CN104078705B - A kind of secondary aluminium cell and electrolyte thereof - Google Patents
A kind of secondary aluminium cell and electrolyte thereof Download PDFInfo
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- CN104078705B CN104078705B CN201410312674.5A CN201410312674A CN104078705B CN 104078705 B CN104078705 B CN 104078705B CN 201410312674 A CN201410312674 A CN 201410312674A CN 104078705 B CN104078705 B CN 104078705B
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- aluminium
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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
-
- 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
- H01M10/056—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
- H01M10/0566—Liquid materials
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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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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Abstract
The invention discloses a kind of secondary aluminium cell, comprise positive pole, negative pole, electrolyte.This positive electrode active materials selects elemental sulfur or organosulfur compound; This negative active core-shell material selects metal aluminum or aluminum alloy; This electrolyte uses the non-water be made up of anhydrous aluminium salt, ionic liquid, organic solvent containing aluminium electrolyte.
Description
Technical field
The invention belongs to electrochemistry and new energy field, relate to a kind of secondary aluminium cell, especially relate to non-water that a kind of use is made up of anhydrous aluminium salt, ionic liquid, the organic solvent secondary aluminium cell containing aluminium electrolyte.
Background technology
Along with the fast development of global economy, advancing by leaps and bounds of the aspect technology such as portable electric appts, electric automobile and space utilization, the demand of the mankind to the Green Chemistry power supply of high-energy safe is more and more urgent.Lithium battery is developed so far, and has become the chemical power source of portable electric appts most practicality, and has extended to electrokinetic cell and energy-storage battery field.But because the aspect such as chemical activity, energy density of elemental lithium self limits, bring insoluble safety issue and battery capacity problem to the large scale development of lithium battery, therefore the high-energy battery of research other new type of safe open become international community general faced by a difficult problem.
Compared with conventional electrode materials, the advantages such as element aluminum and sulphur all have that theoretical energy density is large, aboundresources, cheap, environmentally friendly, use safety.Metallic aluminium theoretical energy density, up to 2980mAh/g, is only second to lithium metal (3682mAh/g), and volume and capacity ratio is 8050mAh/cm
3, be about lithium (2040mAh/cm
3) 4 times, and chemical activity is relatively stable, is desirable negative material; Elementary sulfur also has larger theoretical energy density (1670mAh/g), is the maximum positive electrode of known energy density.Therefore, aluminium-sulfur battery be all from every side a kind of cheap, energy density is high, the ideal battery of use safety.
Licht equals a kind of of the exploitation nineties in 20th century can contain S high specific energy alkaline aqueous solution aluminium-sulfur battery (USPat:5431881,4828492,5648183) by the novel of repid discharge at normal temperatures.This battery take aluminium alloy as anode, to be dissolved in polysulfide in alkaline electrolyte for negative electrode.Because adopt aqueous solution electrolysis liquid, there is passivation effect, corrosion effect in aluminum cell, volume is large, flocculent deposit accessory substance is difficult, specific power is lower, voltage delay, self-discharge rate are comparatively large, work time the problems such as overheated.The aluminium-sulfur battery developed in reality only has the battery open circuit current potential of 1.3V and energy density (the investigationofanovelaqueousaluminum/sulfurbattery.Journ alofPowerSources of 110Wh/kg, 1993,3 (45): 311-323).
Aluminium is the metal that a kind of activity is very strong, and its reduction potential is more negative than hydrogen, is impossible electro-deposition go out aluminium in aluminum saline solution, and namely all use aluminum saline solutions are that electrolytical aluminum cell cannot charge reduction, can only be primary cells.Therefore, want to realize the chargeable of aluminum cell, what first need to solve is exactly the electro-deposition-stripping problem of aluminium in electrolyte.Electrolytical selection decides the working mechanism of secondary aluminium cell to a great extent, affects the specific energy of battery, cycle performance, rate charge-discharge performance, fail safe, storge quality and cost etc.Suitable electrolyte is selected to be the important prerequisite realizing secondary cell high-performance, long-life, fail safe and low cost.
Summary of the invention
(1) goal of the invention
The object of the present invention is to provide large, the chargeable secondary aluminium cell of a kind of capacity.
The object of the present invention is to provide a kind of non-water containing aluminium electrolyte, to realize the electrochemical deposition-stripping of aluminium.
Term " secondary aluminium cell " in the present invention comprises such as " aluminum secondary battery ", " secondary aluminium-sulfur battery ", " rechargeable aluminium battery ", " aluminium storage battery ", " aluminium energy-storage battery " and similar concept.
(2) technical scheme
To achieve these goals, the invention provides a kind of secondary aluminium cell scheme, comprising:
A () comprises the positive pole of electro-chemical activity sulphur-containing substance;
B () is containing the negative pole of aluminium active material;
C non-water that () is made up of anhydrous aluminium salt, ionic liquid and organic solvent is containing aluminium electrolyte.
Here is the preferred positive pole of electrochemical cell of the present invention, negative pole, electrolytical description.
Positive pole
The positive pole of battery of the present invention comprises positive active material, conductive agent, binding agent and collector containing electro-chemical activity sulphur-containing substance.Wherein, term " electro-chemical activity sulphur-containing substance " refers to the positive active material comprising element sulphur here, and wherein, electro-chemical activity relates to fracture or the formation of sulphur-sulphur covalent bond.
Electro-chemical activity sulphur-containing substance described in scheme is elemental sulfur or organosulfur compound.Elemental sulfur comprises sublimed sulfur and high purity sulphur; Organosulfur compound includes but not limited to Polyacetylene sulfide, carbyne polysulfide, many sulfo-s polystyrene, vulcanized polyvinyl chloride, Phenyl polysulfide, sulfurized polyacrylonitrile, many sulfo-s naphthalene, Phenyl polysulfide amine, many thiopyridine, many sulfo-s thiophene, many sulfo-s pyrroles, many thio-furans etc.
Conductive agent described in scheme includes but not limited to graphite-based material, carbon-based material and conducting polymer.Graphite-based material comprises electrically conductive graphite KS6, and carbon-based material comprises that SuperP, Ketjen are black, acetylene black or carbon black.Conducting polymer comprises polyaniline, polypyrrole, polythiophene, polyacetylene, or their mixture.
Adhesive described in scheme is polyvinyl alcohol (PVA), polytetrafluoroethylene (PTFE), sodium carboxymethylcellulose (CMC), Kynoar (PVDF), polystyrenebutadienes copolymer (SBR), Viton and polyurethane, PVP, polyethyl acrylate, polyvinyl chloride, polyacrylonitrile, polycaprolactam, polybutadiene, polyisoprene, polyacrylic acid, and derivative, mixture or copolymer.
Collector includes but not limited to stainless steel, copper, nickel, titanium, aluminium.More preferably the aluminium collector of carbon coating, more easily covers the coating comprising positive active material, has lower contact resistance, and can suppress the corrosion of sulfide.
Negative pole
The negative pole containing aluminium active material described in scheme is metal aluminum or aluminum alloy.Metallic aluminium, the aluminium including but not limited to aluminium foil, aluminium wire, aluminium flake and be deposited on base material; Aluminium alloy, comprises the alloy containing at least one element be selected from Li, Na, K, Ca, Fe, Co, Ni, Cu, Zn, Mn, Sn, Pb, Ma, Ga, In, Cr, Ge and Al.
Electrolyte
Non-water described in scheme is made up of anhydrous aluminium salt, ionic liquid and organic solvent containing aluminium electrolyte.
The aluminium salt of to be the oxidation state of aluminium the be trivalent of the anhydrous aluminium salt described in scheme, comprises the one in aluminium sulfide, aluminum nitrate, aluminum sulfate, thiocyanation aluminium, aluminium chloride, aluminium bromide, silver iodide, aluminum perchlorate, trifluoromethane sulfonic acid aluminium.
Ionic liquid described in scheme is organic salt-aluminum halide system, and the mol ratio of organic salt and aluminum halide is 1:1.1 ~ 3.0.
In organic salt described in scheme-aluminum halide system, the cation of organic salt comprises imidazol ion, pyridinium ion, pyrrolidinium ion, piperidines ion, morpholinium ion, quaternary ammonium salt ion ， quaternary alkylphosphonium salt ion and tertiary sulfosalt ion; The anion of organic salt comprises Cl
-, Br
-, I
-, PF
6 -, BF
4 -, CN
-, SCN
-, [N (CF
3sO
2)
2]
-, [N (CN)
2]
-in one or more mixing.Include but not limited to aluminium chloride-triethylamine hydrochloride, aluminium chloride-chlorination 1-butyl-3-methylimidazole, aluminium chloride-phenyl trimethicone ammonium chloride, aluminium bromide-1-ethyl-3-methyllimidazolium bromide plasma liquid.
In organic salt described in scheme-aluminum halide system, aluminum halide is the one in aluminium chloride, aluminium bromide and silver iodide.
Organic solvent described in scheme is 1,2-dichloroethanes, carrene, benzene, toluene, one or more mixing in dimethylbenzene.
Non-water described in scheme is 0.1mol/L ~ 5mol/L containing the aluminium salt total concentration of dissolving in aluminium electrolyte.
The preparation method of the secondary aluminium-sulfur battery described in scheme is as follows:
Positive electrode active materials, conductive agent, binding agent being made in proportion active material slurry is applied on nickel foam substrate, oven dry rolls makes anode pole piece, battery core loading nickel plating box hat is wound into the negative pole that barrier film and use negative active core-shell material are made, the non-water that reinjects is containing aluminium electrolyte, and secondary aluminium cell is made in sealing.
(3) beneficial effect
(1) comparatively conventional batteries electrode material is compared, the advantages such as element aluminum and sulphur have that theoretical energy density is large, aboundresources, cheap, environmentally friendly, use safety, secondary aluminium cell provided by the invention is all that a kind of capacity is large, cheap, the ideal battery of use safety from every side.
(2) contain in aluminium electrolyte at non-water provided by the invention, the electrochemical reaction at aluminum honeycomb and the interface between sulphur positive pole and electrolyte is reversible, negative reaction shows as the deposition of aluminium-stripping circulation, the disconnection that positive pole reaction is S-S key and bonding, thus achieve aluminium-sulfur battery can discharge and recharge.
Embodiment
Be described further below with reference to the technique effect of embodiment to design of the present invention, concrete structure and generation, to understand object of the present invention, characteristic sum effect fully.The following examples describe several execution mode of the present invention, and they are only illustrative, and nonrestrictive.
Embodiment one
With " trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes ", electrolyte is for example, and in electrolyte, aluminium salt total concentration is about 2.2mol/L, and preparation process is as follows:
1. aluminium chloride/triethylamine hydrochloride ionic liquid is prepared
Under inert gas shielding, slowly added by 0.18mol aluminium chloride in 0.1mol triethylamine hydrochloride, stir 2 hours, obtained aluminium chloride/triethylamine hydrochloride ionic liquid, liquid is faint yellow.
2. aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes mixing material is prepared
In above-mentioned aluminium chloride/triethylamine hydrochloride ionic liquid, add 1,2-dichloroethanes to mixed solution cumulative volume is 100ml, stirs 2 hours, and obtained aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes mixed solution, solution is yellowish-brown.
3. trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes electrolyte is prepared
Under inert gas shielding; 0.04mol trifluoromethane sulfonic acid aluminium is slowly added above-mentioned aluminium chloride/triethylamine hydrochloride ionic liquid-1; in 2-dichloroethanes mixing material; stir 24 hours; i.e. obtained trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes electrolyte.
Embodiment two
For " aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene " electrolyte, in electrolyte, aluminium salt total concentration is about 2.2mol/L, and preparation process is as follows:
1. aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid is prepared
Under inert gas shielding, slowly added by 0.18mol aluminium chloride in 0.1mol chlorination 1-butyl-3-methylimidazole, stir 2 hours, obtained aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid, liquid is faint yellow.
2. aluminium chloride/chlorination 1-butyl-3-methylimidazole liquid-carrene mixing material is prepared
In above-mentioned aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid, add carrene to mixed solution cumulative volume is 100ml, stir 2 hours, obtained aluminium chloride/chlorination 1-butyl-3-methylimidazole liquid-carrene mixed solution, solution is yellowish-brown.
3. aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene electrolyte is prepared
Under inert gas shielding; 0.04mol aluminium bromide is slowly added in above-mentioned aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene mixing material; stir 24 hours, i.e. obtained aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene electrolyte.
With mesoporous carbon-sulphur composite material (sulfur nutrient 60%) for positive electrode, add conductive agent acetylene black, binding agent PVDF(ratio is 7:2:1), making active material slurry is applied on the thick nickel foam substrate of 0.6mm, oven dry roll to 0.33 millimeter be cut into 40mm wide × the long pole piece of 15mm, the glass fibre thick with 0.16mm is non-to be knitted barrier film and is wound into electric stamen loading nickel plating box hat with aluminium flake as the negative pole that negative active core-shell material is made, inject electrolyte prepared by embodiment one, two more respectively, AA type secondary aluminium cell is made in sealing.
Carry out charge-discharge test to battery, charge to 2.2V with 1C, 0.5C discharges, and discharges by voltage 1.2V.
The made battery of embodiment one, open circuit voltage 1.75V, first discharge capacity 517mAh, circulate after 50 times, discharge capacity 262mAh.
The made battery of embodiment two, open circuit voltage 1.77V, first discharge capacity 531mAh, circulate after 50 times, discharge capacity 273mAh.
Although reference embodiment is to invention has been detailed description, but those skilled in the art is to be understood that, when not departing from the spirit and scope of the present invention described in appended claims and equivalent thereof, various amendment and replacement can be made to it.
Claims (6)
1. a secondary aluminium cell, comprise the positive pole comprising electro-chemical activity sulphur-containing substance, containing the negative pole of aluminium active material and by anhydrous aluminium salt, the non-water of ionic liquid and organic solvent composition is containing aluminium electrolyte, wherein ionic liquid is organic salt-aluminum halide system, the mol ratio of organic salt and aluminum halide is 1:1.1 ~ 3.0, it is characterized in that: the aluminium salt of described anhydrous aluminium salt to be the oxidation state of aluminium be trivalent, comprise aluminium sulfide, aluminum nitrate, aluminum sulfate, thiocyanation aluminium, aluminium chloride, aluminium bromide, silver iodide, aluminum perchlorate, one in trifluoromethane sulfonic acid aluminium, described organic solvent is 1, 2-dichloroethanes, carrene, benzene, toluene, one or more mixing in dimethylbenzene.
2. secondary aluminium cell as claimed in claim 1, is characterized in that: described electro-chemical activity sulphur-containing substance is elemental sulfur or organosulfur compound.
3. secondary aluminium cell as claimed in claim 1, is characterized in that: the described negative pole containing aluminium active material is metal aluminum or aluminum alloy.
4. secondary aluminium cell as claimed in claim 1, is characterized in that: the cation of described organic salt comprises imidazol ion, pyridinium ion, pyrrolidinium ion, piperidines ion, morpholinium ion, quaternary ammonium salt ion ， quaternary alkylphosphonium salt ion and tertiary sulfosalt ion; The anion of organic salt comprises Cl
-, Br
-, I
-, PF
6 -, BF
4 -, CN
-, SCN
-, [N (CF
3sO
2)
2]
-, [N (CN)
2]
-in one or more mixing.
5. secondary aluminium cell as claimed in claim 1, is characterized in that: described aluminum halide is the one in aluminium chloride, aluminium bromide and silver iodide.
6. secondary aluminium cell as claimed in claim 1, is characterized in that: described non-water is 0.1mol/L ~ 5mol/L containing the aluminium salt total concentration of dissolving in aluminium electrolyte.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TWI654170B (en) | 2017-12-22 | 2019-03-21 | 財團法人工業技術研究院 | Electrolyte composition and metal-ion battery employing the same |
| US10340552B1 (en) | 2017-12-22 | 2019-07-02 | Industrial Technology Research Institute | Electrolyte composition and metal-ion battery employing the same |
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| CN104294327B (en) * | 2014-10-20 | 2016-07-13 | 中国科学院过程工程研究所 | A kind of il electrolyte and the method preparing light aluminium coat with this electrolyte |
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| WO2017062977A1 (en) * | 2015-10-08 | 2017-04-13 | Everon24 Llc | Rechargeable aluminum ion battery |
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| CN106848387B (en) * | 2017-02-20 | 2019-10-25 | 北京理工大学 | Aluminium ion battery electrolyte and its application and aluminium ion battery |
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| TWI659010B (en) * | 2017-12-22 | 2019-05-11 | 財團法人工業技術研究院 | Electrolyte composition and metal-ion battery employing the same |
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| JPH11135084A (en) * | 1997-10-29 | 1999-05-21 | Bl Engineering:Kk | Battery sealing aluminum lid |
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