CN204156009U - A kind of secondary aluminium cell - Google Patents
A kind of secondary aluminium cell Download PDFInfo
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- CN204156009U CN204156009U CN201420592666.6U CN201420592666U CN204156009U CN 204156009 U CN204156009 U CN 204156009U CN 201420592666 U CN201420592666 U CN 201420592666U CN 204156009 U CN204156009 U CN 204156009U
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- carbon
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- secondary aluminium
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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 utility model discloses a kind of secondary aluminium cell of novel, high energy, comprise positive pole, negative pole and electrolyte.Described positive active material is the coated sulfurized polyacrylonitrile of material with carbon element; Negative pole is for containing aluminum honeycomb, and electrolyte is that non-water is containing aluminium electrolyte.Described secondary aluminium cell specific capacity is high, good cycle, and preparation technology is simple, and suitability for industrialized is produced.
Description
Technical field
The utility model belongs to electrochemistry and new forms of energy product scope, relates to a kind of secondary aluminium cell.
Background technology
Along with developing rapidly of movable electronic and communication apparatus, the demand of secondary cell is more urgent, and more and more tends to the exploitation of battery of intensity, slim, small-sized, light-duty and high-energy-density.The energy density of aluminium is 2980mAh/g, and its quality is light, cheap, aboundresources, use safety, is desirable cell negative electrode material; The energy density of sulphur is 1675mAh/g, nature rich reserves, safety and environmental protection, and cheap, application is in the secondary battery comparatively extensive.Therefore with aluminum metal or aluminium alloy for secondary aluminium-sulfur battery that negative pole and sulfenyl material are positive pole is the battery system of the most attraction meeting demand.
The operation principle of secondary aluminium-sulfur battery is the Reversible redox reaction between sulphur and aluminium.At present, the technical bottleneck of aluminium-sulfur battery is that the intermediate poly sulfide that sulfur-based positive electrode material also exists active material loss, poorly conductive, reduction process produce is soluble in electrolyte, the diffusion of partly soluble poly sulfide arrives metallic aluminium negative terminal surface and produces self discharge reaction and be deposited on negative pole and make the problems such as its passivation, finally causes that sulphur active material utilization is low, capacity attenuation is rapid, cycle performance of battery is poor.
Organic sulfur compound can be obtained the sulphur positive electrode of high stability for the preparation of sulfur-bearing char-forming material as carbon matrix precursor.In the secondary aluminium-sulfur battery that patent CN200910234924.7 provides, polyacrylonitrile mixes with sulphur and heats cyclization occurs, and the sulfurized polyacrylonitrile of formation is that one has long-range π key conjugated system polymer, and this polymer has higher specific capacity.But because the above-mentioned cyclisation degree preparing sulfurized polyacrylonitrile is not high, the conjugatedπbond playing electric action formed is less, thus makes the conductivity of sulfurized polyacrylonitrile lower, causes the utilance of sulphur positive active material low.And still can not avoid the dissolving of electric discharge intermediate product in battery charge and discharge process, circulating battery is poor.Carbon is coated is also one of the most important method improving positive electrode capacity, high rate performance, cyclical stability, and its Main Function is the conductivity improving positive active material, makes material have good chemical property under high magnification.But coated can being with of carbon serves negative effect, such as reduces the density of material, increase operation and cost etc., therefore the preparation technology of sulfur-based positive electrode material need optimize further.
Summary of the invention
(1) goal of the invention
Poor for overcoming sulfur-based positive electrode material conductivity in prior art, reactant is soluble in the defect of electrolyte, the preparation method of the sulfur-based composite anode material that the utility model provides a kind of conductivity is high, reactant is insoluble to electrolyte carbon coated, and specific capacity is high, the secondary aluminium-sulfur battery of good cycle.
Polyacrylonitrile is with sulphur compound, and what reaction generated has stability and the conductivity that long-range π key conjugated system polymer effectively can improve electrode, improves utilance and the electrode specific capacity of active material sulphur simultaneously; The crosslinked action of the two sulphur-carbon chemical bond formed can limit the dissolving of polysulfide to a certain extent, suppresses to shuttle back and forth the destruction of effect to electrode, improves the cycle performance of battery.At the material with carbon element film of the coated one deck nano thickness of polyacrylonitrile/sulphur composite material surface, while raising conductance, avoid the direct contact of active material with electrolyte, the dissolving of polysulfide in electrochemical reaction process can be prevented further.The existence of material with carbon element layer and conducting polymer effectively can also alleviate sulphur bulk effect in charge and discharge process, improves the cycle performance of positive electrode to a great extent.In addition, prepare without the need to adding conductive agent in electrode process, further increase the specific capacity of electrode, energy density is also higher.
(2) technical scheme
For realizing above-mentioned utility model object, the utility model provides following technical scheme:
A kind of secondary aluminium cell, comprise positive pole, negative pole and electrolyte, it is characterized in that, described positive pole is made up of positive electrode material layer and collector, positive electrode material layer is coated on collector, wherein positive electrode is made up of positive active material sulfurized polyacrylonitrile and material with carbon element, and material with carbon element is coated on sulfurized polyacrylonitrile outer surface; Described negative pole is for containing aluminum honeycomb; Described electrolyte is that non-water is containing aluminium electrolyte; Described barrier film is between positive pole and negative pole.
Here is the description of the preferred positive pole of secondary aluminium cell described in the utility model, negative pole, electrolyte and barrier film.
(1) positive pole
The positive pole of secondary aluminium cell described in the utility model comprises positive active material, binding agent and collector.Because coated material with carbon element has good conductivity, without the need to adding conductive agent.
Positive active material described in the utility model is the coated sulfurized polyacrylonitrile of carbon, coated material with carbon element comprise in agraphitic carbon, graphite, Graphene, graphite fibre, carbon fiber, carbon nano-tube any one.
The thickness of material with carbon element coating layer described in the utility model is 5 ~ 10nm.
Positive active material described in the utility model is the coated sulfurized polyacrylonitrile of carbon, and its preparation method is as follows:
1) sulfurized polyacrylonitrile preparation
By polyacrylonitrile and sublimed sulfur, (10:1 ~ 5:1) mixed grinding is even by a certain percentage, puts into the quartz ampoule of sealing, under inert gas (nitrogen or argon gas) condition, heats 5 ~ 8 hours, obtain the sulfurized polyacrylonitrile of black in 200 ~ 300 DEG C of temperature;
Or, polyacrylonitrile is dissolved in solvent dimethylformamide and prepares polyacrylonitrile solution, add Fe catalyst, stir and be heated to 200 DEG C simultaneously, keep 2 hours, then add elemental sulfur or sodium thiosulfate wherein, stir, be heated to 300 ~ 400 DEG C, keep 5 ~ 10 hours, obtain sulfurized polyacrylonitrile;
2) carbon coated material
Take material with carbon element and the sulfurized polyacrylonitrile of certain proportion (1:5 ~ 1:15), mix and be placed in airtight quartz ampoule, under inert gas (nitrogen or argon gas) condition, heat 0.5 ~ 1.5 hour in 300 ~ 400 DEG C of temperature, obtain the sulfurized polyacrylonitrile that positive active material carbon is coated;
Or, material with carbon element is scattered in alcohol solvent and forms mixed solution, sulfurized polyacrylonitrile is placed in one, be uniformly mixed and treat solvent evaporates, then under inert gas (nitrogen or argon gas) condition, be heated to 300 ~ 400 DEG C, keep 5 ~ 10 hours, obtain the sulfurized polyacrylonitrile that positive active material carbon is coated;
Or, adopt chemical gaseous phase depositing process to carry out carbon at sulfurized polyacrylonitrile material surface coated.
Adhesive described in the utility model be aqueous binder LA132(Chengdu mattress happy), 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.Be preferably mattress ground, aqueous binder LA132(Chengdu happy).
Collector described in the utility model comprises 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.
(2) negative pole
Described in the utility model containing aluminum honeycomb active material, comprising: aluminum metal, such as aluminium foil and the aluminium that is 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.
(3) electrolyte
Non-water described in the utility model is organic salt-aluminum halide system ionic liquid containing aluminium electrolyte, and wherein, the mol ratio of organic salt and aluminum halide is 1:1.1 ~ 3.0.
In organic salt described in the utility model-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]
-ion.
Organic salt described in the utility model-aluminum halide system, is characterized in that, described aluminum halide is the one in aluminium chloride, aluminium bromide or silver iodide.
Organic salt described in the utility model-aluminum halide system comprises 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.
(4) barrier film
Secondary aluminium cell described in the utility model also can comprise the barrier film between positive pole and negative pole.Suitable solid porous separator material comprises polyolefin as the one in polyethylene and polypropylene, glass fiber filter paper, ceramic material.Other example being applicable to diaphragm material of the present utility model comprises microporous pseudo-boehmite layer, and it can be the form of free-standing film or be coated directly onto on an electrode.
The preparation method of secondary aluminium cell described in the utility model is as follows: positive electrode active materials, binding agent (ratio is 8:2) are made active material slurry and be applied on the thick collector of 0.6mm, oven dry rolls to about 0.33mm, be cut into 40mm wide × the long pole piece of 15mm is as positive plate, the barrier film thick with 0.16mm and negative pole are wound into battery core and load nickel plating box hat, reinject electrolyte, and secondary aluminium cell is made in sealing.
(3) beneficial effect
The utility model provides the secondary aluminium cell of the coated sulfurized polyacrylonitrile of a kind of just very carbon, compared with the existing technology has following advantage:
(1) in positive electrode, the existence of polyacrylonitrile can improve stability and the conductivity of positive pole, effectively can slow down again the destruction of change in volume to positive pole of sulphur in charge and discharge process, the crosslinked action of sulphur-carbon chemical bond that simultaneous reactions generates can limit the dissolving of polysulfide, suppress to shuttle back and forth the destruction of effect to electrode, effectively improve the cycle performance of secondary aluminium cell.
(2) because coated material with carbon element has good conductivity, the preparation of positive pole, without the need to adding conductive agent, improves specific capacity.
(3) the coated and existence that is conducting polymer of carbon effectively improves the chemical property of positive electrode active materials, on the one hand for the bulk effect in sulphur discharge and recharge provides certain cushion space, after carbon coated, the Electric Field Distribution of material is more even on the other hand, reduces the overpotential polarizing and cause.
(4) adopt different material with carbon elements and different technique to carry out carbon coated, significantly improve the conductivity of carbon coated, improve the high rate performance of battery.
(5) the secondary aluminium cell specific capacity prepared by is high, good cycle, long service life.
(4) accompanying drawing explanation
Fig. 1 is composite positive pole structural representation described in the utility model.
Fig. 2 is the structural representation of secondary aluminium cell described in the utility model.
Fig. 3 is secondary aluminium cell anode structure schematic diagram described in the utility model.
Wherein, 1-sulfurized polyacrylonitrile, 2-material with carbon element layer, 3-upper cover, 4-insulation cushion, 5-positive pole, 6-barrier film, 7-negative pole, 8-housing, 9-positive electrode material layer, 10-collector.
(5) embodiment
Be described further below with reference to the technique effect of drawings and Examples to design of the present utility model, concrete structure and generation, to understand the purpose of this utility model, characteristic sum effect fully.The following examples describe several execution mode of the present utility model, and they are only illustrative, and nonrestrictive.
See accompanying drawing 1, the utility model provides a kind of composite positive pole with high-energy-density and good circulation performance and comprises sulfurized polyacrylonitrile 1, material with carbon element layer 2.Polyacrylonitrile 1 outer cladding carbon 2 forms layer structure.
See accompanying drawing 2, the utility model also provides a kind of secondary aluminium cell applying this composite positive pole.Comprise battery container 8, the cell cover 3 be positioned in battery container 8, insulation cushion 4, positive pole 5, barrier film 6, negative pole 7, housing 8, is wherein separated by insulation cushion 4 between electrode and battery case.
See accompanying drawing 3, secondary aluminium cell anode structure schematic diagram in the utility model.Comprise positive electrode material layer 9 and collector 10, wherein positive electrode material layer 9 is coated on collector 10 and forms anode pole piece.
embodiment 1
(1) prepare sulfurized polyacrylonitrile: by polyacrylonitrile and sublimed sulfur even in 10:1 ratio mixed grinding, put into the quartz ampoule of sealing, under inert gas (nitrogen or argon gas) condition, be warming up to 300 DEG C and keep 8 hours, obtain the sulfurized polyacrylonitrile of black.
(2) carbon coated material: the sucrose and the sulfurized polyacrylonitrile that take 1:8 ratio, mix and be placed in airtight quartz ampoule, under inert gas (nitrogen or argon gas) condition, first be rapidly heated to 200 DEG C, slowly be warming up to 400 DEG C again, keep 1 hour, obtain the sulfurized polyacrylonitrile that positive active material carbon is coated.
(3) secondary aluminium cell is prepared: be 8:2 by sulfurized polyacrylonitrile coated for positive electrode active materials carbon, binding agent LA132(ratio) make active material slurry and be applied on the thick nickel foam substrate of 0.6mm, oven dry rolls to about 0.33mm, be cut into 40mm wide × the long pole piece of 15mm is as positive plate, the glass fibre thick with 0.16mm be non-to be knitted barrier film and negative pole and is wound into battery core and loads nickel plating box hat, reinject aluminium chloride-triethylamine hydrochloride ionic liquid, and AA type cylinder secondary aluminium cell is made in sealing.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.76V, and most high discharge capacity is 683mAh, and after 50 charge and discharge cycles, discharge capacity is 486mAh.
embodiment 2
(1) sulfurized polyacrylonitrile is prepared: polyacrylonitrile is dissolved in solvent dimethylformamide and prepares polyacrylonitrile solution, add Fe catalyst, stir and be heated to 200 DEG C simultaneously, keep 2 hours, then add elemental sulfur wherein, polyacrylonitrile and elemental sulfur ratio are 5:1, stir, be heated to 350 DEG C, keep 10 hours, obtain sulfurized polyacrylonitrile.
(2) carbon coated material: material with carbon element is scattered in alcohol solvent and forms mixed solution, sulfurized polyacrylonitrile is placed in one, material with carbon element and sulfurized polyacrylonitrile ratio are 1:10, be uniformly mixed and treat solvent evaporates, then, under inert gas (nitrogen or argon gas) condition, be first rapidly heated to 200 DEG C, be more slowly heated to 350 DEG C, keep 5 hours, obtain the sulfurized polyacrylonitrile that positive active material carbon is coated.
(3) secondary aluminium cell is prepared: be 8:2 by sulfurized polyacrylonitrile coated for positive electrode active materials carbon, binding agent PVDF(ratio) make active material slurry and be applied on the aluminium collector of the thick carbon coating of 0.6mm, oven dry rolls to about 0.33mm, be cut into 40mm wide × the long pole piece of 15mm is as positive plate, the glass fibre thick with 0.16mm be non-to be knitted barrier film and negative pole and is wound into battery core and loads nickel plating box hat, reinject aluminium chloride-triethylamine hydrochloride ionic liquid, and AA type cylinder secondary aluminium cell is made in sealing.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.70V, and most high discharge capacity is 690mAh, and after 50 charge and discharge cycles, discharge capacity is 503mAh.
embodiment 3
(1) preparation of sulfurized polyacrylonitrile is with embodiment 1.
(2) carbon coated material: change sucrose into cellulose acetate, is first rapidly heated to 300 DEG C, is more slowly warming up to 450 DEG C, and all the other are with embodiment 2.
(3) preparation of secondary aluminium cell is with embodiment 2.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.71V, and most high discharge capacity is 674mAh, and after 50 charge and discharge cycles, discharge capacity is 472mAh.
embodiment 4
(1) preparation of sulfurized polyacrylonitrile is with embodiment 1.
(2) carbon coated material: take acetylene as carbon source, Fe is catalyst, hydrogen and nitrogen are carrier gas, adopt chemical gaseous phase depositing process to carry out carbon at sulfurized polyacrylonitrile material surface in 600 ~ 700 DEG C coated, the sulfurized polyacrylonitrile of obtained positive active material nano-carbon coated.
(3) preparation of secondary aluminium cell is with embodiment 2.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.78V, and most high discharge capacity is 697mAh, and after 50 charge and discharge cycles, discharge capacity is 512mAh.
embodiment 5
(1) preparation of sulfurized polyacrylonitrile is with embodiment 1.
(2) carbon coated material: configuration concentration is the graphene oxide water solution of 10mg/mL; ultrasonic disperse 10h; then the sulfurized polyacrylonitrile prepared is added wherein; add reducing agent ammoniacal liquor to it simultaneously, under ultrasound condition, react 24h, obtain the sulfurized polyacrylonitrile of the few layer graphene lamella of Surface coating; after taking out product washing, drying; under inert nitrogen gas protection, be warming up to 700 DEG C, keep 5 ~ 10h, the sulfurized polyacrylonitrile that obtained positive active material carbon is coated.
(3) preparation of secondary aluminium cell is with embodiment 1.
During battery charging and discharging loop test, carry out charging to 2.5V with 1C, 0.1C discharges, and discharge cut-off voltage is 1.2V.Battery open circuit voltage is 1.72V, and most high discharge capacity is 686mAh, and after 50 charge and discharge cycles, discharge capacity is 480mAh.
Although be described in detail the utility model with reference to embodiment, but those skilled in the art is to be understood that, when the design of the present utility model do not departed from described in appended claims and equivalent thereof and scope, various amendment and replacement can be made to it.
Claims (6)
1. a secondary aluminium cell, comprise positive pole, negative pole and electrolyte, it is characterized in that, described positive pole is made up of positive electrode material layer and collector, positive electrode material layer is coated on collector, wherein positive electrode is made up of positive active material sulfurized polyacrylonitrile and material with carbon element, and material with carbon element is coated on sulfurized polyacrylonitrile outer surface; Described negative pole is for containing aluminum honeycomb; Described electrolyte is that non-water is containing aluminium electrolyte; Described barrier film is between positive pole and negative pole.
2. secondary aluminium cell according to claim 1, it is characterized in that, the coated material with carbon element of described positive active material comprise in agraphitic carbon, graphite, Graphene, graphite fibre, carbon fiber, carbon nano-tube any one, the thickness of material with carbon element coating layer is 5 ~ 10nm.
3. secondary aluminium cell according to claim 1, is characterized in that, the described aluminum honeycomb that contains comprises aluminum metal or aluminium alloy.
4. secondary aluminium cell according to claim 1, is characterized in that, described non-water comprises organic salt-aluminum halide system ionic liquid containing aluminium electrolyte.
5. secondary aluminium cell according to claim 5, 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]
-ion.
6. secondary aluminium cell according to claim 1, is characterized in that, described diaphragm material comprises polyolefin as the one in polyethylene and polypropylene, glass fiber filter paper, ceramic material.
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|---|---|---|---|
| CN201420592666.6U CN204156009U (en) | 2014-10-14 | 2014-10-14 | A kind of secondary aluminium cell |
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|---|---|---|---|
| CN201420592666.6U CN204156009U (en) | 2014-10-14 | 2014-10-14 | A kind of secondary aluminium cell |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104300127A (en) * | 2014-10-14 | 2015-01-21 | 南京中储新能源有限公司 | Sulfur-based composite material coated with carbon, preparation and application thereof |
| CN109546154A (en) * | 2018-12-13 | 2019-03-29 | 北京理工大学 | A kind of aluminium ion battery afflux liquid with protective layer |
| CN110495036A (en) * | 2017-02-13 | 2019-11-22 | 纳米技术仪器公司 | Aluminum secondary battery and manufacturing method with high capacity and high-energy cathode |
| CN111668536A (en) * | 2020-05-27 | 2020-09-15 | 北京科技大学 | A kind of preparation method of metal aluminum-cyano organic secondary battery |
-
2014
- 2014-10-14 CN CN201420592666.6U patent/CN204156009U/en not_active Expired - Fee Related
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104300127A (en) * | 2014-10-14 | 2015-01-21 | 南京中储新能源有限公司 | Sulfur-based composite material coated with carbon, preparation and application thereof |
| CN110495036A (en) * | 2017-02-13 | 2019-11-22 | 纳米技术仪器公司 | Aluminum secondary battery and manufacturing method with high capacity and high-energy cathode |
| CN110495036B (en) * | 2017-02-13 | 2023-12-19 | 纳米技术仪器公司 | Aluminum secondary battery with high capacity and high energy cathode and method of manufacturing the same |
| CN109546154A (en) * | 2018-12-13 | 2019-03-29 | 北京理工大学 | A kind of aluminium ion battery afflux liquid with protective layer |
| CN111668536A (en) * | 2020-05-27 | 2020-09-15 | 北京科技大学 | A kind of preparation method of metal aluminum-cyano organic secondary battery |
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