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CN115367700A - Zinc-copper bimetallic MOF catalyzed MgH 2 Hydrogen storage material, method for the production thereof and use thereof - Google Patents

Zinc-copper bimetallic MOF catalyzed MgH 2 Hydrogen storage material, method for the production thereof and use thereof Download PDF

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CN115367700A
CN115367700A CN202211053007.0A CN202211053007A CN115367700A CN 115367700 A CN115367700 A CN 115367700A CN 202211053007 A CN202211053007 A CN 202211053007A CN 115367700 A CN115367700 A CN 115367700A
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CN115367700B (en
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丁佰锁
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Qingke Chongqing Advanced Materials Research Institute Co ltd
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    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/0005Reversible 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
    • C01B3/001Reversible 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
    • C01B3/0078Composite 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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    • B01J31/00Catalysts comprising hydrides, coordination complexes or organic compounds
    • B01J31/16Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes
    • B01J31/18Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms
    • B01J31/1805Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms the ligands containing nitrogen
    • B01J31/181Cyclic ligands, including e.g. non-condensed polycyclic ligands, comprising at least one complexing nitrogen atom as ring member, e.g. pyridine
    • B01J31/1815Cyclic ligands, including e.g. non-condensed polycyclic ligands, comprising at least one complexing nitrogen atom as ring member, e.g. pyridine with more than one complexing nitrogen atom, e.g. bipyridyl, 2-aminopyridine
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    • B01J31/223At least two oxygen atoms present in one at least bidentate or bridging ligand
    • B01J31/2239Bridging ligands, e.g. OAc in Cr2(OAc)4, Pt4(OAc)8 or dicarboxylate ligands
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/04Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • BPERFORMING OPERATIONS; TRANSPORTING
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    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/10Complexes comprising metals of Group I (IA or IB) as the central metal
    • B01J2531/16Copper
    • BPERFORMING OPERATIONS; TRANSPORTING
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    • B01J2531/00Additional information regarding catalytic systems classified in B01J31/00
    • B01J2531/20Complexes comprising metals of Group II (IIA or IIB) as the central metal
    • B01J2531/26Zinc
    • YGENERAL 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
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    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/32Hydrogen storage

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Abstract

The invention discloses MgH catalyzed by zinc-copper bimetallic MOF 2 The hydrogen storage material comprises the following components in parts by weight: 14 to 29 parts of copper salt, 12 to 27 parts of zinc salt, 30 to 60 parts of organic ligand, 16 to 31 parts of supporting solvent, 17 to 32 parts of organic solvent and 13 to 28 parts of water. The invention also discloses the MgH 2 The preparation method of the hydrogen storage material comprises the following steps: s1, uniformly mixing a supporting solvent, an organic solvent and water of the components to obtain a mixture solvent; s2, sequentially adding copper salt, zinc salt and organic ligand of the components into the mixture solvent, stirring and reacting for 2-5 h at room temperature, and performing centrifugal separation to obtain a solid substance; s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF; s4, drying to obtain the zinc-copper doubleMetal MOF and commercial MgH 2 Mixing and ball milling to obtain the magnesium-based composite hydrogen storage material catalyzed by MOF. The invention also discloses the MgH 2 Use of a hydrogen storage material.

Description

Zinc-copper bimetallic MOF catalyzed MgH 2 Hydrogen storage material, method for the production thereof and use thereof
Technical Field
The invention relates to the technical field of hydrogen storage materials, in particular to MgH catalyzed by zinc-copper bimetal MOF 2 Hydrogen storage material, method for the production and use thereof.
Background
At present, hydrogen is considered one of the most promising energy carriers. The safe and efficient storage of hydrogen is a major requirement for the practical application of hydrogen energy. Therefore, a safety is designedAn effective hydrogen storage material is of great importance for the application of hydrogen fuel cell vehicles. MgH, a simple metal hydride representative of this metal for decades 2 Has the advantages of large hydrogen storage density (7.6 percent by weight), good reversibility, environmental protection, good economic performance and the like. However, due to its thermodynamic stability and slow kinetics, mgH 2 The temperature at which hydrogen is absorbed/released is high, which hinders practical use thereof in fuel cells.
The MgH can be reduced by doping the catalyst 2 The working temperature of hydrogen adsorption/release effectively alleviates the high temperature problem. At present, various catalysts have been reported for increasing MgH 2 Including transition metals, transition metal oxides, hydrides, carbon materials, alloys, and the like. However, the catalyst is prone to aggregation during continuous, vigorous ball milling and subsequent cycling, resulting in a reduction in exposed catalytic sites, which severely affects catalytic performance. Therefore, the development of a superior catalyst having uniform distribution is of great significance for maintaining high catalytic activity of the hydrogen storage material.
Disclosure of Invention
The invention aims to: providing zinc-copper bimetallic MOF catalyzed MgH 2 Hydrogen storage material, method for producing same and use thereof for improving MgH 2 The reversible hydrogen storage performance of the invention is simple in synthesis process, mild in reaction condition, and effectively improves MgH by introducing the zinc-copper bimetallic MOF 2 The hydrogen absorption and desorption behaviors of the hydrogen storage material reduce the hydrogen desorption working temperature, and the preparation method of the catalyst is simple and easy to implement and can be widely applied to most hydrogen storage systems.
In order to achieve the purpose, the invention adopts the following technical scheme:
zinc-copper bimetallic MOF catalyzed MgH 2 The hydrogen storage material comprises the following components in parts by weight: 14 to 29 parts of copper salt, 12 to 27 parts of zinc salt, 30 to 60 parts of organic ligand, 16 to 31 parts of supporting solvent, 17 to 32 parts of organic solvent and 13 to 28 parts of water.
The above-mentioned zinc-copper bimetallic MOF catalyzed MgH 2 A method for preparing a hydrogen storage material,the method comprises the following steps:
s1, uniformly mixing a supporting solvent, an organic solvent and water of the components to obtain a mixture solvent;
s2, sequentially adding copper salt, zinc salt and organic ligand of the components into the mixture solvent, stirring and reacting for 2-5 h at room temperature, and performing centrifugal separation to obtain a solid substance;
s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF;
s4, mixing the dried zinc-copper bimetallic MOF with commercial MgH 2 Mixing and ball milling to obtain the magnesium-based composite hydrogen storage material catalyzed by MOF.
Further, the copper salt is one of cupric nitrate hydrate, copper sulfate hydrate and copper chloride hydrate;
the zinc salt is one of zinc nitrate dihydrate, zinc acetate dihydrate, zinc sulfate hydrate and zinc chloride hydrate;
the organic ligand is one of benzimidazole, trimesic acid, 1,3,5-tri (4-carboxyl phenyl) benzene and 2-methylimidazole;
the supporting solvent is one of ammonia water solution and dimethylformamide;
the organic solvent is one of methanol, ethanol, dichloromethane and acetone.
Further, the copper salt, the zinc salt, the organic ligand, the supporting solvent and the organic solvent are respectively copper nitrate hydrate, zinc nitrate dihydrate, trimesic acid, dimethylformamide and ethanol.
Further, the mixture ratio of the copper salt, the zinc salt, the organic ligand, the supporting solvent, the organic solvent and the water is as follows: 1.
Further, the centrifugal separation conditions in S2 are as follows: the centrifugal speed is 7000-10000 rpm, and the centrifugal time is controlled at 8-15 min.
Further, the washing and drying conditions in S3 are as follows: washing the obtained solid with ethanol and deionized water for 3 times respectively, and finally carrying out vacuum drying through an oven, wherein the drying temperature is 180-250 ℃, and the drying time is 5-8 h.
Further, mgH in S4 2 The mass ratio of the metal MOF to the zinc-copper bimetal MOF is 7-12.
Further, the ball milling time in the S4 is 4.5-5.5 h, and the ball milling rotating speed is controlled at 400-500 rpm.
Further, the zinc-copper bimetal MOF and MgH in S4 2 The ball milling is carried out in a hydrogen atmosphere, the pressure of the hydrogen is 1.8-2.2 MPa, and the ball-to-material ratio is 40-60.
The invention also provides MgH catalyzed by zinc-copper bimetallic MOF prepared by the preparation method 2 A hydrogen storage material.
The invention also provides MgH catalyzed by zinc-copper bimetallic MOF prepared by the preparation method 2 Use of a hydrogen storage material in a fuel cell.
The invention has at least the following beneficial effects:
in the invention, the synthesis process of the bimetallic MOF catalyst is simple, the reaction condition is mild, and the introduction of the zinc-copper bimetallic MOF effectively improves MgH 2 The hydrogen absorption and desorption behaviors of the hydrogen storage material reduce the hydrogen desorption working temperature, and the preparation method of the catalyst is simple and easy to implement and can be widely applied to most hydrogen storage systems.
Drawings
FIG. 1 shows MgH catalyzed by zinc-copper bimetallic MOF according to the invention 2 A PXRD pattern for the hydrogen storage material;
FIG. 2 is MgH catalyzed by zinc-copper bimetallic MOF according to the invention 2 Hydrogen storage material and pure MgH 2 H of (A) to (B) 2 Drawing;
FIG. 3 is MgH catalyzed by zinc-copper bimetallic MOF according to the invention 2 DSC curves of the hydrogen storage material at different temperature rising speeds and corresponding fitting;
FIG. 4 is for pure MgH 2 DSC curves at different ramp rates, and corresponding fits.
Detailed Description
In order that those skilled in the art can better understand the present invention, the following technical solutions are further described with reference to the accompanying drawings and examples.
Example 1
The zinc-copper bimetallic MOF catalyzed MgH of the invention 2 The hydrogen storage material comprises the following raw materials: 22g of a copper salt, 21g of a zinc salt, 43g of an organic ligand, 20g of a supporting solvent, 19g of an organic solvent and 18g of water.
The above-mentioned zinc-copper bimetallic MOF catalyzed MgH 2 The preparation method of the hydrogen storage material comprises the following steps:
s1, uniformly mixing a supporting solvent, an organic solvent and water to obtain a mixture solvent;
s2, sequentially adding copper salt, zinc salt and organic ligand into the mixture solvent, stirring and reacting for 2 hours at room temperature, and performing centrifugal separation to obtain a solid substance;
s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF;
s4, mixing the dried zinc-copper bimetallic MOF with commercial MgH 2 Mixing and ball milling to obtain the magnesium-based composite hydrogen storage material catalyzed by MOF.
Example 2
The zinc-copper bimetallic MOF catalyzed MgH of the invention 2 The hydrogen storage material comprises the following raw materials: 14g of a copper salt, 12g of a zinc salt, 30g of an organic ligand, 16g of a supporting solvent, 17g of an organic solvent and 13g of water.
The above-described zinc-copper bimetallic MOF catalyzed MgH 2 The preparation method of the hydrogen storage material comprises the following steps:
s1, uniformly mixing a supporting solvent, an organic solvent and water to obtain a mixture solvent;
s2, sequentially adding copper salt, zinc salt and organic ligand into the mixture solvent, stirring and reacting for 4 hours at room temperature, and performing centrifugal separation to obtain a solid substance;
s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF;
s4, mixing the dried zinc-copper bimetallic MOF with commercial MgH 2 Mixing and ball milling to obtain the MOF catalyzed magnesium-based composite hydrogen storage material.
Example 3
The zinc-copper bimetallic MOF catalyzed MgH of the invention 2 Hydrogen storage materialThe method comprises the following raw materials: 29g of a copper salt, 27g of a zinc salt, 60g of an organic ligand, 31g of a supporting solvent, 32g of an organic solvent and 28g of water.
The above-described zinc-copper bimetallic MOF catalyzed MgH 2 The preparation method of the hydrogen storage material comprises the following steps:
s1, uniformly mixing a supporting solvent, an organic solvent and water to obtain a mixture solvent;
s2, sequentially adding copper salt, zinc salt and organic ligand into the mixture solvent, stirring and reacting for 5 hours at room temperature, and performing centrifugal separation to obtain a solid substance;
s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF;
s4, mixing the dried zinc-copper bimetallic MOF with commercial MgH 2 Mixing and ball milling to obtain the magnesium-based composite hydrogen storage material catalyzed by MOF.
Example 4
The improvement is based on the embodiment 2:
further, the copper salt is one of copper nitrate hydrate, copper sulfate hydrate or copper chloride hydrate;
the zinc salt is one of zinc nitrate dihydrate, zinc acetate dihydrate, zinc sulfate hydrate or zinc chloride hydrate;
the organic ligand is one of benzimidazole, trimesic acid, 1,3,5-tri (4-carboxyl phenyl) benzene and 2-methylimidazole;
the supporting solvent is one of ammonia water solution and dimethylformamide;
the organic solvent is one of methanol, ethanol, dichloromethane or acetone.
Example 5
The improvement is based on the embodiment 4:
the copper salt, the zinc salt, the organic ligand, the supporting solvent and the organic solvent are respectively copper nitrate hydrate, zinc nitrate dihydrate, trimesic acid, dimethylformamide and ethanol.
Example 6
The improvement is based on the embodiment 2:
further, the mixture ratio of the copper salt, the zinc salt, the organic ligand, the supporting solvent, the organic solvent and the water is as follows: 1.
Example 7
The improvement is carried out on the basis of the embodiment 6:
the mixture ratio of copper salt, zinc salt, organic ligand, supporting solvent, organic solvent and water is as follows: 1:1:0.80:1.8:0.9:1.
Example 8
The improvement is based on the embodiment 6:
the mixture ratio of copper salt, zinc salt, organic ligand, supporting solvent, organic solvent and water is as follows: 1:0.83:2:1:100.
Example 9
The improvement is based on the embodiment 6:
the mixture ratio of copper salt, zinc salt, organic ligand, supporting solvent, organic solvent and water is as follows: 1:1:0.85:2.2:1.1:1.
Example 10
The improvement is based on the embodiment 2:
further, the conditions of the centrifugal separation were: the centrifugal speed is 7000-10000 rpm, and the centrifugal time is controlled to be 8-15 min.
Example 11
The improvement is based on the embodiment 10:
the conditions of the centrifugal separation were: the centrifugal speed is 7000rpm, and the centrifugal time length is controlled at 8min.
Example 12
The improvement is based on the embodiment 10:
the conditions of the centrifugal separation were: the centrifugal speed is 8000rpm, and the centrifugal time is controlled at 10min.
Example 13
The improvement is based on the embodiment 10:
the conditions of the centrifugal separation were: the centrifugal speed is 10000rpm, and the centrifugal time is controlled at 15min.
Example 14
The improvement is based on the embodiment 2:
further, the washing and drying conditions are as follows: washing the obtained solid with ethanol and deionized water for 3 times respectively, and finally carrying out vacuum drying through an oven, wherein the drying temperature is 180-250 ℃, and the drying time is 5-8 h.
Example 15
The improvement is based on the example 14:
the washing and drying conditions are as follows: washing the obtained solid with ethanol and deionized water for 3 times, and vacuum drying in oven at 180 deg.C for 5 hr.
Example 16
The improvement is based on the embodiment 14:
the washing and drying conditions are as follows: washing the obtained solid with ethanol and deionized water for 3 times respectively, and finally performing vacuum drying in an oven at the drying temperature of 200 ℃ for 6h.
Example 17
The improvement is based on the example 14:
the washing and drying conditions are as follows: washing the obtained solid with ethanol and deionized water for 3 times respectively, and finally performing vacuum drying in an oven at the drying temperature of 250 ℃ for 8h.
Example 18
The improvement is based on the embodiment 2:
further, mgH 2 The mass ratio of the zinc-copper bimetallic MOF to the zinc-copper bimetallic MOF is 7-12.
Example 19
The improvement is based on the example 18:
MgH 2 the mass ratio of the zinc-copper bimetallic MOF to the zinc-copper bimetallic MOF is 7:1.
Example 20
The improvement is based on the example 18:
MgH 2 the mass ratio of the metal MOF to the zinc-copper double metal is 10.
Example 21
The improvement is based on the example 18:
MgH 2 the mass ratio of the zinc-copper bimetallic MOF to the zinc-copper bimetallic MOF is 12.
Example 22
The improvement is based on the embodiment 2:
furthermore, the ball milling time is 4.5 to 5.5 hours, and the ball milling rotating speed is controlled to be 400 to 500rpm.
Example 23
The improvement is based on the embodiment 22:
the ball milling time is 4.5h, and the ball milling rotating speed is controlled at 400rpm.
Example 24
The improvement is based on the embodiment 22:
the ball milling time is 5h, and the ball milling rotating speed is controlled at 450rpm.
Example 25
The improvement is based on the embodiment 22:
the ball milling time is 5.5h, and the ball milling rotating speed is controlled at 500rpm.
Example 26
The improvement is based on the embodiment 2:
further, zinc-copper bimetal MOF and MgH 2 The ball milling is carried out in a hydrogen atmosphere, the pressure of the hydrogen is 1.8-2.2 MPa, and the ball-to-material ratio is 40-60.
Example 27
The improvement is based on the embodiment 26:
zinc-copper bimetal MOF and MgH 2 The ball milling of (2) was carried out in a hydrogen atmosphere, and the pressure of hydrogen was 1.8MPa, the ball-to-feed ratio was 40.
Example 28
The improvement is based on the embodiment 26:
zinc-copper bimetal MOF and MgH 2 The ball milling of (2) is carried out in a hydrogen atmosphere, the pressure of the hydrogen is 2MPa, and the ball-to-material ratio is 50.
Example 29
The improvement is based on the embodiment 26:
zinc-copper bimetal MOF and MgH 2 The ball milling of (2) was carried out in a hydrogen atmosphere, and the pressure of hydrogen was 2.2MPa, the ball-to-feed ratio was 60.
Example 30
On the basis of example 8:
in a 250mL glass beaker, dimethylformamide, ethanol, and water were mixed in a volume of 1. Subsequently, 5g of trimesic acid (H3 BTC), 5g of Zn (NO 3) 2. 2.5H2O and 5g of Cu (NO 3) 2. 2.5H2O were dissolved in the solvent mixture with continuous stirring. The resulting solution was then transferred to a glass vial, sealed and placed in an oven heated at 85 ℃ for 20 hours. And washing the obtained solid precipitate with ethanol and deionized water for 3 times respectively, then placing the solid precipitate in an oven at 80 ℃ for vacuum drying to obtain the zinc-copper bimetallic MOF material, and sealing and storing the zinc-copper bimetallic MOF material for later use.
Respectively weighing 0.9gMgH 2 And 0.1g of the zinc-copper bimetallic MOF prepared above was placed in a ball mill, followed by addition of 50g of ball milling beads. Ball milling is carried out for 5h at the rotating speed of 450rpm under the hydrogen pressure of 2 MPa. Obtaining MgH catalyzed by zinc-copper bimetal MOF after ball milling 2 A hydrogen storage material. Testing of MgH catalyzed by Zinc-copper bimetallic MOF 2 PXRD of the hydrogen storage material is shown in FIG. 1.
MgH prepared in inventive example 30 2 The hydrogen storage material is compounded, and the hydrogen absorption dynamic behavior of the compound material is tested: under the condition that the initial hydrogen pressure is 2.5MPa, the dynamic behavior of hydrogen absorption in 3600s of the composite material after complete dehydrogenation is tested by adopting Sievert type PCT testing equipment at 300 ℃, and the result is shown in figure 2, and MgH catalyzed by bimetallic MOF 2 The hydrogen absorption amount of the hydrogen storage material is far larger than that of pure MgH 2 At 60s, the maximum hydrogen absorption can reach 4.5wt%, and pure MgH at this time 2 Only 0.7wt.%, bimetallic MOF catalyzed MgH 2 The hydrogen storage material has better hydrogen absorption reaction rate, can complete hydrogen absorption in 60s, and has shorter hydrogen absorption time than pure MgH 2 The material shows that the introduction of the bimetallic MOF can effectively improve MgH 2 Hydrogen sorption kinetics of the hydrogen storage material.
In the embodiment of the invention, different samples are studied on the hydrogen evolution performance by adopting a differential scanning calorimeter at different temperature rising speeds, the obtained data are fitted by using a Kissinger method, the fitting result is shown in figures 3 and 4, and MgH catalyzed by ZnCu bimetal MOF 2 The hydrogen storage material has lower hydrogen desorption activation energy, and shows that the introduction of the bimetallic MOF can improve MgH 2 Hydrogen storage materialAnd the hydrogen release temperature is reduced, and in addition, the invention also proves that the catalytic effect of the bimetallic site is superior to that of a single catalytic site.
Finally, the above embodiments are only for illustrating the technical solutions of the present invention and not for limiting, although the present invention has been described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions may be made to the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention, and all of them should be covered in the claims of the present invention.

Claims (12)

1. Zinc-copper bimetallic MOF catalyzed MgH 2 The hydrogen storage material is characterized by comprising the following components in parts by weight: 14 to 29 parts of copper salt, 12 to 27 parts of zinc salt, 30 to 60 parts of organic ligand, 16 to 31 parts of supporting solvent, 17 to 32 parts of organic solvent and 13 to 28 parts of water.
2. The zinc-copper bimetallic MOF catalyzed MgH of claim 1 2 The preparation method of the hydrogen storage material is characterized by comprising the following steps:
s1, uniformly mixing a supporting solvent, an organic solvent and water of the components to obtain a mixture solvent;
s2, sequentially adding copper salt, zinc salt and organic ligand of the components into the mixture solvent, stirring and reacting for 2-5 h at room temperature, and performing centrifugal separation to obtain a solid substance;
s3, washing and drying the obtained solid matter to obtain zinc-copper bimetallic MOF;
s4, mixing the dried zinc-copper bimetallic MOF with commercial MgH 2 Mixing and ball milling to obtain the magnesium-based composite hydrogen storage material catalyzed by MOF.
3. The method according to claim 2, wherein the copper salt is one of copper nitrate hydrate, copper sulfate hydrate, and copper chloride hydrate;
the zinc salt is one of zinc nitrate dihydrate, zinc acetate dihydrate, zinc sulfate hydrate and zinc chloride hydrate;
the organic ligand is one of benzimidazole, trimesic acid, 1,3,5-tri (4-carboxyl phenyl) benzene and 2-methylimidazole;
the supporting solvent is one of ammonia water solution and dimethylformamide;
the organic solvent is one of methanol, ethanol, dichloromethane and acetone.
4. The method according to claim 3, wherein the copper salt, the zinc salt, the organic ligand, the supporting solvent and the organic solvent are respectively copper nitrate hydrate, zinc nitrate dihydrate, trimesic acid, dimethylformamide and ethanol.
5. The method according to claim 2, wherein the copper salt, the zinc salt, the organic ligand, the supporting solvent, the organic solvent and the water are mixed in a ratio of: 1.
6. The method according to claim 2, wherein the conditions for the centrifugation in S2 are: the centrifugal speed is 7000-10000 rpm, and the centrifugal time is controlled to be 8-15 min.
7. The method according to claim 2, wherein the washing and drying conditions in S3 are as follows: washing the obtained solid with ethanol and deionized water for 3 times respectively, and finally carrying out vacuum drying through an oven, wherein the drying temperature is 180-250 ℃, and the drying time is 5-8 h.
8. The method of claim 2, wherein: mgH in S4 2 The mass ratio of the zinc-copper bimetallic MOF to the zinc-copper bimetallic MOF is 7-12.
9. The method of claim 2, wherein: the ball milling time in the S4 is 4.5-5.5 h, and the ball milling rotating speed is controlled at 400-500 rpm.
10. The method of claim 2, wherein: the zinc-copper bimetal MOF and MgH in S4 2 The ball milling is carried out in a hydrogen atmosphere, the pressure of the hydrogen is 1.8-2.2 MPa, and the ball-to-material ratio is 40-60.
11. Zinc-copper bimetallic MOF catalyzed MgH prepared by the preparation method of any one of claims 2 to 10 2 A hydrogen storage material.
12. Zinc-copper bimetallic MOF catalyzed MgH prepared by the preparation method of any one of claims 2 to 10 2 Use of a hydrogen storage material in a fuel cell.
CN202211053007.0A 2022-08-31 2022-08-31 MgH catalyzed by zinc-copper bimetallic MOF 2 Hydrogen storage material, preparation method and application thereof Active CN115367700B (en)

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