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CN119309130B - Hydrogen storage alloy reactor, methods for hydrogen storage and dehydrogenation - Google Patents

Hydrogen storage alloy reactor, methods for hydrogen storage and dehydrogenation

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Publication number
CN119309130B
CN119309130B CN202310855073.8A CN202310855073A CN119309130B CN 119309130 B CN119309130 B CN 119309130B CN 202310855073 A CN202310855073 A CN 202310855073A CN 119309130 B CN119309130 B CN 119309130B
Authority
CN
China
Prior art keywords
hydrogen
inner tank
hydrogen storage
tank
reactor according
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Active
Application number
CN202310855073.8A
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Chinese (zh)
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CN119309130A (en
Inventor
程涛
林伟
杨雪
王厚朋
龚雪卉
邹亢
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sinopec Petrochemical Research Institute Co ltd
China Petroleum and Chemical Corp
Original Assignee
Sinopec Petrochemical Research Institute Co ltd
China Petroleum and Chemical Corp
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Priority to CN202310855073.8A priority Critical patent/CN119309130B/en
Publication of CN119309130A publication Critical patent/CN119309130A/en
Application granted granted Critical
Publication of CN119309130B publication Critical patent/CN119309130B/en
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/0005—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes
    • C01B3/001—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes characterised by the uptaking media; Treatment thereof
    • C01B3/0078—Composite solid storage media, e.g. mixtures of polymers and metal hydrides, coated solid compounds or structurally heterogeneous solid compounds
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C3/00—Vessels not under pressure
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C6/00—Methods and apparatus for filling vessels not under pressure with liquefied or solidified gases
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C9/00—Methods or apparatus for discharging liquefied or solidified gases from vessels not under pressure
    • F17C9/02—Methods or apparatus for discharging liquefied or solidified gases from vessels not under pressure with change of state, e.g. vaporisation
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2201/00—Vessel construction, in particular geometry, arrangement or size
    • F17C2201/01—Shape
    • F17C2201/0104—Shape cylindrical
    • F17C2201/0119—Shape cylindrical with flat end-piece
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2201/00—Vessel construction, in particular geometry, arrangement or size
    • F17C2201/03—Orientation
    • F17C2201/032—Orientation with substantially vertical main axis
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2201/00—Vessel construction, in particular geometry, arrangement or size
    • F17C2201/05—Size
    • F17C2201/056—Small (<1 m3)
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0602—Wall structures; Special features thereof
    • F17C2203/0612—Wall structures
    • F17C2203/0626—Multiple walls
    • F17C2203/0629—Two walls
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0634—Materials for walls or layers thereof
    • F17C2203/0636—Metals
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0634—Materials for walls or layers thereof
    • F17C2203/0636—Metals
    • F17C2203/0639—Steels
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0634—Materials for walls or layers thereof
    • F17C2203/0636—Metals
    • F17C2203/0639—Steels
    • F17C2203/0643—Stainless steels
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0634—Materials for walls or layers thereof
    • F17C2203/0636—Metals
    • F17C2203/0646—Aluminium
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0634—Materials for walls or layers thereof
    • F17C2203/0636—Metals
    • F17C2203/0648—Alloys or compositions of metals
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2223/00—Handled fluid before transfer, i.e. state of fluid when stored in the vessel or before transfer from the vessel
    • F17C2223/01—Handled fluid before transfer, i.e. state of fluid when stored in the vessel or before transfer from the vessel characterised by the phase
    • F17C2223/0107—Single phase
    • F17C2223/0138—Single phase solid
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2223/00—Handled fluid before transfer, i.e. state of fluid when stored in the vessel or before transfer from the vessel
    • F17C2223/03—Handled fluid before transfer, i.e. state of fluid when stored in the vessel or before transfer from the vessel characterised by the pressure level
    • F17C2223/031—Not under pressure, i.e. containing liquids or solids only
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C2227/00—Transfer of fluids, i.e. method or means for transferring the fluid; Heat exchange with the fluid
    • F17C2227/03—Heat exchange with the fluid
    • F17C2227/0367—Localisation of heat exchange
    • F17C2227/0369—Localisation of heat exchange in or on a vessel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/32—Hydrogen storage

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Filling Or Discharging Of Gas Storage Vessels (AREA)

Abstract

本发明涉及储氢的技术领域，公开了一种储氢合金反应器、储氢和放氢的方法。一种储氢合金反应器，反应器包括竖直设置的内罐体以及套设在内罐体外部的外罐体；沿内罐体竖直方向，所述内罐体内部水平设置有多个内罐体隔板；沿外罐体竖直方向，所述外罐体内部水平设置有多个外罐体隔板；所述内罐体隔板上开设有开孔，所述开孔用于氢气的流通；所述外罐体隔板呈缺角圆环状，所述外罐体隔板用于导热流体的流通，所述导热流体通过缺角圆环的缺角流通。该储氢合金反应器能够提高传热效率，并且能够更好的控制吸放氢速率。

This invention relates to the technical field of hydrogen storage, and discloses a hydrogen storage alloy reactor, a method for storing and releasing hydrogen. The hydrogen storage alloy reactor includes a vertically arranged inner tank and an outer tank fitted over the inner tank. Along the vertical direction of the inner tank, multiple inner tank baffles are horizontally arranged inside the inner tank. Along the vertical direction of the outer tank, multiple outer tank baffles are horizontally arranged inside the outer tank. The inner tank baffles have openings for hydrogen gas flow. The outer tank baffles are in the shape of a notched annular ring, and are used for the flow of a heat-conducting fluid, which flows through the notched corner of the annular ring. This hydrogen storage alloy reactor can improve heat transfer efficiency and better control the hydrogen absorption and release rates.

Description

Hydrogen storage alloy reactor, hydrogen storage method and hydrogen discharge method
Technical Field
The invention relates to the technical field of hydrogen storage, in particular to a hydrogen storage alloy reactor and a hydrogen storage and release method.
Background
With the increasing global energy demand and serious CO 2 emissions and worsening environmental pollution, people pay more and more attention to developing clean and renewable energy sources. The hydrogen energy is used as secondary energy, has the characteristics of wide sources, cleanness, no carbon, flexibility, high efficiency, wide application scene and the like, can be widely applied to the fields of energy, transportation, industry, building and the like, is an ideal interconnection medium for promoting the clean and high-efficiency utilization of traditional fossil energy and supporting the large-scale development of renewable energy, and gradually becomes an important direction of the global energy technology development.
The hydrogen energy can be stored and transported, the hydrogen storage and transportation efficiency is improved, the hydrogen storage and transportation cost is reduced, and the hydrogen storage and transportation technology is a development key point. Currently, hydrogen storage mainly comprises three modes of gaseous hydrogen storage, liquid hydrogen storage and solid hydrogen storage. The high-pressure gaseous hydrogen storage is a main mode of hydrogen storage at the present stage, and has the advantages of high hydrogen charging and discharging speed and simple container structure. However, the high-pressure gas hydrogen storage has the defects of low volume density, low safety and the like, and meanwhile, the existing high-pressure equipment and high-pressure storage tank technology depend on import. The liquid hydrogen storage means that the hydrogen is liquefied at low temperature and stored in a low-temperature heat-insulating liquid storage tank, and has the advantage of high hydrogen storage density. However, the liquid hydrogen device has high cost, high energy consumption in the liquefaction process and evaporation loss in the use process, and is a problem to be solved urgently at present. Solid hydrogen storage refers to the storage of hydrogen by chemisorption or physical adsorption using metal hydrides, nanomaterials, etc. as carriers. The solid hydrogen storage has the advantages of high hydrogen storage density, low hydrogen storage pressure, high purity of discharged hydrogen, good safety and the like, and is an important direction for the future hydrogen storage development.
Hydrogen storage alloy materials refer to a class of materials that store hydrogen gas in the form of metal hydrides. The hydrogen storage alloy has the advantages of good reversibility of hydrogen absorption and desorption, high density of hydrogen storage per unit volume, high purity of hydrogen desorption and high safety. Metal hydrides are formed from metal alloys and hydrogen that react reversibly at specific temperatures and pressures. The absorption of hydrogen is an exothermic reaction, while the desorption is an endothermic process. The former only occurs when the supply pressure is greater than the equilibrium pressure, and the latter only occurs when the pressure is below the equilibrium pressure. During the hydrogen absorption process, the released heat needs to be removed from the reaction system in time, so that the temperature is kept at a favorable position. This helps to increase the hydrogen absorption rate while increasing the hydrogen storage capacity. When hydrogen release is desired, the endothermic reaction of the desorption process means that external heat is required to maintain a suitable hydrogen release rate. However, the existing hydrogen storage alloy reactor has poor heat transfer performance, which results in poor control of the hydrogen absorption and desorption rate of the hydrogen storage system and low reversible hydrogen storage density. Therefore, improving the heat transfer efficiency of the system is critical to improving the performance of the metal hydride hydrogen storage system.
Disclosure of Invention
The invention aims to solve the problems of poor heat transfer performance and poor hydrogen absorption and desorption rate control of a hydrogen storage reactor in the prior art, and provides a hydrogen storage alloy reactor, a hydrogen storage method and a hydrogen desorption method.
In order to achieve the above object, according to a first aspect of the present invention, there is provided a hydrogen storage alloy reactor, wherein the reactor comprises an inner tank body vertically arranged and an outer tank body sleeved outside the inner tank body, a plurality of inner tank body separators are horizontally arranged inside the inner tank body along the vertical direction of the inner tank body, a plurality of outer tank body separators are horizontally arranged inside the outer tank body along the vertical direction of the outer tank body, openings are formed in the inner tank body separators, the openings are used for hydrogen circulation, the outer tank body separators are in a shape of a broken corner ring, the outer tank body separators are used for circulation of heat conduction fluid, and the heat conduction fluid circulates through the broken corner of the broken corner ring.
In a second aspect, the present invention provides a method for storing and releasing hydrogen, wherein the hydrogen storing process and the hydrogen releasing process are performed in the hydrogen storing alloy reactor according to the first aspect, the method comprising:
the hydrogen storage process comprises the steps of introducing hydrogen into an inner tank body, carrying out hydrogen absorption reaction on a solid hydrogen storage composite material between the hydrogen and a partition board of the inner tank body, and introducing heat conduction fluid into an outer tank body to absorb heat generated by the hydrogen absorption reaction;
And in the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction, and then the heat conduction fluid is introduced into the outer tank body so as to provide heat required by the desorption reaction of the hydrogen.
In the prior art, a hydrogen storage alloy reactor with no gas flow channel and no liquid flow channel exists at the same time is low in hydrogen absorption efficiency and heat exchange efficiency. According to the hydrogen storage alloy reactor provided by the invention, the opening is formed in the partition plate of the inner tank body to form the gas flow passage, so that the hydrogen is ensured to be fully contacted with the solid hydrogen storage composite material in the hydrogen storage process, and each part of the solid hydrogen storage material can absorb the hydrogen, so that the hydrogen absorption efficiency is improved. Simultaneously, be provided with a plurality of outer jar body baffles in the outer jar body, outer jar body baffle makes the internal liquid runner that forms of outer jar, increases heat transfer area, and then improves heat exchange efficiency.
Drawings
FIG. 1 is a schematic structural view of a hydrogen occluding alloy reactor according to the present invention;
FIG. 2 is a schematic cross-sectional view of the inner tank bulkhead of the invention;
FIG. 3 is a schematic illustration of the inner tank bulkhead arrangement of the present invention;
FIG. 4 is a schematic cross-sectional view of an outer can baffle of the present invention;
FIG. 5 is a graph showing the time-dependent change in the hydrogen absorption amount during hydrogen storage according to example 1 of the present invention;
FIG. 6 is a graph showing the temperature of the inner tank over time during hydrogen storage according to example 1 of the present invention;
FIG. 7 is a graph showing the change of the hydrogen discharge ratio with time during the hydrogen discharge in example 1 of the present invention;
FIG. 8 is a graph showing the time-dependent change in the hydrogen absorption amount during hydrogen storage according to example 2 of the present invention;
FIG. 9 is a graph showing the temperature of the inner tank over time during hydrogen storage according to example 2 of the present invention;
FIG. 10 is a graph showing the change of the hydrogen discharge ratio with time during the hydrogen discharge in example 2 of the present invention;
FIG. 11 is a graph showing the time-dependent change in the hydrogen absorption amount during hydrogen storage according to example 3 of the present invention;
FIG. 12 is a graph showing the temperature of the inner tank over time during hydrogen storage according to example 3 of the present invention;
FIG. 13 is a graph showing the change of the hydrogen discharge ratio with time during the hydrogen discharge in example 3 of the present invention;
FIG. 14 is a graph showing the time-dependent change in the hydrogen absorption amount during hydrogen storage according to example 4 of the present invention;
FIG. 15 is a graph showing the temperature of the inner tank over time during hydrogen storage in example 4 of the present invention;
FIG. 16 is a graph showing the change of the hydrogen discharge ratio with time in the hydrogen discharge process of example 4 of the present invention;
FIG. 17 is a schematic structural view of a hydrogen occluding alloy reactor according to comparative example 1 of the present invention;
FIG. 18 is a graph showing the change with time of the hydrogen absorption amount during hydrogen storage in comparative example 1 of the present invention;
FIG. 19 is a graph showing the change of the inner tank temperature with time during hydrogen storage according to comparative example 1 of the present invention;
FIG. 20 is a graph showing the change of the hydrogen discharge ratio with time during the hydrogen discharge of comparative example 1 of the present invention.
Description of the reference numerals
1-Inner tank 2-outer tank
3-Inner tank partition 4-outer tank partition
5-Open pore 6-unfilled corner ring
7-Trachea 8-filter
Detailed Description
The endpoints and any values of the ranges disclosed herein are not limited to the precise range or value, and are understood to encompass values approaching those ranges or values. For numerical ranges, one or more new numerical ranges may be found between the endpoints of each range, between the endpoint of each range and the individual point value, and between the individual point value, in combination with each other, and are to be considered as specifically disclosed herein.
In the description of the present invention, directions or positional relationships such as terms of "vertical", "horizontal", "top", "bottom", etc., are based on the orientations or positional relationships shown in the drawings, are merely for convenience of description of the present invention and are not required to necessarily construct and operate in a specific orientation, and thus should not be construed as limiting the present invention. The terms "coupled," "connected," and "connected" as used herein are to be construed broadly, and may be, for example, fixedly coupled or detachably coupled, and may be directly coupled or indirectly coupled through intermediate members, as will be apparent to those of ordinary skill in the art, in view of the detailed description of the terms.
The first aspect of the present invention provides a hydrogen storage alloy reactor, as shown in fig. 1 to 4, wherein the reactor comprises an inner tank 1 vertically arranged and an outer tank 2 sleeved outside the inner tank 1;
a plurality of inner tank partition boards 3 are horizontally arranged in the inner tank 1 along the vertical direction of the inner tank 1;
A plurality of outer tank partition boards 4 are horizontally arranged in the outer tank 2 along the vertical direction of the outer tank 2;
An opening 5 is formed in the inner tank body partition plate 3, and the opening 5 is used for hydrogen circulation;
the outer tank body partition board 4 is in a shape of a unfilled corner ring 6, the outer tank body partition board 4 is used for circulation of heat conduction fluid, and the heat conduction fluid circulates through the unfilled corner of the unfilled corner ring 6.
In the invention, two tanks are sleeved with each other to be used as a hydrogen storage alloy reactor, the inner tank is used for storing hydrogen and releasing hydrogen, and the outer tank is used for transferring heat, so that the safe transportation of hydrogen can be realized, the rapid heat transfer can be realized by means of the outer tank, and the heat transfer efficiency is improved; further, the hydrogen flows in the gas flow passage of the inner tank body, the flow direction of the hydrogen is regulated and controlled by adjusting the relative position of the holes on the baffle plates of the inner tank body, the heat conduction fluid flows through the unfilled corners of the baffle plates of the outer tank body, and the flow direction of the heat conduction fluid is adjusted by adjusting the relative position of the unfilled corners of the baffle plates of the outer tank body, so that the hydrogen storage efficiency and the heat diffusion efficiency are improved. By adopting the hydrogen storage alloy reactor provided by the invention, when the hydrogen absorption amount of the hydrogen storage alloy reactor reaches 90% of the maximum hydrogen absorption amount, the hydrogen absorption time can be reduced by 17-83% compared with the prior art, and when the hydrogen release amount of the hydrogen storage alloy reactor reaches 90% of the maximum hydrogen release amount, the hydrogen release time can be reduced by 32-90% compared with the prior art.
According to a preferred embodiment of the invention, the height of the inner tank 1 and the outer tank 2 is each independently 50-2000mm, preferably 150-800mm.
According to a preferred embodiment of the invention, the inner diameter of the inner tank 1 is 5-80mm, preferably 10-40mm.
According to a preferred embodiment of the invention, the inner diameter of the outer tank 2 is 15-160mm, preferably 30-90mm.
The advantage of using the preferred embodiment described above is that the heat transfer efficiency of the hydrogen storage material in the radial direction is improved.
According to a preferred embodiment of the present invention, the ratio of the difference in inner diameter of the outer tank 2 and the inner tank 1 to the inner diameter of the inner tank 1 is 0.2-3:1, and more preferably 0.35-2:1. The advantage of adopting this preferred embodiment is that the volume of the outer tank is reduced while meeting the heat transfer requirements during the hydrogen absorption and desorption process.
According to a preferred embodiment of the present invention, the number of the openings 5 is one, and the ratio of the opening area of the openings 5 to the area of the inner tank partition 3 is 0.01-0.2:1, preferably 0.04-0.1:1. The advantage of using this preferred embodiment is that the gas can flow along the openings of adjacent separators to create a flow direction while compromising gas transfer efficiency.
According to a preferred embodiment of the invention, the diameter of the opening 5 is 2-20mm, preferably 2-15mm. The advantage of using this preferred embodiment is that the gas can flow along the openings of adjacent separators to create a flow direction while compromising gas transfer efficiency.
According to a preferred embodiment of the present invention, the ratio of the distance between the center of the inner tank partition 3 and the center of the opening 5 to the inner diameter of the inner tank 1 is 0.15-0.45:1, and more preferably 0.2-0.35:1. The advantage of using this preferred embodiment is that the contact time of the gas with the hydrogen storage material is increased during the gas flow through the openings of the adjacent separator plates.
According to a preferred embodiment of the present invention, the plurality of inner can body partitions 3 are sequentially rotated in the same direction by 90-180 degrees, preferably 120-180 degrees, in the axial direction of the inner can body 1, based on the lowermost inner can body partition 3. The advantage of adopting this kind of preferred embodiment is that the gas flow channel structure that forms makes hydrogen and hydrogen storage material abundant contact, improves heat exchange efficiency.
In the invention, the schematic description indicates that the inner tank body partition plate at the bottommost layer is taken as the first inner tank body partition plate, the first inner tank body partition plate is kept static and is rotated anticlockwise by 90-180 degrees along the axial direction of the inner tank body, after the second inner tank body partition plate is rotated, the second inner tank body partition plate is kept static and is rotated anticlockwise by 90-180 degrees along the axial direction of the inner tank body, and the third inner tank body partition plate is rotated anticlockwise by analogy, so that the openings on the inner tank body partition plates form a gas flow channel structure, such as a snake-shaped flow channel. The foregoing is only schematically illustrated by counterclockwise rotation, and may be clockwise rotation, as long as the rotation directions of the plurality of inner tank separators are kept identical.
In the invention, a plurality of inner tank body partition boards are arranged in the inner tank body, and the full contact between hydrogen and hydrogen storage materials is realized by controlling the space between the inner tank body partition boards. Preferably, the ratio of the maximum distance between the adjacent inner tank partitions 3 to the height of the inner tank 1 is 0.05-0.5:1, and more preferably 0.05-0.35:1. The advantage of using this preferred embodiment is that the gas is deflected in the inner tank and is in sufficient contact with the hydrogen storage material.
According to a preferred embodiment of the invention, the angle of the unfilled ring 6 is 240-355 °, preferably 300-345 °. The advantage of using this preferred embodiment is that fluid flow is controlled by passing the fluid through the gap of the unfilled corner ring while simultaneously compromising fluid transfer flux.
In the invention, it can be understood that the radian of the unfilled corner ring refers to the degree of an included angle between two vertexes of the intrados of the unfilled corner ring and a connecting line of the circle centers, the calculation formula is 360 degrees/2 pi is l/r, wherein l is the length of the intrados of the unfilled corner ring 6, and r is the inner radius of the unfilled corner ring 6.
According to a preferred embodiment of the present invention, the plurality of outer can body partitions 4 are sequentially rotated in the same direction by 90-180 °, preferably 120-180 °, in the axial direction of the outer can body 2, based on the lowermost outer can body partition 4. The advantage of adopting this kind of preferred embodiment is that form the liquid runner structure in the outer jar body, can improve the heat transfer effect. It should be noted that, the "same direction rotation" is the same as the "same direction rotation" of the inner tank partition plate, and will not be described here again.
According to a preferred embodiment of the invention, the ratio of the maximum spacing between adjacent outer tank partitions 4 to the height of the outer tank 2 is 0.05-0.5:1, preferably 0.08-0.25:1. The advantage of adopting this kind of preferred embodiment is that make the liquid form the baffling in outer jar body, improve heat exchange efficiency.
The manner of setting the solid hydrogen storage composite material in the present invention is not particularly limited. Preferably, a solid hydrogen storage composite material is placed between the adjacent inner tank separators 3.
According to the present invention, preferably, the solid hydrogen storage composite comprises a hydrogen storage alloy and/or a thermally conductive material. The advantage of adopting this kind of preferred embodiment is that solid hydrogen storage combined material is formed by hydrogen storage alloy and heat conduction material mixing, can effectively improve the heat transfer coefficient of hydrogen storage material bed body, reduces simultaneously and absorbs the stress variation that hydrogen storage material expansion shrinkage arouses in the hydrogen release process.
In the present invention, the amount of each component material in the solid hydrogen storage composite is not particularly limited as long as the hydrogen storage requirement can be satisfied. Preferably, the mass ratio of the hydrogen storage alloy to the heat conducting material is 1:0.02-0.1.
In the present invention, the kind of the hydrogen absorbing alloy is not particularly limited, and the hydrogen absorbing alloy may be conventionally defined in the art. Preferably, the hydrogen storage alloy is at least one selected from the group consisting of titanium-based hydrogen storage alloy, zirconium-based hydrogen storage alloy, vanadium-based hydrogen storage alloy and rare earth-based hydrogen storage alloy, and more specifically, may be an LaNi 5 alloy, for example.
In the present invention, the kind of the heat conductive material is not particularly limited, and may be a heat conductive material conventionally defined in the art. Preferably, the heat conductive material is selected from at least one of expanded graphite, heat conductive fibers, graphite flakes, carbon nanotubes, aluminum powder, copper powder, titanium powder, aluminum foam, nickel foam, and copper foam.
In the present invention, the kind of the heat transfer fluid is not particularly limited, and may be a heat transfer fluid conventionally defined in the art. Preferably, the heat transfer fluid is selected from at least one of water, ethylene glycol, and heat transfer oil.
According to a preferred embodiment of the present invention, the materials of the inner tank 1, the outer tank 2, the inner tank separator 3 and the outer tank separator 4 are each independently selected from at least one of aluminum, aluminum alloy, copper alloy, carbon steel and stainless steel. The advantages of the adoption of the preferred embodiment are that parameters such as the weight, the cost, the heat conduction property and the like of the tank body can be adjusted according to the application scene.
According to a preferred embodiment of the present invention, an air pipe 7 is disposed at the top of the inner tank 1, and the air pipe 7 is used for introducing hydrogen into the inner tank 1 or releasing hydrogen in the inner tank 1.
According to a preferred embodiment of the invention, the inner diameter of the air tube is 3-10mm.
According to a preferred embodiment of the present invention, a filter 8 is disposed inside the air pipe 7, and the filter 8 is a copper-based and/or stainless steel-based porous sintered body, preferably a copper-based and/or stainless steel-based porous sintered body sintered by a powder metallurgy method.
According to a preferred embodiment of the invention, the accuracy of the filter 8 is 0.5-2 μm.
In a second aspect, the present invention provides a method for storing and releasing hydrogen, wherein the hydrogen storing process and the hydrogen releasing process are performed in the hydrogen storing alloy reactor according to the first aspect, the method comprising:
the hydrogen storage process comprises the steps of introducing hydrogen into an inner tank body 1, carrying out hydrogen absorption reaction on a solid hydrogen storage composite material between the hydrogen and an inner tank body partition board 3, and introducing a heat conducting fluid into an outer tank body 2 so as to absorb heat generated by the hydrogen absorption reaction;
And in the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction, and then the heat conduction fluid is introduced into the outer tank body 2 so as to provide heat required by the desorption reaction of the hydrogen.
In the present invention, the reaction conditions for the hydrogen absorption reaction and desorption reaction (hydrogen desorption reaction) are not particularly limited, and may be selected by those skilled in the art according to actual demands. Preferably, in the hydrogen storage process, the conditions of the hydrogen absorption reaction comprise a temperature of 10-50 ℃ and a pressure of 0.5-50MPa. Preferably, the temperature of the heat conducting fluid is 10-50 ℃ and the flow rate of the heat conducting fluid is 0.1-100L/min in the hydrogen storage process. In the hydrogen release process, the conditions of the desorption reaction comprise the temperature of 30-200 ℃ and the pressure of 0.1-50MPa. Preferably, during the hydrogen desorption, the temperature of the heat conducting fluid is 30-200 ℃, and the flow rate of the heat conducting fluid is 0.05-100L/min.
The present invention will be described in detail by examples.
Example 1
As shown in fig. 1, the hydrogen storage alloy reactor comprises an inner tank 1, an outer tank 2, an inner tank partition 3, an outer tank partition 4, an air pipe 7 and a filter 8, wherein the outer tank 2 is sleeved outside the inner tank 1, and the inner tank 1, the outer tank 2, the inner tank partition 3 and the outer tank partition 4 are all made of 304 stainless steel. The height of the inner tank body 1 is 150mm, the inner diameter is 30mm, the height of the outer tank body 2 is 150mm, the inner diameter is 60mm, the ratio of the inner diameter difference between the outer tank body 2 and the inner tank body 1 to the inner diameter of the inner tank body 1 is 1:1, the air pipe 7 is arranged at the top of the inner tank body 1 and communicated with the inner tank body 1, the diameter of the air pipe 7 is 3mm, the filter 8 is arranged in the air pipe 7, the filter 8 is made of sintered 316L stainless steel, the precision is 2 mu m, and hydrogen enters or exits the inner tank body 1 through the air pipe 7 after being filtered by the filter 8.
As shown in fig. 1-3, along the vertical direction of the inner tank 1, a plurality of inner tank separators 3 are horizontally arranged in the inner tank 1, the outer peripheral wall of each inner tank separator 3 is detachably connected with the inner peripheral wall of the inner tank 1, 1 opening 5 is formed in each inner tank separator 3, the diameter of each opening 5 is 8mm, the area ratio of the opening area of each opening 5 to the inner tank separator 3 is 0.07:1, the inner tank separators 3 sequentially rotate 180 degrees in the same direction along the axial direction of the inner tank 1 based on the adjacent lower inner tank separators 3, the ratio of the maximum distance between the adjacent inner tank separators 3 to the height of the inner tank 1 is 0.33:1, the plurality of inner tank separators 3 are arranged in parallel, the openings 5 on each inner tank separator form a gas flow channel, hydrogen flows in the gas flow channel, solid hydrogen storage composite materials are filled between the adjacent inner tank separators 3 in the inner tank 1, and each solid hydrogen storage composite material comprises a rare earth-based hydrogen storage alloy (composition is LaNi 5) and expanded graphite, wherein the mass ratio of rare earth-based hydrogen storage alloy to the expanded graphite is 0.03:1.
As shown in fig. 1 and 4, along the vertical direction of the outer tank 2, a plurality of outer tank separators 4 are horizontally arranged inside the outer tank 2, the outer tank separators 4 are in the shape of unfilled corner rings 6, the outer cambered surfaces of the unfilled corner rings 6 are detachably connected with the inner peripheral wall of the outer tank 2, the inner cambered surfaces of the unfilled corner rings 6 are detachably connected with the outer peripheral wall of the inner tank 1, the radian of the unfilled corner rings 6 is 300 degrees, and the ratio between the maximum distance between the adjacent outer tank separators 4 and the height of the outer tank 2 is 0.2:1. The outer tank body partition boards 4 are arranged in parallel, the outer tank body partition boards 4 of the adjacent lower layers are used as references, the outer tank body partition boards 4 sequentially rotate 180 degrees in the same direction along the axial direction of the outer tank body 2, a first diversion port (not shown in the figure) is arranged at the top of the outer tank body 2, a second diversion port (not shown in the figure) is arranged at the bottom of the outer tank body 2, heat conduction fluid enters the liquid flow channel of the outer tank body 2 through the first diversion port and is filled in the outer tank body 2, and the heat conduction fluid is deionized water.
In the hydrogen storage process, the pressure of a hydrogen inlet is maintained at 0.8MPa and is introduced into an inner tank body 1 to perform hydrogen absorption reaction with the solid hydrogen storage composite material in the inner tank body 1 under the pressure of the temperature of 293K at the initial temperature;
in the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction at an initial temperature of 343K and a constant outlet pressure of 0.1MPa, and deionized water of 343K is introduced into the outer tank body 2 at a flow rate of 0.2L/min to provide heat for the desorption reaction of hydrogen.
Numerical simulation calculations were performed on the reactor using comsol software. Mass, energy and momentum balance equations are constructed as follows:
mass conservation equation for hydrogen storage material:
mass conservation equation for gas:
Wherein m is a mass change value, epsilon is the porosity of the hydrogen storage material in the inner tank body 1, rho s is the density of the hydrogen storage material, t is the reaction time, u g is the velocity field of hydrogen, and rho g is the gas density.
The velocity field of hydrogen is calculated using darcy's law:
Where K is the permeability, mu g is the hydrogen viscosity coefficient, and P g is the hydrogen pressure.
For the hydrogen absorption reaction process, the reaction rate equation is as follows:
for the hydrogen evolution reaction process, the reaction rate equation is as follows:
Wherein, C a and C d are respectively the pre-finger factors of the hydrogen absorption reaction and the hydrogen release reaction, E a and E d are respectively the activation energy of the hydrogen absorption reaction and the hydrogen release reaction, R g is the gas constant, T is the reaction temperature, P eq is the chemical reaction equilibrium pressure, ρ ss is the density of the hydrogen storage material after the hydrogen absorption is complete, and ρ 0 is the initial density of the hydrogen storage material.
For the equilibrium pressure of the chemical reaction, given by Van't Hoff equation (Van't Hoff equation):
The energy balance equation of the hydrogen absorption and desorption reaction in the inner tank body 1 is as follows:
Wherein M g is the molar mass of hydrogen.
Wherein the effective heat capacity of the hydrogen storage bed body is (ρC) p)e＝ερgCp,g+(1-ε)ρsCp,s
The effective heat conductivity of the hydrogen storage bed body is lambda e＝ελg+(1-ε)λs
Wherein, C p,g and C p,s are the heat capacities of hydrogen and hydrogen storage materials, respectively, and λ g and λ s are the heat conductivities of hydrogen and hydrogen storage materials, respectively.
For a thermally conductive fluid, the mass balance equation is:
Where ρ f is the heat transfer fluid density and u f is the heat transfer fluid velocity field.
For a thermally conductive fluid, the momentum balance equation is as follows:
the heat transfer equation inside the heat transfer fluid is as follows:
wherein:
Where C p,f is the heat transfer fluid heat capacity, λ f is the thermal transfer fluid effective heat conductivity, and P f is the thermal transfer fluid pressure.
For the can wall and separator, the heat transfer equation is as follows:
Where (ρc) solid is the heat capacity of the solid (can wall or separator), and λ solid is the effective thermal conductivity of the solid (can wall or separator).
The heat transfer equation among the inner tank body, the outer tank body and the partition board is q=h (T 1-T2)
Where q is the heat flux, h is the heat transfer coefficient between the two, T 1 and T 2 refer to the respective temperatures of the adjacent two phases with different temperatures (e.g., T 1 and T 2 refer to the temperatures of the inner vessel and the separator, respectively, when calculating the heat transfer between the inner vessel and the separator).
And calculating the change value of each parameter in the reactor along with time by using the equation. As shown in fig. 5, the hydrogen absorption amount was changed with time, and after 334s from the start of the hydrogen absorption reaction, the hydrogen absorption amount in the hydrogen storage alloy reactor reached 90% of the maximum hydrogen absorption amount, and the hydrogen absorption time was reduced by 46% as compared with comparative example 1. As shown in FIG. 6, the total time for the increase of the inner tank temperature over 30K (323K) was 321s, which is a 49% decrease in the overtemperature time compared to comparative example 1.
As shown in FIG. 7, the hydrogen release rate was changed with time, and after 543s of the hydrogen release reaction, the hydrogen release amount of the hydrogen storage alloy reactor released 90% of hydrogen, and the hydrogen release time was reduced by 53% as compared with comparative example 1.
Example 2
The reactor of example 1 and the method of example 1 were employed, except that the height of the inner vessel 1 was 210mm, the inner diameter was 40mm, the height of the outer vessel 2 was 210mm, the inner diameter was 90mm, the ratio of the difference in the inner diameters of the outer vessel 2 and the inner vessel 1 to the inner diameter of the inner vessel 1 was 1.25:1, the gas pipe 7 was disposed at the top of the inner vessel 1 in communication with the inner vessel 1, the diameter of the gas pipe 7 was 10mm, a filter 8 was disposed inside the gas pipe 7, the filter 8 was made of sintered 316L stainless steel with an accuracy of 2. Mu.m, and hydrogen gas was introduced into or discharged from the inner vessel 1 through the gas pipe 7 after being filtered by the filter 8.
As shown in fig. 1-3, along the vertical direction of the inner tank 1, a plurality of inner tank separators 3 are horizontally arranged in the inner tank 1, the outer peripheral wall of each inner tank separator 3 is detachably connected with the inner peripheral wall of the inner tank 1, 1 opening 5 is formed in each inner tank separator 3, the diameter of each opening 5 is 12mm, the area ratio of the opening area of each opening 5 to the inner tank separator 3 is 0.09:1, the inner tank separators 3 sequentially rotate in the same direction by 150 degrees along the axial direction of the inner tank 1 based on the adjacent lower inner tank separators 3, the ratio of the maximum distance between the adjacent inner tank separators 3 to the inner tank height is 0.14:1, the plurality of inner tank separators 3 are arranged in parallel, the openings 5 on each inner tank separator 3 form a gas flow channel, hydrogen flows in the gas flow channel, solid hydrogen storage composite materials are filled between the adjacent inner tank separators 3 in the inner tank 1, and each solid hydrogen storage composite material comprises a rare earth-based hydrogen storage alloy (composition is LaNi 5) and expanded graphite, wherein the mass ratio of the rare earth-based hydrogen storage alloy to the graphite is 0.08:1.
As shown in fig. 1 and 4, along the vertical direction of the outer tank 2, a plurality of outer tank separators 4 are horizontally arranged inside the outer tank 2, the outer tank separators 4 are in the shape of unfilled corner rings 6, the outer cambered surfaces of the unfilled corner rings 6 are detachably connected with the inner peripheral wall of the outer tank 1, the inner cambered surfaces of the unfilled corner rings 6 are detachably connected with the outer peripheral wall of the inner tank 1, the radian of the unfilled corner rings 6 is 345 degrees, and the ratio between the maximum distance between the adjacent outer tank separators 4 and the height of the outer tank 1 is 0.2:1. The outer tank body partition boards 4 are arranged in parallel, the outer tank body partition boards 4 of the adjacent lower layers are used as references, the outer tank body partition boards 4 sequentially rotate in the same direction for 144 degrees along the axial direction of the outer tank body 2, a first diversion port (not shown in the figure) is arranged at the top of the outer tank body 2, a second diversion port (not shown in the figure) is arranged at the bottom of the outer tank body 2, heat conduction fluid enters the outer tank body flow channel through the first diversion port to be filled in the outer tank body 2, and the heat conduction fluid is deionized water.
In the hydrogen storage process, the pressure of a hydrogen inlet is maintained at 0.8MPa and is introduced into an inner tank body 1 to perform hydrogen absorption reaction with the solid hydrogen storage composite material in the inner tank body 1 under the pressure of the temperature of 293K at the initial temperature;
In the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction at the temperature of 343K and the pressure of 0.1MPa at the outlet pressure, and deionized water of 343K is introduced into the outer tank body 2 at the flow rate of 0.48L/min to provide heat for the desorption reaction of hydrogen.
The simulation calculation according to example 1 gave the values of the various parameters in the reactor over time. As shown in fig. 8, the hydrogen absorption amount was changed with time, and after 348s from the start of the hydrogen absorption reaction, the hydrogen absorption amount in the hydrogen storage alloy reactor reached 90% of the maximum hydrogen absorption amount, and the hydrogen absorption time was reduced by 44% as compared with comparative example 1. As shown in FIG. 9, the total time for the increase of the internal tank temperature over 30K (323K) was 363s, which is a 43% decrease in the overtemperature time compared to comparative example 1.
As shown in FIG. 10, the hydrogen release rate was changed with time, and after 483s from the start of the hydrogen release reaction, the hydrogen release amount of the hydrogen storage alloy reactor released 90% of hydrogen, which was 58% less than that of comparative example 1.
Example 3
The reactor of example 1 and the method of example 1 were employed, except that the height of the inner vessel 1 was 720mm, the inner diameter was 10mm, the height of the outer vessel 2 was 720mm, the inner diameter was 30mm, the ratio between the difference in the inner diameters of the outer vessel 2 and the inner vessel 1 and the inner diameter of the inner vessel was 2:1, an air pipe 7 was provided at the top of the inner vessel 1 in communication with the inner vessel 1, the diameter of the air pipe 7 was 4mm, a filter 8 was provided inside the air pipe 7, the filter 8 was made of sintered 316L stainless steel with an accuracy of 2. Mu.m, and hydrogen gas was introduced into or discharged from the inner vessel 1 through the air pipe 7 after being filtered by the filter 8.
As shown in fig. 1-3, along the vertical direction of the inner tank 1, a plurality of inner tank separators 3 are horizontally arranged in the inner tank 1, the outer peripheral wall of each inner tank separator 3 is detachably connected with the inner peripheral wall of the inner tank 1, 1 opening 5 is formed in each inner tank separator 3, the diameter of each opening 5 is 2.4mm, the area ratio of the opening area of each opening 5 to the inner tank separator 3 is 0.058:1, the inner tank separators 3 sequentially rotate in the same direction by 120 degrees along the axial direction of the inner tank 1 based on the adjacent lower inner tank separators 3, the ratio of the maximum distance between the adjacent inner tank separators 3 to the inner tank height is 0.09:1, the plurality of inner tank separators 3 are arranged in parallel, the openings 5 on each inner tank separator 3 form a gas flow channel, hydrogen flows in the gas flow channel, solid hydrogen storage composite materials are filled between the adjacent inner tank separators 3 in the inner tank 1, and each solid hydrogen storage composite material comprises a rare earth-based hydrogen storage alloy (LaNi 5) and expanded graphite, wherein the mass ratio of the rare earth-based hydrogen storage alloy to the expanded graphite is 0.08:1.
As shown in fig. 1 and 4, along the vertical direction of the outer tank 2, a plurality of outer tank separators 4 are horizontally arranged inside the outer tank 2, the outer tank separators 4 are in the shape of unfilled corner rings 6, the outer cambered surfaces of the unfilled corner rings 6 are detachably connected with the inner peripheral wall of the outer tank 1, the radian of the unfilled corner rings 6 is 330 degrees, and the ratio between the maximum distance between the adjacent outer tank separators 4 and the height of the outer tank is 0.09:1. The outer tank body partition boards 4 are arranged in parallel, the outer tank body partition boards 4 of the adjacent lower layers are used as references, the outer tank body partition boards 4 sequentially rotate in the same direction by 120 degrees along the axial direction of the outer tank body 2, a first diversion port (not shown in the figure) is arranged at the top of the outer tank body 2, a second diversion port (not shown in the figure) is arranged at the bottom of the outer tank body 2, heat conduction fluid enters the outer tank body flow channel through the first diversion port to be filled in the outer tank body 2, and the heat conduction fluid is deionized water.
In the hydrogen storage process, the pressure of a hydrogen inlet is maintained at 0.8MPa and is introduced into the inner tank body 1 to perform hydrogen absorption reaction with the solid hydrogen storage composite material in the inner tank body 1 under the pressure of the temperature of 293K at the initial temperature;
In the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction at 343K under the constant pressure of 0.1MPa at the outlet pressure, and the 343K deionized water is introduced into the outer tank body 2 at the flow of 0.05L/min to provide heat for the desorption reaction of the hydrogen.
The simulation calculation according to example 1 gave the values of the various parameters in the reactor over time. As shown in fig. 11, the hydrogen absorption amount was changed with time, and after 106s from the start of the hydrogen absorption reaction, the hydrogen absorption amount in the hydrogen storage alloy reactor reached 90% of the maximum hydrogen absorption amount, and the hydrogen absorption time was reduced by 83% as compared with comparative example 1. As shown in FIG. 12, the total time for the increase of the inner tank temperature over 30K (323K) was 108s, which is a 83% decrease in the overtemperature time compared to comparative example 1.
As shown in FIG. 13, the hydrogen release rate was changed with time, and after the start of the hydrogen release reaction for 117 seconds, the hydrogen release amount of the hydrogen storage alloy reactor released 90% of hydrogen, which was reduced by 90% as compared with comparative example 1.
Example 4
The reactor of example 1 and the method of example 1 were employed, except that the height of the inner vessel 1 was 100mm, the inner diameter was 60mm, the height of the outer vessel 2 was 100mm, the inner diameter was 80mm, the ratio of the difference between the inner diameters of the outer vessel 2 and the inner vessel 1 to the inner diameter of the inner vessel 1 was 0.33:1, the gas pipe 7 was disposed at the top of the inner vessel 1 in communication with the inner vessel 1, the diameter of the gas pipe 7 was 6mm, a filter 8 was disposed inside the gas pipe 7, the filter 8 was made of sintered 316L stainless steel with an accuracy of 2. Mu.m, and hydrogen gas was introduced into or discharged from the inner vessel 1 through the gas pipe 7 after being filtered by the filter 8.
As shown in fig. 1-3, along the vertical direction of the inner tank 1, a plurality of inner tank separators 3 are horizontally arranged in the inner tank 1, the outer peripheral wall of each inner tank separator 3 is detachably connected with the inner peripheral wall of the inner tank 1, 1 opening 5 is formed in each inner tank separator 3, the diameter of each opening 5 is 6mm, the area ratio of the opening area of each opening 5 to the inner tank separator 3 is 0.01:1, the inner tank separators 3 rotate in the same direction by 60 degrees in sequence along the axial direction of the inner tank 1 based on the adjacent lower inner tank separators 3, the ratio of the maximum distance between the adjacent inner tank separators 3 to the height of the inner tank 1 is 0.2:1, the plurality of inner tank separators 3 are arranged in parallel, the openings 5 on each inner tank separator 3 form a gas flow channel, hydrogen flows in the gas flow channel, solid hydrogen storage composite materials are filled between the adjacent inner tank separators 3 in the inner tank 1, and each solid hydrogen storage composite material comprises a rare earth-based hydrogen storage alloy (composition is LaNi 5) and expanded graphite, wherein the mass ratio of rare earth-based hydrogen storage alloy to the expanded graphite is 0.03:1.
As shown in fig. 1 and 4, along the vertical direction of the outer tank 2, a plurality of outer tank separators 4 are horizontally arranged inside the outer tank 2, the outer tank separators 4 are in the shape of unfilled corner rings 6, the outer cambered surfaces of the unfilled corner rings 6 are detachably connected with the inner peripheral wall of the outer tank 1, the inner cambered surfaces of the unfilled corner rings 6 are detachably connected with the outer peripheral wall of the inner tank 1, the radian of the unfilled corner rings 6 is 240 degrees, and the ratio of the maximum distance between the adjacent outer tank separators 4 to the height of the outer tank 4 is 0.42:1. The outer tank body partition boards 4 are arranged in parallel, the outer tank body partition boards 4 of the adjacent lower layers are used as references, the outer tank body partition boards 4 sequentially rotate in the same direction by 90 degrees along the axial direction of the outer tank body 2, a first diversion port (not shown in the figure) is arranged at the top of the outer tank body 2, a second diversion port (not shown in the figure) is arranged at the bottom of the outer tank body 2, heat conduction fluid enters the outer tank body flow channel through the first diversion port to be filled in the outer tank body 2, and the heat conduction fluid is deionized water.
In the hydrogen storage process, the pressure of a hydrogen inlet is maintained at 0.8MPa and is introduced into an inner tank body 1 to perform hydrogen absorption reaction with the solid hydrogen storage composite material in the inner tank body 1 under the pressure of the temperature of 293K at the initial temperature;
in the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction at the temperature of 343K and the pressure of 0.1MPa at the outlet pressure, and the 343K deionized water is introduced into the outer tank body 2 at the flow of 0.5L/min to provide heat for the desorption reaction of the hydrogen.
The simulation calculation according to example 1 gave the values of the various parameters in the reactor over time. As shown in fig. 14, the hydrogen absorption amount was changed with time, and after 518s from the start of the hydrogen absorption reaction, the hydrogen absorption amount in the hydrogen storage alloy reactor reached 90% of the maximum hydrogen absorption amount, and the hydrogen absorption time was reduced by 17% as compared with comparative example 1. As shown in FIG. 15, the total time for the increase of the inner tank temperature over 30K (323K) was 540s, which is a 15% decrease in the overtemperature time compared to comparative example 1.
As shown in FIG. 16, the hydrogen release rate was changed with time, and after 784s from the start of the hydrogen release reaction, the hydrogen release amount of the hydrogen storage alloy reactor released 90% of hydrogen, which was 32% less than that of comparative example 1.
Comparative example 1
According to the method of example 2, except that the inner tank 1 is not provided with the inner tank partition plate 3 inside and the outer tank 2 is not provided with the outer tank partition plate 4 inside in comparative example 1, as shown in fig. 17.
In the hydrogen storage process, the pressure of a hydrogen inlet is maintained at 0.8MPa and is introduced into an inner tank body to perform hydrogen absorption reaction with the solid hydrogen storage composite material in the inner tank body 1 under the pressure of the temperature of 293K at the initial temperature;
In the hydrogen release process, the solid hydrogen storage composite material adsorbed with hydrogen is subjected to desorption reaction at an initial temperature of 343K and a constant outlet pressure of 0.1MPa, and deionized water of 343K is introduced into the outer tank body 2 at a flow rate of 0.48L/min to provide heat for the desorption reaction of hydrogen.
The simulation calculation according to example 1 gave the values of the various parameters in the reactor over time. As shown in fig. 18, the hydrogen absorption amount varies with time, and after 621s from the start of the hydrogen absorption reaction, the hydrogen absorption amount of the hydrogen absorbing alloy reactor reaches 90% of the maximum hydrogen absorption amount. As shown in fig. 19, the total time for the inner tank temperature to rise above 30K (323K) is 632s.
As shown in FIG. 20, the hydrogen release rate was changed with time, and after 1160s of the hydrogen release reaction, the hydrogen gas was released from the hydrogen storage alloy reactor in an amount of 90%.
As is apparent from the above examples and comparative examples, the hydrogen absorbing alloy reactor provided by the present invention has the effect of increasing the reaction rate of hydrogen absorption and desorption and reducing the temperature of the tank container.
The preferred embodiments of the present invention have been described in detail above, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, a number of simple variants of the technical solution of the invention are possible, including combinations of the individual technical features in any other suitable way, which simple variants and combinations should likewise be regarded as being disclosed by the invention, all falling within the scope of protection of the invention.

Claims (35)

1.一种储氢合金反应器，其特征在于，所述反应器包括竖直设置的内罐体（1）以及套设在内罐体（1）外部的外罐体（2）；1. A hydrogen storage alloy reactor, characterized in that the reactor comprises a vertically arranged inner tank (1) and an outer tank (2) sleeved outside the inner tank (1). 沿内罐体（1）竖直方向，所述内罐体（1）内部水平设置有多个内罐体隔板（3）；Along the vertical direction of the inner tank (1), multiple inner tank partitions (3) are horizontally arranged inside the inner tank (1). 沿外罐体（2）竖直方向，所述外罐体（2）内部水平设置有多个外罐体隔板（4）；Along the vertical direction of the outer tank (2), multiple outer tank partitions (4) are horizontally arranged inside the outer tank (2). 所述内罐体隔板（3）上开设有开孔（5），所述开孔（5）用于氢气的流通；The inner tank partition (3) is provided with an opening (5) for the flow of hydrogen. 所述外罐体隔板（4）呈缺角圆环（6）状，所述外罐体隔板（4）用于导热流体的流通，所述导热流体通过缺角圆环（6）的缺角流通；The outer tank partition (4) is in the shape of a notched ring (6). The outer tank partition (4) is used for the flow of heat-conducting fluid. The heat-conducting fluid flows through the notched corner of the notched ring (6). 所述开孔（5）的个数为一个，所述开孔（5）的开孔面积与内罐体隔板（3）的面积比为0.01-0.2：1；The number of openings (5) is one, and the ratio of the opening area of the opening (5) to the area of the inner tank partition (3) is 0.01-0.2:1; 所述内罐体隔板（3）的圆心与开孔（5）的圆心之间的距离与内罐体（1）的内径比值为0.15-0.45：1；The ratio of the distance between the center of the inner tank partition (3) and the center of the opening (5) to the inner diameter of the inner tank (1) is 0.15-0.45:1; 以最底层的内罐体隔板（3）为基准，多个内罐体隔板（3）沿内罐体（1）的轴向依次同向转动90-180°；Based on the bottom inner tank partition (3), multiple inner tank partitions (3) rotate in the same direction for 90-180° along the axial direction of the inner tank (1); 所述缺角圆环（6）的弧度为240-355°；The arc of the missing corner ring (6) is 240-355°; 以最底层的外罐体隔板（4）为基准，多个外罐体隔板（4）沿外罐体（2）的轴向依次同向转动90-180°。Based on the bottom outer tank partition (4), multiple outer tank partitions (4) rotate in the same direction for 90-180° along the axial direction of the outer tank (2). 2.根据权利要求1所述的反应器，其中，所述内罐体（1）和外罐体（2）的高度各自独立地为50-2000mm。2. The reactor according to claim 1, wherein the height of the inner tank (1) and the outer tank (2) is independently 50-2000 mm. 3.根据权利要求2所述的反应器，其中，所述内罐体（1）和外罐体（2）的高度各自独立地为150-800mm。3. The reactor according to claim 2, wherein the height of the inner tank (1) and the outer tank (2) is independently 150-800 mm. 4.根据权利要求1所述的反应器，其中，所述内罐体（1）的内径为5-80mm。4. The reactor according to claim 1, wherein the inner diameter of the inner tank (1) is 5-80 mm. 5.根据权利要求4所述的反应器，其中，所述内罐体（1）的内径为10-40mm。5. The reactor according to claim 4, wherein the inner diameter of the inner tank (1) is 10-40 mm. 6.根据权利要求1所述的反应器，其中，所述外罐体（2）的内径为15-160mm。6. The reactor according to claim 1, wherein the inner diameter of the outer tank (2) is 15-160 mm. 7.根据权利要求6所述的反应器，其中，所述外罐体（2）的内径为30-90mm。7. The reactor according to claim 6, wherein the inner diameter of the outer tank (2) is 30-90 mm. 8.根据权利要求1所述的反应器，其中，所述外罐体（2）和内罐体（1）的内径差与内罐体（1）的内径的比值为0.2-3：1。8. The reactor according to claim 1, wherein the ratio of the difference in inner diameter between the outer tank (2) and the inner tank (1) to the inner diameter of the inner tank (1) is 0.2-3:1. 9.根据权利要求8所述的反应器，其中，所述外罐体（2）和内罐体（1）的内径差与内罐体（1）的内径的比值为0.35-2：1。9. The reactor according to claim 8, wherein the ratio of the difference in inner diameter between the outer tank (2) and the inner tank (1) to the inner diameter of the inner tank (1) is 0.35-2:1. 10.根据权利要求1所述的反应器，其中，所述开孔（5）的开孔面积与内罐体隔板（3）的面积比为0.04-0.1：1。10. The reactor according to claim 1, wherein the ratio of the opening area of the opening (5) to the area of the inner tank partition (3) is 0.04-0.1:1. 11.根据权利要求1所述的反应器，其中，所述开孔（5）的直径为2-20mm。11. The reactor according to claim 1, wherein the diameter of the opening (5) is 2-20 mm. 12.根据权利要求11所述的反应器，其中，所述开孔（5）的直径为2-15mm。12. The reactor according to claim 11, wherein the diameter of the opening (5) is 2-15 mm. 13.根据权利要求1所述的反应器，其中，所述内罐体隔板（3）的圆心与开孔（5）的圆心之间的距离与内罐体（1）的内径比值为0.2-0.35：1。13. The reactor according to claim 1, wherein the ratio of the distance between the center of the inner tank partition (3) and the center of the opening (5) to the inner diameter of the inner tank (1) is 0.2-0.35:1. 14.根据权利要求1所述的反应器，其中，以最底层的内罐体隔板（3）为基准，多个内罐体隔板（3）沿内罐体（1）的轴向依次同向转动120-180°。14. The reactor according to claim 1, wherein, with the bottom inner tank partition (3) as a reference, the plurality of inner tank partitions (3) rotate sequentially in the same direction for 120-180° along the axial direction of the inner tank (1). 15.根据权利要求1所述的反应器，其中，相邻内罐体隔板（3）之间的最大间距与内罐体（1）高度的比值为0.05-0.5：1。15. The reactor according to claim 1, wherein the ratio of the maximum distance between adjacent inner tank partitions (3) to the height of the inner tank (1) is 0.05-0.5:1. 16.根据权利要求15所述的反应器，其中，所述相邻内罐体隔板（3）之间的最大间距与内罐体（1）高度的比值为0.05-0.35：1。16. The reactor according to claim 15, wherein the ratio of the maximum distance between the adjacent inner tank partitions (3) to the height of the inner tank (1) is 0.05-0.35:1. 17.根据权利要求1所述的反应器，其中，所述缺角圆环（6）的弧度为300-345°。17. The reactor according to claim 1, wherein the arc of the notched annulus (6) is 300-345°. 18.根据权利要求1所述的反应器，其中，以最底层的外罐体隔板（4）为基准，多个外罐体隔板（4）沿外罐体（2）的轴向依次同向转动120-180°。18. The reactor according to claim 1, wherein, with the bottom outer tank partition (4) as a reference, a plurality of outer tank partitions (4) rotate sequentially in the same direction for 120-180° along the axial direction of the outer tank (2). 19.根据权利要求1所述的反应器，其中，相邻外罐体隔板（4）之间的最大间距与外罐体（2）高度的比值为0.05-0.5：1。19. The reactor according to claim 1, wherein the ratio of the maximum distance between adjacent outer tank partitions (4) to the height of the outer tank (2) is 0.05-0.5:1. 20.根据权利要求19所述的反应器，其中，所述相邻外罐体隔板（4）之间的最大间距与外罐体（2）高度的比值为0.08-0.25：1。20. The reactor according to claim 19, wherein the ratio of the maximum distance between the adjacent outer tank partitions (4) to the height of the outer tank (2) is 0.08-0.25:1. 21.根据权利要求15所述的反应器，其中，所述相邻内罐体隔板（3）之间放置有固体储氢复合材料，所述固体储氢复合材料包括储氢合金和/或导热材料。21. The reactor according to claim 15, wherein a solid hydrogen storage composite material is placed between the adjacent inner tank partitions (3), the solid hydrogen storage composite material comprising a hydrogen storage alloy and/or a thermally conductive material. 22.根据权利要求21所述的反应器，其中，所述储氢合金和导热材料的质量比为1：0.02-0.1。22. The reactor according to claim 21, wherein the mass ratio of the hydrogen storage alloy to the thermally conductive material is 1:0.02-0.1. 23.根据权利要求21所述的反应器，其中，所述储氢合金选自钛系储氢合金、锆系储氢合金、钒系储氢合金和稀土系储氢合金中的至少一种。23. The reactor according to claim 21, wherein the hydrogen storage alloy is selected from at least one of titanium-based hydrogen storage alloys, zirconium-based hydrogen storage alloys, vanadium-based hydrogen storage alloys, and rare earth-based hydrogen storage alloys. 24.根据权利要求23所述的反应器，其中，所述导热材料选自膨胀石墨、导热纤维、石墨片、碳纳米管、铝粉、铜粉、钛粉、泡沫铝、泡沫镍和泡沫铜中的至少一种。24. The reactor according to claim 23, wherein the thermally conductive material is selected from at least one of expanded graphite, thermally conductive fiber, graphite sheet, carbon nanotube, aluminum powder, copper powder, titanium powder, aluminum foam, nickel foam, and copper foam. 25.根据权利要求1所述的反应器，其中，所述导热流体选自水、乙二醇和导热油中的至少一种。25. The reactor according to claim 1, wherein the heat transfer fluid is selected from at least one of water, ethylene glycol, and heat transfer oil. 26.根据权利要求1所述的反应器，其中，所述内罐体（1）、外罐体（2）、内罐体隔板（3）以及外罐体隔板（4）的材质各自独立地选自铝、铝合金、铜、铜合金、碳钢和不锈钢中的至少一种。26. The reactor according to claim 1, wherein the materials of the inner tank (1), the outer tank (2), the inner tank partition (3) and the outer tank partition (4) are each independently selected from at least one of aluminum, aluminum alloy, copper, copper alloy, carbon steel and stainless steel. 27.根据权利要求1所述的反应器，其中，所述内罐体（1）的顶部设置有气管（7），所述气管（7）用于向内罐体（1）通入氢气或者释放内罐体（1）中的氢气。27. The reactor according to claim 1, wherein a gas pipe (7) is provided at the top of the inner tank (1), the gas pipe (7) being used to introduce hydrogen into the inner tank (1) or to release hydrogen from the inner tank (1). 28.根据权利要求27所述的反应器，其中，所述气管（7）内部设置有过滤器（8），所述过滤器（8）为铜基和/或不锈钢基多孔烧结体。28. The reactor according to claim 27, wherein a filter (8) is provided inside the gas pipe (7), the filter (8) being a copper-based and/or stainless steel-based porous sintered body. 29.根据权利要求28所述的反应器，其中，所述过滤器（8）为通过粉末冶金方法烧结而成的铜基和/或不锈钢基多孔烧结体。29. The reactor according to claim 28, wherein the filter (8) is a copper-based and/or stainless steel-based porous sintered body formed by powder metallurgy. 30.根据权利要求28所述的反应器，其中，所述过滤器（8）的精度为0.5-2μm。30. The reactor according to claim 28, wherein the filter (8) has an accuracy of 0.5-2 μm. 31.一种储氢和放氢的方法，其中，储氢过程和放氢过程于权利要求1-30中任意一项所述的储氢合金反应器中进行，该方法包括：31. A method for storing and releasing hydrogen, wherein the hydrogen storage process and the hydrogen release process are carried out in a hydrogen storage alloy reactor according to any one of claims 1-30, the method comprising: 储氢过程：将氢气通入内罐体（1），氢气与内罐体隔板（3）之间的固体储氢复合材料进行吸氢反应，并将导热流体通入外罐体（2），以吸取吸氢反应产生的热量；Hydrogen storage process: Hydrogen gas is introduced into the inner tank (1), and the hydrogen gas and the solid hydrogen storage composite material between the inner tank partition (3) undergo hydrogen absorption reaction. Heat-conducting fluid is introduced into the outer tank (2) to absorb the heat generated by the hydrogen absorption reaction. 放氢过程：将吸附有氢气的固体储氢复合材料进行解吸反应，然后将导热流体通入外罐体（2），以提供氢气的解吸反应所需热量。Hydrogen release process: The solid hydrogen storage composite material adsorbed with hydrogen is subjected to a desorption reaction, and then a heat-conducting fluid is introduced into the outer tank (2) to provide the heat required for the desorption reaction of hydrogen. 32.根据权利要求31所述的方法，其中，32. The method according to claim 31, wherein, 在储氢过程中，所述吸氢反应的条件包括：温度为10-50℃，压力为0.5-50MPa。During hydrogen storage, the conditions for the hydrogen absorption reaction include: a temperature of 10-50℃ and a pressure of 0.5-50MPa. 33.根据权利要求31所述的方法，其中，在储氢过程中，导热流体的温度为10-50℃，导热流体的流速为0.1-100L/min。33. The method according to claim 31, wherein, during the hydrogen storage process, the temperature of the heat transfer fluid is 10-50°C and the flow rate of the heat transfer fluid is 0.1-100 L/min. 34.根据权利要求31所述的方法，其中，34. The method according to claim 31, wherein, 在放氢过程中，所述解吸反应的条件包括：温度为30-200℃，压力为0.1-50MPa。During the hydrogen release process, the desorption reaction conditions include: a temperature of 30-200℃ and a pressure of 0.1-50MPa. 35.根据权利要求31所述的方法，其中，在放氢过程中，导热流体的温度为30-200℃，导热流体的流速为0.05-100L/min。35. The method according to claim 31, wherein, during the hydrogen release process, the temperature of the heat transfer fluid is 30-200°C, and the flow rate of the heat transfer fluid is 0.05-100 L/min.
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