Continuous reaction device and method applied to solid hydrogen storage material and application

By designing a multi-reactor continuous reaction device and adopting screw conveying units and reaction tubes, the heat transfer problem of magnesium-based hydrogen storage materials was solved, achieving efficient continuous production. It is suitable for the reaction of materials in various phases and promotes the development of the hydrogen energy industry.

CN121648832APending Publication Date: 2026-03-13大连富德金煜新能源有限公司
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2024-09-11
Publication Date
2026-03-13

AI Technical Summary

Technical Problem

Existing technologies make it difficult to achieve efficient and continuous production of magnesium-based hydrogen storage materials. The heat transfer problem has not been effectively solved, and the equipment cannot achieve continuous operation, which affects its application and promotion in energy storage, chemical industry, metallurgy, transportation, construction and other fields.

Method used

Design a continuous reaction device comprising multiple reactors, employing screw conveyor units and reaction tubes, combined with stirring shafts, jacket structures, and heat exchange media to achieve efficient heat transfer and mixing. It is suitable for reactions of materials in various phases and can meet different needs through series and parallel combinations.

Benefits of technology

It has enabled the efficient and continuous production of magnesium-based hydrogen storage materials, improved heat transfer efficiency, prevented particle sintering, and is applicable to the reaction of materials in various phases, thus promoting the development of the hydrogen energy industry.

✦ Generated by Eureka AI based on patent content.

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Abstract

The invention provides a continuous reaction device and method applied to a solid hydrogen storage material and application, the reaction device comprises a plurality of reactors, and when there are a plurality of reactors, the plurality of reactors are connected in parallel and / or in series; the reactor comprises a driving unit, a screw conveying unit and a reaction tube, the screw conveying unit comprises a plurality of stirring shafts which are arranged in parallel, and spiral blades are arranged on the stirring shafts; the plurality of stirring shafts are arranged in the reaction tube in a penetrating manner; the plurality of driving units are respectively connected with the plurality of stirring shafts and drive the plurality of stirring shafts to rotate; and a jacket is sleeved outside the reaction tube. The continuous reaction device applied to the solid hydrogen storage material has the advantages of high heat exchange efficiency and uniform mixing, can realize a series of processes of loading, production, unloading and the like, and has the characteristics of stirring solid-solid, solid-liquid, liquid-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid, gas-liquid and the like. And the method has very good application prospect and large-scale industrial popularization potential in the field of reaction of various phase-state materials such as gas-solid and the like.
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Description

Technical Field

[0001] This invention relates to reaction tube technology, and more particularly to a continuous reaction apparatus, method, and application for solid hydrogen storage materials. Background Technology

[0002] Hydrogen energy, as a clean and efficient energy source, holds significant strategic importance in addressing the global energy crisis and environmental pollution. Developing efficient hydrogen storage technologies is crucial for reducing hydrogen costs and enabling large-scale application. Magnesium hydride-based hydrogen storage materials can reversibly store and release hydrogen under certain temperature and pressure conditions, possessing advantages such as large hydrogen storage capacity, high energy density, safety, efficiency, convenience, high hydrogen purity, and excellent cycle life performance, making them considered one of the effective means of future hydrogen storage and transportation. However, their high mechanical stability (hydrogen release enthalpy change ΔH = 75 kJ / mol) and slow dehydrogenation kinetics below 300℃ limit their practical application. Currently, researchers mainly optimize and modify magnesium-based hydrogen storage materials through alloying, nano-sizing, catalyst addition, and composite methods. Among these, optimization techniques such as reducing particle size to shorten the spatiotemporal mass transfer distance and adding catalysts integrated with the magnesium hydride matrix are difficult to implement on a large scale in engineering. Furthermore, hydrogen storage materials exhibit significant thermal effects during their preparation and storage processes. Due to the poor thermal conductivity of powder materials, the heat of hydrogen absorption is difficult to remove effectively and promptly, leading to problems such as particle sintering and agglomeration, which severely impacts the hydrogen absorption and desorption reaction rates and cycle life of the hydrogen storage materials. Traditionally, methods such as adding thermally conductive agents to hydrogen storage material powders, powder briquetting, and arranging coil or tube heat exchange structures within containers can be used to enhance reaction heat transfer. However, the heat transfer problem remains unresolved, and continuous operation of the devices is not feasible. These issues severely hinder the large-scale preparation, application, and promotion of solid-state hydrogen storage materials made of metal hydrides.

[0003] Therefore, there is an urgent need to develop a reactor capable of a one-pot process for preparing magnesium-based hydrogen storage materials. This reactor should not only enable the hydrogenation reaction of magnesium powder but also effectively enhance heat and mass transfer, reduce particle size, facilitate interaction between the catalyst and the magnesium hydride matrix, prevent particle sintering and agglomeration, and improve the processing capacity of the device. Ultimately, this would allow for large-scale, continuous, and efficient preparation of magnesium-based hydrogen storage materials. This will greatly promote the application and widespread use of magnesium-based hydrogen storage materials in energy storage, chemical engineering, metallurgy, transportation, and construction. Summary of the Invention

[0004] The purpose of this invention is to address the problem that existing screw reactors are unsuitable for the production of hydrogen storage materials by proposing a continuous reaction device for solid hydrogen storage materials. This device has the advantages of high heat exchange efficiency and uniform mixing, and can realize a series of continuous and efficient production processes such as loading, production, and unloading. It has very good application prospects and large-scale industrial promotion potential in the field of material reactions involving various phases such as solid-solid, solid-liquid, liquid-liquid, gas-liquid, and gas-solid reactions. It is especially suitable for the continuous and efficient production of hydrogen storage materials, solving the bottleneck problems of existing hydrogen storage and release technologies, promoting the development of the hydrogen energy industry, and meeting the future needs of large-scale hydrogen storage and use.

[0005] It should be noted that, in this invention, unless otherwise specified, the specific meaning of "comprising" in relation to composition and description includes both open-ended meanings such as "comprising," "including," etc., and closed-ended meanings such as "composed of," "consisting of," etc., and similar meanings.

[0006] To achieve the above objectives, the technical solution adopted by the present invention is: a continuous reaction device for solid hydrogen storage materials, comprising one or more reactors, wherein when there are multiple reactors, the multiple reactors are connected in parallel and / or in series, and the reactor includes a drive unit, a screw conveying unit, and a reaction tube; the screw conveying unit includes multiple parallel stirring shafts, and the stirring shafts are provided with helical blades; the multiple stirring shafts pass through the reaction tube; there are multiple drive units, each connected to multiple stirring shafts, driving the multiple stirring shafts to rotate; the reaction tube is fitted with a jacket.

[0007] Furthermore, the drive unit includes a motor, a reducer, and a sealing structure, which can be a magnetic coupler, a mechanical seal, or a packing seal. The motor is connected to the stirring shaft via the reducer, and the sealing structure is used to seal between the reducer and the reaction tube. When the sealing structure uses a magnetic coupler, the motor provides power, connects to the reducer, and the reducer amplifies the motor's output torque before transmitting it to the magnetic coupler. The inner magnet of the magnetic coupler is connected to the stirring shaft, and the outer magnet is connected to the reducer's output shaft. The reducer's output shaft is connected to the stirring shaft inside the reaction tube via a coupling to synchronously transmit the drive torque.

[0008] Furthermore, the reaction tube is a horizontal, high-temperature and pressure-resistant reactor. The reaction tube is made of high-temperature resistant material and has a high-pressure resistant structure to meet the reaction temperature and pressure requirements for material production.

[0009] Furthermore, a safety valve port is provided on the reaction tube.

[0010] Furthermore, the reaction tube is provided with an inlet and an outlet. The inlet includes one or more of a gas inlet, a liquid inlet, and a solid inlet, and the outlet includes one or more of a gas outlet, a liquid outlet, and a solid outlet. A flow valve is provided on the inlet, and a flow meter is provided on the outlet.

[0011] Furthermore, a temperature sensor and a pressure sensor are installed inside the reaction tube.

[0012] Furthermore, a heat exchange medium is provided within the jacket, including but not limited to heat transfer oil. The jacket heat exchange medium inlet is located near the reaction tube outlet, and the jacket heat exchange medium outlet is located near the reaction tube inlet.

[0013] Furthermore, there are multiple jackets arranged sequentially along the axial direction of the reaction tube, each controlling the temperature independently. The number of jackets is 2-6. The jackets can be independently controlled according to different reaction stages.

[0014] Furthermore, an insulation layer is provided on the outer side of the jacket.

[0015] Furthermore, the jacket is provided with fins to increase the heat dissipation area.

[0016] Furthermore, the reaction tube contains spheres, which are selected from steel balls, zirconium balls, ceramics, etc. These spheres can further break down the raw materials, increase heat transfer, prevent dead zones, and also serve as catalyst carriers.

[0017] Furthermore, a gas distributor is laid axially at the bottom of the inner side of the reaction tube.

[0018] Furthermore, the number of stirring shafts is 2-4.

[0019] Furthermore, the multiple stirring shafts rotate in the same direction and / or in opposite directions.

[0020] Furthermore, the multiple stirring shafts rotate at the same speed and / or at different speeds.

[0021] Furthermore, the gas distributor consists of multiple arc-shaped plates disposed at the bottom inner side of the reaction tube, which cooperate with multiple stirring shafts. Each arc-shaped plate maintains a certain gap with the helical blades on the stirring shafts. To address the issue that having two shafts inside the reaction tube would result in a larger vertical space than horizontal space within the reactor, this invention incorporates arc-shaped plates at the bottom of the reaction tube to reduce the bottom space, preventing material from accumulating and becoming trapped, thus avoiding dead zones.

[0022] Furthermore, the chamber between the lower part of the arc plate and the inner wall of the reaction tube is connected to the cold hydrogen inlet. A vent hole is provided on the arc plate, and the cold hydrogen inlet is located on the end cap of the reaction tube for introducing cold hydrogen. Raw material gas (such as hydrogen) enters the reaction tube through a gas inlet and / or a gas distributor. The raw material gas entering through the gas distributor can agitate the material inside the reaction tube and achieve heat transfer. When magnesium powder reacts with hydrogen to prepare magnesium hydride or when magnesium hydride is hydrolyzed, hydrogen enters the reaction tube through the gas inlet and the gas distributor.

[0023] Furthermore, the vent holes are nanopores, allowing hydrogen gas to freely enter and exit while ensuring that magnesium powder does not leak below the multiple curved plates. The nanopores are created by laser drilling.

[0024] Furthermore, the spiral blades of the screw conveyor unit are welded to the stirring shaft, and the pitch of the spiral blades is determined by the hydrogen storage / release time of the reactant and the total length of the reaction tube.

[0025] Furthermore, the helical blades on the multiple stirring shafts are arranged in a staggered pattern, with the installation gaps ensuring proper meshing between the shafts. This staggered arrangement of the helical blades enables the mutual transfer and compression of materials. The helical blades transfer materials according to the reaction requirements; while one stirring shaft's helical blade is radially tumbling and mixing the material, it also transfers material to the helical blades of another stirring shaft. This radial transfer of material within the helical blades increases the reaction time within the reaction tube and ensures uniform mixing of the materials.

[0026] Furthermore, one end of the stirring shaft is connected to the drive unit, and the other end is provided with a thrust bearing.

[0027] Furthermore, the stirring shaft is a hollow shaft, with rotary joints connecting the input and output ends of the hollow shaft. When the stirring shaft is a hollow shaft, a mechanical seal or a packing seal is selected as the sealing structure.

[0028] Furthermore, a heat exchange medium is circulated through the hollow shaft, including but not limited to heat transfer oil. The heat exchange medium can displace excess reaction heat generated inside the reaction tube, and can also provide a heat source medium during the hydrogen release stage of the reaction tube to heat the inside of the reaction tube and ensure the temperature uniformity of the entire reaction tube.

[0029] Furthermore, the spiral blade is a blade that can propel the material forward and / or knead the material. Preferably, the spiral blade is a continuous spiral blade, a single diamond-shaped blade, or a toothed blade.

[0030] Furthermore, the number of reactors is 2-8, preferably 2-4.

[0031] Furthermore, when multiple reactors are connected in series, they are sequentially connected end-to-end. Taking two reactors connected in series as an example, the outlet of the first-stage reactor is connected to the inlet of the second-stage reactor. The reaction tube of the first-stage reactor is fixed above the reaction tube of the second-stage reactor and communicates with it. The second-stage reactor is equipped with legs to jointly support both reactors. The spiral blades of the second-stage reactor push the material in the opposite direction, effectively conveying the material from the first-stage reactor to the inlet of the second-stage reactor. Sufficient installation distance is maintained between the first-stage and second-stage reactors, and each reactor is equipped with an independent heating jacket structure to meet the temperature requirements of each reactor at different reaction stages.

[0032] Furthermore, when multiple reactors are connected in series, a pulverizing device is installed in the pipeline between adjacent reactors.

[0033] Furthermore, the crushing device is a high-speed shear head or a crushing valve. The material exiting the upper-stage reactor is crushed by the high-speed shear or crushing valve and then discharged to the lower-stage reactor. High-speed shearing can crush falling materials (e.g., magnesium powder) through high-speed shearing, refining the material, reducing particle size, accelerating the hydrogen storage rate, and increasing the hydrogen storage density. The crushing valve can shear and crush the material passing through the valve body through the relative movement of the stator and rotor within the valve.

[0034] Furthermore, when multiple reactors are connected in series, level gauges are installed in the pipelines between adjacent reactors. Taking two reactors connected in series as an example, to better monitor the loading and unloading between the two reactors, level gauges are installed in the pipeline between the first-stage reactor and the second-stage reactor, below the high-speed shear head. When the material level in the pipeline is higher than the set value, it is determined whether the stirring shafts of the first-stage and second-stage reactors are rotating. If stirring is still ongoing, it is preliminarily determined that the spiral stirring speed of the second-stage reactor is low, and the stirring shaft speed of the second-stage reactor needs to be increased to speed up the discharge and prevent material accumulation from affecting the entire reaction device. When it is determined that the stirring shaft of the second-stage reactor is not rotating, the first-stage reactor is immediately stopped to prevent the second-stage reactor from getting stuck in the entire second-stage reaction tube due to material accumulation.

[0035] Furthermore, the continuous reaction device applied to solid hydrogen storage materials also includes a control unit, which is communicatively connected to a temperature sensor, a pressure sensor, a motor, a flow meter, a flow valve, and a level gauge.

[0036] Another objective of this invention is to disclose a continuous reaction method for solid hydrogen storage materials, comprising the following steps: raw materials enter the reaction tube through the feed inlet, a drive unit drives multiple stirring shafts with helical blades to rotate, the helical blades rotate with the stirring shafts, pushing the raw materials from the reactor feed inlet to the reactor outlet, during which the raw materials react under specified temperature, pressure and stirring speed, the raw materials are repeatedly crushed and squeezed by multiple stirring shafts during the reaction, achieving layer-by-layer peeling and effective kneading of the raw materials, and the heat generated during the reaction is removed in time by a heat exchange device.

[0037] Furthermore, the continuous magnesium-based hydrogen storage material pyrolysis hydrogen production reaction conditions include: a temperature of 150-400℃, a pressure of 0.01-1.5MPa, and a stirring shaft speed of 20-40rpm.

[0038] Furthermore, the reaction conditions for hydrogen absorption by continuous magnesium-based hydrogen storage materials include: a temperature of 25-420℃, a pressure of 0.2-10MPa, and a stirring shaft speed of 5-100rpm.

[0039] Furthermore, the continuous magnesium-based hydrogen storage material hydrolysis hydrogen production reaction conditions include: a temperature of 30-300℃, a pressure of 0.1-2.0 MPa, and a stirring shaft speed of 5-100 rpm.

[0040] Another object of the present invention is to disclose the use of a continuous reaction device for solid hydrogen storage materials in the fields of solid-solid reaction, liquid-solid reaction, gas-solid reaction, liquid-liquid reaction or gas-liquid reaction.

[0041] Furthermore, the continuous reaction device applied to solid hydrogen storage materials is particularly suitable for hydrogen absorption by magnesium-based hydrogen storage materials (such as magnesium hydride preparation), hydrogen production by hydrolysis of magnesium-based hydrogen storage materials, hydrogen production by hydrolysis-pyrolysis coupling of magnesium-based hydrogen storage materials, hydrogen production by pyrolysis of magnesium-based hydrogen storage materials, or thermal storage of thermochemical thermal storage materials.

[0042] Furthermore, the thermochemical thermal storage material includes carbonate thermal storage, hydroxide thermal storage, oxide thermal storage, or metal hydride thermal storage, etc.

[0043] Another objective of this invention is to disclose a continuous reaction system for solid hydrogen storage materials, comprising a raw material silo, an isolation silo, the continuous reaction device for solid hydrogen storage materials, and a collection tank connected in sequence.

[0044] Furthermore, there are multiple isolation chambers connected in parallel, meaning that the inlet and outlet of each isolation chamber are respectively connected to the raw material warehouse and the continuous reaction device used for solid hydrogen storage materials. The isolation chamber is a key piece of equipment for raw material transportation, used for pressure regulation of the raw materials.

[0045] Furthermore, the isolation chamber is equipped with a heating device for heating the raw materials.

[0046] Furthermore, the isolation chamber is connected to an inflation tank and a first gas recovery tank, which are used to replenish or replace the pressure in the isolation chamber.

[0047] Furthermore, the continuous reaction device applied to solid hydrogen storage materials is placed at an angle of 0 to 20 degrees to the horizontal direction, that is, the feed end of the reaction tube is higher than the discharge end, so as to ensure that the material is completely discharged under the action of stirring and gravity.

[0048] Furthermore, the collection tank is connected to a second gas recovery tank and a filling tank. The collection tank is used to hold the finished product (such as magnesium hydride), and the gas (such as hydrogen) in the collection tank is collected through the second gas recovery tank. The filling tank fills the collection tank with argon gas for inert gas protection.

[0049] Furthermore, a buffer tank is provided between the isolation chamber and the continuous reaction device applied to solid hydrogen storage materials. When there are multiple isolation chambers, the multiple isolation chambers alternately feed and fill with hydrogen. In order to ensure that the material entering the reactor is uninterrupted, a buffer tank is added between the isolation chamber and the reactor to ensure that the feeding is uninterrupted during the switching process of multiple isolation chambers.

[0050] Furthermore, a cooling tank is provided between the continuous reaction device for solid hydrogen storage materials and the collection tank.

[0051] Furthermore, the continuous reaction system applied to solid hydrogen storage materials also includes a heat transfer oil furnace, wherein the heat transfer oil inlet and outlet are connected to the outlet and inlet of the jacket, respectively.

[0052] Another objective of this invention is to disclose a continuous reaction method for solid-state hydrogen storage materials, comprising the following steps: raw materials in a feedstock silo are unloaded by gravity into an isolation silo; the raw materials are heated and / or pressurized in the isolation silo before entering a continuous reaction device for solid-state hydrogen storage materials; and the reacted materials are cooled, collected, and stored. This method enables the simultaneous completion of hydrogen storage and release reactions and unloading, thereby realizing a series of processes including loading, production, and unloading.

[0053] Furthermore, the two isolation chambers are connected in parallel to alternately supply raw materials to the continuous reaction device used for solid hydrogen storage materials, thereby achieving continuous feeding.

[0054] Furthermore, the raw material enters the reaction tube through the feed inlet, and the drive unit drives multiple stirring shafts with helical blades to rotate. The helical blades rotate with the stirring shafts, pushing the raw material from the reactor feed inlet to the reactor outlet. During this process, the raw material reacts under specified temperature, pressure and stirring speed. During the reaction, the raw material is repeatedly crushed and squeezed by multiple stirring shafts, realizing the layer-by-layer peeling and effective kneading of the raw material. The heat generated during the reaction is removed in time by the heat exchange device.

[0055] Furthermore, the gas pipeline connected to the isolation chamber is pressurized or purged as needed by the reaction device.

[0056] Furthermore, the continuous reaction device applied to solid hydrogen storage materials comprises multiple reactors connected in series and / or in parallel. Each reactor can individually control the reaction temperature and adjust the stirring speed according to the reaction stage to achieve the best mixing effect.

[0057] Another object of the present invention is to disclose the use of a continuous reaction system for solid hydrogen storage materials in the fields of solid-solid reaction, liquid-solid reaction, gas-solid reaction, liquid-liquid reaction or gas-liquid reaction.

[0058] Furthermore, the continuous reaction system applied to solid hydrogen storage materials is particularly suitable for hydrogen absorption by magnesium-based hydrogen storage materials (such as the preparation of magnesium hydride), hydrogen production by hydrolysis of magnesium-based hydrogen storage materials, hydrogen production by hydrolysis-pyrolysis coupling of magnesium-based hydrogen storage materials, hydrogen production by pyrolysis of magnesium-based hydrogen storage materials, or thermal storage of thermochemical thermal storage materials.

[0059] Furthermore, the thermochemical thermal storage material includes carbonate thermal storage, hydroxide thermal storage, oxide thermal storage, or metal hydride thermal storage, etc.

[0060] This invention relates to a continuous reaction apparatus, method, and application for solid hydrogen storage materials, and has the following advantages compared with existing technologies:

[0061] 1) High-efficiency heat exchange;

[0062] The reactor used in this invention is a high-efficiency heat exchange reactor integrating multiple heat transfer structures. The reaction tube is a horizontal tubular structure with a large specific surface area, a large heat transfer area per unit volume, and high heat transfer efficiency. In addition to introducing hydrogen through the reaction gas source inlet, a gas (such as hydrogen) distributor is also installed at the bottom of the reaction tube. This distributor not only purges and loosens the material (such as magnesium powder) on the reactor wall but also allows hydrogen to pass through the material layer from bottom to top, enhancing the heat transfer reaction. When the reaction is violently exothermic, a lower-temperature gas (cold hydrogen) can be introduced through the gas distributor to effectively replace the heat. Inside the reaction tube, the stirring spiral blades continuously tumble and mix the material during the reaction, effectively dissipating the heat from the reaction tube wall. A heat transfer oil jacket is installed outside the reaction tube, and multiple fins are welded to the outer wall of the reaction tube to enhance the heat transfer of the heat from the heat transfer oil to the reaction tube. The stirring shaft can be a hollow shaft, and a heat exchange medium can be introduced inside to homogenize the entire temperature field.

[0063] 2) Applicable to reactions with different reaction times;

[0064] The driving device used in this invention consists of a motor and a reducer. The speed of the stirring shaft can be adjusted by a frequency converter, so the material conveying time in the reaction tube is adjustable, which is suitable for reactions of various reactants with different reaction times.

[0065] 3) Multiple reactors can be freely combined in series and / or parallel;

[0066] Multiple reactors can be freely combined in series and / or parallel. Series connection allows for adjustment of reaction time, while parallel connection allows for adjustment of throughput. The outlet of the upper reactor is connected to the inlet of the lower reactor to achieve series connection, which is suitable for materials with long reaction times. The feeding system connects to the feed inlets of multiple reactors to achieve parallel connection, ensuring large-scale material throughput.

[0067] 4) Wide range of applications;

[0068] This invention has a wide range of applications in continuous reaction devices for solid hydrogen storage materials, and is suitable for material reactions in various phases such as solid-solid, solid-liquid, liquid-liquid, gas-liquid, and gas-solid.

[0069] 5) Independent temperature control;

[0070] When multiple reactors are connected in series or in parallel, each reactor is independently equipped with a heat transfer oil jacket. The temperature of the reaction tube of each reactor can be independently controlled according to the process requirements of the reaction process, so as to meet the different temperature and pressure requirements of different stages of the reaction.

[0071] 6) Advantages of horizontal containers;

[0072] The reaction tube of this invention is a horizontal reaction vessel, which has a smaller height-to-diameter ratio than a vertical reaction tube of the same volume. After the hydrogen gas is introduced, the pressure drop is small and the gas loss is small, which is beneficial to the rapid reaction of materials and the expansion of product volume.

[0073] 7) Skid-mounted design takes up little space and is easy to scale up;

[0074] Multiple reactors can be connected in series or in parallel, with similar overall structural dimensions, facilitating skid-mounted design and requiring minimal footprint in various engineering applications. Furthermore, they are easily scaled up for large-scale production.

[0075] 8) Different screw types process different types of materials, resulting in a wide range of raw materials that can be processed;

[0076] The reactor of this invention can employ various blade forms, such as continuous spiral blades, single diamond-shaped blades, or toothed blades, to push materials in different ways, including plug flow, turbulent mixture, and kneading. The reactor is suitable for various materials and reaction conditions.

[0077] 9) The high-speed shear head removes the oxide layer or magnesium hydride from the surface of magnesium hydride, shortening the reaction time and increasing the hydrogen storage capacity;

[0078] The present invention provides a high-speed shear head in the pipeline between adjacent reactors. The high-speed shear head shears and crushes the material discharged from the outlet, which not only refines the material, but also effectively disperses the material, making it easier for the next stage reactor to uniformly transport the material.

[0079] 10) A sphere is installed inside the reaction tube;

[0080] This invention allows for the addition of spheres within the reaction tube. These spheres move along with the helical blades within the tube, and their rising and falling motion during this movement acts as a crushing and breaking agent for the materials. Furthermore, the spheres can be coated with catalyst components as needed for the material reaction, dynamically participating in the reaction process. As good conductors of heat, the spheres absorb heat within the reaction tube and conduct it during their movement.

[0081] 12) Continuous production: Magnesium powder isolation chamber + continuous reaction unit (plug flow) applied to solid hydrogen storage materials;

[0082] This invention relates to a continuous reaction system for solid-state hydrogen storage materials. Raw materials are transported from a raw material silo to the reaction unit via an isolation silo, which is a key component for continuous raw material transport. The raw materials are heated and pressurized within the isolation silo before being transported to the reaction unit. Two isolation silos are connected in parallel with the reaction unit, alternately supplying materials to achieve continuous feeding. After feeding into the isolation silos, the reaction unit activates its stirring device under positive pressure. The raw materials react at specified temperature, pressure, and stirring speed. The stirring shaft speed is controlled within the reaction unit, causing the spiral blades to push the raw materials horizontally from the inlet to the outlet. The hydrogen storage, release, and unloading processes are completed simultaneously, thus realizing a series of continuous production processes including loading, production, and unloading.

[0083] 13) The dual-axis arrangement of helical blades can effectively delay the reaction time of materials in the reactor by mixing and kneading materials through dual-axis mixing.

[0084] By precisely controlling the kneading gap between the spiral blades, the stirring shaft and blades work together to effectively scrape and collide the material in the gap during the rotation of the blade assembly. The powder particles are effectively squeezed and crushed. The spiral blades continuously stir, and the material is squeezed and crushed multiple times in the reactor for a long time, achieving the layer-by-layer peeling of the material. At the same time, it can also achieve the effective kneading of catalysts and additives at high temperatures, thereby achieving the purpose of shearing, mixing and kneading the material. Attached Figure Description

[0085] Figure 1 A schematic diagram of a continuous reaction device used in solid hydrogen storage materials;

[0086] Figure 2 for Figure 1 Schematic diagram of the cross-section of the reaction tube;

[0087] Figure 3 This is a schematic diagram of a continuous reaction system applied to solid hydrogen storage materials. Detailed Implementation

[0088] The technical solutions of the embodiments of this application will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only a part of the embodiments of this application, and not all of them. All other embodiments obtained by those skilled in the art based on the embodiments of this application without creative effort are within the scope of protection of this application.

[0089] In the description of this application, it should be noted that, unless otherwise expressly specified and limited, the terms "connected" and "linked" should be interpreted broadly. For example, they can refer to a fixed connection, a detachable connection, or an integral connection; they can refer to a mechanical connection, an electrical connection, or a connection that allows for mutual communication; they can refer to a direct connection or an indirect connection through an intermediate medium; they can refer to the internal communication of two elements or the interaction between two elements. Those skilled in the art can understand the specific meaning of the above terms in this application according to the specific circumstances. In the description of this application, "multiple" means two or more, unless otherwise expressly and specifically limited. Furthermore, the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Thus, features defined with "first" and "second" may explicitly or implicitly include one or more features.

[0090] The following disclosure provides many different implementations or examples for carrying out different structures of this application. To simplify the disclosure of this application, the components and arrangements of specific examples are described below. Of course, these are merely examples and are not intended to limit this application.

[0091] Example 1: Hydrogen production by magnesium hydride pyrolysis

[0092] This embodiment discloses a continuous reaction device for solid hydrogen storage materials, comprising two reactors connected in parallel.

[0093] The reactor is as follows Figure 1 The device includes a drive unit, a screw conveyor unit, and a reaction tube. The screw conveyor unit includes two parallel stirring shafts 9, each with a helical blade 8. The two stirring shafts pass through the reaction tube and are at the same horizontal height. There are two drive units, each connected to one of the two stirring shafts 9, which drive the two stirring shafts 9 to rotate inward. The reaction tube is fitted with a jacket 6.

[0094] The drive unit includes a motor 1, a reducer 2, and a magnetic coupler 3. The motor 1 is connected to the stirring shaft 9 via the reducer 2 and the magnetic coupler 3, driving the stirring shaft 9 to rotate. The motor 1 provides power, and the reducer 2 amplifies the output torque of the motor before transmitting it to the magnetic coupler 3. The inner magnet of the magnetic coupler 3 is connected to the stirring shaft 9, and the outer magnet is connected to the output shaft of the reducer 2. The output shaft of the reducer 2 is connected to the stirring shaft 9 inside the reactor via a coupling, synchronously transmitting the drive torque.

[0095] The reaction tube is a horizontal, high-temperature and pressure-resistant reactor. It is made of high-temperature resistant material and has a high-pressure resistant structure to meet the reaction temperature and pressure requirements for material production. A solid inlet 10 is located at the top of one end of the reaction tube, while a gas outlet 13 and a solid outlet 11 are located at the top and bottom of the other end, respectively. Magnesium hydride enters the reaction tube through the solid inlet 10, and the solid product obtained from the pyrolysis of magnesium hydride is discharged through the solid outlet 11, while hydrogen gas is discharged through the gas outlet 13. A flow meter is installed at the gas outlet 13. Temperature and pressure sensors are installed inside the reaction tube. A safety valve is also installed on the reaction tube.

[0096] The jacket 6 contains a heat exchange medium, which in this embodiment is heat transfer oil. The heat exchange medium inlet of the jacket 6 is located near the gas outlet 13 and the solid outlet 11, and the heat exchange medium outlet of the jacket 6 is located near the solid inlet 10. An insulation layer 4 is provided on the outside of the jacket 6. Fins are provided inside the jacket 6 to increase the heat exchange area.

[0097] The spiral blades 8 of the screw conveyor unit are welded to the stirring shaft. The pitch of the spiral blades is determined by the hydrogen storage / release time of the reactants and the total length of the reaction tube. The spiral blades 8 on the two stirring shafts are staggered, and the installation gap is sufficient to ensure the meshing effect between the two stirring shafts. The staggered arrangement of the spiral blades on the two stirring shafts enables mutual transfer and compression of materials. The spiral blades transfer materials according to the reaction requirements. During the radial mixing of materials by one stirring shaft's spiral blade, materials are also transferred to the spiral blades of the other stirring shaft, thus achieving radial transfer of materials within the spiral blades, increasing the reaction time in the reaction tube, and uniformly mixing the materials. The spiral blades of the two stirring shafts rotate at opposite speeds, achieving layer-by-layer peeling and effective kneading of the raw materials. The end of the stirring shaft closest to the material movement direction is connected to a thrust bearing, which provides axial reaction force to the spiral blades along with the material. The spiral blades 8 are continuous spiral blades or single diamond-shaped blades.

[0098] The continuous reaction device for solid hydrogen storage materials also includes a control unit, which is communicatively connected to a temperature sensor, a pressure sensor, a motor, a flow meter, a flow valve, and a level gauge.

[0099] When the magnesium-based solid hydrogen storage material releases hydrogen, in this embodiment, the continuous reaction device used for solid hydrogen storage materials completes the hydrogen replacement and preheats to 250°C using the heat transfer oil in the jacket. The valve between the isolation chamber and the feed inlet of the continuous reaction device used for solid hydrogen storage materials is opened, and the atmospheric pressure magnesium hydride powder silo discharges the powder through the isolation chamber into the continuous reaction device used for solid hydrogen storage materials.

[0100] The motor is started, driving the reducer and magnetic coupler, which in turn starts the screw conveyor unit. As the stirring shaft moves, the spiral blades push the material, conveying it to the reactor outlet. Magnesium powder reacts at 340℃, 0.3MPa, and 20rpm. The stirring shaft speed is controlled to ensure the spiral blades push the magnesium hydride powder horizontally from the inlet to the outlet of the reaction tube. During the reaction, the raw materials are repeatedly crushed and compressed by the two stirring shafts, achieving layer-by-layer separation and effective kneading. The heat generated during the reaction is promptly removed by a heat exchanger.

[0101] During pyrolysis, magnesium hydride powder is discharged from the silo by gravity into the reaction unit under constant pressure. The external heat transfer oil system then provides heat to the continuous reaction unit used for solid-state hydrogen storage materials. Magnesium hydride has a low thermal conductivity, a high length-to-diameter ratio in the reaction tubes, a large specific surface area, and high thermal efficiency, facilitating heat transfer from the external heat transfer oil into the reaction unit. Furthermore, the spiral blades inside the reaction unit continuously agitate the reaction, transferring heat from the heat transfer oil on the reaction tube walls through the magnesium hydride powder, resulting in a more uniform temperature field throughout the reaction unit. The discharge rate can be controlled by adjusting the stirring speed of the reaction unit according to the reaction state.

[0102] When the hydrogen demand is low, one reactor can be started. When the hydrogen demand is high, multiple reactors can be connected in parallel, and the stroke rate of each reactor can be increased. As the screw propels the material, the hydrogen release reaction and unloading are completed simultaneously, achieving continuous unloading after hydrogen release.

[0103] Example 2: Preparation of magnesium hydride

[0104] This embodiment discloses a continuous reaction system applied to solid hydrogen storage materials, the structure of which is as follows: Figure 3 As shown, the system includes a raw material silo 101, an isolation silo 102, an aeration tank 103, a first gas recovery tank 104, a buffer tank 105, a heat transfer oil furnace 106, a continuous reaction device 107 for solid hydrogen storage materials, a second gas recovery tank 108, a cooling tank 109, and a collection tank 110. The raw material silo 101, isolation silo 102, buffer tank 105, continuous reaction device 107 for solid hydrogen storage materials, cooling tank 109, and collection tank 110 are connected sequentially. The inlet and outlet of the heat transfer oil 106 are respectively connected to the outlet and inlet of the jacket 6 of the continuous reaction device 107 for solid hydrogen storage materials. The collection tank 110 is also connected to the second gas recovery tank 108.

[0105] In this embodiment, there are two isolation chambers 102 connected in parallel. The inlet and outlet of each isolation chamber 102 are respectively connected to the raw material chamber 101 and the continuous reaction device 107 used for solid hydrogen storage materials. The isolation chamber is used to regulate the pressure of the raw material. A heating device is also installed in each isolation chamber 102 for heating the raw material. Each isolation chamber 102 is individually connected to a gas filling tank 103 and a first gas recovery tank 104 for pressure replenishment or replacement.

[0106] The continuous reaction device for solid hydrogen storage materials includes two reactors connected in series, which are the same as those in Example 1. The difference is that the drive unit includes a motor 1, a reducer 2, and a mechanical seal. The motor is connected to the stirring shaft via the reducer, and the mechanical seal seals the area between the reducer and the reaction tube. The stirring shaft 9 is a hollow shaft, with a heat exchange medium introduced into its inner cavity. Rotary joints 5 are connected to both ends of the hollow shaft; one end of each rotary joint 5 is connected to the hollow shaft, and the other end is connected to the heat exchange medium inlet pipeline. The spiral blades 8 are toothed, enabling the materials to be kneaded together.

[0107] like Figure 2As shown, two arc-shaped plates 7 are provided on the inner bottom of the reaction tube 14, which cooperate with two stirring shafts (first stirring shaft 15 and second stirring shaft 18). The cross-section of the two arc-shaped plates 7 along the radial direction of the reaction tube is W-shaped, and the two arc-shaped plates 7 maintain a certain gap with the helical blades on the two stirring shafts. To solve the problem that setting up two shafts in the reaction tube would cause the vertical space of the reactor to be greater than the horizontal space, this invention sets arc-shaped plates at the bottom of the reaction tube to reduce the bottom space and prevent the bottom material from settling and forming a dead zone. The chamber between the arc-shaped plates and the inner wall of the reaction tube is connected to the cold hydrogen inlet 17, which is set on the end cap of the reaction tube for introducing cold hydrogen. The arc-shaped plates are provided with nanopores, which can allow hydrogen to enter and exit freely while ensuring that solid raw materials do not leak to the bottom of the two arc-shaped plates. The nanopores are made by laser drilling.

[0108] In addition to introducing hydrogen through gas inlet 12, the cold hydrogen introduced at the bottom of the reaction tube not only has the effect of purging and loosening the material on the reactor wall, but also allows the cold hydrogen to pass through the material layer from bottom to top to enhance the heat transfer reaction.

[0109] The reaction tube of the first-stage reactor is fixed above the reaction tube of the second-stage reactor. The solids conveying port of the first-stage reactor is connected to the feed port of the second-stage reactor. The second-stage reactor is equipped with support legs to jointly support both reactors. The spiral blades of the second-stage reactor push the material in the opposite direction, effectively conveying the material from the first-stage reactor to the feed port of the second-stage reactor. Sufficient installation distance is maintained between the first-stage and second-stage reactors. Each reactor has an independent heating jacket structure to meet the temperature requirements of each reactor at different reaction stages.

[0110] A pulverizing device, specifically a high-speed shear head, is installed in the pipeline between the two reactors. Material from the solid feed inlet of the first-stage reactor is crushed by a high-speed shear or a crushing valve before being discharged into the second-stage reactor. The high-speed shearing process refines the falling magnesium powder, reducing particle size and accelerating the hydrogen storage rate, thus increasing the hydrogen storage density.

[0111] To better monitor the loading and unloading between the two-stage reactors, a level gauge is installed in the pipeline between the first-stage and second-stage reactors, below the high-speed shear line. When the detected material level in the pipeline is higher than the set value, it is determined whether the stirring shafts of the first-stage and second-stage reactors are rotating. If stirring is still ongoing, it is preliminarily determined that the spiral stirring speed of the second-stage reactor is low, and the stirring shaft speed of the second-stage reactor needs to be increased to accelerate the discharge and prevent material accumulation from affecting the entire reaction unit. If it is determined that the stirring shaft of the second-stage reactor is not rotating, the first-stage reactor is immediately shut down to prevent the second-stage reactor from becoming stuck due to material accumulation within the entire second-stage reaction tube.

[0112] The continuous reaction device for solid hydrogen storage materials also includes a control unit, which is communicatively connected to a temperature sensor, a pressure sensor, a motor, a flow meter, a flow valve, and a level gauge.

[0113] Applying this embodiment to the continuous reaction system for solid hydrogen storage materials for the preparation of magnesium hydride includes the following steps:

[0114] The method for preparing magnesium hydride using the above reaction system is as follows: A raw material silo 101 (atmospheric pressure magnesium powder silo) is connected to two isolation silos 102. Under a nitrogen protective atmosphere, after air replacement is completed in both isolation silos 102, the ball valve between the atmospheric pressure magnesium powder silo and the isolation silos 102 is opened for material transfer. When one isolation silo 102 is full, the ball valve between the two silos is closed, and the hydrogen inlet valve of the isolation silo 102 is opened. Hydrogen is introduced into the isolation silo 102 through the gas filling tank 103 until the pressure is 0.5 MPa higher than the operating pressure of the reaction device, then the hydrogen valve is closed. The other isolation silo 102 undergoes the same operation. The ball valve between one of the isolation silos 102 and the buffer tank 105 is opened, and the magnesium powder from the isolation silo is filled into the buffer tank 105. The pressure in the buffer tank is slightly higher than that in the reactor by 0.2 MPa. The magnesium powder is continuously supplied to the continuous reaction device for solid hydrogen storage materials by gravity and pressure difference from the buffer tank 105. In the continuous reaction device for solid hydrogen storage materials, the material undergoes a continuous hydrogen storage reaction under certain temperature and pressure. After the reaction is completed, the material enters the cooling tank 109 through the outlet of the reaction device. When a certain cooling temperature is reached, the magnesium powder can be sealed into the collection tank 110.

[0115] In the preparation of magnesium-based solid hydrogen storage materials, before releasing magnesium powder from the atmospheric pressure magnesium powder silo to the isolation chamber, the inert protective gas inside the isolation chamber is vacuum-evacuated and discharged. After discharge, hydrogen gas is introduced into the isolation chamber at a pressure higher than that inside the reaction device. The continuous reaction device for solid hydrogen storage materials completes the hydrogen replacement and preheats the powder to 150°C using heat transfer oil in the jacket. Initially, the heat transfer oil temperature is controlled to allow a core-shell-like structure to form on the surface of the magnesium powder, preventing caking and ensuring subsequent hydrogen storage. The raw material inlet valve between the isolation chamber and the continuous reaction device for solid hydrogen storage materials is opened, and the magnesium powder is fed into the continuous reaction device for solid hydrogen storage materials under the combined action of gravity and pressure difference. After the reaction, the material is cooled, collected, and stored.

[0116] When a continuous reaction device for solid-state hydrogen storage materials includes a single reactor, the temperature range is controlled between 240 and 420°C depending on the reaction stage. When the continuous reaction device includes multiple reactors connected in series, the temperature of each reactor can be individually controlled according to the preheating and enhanced reaction sections. The first-stage reactor can use a jacketed heating medium to preheat the reaction tubes, with the preheating temperature controlled between 200 and 220°C. After reaching the preheating temperature, the material enters the second-stage reactor through the outlet of the first-stage reactor. The material in the second-stage reactor, having been preheated by the first-stage reactor, has reached the reaction temperature. During the hydrogen storage reaction, the reaction continuously releases heat. The external jacket of the second-stage reactor can use a heat exchange medium to effectively remove heat, controlling the temperature of the enhanced reaction section between 300 and 420°C.

[0117] Each reactor can be configured with different helical blade pitches and stirring speeds depending on the reaction section and temperature. This dual independent setting of temperature and stirring allows for better adaptation to reaction requirements and achieves optimal hydrogen storage performance.

[0118] Specifically, the reaction process within the continuous reaction device applied to solid-state hydrogen storage materials is as follows: The motor is started, driving the reducer and magnetic coupler, which in turn activates the screw conveyor unit. As the stirring shaft moves, the spiral blades push the material, conveying it spirally to the reactor outlet. While the magnesium powder moves spirally with the spiral blades, hydrogen gas is introduced into the reaction gas inlet of the reaction tube. Simultaneously, the nanopores on the bottom arc plate 7 of the reaction tube continuously deliver cold hydrogen into the reaction tube. The horizontal reaction tube has a small diameter, resulting in low hydrogen resistance. The packing material in the reaction tube is controllable, and sufficient gas phase space is reserved to facilitate hydrogen flow within the tube. The magnesium powder reacts at a temperature of 300℃, a pressure of 3.0 MPa, and a stirring speed of 20 rpm. The stirring shaft speed is controlled within the reactor, causing the spiral blades to push the magnesium powder horizontally from the reaction tube inlet to the reaction tube outlet. During the reaction, the raw materials are repeatedly crushed and compressed by the two stirring shafts, achieving layer-by-layer peeling and effective kneading. The heat generated during the reaction is promptly removed by the heat exchange device. The discharge pipe of the first-stage reactor connects to the inlet of the second-stage reactor. Before the material flows through the discharge pipe, the high-speed shear head or crushing valve of the discharge pipe is activated to shear and crush the flowing material before it falls into the inlet of the second-stage reactor. The second-stage reactor reverses the material flow, and the magnesium powder is pulverized within the reaction tube, accelerating the hydrogen storage rate and increasing the hydrogen storage density. The heat transfer oil temperature of the second-stage reactor is set to 300℃ to complete hydrogenation under high temperature and high pressure. As the screw propels the material, the hydrogen storage reaction and unloading are completed simultaneously, thus realizing loading and unloading and continuous production.

[0119] Example 3: Hydrolysis of magnesium hydride

[0120] The continuous reaction system for solid hydrogen storage materials applied in this embodiment is basically the same as that in Embodiment 2. The difference is that the reaction tube is placed at a 20-degree angle to the horizontal direction, that is, the feed end of the reaction tube is higher than the discharge end, so as to ensure that the material is completely discharged under the action of stirring and gravity.

[0121] During the hydrolysis of magnesium-based solid hydrogen storage materials, the reaction apparatus first completes hydrogen replacement. The raw material inlet valves of the magnesium powder isolation chamber 102 and the continuous reaction apparatus 107 (used for solid hydrogen storage materials) are then opened. The raw material chamber 101 (also called the atmospheric pressure magnesium hydride powder chamber) releases the powder through the magnesium powder isolation chamber 102 into the continuous reaction apparatus 107. Water is then introduced into the reactor, and the magnesium hydride hydrolyzes to produce hydrogen gas, releasing a large amount of heat energy. The magnesium hydride hydrolysis reaction conditions are 30 degrees Celsius, 20 rpm, and 1.0 MPa.

[0122] In addition, the stirring shaft 9 is a hollow shaft, with heat exchange medium introduced into its inner cavity. Rotary joints 5 are connected to both ends of the hollow shaft. One end of each rotary joint connects to the hollow shaft, and the other end connects to the heat exchange medium inlet pipeline. The rotary joint 5 is a continuous type, with one end connected to the hollow shaft first, then to the reducer output end, and the other end connected to the heat exchange medium outlet pipeline. When the hydrolysis reaction releases a large amount of heat, one pipeline of the heat transfer oil system is used to connect to one end of the rotary joint. After the reaction starts, both pipelines of the heat transfer oil system are cooled, the outer jacket of the reaction tube is cooled, and the heat transfer oil in the hollow shaft of the stirring shaft cools, achieving simultaneous internal and external cooling of the reaction tube. Temperature detection of the inner wall of the reaction tube ensures that the hydrolysis reaction remains at the optimal reaction temperature. The magnesium hydroxide produced by the reaction moves with the material driven by the screw, and the hydrogen release reaction and unloading are completed simultaneously, thus realizing loading and unloading and continuous production.

[0123] Example 4: Hydrothermal Coupling of Magnesium-Based Solid Hydrogen Storage Materials

[0124] The continuous reaction apparatus for solid hydrogen storage materials disclosed in Examples 1 and 2 is also suitable for coupled hydrolysis and pyrolysis reactions. The magnesium-based solid hydrogen storage material reacts with water, releasing a large amount of heat, which can be used to pyrolyze magnesium hydride to produce hydrogen. A motor is connected to a reducer, which is a two-end type. One end is connected to a rotary joint, and the other end is connected to a coupling. The coupling connects to the reactor stirring shaft, which is a hollow shaft with a layer of stainless steel wire mesh inside. Magnesium hydride fills the hollow shaft. The fixed-end hollow shaft is fixed by bearings, and a bearing cap is led out and connected to a cooling water outlet pipeline. The rotary joint at the reducer end is connected to a cooling water inlet pipeline. A control valve is installed on the cooling water inlet pipeline to strictly control the amount of water entering the hollow shaft. The reaction process and heat supply are controlled by controlling the water flow. Multiple temperature measuring points are set inside the reaction tube to monitor the temperature in real time. When the temperature exceeds the pyrolysis temperature, the cooling of the external jacket heat transfer oil and the cooling water inside the hollow shaft are increased to strictly control the hydrolysis temperature.

[0125] Example 5: Coupling of calcium-based thermal storage materials

[0126] The continuous reaction apparatus for solid-state hydrogen storage materials disclosed in Examples 1 and 2 is also applicable to calcium-based coupling. The magnesium hydride hydrogen storage process within the reaction apparatus is exothermic, and the heat of reaction should be promptly removed from the container to prevent magnesium hydride caking due to high temperatures. Heat exchange is achieved using heat transfer oil within the reaction apparatus jacket; this heat is a high-grade heat source and easily collected. The heat transfer oil outlet is connected to a calcium-based material heat storage device. Calcium carbonate or calcium hydroxide absorbs heat during the calcination and decomposition process and stores it as chemical energy. During the magnesium hydride hydrogen release process, the reaction product calcium oxide releases heat through carbonation or hydration reactions. Repeating this reaction multiple times achieves heat storage and heat release cycling during the magnesium hydride hydrogen storage and release process.

[0127] In Examples 2 and 3, the hollow shaft serves only as a channel for heating or heat extraction media. In Examples 4 and 5, the hollow shaft functions as a small reaction chamber, providing heat for the hydrolysis reaction and calcium-based coupled heat storage and release.

[0128] 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 them; although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present invention.

Claims

1. A continuous reaction device for solid hydrogen storage materials, characterized in that, The device includes one or more reactors, which are connected in parallel and / or in series when there are multiple reactors. Each reactor includes a drive unit, a screw conveyor unit, and a reaction tube. The screw conveyor unit includes multiple parallel stirring shafts with helical blades. The multiple stirring shafts pass through the reaction tube. There are multiple drive units, each connected to a stirring shaft, which drive the stirring shafts to rotate. The reaction tube is fitted with a jacket.

2. The continuous reaction apparatus for solid hydrogen storage materials according to claim 1, characterized in that, The drive unit includes a motor, a reducer, and a sealing structure. The motor is connected to the stirring shaft through the reducer and drives the stirring shaft to rotate. The sealing structure is used to seal between the reducer and the reaction tube.

3. The continuous reaction apparatus for solid hydrogen storage materials according to claim 1 or 2, characterized in that, The reaction tube is a horizontal high-temperature and pressure-resistant reaction vessel; And / or, the reaction tube is provided with a safety valve port; And / or, the reaction tube is provided with an inlet and an outlet, the inlet including one or more of a gas inlet, a liquid inlet and a solid inlet, and the outlet including one or more of a gas outlet, a liquid outlet and a solid outlet; And / or, a temperature sensor and a pressure sensor are provided inside the reaction tube; And / or, the jacket is provided with a heat exchange medium, preferably heat transfer oil; And / or, there are multiple jackets, and the multiple jackets are arranged sequentially along the axial direction of the reaction tube; And / or, an insulation layer is provided on the outside of the jacket; And / or, the jacket is provided with fins; And / or, a sphere is provided inside the reaction tube; And / or, a gas distributor is laid along the axial direction at the bottom of the inner side of the reaction tube. Preferably, the gas distributor is a plurality of arc plates arranged at the bottom of the inner side of the reaction tube and cooperating with a plurality of stirring shafts. The plurality of arc plates maintain a certain gap with the spiral blades on the plurality of stirring shafts. The chamber between the lower part of the arc plate and the inner wall of the reaction tube is connected to the cold hydrogen inlet. The arc plate is provided with nanopores. And / or, the helical blades on the multiple stirring shafts are arranged in an alternating pattern; And / or, the end of the stirring shaft closest to the direction of material movement is connected to a thrust bearing; And / or, the stirring shaft is a hollow shaft, with a rotary joint connecting the input start end and the output end of the hollow shaft; And / or, the spiral blade is a blade that can propel the material forward and / or knead the material. Preferably, the spiral blade is a continuous spiral blade, a single diamond-shaped blade, or a toothed blade.

4. The continuous reaction apparatus for solid hydrogen storage materials according to any one of claims 1 to 3, characterized in that, When multiple reactors are connected in series, a crushing device is installed in the pipeline between adjacent reactors. Preferably, the crushing device is a high-speed shear head or a crushing valve. And / or, when multiple reactors are connected in series, level gauges are installed in the pipelines between adjacent reactors.

5. A continuous reaction method for solid hydrogen storage materials, characterized in that, Includes the following steps: The drive unit drives multiple stirring shafts with spiral blades to rotate, pushing the raw materials from the reactor inlet to the reactor outlet. During the reaction, the raw materials are continuously cut and kneaded, and the heat generated during the reaction is removed in time by the heat exchange device.

6. The continuous reaction method for solid hydrogen storage materials according to claim 5, characterized in that, The continuous pyrolysis hydrogen production reaction conditions for magnesium-based hydrogen storage materials include: temperature of 150-400℃, pressure of 0.01-1.5MPa, and stirring shaft speed of 20-40rpm. And / or, the reaction conditions for continuous magnesium-based hydrogen storage material to absorb hydrogen include: temperature of 25-420℃, pressure of 0.2-10MPa, and stirring shaft speed of 5-100rpm; And / or, the continuous magnesium-based hydrogen storage material hydrolysis hydrogen production reaction conditions include: temperature of 30-300℃, pressure of 0.1-2.0Mpa, and stirring shaft speed of 5-100rpm.

7. A continuous reaction system for solid hydrogen storage materials, characterized in that, It includes a raw material silo, an isolation silo, a continuous reaction apparatus for solid hydrogen storage materials as described in any one of claims 1-4, and a collection tank, which are connected in sequence.

8. The continuous reaction system for solid hydrogen storage materials according to claim 7, characterized in that, The isolation chambers are multiple, and the multiple isolation chambers are connected in parallel; And / or, a heating device is provided inside the isolation chamber; And / or, the isolation chamber is respectively connected to an inflation tank and a first gas recovery tank; And / or, the continuous reaction device applied to solid hydrogen storage materials is placed at an angle of 0 to 20 degrees in the horizontal direction, so that the outlet is lower than the inlet; And / or, the collection tank is connected to a second gas recovery tank; And / or, a buffer tank is provided between the isolation chamber and the continuous reaction device applied to solid hydrogen storage materials; And / or, a cooling tank is provided between the continuous reaction device for solid hydrogen storage materials and the collection tank; And / or, the continuous reaction system applied to solid hydrogen storage materials further includes a heat transfer oil furnace, wherein the heat transfer oil inlet and outlet are respectively connected to the outlet and inlet of the jacket.

9. A continuous reaction method for solid hydrogen storage materials, characterized in that, Includes the following steps: The raw materials in the raw material silo are unloaded by gravity into the isolation silo. After being heated and / or pressurized in the isolation silo, the raw materials enter the continuous reaction device used for solid hydrogen storage materials. The reacted materials are collected and stored.

10. The use of the continuous reaction apparatus for solid hydrogen storage materials according to any one of claims 1-4 and the continuous reaction system for solid hydrogen storage materials according to claim 7 or 8 in the field of solid-solid reaction, liquid-solid reaction, gas-solid reaction, liquid-liquid reaction or gas-liquid reaction, especially in the field of magnesium-based hydrogen storage material reaction.

Citation Information

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