CN110980636A - Magnesium hydride hydrogen storage composite material containing porous material and preparation method thereof - Google Patents
Magnesium hydride hydrogen storage composite material containing porous material and preparation method thereof Download PDFInfo
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- CN110980636A CN110980636A CN201911420422.3A CN201911420422A CN110980636A CN 110980636 A CN110980636 A CN 110980636A CN 201911420422 A CN201911420422 A CN 201911420422A CN 110980636 A CN110980636 A CN 110980636A
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- hydrogen storage
- porous material
- magnesium hydride
- storage composite
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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
- C01B3/0005—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes
- C01B3/001—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes characterised by the uptaking medium; Treatment thereof
- C01B3/0084—Solid storage mediums characterised by their shape, e.g. pellets, sintered shaped bodies, sheets, porous compacts, spongy metals, hollow particles, solids with cavities, layered solids
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- 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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- Inorganic Chemistry (AREA)
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Abstract
The invention belongs to the technical field of inorganic porous materials, and particularly relates to a magnesium hydride hydrogen storage composite material containing a porous material and a preparation method thereof. The magnesium hydride hydrogen storage composite material containing the porous material is formed by compounding magnesium hydride and the porous material, the weight ratio of the magnesium hydride to the porous material is 0.1-1.2:1, and the porous material is graphite and SiO2Or Al2O3Mixing magnesium hydride with the porous material; the mixture is then shaped by compression to produce a magnesium hydride hydrogen storage composite. The invention uses the porous material with adjustable pore diameter as the carrier, so that the hydrogen storage performance of the magnesium hydride is combined with the excellent pore channels, high specific surface area and other performances of the porous material, and the hydrogen storage material has good characteristics in the aspects of hydrogen adsorption and desorption kinetics. The invention compositely forms the hydrogen storage material by compression, can improve the hydrogen storage density per unit volume and improve the mechanical strength.
Description
Technical Field
The invention belongs to the technical field of inorganic porous materials, and particularly relates to a magnesium hydride hydrogen storage composite material containing a porous material and a preparation method thereof.
Background
Magnesium-based metal hydrogen storage materials have been considered as ideal hydrogen storage materials because of their large hydrogen storage capacity, light weight, low price and abundant resources. However, magnesium and its alloys also have three disadvantages: 1. the hydrogen absorption and desorption speed is slow, and the reaction kinetic performance is poor; 2. the hydride is stable, and higher temperature is needed for hydrogen discharge; 3. the practical application of magnesium-based metal hydrogen storage materials is seriously hindered by the defects that a compact oxide film is easily formed on the surface of magnesium and magnesium alloy.
Therefore, scientists in various countries have made researches around the preparation, nanocrystallization and recombination of magnesium-based hydrogen storage materials to overcome the above-mentioned drawbacks, and have made a favorable progress while keeping the hydrogen storage amount large and the hydrogen release temperature low.
Hydrogen is used in many industrial fields, in particular as a fuel (for example in the field of heat engines or fuel cells), or as a reagent (for example for hydrogenation reactions). Within this framework, it is desirable to store hydrogen in a small volume in a safe container, taking into account the volume of gaseous hydrogen and its explosiveness. Due to the conventional preparation method, the particle size of the magnesium-based hydrogen storage material is difficult to further reduce, and the development of a magnesium-based material which really has the physical effect of a nano material becomes the key for preparing the magnesium-based hydrogen storage material with good hydrogen storage performance.
The porous material has the characteristics of extremely high specific surface area, regular and ordered pore channel structure, narrow pore size distribution, continuously adjustable pore size and the like, so that the porous material plays a role in the adsorption and separation of macromolecules, particularly catalytic reaction, which are difficult to complete by a plurality of microporous zeolite molecular sieves. Moreover, the ordered pore channel of the material can be used as a ' microreactor ', and a uniform and stable ' guest ' material with a nano scale is assembled in the ' microreactor to form a ' host-guest material ', and the host-guest effect between the host and the guest and the possible small-size effect, quantum size effect and the like of the guest material can make the material hopefully be widely applied to the fields of electrode materials, photoelectric devices, microelectronic technologies, chemical sensors, nonlinear optical materials and the like. Therefore, since its birth, porous materials attract the international interest in the research fields of multiple subjects such as physics, chemistry, biology, materials and information, and are now one of the hot frontier fields across multiple subjects internationally.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: the magnesium hydride hydrogen storage composite material is compounded with the porous material by using the porous material with adjustable pore diameter as a carrier, so that the hydrogen storage performance of the magnesium hydride is combined with the excellent pore channels, high specific surface area and other performances of the porous material, and the hydrogen storage material has good characteristics in the aspects of hydrogen adsorption and desorption kinetics; meanwhile, the invention also provides a preparation method of the compound, which is simple, easy to operate, scientific and reasonable and suitable for industrial production.
The magnesium hydride hydrogen storage composite material containing the porous material is formed by compounding magnesium hydride and the porous material, and the weight ratio of the magnesium hydride to the porous material is 0.1-1.2: 1.
The porous material is graphite or SiO2Or Al2O3Preferably expanded natural graphite, which has a relatively large porosity, which increases its hydrogen storage capacity.
The particle size of the porous material is 5-35 μm.
The hydrogen storage composite is formed by compressing the material. The compressed form may impart mechanical strength to the material that facilitates handling.
The magnesium hydride hydrogen storage composite material containing the porous material comprises the following steps:
(1) mixing magnesium hydride with the porous material;
(2) the mixture is shaped by compression.
The magnesium hydride used to prepare the material is in powder form, preferably with a grain size of 3.5-7.5 μm.
Powder mixing may be carried out in a conventional manner, such as in a mixer. Mixing is preferably carried out at room temperature and atmospheric pressure.
The mixture is preferably compressed uniaxially, for example in a granulator.
It is advantageous to carry out the mixing and compression under a controlled atmosphere, especially when pyrophoric activated magnesium is used.
In particular, the external force applied during compression is selected according to the desired porosity of the material. For example, 1t/cm has been demonstrated2The compression of (a) can result in material particles having a porosity of 0.3.
Compression increases the volumetric stored hydrogen density and improves mechanical strength over a fluidized bed of magnesium hydride. Furthermore, the material thus obtained is no longer pyrophoric and is easier to handle.
The shaped material may then be subjected to mechanical processing, in particular in order to obtain a size suitable for the tank.
Other properties of the material related to hydrogen storage, such as hydrogen adsorption and desorption kinetics, are not affected by the material formation.
The material is conveniently handled even when incorporated with active magnesium hydride and has an improved hydrogen storage volume capability.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention uses the porous material with adjustable aperture as the carrier, and compounds the magnesium hydride and the porous material, so that the hydrogen storage performance of the magnesium hydride is combined with the excellent pore channels, high specific surface area and other performances of the porous material, and the hydrogen storage material has good characteristics in the aspects of hydrogen adsorption and desorption dynamics.
2. The invention compositely forms the hydrogen storage material by compression, can improve the hydrogen storage density per unit volume and improve the mechanical strength. Furthermore, the material thus obtained is no longer pyrophoric and is easier to handle.
Detailed Description
The present invention will be further described with reference to the following examples.
The starting materials used in the examples are commercially available unless otherwise specified.
Example 1
The magnesium hydride hydrogen storage composite material containing the porous material comprises the following steps:
47.5g of activated magnesium hydride powder having an average grain size of 4.0 μm was mixed with 35g of Expanded Natural Graphite (ENG) having an average grain size of 6.0 μm in a sealed mixer (inside a glove box under a controlled atmosphere).
The powder mixture was then poured into the die of a hardened steel pelletizer, also located in a glove box. The pelletizer was removed from the glove box in an air tight bag and placed under the press.
Passing intensity of 1t/cm2(108Pa) to compress the powder in the granulator.
Example 2
The magnesium hydride hydrogen storage composite material containing the porous material comprises the following steps:
in a sealed mixer (inside a glove box under a controlled atmosphere), 45g of activated magnesium hydride powder having an average grain size of 7.0 μm was mixed with 45g of activated alumina having an average grain size of 20 μm.
The powder mixture was then poured into the die of a hardened steel pelletizer, also located in a glove box. The pelletizer was removed from the glove box in an air tight bag and placed under the press.
Passing intensity of 1t/cm2(108Pa) to compress the powder in the granulator.
Example 3
The magnesium hydride hydrogen storage composite material containing the porous material comprises the following steps:
in a sealed mixer (inside a glove box under a controlled atmosphere), 45g of activated magnesium hydride powder having an average grain size of 3.5 μm was mixed with 100g of silica having an average grain size of 30 μm.
The powder mixture was then poured into the die of a hardened steel pelletizer, also located in a glove box. The pelletizer was removed from the glove box in an air tight bag and placed under the press.
Passing intensity of 1t/cm2(108Pa) to compress the powder in the granulator.
Examples 1-3 a compressed material having a diameter of 8cm was recovered and the material could be treated in an open environment for several minutes. However, it is preferred to store the composite material under a controlled atmosphere to avoid the risk of temperature increases and surface oxidation.
The density of the material in the different particles obtained was calculated by weighing and measuring the dimensions. The porosity was calculated from the theoretical and measured densities.
The particles have mechanical strength and stability and are sufficiently oxidizable to allow handling under conventional conditions (i.e., outside the glove box) for incorporation into a hydrogen storage tank.
The resulting granules have excellent mechanical strength. Thus, it can be machined for the purpose of, for example, adjusting the outer diameter to the diameter of the composite storage tank, or perforated for the insertion of heating elements and thermocouples. Similarly, no cracking or build-up of fine powder was observed at the bottom of the tank after repeated hydrogen cycles.
Performance detection
The magnesium hydride hydrogen storage composite particles obtained in examples 1-3 were reduced in diameter from 8cm to 7cm by mechanical processing, and 250g of the particles were charged to an internal diameter of 7cm and a volume of 270cm3The stainless steel cylindrical storage tank. The tank is equipped with heating means. The tank was then heated to 300 ℃ and placed under a hydrogen pressure of 8 bar.
The volume of hydrogen adsorbed over 3 hours was recorded using a flow meter. The temperature was trace recorded with probe devices placed in the center and around the tank. The test was conducted under the same conditions of realization, except that 110g of the activated magnesium hydride powder was used as a comparative example and the test data are shown in Table 1.
TABLE 1 EXAMPLES 1-3 AND COMPARATIVE EXAMPLES magnesium hydride Hydrogen storage Material test data
As can be seen from the data in Table 1, the magnesium hydride hydrogen storage composite material containing the porous material prepared in examples 1-3 has a more than two-fold capacity for increasing the volume of adsorbed hydrogen from 65L to 175L. A comparison of the temperatures generated at the center and periphery of the tank further shows that the temperatures are more uniform within the material according to the invention.
Of course, the foregoing is only a preferred embodiment of the invention and should not be taken as limiting the scope of the embodiments of the invention. The present invention is not limited to the above examples, and equivalent changes and modifications made by those skilled in the art within the spirit and scope of the present invention should be construed as being included in the scope of the present invention.
Claims (6)
1. A magnesium hydride hydrogen storage composite material containing a porous material is characterized in that: the magnesium hydride and the porous material are compounded, and the weight ratio of the magnesium hydride to the porous material is 0.1-1.2: 1.
2. The magnesium hydride hydrogen storage composite comprising a porous material of claim 1, wherein: the porous material is graphite or SiO2Or Al2O3One or more of (a).
3. The magnesium hydride hydrogen storage composite containing porous material of claim 1 or wherein: the particle size of the porous material is 5-35 μm.
4. The magnesium hydride hydrogen storage composite comprising a porous material of claim 1, wherein: the particle size of the magnesium hydride is 3.5-7.5 μm.
5. A method of preparing a magnesium hydride hydrogen storage composite containing a porous material as claimed in claim 1, wherein: the method comprises the following steps:
(1) mixing magnesium hydride with the porous material in a mixer;
(2) the mixture is shaped by compression.
6. The method of preparing a magnesium hydride hydrogen storage composite containing a porous material as claimed in claim 5, wherein: and (2) performing the compression in a granulator.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111850366A (en) * | 2020-06-12 | 2020-10-30 | 榆林学院 | Oxide-loaded magnesium-nickel alloy hydrogen storage composite material and preparation method thereof |
| CN114314793A (en) * | 2022-01-06 | 2022-04-12 | 青岛诺康新氢源研究院有限公司 | Hydrogen production particle capable of generating porous structure on site and preparation method and application thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101428756A (en) * | 2008-11-27 | 2009-05-13 | 中山大学 | Automatic hydrogen production method by using hydroboron composition |
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2019
- 2019-12-31 CN CN201911420422.3A patent/CN110980636A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101428756A (en) * | 2008-11-27 | 2009-05-13 | 中山大学 | Automatic hydrogen production method by using hydroboron composition |
Non-Patent Citations (3)
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| W.OELERICH ET AL.: "Metal oxides as catalysts for improved hydrogen sorption in nanocrystalline Mg-based materials", 《JOURNAL OF ALLOYS AND COMPOUNDS》 * |
| 卢国俭等: "大容量镁基储氢材料及其储氢性能", 《现代化工》 * |
| 王晓燕: "沸石分子筛及镁复合物的制备与储氢性能研究", 《中国优秀硕士学位论文全文数据库》 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111850366A (en) * | 2020-06-12 | 2020-10-30 | 榆林学院 | Oxide-loaded magnesium-nickel alloy hydrogen storage composite material and preparation method thereof |
| CN111850366B (en) * | 2020-06-12 | 2021-06-18 | 榆林学院 | Oxide-loaded magnesium-nickel alloy hydrogen storage composite material and preparation method thereof |
| CN114314793A (en) * | 2022-01-06 | 2022-04-12 | 青岛诺康新氢源研究院有限公司 | Hydrogen production particle capable of generating porous structure on site and preparation method and application thereof |
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Inventor after: Wang Ming Inventor after: Zhao Zengdian Inventor after: Xia Xianchang Inventor after: Hao Xiaoming Inventor after: Fu Qiang Inventor after: Zhang Fang Inventor after: Yu Rujun Inventor after: Guanfeng Steel Inventor after: Chen Yanyan Inventor after: Yang Kun Inventor after: Lv Junnan Inventor after: Yang Liening Inventor before: Wang Ming Inventor before: Zhao Zengdian Inventor before: Xia Xianchang Inventor before: Hao Xiaoming Inventor before: Fu Qiang Inventor before: Zhang Fang Inventor before: Yu Rujun Inventor before: Guanfeng Steel Inventor before: Chen Yanyan Inventor before: Yang Kun Inventor before: Lv Junnan Inventor before: Yang Liening |