CN105529462A - High-performance aluminium ion battery and preparation method - Google Patents
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Abstract
The invention discloses a high-performance aluminium ion battery and a preparation method. The battery comprises a positive electrode, a negative electrode, an electrolyte and a diaphragm for connecting the positive electrode and the negative electrode, wherein the positive electrode adopts a graphene-nickel composite material, wherein the nickel adopts nano-scale nickel granules embedded in the graphene; the diameter of the nickel granules is 0.5-10 [mu]m; the negative electrode adopts an aluminum manganese alloy, wherein the mass of the Mn accounts for 3-8% of the total mass of the aluminum manganese alloy; and the electrolyte adopts a mixture consisting of Al3+, Cl- and [EMIm], wherein the molar ratio of [EMIm] to Al3+ is greater than 3:2 and less than 4:1. The high-performance aluminium ion battery is relatively high in thermal stability, so that the safety problem existing in the current lithium ion battery can be solved, and the problem of explosion as the lithium ion secondary battery can be avoided; in addition, the battery prepared by the invention is better in performance than that of the reported aluminium ion secondary battery; and the charge-discharge platform of the battery can reach more than 3.5V, the cycling life can reach more than 5,000 times, and the energy density of the battery can reach more than 90Wh/Kg.
Description
Technical field
The present invention relates to high-performance aluminum ion battery and preparation method, belong to ion battery field.
Background technology
Current, a large amount of in the instrument such as notebook computer, mobile phone what use is all the lithium rechargeable battery of liquid electrolyte.But, because liquid electrolyte needs to be packaged in the metal-back of sealing, when some improper use, such as, when battery works in high temperature environments, outside heat is delivered to inside battery by metal shell, or inside battery heat release when discharging current is larger, inside battery or outside are understood overheated and inner pressure of battery are increased considerably, thus battery explosion is made due to liquid electrolyte thermally labile, therefore the lithium rechargeable battery of liquid electrolyte is used to there is potential safety hazard, limit further developing of liquid electrolyte lithium rechargeable battery, therefore the key that lithium ion battery security is research and development lithium rechargeable battery is improved.
Chinese patent CN103915611A discloses a kind of water system aluminium ion battery anode material and preparation method thereof, and this material is made up of nano titania leaf, and the chemical composition of nano titania leaf is TiO
1.976(NH)
0.024, average length is 50nm, and width is 10nm, and specific area is 314.2m
2/ g.Cycle-index can be brought up to 200 times by battery prepared by this invention, but its charging/discharging voltage is still lower, at below 2V, well below lithium rechargeable battery commercial at present.
Chinese patent CN101937994A provides graphene/aluminum composite cathode material of a kind of lithium ion battery and preparation method thereof, and described negative material is 1: 0.1 ~ 100 to form by Graphene and aluminium in mass ratio, and capacity reaches 600 ~ 1200mAh/g.The battery invented is under the current density of 1-500mA/mg, and slaking is carried out in discharge and recharge 1-100 circulation, obtains silicon/carbon/graphite in lithium ion batteries alkene/aluminum honeycomb material after slaking.But the discharge platform of this battery is at below 1V, far below lithium rechargeable battery commercial at present.
Chinese patent CN104241596A proposes a kind of rechargeable aluminium ion battery and preparation method thereof, and its positive pole adopts the material with carbon element of graphite-structure, and negative pole is rafifinal, and electrolyte is the mixture of anhydrous Aluminum chloride and 3-methylimidazole compounds.This invention adopts aluminium ion as conductive ion, avoids use lithium ion, has also evaded the conductivity issues because lithium ion causes thus.But the discharge platform of the battery of this invention is at below 2.4V, more much lower than the 4.2V of lithium ion battery, and its cycle-index is low.
The secondary aluminium cell that CN104183824A discloses a kind of secondary aluminium cell positive electrode and is made up of this positive pole.Described secondary aluminium cell comprises positive pole, containing aluminum honeycomb and nonaqueous electrolytic solution.Positive electrode is the composite material of Graphene/quinones, and wherein quinones is any one in quinone and corresponding derivative, and negative pole is metal aluminum or aluminum alloy, and electrolyte is that non-water is containing aluminium electrolyte.This battery adopts aluminium ion conduction, but its charging/discharging voltage is no more than 2V, and the capacity attenuation after 50 times that circulates is serious.
Summary of the invention
Goal of the invention: in order to overcome the deficiencies in the prior art, the invention provides a kind of high-performance aluminum ion battery and preparation method, can overcome the safety issue of current lithium ion battery, can not produce the explosion issues of lithium rechargeable battery.
Technical scheme: for achieving the above object, a kind of high-performance aluminum ion battery of the present invention, comprise the barrier film of the described positive pole of positive pole, negative pole, electrolyte and connection and negative pole, the composite material of described just very graphene-nickel, wherein nickel is that nano-scale particle is embedded in Graphene, and the diameter of nickel particle is between 0.5 micron to 10 microns; Described negative pole is alumal, and wherein the quality of Mn accounts for the 3-8% of alumal gross mass; Described electrolyte is for including Al
3+, Cl
-, [EMIm]
+the mixture formed, wherein [EMIm]
+with Al
3+mol ratio is greater than 3:2, is less than 4:1.
As preferably, the thickness of described Graphene is 50-2000 micron, and nickel thickness is 0.5-5 millimeter, the quality of nickel be composite material total amount 1-20%.
As preferably, the mass content sum total of other impurity elements in described alumal beyond manganese, aluminium is less than 0.1%, and alumal thickness is 0.2-2 millimeter.
As preferably, the thickness of described barrier film is 10-50 micron.
A preparation method for high-performance aluminum ion battery described above, comprises the following steps:
(1) graphite powder is added be equipped with in the container of the concentrated sulfuric acid, container is placed in ice bath, stir, the potassium permanganate powder added again, the mass ratio of graphite powder and potassium permanganate is 1:1.5-1:2, temperature less than 20 DEG C is kept to stir, by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then rate of addition be less than 5 ml/min in solution, add deionized water and concentration is the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, diameter is added between the nickel powder of 0.5 micron to 10 microns, the quality of nickel powder is less than 1/5 of graphite powder, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then hydrazine hydrate 5-10 milliliter is dripped and uniform stirring, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is replaced washing 4 times with deionized water, methyl alcohol, ethanol respectively, last fully dry under 60 DEG C of conditions, the product obtained is exactly graphene-nickel compound foil, as positive pole;
(3) by [EMIm] Cl and AlCl
3mix by a certain percentage, obtain electrolyte, wherein [EMIm]
+with Al
3+mol ratio is greater than 3:2, is less than 4:1;
(4) arrange according to the order of graphene-nickel compound foil, barrier film, alumal, wherein graphene-nickel is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, just obtaining high-performance aluminum ion battery.
Beneficial effect: high-performance aluminum ion battery of the present invention, there is higher thermal stability, can overcome the safety issue of current lithium ion battery, the explosion issues of lithium rechargeable battery can not be produced, and the battery prepared of the present invention is than the superior performance of the aluminium ion secondary cell reported.The charge and discharge platform of this battery can reach more than 3.5V, and cycle life can reach more than 5000 times, and the energy density of battery can reach more than 90Wh/Kg.
Embodiment
(1) 5 grams of graphite powders are added in the container that 100 milliliters of concentrated sulfuric acids are housed, container is placed in ice bath, stir 30 minutes, this chronothermometer is shown as 0 DEG C, slowly add 9 grams of potassium permanganate powder, stir, and guarantee that the temperature of reaction system in this process is below 20 DEG C, then by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then in solution, 100 ml deionized water are added slowly and 10 ml concns are the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, add the nickel powder 1 gram of diameter 0.9 micron, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then the hydrazine hydrate dripped 5 milliliters, uniform stirring during dropping, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is used deionized water respectively, methyl alcohol, ethanol replaces washing 4 times, finally pour in the mould of 5cm*2cm*5cm, fully dry under 60 DEG C of conditions, obtain the graphene-nickel thin slice of 5cm*2cm*0.093cm size, as the positive pole of battery,
(3) electrolyte is prepared: by [EMIm] Cl and AlCl
3mix in the ratio of 4:1;
(4) prepare PP/PE/PP barrier film, thickness is 50 microns;
(5) negative plate is prepared: its material is alumal, and wherein the mass content of manganese is 3%, and thickness is 0.4 millimeter;
(6) order of above material according to graphene-nickel thin slice, PE barrier film, alumal arranged, wherein Graphene is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, obtaining aluminium ion secondary cell;
(7) battery testing: adopt Land electrochemical test system, tests the charge and discharge platform of this battery is 3.5V, and circulate after 8000 times, its capacitance loss 6%, the energy density of battery is 102Wh/Kg.
Embodiment 2
(1) 5 grams of graphite powders are added in the container that 100 milliliters of concentrated sulfuric acids are housed, container is placed in ice bath, stir 30 minutes, this chronothermometer is shown as 0 DEG C, slowly add 9 grams of potassium permanganate powder, stir, and guarantee that the temperature of reaction system in this process is below 20 DEG C, then by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then in solution, 100 ml deionized water are added slowly and 10 ml concns are the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, diameter is added between the nickel powder 0.1 gram of 0.5 micron, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then the hydrazine hydrate dripped 8 milliliters, uniform stirring during dropping, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is used deionized water respectively, methyl alcohol, ethanol replaces washing 4 times, finally pour in the mould of 5cm*2cm*5cm, fully dry under 60 DEG C of conditions, obtain the graphene-nickel thin slice of 5cm*2cm*0.005cm size, as the positive pole of battery,
(3) electrolyte is prepared: by [EMIm] Cl and AlCl
3mix in the ratio of 2:1;
(4) prepare PE barrier film, thickness is 38 microns;
(5) negative plate is prepared: its material is alumal, and wherein the mass content of manganese is 5.3%, and thickness is 2 millimeters;
(6) order of above material according to graphene-nickel thin slice, PE barrier film, alumal arranged, wherein Graphene is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, obtaining aluminium ion secondary cell;
(7) battery testing: adopt Land electrochemical test system, tests the charge and discharge platform of this battery is 3.8V, and circulate after 10000 times, its capacitance loss 9%, the energy density of battery reaches 105Wh/Kg.
Embodiment 3
(1) 5 grams of graphite powders are added in the container that 100 milliliters of concentrated sulfuric acids are housed, container is placed in ice bath, stir 30 minutes, this chronothermometer is shown as 0 DEG C, slowly add 9 grams of potassium permanganate powder, stir, and guarantee that the temperature of reaction system in this process is below 20 DEG C, then by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then in solution, 100 ml deionized water are added slowly and 10 ml concns are the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, diameter is added between the nickel powder 0.8 gram of 5 microns, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then the hydrazine hydrate dripped 5 milliliters, uniform stirring during dropping, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is used deionized water respectively, methyl alcohol, ethanol replaces washing 4 times, finally pour in the mould of 5cm*2cm*5cm, fully dry under 60 DEG C of conditions, obtain the graphene platelet of 5cm*2cm*0.035cm size, as the positive pole of battery,
(3) electrolyte is prepared: by [EMIm] Cl and AlCl
3mix in the ratio of 3:1;
(4) prepare PP/PE/PP barrier film, thickness is 20 microns;
(5) negative plate is prepared: its material is alumal, and wherein the mass content of manganese is 6%, and thickness is 0.2 millimeter;
(6) order of above material according to graphene-nickel thin slice, PE barrier film, alumal arranged, wherein graphene-nickel thin slice is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, obtaining aluminium ion secondary cell;
(7) battery testing: adopt Land electrochemical test system, tests the charge and discharge platform of this battery is 3.9V, and circulate after 8000 times, its capacitance loss 6%, the energy density of battery reaches 108Wh/Kg.
Embodiment 4
(1) 5 grams of graphite powders are added in the container that 100 milliliters of concentrated sulfuric acids are housed, container is placed in ice bath, stir 30 minutes, this chronothermometer is shown as 0 DEG C, slowly add 10 grams of potassium permanganate powder, stir, and guarantee that the temperature of reaction system in this process is below 20 DEG C, then by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then in solution, 100 ml deionized water are added slowly and 10 ml concns are the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow,
(2) in above-mentioned solution, add the nickel powder 0.1 gram of diameter 10 microns, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then the hydrazine hydrate dripped 10 milliliters, uniform stirring during dropping, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is used deionized water respectively, methyl alcohol, ethanol replaces washing 4 times, finally pour in the mould of 5cm*2cm*5cm, fully dry under 60 DEG C of conditions, obtain the graphene-nickel thin slice of 5cm*2cm*0.20cm size, as the positive pole of battery,
(3) electrolyte is prepared: by [EMIm] Cl and AlCl
3mix in the ratio of 3:2;
(4) prepare PE barrier film, thickness is 18 microns;
(5) negative plate is prepared: its material is alumal, and wherein the mass content of manganese is 5%, and thickness is 0.5 millimeter;
(6) order of above material according to graphene-nickel thin slice, PE barrier film, alumal arranged, wherein Graphene is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, obtaining aluminium ion secondary cell;
(7) battery testing: adopt Land electrochemical test system, tests the charge and discharge platform of this battery is 3.6V, and circulate after 8000 times, its capacitance loss 8%, the energy density of battery reaches 101Wh/Kg.
Embodiment 5
(1) 5 grams of graphite powders are added in the container that 100 milliliters of concentrated sulfuric acids are housed, container is placed in ice bath, stir 30 minutes, this chronothermometer is shown as 0 DEG C, slowly add 6 grams of potassium permanganate powder, stir, and guarantee that the temperature of reaction system in this process is below 20 DEG C, then by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then in solution, 100 ml deionized water are added slowly and 10 ml concns are the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, diameter is added between the nickel powder 0.3 gram of 3 microns, vibrating dispersion in ultrasonic disperse instrument, obtain the hydrazine hydrate 5 milliliters that then stable dispersion liquid drips, uniform stirring during dropping, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is used deionized water respectively, methyl alcohol, ethanol replaces washing 4 times, finally pour in the mould of 5cm*2cm*5cm, fully dry under 60 DEG C of conditions, obtain the graphene-nickel thin slice of 5cm*2cm*0.086cm size, as the positive pole of battery,
(3) electrolyte is prepared: by [EMIm] Cl and AlCl
3mix in the ratio of 7:2;
(4) prepare PP barrier film, thickness is 10 microns;
(5) negative plate is prepared: its material is alumal, and wherein the mass content of manganese is 4.5%, and thickness is 0.2 millimeter;
(6) order of above material according to graphene-nickel thin slice, PE barrier film, alumal arranged, wherein Graphene is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, obtaining aluminium ion secondary cell;
(7) battery testing: adopt Land electrochemical test system, tests the charge and discharge platform of this battery is 3.8V, and circulate after 8000 times, its capacitance loss 7%, the energy density of battery reaches 102Wh/Kg;
The above is only the preferred embodiment of the present invention; be noted that for those skilled in the art; under the premise without departing from the principles of the invention, can also make some improvements and modifications, these improvements and modifications also should be considered as protection scope of the present invention.
Claims (5)
1. a high-performance aluminum ion battery, it is characterized in that: the barrier film comprising the described positive pole of positive pole, negative pole, electrolyte and connection and negative pole, the composite material of described just very graphene-nickel, wherein nickel is that nano-scale particle is embedded in Graphene, and the diameter of nickel particle is between 0.5 micron to 10 microns; Described negative pole is alumal, and wherein the quality of Mn accounts for the 3-8% of alumal gross mass; Described electrolyte is for including Al
3+, Cl
-, [EMIm]
+the mixture formed, wherein [EMIm]
+with Al
3+mol ratio is greater than 3:2, is less than 4:1.
2. high-performance aluminum ion battery according to claim 1, is characterized in that: the thickness of described Graphene is 50-2000 micron, and nickel thickness is 0.5-5 millimeter, the quality of nickel be composite material total amount 1-20%.
3. high-performance aluminum ion battery according to claim 2, is characterized in that: the mass content sum total of other impurity elements in described alumal beyond manganese, aluminium is less than 0.1%, and alumal thickness is 0.2-2 millimeter.
4. high-performance aluminum ion battery according to claim 3, is characterized in that: the thickness of described barrier film is 10-50 micron.
5. a preparation method for high-performance aluminum ion battery according to claim 4, is characterized in that, comprise the following steps:
(1) graphite powder is added be equipped with in the container of the concentrated sulfuric acid, container is placed in ice bath, stir, the potassium permanganate powder added again, the mass ratio of graphite powder and potassium permanganate is 1:1.5-1:2, temperature less than 20 DEG C is kept to stir, by the solution warms after stirring to 35 DEG C of Keep agitation 30 minutes, then rate of addition be less than 5 ml/min in solution, add deionized water and concentration is the hydrogen peroxide of 30%, and mixture is warmed up to 98 DEG C of Keep agitation 15 minutes, until mixture color becomes glassy yellow;
(2) in above-mentioned solution, diameter is added between the nickel powder of 0.5 micron to 10 microns, the quality of nickel powder is less than 1/5 of graphite powder, vibrating dispersion in ultrasonic disperse instrument, obtain stable dispersion liquid, then hydrazine hydrate 5-10 milliliter is dripped and uniform stirring, and this solution is put into after oil bath is heated to 100 DEG C, isothermal reaction 30 minutes, then filter with pellicle, the product obtained is replaced washing 4 times with deionized water, methyl alcohol, ethanol respectively, last fully dry under 60 DEG C of conditions, the product obtained is exactly graphene-nickel compound foil, as positive pole;
(3) by [EMIm] Cl and AlCl
3mix by a certain percentage, obtain electrolyte, wherein [EMIm]
+with Al
3+mol ratio is greater than 3:2, is less than 4:1;
(4) arrange according to the order of graphene-nickel compound foil, barrier film, alumal, wherein graphene-nickel is positive pole, and alumal is negative pole, injects electrolyte and encapsulates, just obtaining high-performance aluminum ion battery.
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JP2001023650A (en) * | 1999-07-12 | 2001-01-26 | Tomoji Tanaka | Aluminum battery |
CN104241650A (en) * | 2013-06-14 | 2014-12-24 | 中国科学院上海硅酸盐研究所 | Composite positive electrode material based on 3D graphene and preparation method thereof |
CN104078714A (en) * | 2014-07-08 | 2014-10-01 | 南京中储新能源有限公司 | Graphene secondary aluminum battery and preparation method for anode composite material of graphene secondary aluminum battery |
CN104993130A (en) * | 2015-05-25 | 2015-10-21 | 石嘴山市天和创润新材料科技有限公司 | Non-aqueous solution aluminum ion secondary battery and preparation method thereof |
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