CN109037666A - Metal hydride graphene battery and graphene battery - Google Patents
Metal hydride graphene battery and graphene battery Download PDFInfo
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- CN109037666A CN109037666A CN201810871598.XA CN201810871598A CN109037666A CN 109037666 A CN109037666 A CN 109037666A CN 201810871598 A CN201810871598 A CN 201810871598A CN 109037666 A CN109037666 A CN 109037666A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/383—Hydrogen absorbing alloys
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
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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
- Y02E60/10—Energy storage using batteries
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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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The present invention relates to field of batteries, and in particular to a kind of metal hydride graphene battery and graphene battery.The just extremely Graphene electrodes made of flake graphite raw material of metal hydride graphene battery, the cathode of the metal hydride graphene battery is metal hydride, the electrolyte of the metal hydride graphene battery is alkaline solution, the diaphragm of the metal hydride graphene battery is polymer, the dosage of the metal hydride is 1-2 times of the Graphene electrodes quality, and the concentration of the alkaline solution is 3-8mol/L.Its, overcharging resisting over-discharge small with self discharge, discharging voltage balance, good mechanical property, long service life, cycle-index is up to thousands of or even up to ten thousand secondary, the wide advantage of use temperature range.
Description
Technical field
The present invention relates to field of batteries, and in particular to a kind of metal hydride graphene battery and graphene battery.
Background technique
Natural energy source constantly consumes at present, exhausted at last, and the cry for seeking new energy is higher and higher.Space industry and
Demand of the sophisticated weapon to high-performance secondary cell is very urgent.Metal nickel hydride (MH-Ni) battery has used nickel oxide
Electrode is anode, and for metal hydride as cathode, energy density is high;Can high current fast charging and discharging, and memory-less effect.Due to
High-voltage nickel-hydrogen battery needs high pressure hydrogen and hydrogen-storage tank, it is also necessary to noble metal catalyst, it is at high cost, and it is dangerous, it is not suitable as
Civil battery.
Nickel oxyhydroxide in metal nickel hydride (MH-Ni) battery, Charging state active material are NiOOH, and electric discharge state is living
Property substance be Ni (OH)2.Under the conditions of overcharge, anode meeting volume expansion causes electrode cracking, picking, influences battery capacity
And cycle life, or even failure.
In recent years, people start the materials such as active carbon, carbon nanotube, graphene and technical application to metal nickel hydride
In terms of the improvement of battery and nickel electrode, nickel carbon electrode and nickel carbon supercapacitor etc. are also developed in succession.
But current carbon material is to be added in anode to improve its electric conductivity in the form of conductive agent, can not fundamentally be solved
It is excellent cannot to give full play to the carbon material especially high-ratio surface of graphite alkenes material, highly conductive and high thermal conductivity performance for certainly problem
Gesture, this problem limit metal-hydrogen nickel battery and nickel carbon supercapacitor in the application in wider, broader field.
Summary of the invention
The purpose of the present invention is to provide a kind of metal hydride graphene battery, circulation longevity high with energy density
The advantages of ordering length, having a safety feature.
Another object of the present invention is to provide a kind of graphene battery, which can give full play to graphene
The characteristics of material, the advantages of capable of effectively playing metal hydride graphene battery.
The present invention solves its technical problem and adopts the following technical solutions to realize:
The present invention proposes a kind of metal hydride graphene battery, the just extremely sheet stone of metal hydride graphene battery
Graphene electrodes made of black raw material, the cathode of the metal hydride graphene battery are metal hydride, the metallic hydrogen
The electrolyte of compound graphene battery is alkaline solution, and the diaphragm of the metal hydride graphene battery is polymer, described
The dosage of metal hydride is 1-2 times of the Graphene electrodes quality, and the concentration of the alkaline solution is 3-8mol/L.
The present invention proposes a kind of graphene battery comprising above-mentioned metal hydride graphene battery.
The beneficial effect of metal hydride graphene battery and graphene battery of the present invention is: the embodiment of the present invention provides
Metal hydride graphene battery, graphene anode does not need conductive black, binder etc. in the battery, guarantees metal hydride
The stability of object graphene battery can be improved its Rechargeability.The battery has longer service life, cycle-index reachable
Thousands of or even up to ten thousand time, use temperature range is wide, can within the scope of -40 DEG C~+40 DEG C normal use.Guarantee the metallic hydrogen simultaneously
Compound graphene battery also has many advantages, such as small self discharge, overcharging resisting over-discharge, discharging voltage balance, good mechanical property.
Detailed description of the invention
It in order to more clearly explain the embodiment of the invention or the technical proposal in the existing technology, below will be to institute in embodiment
Attached drawing to be used is needed to be briefly described.
Fig. 1 is the graphene of embodiment 1 to Mg2The battery charging and discharging curve of Ni cathode at room temperature;
Fig. 2 is the graphene of embodiment 1 to Mg2Battery charging and discharging curve of the Ni cathode at -10 DEG C;
Fig. 3 is the graphene of embodiment 1 to Mg2Ni negative battery 3 times cyclic voltammetry curve, sweep speed 0.1V/
S;
Fig. 4 is the graphene of embodiment 1 to Mg2Ni negative battery pulse charge curve;
Fig. 5 is the graphene of embodiment 1 to Mg2Ni negative battery cyclic curve.
Specific embodiment
It in order to make the object, technical scheme and advantages of the embodiment of the invention clearer, below will be in the embodiment of the present invention
Technical solution be clearly and completely described.The person that is not specified actual conditions in embodiment, according to normal conditions or manufacturer builds
The condition of view carries out.Reagents or instruments used without specified manufacturer is the conventional production that can be obtained by commercially available purchase
Product.
In the description of the present invention, it should be noted that term " first ", " second " etc. are only used for distinguishing description, without
It can be interpreted as indication or suggestion relative importance.
The metal hydride graphene battery and graphene battery of the embodiment of the present invention are specifically described below.
A kind of metal hydride graphene battery provided in an embodiment of the present invention, the anode of metal hydride graphene battery
For Graphene electrodes made of flake graphite raw material, the cathode of metal hydride graphene battery is metal hydride, metallic hydrogen
The electrolyte of compound graphene battery is alkaline solution, and the diaphragm of the metal hydride graphene battery is polymer, metal
The dosage of hydride is 1-2 times of Graphene electrodes quality, and the concentration of alkaline solution is 3-8mol/L.And the metal hydride used
Object is hydrogen-storage alloy, in addition to using general formula that Mg also can be used other than the metal material of MH2Ni、LaNi5, the metals such as TiFe.
Further, alkaline solution is strong base solution, preferably potassium hydroxide or sodium hydroxide.The metal hydride graphite
Alkene battery enables to metal hydride graphene battery with longer using above-mentioned anode, cathode, diaphragm and aforementioned proportion
Service life, cycle-index up to thousands of or even up to ten thousand time, use temperature range is wide, can be within the scope of -40 DEG C~+40 DEG C just
It is often used.Simultaneously guarantee the metal hydride graphene battery also have small self discharge, overcharging resisting over-discharge, discharging voltage balance,
The advantages that good mechanical property.
Diaphragm is membrane for polymer made of nylon fiber, polypropylene fiber, vinylon fibre etc..
Further, the preparation of the Graphene electrodes is prepared by following methods:
The flake graphite material of electrophoresis impregnation is that graphite flake and metal electrode are formed two electrode loops, utilizes the electricity of electrophoresis
The method of chemical method and ultrasonic wave added obtains impregnation graphite flake after the reaction that is powered.Specifically, by graphite flake and platinized platinum electricity
Pole forms two electrode loops, immerses in conducting resinl, the method for selecting the electrochemical method and ultrasonic wave added of electrophoresis, and be powered reaction.
The voltage reacted that is powered is 1-4V, and the time is 0.5-5 hours.Energization dries 10-48 in the environment of 30-60 DEG C after reaction
Hour.
Further, conducting resinl is the adhesive with certain electric conductivity after a kind of solidification, and conducting resinl is generally by matrix
Material and conductive filler are constituted, and basis material usually links together conducting particles, form conductive network, and final realize is glued
The conductive connection of material.Basis material includes performed polymer, curing agent, catalyst, plasticizer, diluent and other auxiliary agents.And it leads
Electric filler is using silver, and high temperature is not oxidizable and relative low price.
Specifically, conducting resinl is epoxy resin, methylhexahydrophthalic anhydride and 1- (2- cyanogen second in the embodiment of the present invention
Base) -2-ethyl-4-methylimidazole using mass ratio be 1:0.6-0.9:0.015-0.019 mix as basis material, using nanometer
Argent grain is conductive filler.The amount of basis material is 30wt%, and the dosage of conductive filler is 0.2-0.8wt%.
Further, organic electrolyte solution used in forming circuit process includes organic solvent and electrolytic salt, excellent
Choosing, organic solvent includes organic compounds containing sulfur, linear carbonate, carboxylate or ether solvent, and the electrolytic salt includes
LiClO4And Et3NHC, it is further preferred that the organic compounds containing sulfur includes dimethyl sulfoxide, linear carbonate includes carbonic acid diformazan
Ester, diethyl carbonate or methyl ethyl carbonate.Above-mentioned solvent and expanded graphite have good wetability, form the high electricity of conductivity
Liquid is solved, and intercalation stripping can be cooperateed in graphite layers.
The activator of more potential steps is one or both of potassium nitrate, dodecyl sodium sulfate, phosphoric acid.
It is working electrode by the cured flake graphite material of obtained conducting resinl, mercury-mercurous sulfate electrode is reference electrode,
Platinum plate electrode is auxiliary electrode, forms three electrode loops.More potential step methods are selected, the working electrode after having reacted is graphene
Electrode.At this point, the voltage that more potential step methods use is 1.5-3V, time 5-30S, number is 1-20 times.
The flake graphite alkene material cured to conducting resinl is cleaned and is dried more potential step methods after reaction.Clearly
Washing is floating powder in order to remove electrode surface, while making the crystallization miniaturization of the active material in electrode, lattice defect and true
Real surface area increases, and then promotes its conductive effect.
Further, washing is benefit 5-10 times wash with distilled water, and drying is to dry 12-48 in the environment of 30-60 DEG C
Hour.
Using Graphene electrodes as anode, metal hydride is cathode, and using alkaline solution as electrolyte, assembling obtains metal
Hydride graphene battery.
The embodiment of the present invention also provides a kind of graphene battery comprising above-mentioned metal hydride graphene battery.
Feature and performance of the invention are described in further detail with reference to embodiments.
Embodiment 1
A kind of metal hydride graphene battery provided in this embodiment, the just extremely piece of metal hydride graphene battery
Graphene electrodes made of shape graphite raw material, the cathode of metal hydride graphene battery are metal hydride, metal hydride
The electrolyte of graphene battery is sodium hydroxide solution, and the dosage of metal hydride is 1 times of Graphene electrodes quality, hydroxide
The concentration of sodium solution is 3mol/L, and the diaphragm of metal hydride graphene battery is polymer, is to gather made of nylon fiber
Close object diaphragm.
Wherein, Graphene electrodes are that exfoliated graphite sheet and platinum plate electrode are formed two electrode loops, are immersed in conducting resinl,
The method for selecting the electrochemical method and ultrasonic wave added of electrophoresis obtains impregnation graphite electrode material after the reaction that is powered.Be powered reaction
Voltage be 1V, the time be 5 hours.Energization is dried 48 hours in the environment of 30 DEG C after reaction.Conducting resinl is asphalt mixtures modified by epoxy resin
Rouge, methylhexahydrophthalic anhydride and 1- (2- cyanoethyl) -2-ethyl-4-methylimidazole are 1:0.6:0.015 with mass ratio
Mixing is used as basis material, uses nano-Ag particles for conductive filler.The amount of basis material is 30wt%, the dosage of conductive filler
For 0.2wt%.Organic electrolyte solution includes dimethyl sulfoxide and Et3NHC, the activator of more potential steps are potassium nitrate.
It is working electrode by obtained impregnation graphite electrode, mercury-mercurous sulfate electrode is reference electrode, supplemented by platinum plate electrode
Electrode is helped, three electrode loops are formed.More potential step methods are selected, the working electrode after having reacted is Graphene electrodes.At this point, more
The voltage that potential step method uses is 1.5V, time 30S, and number is 20 times.
Graphene electrodes benefit is dried 12 hours after 5 times in the environment of 60 DEG C wash with distilled water.
Using Graphene electrodes as cathode, metal hydride is anode, and electrolyte is added and metallic hydrogen can be obtained in diaphragm
Compound graphene battery.
Embodiment 2-3
The metal hydride graphene electricity that the metal hydride graphene battery and embodiment 1 that embodiment 2-3 is provided provide
The basis in pond is consistent, and difference is that the ratio of each substance is different.And the preparation method of Graphene electrodes is essentially identical, area
It is not that operating condition changes.
Embodiment 2
The dosage of metal hydride is 1.5 times of Graphene electrodes quality in metal hydride graphene battery, and alkalinity is molten
Liquid is potassium hydroxide, and the concentration of potassium hydroxide solution is 5mol/L.The diaphragm of metal hydride graphene battery is polypropylene fiber
Manufactured membrane for polymer.
When preparing Graphene electrodes, the voltage for the reaction that is powered is 4V, time 0.5h, is powered after reaction at 60 DEG C
It is dried 10 hours under environment.Conducting resinl is epoxy resin, methylhexahydrophthalic anhydride and 1- (2- cyanoethyl) -2- ethyl -
4-methylimidazole is that 1:0.9:0.019 is mixed as basis material using mass ratio, uses nano-Ag particles for conductive filler.Matrix
The amount of material is 30wt%, and the dosage of conductive filler is 0.8wt%.Organic electrolyte solution includes diethyl carbonate, carbonic acid first
Ethyl ester and LiClO4, the activator of more potential steps is dodecyl sodium sulfate and phosphoric acid.
The voltage that more potential step methods use is 3V, time 5S, and number is 15 times.
Graphene electrodes benefit is dried 48 hours after 10 times in the environment of 30 DEG C wash with distilled water.
Embodiment 3
The dosage of metal hydride is 2 times of Graphene electrodes quality, sodium hydroxide in metal hydride graphene battery
The concentration of solution is 8mol/L.The diaphragm of metal hydride graphene battery is membrane for polymer made of vinylon fibre.
When preparing Graphene electrodes, the voltage for the reaction that is powered is 2V, time 3h, and be powered the ring at 41 DEG C after reaction
It is dried 30 hours under border.Conducting resinl is epoxy resin, methylhexahydrophthalic anhydride and 1- (2- cyanoethyl) -2- ethyl -4-
Methylimidazole is that 1:0.7:0.018 is mixed as basis material using mass ratio, uses nano-Ag particles for conductive filler.Matrix material
The amount of material is 30wt%, and the dosage of conductive filler is 0.5wt%.Organic electrolyte solution includes methyl ether, diethyl carbonate, carbonic acid
Methyl ethyl ester and LiClO4, the activator of more potential steps is dodecyl sodium sulfate.
The voltage that more potential step methods use is 2V, time 25S, and number is 10 times.
Graphene electrodes benefit is dried 30 hours after 8 times in the environment of 45 DEG C wash with distilled water.
Experimental example 1
Electrochemistry quality detection is carried out to the Graphene electrodes that embodiment 1 provides, the data for being directed to capacity are with whole
It is calculated on the basis of body battery quality, specific testing result is referring to Fig. 1-5.Wherein, Fig. 1 is the graphene pair of embodiment 1
Mg2The battery charging and discharging curve of Ni cathode at room temperature;Fig. 2 is the graphene of embodiment 1 to Mg2Electricity of the Ni cathode at -10 DEG C
Pond charging and discharging curve;Fig. 3 is the graphene of embodiment 1 to Mg2Ni negative battery 3 times cyclic voltammetry curve;Fig. 4 is embodiment
1 graphene is to Mg2Ni negative battery pulse charge curve;Fig. 5 is the graphene of embodiment 1 to Mg2Ni negative battery circulation is bent
Line.According to Fig. 1-5 it is found that the metal hydride graphene battery discharging voltage balance, automatic discharging of the present embodiment are small.
In conclusion metal hydride graphene battery provided in an embodiment of the present invention has longer service life, follows
For ring number up to thousands of or even up to ten thousand time, use temperature range is wide, can within the scope of -40 DEG C~+40 DEG C normal use.It protects simultaneously
Demonstrate,proving the metal hydride graphene battery also has small self discharge, overcharging resisting over-discharge, discharging voltage balance, good mechanical property etc. excellent
Point.
Embodiments described above is a part of the embodiment of the present invention, instead of all the embodiments.Reality of the invention
The detailed description for applying example is not intended to limit the range of claimed invention, but is merely representative of selected implementation of the invention
Example.Based on the embodiments of the present invention, obtained by those of ordinary skill in the art without making creative efforts
Every other embodiment, belongs to the present invention.
Claims (10)
1. a kind of metal hydride graphene battery, which is characterized in that the just extremely piece of the metal hydride graphene battery
Graphene electrodes made of shape graphite raw material, the cathode of the metal hydride graphene battery are metal hydride, the gold
The electrolyte for belonging to hydride graphene battery is alkaline solution, and the dosage of the metal hydride is the Graphene electrodes quality
1-2 times, the concentration of the alkaline solution is 3-8mol/L.
2. metal hydride graphene battery according to claim 1, which is characterized in that the Graphene electrodes are electricity consumptions
Swim impregnation graphite flake as working electrode, metal electrode be auxiliary electrode, mercury-mercurous sulfate electrode is that reference electrode is formed
After three electrode loops, the Graphene electrodes material that is obtained through excessive potential step method.
3. metal hydride graphene battery according to claim 2, which is characterized in that the electricity that more potential step methods use
Pressure is 1.5-3V, and time 5-30S, number is 1-20 times.
4. metal hydride graphene battery according to claim 2, which is characterized in that the graphite of the electrophoresis impregnation is thin
Piece is that graphite flake and metal electrode are formed two electrode loops, using the method for the electrochemical method and ultrasonic wave added of electrophoresis, is led to
Impregnation graphite material is obtained after electricity reaction.
5. metal hydride graphene battery according to claim 4, which is characterized in that the voltage for the reaction that is powered is 1-
4V, time are 0.5-5 hours.
6. metal hydride graphene battery according to claim 4, which is characterized in that be powered after reaction in 30-
Baking and curing 10-48 hours in the environment of 60 DEG C.
7. metal hydride graphene battery according to claim 2, which is characterized in that more potential step method reactions terminate
After cleaned and dried.
8. metal hydride graphene battery according to claim 6, which is characterized in that the mode of cleaning include alkali cleaning,
Pickling, organic solvent wash or wash in any one or more.
9. metal hydride graphene battery according to claim 8, which is characterized in that washing be benefit wash with distilled water
5-10 times, drying is dried 12-48 hours in the environment of 30-60 DEG C.
10. a kind of graphene battery, which is characterized in that including metal hydride graphite described in any one of claim 1-9
Alkene battery.
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CN110289390A (en) * | 2019-06-24 | 2019-09-27 | 盐城市新能源化学储能与动力电源研究中心 | A kind of 3D graphite alkylene carbon electrode, preparation method and full battery |
CN110299508A (en) * | 2019-06-24 | 2019-10-01 | 盐城市新能源化学储能与动力电源研究中心 | A kind of 3D graphite alkylene carbon anode full battery and preparation method thereof |
CN112447945A (en) * | 2019-09-04 | 2021-03-05 | 盐城市新能源化学储能与动力电源研究中心 | 3D graphene carbon-nickel-metal hydride battery and preparation method thereof |
CN112447944A (en) * | 2019-09-04 | 2021-03-05 | 盐城市新能源化学储能与动力电源研究中心 | 3D graphene based carbon-lead battery and preparation method thereof |
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CN112447945B (en) * | 2019-09-04 | 2022-06-28 | 盐城师范学院 | 3D graphene based carbon-nickel hydride battery and preparation method thereof |
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