CN104393290B - A kind of employing MoS2aluminium ion battery for positive electrode and preparation method thereof - Google Patents
A kind of employing MoS2aluminium ion battery for positive electrode and preparation method thereof Download PDFInfo
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- H01M4/02—Electrodes composed of, or comprising, active material
- 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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- H01M4/5815—Sulfides
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- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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- H—ELECTRICITY
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- H01M10/00—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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- H—ELECTRICITY
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- 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
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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
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- 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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
A kind of employing MoS2Aluminium ion battery for positive electrode and preparation method thereof, belongs to cell art, can be widely applied to the field such as electronic industry, communication industry, it is possible to be applied to the electrokinetic cell of electric automobile.The aluminium ion battery of the present invention comprises positive active material, negative pole, diaphragm material, liquid aluminium ion electrolyte and electrolytic cell device, and wherein positive active material is MoS2, negative pole is high-purity aluminium flake, and liquid ion electrolyte is containing Al3+The nonaqueous solution electrolysis liquid of ion.Aluminium ion secondary cell provided by the present invention can be repeatedly charged and discharged, have high power capacity, efficiency for charge-discharge is high, good cycling stability and charge-discharge characteristic excellent, and electrode material wide material sources, preparation easily, low cost, environmental protection and cheap.
Description
Technical field
The invention belongs to a kind of employing MoS2Aluminium ion battery for positive electrode and preparation method thereof, can be as new green power battery applications in fields such as electronic industry, communications industry and power battery of electric vehicle.
Background technology
Currently, the non-renewable Fossil fuel such as coal, oil and natural gas is the most exhausted, and environmental pollution and greenhouse effect increasingly sharpen, and energy crisis and environmental conservation become two hang-ups that the world faces.Therefore, exploitation new green power and energy storage device increasingly attract much attention.Since Sony Corporation of Japan successfully releases lithium ion battery, lithium ion battery is just widely used in many-sides such as electronic product, power source, military fields rapidly, currently develops to the electrokinetic cell industrial aspect of electric automobile.But owing to the limitation of lithium resource causes cost intensive and bigger potential safety hazard to limit the further development of lithium ion battery.Thus, in recent years, as aiming at high capacity, the ionic conductor of lithium ion can be replaced, use the class rechargeable battery research of polycation to become increasingly active.
Aluminium element content in the earth's crust is only second to oxygen and silicon, occupies the 3rd, is the metallic element that in the earth's crust, content is the abundantest, and cost of winning is low, low price, if as battery material, the Al of aluminium ion rechargeable battery exchange trivalent3+, it is expected to capacity is greatly improved, so multivalent ion battery based on aluminium ion embedding and deintercalation is expected to be used for extensive energy storage device.Therefore, develop that specific capacity is high, security performance is good, the novel multivalent ion battery of good cycling stability, there is highly important commercial exploitation.
Summary of the invention
The present invention provides a kind of novel secondary battery that may replace lithium ion battery, and multivalent ion rechargeable battery and preparation method thereof, it is achieved that the high power capacity discharge and recharge of rechargeable aluminium ion battery, and good cycle and security performance are high.
For achieving the above object, the present invention provides techniques below scheme:
The rechargeable aluminium ion battery that the present invention proposes, its operation principle and existing lithium ion battery, sodium-ion battery operation principle are similar.
A kind of employing MoS2For the aluminium ion battery of positive electrode, its feature comprises positive active material and conductive material and composite, negative pole and the aluminium ion nonaqueous solution electrolysis liquid of binding agent composition and electrolytic cell device, and wherein positive active material is MoS2, negative pole is rafifinal；Aluminium ion nonaqueous solution electrolysis liquid is mixed in proportion with anhydrous Aluminum chloride by 3-Methylimidazole. compounds and forms.
Described MoS2Material is micron order that is commercially available or that prepared by chemical method and physical method or nanoscale MoS2, wherein chemical method includes chemical vapour deposition technique, high temperature vulcanized method, presoma decomposition method, hydro-thermal method and solwution method etc.；Physical method includes mechanical milling method, plasma spraying method and high-voltage arc method etc..
Conductive material employed in described composite is platinum slurry, silver slurry, amorphous carbon and Super-P, wherein to add 10% when using amorphous carbon and the Super-P binding agent of (mass fraction).
Described binding agent is the one in Kynoar (PVDF) or politef (PTFE).
Described 3-Methylimidazole. compounds includes one or more in 1-butyl-3-methylimidazolium chloride, 1-propyl group-3-Methylimidazole. villaumite, 1-ethyl-3-methylimidazole chloride, 1-butyl-3-methyl imidazolium tetrafluoroborate, 1-butyl-3-Methylimidazole. hexafluorophosphate.
In the electrolyte of described aluminium ion battery, the mass ratio of anhydrous Aluminum chloride and 3-Methylimidazole. compounds is 1.1:1-1.6:1, is preferably in a proportion of 1.3:1.
Described electrolytic cell device is glass electrolyzer or plastics electrolyzer.
MoS used as described above2For the preparation method of the aluminium ion battery of positive electrode, including following preparation process:
1) by positive electrode MoS2The composite formed with conductive material and binding agent thereof is uniformly fixed on the inert metal paillon foil collector that polishing is clean, and wraps up with diaphragm material, and wherein inert metal paillon foil collector is molybdenum sheet, titanium sheet, nickel foam or the noble metal such as gold and platinum family；
2) it is the rafifinal of 0.2-2mm by thickness, as negative material after cleaning；
3) preparation is containing the Al that can move freely3+The nonaqueous solution electrolysis liquid of ion；
4) after getting out positive electrode, negative material and aluminium ion nonaqueous solution electrolysis liquid, assembled battery in oxygen-free environment (in glove box)；
5) after set of cells installs, its electrode is entirely insertable in electrolyte, after the whole wetting electrode of liquid to be electrolysed, carries out charge-discharge test again.
The electrolytic cell device of aluminium ion used in battery is glass electrolyzer or plastics electrolyzer.
In above-mentioned aluminium ion battery preparation method step (1), described diaphragm material is for having ion permeability and not reacting with both positive and negative polarity, and there is stable chemical property, good mechanical performance and electrochemical stability, such as microporous polyolefin film diaphragm material and glass fiber material.
In above-mentioned aluminium ion battery preparation method step (1), described MoS2Material mixes in proportion with conductive material, is then fixed on inert metal collector, and as positive pole, wherein fixed form can be to smear, suppress and bonding.
In above-mentioned aluminium ion battery preparation method step (1), if use amorphous carbon or Super-P as conductive material, MoS2Material usage is 50-85% (mass fraction), conductive material is 10-40% (mass fraction), binding agent is 5-10% (mass fraction).If use platinum slurry or silver slurry as conductive material, MoS2Material usage is 60-90% (mass fraction), conductive material is 10-40% (mass fraction).
In above-mentioned aluminium ion battery preparation method step (2), first rafifinal is cut into lamellar, then it is smoothed with sand papering, it is carried out again, the method wherein cleaned is, with organic liquid, such as dehydrated alcohol or acetone soak ultrasonic vibration, then it is dried in 60-120 degree Celsius of baking oven.
In above-mentioned aluminium ion battery preparation method step (3), containing Al3+The liquid nonaqueous solution electrolysis liquid of ion must be prepared in glove box, can use after then its essence being put more than 12 hours.
The present invention uses MoS2As positive pole, rafifinal, as negative pole, constitutes a kind of chargeable aluminium ion battery.Owing to the present invention has carried out fine selection to positive and negative pole material, barrier film and electrolyte thereof etc. by experimentation, and combine tight preparation method, so the invention have the characteristics that: propose a kind of novel multivalent ion, i.e. aluminium ion battery system, which also promotes the development of energy storage device；Owing to aluminium element is at the rich reserves of the earth's crust, low price, greatly reduces the preparation cost of battery, also improve the security performance of ion battery simultaneously；MoS2Chemical stability and Heat stability is good, specific surface area is big, surface activity is high, therefore have uniqueness physics and chemical characteristic, so having a wide range of applications in terms of electrochemical energy storage；Barrier film has good insulating properties, has good transparent performance to electrolyte ion, has preferable chemical stability and electrochemical stability；Aluminium ion electrolyte, conductivity is high, and in Heat stability is good, with battery, positive and negative pole material, barrier film and binding agent etc. do not occur chemical reaction；The aluminium ion battery of the present invention can be widely applied to the field such as electronic industry, communication industry, it is possible to is applied to the electrokinetic cell of electric automobile.
Accompanying drawing explanation
Fig. 1 is 2 circle charge-discharge performance test curves before aluminium ion battery prepared by embodiment 1；
Fig. 2 is the cycle performance test curve of the aluminium ion battery of embodiment 2 preparation.
Detailed description of the invention
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
Use MoS2As positive active material, positive plate assembles and presses MoS2: platinum slurry mass ratio is that the ratio mixing of 70:30 is uniform, is then spread upon by gelling material on the molybdenum sheet of 10mm × 20mm uniformly, finally wraps up as anode with GF/D diaphragm material after 60-120 degree Celsius of baking oven stands and dry for more than 12 hours.Negative pole is rafifinal, it is soaked 1-2 hour in dehydrated alcohol, and ultrasonic vibration is dried, is cut into the lamellar of 10mm × 20mm as negative pole.Anhydrous Aluminum chloride and 1-ethyl-3-methylimidazole chloride are configured to ionic liquid for 1.3:1 in mass ratio in the glove box of ar gas environment, as the aluminium ion battery electrolyte of the present invention.Finally ready positive pole, negative pole and electrolyte are assembled into battery in glove box.After battery installs 12 hours, between 0.5-2.15V, carry out charge-discharge test.
Embodiment 2
Use MoS2As positive active material, it is mixed with the ratio that conductive material Super-P and polyfluortetraethylene of binding element (PTFE) are 75:15:10 in mass ratio, join in dehydrated alcohol and disperse, and be shelved in the baking oven of 60 degrees Celsius after ultrasonic vibration 20-30min mix homogeneously and to be dried to gel, then gelling material is spread upon uniformly on the molybdenum sheet of 10mm × 20mm, finally wrap up as anode with GF/D diaphragm material after 60-120 degree Celsius of baking oven stands and dry for more than 12 hours.Negative pole is rafifinal, it is soaked 1-2 hour in dehydrated alcohol, and ultrasonic vibration is dried, is cut into the lamellar of 10mm × 20mm as negative pole.Anhydrous Aluminum chloride and 1-ethyl-3-methylimidazole chloride are configured to ionic liquid for 1.3:1 in mass ratio in the glove box of ar gas environment, as the aluminium ion battery electrolyte of the present invention.Finally ready positive pole, negative pole and electrolyte are assembled into battery in glove box.After battery installs 12 hours, between 0.5-2.15V, carry out charge-discharge test.
Claims (11)
1. one kind uses MoS2Aluminium ion battery for positive electrode, it is characterised in that comprise positive active material
The composite, negative pole and the aluminium ion nonaqueous solution electrolysis liquid that form with conductive material and binding agent thereof and electrolyzer
Device, wherein positive active material is MoS2, negative pole is rafifinal；Aluminium ion nonaqueous solution electrolysis liquid is by 3-
Methylimidazole. compounds is mixed in proportion with anhydrous Aluminum chloride and forms.
Use MoS the most as claimed in claim 12Aluminium ion battery for positive electrode, it is characterised in that institute
State MoS2Material is micron order that is commercially available or that prepared by chemical method and physical method or nanoscale MoS2,
Wherein chemical method includes chemical vapour deposition technique, high temperature vulcanized method, presoma decomposition method, hydro-thermal method and solution
Method；Physical method includes mechanical milling method, plasma spraying method and high-voltage arc method.
Use MoS the most as claimed in claim 12Aluminium ion battery for positive electrode, it is characterised in that institute
The binding agent stated is the one in Kynoar or politef.
Use MoS the most as claimed in claim 12Aluminium ion battery for positive electrode, it is characterised in that institute
State 3-Methylimidazole. compounds include 1-butyl-3-methylimidazolium chloride, 1-propyl group-3-Methylimidazole. villaumite,
1-ethyl-3-methylimidazole chloride, 1-butyl-3-methyl imidazolium tetrafluoroborate, 1-butyl-3-Methylimidazole. six
One or more in fluorophosphate.
Use MoS the most as claimed in claim 12Aluminium ion battery for positive electrode, it is characterised in that institute
State anhydrous Aluminum chloride and 3-Methylimidazole. compounds in the aluminium ion nonaqueous solution electrolysis liquid of aluminium ion battery
Mass ratio is 1.1:1 to 1.6:1.
Employing MoS the most according to claim 12For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, the preparation process including following:
1) by positive electrode MoS2Uniformly be fixed on the clean inert metal paillon foil collector of polishing, and with every
Membrane material wraps up, and wherein inert metal paillon foil collector is molybdenum sheet, titanium sheet, nickel foam or gold and platinum group metal；
2) it is the rafifinal of 0.2-2mm by thickness, as negative material after cleaning；
3) preparation is containing the Al that can move freely3+The nonaqueous solution electrolysis liquid of ion；
4) after getting out positive electrode, negative material and aluminium ion nonaqueous solution electrolysis liquid, at oxygen-free environment
Middle assembled battery；
5), after set of cells installs, its electrode is entirely insertable in aluminium ion nonaqueous solution electrolysis liquid, treats aluminium ion
Charge-discharge test is carried out again after the whole wetting electrode of nonaqueous solution electrolysis liquid.
Employing MoS the most according to claim 62For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, in step (1), described diaphragm material has ion permeability and does not reacts with both positive and negative polarity,
And there is stable chemical property, good mechanical performance and electrochemical stability, including microporous polyolefin film
Diaphragm material and glass fiber material.
Employing MoS the most according to claim 62For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, in step (1), MoS2Material the most uniformly mixes with conductive material, is then consolidated
Being scheduled on inert metal collector, as positive pole, wherein fixed form is for smearing, suppress and being bonding.
Employing MoS the most according to claim 62For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, in step (1), when using amorphous carbon or Super-P as conductive material, MoS2
Material usage is 50-85%, conductive material is 10-40%, binding agent is 5-10%；Using platinum slurry or silver slurry
During as conductive material, MoS2Material usage is 60-90%, conductive material is 10-40%.
Employing MoS the most according to claim 62For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, in step (2), first rafifinal is cut into lamellar, then it is put down with sand papering
Sliding, then be carried out, the method wherein cleaned is, with dehydrated alcohol or acetone soak ultrasonic vibration,
Then it is dried in 60-120 degree Celsius of baking oven.
11. employing MoS according to claim 62For the preparation method of the aluminium ion battery of positive electrode,
It is characterized in that, in step (3), containing Al3+The liquid nonaqueous solution electrolysis liquid of ion must be at glove box
In prepare, could use after then being stood more than 12 hours.
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| CN104993130A (en) * | 2015-05-25 | 2015-10-21 | 石嘴山市天和创润新材料科技有限公司 | Non-aqueous solution aluminum ion secondary battery and preparation method thereof |
| CN105016391A (en) * | 2015-07-23 | 2015-11-04 | 江苏新光环保工程有限公司 | Preparation method of three- dimensional MoS2 |
| WO2017057345A1 (en) | 2015-10-02 | 2017-04-06 | 株式会社インキュベーション・アライアンス | Positive electrode for aluminum secondary battery, and aluminum secondary battery |
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| KR102043331B1 (en) | 2016-05-17 | 2019-11-11 | 인더스트리얼 테크놀로지 리서치 인스티튜트 | Metal-ion battery |
| CN106450269B (en) * | 2016-11-11 | 2019-10-11 | 中国科学院金属研究所 | A kind of aluminium ion secondary battery positive electrode material, preparation method and applications |
| TWI611618B (en) | 2016-12-16 | 2018-01-11 | 財團法人工業技術研究院 | Metal-ion battery |
| CN107275615A (en) * | 2017-06-29 | 2017-10-20 | 厦门大学 | A kind of sulphur copper compound C-base composte material is the aluminium ion battery of positive pole |
| CN107293693B (en) * | 2017-08-18 | 2019-08-13 | 北京理工大学 | Positive electrode and preparation method thereof for aluminium-sulfur battery |
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| KR102106859B1 (en) * | 2018-08-28 | 2020-05-06 | 한국에너지기술연구원 | Aluminum secondary battery using exfoliated transition metal chalcogenide and graphene composite as cathode active material and method for manufacturing of the same |
| CN111320207B (en) * | 2018-12-14 | 2021-09-24 | 中国科学院大连化学物理研究所 | Preparation and application of molybdenum sulfide material |
| CN109742370A (en) * | 2019-01-11 | 2019-05-10 | 北京航空航天大学 | A kind of self-supporting carried by nano carbon fiber molybdenum disulfide composite material and preparation method and application |
| CN110380042B (en) * | 2019-08-08 | 2021-01-15 | 山东大学 | Anode material of aluminum secondary battery, battery and preparation method |
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| US9012072B2 (en) * | 2007-01-25 | 2015-04-21 | Bar-Ilan University | Rechargeable magnesium battery |
| CN102024996B (en) * | 2010-11-26 | 2012-12-19 | 南开大学 | High-performance rechargeable magnesium battery and manufacturing method thereof |
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