CN112777564A - Magnesium-nickel-petroleum coke active carbon composite hydrogen storage material and preparation method thereof - Google Patents
Magnesium-nickel-petroleum coke active carbon composite hydrogen storage material and preparation method thereof Download PDFInfo
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- CN112777564A CN112777564A CN202110130698.9A CN202110130698A CN112777564A CN 112777564 A CN112777564 A CN 112777564A CN 202110130698 A CN202110130698 A CN 202110130698A CN 112777564 A CN112777564 A CN 112777564A
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- 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
- C01B3/0078—Composite solid storage mediums, i.e. coherent or loose mixtures of different solid constituents, chemically or structurally heterogeneous solid masses, coated solids or solids having a chemically modified surface region
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- 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
Abstract
The invention relates to a magnesium-nickel-petroleum coke active carbon composite hydrogen storage material and a preparation method thereof, belonging to the technical field of hydrogen storage alloy materials. The method comprises the following steps of 1: preparing petroleum coke activated carbon; step 2: preparing Mg-Ni hydrogen storage alloy; and step 3: loading of the composite hydrogen storage material: 31) uniformly mixing the petroleum coke activated carbon prepared in the step 1 and the Mg-Ni hydrogen storage alloy prepared in the step 2, and then placing the mixture in a muffle furnace protected by argon atmosphere for high-temperature sintering; 32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment; 33) and (3) placing the activated composite hydrogen storage material in a tabletting machine, and extruding into a cylinder shape. The invention can generate the ball cage effect by utilizing the dense aperture and clearance of the petroleum coke active carbon, effectively limits the discrete aggregation of the pulverized hydrogen storage alloy, and has the advantages of high hydrogen storage capacity, high hydrogen absorption and desorption rate, low strain accumulation and the like.
Description
Technical Field
The invention relates to the technical field of hydrogen storage alloy materials, and particularly provides a magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material and a preparation method thereof.
Background
Energy is an important basis on which human society depends to survive, fossil fuels used in large quantities at present are non-renewable and seriously polluted, energy challenges of different degrees are brought to various countries in the world, renewable clean energy is searched for and replaced, and the natural trend of economic development is formed.
The principle of hydrogen storage is that hydrogen reacts with alloy to generate reversible metal hydride for storage, the density of hydrogen storage is about 1000 times of that of hydrogen in standard condition, and adsorbed hydrogen can be released rapidly by regulating temperature and pressure. The hydrogen-storing alloy is AB5Type AB2Type, AB type, magnesium alloy and AB3Type, in which the theoretical hydrogen storage capacity of the magnesium-based hydrogen storage alloy is large (MgH)27.6 wt%), low cost and is of wide concern to researchers. But has higher thermal stability and poorer hydrogen absorption and desorption kinetics, thereby restricting the practical use of the catalyst. Meanwhile, the single method for filling the hydrogen storage alloy can lead the expansion stress of the alloy in the bed body to be continuously increased along with the cycle times, and further generate the profit aggregation effect to lead the reaction bed to deform and lose efficacy.
Aiming at the problems, the method of mixing and filling the heat conduction rate of hydrogen absorption and desorption of the hydrogen storage alloy by adopting the heat conduction materials such as foam metal and the like and the hydrogen storage alloy is a conventional method for improving the heat conduction rate of hydrogen absorption and desorption of the hydrogen storage alloy, but the overall mass hydrogen storage density is greatly reduced. The carbon material, especially the carbon nano tube, has the characteristics of low density, low price, high thermal conductivity and the like, and can also effectively improve the hydrogen absorption and desorption rate, but the preparation process of the nano material is complex, the cost is high, and the loading is completely uniform, so that the preparation method still has great difficulty. The high-sulfur petroleum coke super activated carbon (HSPC) is a supercritical gas adsorption material and has a molecular weight of more than 3500m2The specific surface area of the alloy per gram is large, the microporous structure is rich, the carbon structure of the alloy has good thermal conductivity, and the hydrogen absorption and desorption reaction rate of the Mg-Ni alloy can be improved after the scientific and reasonable load is carried.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a magnesium-nickel-petroleum coke active carbon composite hydrogen storage material and a preparation method thereof. Has the advantages of high hydrogen storage capacity, high hydrogen absorption and desorption rate, low strain accumulation and the like.
In order to solve the technical problems, the invention provides the following technical scheme:
in one aspect, the invention provides a preparation method of a magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material, which comprises the following steps:
step 1: preparing petroleum coke activated carbon;
step 2: preparing Mg-Ni hydrogen storage alloy;
and step 3: loading of the composite hydrogen storage material:
31) uniformly mixing the petroleum coke activated carbon prepared in the step 1 and the Mg-Ni hydrogen storage alloy prepared in the step 2, and then placing the mixture in a muffle furnace protected by argon atmosphere for high-temperature sintering;
32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment;
33) and placing the activated composite hydrogen storage material in a tabletting machine, and extruding into a cylindrical sheet shape. The height of the cylindrical sheet is 0.5-2cm, and the diameter can be designed according to the commonly used cylindrical hydrogen storage reactor on the market.
Further, the step 1 specifically comprises:
11) mixing high-sulfur petroleum coke with KOH according to the mass ratio of 1: 3-1: 4, and carrying out chemical activation and high-temperature carbonization in a tubular furnace under the protection of high-purity nitrogen: raising the temperature to 400-500 ℃ at a heating rate of 5-10 ℃/min, keeping the temperature for 1-2 h, then raising the temperature to 700-800 ℃, keeping the temperature for 1-2 h, and cooling to room temperature for later use;
12) adding a 1mol/L HCl solution into the mixture to adjust the pH value to 7;
13) drying the activated carbon and grinding the dried activated carbon to an average particle size of 100 microns for later use.
Further, the step 2 specifically comprises:
21) putting Mg powder and Ni powder in a mass ratio of 84: 16-89: 11 into a ball mill, performing ball milling in a vacuum atmosphere, controlling the ball-material ratio to be 20: 1-40: 1, and the time to be 4-6 h, and milling until the average particle size is 40-60 mu m for later use;
22) placing the ball-milled Mg-Ni alloy in a hydrogenation reactor, controlling the hydrogen pressure to be 5-6 Mpa, the activation temperature to be-300 ℃ and the time to be 2 hours.
Preferably, in the step 31), the mass ratio of the petroleum coke activated carbon to the Mg-Ni hydrogen storage alloy is 1: 19-1: 4.
Preferably, the petroleum coke active carbon prepared in the step 1 and the Mg-Ni hydrogen storage alloy prepared in the step 2 are mixed in a shaking table for 0.5 to 1 hour.
Further, in the step 32), the activation treatment specifically includes: the temperature is 300 ℃, the hydrogen pressure is 5Mpa, the hydrogen absorption and desorption cycle is 2 hours, the cycle is 5 times totally, and the surface powder is discarded.
On the other hand, the invention also provides a magnesium nickel-petroleum coke active carbon composite hydrogen storage material which is prepared by the preparation method of the magnesium nickel-petroleum coke active carbon composite hydrogen storage material.
The composite hydrogen storage material comprises petroleum coke activated carbon and Mg-Ni alloy, the shape of the composite hydrogen storage material is a compact disc, the internal structure of the composite hydrogen storage material is a porous structure, the composite mode of the petroleum coke activated carbon and the hydrogen storage alloy is high-temperature molten state mixing and mechanical tabletting, the mass proportion of the petroleum coke activated carbon is 5-20% of that of the composite hydrogen storage material, the preparation mode of the Mg-Ni alloy is high-energy mechanical ball milling, and the Mg-Ni alloy is completely activated before modification. The hydrogen can be absorbed in a two-stage way, namely in a two-temperature range of high temperature (Mg-Ni alloy) and low temperature (activated carbon), and the integral hydrogen storage amount is more than 5 wt%.
According to the invention, Mg-Ni alloy is loaded on the surface and in the pores of the petroleum coke activated carbon through high-temperature sintering and tabletting technologies, and hydrogen is stored in a supercritical adsorption and chemical adsorption double hydrogen storage mode in a limited space, so that on one hand, the catalytic action of the petroleum coke activated carbon obviously improves the current situation of low hydrogen adsorption and desorption kinetics of Mg-Ni alloy, on the other hand, the dense pore diameter and gaps of the petroleum coke activated carbon can generate a ball cage effect to form an immobilized unit loading mode, the discrete aggregation of pulverized hydrogen storage alloy is effectively limited, and the risk of reaction bed plastic deformation failure caused by stress accumulation generated by a single hydrogen storage alloy loading method is greatly reduced. The composite hydrogen storage material has the characteristics of high hydrogen storage capacity, high hydrogen absorption and desorption rate, low strain accumulation and the like, the total hydrogen storage capacity is more than 5 wt% under the conditions of low temperature, high pressure, high temperature and high pressure, the stability of the hydrogen storage reaction bed equipment is improved, and the composite hydrogen storage material can be used as one of the choices of high-efficiency hydrogen storage application materials.
Compared with the prior art, the invention has the following beneficial effects:
1. the composite hydrogen storage material has a supercritical adsorption and chemical adsorption double hydrogen storage mode simultaneously during hydrogen absorption, and can fully utilize the outer space of the hydrogen storage alloy and increase the whole hydrogen storage capacity.
2. The fully pulverized Mg-Ni alloy is fully fused with the wall surface, the gap and the aperture of the petroleum coke activated carbon through high-temperature oxygen-free sintering and hydrogen absorption pulverization circulation, the contact area is further increased after mechanical tabletting treatment, and the integral heat conductivity coefficient of the composite Mg-Ni alloy is effectively improved.
3. The rich pore structure in the petroleum coke activated carbon can provide a stable and smooth hydrogen channel for the hydrogen storage alloy, and is beneficial to improving the hydrogen absorption and desorption rate of the hydrogen storage alloy.
4. The dense pore diameter and the dense gap of the petroleum coke activated carbon are used as ball cages to limit the deposition accumulation effect of the pulverized alloy, an immobilized unit load mode is formed, the phenomenon of uneven stress caused by hydrogen absorption and desorption pulverization of a single Mg-Ni alloy reaction bed is greatly relieved, and the safety and the reliability of hydrogen storage equipment are guaranteed.
Drawings
FIG. 1 is a schematic view of loading of magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material in example 1 of the present invention;
FIG. 2 is a schematic disc packing diagram of the Mg-Ni-Petroleum coke activated carbon composite hydrogen storage material prepared in example 1 of the present invention;
fig. 3 is a flow chart of a preparation process of the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material in example 1 of the present invention.
Detailed Description
In order to make the technical problems, technical solutions and advantages to be solved by the present invention clearer, the following detailed description is made with reference to the accompanying drawings and specific embodiments.
The materials used in the examples and comparative examples were commercially available unless otherwise specified.
The invention provides a magnesium-nickel-petroleum coke active carbon composite hydrogen storage material and a preparation method thereof, and the specific embodiment is as follows.
Example 1
A preparation method of magnesium nickel-petroleum coke active carbon composite hydrogen storage material is shown in figure 1, and comprises the following steps:
step 1: preparing petroleum coke activated carbon:
11) mixing high-sulfur petroleum coke with KOH according to the mass ratio of 1:3, putting the mixture into a tubular furnace, and performing chemical activation and high-temperature carbonization under the protection of high-purity nitrogen: raising the temperature to 400 ℃ at the heating rate of 5 ℃/min, keeping the temperature for 1h for chemical activation, then raising the temperature to 800 ℃ and keeping the temperature for 1h for high-temperature carbonization, and cooling to room temperature for later use;
12) adding a 1mol/L HCl solution into the mixture to adjust the pH value to 7;
13) drying the activated carbon and grinding the dried activated carbon to an average particle size of 100 microns for later use;
step 2: preparing Mg-Ni hydrogen storage alloy:
21) putting Mg powder and Ni powder in a mass ratio of 84:16 into a ball mill, carrying out ball milling in a vacuum atmosphere, controlling the ball-material ratio to be 20: 1-30: 1, and grinding for 3-5 h until the average particle size is 40-60 mu m for later use;
22) placing the ball-milled Mg-Ni alloy in a hydrogenation reactor, controlling the hydrogen pressure to be 5Mpa, the activation temperature to be 300 ℃ and the time to be 2 h;
and step 3: loading of the composite hydrogen storage material:
31) putting petroleum coke activated carbon and Mg-Ni hydrogen storage alloy in a weight ratio of 1:19 into a shaking table in a glove box, vibrating and mixing for 0.5h in argon atmosphere, and then putting the mixture into a muffle furnace protected by argon atmosphere for high-temperature sintering at 1500 ℃ for 1 h;
32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment, wherein the temperature is 300 ℃, the hydrogen pressure is 5Mpa, the hydrogen absorption and desorption cycle is 2h, the cycle is 5 times totally, and the surface powder is discarded;
33) and placing the activated composite hydrogen storage material in a glove box tabletting machine, and extruding into a cylindrical sheet suitable for a reactor.
The invention provides a magnesium-nickel-petroleum coke active carbon composite hydrogen storage material formed by mixed sintering and tabletting, as shown in figure 1, the particle size of Mg-Ni alloy after high-energy ball milling and a plurality of hydrogen absorption and desorption cycles is further reduced, the alloy is loaded among pore structures rich in petroleum coke active carbon, part of Mg-Ni alloy 3 enters a macroporous structure 1, the heat transfer efficiency is rapidly improved due to the structural integration, the pore diameter of the active carbon is filled with a large amount of molecular hydrogen under high pressure, the molecular hydrogen and the Mg-Ni alloy 3 rapidly react to form atomic hydrogen, and it is necessary to point out that the dispersion force between nonpolar molecular hydrogen and the active carbon in the hydrogen desorption process can accelerate the precipitation of the molecular hydrogen, so the hydrogen absorption and desorption efficiency of the part of Mg-Ni alloy 3 is greatly improved.
Part of Mg-Ni alloy 3 is inserted into the structures of the mesopores and the micropores 2, in a plurality of hydrogen absorption and desorption reaction cycles, the Mg-Ni alloy 3 is gradually pulverized, alloy powder is limited by the structures of the mesopores and the micropores 2 and flows along with the action of air flow and gravity in a limited area, the alloy powder cannot contact with powder in other areas, the stress accumulation phenomenon at the rear end part and the lower part of a single hydrogen storage alloy reaction bed is weakened, and the safety of the reaction bed is improved.
Part of the Mg-Ni alloy 3 is fixed on the surface or in the gap outside the structures of the macropore 1 and the mesopore 2 and the micropore 2, the part of the Mg-Ni alloy 3 only improves the heat conductivity coefficient of solid phase heat transfer, and the hydrogen storage efficiency and the stress relief degree are not greatly improved for the whole structure, so the Mg-Ni alloy 3 is pulverized and removed in advance in the hydrogen absorption and desorption reaction before the tabletting and forming step, only the Mg-Ni alloy 3 inserted in the structures of the macropore 1 or the mesopore 2 and the micropore 2 is reserved, and the cost performance of the whole composite hydrogen storage material is enhanced.
The forming process mainly comprises the following steps: shaking table vibration mixing in argon atmosphere, muffle furnace sintering under argon atmosphere protection, hydrogen absorption and desorption circulation for 5 times, impurity removal, and tabletting and forming. The Mg-Ni alloy and the active carbon are fully mixed through a shaking table, then high-temperature oxygen-free sintering is carried out, the alloy is melted on the premise of not damaging the pore structure of the active carbon, then a plurality of circulating hydrogen absorption pulverization are carried out to remove the surface alloy powder, the hydrogen storage alloy is uniformly distributed in the internal space of the active carbon to form a ball cage effect, the contact area between the composite materials is further increased through the final tabletting process, the ball cage effect is enhanced, the material stability is further improved, and the safe and efficient material with high hydrogen storage capacity, rapid hydrogen absorption and desorption and low strain accumulation is prepared. The composite material relates to the technology of vacuum oxygen-free sintering, hydrogen absorption circulation and mechanical tabletting, and has simple process and lower manufacturing cost.
As shown in fig. 2, the magnesium nickel-petroleum coke activated carbon composite hydrogen storage material sample finally prepared by the invention is in a flat cylindrical shape, and can be applied to a cylindrical hydrogen storage reactor commonly used in the market, and the composite hydrogen storage material has a rich pore diameter structure, and a hydrogen channel is not required to be arranged, so that the space utilization of the reactor is maximized, and the composite hydrogen storage material can be simply stacked and filled without arranging an expansion slow release region.
Example 2
A preparation method of a magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material comprises the following steps:
and step 3: loading of the composite hydrogen storage material:
31) putting petroleum coke activated carbon and Mg-Ni hydrogen storage alloy in a weight ratio of 1:9 into a shaking table in a glove box, vibrating and mixing for 0.h in argon atmosphere, and then putting the mixture into a muffle furnace protected by argon atmosphere for high-temperature sintering at 1500 ℃ for 1 h;
32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment, wherein the hydrogenation temperature is 220 ℃, the hydrogen pressure is 2Mpa, the hydrogen absorption and desorption time is 10min, carrying out hydrogen absorption and desorption cycles for 5 times totally, and discarding surface powder;
33) and placing the activated composite hydrogen storage material in a glove box tabletting machine, and extruding into a cylindrical sheet suitable for a reactor.
Example 3
A preparation method of a magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material comprises the following steps:
and step 3: loading of the composite hydrogen storage material:
31) putting petroleum coke activated carbon and Mg-Ni hydrogen storage alloy in a weight ratio of 1:4 into a shaking table in a glove box, vibrating and mixing for 1h in argon atmosphere, and then putting the mixture into a muffle furnace protected by argon atmosphere for high-temperature sintering at 1500 ℃ for 2 h;
32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment, wherein the hydrogenation temperature is 250 ℃, the hydrogen pressure is 1Mpa, the hydrogen absorption and desorption time is 10min, carrying out hydrogen absorption and desorption cycles for 5 times totally, and discarding surface powder;
33) and placing the activated composite hydrogen storage material in a glove box tabletting machine, and extruding into a cylindrical sheet suitable for a reactor.
Comparative example 1
The petroleum coke activated carbon of step 1 of the comparative example is replaced by the conventional activated carbon, and the rest conditions are the same as those of the example 1.
Performance tests of the hydrogen storage materials prepared in the above examples 1-3 and comparative example 1 were carried out, and the test results of hydrogen absorption and desorption under different pressures and temperatures are shown in Table 1 according to GB/T33291-2016 'hydride reversible hydrogen absorption and desorption pressure-composition-isotherm (P-C-T) test method'.
TABLE 1
As can be seen from the above table, under the same hydrogen absorption and desorption conditions, the hydrogen storage capacity of the composite hydrogen storage material prepared by the invention is improved by more than 21% compared with that of the conventional activated carbon, and the hydrogen desorption time is not greatly different, but the composite hydrogen storage material prepared by the invention can reach hydrogen absorption saturation in a short time, and after hydrogen absorption and desorption are repeated for many times, the volume change rate is small, and the alloy pulverization phenomenon is greatly improved.
In addition, in the embodiments 1 to 3, the hydrogen absorption saturation can be quickly achieved under a lower hydrogen absorption pressure or temperature, and meanwhile, the hydrogen storage capacity is also larger.
In conclusion, the petroleum coke activated carbon is utilized to successfully load the hydrogen storage alloy, and a stable and smooth hydrogen channel is provided for the hydrogen storage alloy through the abundant pore structure in the petroleum coke activated carbon, so that the hydrogen absorption and desorption rate and capacity of the petroleum coke activated carbon are greatly improved.
While the foregoing is directed to the preferred embodiment of the present invention, it will be understood by those skilled in the art that various changes and modifications may be made without departing from the spirit and scope of the invention as defined in the appended claims.
Claims (7)
1. The preparation method of the magnesium-nickel-petroleum coke active carbon composite hydrogen storage material is characterized by comprising the following steps:
step 1: preparing petroleum coke activated carbon;
step 2: preparing Mg-Ni hydrogen storage alloy;
and step 3: loading of the composite hydrogen storage material:
31) uniformly mixing the petroleum coke activated carbon prepared in the step 1 and the Mg-Ni hydrogen storage alloy prepared in the step 2, and then placing the mixture in a muffle furnace protected by argon atmosphere for high-temperature sintering;
32) placing the sintered composite hydrogen storage material in a hydrogenation reactor for activation treatment;
33) and placing the activated composite hydrogen storage material in a tabletting machine, and extruding into a cylindrical sheet shape.
2. The preparation method of the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material according to claim 1, wherein the step 1 is specifically as follows:
11) mixing high-sulfur petroleum coke with KOH according to the mass ratio of 1: 3-1: 4, and carrying out chemical activation and high-temperature carbonization in a tubular furnace under the protection of high-purity nitrogen: raising the temperature to 400 ℃ at a heating rate of 5-10 ℃/min, keeping the temperature for 1-2 h, then raising the temperature to 800 ℃, keeping the temperature for 1-2 h, and cooling to room temperature for later use;
12) adding a 1mol/L HCl solution into the mixture to adjust the pH value to 7;
13) drying the activated carbon and grinding the dried activated carbon to an average particle size of 100 microns for later use.
3. The preparation method of the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material according to claim 1, wherein the step 2 specifically comprises the following steps:
21) putting Mg powder and Ni powder in a mass ratio of 84: 16-89: 11 into a ball mill, performing ball milling in a vacuum atmosphere, controlling the ball-material ratio to be 20: 1-40: 1, and the time to be 4-6 h, and milling until the average particle size is 40-60 mu m for later use;
22) and (3) placing the ball-milled Mg-Ni alloy in a hydrogenation reactor, controlling the hydrogen pressure to be 5-6 Mpa, the activation temperature to be 300 ℃, and the time to be 2 hours.
4. The preparation method of the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material as claimed in claim 1, wherein in the step 31), the mass ratio of the petroleum coke activated carbon to the Mg-Ni hydrogen storage alloy is 1: 19-1: 9.
5. The method for preparing the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material according to claim 4, wherein the mixing of the petroleum coke activated carbon prepared in the step 1 and the Mg-Ni hydrogen storage alloy prepared in the step 2 is carried out in a shaking table for 0.5-1 h.
6. The method for preparing the magnesium-nickel-petroleum coke activated carbon composite hydrogen storage material according to claim 1, wherein in the step 32), the activation treatment specifically comprises the following steps: the temperature is 300 ℃, the hydrogen pressure is 5Mpa, the hydrogen absorption and desorption are circulated for 2h and 5 times, and the surface powder is discarded.
7. A magnesium nickel-petroleum coke active carbon composite hydrogen storage material is characterized by being prepared by the preparation method of the magnesium nickel-petroleum coke active carbon composite hydrogen storage material according to any one of claims 1 to 6.
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