry is energy-intensive and emits greenhouse gases. The Haber-Bosch process still suffers from limitations such as high requirements for the purity of raw materials like hydrogen and nitrogen, high energy consumption, and high dependence on catalysts. Furthermore, industrial ammonia transportation primarily involves liquefying ammonia under high pressure at room temperature, storing it in high-pressure cylinders, and then transporting it, further increasing industrial production costs. Compared to the energy-intensive Haber-Bosch ammonia production process, the process of preparing ammonia through the hydrolysis of metal nitrides is energy-efficient, less environmentally polluting, and uses readily available raw materials, making it a viable alternative. Magnesium nitride (Mg3N2), as an ammonia carrier, has advantages such as high safety and stable physicochemical properties, and is one of the commonly used materials for hydrolysis ammonia production. Magnesium nitride reacts with water to produce magnesium hydroxide, which can be recovered and smelted to obtain metallic magnesium again, contributing to sustainable industrial ammonia production. Magnesium nitride is usually obtained by nitriding metallic magnesium powder to produce 3Mg + N2(g) = Mg3N2. The reaction of magnesium nitride hydrolysis to produce ammonia is Mg3N2 + 6H2O = 3Mg(OH)2 + 2NH3(g).

[0004] In existing technologies, ammonia production still faces the following technical challenges: 1. The Haber-Bosch ammonia production process has high energy consumption, requiring high pressure (150–300 atm) and high temperature (400–500℃), and is highly dependent on catalyst activation of inert N2 molecules. The synthesis efficiency of the Haber-Bosch ammonia production reaction using an iron-based catalyst is only 10–20%, and a large amount of unreacted N2 / H2 needs to be recycled and compressed. The high-pressure system and gas circulation system required for the reaction further increase the costs of industrial production and equipment maintenance. Using nitride hydrolysis to produce ammonia has the advantages of low energy consumption and high ammonia production efficiency and is considered a viable alternative to the Haber-Bosch ammonia production process. However, it still suffers from low metal nitriding efficiency and the need to replenish / clean up hydrolysis reactants / products, resulting in discontinuous production and difficulty in achieving industrial-scale production.

[0005] 2. Existing processes for producing ammonia by hydrolysis of magnesium nitride typically involve placing magnesium nitride in a sealed device and continuously adding water as the reaction solution. Magnesium nitride reacts with water to produce magnesium oxide, releasing ammonia gas. The ammonia gas is absorbed by an absorbent to produce ammonia water, which is then used for further applications. This method results in low ammonia production efficiency, hindering the sustainable production and use of ammonia. The hydrolysis of magnesium nitride produces magnesium hydroxide: Mg3N2 + 6H2O = 3Mg(OH)2 + 2NH3(g).

[0006] Because the reaction process in existing magnesium nitride hydrolysis ammonia production systems is uncontrollable, sustainable ammonia production requires replenishing the reaction unit and separating and recovering the products after the magnesium nitride hydrolysis feedstock is completely consumed. In existing hydrolysis ammonia production systems, it is difficult to conveniently separate and recover solid reaction products from the reaction unit, resulting in unsustainable ammonia production and failing to meet actual usage demands. Furthermore, the storage and transportation of ammonia gas produced by the hydrolysis unit further increases operating costs. Therefore, there is an urgent need for an integrated, continuous magnesium nitride hydrolysis ammonia supply system to solve these problems. Summary of the Invention

[0007] To address the shortcomings of existing technologies, the present invention aims to provide an integrated continuous magnesium nitridation hydrolysis ammonia supply system and method to solve the problems mentioned in the background. The present invention has a reasonable structure, and the reaction process in the metal nitridation and hydrolysis ammonia production system is controllable, the reaction is continuous, the products are easy to recover, the ammonia is easy to store, and the maintenance time is short.

[0008] To achieve the above objectives, the present invention provides an integrated continuous magnesium nitridation hydrolysis ammonia supply system, comprising: a high-temperature reaction unit, a continuous hydrolysis reaction unit, a waste recovery unit, and a control unit; the high-temperature reaction unit is used for the nitridation reaction of magnesium powder and nitrogen, and the unreacted nitrogen is condensed and recirculated to participate in the nitridation reaction again; the continuous hydrolysis reaction unit is used to receive magnesium nitride generated by the nitridation reaction in the high-temperature reaction unit, drive the magnesium nitride to flow and contact the sprayed reaction liquid to undergo a hydrolysis reaction, generating ammonia and solid reaction byproducts; the waste recovery unit is used to clean and collect the solid reaction byproducts flowing in the hydrolysis reaction unit; the control unit is connected to the high-temperature reaction unit and the continuous hydrolysis reaction unit respectively, and is used to collect the operating parameters of the nitridation reaction and the hydrolysis reaction in real time, analyze and process the collected operating parameters, and adjust the process parameters of the nitridation reaction and the hydrolysis reaction to control the stable development of the magnesium powder and nitrogen nitridation reaction and the hydrolysis reaction.

[0009] Preferably, the high-temperature reaction unit includes a storage and feeding device, a high-temperature reaction vessel, and a nitrogen circulation path; the storage and feeding device includes an inlet, a storage tank, and a regulating valve, the inlet being located at the top of the storage tank, the regulating valve being located at the bottom of the storage tank, and the bottom of the regulating valve communicating with the inlet end of the high-temperature reaction vessel; the nitrogen circulation path includes a condenser, and the outlet of the high-temperature reaction vessel, the condenser, and the return port of the high-temperature reaction vessel are connected in series in the direction of gas flow, wherein the gas flow returns from the outlet to the return port after passing through the condenser; a filter is installed on the high-temperature reaction vessel through a pipeline, and an inlet for conveying nitrogen is installed on the filter through a pipeline. An intake valve is provided on the air inlet; the control unit includes an acquisition module for real-time acquisition of operating parameters of the nitriding and hydrolysis reactions, and a processing module for analyzing and adjusting the process parameters of the nitriding and hydrolysis reactions based on the acquired operating parameters; the acquisition module includes a first temperature sensor installed in the high-temperature reaction vessel, and the processing module includes a PLC controller; the PLC controller is connected to the first temperature sensor and the heater in the high-temperature reaction vessel; the operating parameters of the nitriding reaction include the nitriding reaction temperature and the holding time; the process parameters of the nitriding reaction include a nitriding reaction temperature of 973-1073K and a holding time of 0-30min.

[0010] Preferably, the continuous hydrolysis reaction unit includes a reactant feeding tank for receiving reactants to generate magnesium nitride from the nitriding reaction, a circulating reaction tank, and a spraying assembly for spraying the reaction liquid; the circulating reaction tank includes a reaction tank body, inside which multiple sets of transmission devices are rotatably arranged, adjacent transmission devices are connected by a corrosion-resistant membrane, and the multiple sets of transmission devices are arranged in a rectangular array, the corrosion-resistant membrane surrounds the outer periphery of the rectangular array and extends to cover all transmission devices; the reactant feeding tank is disposed inside the reaction tank body and is used to feed reactants to the top of the corrosion-resistant membrane located at the bottom, and the bottom of the reactant feeding tank... The reactor is equipped with a feeder located above the lowest corrosion-resistant film. A spray assembly is located inside the reactor body and is used to spray the magnesium nitride reaction solution onto the top of the lowest corrosion-resistant film. The spray assembly includes a water tank located inside the reactor body, a heating plate for heating the reaction solution in the water tank to a set temperature, and a sprayer for spraying the reaction solution from the water tank onto the surface of the lowest corrosion-resistant film. The heating plate is located inside the water tank, and the sprayer is located below the water tank and connected to the water tank via a pipe. The water tank is connected to an external water tank's inlet via a pipe.

[0011] Preferably, the transmission device includes a motor mounted on the side wall of the reaction tank body, and a conveyor shaft rotatably mounted inside the reaction tank body and connected to the output shaft of the motor; the corrosion-resistant film is wound on the conveyor shafts of multiple transmission devices; the acquisition module also includes a mass sensor in the feeder, a speed sensor mounted on the conveyor shaft, and a second temperature sensor mounted on the water tank; the PLC controller is connected to the mass sensor, speed sensor, second temperature sensor, discharge valve in the feeder, motor, and heating plate, respectively; the operating parameters of the hydrolysis reaction include the hydrolysis reaction temperature, the transmission speed of the corrosion-resistant film, and the temperature of the reaction liquid in the water tank; the process parameters of the hydrolysis reaction include a hydrolysis reaction temperature of 273-373K and a transmission speed of 0-10 mm / min for the corrosion-resistant film. -1 The temperature of the reaction liquid in the water tank is 273-373K.

[0012] Preferably, it further includes an ammonia collection unit for receiving ammonia gas generated in the hydrolysis reaction in the continuous hydrolysis reaction unit, and for drying and collecting the ammonia gas; the ammonia collection unit includes an exhaust port, an outlet valve, a dryer, a vacuum pump, connecting valves, and an ammonia collection chamber; the exhaust port is located at the top of the circulating reaction tank of the continuous hydrolysis reaction unit and is used to discharge the ammonia gas generated in the hydrolysis reaction; the exhaust port is equipped with an outlet valve, which is connected to the inlet end of the dryer through a pipeline, and the outlet end of the dryer is connected to the inlet port of the vacuum pump through a pipeline; the exhaust port of the vacuum pump is connected to the valve and the ammonia collection chamber in sequence through a pipeline.

[0013] Preferably, the waste recycling unit includes a solid scraper, a funnel, and a collection trough. Both the solid scraper and the funnel are disposed inside the reaction tank body. The solid scraper is used to clean the solid reaction byproducts at the top of the corrosion-resistant film at the bottom into the funnel. The solid scraper is located at the lower part of the feeder on the side away from the spray assembly. The solid scraper includes a blade body with an inclined surface on its sidewall. A through groove connected to the inclined surface and matching the corrosion-resistant film is formed on the sidewall of the blade body. A file is provided on the inclined surface to contact the corrosion-resistant film. A sealing cap is provided at the top of the funnel. A rotating shaft is rotatably mounted on the reaction tank body. A lever connected to the sealing cap is mounted on the rotating shaft. The lever rotates with the rotating shaft to drive the sealing cap to open and close. The collection trough is located at the bottom of the reaction tank body. The funnel communicates with the collection trough, which is directly below the funnel, and is used to collect the solid reaction byproducts discharged from the funnel.

[0014] Preferably, it also includes a water inlet rinsing device for cleaning the surface of the corrosion-resistant film. The water inlet rinsing device includes a water inlet and a water outlet opened on the reaction tank body. The water outlet is located below the water inlet. The water inlet is connected to a water inlet valve, and the water outlet is connected to a water outlet valve.

[0015] Preferably, the material of the corrosion-resistant film includes one or more of polyurethane, polytetrafluoroethylene, or polyethylene corrosion-resistant materials.

[0016] Preferably, the reaction solution is one or more of tap water, deionized water, or ultrapure water; the cleaning solution injected into the inlet of the water inlet rinsing device is a dilute acid, which includes one or more of dilute sulfuric acid, dilute hydrochloric acid, or dilute nitric acid; the magnesium powder in the nitriding reaction includes one or more of spherical magnesium powder and block magnesium powder, wherein the particle size is at the micron or nanometer level.

[0017] This invention provides an integrated continuous magnesium nitridation hydrolysis ammonia supply method, comprising the following steps: S1, nitridation reaction: Magnesium powder is fed into the storage tank through the inlet at the top of the storage tank via the storage and feeding device of the high-temperature reaction unit. The regulating valve at the bottom of the storage tank is adjusted to control the magnesium powder to be uniformly conveyed to the feed end of the high-temperature reaction tank. The air inlet valve on the pipeline connected to the filter is opened, and nitrogen gas is introduced into the high-temperature reaction tank through the air inlet, so that the magnesium powder and nitrogen gas undergo a nitridation reaction in the high-temperature reaction tank to generate magnesium nitride. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction tank, condensed by the condenser according to the airflow direction, and then flows back into the high-temperature reaction tank from the return port to participate in the nitridation reaction again, thereby realizing nitrogen gas circulation.

[0018] S2. Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank of the continuous hydrolysis reaction unit. The reactant feeding tank feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film located at the bottom of the circulating reaction tank through the feeder at the bottom. The spray assembly is started, and the water inlet of the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride on the top of the corrosion-resistant film. At the same time, multiple sets of transmission devices arranged in a rectangular array in the reaction tank body are started to drive the corrosion-resistant film connected between adjacent transmission devices to move, and drive the magnesium nitride to flow with the corrosion-resistant film, so that the magnesium nitride can fully contact the sprayed reaction liquid and continuously undergo hydrolysis reaction to generate ammonia and solid reaction byproducts.

[0019] S3. Waste Recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film causes the solid reaction byproducts to move and come into contact with the solid scraper, continuously cleaning the solid reaction byproducts located at the top of the bottom corrosion-resistant film into the funnel. The solid reaction byproducts fall through the funnel into the collection tank at the bottom of the reaction tank body, directly below the funnel, thus completing the cleaning and centralized collection of solid waste.

[0020] S4. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port at the top of the circulating reaction tank. The exhaust valve on the exhaust port is opened, allowing the ammonia to enter the inlet of the dryer through the pipeline. After being dried by the dryer, the ammonia is discharged from the outlet of the dryer and enters the inlet of the vacuum pump. The vacuum pump is started, and the dried ammonia is transported from the exhaust port of the vacuum pump to the connecting valve. After being regulated by the connecting valve, it is introduced into the ammonia collection chamber, completing the drying and sealed collection of ammonia.

[0021] S5. Continuous operation and maintenance: The system is kept in a closed state throughout the process, and raw materials and reaction liquids are continuously added to each unit to ensure continuous reaction. According to the cleanliness of the corrosion-resistant film surface, the sealing cover of the funnel is closed, the inlet valve of the water inlet flushing device is opened, and the cleaning liquid is sprayed onto the corrosion-resistant film through the water inlet on the reaction tank body. The waste liquid after cleaning is discharged through the drain outlet located below the water inlet. The waste liquid discharge is controlled by the drain valve to achieve stable operation of integrated continuous magnesium nitride hydrolysis ammonia supply.

[0022] Beneficial effects: Compared with the Haber-Bosch ammonia production process, which has low raw material conversion rate and high energy consumption, this invention is based on magnesium nitride hydrolysis for ammonia production with high conversion rate and low energy consumption. The integrated system highly integrates the nitridation of metal raw materials, nitride hydrolysis and ammonia storage / use, and the modular design makes the system easy to maintain.

[0023] This system utilizes magnesium powder and nitrogen in a high-temperature reaction unit for nitridation. Unreacted nitrogen is condensed and recycled back to participate in the nitridation reaction, thus recycling nitrogen and improving its utilization rate. This effectively addresses the low raw material utilization problem of traditional hydrolysis ammonia production systems. The continuous hydrolysis reaction unit receives the magnesium nitride generated from the nitridation reaction and drives its flow to contact the sprayed reaction liquid, resulting in ammonia and reaction byproducts. The flowing magnesium nitride spraying facilitates the hydrolysis reaction, and a waste recovery unit cleans and collects the flowing reaction byproducts, enabling their separation and recovery. The continuous flow of magnesium nitride and the cleaning and collection of flowing reaction byproducts ensure continuous ammonia supply. An ammonia collection unit collects the ammonia, allowing for immediate use and eliminating the need for traditional liquid ammonia transportation via steel cylinders, saving costs and facilitating subsequent use.

[0024] Compared to traditional hydrolysis reaction devices, this system has a simpler structure, is easier to operate, and requires less maintenance, thus extending the lifespan of the device and reducing production costs. For the cleaning and recovery of solid products from the hydrolysis reaction in the integrated system, the internally designed solid scraper can clean the solid reaction byproducts remaining on the surface of the corrosion-resistant film without opening the device and transfer them to the product collection tank for collection. In addition, the provided water inlet rinsing device can assist in cleaning the solid residues remaining on the surface of the corrosion-resistant film. Attached Figure Description

[0025] Other features, objects, and advantages of the invention will become more apparent from the following detailed description of non-limiting embodiments with reference to the accompanying drawings.

[0026] Figure 1 This is a schematic diagram of an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention.

[0027] Figure 2 This is a schematic diagram of a solid scraper in an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention.

[0028] Figure 3 This is a side view of the connection between the funnel and the sealing cap in an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention.

[0029] Figure 4 This is a top view of the closed state of the connection between the funnel and the sealing cap in an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention.

[0030] Figure 5 This is a top view of the funnel and sealing cap connection in an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention, in the open state.

[0031] Figure 6 The image shows the XRD pattern of magnesium nitride, which is the result of complete nitridation of magnesium powder in an integrated continuous magnesium nitridation hydrolysis ammonia supply system according to Embodiment 1 of the present invention.

[0032] Figure 7 This is a graph showing the ammonia production curves of magnesium nitride at different temperatures in an integrated continuous magnesium nitride hydrolysis ammonia supply system according to an embodiment of the present invention.

[0033] Figure 8 This is a schematic diagram of the control system according to the present invention.

[0034] The components include: 1. Feed inlet; 1001. High-temperature reaction unit; 1002. Continuous hydrolysis reaction unit; 1003. Ammonia collection unit; 1004. Waste recycling unit; 2. Storage tank; 3. Regulating valve; 4. High-temperature reaction tank; 5. Air inlet; 6. Air inlet valve; 7. Filter; 8. Condenser; 9. Nitrogen circulation path; 10. Reactant feeding tank; 11. Feeder; 12. Transmission device; 121. Electric motor; 122. Conveyor shaft; 13. Corrosion-resistant film; 14. Spray assembly; 141. Water tank; 142. Heating plate; 143. Spray nozzle. 15. Scraper for solids; 151. Blade body; 152. Inclined surface; 153. Through groove; 154. File; 16. Funnel; 161. Sealing cover; 162. Paddle; 163. Rotating shaft; 17. Exhaust port; 18. Exhaust valve; 19. Dryer; 20. Vacuum pump; 21. Connecting valve; 22. Ammonia collection chamber; 23. Water inlet; 24. Water inlet; 25. Water inlet valve; 26. Drain outlet; 27. Drain valve; 28. Circulating reaction tank; 29. ​​Water inlet flushing device; 30. Storage and feeding device; 31. Collection tank; 32. Control unit.

[0035] The accompanying drawings are provided to further understand the embodiments and form part of the specification. They are used together with the embodiments for explanation and do not constitute a limitation on the embodiments. Detailed Implementation

[0036] The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection.

[0037] In the description of the embodiments, it should be understood that the terms "upper", "lower", "front", "rear", "left", "right", "top", "bottom", "inner", "outer", etc., indicate the orientation or positional relationship based on the orientation or positional relationship shown in the drawings. They are only for the convenience of describing the embodiments and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation. Therefore, they should not be construed as limitations on the embodiments.

[0038] like Figure 1As shown, this embodiment of the invention provides an integrated continuous magnesium nitridation hydrolysis ammonia supply system, including: a high-temperature reaction unit 1001, a continuous hydrolysis reaction unit 1002, a waste recovery unit 1004, and a control unit 32; the high-temperature reaction unit 1001 is used for magnesium powder and nitrogen to undergo a nitridation reaction, and unreacted nitrogen is condensed and refluxed to participate in the nitridation reaction again; the continuous hydrolysis reaction unit 1002 is used to receive magnesium nitride generated by the nitridation reaction in the high-temperature reaction unit 1001, drive the magnesium nitride to flow and contact the sprayed reaction liquid to undergo a hydrolysis reaction, generating ammonia and solid reaction byproducts; the waste recovery unit 1004 is used to clean and collect the solid reaction byproducts flowing in the hydrolysis reaction unit; the control unit 32 is connected to the high-temperature reaction unit 1001 and the continuous hydrolysis reaction unit 1002 respectively, and is used to collect the operating parameters of the nitridation reaction and the hydrolysis reaction in real time, analyze and process the collected operating parameters, and adjust the process parameters of the nitridation reaction and the hydrolysis reaction to control the stable development of the magnesium powder and nitrogen to complete the nitridation reaction and the hydrolysis reaction. This design utilizes magnesium powder and nitrogen gas in a high-temperature reaction unit 1001 for nitridation. Unreacted nitrogen gas is condensed and recirculated to participate in the nitridation reaction, thus recycling nitrogen gas, improving nitrogen utilization, and increasing the nitridation efficiency of magnesium powder. This effectively addresses the low raw material utilization problem of traditional hydrolysis ammonia production systems. A continuous hydrolysis reaction unit 1002 receives the magnesium nitride generated from the nitridation reaction and drives its flow to contact the sprayed reaction liquid, resulting in a hydrolysis reaction that generates ammonia gas and solid reaction byproducts. The hydrolysis reaction occurs through the spraying of flowing magnesium nitride. In conjunction with a waste recovery unit 1004, the flowing solid reaction byproducts are cleaned and collected. After the magnesium nitride hydrolysis raw material is completely consumed, the system can promptly replenish the magnesium nitride raw material and separate and recover the solid reaction byproducts to achieve continuous ammonia supply. The control unit 32 is connected to the high-temperature reaction unit 1001 and the continuous hydrolysis reaction unit 1002 respectively to collect the operating parameters of the nitride and hydrolysis reactions in real time. The system analyzes and processes the collected operating parameters and adjusts the process parameters of the nitride and hydrolysis reactions to control the stable progress of the magnesium powder and nitrogen nitride and hydrolysis reactions. This ensures that the reaction process in the magnesium nitride and hydrolysis ammonia production system is controllable, facilitates the separation and recovery of the solid reaction byproducts, and improves the sustainability of the reaction.

[0039] Reference Figure 1The high-temperature reaction unit 1001 includes a storage and feeding device 30, a high-temperature reaction tank 4, and a nitrogen circulation passage 9. The storage and feeding device 30 includes an inlet 1, a storage tank 2, and a regulating valve 3. The inlet 1 is located at the top of the storage tank 2, and the regulating valve 3 is located at the bottom of the storage tank 2. The bottom of the regulating valve 3 is connected to the inlet end of the high-temperature reaction tank 4. The nitrogen circulation passage 9 includes a condenser 8, an outlet of the high-temperature reaction tank 4, a condenser 8, and a return port of the high-temperature reaction tank 4, which are connected in series according to the airflow direction. The airflow flows from the outlet through the condenser 8 and then back to the return port. A filter 7 is installed on the high-temperature reaction tank 4 through a pipeline. An inlet 5 for conveying nitrogen is installed on the filter 7 through a pipeline. An inlet valve 6 is installed on the inlet 5. This design is applied to the high-temperature reaction unit 1001. The storage and feeding device 30 in 01 feeds magnesium powder into the storage tank 2 through the feed inlet 1 at the top of the storage tank 2. The regulating valve 3 at the bottom of the storage tank 2 is adjusted to control the magnesium powder to be fed to the feed end of the high-temperature reaction tank 4 at a uniform speed, thus controlling the magnesium powder nitriding process. Then, the air inlet valve 6 is opened, and nitrogen gas is introduced into the high-temperature reaction tank 4 through the air inlet 5, so that the magnesium powder and nitrogen gas undergo a nitriding reaction in the high-temperature reaction tank 4 to generate magnesium nitride. Among them, the unreacted nitrogen gas is discharged from the air outlet of the high-temperature reaction tank 4, condensed by the condenser 8 according to the air flow direction, and then flows back into the high-temperature reaction tank 4 through the return port to participate in the nitriding reaction again, realizing nitrogen gas circulation and recycling, improving the nitrogen gas utilization rate, improving the nitriding efficiency of magnesium powder, and effectively improving the problem of low raw material utilization rate in traditional high-temperature nitriding reaction systems.

[0040] The control unit 32 includes a data acquisition module for real-time acquisition of operating parameters of the nitriding and hydrolysis reactions, and a processing module for analyzing and adjusting the process parameters of the nitriding and hydrolysis reactions based on the acquired operating parameters. The data acquisition module includes a first temperature sensor installed in the high-temperature reaction vessel 4, and the processing module includes a PLC controller. The PLC controller is connected to the first temperature sensor and the heater in the high-temperature reaction vessel 4. The operating parameters of the nitriding reaction include the nitriding reaction temperature and the holding time. The process parameters of the nitriding reaction include a nitriding reaction temperature of 973-1073K and a holding time of 0-30min. This design monitors the nitriding reaction temperature in the high-temperature reaction vessel 4 through the first temperature sensor. When the temperature is lower than the set value, a signal is sent to the PLC controller. The PLC controller controls the heater to heat to the set value, and the high-temperature reaction vessel 4 is held at the set temperature for the set time. This facilitates real-time acquisition of the operating parameters of the nitriding reaction, analysis and processing of the acquired operating parameters, and adjustment of the process parameters of the nitriding reaction to ensure the stable progress of the nitriding reaction between magnesium powder and nitrogen.

[0041] The continuous hydrolysis reaction unit 1002 includes a reactant feeding tank 10 for receiving reactants to generate magnesium nitride from the nitriding reaction, a circulating reaction tank 28, and a spray assembly 14 for spraying the reaction liquid. The circulating reaction tank 28 includes a reaction tank body, inside which multiple sets of transmission devices 12 are rotatably arranged. Adjacent transmission devices 12 are connected by a corrosion-resistant membrane 13. The multiple sets of transmission devices 12 are arranged in a rectangular array. The corrosion-resistant membrane 13 surrounds the outer periphery of the rectangular array and extends to cover all transmission devices 12. The reactant feeding tank 10 is located inside the reaction tank body and is used to feed reactants to the top of the corrosion-resistant membrane 13 located at the bottom. A feeder 11 is provided at the bottom of the reactant feeding tank 10. The feeder 11 is located above the bottommost corrosion-resistant film 13; the spray assembly 14 is located inside the reaction tank body and is used to spray the magnesium nitride reaction liquid onto the top of the bottommost corrosion-resistant film 13; the spray assembly 14 includes a water tank 141 located inside the reaction tank body, a heating plate 142 for heating the reaction liquid in the water tank 141 to a set temperature, and a sprayer 143 for spraying the reaction liquid in the water tank 141 onto the surface of the bottommost corrosion-resistant film 13; the heating plate 142 is located inside the water tank 141, the sprayer 143 is located below the water tank 141 and is connected to the water tank 141 through a pipeline, and the water tank 141 is connected to the water inlet 23 of an external water tank through a pipeline. The design utilizes a reactant feeding tank 10 to store the generated magnesium nitride. The reactant feeding tank 10, via a bottom feeder 11, uniformly adds magnesium nitride to the top of the corrosion-resistant film 13 at the bottom of the circulating reaction tank 28. Then, the sprayers 143 in the spray assembly 14 are activated, and the reaction liquid, heated to a set temperature by the heating plate 142 in the water tank 141, is continuously sprayed onto the magnesium nitride on top of the corrosion-resistant film 13. Simultaneously, multiple sets of transmission devices 12 arranged in a rectangular array within the reaction tank are activated, moving the corrosion-resistant film 13 connected to adjacent transmission devices 12. This drives the magnesium nitride to flow with the corrosion-resistant film 13, ensuring sufficient contact between the magnesium nitride and the sprayed reaction liquid, continuously undergoing a hydrolysis reaction to generate... Ammonia and solid reaction byproducts; by adjusting the feed rate of magnesium nitride in the hydrolysis reactant feeding tank 10, the temperature of the reaction liquid in the spray assembly 14, and the moving speed of the corrosion-resistant film 13 driven by the transmission device 12, the ammonia production rate and amount in the magnesium nitride hydrolysis process can be controlled; through the separate design of the reactant feeding zone and the hydrolysis reaction zone, the accumulation of nitride in a fixed position in the reaction device can be effectively avoided, thus reducing the hydrolysis reaction rate, while increasing the contact area of ​​the hydrolysis reaction and increasing the ammonia production per unit time; by connecting the high-temperature reaction unit 1001 and the continuous hydrolysis reaction unit 1002, the magnesium powder nitriding device and the magnesium nitride hydrolysis reaction device are connected, realizing the integration of magnesium nitride synthesis and hydrolysis.

[0042] Reference Figure 1 and Figure 8The transmission device 12 includes a motor 121 mounted on the side wall of the reaction tank body, and a conveyor shaft 122 rotatably mounted inside the reaction tank body and connected to the output shaft of the motor 121; the corrosion-resistant film 13 is wound around the conveyor shafts 122 of multiple transmission devices 12; the acquisition module also includes a mass sensor in the feeder 11, a speed sensor mounted on the conveyor shaft 122, and a second temperature sensor mounted on the water tank 141; the PLC controller is connected to the mass sensor, speed sensor, second temperature sensor, discharge valve in the feeder 11, motor 121, and heating plate 142 respectively; the operating parameters of the hydrolysis reaction include the hydrolysis reaction temperature, the transmission speed of the corrosion-resistant film 13, and the temperature of the reaction liquid in the water tank 141; the process parameters of the hydrolysis reaction include a hydrolysis reaction temperature of 273-373K and a transmission speed of 0-10mm for the corrosion-resistant film 13. -1 The temperature of the reaction solution in water tank 141 is 273-373K. This design utilizes multiple sets of transmission devices 12, each with a motor 121 driving a conveyor shaft 122. The conveyor shaft 122 then rotates the corrosion-resistant film 13 on it, facilitating the rectangular movement of the corrosion-resistant film 13. A second temperature sensor monitors the temperature of the reaction solution in water tank 141, a speed sensor monitors the movement speed of the corrosion-resistant film 13, and a mass sensor controls the amount of magnesium nitride discharged from the discharge valve of the feeder 11. This allows for real-time acquisition of the hydrolysis reaction's operating parameters. The collected parameters are then analyzed and processed to adjust the process parameters of the hydrolysis reaction, ensuring its stable operation.

[0043] It also includes an ammonia collection unit 1003 for receiving ammonia gas generated by the hydrolysis reaction in the continuous hydrolysis reaction unit 1002, and for drying and collecting the ammonia gas; the ammonia collection unit 1003 includes an exhaust port 17, an exhaust valve 18, a dryer 19, a vacuum pump 20, a connecting valve 21, and an ammonia collection chamber 22; the exhaust port 17 is located at the top of the circulating reaction tank 28 of the continuous hydrolysis reaction unit 1002 and is used to discharge the ammonia gas generated by the hydrolysis reaction; the exhaust port 17 is equipped with an exhaust valve 18, which is connected to the inlet end of the dryer 19 through a pipeline, and the outlet end of the dryer 19 is connected to the inlet port of the vacuum pump 20 through a pipeline; the exhaust port of the vacuum pump 20 is connected to the valve 21 and the ammonia collection chamber 22 in sequence through a pipeline. This design allows ammonia gas to be discharged from the exhaust port 17 at the top of the circulating reaction tank 28 by opening the exhaust valve 18 on the exhaust port 17. The ammonia gas then enters the inlet of the dryer 19 through a pipeline. After being dried by the dryer 19, it is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. Then, the vacuum pump 20 is started, and the dried ammonia gas is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, it is introduced into the ammonia gas collection chamber 22, completing the drying and sealed collection of ammonia gas. This facilitates the collection of ammonia gas, allowing it to be used immediately after production. It solves the problem of transporting liquid ammonia through steel cylinders in the traditional way, saves costs, and facilitates subsequent use. The ammonia gas collection chamber 22 can be connected to external equipment to use the prepared ammonia gas.

[0044] Reference Figure 1 and Figure 2 The waste recycling unit 1004 includes a solid scraper 15, a funnel 16, and a collection tank 31. Both the solid scraper 15 and the funnel 16 are located inside the reaction tank body. The solid scraper 15 is used to clean the solid reaction byproducts at the top of the lowest corrosion-resistant film 13 into the funnel 16. The solid scraper 15 is located at the lower part of the feeder 11 on the side away from the spray assembly 14. The solid scraper 15 includes a blade body 151, with a slope 152 on the side wall of the blade body 151. A through groove 153, connected to the slope 152 and matching the corrosion-resistant film 13, is provided on the slope 152. A file 154, in contact with the corrosion-resistant film 13, is provided on the slope 152. (See reference...) Figure 3 , Figure 4 and Figure 5The top of the funnel 16 is provided with a sealing cover 161. A rotating shaft 163 is rotatably provided on the reaction tank body. A lever 162 connected to the sealing cover 161 is provided on the rotating shaft 163. The lever 162 rotates with the rotating shaft 163 to drive the sealing cover 161 to open and close. During the hydrolysis reaction, the sealing cover 161 is in the open state. When cleaning with the water inlet flushing device 29, the sealing cover 161 is in the closed state. The collection tank 31 is provided at the bottom of the reaction tank body. The funnel 16 is connected to the collection tank 31. The collection tank 31 is directly below the funnel 16 and is used to collect the solid reaction byproducts discharged from the funnel 16. The funnel 16 is provided on the lower side of the inner wall of the reaction tank body and is connected to the collection tank 31. It is used to collect solids. The scraper 15 scrapes off the solid reaction byproducts. This design uses multiple sets of transmission devices 12 to drive the corrosion-resistant film 13 to move, which in turn moves the solid reaction byproducts to contact the solid scraper 15. Since the blade 151 of the solid scraper 15 is provided with an inclined surface 152, the accumulated solid reaction byproducts move along the inclined surface 152. The corrosion-resistant film 13 passes through the through groove 153. Under the action of the file 154 contacting the corrosion-resistant film 13, the solid reaction byproducts at the top of the bottom corrosion-resistant film 13 are continuously cleaned into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste. This facilitates the separation of reaction byproducts from the corrosion-resistant film 13, making it easy to clean and recycle the reaction byproducts without affecting the continued transport of magnesium nitride by the corrosion-resistant film 13, achieving continuous hydrolysis reaction and saving maintenance time.

[0045] It also includes a water inlet rinsing device 29 for cleaning the surface of the corrosion-resistant film 13. The water inlet rinsing device 29 includes an inlet 24 and a drain 26 opened on the reaction tank body. The drain 26 is located below the inlet 24. The inlet 24 is connected to an inlet valve 25, and the drain 26 is connected to a drain valve 27. This design uses the inlet valve 25 of the inlet flushing device 29 to spray cleaning fluid onto the corrosion-resistant membrane 13 through the inlet 24 on the reaction tank body, thus rinsing the moving corrosion-resistant membrane 13. The waste liquid after cleaning is discharged through the drain outlet 26 located below the inlet 24, and the waste liquid discharge is controlled by the drain valve 27, achieving stable operation of integrated continuous magnesium nitride hydrolysis for ammonia supply. The inlet flushing device 29 can also be filled with dilute acid to dissolve residual magnesium hydroxide. When hydrolyzing through the funnel 16, the sealing cover 161 is in the open state, and when cleaning with the flushing device 29, the sealing cover 161 is in the closed state to prevent the cleaning liquid from entering the collection tank 31 from the funnel 16.

[0046] The corrosion-resistant film 13 is made of one or more of the following materials: polyurethane, polytetrafluoroethylene, or polyethylene. The corrosion-resistant film 13 is replaceable and can be replaced with a new one after long-term use.

[0047] The reaction solution is one or more of tap water, deionized water, or ultrapure water; the cleaning solution injected into the inlet 24 of the water inlet rinsing device 29 is a dilute acid, including one or more of dilute sulfuric acid, dilute hydrochloric acid, or dilute nitric acid; the magnesium powder in the nitriding reaction includes one or more of spherical magnesium powder and block magnesium powder, wherein the particle size is at the micron or nanometer level.

[0048] This invention provides an integrated continuous magnesium nitridation hydrolysis ammonia supply method, comprising the following steps: S1, nitridation reaction: Magnesium powder is fed into storage tank 2 through the storage and feeding device 30 of the high-temperature reaction unit 1001 via the inlet 1 at the top of storage tank 2; the regulating valve 3 at the bottom of storage tank 2 is adjusted to control the magnesium powder to be uniformly conveyed to the inlet end of high-temperature reaction tank 4; the air inlet valve 6 on the pipeline connected to filter 7 is opened, and nitrogen gas is introduced into high-temperature reaction tank 4 through air inlet 5, so that magnesium powder and nitrogen gas undergo nitridation reaction in high-temperature reaction tank 4 to generate magnesium nitride; unreacted nitrogen gas is discharged from the outlet of high-temperature reaction tank 4, condensed by condenser 8 according to the airflow direction, and then flows back into high-temperature reaction tank 4 from the return port to re-participate in the nitridation reaction, thereby realizing nitrogen gas circulation.

[0049] S2, Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank 10 of the continuous hydrolysis reaction unit 1002. The reactant feeding tank 10 feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film 13 located at the bottom of the circulating reaction tank 28 through the feeder 11 at the bottom. The spray assembly 14 is started and the water inlet 23 connected to the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride on the top of the corrosion-resistant film 13. At the same time, multiple sets of transmission devices 12 arranged in a rectangular array in the reaction tank body are started to drive the corrosion-resistant film 13 connected between adjacent transmission devices 12 to move, and drive the magnesium nitride to flow with the corrosion-resistant film 13, so that the magnesium nitride is in full contact with the sprayed reaction liquid and the hydrolysis reaction continues to occur, generating ammonia and solid reaction byproducts.

[0050] S3. Waste Recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film 13 causes the solid reaction byproducts to move and come into contact with the solid scraper 15, continuously cleaning the solid reaction byproducts located at the top of the bottom corrosion-resistant film 13 into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste.

[0051] S4. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port 17 at the top of the circulating reaction tank 28. The exhaust valve 18 on the exhaust port 17 is opened, allowing the ammonia to enter the inlet of the dryer 19 through the pipeline. After being dried by the dryer 19, the ammonia is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. The vacuum pump 20 is started, and the dried ammonia is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, the ammonia is introduced into the ammonia collection chamber 22, completing the drying and sealed collection of ammonia.

[0052] S5. Continuous operation and maintenance: The system is kept in a closed state throughout the process, and raw materials and reaction liquid are continuously added to each unit to ensure continuous reaction. According to the cleanliness of the surface of the corrosion-resistant film 13, the sealing cover 161 of the funnel 16 is closed, the inlet valve 25 of the water inlet flushing device 29 is opened, and the cleaning liquid is sprayed onto the corrosion-resistant film 13 through the water inlet 24 on the reaction tank body. The waste liquid after cleaning is discharged through the drain outlet 26 located below the water inlet 24. The waste liquid discharge is controlled by the drain valve 27 to achieve stable operation of integrated continuous magnesium nitride hydrolysis ammonia supply.

[0053] Reference Figures 1-8 When continuous magnesium nitride hydrolysis is required to supply ammonia, the following is an example from this application.

[0054]

Example 1

[0055] S11, Nitriding Reaction: Micron-sized Mg powder is fed into storage tank 2 through the inlet 1 at the top of storage tank 2 via the storage and feeding device 30 of the high-temperature reaction unit 1001. When the temperature of the high-temperature nitriding reaction chamber rises to 1073K, the regulating valve 3 at the bottom of storage tank 2 is adjusted to control 10g of magnesium powder to be uniformly fed to the inlet end of the high-temperature reaction tank 4. At the same time, the air inlet valve 6 is opened, and nitrogen gas is introduced into the high-temperature reaction tank 4 through the air inlet 5, so that the magnesium powder and nitrogen gas undergo a nitriding reaction in the high-temperature reaction tank 4 to generate magnesium nitride. The reaction temperature of the high-temperature reaction tank 4 is 1073K, and the heat preservation reaction time is set to 10min. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction tank 4, condensed by the condenser 8 according to the airflow direction, and then flows back into the high-temperature reaction tank 4 through the return port to re-participate in the nitriding reaction, realizing nitrogen gas circulation.

[0056] S12, Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank 10 of the continuous hydrolysis reaction unit 1002. The reactant feeding tank 10 feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film 13 at the bottom of the circulating reaction tank 28 through the feeder 11 at the bottom. The spray assembly 14 is activated, and the water inlet 23 connected to the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride at the top of the corrosion-resistant film 13 at a water temperature of 353K. When the hydrolysis reaction temperature is 353K, the magnesium nitride hydrolysis reaction rate reaches its maximum. At the same time, multiple sets of transmission devices 12 arranged in a rectangular array within the reaction tank are activated, driving the corrosion-resistant film 13 connected between adjacent transmission devices 12 to rotate and move at a speed of 1 mm / min. -1 The movement drives the magnesium nitride to flow with the corrosion-resistant film 13, allowing the magnesium nitride to come into full contact with the sprayed hot water, and continuously undergo hydrolysis to generate ammonia and solid reaction byproducts.

[0057] S13 Waste Recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film 13 causes the solid reaction byproducts to move and come into contact with the solid scraper 15, continuously cleaning the solid reaction byproducts at the top of the bottom corrosion-resistant film 13 into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste.

[0058] S14. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port 17 at the top of the circulating reaction tank 28. The exhaust valve 18 on the exhaust port 17 is opened, allowing the ammonia to enter the inlet of the dryer 19 through the pipeline. After being dried by the dryer 19, the ammonia is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. The vacuum pump 20 is started, and the dried ammonia is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, the ammonia is introduced into the ammonia collection chamber 22, completing the drying and sealed collection of ammonia.

[0059] S15. Continuous Operation and Maintenance: Maintain the system in a closed state throughout the process, continuously replenish raw materials and reaction solutions to each unit to ensure continuous reaction; depending on the cleanliness of the surface of the corrosion-resistant film 13, close the sealing cover 161 of the funnel 16, open the inlet valve 25 of the water inlet flushing device 29, and spray cleaning solution onto the corrosion-resistant film 13 through the inlet 24 on the reaction tank body. The waste liquid after cleaning is discharged through the drain outlet 26 located below the inlet 24, and the waste liquid discharge is controlled by the drain valve 27, realizing the stable operation of the integrated continuous magnesium nitride hydrolysis ammonia supply. Magnesium nitride obtained in Example 1 was characterized by XRD, referring to... Figure 6 It can be seen that no magnesium powder residue remains after the nitriding reaction; refer to Figure 7 The hydrolysis rate of magnesium nitride reaches its maximum at a hydrolysis temperature of 353 K; among which, Figure 6In the figure, the X-axis represents 2θ (°) and the Y-axis represents the peak intensity (au). Figure 7 The X-axis represents the reaction time (s), and the Y-axis represents the ammonia production (ml / g).

[0060]

Example 2

[0061] S21, Nitriding Reaction: Micron-sized Mg powder is fed into storage tank 2 through the inlet 1 at the top of storage tank 2 via the storage and feeding device 30 of the high-temperature reaction unit 1001. When the temperature of the high-temperature nitriding reaction chamber rises to 1073K, the regulating valve 3 at the bottom of storage tank 2 is adjusted to control 10g of magnesium powder to be uniformly fed to the inlet end of the high-temperature reaction tank 4. At the same time, the air inlet valve 6 is opened, and nitrogen gas is introduced into the high-temperature reaction tank 4 through the air inlet 5, so that the magnesium powder and nitrogen gas undergo a nitriding reaction in the high-temperature reaction tank 4 to generate magnesium nitride. The reaction temperature of the high-temperature reaction tank 4 is 1073K, and the reaction time is set to 10min. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction tank 4, condensed by the condenser 8 according to the airflow direction, and then flows back into the high-temperature reaction tank 4 through the return port to participate in the nitriding reaction again, realizing nitrogen gas circulation.

[0062] S22, Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank 10 of the continuous hydrolysis reaction unit 1002. The reactant feeding tank 10 feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film 13 at the bottom of the circulating reaction tank 28 through the feeder 11 at the bottom. The spray assembly 14 is started, and the water inlet 23 connected to the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride at the top of the corrosion-resistant film 13 at a water temperature of 323K. At the same time, multiple sets of transmission devices 12 arranged in a rectangular array in the reaction tank body are started to drive the corrosion-resistant film 13 connected between adjacent transmission devices 12 to rotate and move at a speed of 1 mm / min. -1 The movement drives the magnesium nitride to flow with the corrosion-resistant film 13, allowing the magnesium nitride to come into full contact with the sprayed hot water, and continuously undergo hydrolysis to generate ammonia and solid reaction byproducts.

[0063] S23. Waste recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film 13 causes the solid reaction byproducts to move and come into contact with the solid scraper 15, continuously cleaning the solid reaction byproducts at the top of the bottom corrosion-resistant film 13 into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste.

[0064] S24. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port 17 at the top of the circulating reaction tank 28. The exhaust valve 18 on the exhaust port 17 is opened, allowing the ammonia to enter the inlet of the dryer 19 through the pipeline. After being dried by the dryer 19, the ammonia is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. The vacuum pump 20 is started, and the dried ammonia is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, the ammonia is introduced into the ammonia collection chamber 22, completing the drying and sealed collection of ammonia.

[0065] S25. Continuous operation and maintenance: Maintain the system in a closed state throughout the process, continuously replenish raw materials and reaction liquid to each unit to ensure continuous reaction; depending on the cleanliness of the surface of the corrosion-resistant film 13, close the sealing cover 161 of the funnel 16, open the inlet valve 25 of the water inlet flushing device 29, spray cleaning liquid onto the corrosion-resistant film 13 through the water inlet 24 on the reaction tank body, and discharge the waste liquid after cleaning through the drain outlet 26 located below the water inlet 24. Control the discharge of waste liquid through the drain valve 27 to achieve stable operation of integrated continuous magnesium nitride hydrolysis ammonia supply.

[0066]

Example 3

[0067] S31, Nitriding Reaction: Micron-sized Mg powder is fed into storage tank 2 through the inlet 1 at the top of storage tank 2 via the storage and feeding device 30 of the high-temperature reaction unit 1001. When the temperature of the high-temperature nitriding reaction chamber rises to 1073K, the regulating valve 3 at the bottom of storage tank 2 is adjusted to control 10g of magnesium powder to be uniformly fed to the inlet end of the high-temperature reaction tank 4. At the same time, the air inlet valve 6 is opened, and nitrogen gas is introduced into the high-temperature reaction tank 4 through the air inlet 5, so that the magnesium powder and nitrogen gas undergo a nitriding reaction in the high-temperature reaction tank 4 to generate magnesium nitride. The reaction temperature of the high-temperature reaction tank 4 is 1073K, and the reaction time is set to 10min. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction tank 4, condensed by the condenser 8 according to the airflow direction, and then flows back into the high-temperature reaction tank 4 through the return port to participate in the nitriding reaction again, realizing nitrogen gas circulation.

[0068] S32, Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank 10 of the continuous hydrolysis reaction unit 1002. The reactant feeding tank 10 feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film 13 at the bottom of the circulating reaction tank 28 through the feeder 11 at the bottom. The spray assembly 14 is started, and the water inlet 23 connected to the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride at the top of the corrosion-resistant film 13 at a water temperature of 303K. At the same time, multiple sets of transmission devices 12 arranged in a rectangular array in the reaction tank body are started to drive the corrosion-resistant film 13 connected between adjacent transmission devices 12 to rotate and move at a speed of 1 mm / min. -1The movement drives the magnesium nitride to flow with the corrosion-resistant film 13, allowing the magnesium nitride to come into full contact with the sprayed hot water, and continuously undergo hydrolysis to generate ammonia and solid reaction byproducts.

[0069] S33. Waste Recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film 13 causes the solid reaction byproducts to move and come into contact with the solid scraper 15, continuously cleaning the solid reaction byproducts at the top of the bottom corrosion-resistant film 13 into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste.

[0070] S34. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port 17 at the top of the circulating reaction tank 28. The exhaust valve 18 on the exhaust port 17 is opened, allowing the ammonia to enter the inlet of the dryer 19 through the pipeline. After being dried by the dryer 19, the ammonia is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. The vacuum pump 20 is started, and the dried ammonia is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, the ammonia is introduced into the ammonia collection chamber 22, completing the drying and sealed collection of ammonia.

[0071] S35. Continuous operation and maintenance: The system is kept in a closed state throughout the process, and raw materials and reaction liquid are continuously added to each unit to ensure continuous reaction. According to the cleanliness of the surface of the corrosion-resistant film 13, the sealing cover 161 of the funnel 16 is closed, the inlet valve 25 of the water inlet flushing device 29 is opened, and the cleaning liquid is sprayed onto the corrosion-resistant film 13 through the water inlet 24 on the reaction tank body. The waste liquid after cleaning is discharged through the drain outlet 26 located below the water inlet 24. The waste liquid discharge is controlled by the drain valve 27 to achieve stable operation of integrated continuous magnesium nitride hydrolysis ammonia supply.

[0072]

Example 4

[0073] S41, Nitriding Reaction: Micron-sized Mg powder is fed into storage tank 2 through the inlet 1 at the top of storage tank 2 via the storage and feeding device 30 of the high-temperature reaction unit 1001. When the temperature of the high-temperature nitriding reaction chamber rises to 1073K, the regulating valve 3 at the bottom of storage tank 2 is adjusted to control 10g of magnesium powder to be uniformly fed to the inlet end of the high-temperature reaction tank 4. At the same time, the air inlet valve 6 is opened, and nitrogen gas is introduced into the high-temperature reaction tank 4 through the air inlet 5, so that the magnesium powder and nitrogen gas undergo a nitriding reaction in the high-temperature reaction tank 4 to generate magnesium nitride. The reaction temperature of the high-temperature reaction tank 4 is 1073K, and the reaction time is set to 10min. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction tank 4, condensed by the condenser 8 according to the airflow direction, and then flows back into the high-temperature reaction tank 4 through the return port to participate in the nitriding reaction again, realizing nitrogen gas circulation.

[0074] S42, Hydrolysis Reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank 10 of the continuous hydrolysis reaction unit 1002. The reactant feeding tank 10 feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film 13 at the bottom of the circulating reaction tank 28 through the feeder 11 at the bottom. The spray assembly 14 is activated, and the water inlet 23 connected to the external water tank is connected through the pipeline to continuously spray the reaction liquid onto the magnesium nitride at the top of the corrosion-resistant film 13 at a water temperature of 273K. At the same time, multiple sets of transmission devices 12 arranged in a rectangular array within the reaction tank are activated to drive the corrosion-resistant film 13 connected between adjacent transmission devices 12 to rotate and move at a speed of 1 mm / min. -1 The movement drives the magnesium nitride to flow with the corrosion-resistant film 13, allowing the magnesium nitride to come into full contact with the sprayed hot water, and continuously undergo hydrolysis to generate ammonia and solid reaction byproducts.

[0075] S43. Waste recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film 13 causes the solid reaction byproducts to move and come into contact with the solid scraper 15, continuously cleaning the solid reaction byproducts at the top of the bottom corrosion-resistant film 13 into the funnel 16. The solid reaction byproducts fall through the funnel 16 into the collection tank 31 at the bottom of the reaction tank body, directly below the funnel 16, thus completing the cleaning and centralized collection of solid waste.

[0076] S44. Ammonia Collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port 17 at the top of the circulating reaction tank 28. The exhaust valve 18 on the exhaust port 17 is opened, allowing the ammonia to enter the inlet of the dryer 19 through the pipeline. After being dried by the dryer 19, the ammonia is discharged from the outlet of the dryer 19 and enters the inlet of the vacuum pump 20. The vacuum pump 20 is started, and the dried ammonia is transported from the exhaust port of the vacuum pump 20 to the connecting valve 21. After being regulated by the connecting valve 21, the ammonia is introduced into the ammonia collection chamber 22, completing the drying and sealed collection of ammonia.

[0077] S45. Continuous operation and maintenance: Maintain the system in a closed state throughout the process, continuously replenish raw materials and reaction liquid to each unit to ensure continuous reaction; depending on the cleanliness of the surface of the corrosion-resistant film 13, close the sealing cover 161 of the funnel 16, open the inlet valve 25 of the water inlet flushing device 29, spray cleaning liquid onto the corrosion-resistant film 13 through the water inlet 24 on the reaction tank body, and discharge the waste liquid after cleaning through the drain outlet 26 located below the water inlet 24. Control the discharge of waste liquid through the drain valve 27 to achieve stable operation of integrated continuous magnesium nitride hydrolysis ammonia supply.

[0078] It should be noted that, in this document, relational terms such as "first" and "second" are used only to distinguish one entity or operation from another, and do not necessarily require or imply any such actual relationship or order between these entities or operations. Furthermore, the terms "comprising," "including," or any other variations thereof are intended to cover non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements includes not only those elements but also other elements not expressly listed, or elements inherent to such process, method, article, or apparatus.

[0079] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit it. Although the present invention has been described in detail with reference to the above embodiments, those skilled in the art should understand that modifications or equivalent substitutions can still be made to the specific implementation of the present invention. Any modifications or equivalent substitutions that do not depart from the spirit and scope of the present invention should be covered within the scope of protection of the claims of the present invention.

Claims

1. An integrated continuous magnesium nitride hydrolysis ammonia supply system, characterized in that, include: The high-temperature reaction unit (1001), the continuous hydrolysis reaction unit (1002), the waste recycling unit (1004), and the control unit (32) are included. The high-temperature reaction unit (1001) is used for the nitriding reaction of magnesium powder and nitrogen, and the unreacted nitrogen is condensed and then refluxed to participate in the nitriding reaction again. The continuous hydrolysis reaction unit (1002) is used to receive magnesium nitride generated by the nitriding reaction in the high-temperature reaction unit (1001), drive the magnesium nitride to flow and contact the sprayed reaction liquid to undergo hydrolysis reaction, and generate ammonia and solid reaction byproducts. The waste recycling unit (1004) is used to clean and collect the solid reaction byproducts flowing within the hydrolysis reaction unit; The control unit (32) is connected to the high-temperature reaction unit (1001) and the continuous hydrolysis reaction unit (1002) respectively, and is used to collect the operating parameters of the nitriding reaction and the hydrolysis reaction in real time, analyze and process the collected operating parameters, and adjust the process parameters of the nitriding reaction and the hydrolysis reaction to control the magnesium powder and nitrogen to complete the nitriding reaction and the hydrolysis reaction stably.

2. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 1, characterized in that, The high-temperature reaction unit (1001) includes a storage and feeding device (30), a high-temperature reaction vessel (4), and a nitrogen circulation path (9); The storage and feeding device (30) includes a feed inlet (1), a storage tank (2) and a regulating valve (3). The feed inlet (1) is located at the top of the storage tank (2), and the regulating valve (3) is located at the bottom of the storage tank (2). The bottom of the regulating valve (3) is connected to the feed end of the high-temperature reaction vessel (4). The nitrogen circulation path (9) includes a condenser (8), the outlet of the high-temperature reaction vessel (4), the condenser (8) and the return port of the high-temperature reaction vessel (4) are connected in series in the order of gas flow direction, wherein the gas flow flows from the outlet through the condenser (8) and then back to the return port. The high-temperature reaction vessel (4) is equipped with a filter (7) through a pipeline, and the filter (7) is equipped with an air inlet (5) for conveying nitrogen through a pipeline, and the air inlet (5) is equipped with an air inlet valve (6); The control unit (32) includes a data acquisition module for real-time acquisition of operating parameters of nitriding and hydrolysis reactions, and a processing module for analyzing and adjusting the process parameters of nitriding and hydrolysis reactions based on the acquired operating parameters. The acquisition module includes a first temperature sensor installed in the high-temperature reaction vessel (4), and the processing module includes a PLC controller; The PLC controller is connected to the first temperature sensor in the high-temperature reaction vessel (4) and the heater in the high-temperature reaction vessel (4); The operating parameters of the nitriding reaction include the nitriding reaction temperature and the holding time; The process parameters for the nitriding reaction include a nitriding reaction temperature of 973-1073K and a holding time of 0-30min.

3. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 2, characterized in that, The continuous hydrolysis reaction unit (1002) includes a reactant feeding tank (10) for receiving the reactants for the formation of magnesium nitride by the nitriding reaction, a circulating reaction tank (28), and a spraying assembly (14) for spraying the reaction liquid. The circulating reaction tank (28) includes a reaction tank body, and multiple sets of transmission devices (12) are rotatably arranged inside the reaction tank body. Adjacent transmission devices (12) are connected by a corrosion-resistant film (13). The multiple sets of transmission devices (12) are arranged in a rectangular array. The corrosion-resistant film (13) surrounds the outer periphery of the rectangular array and extends to cover all transmission devices (12). The reactant feeding tank (10) is located inside the reaction tank body and is used to feed the top of the corrosion-resistant film (13) located at the bottom. A feeder (11) is provided at the bottom of the reactant feeding tank (10) and the feeder (11) is located above the corrosion-resistant film (13) at the bottom. The spray assembly (14) is disposed inside the reaction tank body and is used to spray the magnesium nitride reaction liquid onto the top of the corrosion-resistant film (13) located at the bottom. The spray assembly (14) includes a water tank (141) disposed inside the reaction tank body, a heating plate (142) for heating the reaction liquid in the water tank (141) to a set temperature, and a sprayer (143) for spraying the reaction liquid in the water tank (141) onto the surface of the corrosion-resistant film (13) located at the bottom. The heating plate (142) is located inside the water tank (141), the sprayer (143) is located below the water tank (141) and is connected to the water tank (141) through a pipe, and the water tank (141) is connected to the water inlet (23) of an external water tank through a pipe.

4. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 3, characterized in that, The transmission device (12) includes an electric motor (121) disposed on the side wall of the reaction tank body, and a conveying shaft (122) rotatably disposed inside the reaction tank body and connected to the output shaft of the electric motor (121); The corrosion-resistant film (13) is wound on the conveyor shaft (122) of the multiple sets of transmission devices (12); The acquisition module also includes a mass sensor in the feeder (11), a speed sensor on the conveyor shaft (122) and a second temperature sensor on the water tank (141). The PLC controller is connected to the mass sensor, the speed sensor, the second temperature sensor, the unloading valve in the feeder (11), the motor (121) and the heating plate (142) respectively. The operating parameters of the hydrolysis reaction include the hydrolysis reaction temperature, the transmission speed of the corrosion-resistant film (13), and the temperature of the reaction liquid in the water tank (141); The process parameters of the hydrolysis reaction include a hydrolysis reaction temperature of 273-373 K, a driving speed of the corrosion-resistant film (13) of 0-10 mmin -1 , and a reaction liquid temperature in the water tank (141) of 273-373 K.

5. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 1, characterized in that, It also includes an ammonia collection unit (1003) for receiving ammonia gas generated by the hydrolysis reaction in the continuous hydrolysis reaction unit (1002) and collecting the ammonia gas after drying; The ammonia collection unit (1003) includes an exhaust port (17), an exhaust valve (18), a dryer (19), a vacuum pump (20), a connecting valve (21), and an ammonia collection chamber (22); The exhaust port (17) is located at the top of the circulating reaction tank (28) of the continuous hydrolysis reaction unit (1002) and is used to discharge the ammonia gas generated by the hydrolysis reaction. The exhaust port (17) is equipped with an exhaust valve (18), which is connected to the air inlet of the dryer (19) through a pipeline. The air outlet of the dryer (19) is connected to the air inlet of the vacuum pump (20) through a pipeline. The exhaust port of the vacuum pump (20) is connected in sequence to the valve (21) and the ammonia collection chamber (22) via a pipeline.

6. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 3, characterized in that, The waste recycling unit (1004) includes a solid scraper (15), a funnel (16) and a collection tank (31). The solid scraper (15) and the funnel (16) are both located inside the reaction tank body. The solid scraper (15) is used to clean the solid reaction byproducts generated on the top of the corrosion-resistant film (13) at the bottom to the funnel (16). The solid scraper (15) is arranged in the lower part of the feeder (11) away from the spray assembly (14). The solid scraper (15) includes a blade body (151), the side wall of the blade body (151) is provided with a bevel (152), the side wall of the blade body (151) is provided with a through groove (153) that is connected to the bevel (152) and matches the corrosion-resistant film (13), and a file (154) that is in contact with the corrosion-resistant film (13) is provided on the bevel (152). The collection tank (31) is located at the bottom of the reaction tank body. The funnel (16) is connected to the collection tank (31). The collection tank (31) is directly below the funnel (16) and is used to collect the solid reaction byproducts discharged from the funnel (16). The funnel (16) is provided with a sealing cover (161) at the top. A rotating shaft (163) is rotatably provided on the reaction tank body. A paddle (162) connected to the sealing cover (161) is provided on the rotating shaft (163). The paddle (162) rotates with the rotating shaft (163) to drive the sealing cover (161) to open and close.

7. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 3, characterized in that, It also includes a water inlet rinsing device (29) for cleaning the surface of the corrosion-resistant film (13), the water inlet rinsing device (29) includes a water inlet (24) and a drain outlet (26) opened on the reaction tank body, the drain outlet (26) is located below the water inlet (24), the water inlet (24) is connected to a water inlet valve (25), and the drain outlet (26) is connected to a drain valve (27).

8. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 3, characterized in that, The corrosion-resistant film (13) is made of one or more of the following materials: polyurethane, polytetrafluoroethylene, or polyethylene.

9. The integrated continuous magnesium nitride hydrolysis ammonia supply system according to claim 7, characterized in that, The reaction solution is one or more of tap water, deionized water, or ultrapure water; The water inlet (24) of the water inlet flushing device (29) is injected with a dilute acid as the cleaning solution, which includes one or more of dilute sulfuric acid, dilute hydrochloric acid or dilute nitric acid; The magnesium powder used in the nitriding reaction includes one or more of spherical and blocky magnesium powders, wherein the particle size is at the micrometer or nanometer level.

10. An integrated continuous magnesium nitride hydrolysis ammonia supply method, applied to the integrated continuous magnesium nitride hydrolysis ammonia supply system as described in any one of claims 1-9, characterized in that, Includes the following steps: S1, Nitriding reaction: Magnesium powder is fed into storage tank (2) through the inlet (1) at the top of storage tank (2) via the storage and feeding device (30) of the high temperature reaction unit (1001). The regulating valve (3) at the bottom of storage tank (2) is adjusted to control the magnesium powder to be uniformly conveyed to the feed end of the high temperature reaction tank (4). Open the air inlet valve (6) on the pipeline connected to the filter (7), and introduce nitrogen gas into the high-temperature reaction tank (4) through the air inlet (5) so that the magnesium powder and nitrogen gas can undergo a nitriding reaction in the high-temperature reaction tank (4) to generate magnesium nitride. Unreacted nitrogen gas is discharged from the outlet of the high-temperature reaction vessel (4), condensed by the condenser (8) according to the gas flow direction, and then flows back into the high-temperature reaction vessel (4) from the return port to participate in the nitriding reaction again, thus realizing nitrogen gas circulation. S2, hydrolysis reaction: The magnesium nitride generated in step S1 is transported to the reactant feeding tank (10) of the continuous hydrolysis reaction unit (1002). The reactant feeding tank (10) feeds magnesium nitride at a constant speed to the top of the corrosion-resistant film (13) at the bottom of the circulating reaction tank (28) through the feeder (11) at the bottom. Start the spray assembly (14), connect the water inlet (23) of the external water tank through the pipeline, and continuously spray the reaction liquid onto the magnesium nitride on top of the corrosion-resistant film (13); At the same time, multiple sets of transmission devices (12) arranged in a rectangular array within the reaction tank are activated, driving the corrosion-resistant film (13) connected between adjacent transmission devices (12) to move, driving magnesium nitride to flow with the corrosion-resistant film (13), so that magnesium nitride can fully contact the sprayed reaction liquid and continuously undergo hydrolysis reaction to generate ammonia and solid reaction byproducts. S3. Waste recycling: During the hydrolysis reaction in step S2, the movement of the corrosion-resistant film (13) causes the solid reaction byproducts to move and come into contact with the solid scraper (15), continuously cleaning the solid reaction byproducts located at the top of the bottom corrosion-resistant film (13) into the funnel (16). The solid reaction byproducts fall through the funnel (16) into the collection tank (31) at the bottom of the reaction tank body directly below the funnel (16), thus completing the cleaning and centralized collection of solid waste. S4. Ammonia collection: The ammonia produced by the hydrolysis reaction in step S2 is discharged from the exhaust port (17) at the top of the circulating reaction tank (28). The exhaust valve (18) on the exhaust port (17) is opened so that the ammonia enters the inlet of the dryer (19) through the pipeline. After being dried by the dryer (19), it is discharged from the outlet of the dryer (19) and enters the inlet of the vacuum pump (20). Start the vacuum pump (20) to deliver the dried ammonia gas from the exhaust port of the vacuum pump (20) to the connecting valve (21). After being regulated by the connecting valve (21), the ammonia gas is introduced into the ammonia gas collection chamber (22) to complete the drying and sealed collection of ammonia gas. S5. Continuous operation and maintenance: Maintain the system in a closed state throughout the process, continuously replenish raw materials and reaction solutions to each unit, and ensure the continuous operation of the reaction; Based on the surface cleanliness of the corrosion-resistant film (13), close the sealing cover (161) of the funnel (16), open the inlet valve (25) of the inlet flushing device (29), spray the cleaning liquid onto the corrosion-resistant film (13) through the inlet (24) on the reaction tank body, and discharge the waste liquid after cleaning through the drain outlet (26) located below the inlet (24). Control the discharge of waste liquid through the drain valve (27) to achieve stable operation of integrated continuous magnesium nitride hydrolysis for ammonia supply.

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