CN109301245B - Aluminum-graphite double-ion battery and preparation method thereof - Google Patents
Aluminum-graphite double-ion battery and preparation method thereof Download PDFInfo
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Abstract
An aluminum-graphite double-ion battery and a preparation method thereof are disclosed, wherein a positive electrode is obtained by respectively carrying out plasma treatment on graphite powder or graphite paper, pure aluminum or aluminum alloy foamed aluminum prepared by a foaming process is used as a negative electrode, and an electrolyte is prepared and assembled to obtain the aluminum-graphite double-ion battery; according to the invention, the distance between graphite layers is enlarged by regulating and controlling the treatment conditions so that anions can be rapidly embedded and removed, and the volume change of aluminum in the charging and discharging process is reduced through the three-dimensional network structure of foamed aluminum, so that the cycling stability of the battery is greatly improved, the working voltage (3.8-4.6V) of the battery can be obviously improved, the defects of poor cycling stability, low capacity and the like of the conventional aluminum-graphite double-ion battery are overcome, and the quality, the volume and the manufacturing cost of the battery are greatly reduced, so that the energy density of the whole battery is comprehensively improved.
Description
Technical Field
The invention relates to a technology in the field of secondary batteries, in particular to an aluminum-graphite double-ion battery which takes a graphite material treated by plasma as a positive electrode and foamed aluminum as a negative electrode material.
Background
The existing lithium ion battery has low capacity and cannot meet the requirements of high energy density, cleanness and low cost in the future due to the use of transition elements which are harmful to a certain extent. There are now new, environmentally friendly, and high energy density secondary battery technologies that are increasingly emerging, including potassium ion batteries, sodium ion batteries, magnesium ion batteries, and aluminum ion batteries. One of the materials uses graphite material as anode material and aluminum as cathode material, PF is used during charging6 -Into the graphite layers, lithium ions enterThe lithium aluminum alloy is formed when the lithium aluminum alloy enters the surface of the metal aluminum, lithium in the negative electrode is extracted and enters the electrolyte when the lithium aluminum alloy is discharged, and PF6Detachment from the graphite layers into the electrolyte. The novel reaction mechanism not only obviously improves the working voltage (3.8-4.6V) of the battery, but also greatly reduces the quality, the volume and the manufacturing cost of the battery, thereby comprehensively improving the energy density of the full battery.
However, the drawbacks of the prior art described above include: (1) the metal aluminum foil is easy to corrode in the charging and discharging processes, so that the cycle life of the battery is greatly shortened; (2) graphite interlayer spacing (0.336nm) less than PF6The diameter of (0.436nm) of the aluminum-graphite bi-ion battery is limited in anion intercalation capacity, so that the current aluminum-graphite bi-ion battery has the problems of poor cycle stability and low capacity.
Disclosure of Invention
The invention mainly aims to overcome the defects of the conventional aluminum-graphite double-ion technology and provides an aluminum-graphite double-ion battery and a preparation method thereof.
The invention is realized by the following technical scheme:
the invention relates to a preparation method of an aluminum-graphite double-ion battery, which is characterized in that a graphite material is respectively subjected to plasma treatment to obtain a positive electrode, foamed aluminum is used as a negative electrode, and an electrolyte is prepared and assembled to obtain the aluminum-graphite double-ion battery.
The graphite material is graphite powder or graphite paper, preferably, the graphite powder, a binder solution and a conductive agent are mixed to obtain positive electrode slurry, and the positive electrode slurry is coated, dried, rolled, cut and die-cut to obtain the positive electrode slurry, or the graphite powder is subjected to acid treatment, thermal expansion, desulfurization process and rolling to prepare the corresponding graphite paper.
The binder solution comprises: polyvinylidene fluoride solution, sodium carboxymethyl cellulose, LA133N2, AB glue, etc.
The conductive agent comprises: conductive carbon black, KS-6, carbon nanotubes, or graphene.
The plasma treatment is as follows: placing the graphite material into a plasma generating device, introducing oxygen, nitrogen or argon, controlling the flow rate at 0.1-0.5L/min, controlling the power at 200-400W, maintaining the pressure at 50-200Pa, and treating for 30-120 mins.
The foamed aluminum is pure aluminum or aluminum alloy foam prepared by a foaming process.
The thickness of the foamed aluminum is 1-5mm, and the volume density is 0.4-1.0g/cm3The porosity is 60-90%, the purity is 99.0-99.99%, and the foamed aluminum is degreased and alkaline-etched to remove surface oil stain and metal oxide.
The electrolyte comprises dimethyl carbonate, diethyl carbonate, dimethyl sulfone or nitrile solvent serving as a solvent, lithium hexafluorophosphate or lithium perchlorate serving as an electrolyte, vinylene carbonate, ethylene sulfite, propylene sulfite, 1, 3-dioxolane or acetonitrile serving as an additive and a diaphragm.
The additive is preferably used in an amount of 0.1 to 5 wt% based on the total mass of the electrolyte.
The diaphragm is a porous polypropylene film, a porous composite polymer film, glass fiber paper or a porous ceramic diaphragm.
The assembling is as follows: and (3) taking the graphite material subjected to plasma treatment as a positive electrode material, taking the cut foamed aluminum as a negative electrode sheet, laminating the positive electrode sheet and the cut foamed aluminum into a battery cell through a diaphragm, placing the battery cell into an aluminum-plastic film bag, sequentially performing side top sealing, injecting electrolyte, and packaging to obtain a soft package or button battery.
The invention relates to an aluminum-graphite double-ion battery prepared by the method, which adopts plasma generated by ionized oxygen, nitrogen or argon to act on the surface of a graphite material as a positive electrode material, so that the distance between graphite layers is enlarged to enable anions to be rapidly embedded and removed; the foamed aluminum with a three-dimensional network structure is used as a negative electrode material, so that the volume change of aluminum in the charging and discharging process is reduced, and the cycling stability of the battery is greatly improved.
Technical effects
Compared with the prior art, the method has the advantages that the graphite layer spacing is greatly increased by processing the graphite by the plasma, and the speed and the quantity of anions inserted into the graphite layers are increased; on the other hand, the foamed aluminum with the three-dimensional network structure is used as a negative electrode material, so that more lithium can be accommodated, the volume change of the aluminum negative electrode in the charging and discharging process can be greatly relieved, and the capacity and the cycle life of the battery are improved.
Drawings
Fig. 1 is a schematic diagram of a capacity cycle curve of the aluminum-graphite secondary battery button cell of example 1;
fig. 2 is a schematic diagram of a capacity cycle curve of the soft pack battery of the aluminum-graphite secondary battery of example 2;
fig. 3 is a schematic diagram of a capacity cycle curve of the soft pack battery of the aluminum-graphite secondary battery of example 3.
Detailed Description
Example 1
The embodiment comprises the following steps:
argon plasma treatment of graphite powder as anode: 10g of graphite powder is taken, argon is introduced, the gas flow rate is controlled at 0.1L/min, the gas pressure is controlled at 50Pa, the plasma power is 200W, and the treatment time is 50 min.
Preparing an electrode anode: adding 7g of argon plasma-treated graphite powder, 2g of carbon black and 1g of polyvinylidene fluoride into 20mL of nitrogen methyl pyrrolidone solution, and fully grinding to obtain uniform slurry; the slurry was then uniformly coated on the aluminum foil surface and vacuum dried. And cutting the dried electrode slice into a wafer with the diameter of 14mm, and compacting the wafer to be used as the battery anode for standby.
Preparing a battery cathode: taking the thickness of 1mm, the porosity of 90 percent and the volume density: 0.5g/cm3The foamed aluminum is cut into circular sheets with the diameter of 16mm, washed by alkali solution and acetone, and dried to be used as a negative current collector for standby.
Fourthly, preparing electrolyte, namely preparing 4MLiPF in the glove box6The EMC solution is placed in a glove box and stirred for 24hrs by magnetic force, then vinylene carbonate with the mass fraction of 2 percent is added as an additive,fully and uniformly stirring the mixture to be used as electrolyte for standby.
Assembling the battery: and (3) in a glove box protected by inert gas, tightly stacking the prepared negative current collector, the diaphragm and the battery positive electrode in sequence, dropwise adding electrolyte to completely soak the diaphragm, and packaging the stacked part into a button battery shell to finish battery assembly.
The coulombic efficiency of the battery prepared by the embodiment is up to 97.2% through testing, and the discharge capacity is 138 mAh/g.
Example 2
The embodiment comprises the following steps:
oxygen plasma treatment of graphite paper as positive electrode: taking 0.5mm thick graphite paper, washing with ethanol at a size of 6cm by 6cm, drying in a vacuum drying oven, placing the dried graphite paper in a plasma generating device, introducing oxygen, controlling the gas flow rate at 0.3L/min, controlling the gas pressure at 90Pa, controlling the plasma power at 300W, and processing for 90 min.
Secondly, taking the thickness of 3mm, the porosity of 80 percent and the volume density: 0.7g/cm3Cutting the foamed aluminum into 6 cm-6 cm pole pieces, cleaning with an alkali solution and acetone, and airing to serve as a negative current collector for later use.
Thirdly, preparing electrolyte, namely 4M EMC solution of lithium perchlorate, and adding ethylene sulfite with the mass fraction of 2% as an additive.
Preparing a diaphragm: cutting the porous polypropylene film into circular sheets with the width of 6.5cm multiplied by 6.5cm, cleaning the circular sheets with acetone, and airing the circular sheets to be used as diaphragms for later use.
Assembling the soft package battery: punching an aluminum-plastic film into an aluminum-plastic film bag with the thickness of 6cm multiplied by 6cm, laminating a positive plate and a negative plate into a battery cell through a diaphragm, placing the battery cell in the aluminum-plastic film bag, sequentially performing side top sealing, injecting electrolyte, standing, sealing, forming, and grading to obtain a soft package battery;
the coulombic efficiency of the battery prepared by the embodiment is up to 97.8% through testing, the discharge capacity is 111mAh/g, and the cycle is 1000 circles.
Example 3
The embodiment comprises the following steps:
argon plasma treatment of a graphite electrode as a positive electrode: cutting 0.5 mm-thick graphite paper into 5cm × 5cm shapes, cleaning with ethanol, drying in a vacuum drying oven, placing the dried graphite paper in a plasma generator, introducing argon gas, controlling the gas flow rate at 0.5L/min, the gas pressure at 200Pa, the plasma power at 400W, and processing for 120 min.
Selecting the material with the thickness of 4mm, the porosity of 70 percent and the volume density: 0.8g/cm3Cutting the foamed aluminum into 5 cm-5 cm pole pieces, cleaning with an alkali solution and acetone, and airing to serve as a negative current collector for later use.
Preparing electrolyte, namely 4M ethyl methyl carbonate solution of lithium tetrafluoroborate, and adding a cyclobutyl sulfone additive with the mass fraction of 2%.
Assembling the soft package battery: punching an aluminum-plastic film into an aluminum-plastic film bag of 5cm multiplied by 5cm, laminating a positive plate and a negative plate into a battery cell through a diaphragm, placing the battery cell in the aluminum-plastic film bag, sequentially performing side top sealing, injecting electrolyte, standing, sealing, forming, and grading to obtain a soft package battery;
the coulombic efficiency of the battery prepared by the embodiment is tested to reach 94.5%, and the discharge capacity is 109 mAh/g.
The foregoing embodiments may be modified in many different ways by those skilled in the art without departing from the spirit and scope of the invention, which is defined by the appended claims and all changes that come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein.
Claims (2)
1. The preparation method of the aluminum-graphite double-ion battery is characterized by comprising the following steps of:
oxygen plasma treatment of graphite paper as positive electrode: taking 0.5mm thick graphite paper with the size of 6cm multiplied by 6cm, cleaning the graphite paper with ethanol, placing the graphite paper in a vacuum drying oven for drying treatment, placing the dried graphite paper in a plasma generating device, introducing oxygen, controlling the gas flow rate at 0.3L/min, controlling the gas pressure at 90Pa, controlling the plasma power at 300W, and treating for 90 min;
② taking the material with the thickness of 3mm, the porosity of 80 percent and the volume density of 0.7g/cm3Cutting the foamed aluminum into 6cm multiplied by 6cm pole pieces, cleaning with an alkali solution and acetone, and airing to serve as a negative current collector for later use;
preparing electrolyte: adding 2% by mass of ethylene sulfite into 4M of EMC solution of lithium perchlorate to serve as an additive;
preparing a diaphragm: cutting the porous polypropylene film into a wafer with the width of 6.5cm multiplied by 6.5cm, cleaning the wafer with acetone, and airing the wafer to be used as a diaphragm for later use;
assembling the soft package battery: punching the aluminum-plastic film into 6cm multiplied by 6cm aluminum-plastic film bags, laminating the positive plate and the negative plate into a battery cell through a diaphragm, placing the battery cell into the aluminum-plastic film bags, sequentially performing side top sealing, injecting electrolyte, standing, sealing, forming and grading to obtain the soft package battery.
2. The preparation method of the aluminum-graphite double-ion battery is characterized by comprising the following steps of:
argon plasma treatment of a graphite electrode as a positive electrode: cutting 0.5 mm-thick graphite paper into a shape of 5cm multiplied by 5cm, cleaning with ethanol, drying in a vacuum drying oven, placing the dried graphite paper in a plasma generating device, introducing argon gas, controlling the gas flow rate at 0.5L/min, the gas pressure at 200Pa, the plasma power at 400W, and the processing time at 120 min;
② taking the material with the thickness of 4mm, the porosity of 70 percent and the volume density of 0.8g/cm3Cutting the foamed aluminum into pole pieces of 5cm multiplied by 5cm, cleaning with an alkali solution and acetone, and airing to serve as a negative current collector for later use;
preparing electrolyte: adding a cyclobutyl sulfone additive with the mass fraction of 2% into a 4M ethyl methyl carbonate solution of lithium tetrafluoroborate;
assembling the soft package battery: punching the aluminum-plastic film into a 5cm multiplied by 5cm aluminum-plastic film bag, laminating the positive plate and the negative plate into a battery cell through a diaphragm, placing the battery cell in the aluminum-plastic film bag, sequentially performing side top sealing, injecting electrolyte, standing, sealing, forming, and grading to obtain the soft package battery.
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