CN106941188B - One kind can charge and discharge aluminium ion battery and its preparation process - Google Patents
One kind can charge and discharge aluminium ion battery and its preparation process Download PDFInfo
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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
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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- H—ELECTRICITY
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- H01M10/05—Accumulators with non-aqueous electrolyte
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- H—ELECTRICITY
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- 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
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- 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
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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
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Abstract
One kind can charge and discharge aluminium ion battery and its preparation process, be related to aluminium ion battery, just extremely Li3VO4C-base composte material, the carbon-based material include the mixture of any one of carbon nanotube, carbon nano-fiber, graphene, amorphous carbon or two kinds.Cathode is rafifinal or aluminium-containing alloy, and electrolyte is non-aqueous electrolyte containing aluminium ion.Provided aluminium ion battery has many advantages, such as that specific capacity height, good cycling stability, raw material are cheap and environmentally friendly, and first circle specific discharge capacity is up to 137mAhg‑1, which can be widely applied to the various fields such as telecommunications, electric car.
Description
Technical field
The present invention relates to aluminium ion batteries, can charge and discharge aluminium ion battery and its preparation process more particularly, to one kind.
Background technique
Lithium ion battery has always been considered as being one of most promising electrochemical energy storage system because its energy density it is high,
It has extended cycle life, work potential height.But recently as a wide range of promotion and application of lithium ion battery, lithium resource faces withered
It exhausts, price even more rises year by year.Secondly, its use common are machine electrolyte, inflammable and explosive, safety is poor.Furthermore volume
Specific energy density is low.And bauxite resource is abundant, every annual mining volume is more than 1000 times of lithium, cheap.And use ionic liquid
As electrolyte, ionic liquid steam forces down, without combustibility the advantages that the significant increase security performance of aluminium ion battery, then
Person, the energy density per unit volume metric density of aluminum honeycomb are significantly larger than lithium, and that there are also bendable folding endurances is strong, environmentally friendly etc. for additional aluminium ion battery
Advantage, therefore for following wearable device battery, easily collide dangerous inflammable and explosive automobile batteries, extensive intelligence
The fields such as power grid energy storage, aluminium ion battery have great application prospect and application value.
Currently, the research of aluminium ion battery is still in initial stage, positive electrode can select narrow range, in the aluminium having been reported that
In ion battery positive electrode, such as embedding off line manages profile strand foam graphite (Lin, M.C.et al.An ultrafast
Rechargeable aluminium-ion battery [J] .Nature, 2015), research uses pyrolytic graphite and three-dimensional foam
For graphite as aluminium ion cell positive material, cycle performance is although excellent, but its specific capacity is low, causes the energy density per unit volume of system
It is low.For another example transformation mechanism profile material FeS2(document: Mori, T.et al.Discharge/charge reaction
mechanisms of FeS2cathode material for aluminum rechargeable batteries at 55
DEG C .Journal of Power Sources, 2016), although its specific capacity is high, cycle performance is bad.Therefore, exploitation is high
Specific capacity, long circulation life aluminium ion cell positive material be particularly important.
But patent and document so far has not been reported about Li3VO4C-base composte material is as anode and uses this
The aluminium ion battery of kind anode.
Summary of the invention
The object of the present invention is to provide one kind can charge and discharge aluminium ion battery and its preparation process.
It is described can charge and discharge aluminium ion battery include anode, battery cathode, non-aqueous electrolyte containing aluminium ion, in electricity
Solve the diaphragm of the metal foil collector that electrochemicaUy inert is showed in liquid, the connection anode and cathode；The anode is
Li3VO4C-base composte material, battery cathode are metallic aluminium or its alloy.
The Li3VO4Carbon content can be 10%~30% by mass percentage in C-base composte material；The carbon-based material
It can be selected from least one of carbon nanotube, carbon nano-fiber, graphene, amorphous carbon etc.；
The Li3VO4C-base composte material the preparation method is as follows: prepare V2O5And Li2CO3Solution, by V2O5With
Li2CO3Solution mixes, addition carbon-based material, after magnetic agitation 4h, acquired solution is placed in spray dryer and is done by spraying
It is dry, gained powder is then calcined to 4~7h at 550 DEG C and obtains Li3VO4C-base composte material.
The negative electrode material is that metallic aluminium of the purity greater than 90% or metallic aluminium are formed with copper, silver, nickel, lead, tin, bismuth, iron
Alloy.
The non-aqueous electrolyte containing aluminium ion includes aluminum halide and ionic liquid, and the aluminum halide and ionic liquid rub
You are than being (1.1~2) ︰ 1；The anion of the ionic liquid includes Cl-, Br-, I-, PF6 -, BF6 -, CN-, SCN-, [N
(CF3SO2)2]-Or [N (CN)2]-Plasma；The cation of the ionic liquid includes imidazol ion, pyridinium ion, pyrroles
Ion, piperidines ion, morpholinium ion, quaternary ammonium salt ion, quaternary phosphonium salt ion or tertiary sulfosalt ion etc..
The inert metal paillon collector includes tantalum piece, niobium sheet, molybdenum sheet, titanium sheet, stainless steel substrates, gold and platinum group metal
Deng.
The diaphragm of the connection anode and cathode includes but is not limited to polyolefins, the optional autohemagglutination of polyolefins
One of ethylene and polypropylene, glass fiber filter paper, ceramic material etc..
It is described can charge and discharge aluminium ion battery preparation process the following steps are included:
1) by Li3VO4C-base composte material, conductive material, binder proportionally weigh uniform mixing respectively, and work is made
Property material paste is equably applied on inert metal collector, is dried in 60~100 DEG C of baking ovens, be made with a thickness of 0.5~
2mm sheet composite positive pole；
2) it by with a thickness of the metal aluminum or aluminum alloy of 0.1~1mm, is polished with fine sandpaper two-sided, after washes of absolute alcohol,
It dries to get negative electrode material is arrived；
3) by ionic liquid at 80~150 DEG C of vacuum oven dry 12h, subsequent aluminum halide and ionic liquid with mole
Than for (1.1~2) ︰ 1 are mixed in the glove box of ar gas environment, room temperature magnetic agitation 0.5h, that is, are configured to containing can freely move
The dynamic liquid of nonaqueous solution electrolysis containing aluminium ion；
4) finally by negative electrode material that the positive electrode step 2) that step 1) obtains obtains and step 3) obtain containing aluminium from
Sub- nonaqueous solution electrolysis liquid and diaphragm are completed in glove box, obtain aluminium ion soft-package battery or button cell, i.e.,
Li3VO4C-base composte material is the aluminium ion battery of anode；
5) after battery pack installs, charge-discharge test is carried out again after standing 12~20h.
The present invention uses a kind of Li3VO4C-base composte material is the aluminium ion battery of anode, electrochemical specific capacity is high,
Cycle performance is excellent, which can be widely applied to the various fields such as telecommunications, electric car.
Compared with prior art, the beneficial effects of the present invention are: using Li3VO4C-base composte material as positive electrode,
Rafifinal or aluminium-containing alloy as negative electrode material, constitute it is a kind of can charge and discharge aluminium ion battery.Since the present invention is to positive and negative
Pole material, diaphragm, collector and electrolyte etc. have carried out fine selection by experimental study, and combine above-mentioned be previously mentioned
Preparation method, so the present invention is it can be gathered that following features: proposing a kind of novel multivalent ion battery, i.e. aluminium ion cell body
System；Bauxite resource rich reserves, every annual mining volume is more than 1000 times of lithium, cheap, greatly reduces the preparation cost of battery；
Li3VO4C-base composte material is readily synthesized, low in cost, and environmentally friendly, therefore is had in electrochemical energy storage field and greatly answered
Use prospect；Ionic liquid as a kind of novel aluminium ion battery electrolyte, have electrochemical window mouth width, ionic conductivity it is high,
The advantages that without combustibility；Aluminium ion battery provided by the present invention have specific capacity height, good cycling stability, raw material cheaply and
The advantages that environmentally friendly, first circle specific discharge capacity are up to 137mAh g-1, after recycling 100cycle, specific discharge capacity is
47mAh g-1, cyclical stability with higher.Aluminium ion battery of the invention can be applied to multiple fields, as telecommunications,
Electric car etc..
Detailed description of the invention
Fig. 1 is the cyclic voltammetry curve of aluminium ion battery first lap prepared by the embodiment of the present invention 1.
Fig. 2 is aluminium ion battery first lap charge-discharge test curve prepared by the embodiment of the present invention 1.
Fig. 3 is 100 circle cycle performance test curves before aluminium ion battery prepared by the embodiment of the present invention 1.
Specific embodiment
The present invention will be described in more detail below by specific embodiment, but protection scope of the present invention is not limited
In these embodiments.
[embodiment 1]
The aluminium ion cell positive material of the present embodiment is made with the following method: preparing V2O5And Li2CO3Solution, massage
You are than being 3:1 by V2O5Solution and Li2CO3Solution mixes, addition 0.9g glucose, after room temperature magnetic agitation 4h, by acquired solution
It is placed in spray dryer and is spray-dried, gained powder is then calcined to 5h at 550 DEG C and obtains Li3VO4Amorphous carbon
Composite material.The material is mixed according to 7 ︰ of mass ratio, 2 ︰ 1 and ground with conductive agent acetylene black, binder polyvinylidene fluoride (PVDF)
Mill uniformly, is sized mixing with N-Methyl pyrrolidone (NMP), is stirred, and (thickness on sizeable stainless (steel) wire is coated on
0.01mm), it is dried overnight at 80 DEG C of vacuum drying oven, is fabricated to anode pole piece.High-purity aluminium flake is two-sided to be polished with fine sandpaper, uses second
Alcohol is dried after impregnating 1~2h, is cut into sizeable sheet as cathode.By anhydrous aluminum chloride and 1- ethyl -3- methyl-chlorine
Change imidazoles is that 1.3 ︰ 1 in the glove box of ar gas environment are configured to aluminium ion battery electrolyte in molar ratio.Using PE film as every
Film.Ready anode, cathode, diaphragm and electrolyte are finally assembled into Soft Roll aluminium ion battery in glove box.Battery dress
After good 16h, charge-discharge test is carried out between 0.05~0.95V.By Fig. 2 and Fig. 3 it is found that using Li3VO4C-base composte material
For the aluminium ion battery of anode, its first circle specific discharge capacity is up to 137mAh g-1, after recycling 100cycle, specific discharge capacity is
47mAh g-1.From cyclic voltammetry as can be seen that its process includes a pair of reversible redox peaks, Fig. 1 is seen.
[embodiment 2]
The aluminium ion cell positive material of the present embodiment is made with the following method: preparing V2O5And Li2CO3Solution, massage
You are than being 3 ︰ 1 by V2O5Solution and Li2CO3Solution mixing, is added the processed carbon nanotube (CNT) of 0.5g, and room temperature magnetic force stirs
After mixing 4h, acquired solution is placed in spray dryer and is spray-dried, then gained powder calcined into 5h at 550 DEG C and obtained
Obtain Li3VO4- CNT composite material.By the material and conductive agent acetylene black, binder polyvinylidene fluoride (PVDF) according to mass ratio
7 ︰, 2 ︰, 1 mixed grinding is uniform, is sized mixing, is stirred with N-Methyl pyrrolidone (NMP), is coated on sizeable stainless
On steel mesh (thickness 0.01mm), is dried overnight at 80 DEG C of vacuum drying oven, be fabricated to anode pole piece.High-purity aluminium flake is two-sided to use fine sand
Paper polishing, dries after impregnating 1~2h with ethyl alcohol, is cut into sizeable sheet as cathode.By anhydrous aluminum chloride and 1- second
Base -3- methyl-imidazolium chloride is that 1.3 ︰ 1 in the glove box of ar gas environment are configured to aluminium ion battery electrolyte in molar ratio.
Using PE film as diaphragm.Ready anode, cathode, diaphragm and electrolyte are finally assembled into Soft Roll aluminium ion in glove box
Battery.After battery installs 16h, charge-discharge test is carried out between 0.05~0.95V.
[embodiment 3]
The aluminium ion cell positive material of the present embodiment is made with the following method: preparing V2O5And Li2CO3Solution, massage
You are than being 3 ︰ 1 by V2O5Solution and Li2CO3Solution mixing, is added 0.9g glucose and the processed carbon nanotube of 0.5g, room
After warm magnetic agitation 4h, acquired solution is placed in spray dryer and is spray-dried, then by gained powder at 550 DEG C
It calcines 5h and obtains Li3VO4Amorphous carbon-CNT composite material.The material and conductive agent acetylene black, binder are gathered into inclined difluoro second
Alkene (PVDF) is uniform according to mass ratio 7 ︰, 2 ︰, 1 mixed grinding, is sized mixing, is stirred with N-Methyl pyrrolidone (NMP), applies
It is overlying on sizeable stainless (steel) wire (thickness 0.01mm), is dried overnight at 80 DEG C of vacuum drying oven, be fabricated to anode pole piece.
High-purity aluminium flake is two-sided to be polished with fine sandpaper, is dried after impregnating 1~2h with ethyl alcohol, is cut into sizeable sheet as cathode.
It is in molar ratio that 1.3 ︰ 1 are configured in the glove box of ar gas environment by anhydrous aluminum chloride and 1- ethyl -3- methyl-imidazolium chloride
Aluminium ion battery electrolyte.Using PE film as diaphragm.Finally ready anode, cathode, diaphragm and electrolyte in glove box
Inside it is assembled into Soft Roll aluminium ion battery.After battery installs 16h, charge-discharge test is carried out between 0.05~0.95V.
[embodiment 4]
The aluminium ion cell positive material of the present embodiment is made with the following method: preparing V2O5And Li2CO3Solution, massage
You are than being 3 ︰ 1 by V2O5Solution and Li2CO3Solution mixes, addition 0.5g graphene, after room temperature magnetic agitation 4h, by acquired solution
It is placed in spray dryer and is spray-dried, gained powder is then calcined to 5h at 550 DEG C and obtains Li3VO4Graphene is multiple
Condensation material.By the material and conductive agent acetylene black, binder polyvinylidene fluoride (PVDF) according to 7 ︰ of mass ratio, 2 ︰, 1 mixed grinding
Uniformly, it is sized mixing, is stirred with N-Methyl pyrrolidone (NMP), be coated on (thickness on sizeable stainless (steel) wire
0.01mm), it is dried overnight at 80 DEG C of vacuum drying oven, is fabricated to anode pole piece.High-purity aluminium flake is two-sided to be polished with fine sandpaper, uses second
Alcohol is dried after impregnating 1~2h, is cut into sizeable sheet as cathode.By anhydrous aluminum chloride and 1- ethyl -3- methyl-chlorine
Change imidazoles is that 1.3 ︰ 1 in the glove box of ar gas environment are configured to aluminium ion battery electrolyte in molar ratio.Using PE film as every
Film.Ready anode, cathode, diaphragm and electrolyte are finally assembled into Soft Roll aluminium ion battery in glove box.Battery dress
After good 16h, charge-discharge test is carried out between 0.05~0.95V.
[embodiment 5]
The aluminium ion cell positive material of the present embodiment is made with the following method: preparing V2O5And Li2CO3Solution, massage
You are than being 3 ︰ 1 by V2O5Solution and Li2CO3Solution mixing, is added 0.5g carbon nano-fiber (CNF), after room temperature magnetic agitation 4h,
Acquired solution is placed in spray dryer and is spray-dried, gained powder is then calcined to 5h acquisition at 550 DEG C
Li3VO4- CNF composite material.By the material and conductive agent acetylene black, binder polyvinylidene fluoride (PVDF) according to 7 ︰ of mass ratio
2 ︰, 1 mixed grinding is uniform, is sized mixing, is stirred with N-Methyl pyrrolidone (NMP), is coated on sizeable stainless steel
(thickness 0.01mm) on the net dries overnight at 80 DEG C of vacuum drying oven, is fabricated to anode pole piece.High-purity aluminium flake is two-sided to use fine sandpaper
Polishing dries after impregnating 1~2h with ethyl alcohol, is cut into sizeable sheet as cathode.By anhydrous aluminum chloride and 1- ethyl-
3- methyl-imidazolium chloride is that 1.3 ︰ 1 in the glove box of ar gas environment are configured to aluminium ion battery electrolyte in molar ratio.By PE
Film is as diaphragm.Ready anode, cathode, diaphragm and electrolyte are finally assembled into Soft Roll aluminium ion electricity in glove box
Pond.After battery installs 16h, charge-discharge test is carried out between 0.05~0.95V.
Claims (9)
1. one kind can charge and discharge aluminium ion battery, it is characterised in that including anode, battery cathode, the electricity of non-water system containing aluminium ion
Solve the diaphragm of liquid, the metal foil collector for showing electrochemicaUy inert in the electrolytic solution, the connection anode and cathode；The electricity
Pond just extremely Li3VO4C-base composte material, battery cathode are metallic aluminium or its alloy；
The non-aqueous electrolyte containing aluminium ion includes aluminum halide and ionic liquid, the molar ratio of the aluminum halide and ionic liquid
For (1.1~2) ︰ 1；The anion of the ionic liquid includes Cl-, Br-, I-, PF6 -, BF6 -, CN-, SCN-, [N (CF3SO2)2]-
Or [N (CN)2]-Ion；The cation of the ionic liquid includes imidazol ion, pyridinium ion, pyrrolidinium ion, piperidines
Ion, morpholinium ion, quaternary ammonium salt ion, quaternary phosphonium salt ion or tertiary sulfosalt ion.
2. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the Li3VO4C-base composte material
Middle carbon content is 10%~30% by mass percentage.
3. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the Li3VO4C-base composte material
In carbon material be selected from least one of carbon nanotube, carbon nano-fiber, graphene, amorphous carbon.
4. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the Li3VO4C-base composte material
The preparation method is as follows: prepare V2O5And Li2CO3Solution, by V2O5And Li2CO3Solution mixing, is added carbon-based material, magnetic agitation
After 4h, acquired solution is placed in spray dryer and is spray-dried, gained powder is then calcined to 4~7h at 550 DEG C
Obtain Li3VO4C-base composte material.
5. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the negative electrode material is greater than for purity
The alloy that 90% metallic aluminium or metallic aluminium is formed with copper, silver, nickel, lead, tin, bismuth, iron.
6. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the inert metal paillon collector
Including tantalum piece, niobium sheet, molybdenum sheet, titanium sheet, stainless steel substrates, gold and platinum group metal.
7. one kind as described in claim 1 can charge and discharge aluminium ion battery, it is characterised in that the connection anode and cathode
Diaphragm include polyolefins.
8. one kind as claimed in claim 7 can charge and discharge aluminium ion battery, it is characterised in that the polyolefins be selected from polyethylene,
One of polypropylene, glass fiber filter paper, ceramic material.
9. as described in claim 1 can charge and discharge aluminium ion battery preparation process, it is characterised in that the following steps are included:
1) by Li3VO4C-base composte material, conductive material, binder proportionally weigh uniform mixing respectively, and active material is made
Slurry material is equably applied on inert metal collector, is dried, is made with a thickness of 0.5~2mm piece in 60~100 DEG C of baking ovens
Shape composite positive pole；
2) it by with a thickness of the metal aluminum or aluminum alloy of 0.1~1mm, is polished with fine sandpaper two-sided, after washes of absolute alcohol, is done
It is dry to get arrive negative electrode material；
3) by ionic liquid, dry 12h, subsequent aluminum halide and ionic liquid are at 80~150 DEG C of vacuum oven with molar ratio
(1.1~2) ︰ 1 are mixed in the glove box of ar gas environment, room temperature magnetic agitation 0.5h, that is, are configured to containing can move freely
The liquid of nonaqueous solution electrolysis containing aluminium ion；
4) finally negative electrode material that the positive electrode step 2) that step 1) obtains obtains is obtained with step 3) non-containing aluminium ion
Aqueous solution electrolysis liquid and diaphragm are completed in glove box, obtain aluminium ion soft-package battery or button cell, i.e.,
Li3VO4C-base composte material is the aluminium ion battery of anode；
5) after battery pack installs, charge-discharge test is carried out again after standing 12~20h.
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| CN109346670A (en) * | 2018-10-19 | 2019-02-15 | 深圳中科瑞能实业有限公司 | Energy storage device aluminum honeycomb, energy storage device and preparation method thereof |
| CN110010888B (en) * | 2019-04-01 | 2020-11-20 | 北京工业大学 | Chargeable and dischargeable water-series aluminum ion battery and preparation method thereof |
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