CN104993130A - Non-aqueous solution aluminum ion secondary battery and preparation method thereof - Google Patents
Non-aqueous solution aluminum ion secondary battery and preparation method thereof Download PDFInfo
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- 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
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
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- 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
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Abstract
Belonging to the technical field of batteries, the invention relates to a non-aqueous solution aluminum ion secondary battery and a preparation method thereof. The secondary battery can be widely applied in electronics, communication, electric vehicle and other fields. The aluminum ion battery provided by the invention contains a battery anode, a battery cathode, a diaphragm and an aluminum-containing non-aqueous solution electrolyte. Specifically, the cathode active material can be carbon, graphite, carbon nanotube, graphene, super carbon, WS2 and MoS2, V2O5, TiO2 and other materials having nano-layered, tubular, linear and other structures, and the anode is aluminum-containing metal or alloy. The non-aqueous solution aluminum ion secondary battery provided by the invention has the characteristics of high specific capacity, high coulomb efficiency, long service life and environmental protection, safety and reliability, stable cycle performance, and quick charging, etc.
Description
Technical field
The invention belongs to new green power cell art, be specifically related to a kind of non-aqueous solution aluminium ion secondary cell and preparation method thereof.
Background technology
In recent years, ambient pressure, greenhouse effect etc. that continuous minimizing and use thereof along with non-regeneration energy (as: oil, coal, natural gas) bring, develop and utilize clean reproducible energy to become the focus of current research.Wherein electric energy becomes the key factor of whole renewable and clean energy resource forest ecosystem because it is in the core stage of various energy resources conversion.But, the efficiency utilization of these electric energy be realized, then relate to the storage problem of electric energy.The charge and discharge of secondary cell is current solution electrical power storage is the most also most promising mode.Current, secondary cell is still based on lithium ion battery, and lithium ion battery is widely used on the electronic product such as mobile phone, computer and other portable type electronic products because of its higher energy density and high voltage platform.But by the impact of global lithium reserves, the production cost of lithium ion battery is difficult to reduce always.Meanwhile, the widely used carbon negative pole material of current business makes it in use there is potential safety hazard.By the impact of above various factors, the scientific research personnel of countries in the world takes up to research and develop novel rechargeable battery, and wherein aluminium ion battery is because the low cost of aluminium element abundant in the earth's crust and exploitation has made it slowly the enter into sight line of people.Relative to traditional lithium ion, aluminium ion can shift three electronics, and therefore its specific capacity has very large potentiality to be exploited.In addition aluminium ion radius is also less than lithium ion radius, is conducive to the deintercalation of ion on electrode material, thus is conducive to the structure of holding electrode material in theory, improves circulating battery stability, extends battery.In fact, recent result of study shows: aluminium ion secondary cell still can remain good stable circulation under long high rate charge-discharge, demonstrates aluminium ion battery feasibility in actual applications thus.But current aluminium ion battery manufacturing process is not mature enough, the selection for material does not reach market tolerance interval yet.Therefore, optimize the positive pole of aluminium ion battery, negative material and electrolyte composition, reduction battery cost is enhanced productivity, and the commercial applications realizing aluminium ion battery is of great significance.
Summary of the invention
The invention provides a kind of novel secondary battery replacing lithium ion battery, and multivalent ion rechargeable battery and preparation method thereof.Achieve the height ratio capacity of non-aqueous solution aluminium ion secondary cell, high coulombic efficiency and long-lived environmental protection, safe and reliable, stable cycle performance, the features such as quickly-chargeable.
For achieving the above object, the invention provides following technical scheme:
The rechargeable aluminium ion battery that the present invention proposes, its operation principle and existing lithium ion battery, sodium-ion battery operation principle have similarity.
A kind of non-aqueous solution aluminium ion secondary cell, it is characterized in that comprising anode, negative pole, barrier film, containing aluminium non-aqueous electrolyte and electrolytic cell device.Wherein anode is by positive active material and conductive agent, binding agent, mixing or separately and plus plate current-collecting body be combined as anode; Negative pole is aluminiferous metals or alloy; Be made up of by a certain percentage aluminum halide and ionic liquid containing aluminium non-aqueous electrolyte.
Described positive active material be mass fraction be greater than 90% carbon, graphite, carbon nano-tube, Graphene, super carbon and WS
2, MoS
2, V
2o
5, TiO
2etc. possessing nano lamellar, tubulose, the isostructural material of wire.
Described conductive agent is carbon nano-tube, super carbon, amorphous carbon, silver slurry etc.; Described binding agent is Kynoar, polytetrafluoroethylene or silver slurry etc.
Described anode select conductive agent, binding agent to mix by positive active material according to self-conductive, caking property or separately and plus plate current-collecting body adopt be coated with, bond, the mode such as spreading is combined into.
Described plus plate current-collecting body is made by including but are not limited to molybdenum, titanium, tantalum, lead, vitreous carbon, nickel foam or gold and platinum group metal etc.
Described negative pole aluminiferous metals or alloy are metallic aluminium or the alloy that formed such as metallic aluminium and copper, iron, nickel, lead, bismuth, tin, silver that purity is greater than 90%.
Described barrier film is for having ion permeability and not reacting with both positive and negative polarity, and there is the material of stable chemical property, good mechanical performance and electrochemical stability, specifically include but are not limited to microporous polyolefin film diaphragm material, glass fiber material or ceramic material.
The described aluminum halide contained in aluminium non-aqueous electrolyte is the one in aluminum fluoride, aluminium chloride, aluminium bromide and silver iodide.
The described cation containing aluminium non-aqueous electrolyte intermediate ion liquid includes but are not limited to imidazoles drone ion, pyridinium ion, pyrroles's drone ion, piperidines drone ion, morpholine drone ion, quaternary ammonium salt ion, quaternary alkylphosphonium salt ion and tertiary sulfosalt ion; Anion includes but are not limited to F-, Cl-, Br-, I-, PF
6-, CN-, SCN-, [N (CF
3sO
2)]-, [N (CN)
2]-plasma.
The described ratio containing aluminum halide in aluminium non-aqueous electrolyte and ionic liquid is 0.4:1-2.4:1.
The electrolytic cell device that described electrolytic cell device is the vial of band polytetrafluoroethylene lid, the material of soft bag that aluminum plastic film is made and polytetrafluoroethylene or other resistance to the present invention electrolyte corrosion used is made.
Described non-aqueous solution aluminium ion secondary cell, comprises following preparation process:
1) mass fraction is greater than the carbon of 90%, graphite, carbon nano-tube, Graphene, super carbon and WS
2, MoS
2, V
2o
5, TiO
2select the mixing of conductive agent, binding agent Deng positive active material according to self-conductive, caking property or be coated with alone, bond or positive pole is made in spreading on plus plate current-collecting body, separating battery positive and negative electrode with barrier film simultaneously;
2) using thickness be 0.1-2mm metal aluminum or aluminum alloy cleaning after as negative pole;
3) preparation is containing aluminium non-aqueous electrolyte;
4) positive pole, negative pole and containing after aluminium non-aqueous electrolyte is got out, assembled battery in anaerobic water-less environment;
5), after battery pack installs, add containing aluminium non-aqueous electrolyte, positive pole, negative pole and barrier film are all immersed containing in aluminium non-aqueous electrolyte.
In above-mentioned aluminium ion battery preparation method step (1), described carbon, graphite, carbon nano-tube, Graphene, super carbon do not need to mix with conductive agent, and WS
2, MoS
2, V
2o
5, TiO
2the conductive agent that the positive electrode active materials poor etc. conductivity need be 1%-20% with mass fraction mixes.
In above-mentioned aluminium ion battery preparation method step (1), described carbon, graphite, carbon nano-tube, Graphene, super carbon and WS
2, MoS
2, V
2o
5, TiO
2all can select to mix with the binding agent of mass fraction at 0%-20% Deng positive active material.
In above-mentioned aluminium ion battery preparation method step (2), first metal aluminum or aluminum alloy is cut into sheet, then it is level and smooth with sand papering, clean again, the method of wherein cleaning is, soak and ultrasonic vibration with absolute ethyl alcohol or acetone, then in 60-120 DEG C of baking oven, carry out drying.
In above-mentioned aluminium ion battery preparation method step (3), described in, must prepare in anaerobic water-less environment containing aluminium non-aqueous electrolyte, and leave standstill within more than 12 hours, could use.
The present invention uses carbon, graphite, carbon nano-tube, WS
2and MoS
2etc. possessing the material of nanometer laminated structure as positive pole, albronze, as negative pole, constitutes a kind of non-aqueous solution aluminium ion secondary cell.Due to the present invention align, negative material, barrier film and electrolyte thereof etc. study by experiment and have carried out meticulous selection, and in conjunction with tight preparation method, so the present invention has following characteristics: belong to a kind of novel multivalent ion, i.e. aluminium ion battery system, which also promotes the development of energy storage device; Because aluminium element is at the rich reserves of the earth's crust, low price, greatly reduces the preparation cost of battery; The use of aluminium alloy negative electrode effectively can reduce the generation of negative electrode dendritic crystal in long-time charge and discharge process, thus avoids battery short circuit, reduces potential safety hazard; Carbon, graphite, carbon nano-tube, Graphene, super carbon and WS
2, MoS
2, V
2o
5, TiO
2etc. possess nano lamellar, tubulose, the isostructural material of wire chemical stability and Heat stability is good, specific area is large, surface activity is high, have a wide range of applications in electrochemical energy storage; Barrier film has good insulation property, has good transparent performance to electrolyte ion, has good chemical stability and electrochemical stability; Aluminium ion electrolyte, conductance is high, Heat stability is good, with positive and negative pole material, barrier film and binding agent etc. in battery, chemical reaction does not occur; Aluminium ion battery of the present invention can be widely used in the field such as electronic industry, communication industry, also can be applicable to the electrokinetic cell of electric automobile.
Accompanying drawing explanation
Fig. 1 is the structural representation of battery of the present invention;
Fig. 2 is the cycle performance test curve of aluminium ion battery prepared by the present invention.
In Fig. 1,1 is electrolytic cell device; 2 is battery cathode; 3 is barrier film; 4 is electrolysis of solutions matter; 5 is anode; 6 is plus plate current-collecting body.
Embodiment
The present invention will be described in more detail by specific embodiment below, but protection scope of the present invention is not limited to these embodiments.
Embodiment 1:
Positive active material is carbon nano-tube (CNT), and binding agent is polytetrafluoroethylene (PTFE).Both 9:1 in mass ratio, and spray alcohol and make both mix, finally obtain colloid substance.Above-mentioned colloid substance is evenly coated on plus plate current-collecting body molybdenum sheet, and is placed in lasting dry 24 hours of 120 DEG C of baking ovens, obtain the present invention's anode.Get the Cu that 0.25mm is thick
11al
9alloy, dry after ultrasonic cleaning a few hours in absolute ethyl alcohol, obtain battery cathode.Barrier film is glass fibre, and electrolyte is by AlI
3be mixedly configured into containing aluminium non-aqueous electrolyte with the ratio of 1-butyl-3-methylimidazolium chloride salt 1.5:1 in molar ratio.Electrolytic cell is the soft bag of laminated aluminum film.Being assembled in the glove box being full of argon gas of whole battery is carried out, and in glove box, the content of oxygen and water is less than 0.1ppm.The battery assembled will leave standstill 24 hours, to ensure that active material infiltrates well at electrolyte.
Embodiment 2:
Positive active material is WS
2, by its with conductive agent Super-P, polyfluortetraethylene of binding element (PTFE) in mass ratio 7.5:1.5:1 mix, and be placed in a certain amount of alcohol and disperse, within ultrasonic 60 minutes, make three's Homogeneous phase mixing.Mixture is placed in 60 DEG C of baking ovens and is dried to glue, be evenly coated in by gluey active material on plus plate current-collecting body molybdenum sheet, gained positive pole dry 24 hours in 120 DEG C of baking ovens obtain the present invention's positive pole.Negative pole is that ultrasonic cleaning a few hours thickness is the metallic aluminium of 0.20mm in alcohol.Barrier film is glass fibre, and electrolyte is AlCl
3mix with the ratio of 1-propyl group-3-methylimidazolium chloride salt 1.3:1 be in molar ratio made into containing aluminium non-aqueous electrolyte.Electrolytic cell device is that vial coordinates polytetrafluoroethylene lid to make.Whole battery be assembled in oxygen, water content is less than in the glove box of 0.1ppm.The battery assembled will leave standstill more than 24 hours, to ensure the good contact of positive active material and electrolyte.
Claims (10)
1. a non-aqueous solution aluminium ion secondary cell, is characterized in that, described secondary cell comprises anode and battery cathode; Described anode comprises the positive active material and plus plate current-collecting body with nanostructure, and described positive active material is fixed on described plus plate current-collecting body.
2. a kind of non-aqueous solution aluminium ion secondary cell according to claim 1, is characterized in that, described positive active material is carbon, graphite, carbon nano-tube, Graphene, super carbon, the WS that mass fraction is greater than 90%
2, MoS
2, V
2o
5or TiO
2etc. the material possessing nano lamellar, tubulose or linear structure.
3. a kind of non-aqueous solution aluminium ion secondary cell according to claim 1, it is characterized in that, described anode also comprises conductive agent and binding agent, described positive active material conductive agent and binding agent mixing.
4. a kind of non-aqueous solution aluminium ion secondary cell according to claim 3, it is characterized in that, described secondary cell also comprises barrier film, containing aluminium non-aqueous electrolyte and electrolytic cell device, described electrolytic cell device has an accommodation space, described accommodation space is filled described containing aluminium non-aqueous electrolyte, described anode, battery cathode and barrier film are placed in described containing aluminium non-aqueous electrolyte, and described barrier film is placed between described anode and battery cathode.
5. a kind of non-aqueous solution aluminium ion secondary cell according to claim 4, is characterized in that, described conductive agent is carbon nano-tube, super carbon, amorphous carbon, silver slurry;
Described binding agent is Kynoar, polytetrafluoroethylene or silver slurry;
Described plus plate current-collecting body is made up of molybdenum, titanium, tantalum, lead, vitreous carbon, nickel foam, gold or platinum group metal;
Described electrolytic cell device is made up of the resistance to aluminium plastic material corroded containing aluminium non-aqueous electrolyte, is specially the vial of band polytetrafluoroethylene lid, soft bag, polytetrafluoroethylene or other resistance to electrolytic cell device made containing the material of aluminium non-aqueous electrolyte corrosion that aluminum plastic film is made;
Described battery cathode is metallic aluminium or the alloy that formed of metallic aluminium and copper, iron, nickel, lead, bismuth, tin, silver that mass fraction is greater than 90%
Described barrier film is microporous polyolefin film diaphragm material, glass fiber material or ceramic material.
6. a kind of non-aqueous solution aluminium ion secondary cell according to claim 4, is characterized in that, the described aluminum halide contained in aluminium non-aqueous electrolyte is the one in aluminum fluoride, aluminium chloride, aluminium bromide and silver iodide.
7. a kind of non-aqueous solution aluminium ion secondary cell according to claim 6, it is characterized in that, the described cation containing aluminium non-aqueous electrolyte intermediate ion liquid comprises imidazoles drone ion, pyridinium ion, pyrroles's drone ion, piperidines drone ion, morpholine drone ion, quaternary ammonium salt ion, quaternary alkylphosphonium salt ion and tertiary sulfosalt ion; Anion comprises F-, Cl-, Br-, I-, PF
6-, CN-, SCN-, [N (CF
3sO
2)]-, [N (CN)
2]-ion.
8. a kind of non-aqueous solution aluminium ion secondary cell according to claim 7, is characterized in that, the described ratio containing aluminum halide in aluminium non-aqueous electrolyte and ionic liquid is 0.4:1-2.4:1.
9. a preparation method for non-aqueous solution aluminium ion secondary cell, for the preparation of the non-aqueous solution aluminium ion secondary cell one of the claims 4-8 Suo Shu, is characterized in that, comprise the following steps:
1) by positive active material or be fixed on described plus plate current-collecting body with the positive active material that conductive agent, binding agent mix; Fixed form is for adopting coating, bonding or spreading; Separate battery positive and negative electrode with barrier film simultaneously;
Described positive active material is carbon, graphite, carbon nano-tube, Graphene, super carbon, the WS that mass fraction is greater than 90%
2, MoS
2, V
2o
5or TiO
2possesses the material of nano lamellar, tubulose, linear structure;
2) using thickness be 0.1-2mm metal aluminum or aluminum alloy cleaning after as negative pole;
3) preparation is containing aluminium non-aqueous electrolyte;
4) anode, battery cathode and containing after aluminium non-aqueous electrolyte is got out, assembled battery in anaerobic water-less environment;
5), after battery pack installs, add containing aluminium non-aqueous electrolyte, anode, negative pole and barrier film are all immersed containing in aluminium non-aqueous electrolyte.
10. the preparation method of a kind of non-aqueous solution aluminium ion secondary cell according to claim 9, is characterized in that, in described step (1), carbon, graphite, carbon nano-tube, Graphene, super carbon do not need to mix with conductive agent, described WS
2, MoS
2, V
2o
5, TiO
2the conductive agent that the poor positive electrode active materials of conductivity need be 1%-20% with mass fraction mixes;
In described step (1), carbon, graphite, carbon nano-tube, Graphene, super carbon and WS
2, MoS
2, V
2o
5, TiO
2the binding agent that positive active material can be all 0%-20% with mass fraction mixes;
Described step (2) is: first metal aluminum or aluminum alloy is cut into sheet, then it is level and smooth with sand papering, then clean, the method for wherein cleaning is, soak and ultrasonic vibration with absolute ethyl alcohol or acetone, then in 60-120 DEG C of baking oven, carry out drying;
Step (3) is: prepare in anaerobic water-less environment containing aluminium non-aqueous electrolyte, and leaves standstill more than 12 hours.
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