CN104078705A - Secondary aluminium cell and electrolyte thereof - Google Patents
Secondary aluminium cell and electrolyte thereof Download PDFInfo
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- CN104078705A CN104078705A CN201410312674.5A CN201410312674A CN104078705A CN 104078705 A CN104078705 A CN 104078705A CN 201410312674 A CN201410312674 A CN 201410312674A CN 104078705 A CN104078705 A CN 104078705A
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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 secondary aluminium cell. The secondary aluminium cell comprises a cathode, an anode and electrolyte, wherein elemental sulfur or organosulfur compounds are selected as cathode active materials; metallic aluminium or aluminium alloys is/are selected as anode active materials; and non-aqueous aluminium-containing electrolyte formed by anhydrous aluminium salts, an ionic liquid and an organic solvent is used.
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 comprised of anhydrous aluminium salt, ionic liquid, organic solvent containing the secondary aluminium cell of aluminium electrolyte.
Background technology
Along with the fast development of global economy, the advancing by leaps and bounds of the aspect technology such as portable electric appts, electric automobile and space utilization, the mankind are more and more urgent to the demand of the Green Chemistry power supply of high-energy safe.Lithium battery is developed so far, and has become the chemical power source of the tool practicality of portable electric appts, and has extended to electrokinetic cell and energy-storage battery field.But due to aspect restrictions such as the chemical activity of elemental lithium self, energy densities, brought insoluble safety issue and battery capacity problem to the large scale development of lithium battery, therefore the high-energy battery of open other new type of safe of research becomes the difficult problem that international community generally faces.
Compare with traditional electrode material, element aluminum and sulphur all have the advantages such as theoretical energy density is large, aboundresources, cheap, environmentally friendly, use is safe.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 positive electrode of known energy density maximum.Therefore, aluminium-sulfur battery be all from every side a kind of cheap, energy density is high, use safe ideal battery.
Licht equals the nineties in 20th century exploitation a kind of at normal temperatures can repid discharge novel containing aluminium-sulfur battery of S high specific energy alkaline aqueous solution (US Pat:5431881,4828492,5648183).This battery be take aluminium alloy as anode, and the polysulfide being dissolved in alkaline electrolyte of take is 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 large, the problems such as overheated during work.The aluminium-sulfur battery of developing in reality only has the battery Open Circuit Potential of 1.3V and the energy density of 110Wh/kg (investigation of a novel aqueous aluminum/sulfur battery. Journal of Power Sources, 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 all use aluminum saline solutions are the reduction of cannot charging of electrolytical aluminum cell, can only be primary cells.Therefore, want to realize the chargeable of aluminum cell, what first need solution is exactly electro-deposition-stripping problem of the aluminium in electrolyte.Electrolytical selection is determining the working mechanism of secondary aluminium cell to a great extent, affects specific energy, cycle performance, rate charge-discharge performance, fail safe, storge quality and the cost etc. of battery.Selecting suitable electrolyte is the important prerequisite that realizes 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 in the present invention " two aluminium primary cells " for example comprises " 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) positive pole that comprises electro-chemical activity sulphur-containing substance;
(b) contain the negative pole of aluminium active material;
(c) the non-water being comprised of anhydrous aluminium salt, ionic liquid, organic solvent is containing aluminium electrolyte.
The preferred positive pole of electrochemical cell of the present invention, negative pole, electrolytical description below.
Anodal
The positive pole of battery of the present invention comprises positive active material, conductive agent, binding agent and the collector that contains electro-chemical activity sulphur-containing substance.Wherein, term " electro-chemical activity sulphur-containing substance " refers to the positive active material that comprises 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 sulfo-s pyridine, 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 Super P, 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), polystyrene butadiene 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 that comprises 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, includes but not limited to aluminium foil, aluminium wire, aluminium flake and is deposited on the aluminium on base material; Aluminium alloy, comprises and contains at least one element of being selected from Li, Na, K, Ca, Fe, Co, Ni, Cu, Zn, Mn, Sn, Pb, Ma, Ga, In, Cr, Ge and the alloy of Al.
Electrolyte
Non-water described in scheme is comprised of anhydrous aluminium salt, ionic liquid, organic solvent containing aluminium electrolyte.
The aluminium salt that the oxidation state that anhydrous aluminium salt described in scheme is aluminium is trivalent, includes but not limited to aluminium sulfide, aluminum nitrate, aluminum sulfate, thiocyanation aluminium, aluminium chloride, aluminium bromide, silver iodide, aluminum perchlorate, trifluoromethane sulfonic acid aluminium etc.
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-aluminum halide system described in scheme, the cation of organic salt comprises imidazol ion, pyridinium ion, pyrroles's ion, piperidines ion, morpholine 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]
-plasma.Include but not limited to aluminium chloride-triethylamine hydrochloride, aluminium chloride-chlorination 1-butyl-3-methylimidazole, aluminium chloride-phenyl trimethyl ammonium chloride, aluminium bromide-1-ethyl-3-methyllimidazolium bromide plasma liquid.
In organic salt-aluminum halide system described in scheme, aluminum halide is a kind of 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 are made to active material slurry to be in proportion applied on nickel foam substrate, oven dry rolls makes anode pole piece, with barrier film and use negative pole that negative active core-shell material is made to be wound into battery core to pack nickel plating box hat into, the non-water that reinjects is containing aluminium electrolyte, and secondary aluminium cell is made in sealing.
(3) beneficial effect
(1) compared with conventional batteries electrode material, compare, element aluminum and sulphur have that theoretical energy density is large, aboundresources, cheap, environmentally friendly, use the advantages such as safety, secondary aluminium cell provided by the invention be all from every side a kind of capacity large, cheap, use safe ideal battery.
(2) at non-water provided by the invention, contain in aluminium electrolyte, the electrochemical reaction at the interface between aluminium negative pole and sulphur positive pole and electrolyte is reversible, negative reaction shows as deposition-stripping circulation of aluminium, and anodal reaction is disconnection and the bonding of S-S key, thereby has realized discharging and recharging of aluminium-sulfur battery.
Embodiment
Below with reference to embodiment, the technique effect of design of the present invention, concrete structure and generation is described further, to understand fully object of the present invention, feature and effect.The following examples have been described several execution mode of the present invention, and they are only illustrative, and nonrestrictive.
Embodiment mono-
With " trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes " electrolyte, be example, in electrolyte, aluminium salt total concentration is about 2.2mol/L, and preparation process is as follows:
1. prepare aluminium chloride/triethylamine hydrochloride ionic liquid
Under inert gas shielding, 0.18mol aluminium chloride is slowly added in 0.1mol triethylamine hydrochloride, stir 2 hours, make aluminium chloride/triethylamine hydrochloride ionic liquid, it is faint yellow that liquid is.
2. prepare aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes mixing material
To adding 1,2-dichloroethanes to mixed solution cumulative volume in above-mentioned aluminium chloride/triethylamine hydrochloride ionic liquid, be 100ml, stir 2 hours, make aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes mixed solution, solution is yellowish-brown.
3. prepare trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes electrolyte
Under inert gas shielding; 0.04mol trifluoromethane sulfonic acid aluminium is slowly added to above-mentioned aluminium chloride/triethylamine hydrochloride ionic liquid-1; in 2-dichloroethanes mixing material; stir 24 hours; make trifluoromethane sulfonic acid aluminium-aluminium chloride/triethylamine hydrochloride ionic liquid-1,2-dichloroethanes electrolyte.
Embodiment bis-
" aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene " electrolyte of take is example, and in electrolyte, aluminium salt total concentration is about 2.2mol/L, and preparation process is as follows:
1. prepare aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid
Under inert gas shielding, 0.18mol aluminium chloride is slowly added in 0.1mol chlorination 1-butyl-3-methylimidazole, stir 2 hours, make aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid, it is faint yellow that liquid is.
2. prepare the sub-liquid-carrene of aluminium chloride/chlorination 1-butyl-3-methylimidazole mixing material
To adding carrene to mixed solution cumulative volume in above-mentioned aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid, be 100ml, stir 2 hours, make the sub-liquid-carrene of aluminium chloride/chlorination 1-butyl-3-methylimidazole mixed solution, solution is yellowish-brown.
3. prepare aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene electrolyte
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, make aluminium bromide-aluminium chloride/chlorination 1-butyl-3-methylimidazole ionic liquid-carrene electrolyte.
Mesoporous carbon-sulphur the composite material (sulphur mass fraction 60%) of take is positive electrode, adding conductive agent acetylene black, binding agent PVDF(ratio is 7:2:1), making active material slurry is applied on the nickel foam substrate that 0.6mm is thick, oven dry roll to 0.33 millimeter be cut into 40mm wide * the long pole piece of 15mm, be wound into electric stamen with the thick non-negative pole of knitting barrier film and making as negative active core-shell material with aluminium flake of glass fibre of 0.16mm and pack nickel plating box hat into, inject respectively the electrolyte of embodiment mono-, two preparations, AA type secondary aluminium cell is made in sealing again.
Battery is discharged and recharged to experiment, with 1C, charge to 2.2V, 0.5C electric discharge, electric discharge is by voltage 1.2V.
The made battery of embodiment mono-, open circuit voltage 1.75V, discharge capacity 517mAh, circulates after 50 times first, discharge capacity 262mAh.
The made battery of embodiment bis-, open circuit voltage 1.77V, discharge capacity 531mAh, circulates after 50 times first, discharge capacity 273mAh.
Although the present invention is described in detail with reference to embodiment, but those skilled in the art is to be understood that, in the situation that do not depart from the spirit and scope of the present invention described in appended claims and equivalent thereof, can make various modifications and replacement to it.
Claims (9)
1. a secondary aluminium cell, comprising:
(a) positive pole that comprises electro-chemical activity sulphur-containing substance;
(b) contain the negative pole of aluminium active material;
(c) the non-water being comprised of anhydrous aluminium salt, ionic liquid, organic solvent is containing aluminium electrolyte.
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, it is characterized in that: the aluminium salt that the oxidation state that described anhydrous aluminium salt is aluminium is trivalent, includes but not limited to aluminium sulfide, aluminum nitrate, aluminum sulfate, thiocyanation aluminium, aluminium chloride, aluminium bromide, silver iodide, aluminum perchlorate, trifluoromethane sulfonic acid aluminium etc.
5. secondary aluminium cell as claimed in claim 1, is characterized in that: described ionic liquid is organic salt-aluminum halide system, and the mol ratio of organic salt and aluminum halide is 1:1.1～3.0.
6. secondary aluminium cell as claimed in claim 5, is characterized in that: the cation of described organic salt comprises imidazol ion, pyridinium ion, pyrroles's ion, piperidines ion, morpholine 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]
-plasma.
7. secondary aluminium cell as claimed in claim 5, is characterized in that: described aluminum halide is a kind of in aluminium chloride, aluminium bromide and silver iodide.
8. secondary aluminium cell as claimed in claim 1, is characterized in that: described organic solvent is 1,2-dichloroethanes, carrene, benzene, toluene, one or more mixing in dimethylbenzene.
9. 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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|---|---|---|---|
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|---|---|---|---|
| CN201410312674.5A CN104078705B (en) | 2014-07-03 | 2014-07-03 | A kind of secondary aluminium cell and electrolyte thereof |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104294327A (en) * | 2014-10-20 | 2015-01-21 | 中国科学院过程工程研究所 | Ionic liquid electrolyte and method for preparing bright aluminum coating by use of ionic liquid electrolyte |
| CN104393264A (en) * | 2014-12-01 | 2015-03-04 | 杨成 | High-capacity battery and preparation method thereof |
| CN106848387A (en) * | 2017-02-20 | 2017-06-13 | 北京理工大学 | Aluminium ion battery electrolyte and its application and aluminium ion battery |
| CN107665987A (en) * | 2016-07-29 | 2018-02-06 | 横店集团东磁股份有限公司 | A kind of battery and its assemble method using brominated ionic liquid as positive active material |
| CN109148942A (en) * | 2017-06-28 | 2019-01-04 | 福建省辉锐材料科技有限公司 | A kind of preparation method of novel aluminum Dual-ion cell |
| 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 |
| US10587009B2 (en) | 2017-12-22 | 2020-03-10 | Industrial Technology Research Institute | Electrolyte composition and metal-ion battery employing the same |
| CN111261930A (en) * | 2018-11-30 | 2020-06-09 | 杭州怡莱珂科技有限公司 | Aluminum ion battery solid electrolyte solution and battery |
| CN114006129A (en) * | 2015-10-08 | 2022-02-01 | 艾沃伦24公司 | Chargeable aluminium ion battery |
| TWI847940B (en) * | 2023-12-19 | 2024-07-01 | 亞福儲能股份有限公司 | Aluminum battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| CN104294327A (en) * | 2014-10-20 | 2015-01-21 | 中国科学院过程工程研究所 | Ionic liquid electrolyte and method for preparing bright aluminum coating by use of ionic liquid electrolyte |
| CN104393264A (en) * | 2014-12-01 | 2015-03-04 | 杨成 | High-capacity battery and preparation method thereof |
| CN114006129A (en) * | 2015-10-08 | 2022-02-01 | 艾沃伦24公司 | Chargeable aluminium ion battery |
| CN107665987B (en) * | 2016-07-29 | 2020-03-27 | 横店集团东磁股份有限公司 | Battery using bromine-containing ionic liquid as positive electrode active material and assembling method thereof |
| CN107665987A (en) * | 2016-07-29 | 2018-02-06 | 横店集团东磁股份有限公司 | A kind of battery and its assemble method using brominated ionic liquid as positive active material |
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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 |
| CN109148942A (en) * | 2017-06-28 | 2019-01-04 | 福建省辉锐材料科技有限公司 | A kind of preparation method of novel aluminum Dual-ion cell |
| US10587009B2 (en) | 2017-12-22 | 2020-03-10 | Industrial Technology Research Institute | Electrolyte composition and metal-ion battery employing the same |
| 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 |
| CN111261930A (en) * | 2018-11-30 | 2020-06-09 | 杭州怡莱珂科技有限公司 | Aluminum ion battery solid electrolyte solution and battery |
| CN111261930B (en) * | 2018-11-30 | 2021-05-07 | 杭州怡莱珂科技有限公司 | Aluminum ion battery solid electrolyte solution and battery |
| TWI847940B (en) * | 2023-12-19 | 2024-07-01 | 亞福儲能股份有限公司 | Aluminum battery |
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|---|---|
| CN104078705B (en) | 2016-03-23 |
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