CN101752627B - High-energy-density metal lithium-air battery and production method thereof - Google Patents
High-energy-density metal lithium-air battery and production method thereof Download PDFInfo
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- CN101752627B CN101752627B CN2010100230274A CN201010023027A CN101752627B CN 101752627 B CN101752627 B CN 101752627B CN 2010100230274 A CN2010100230274 A CN 2010100230274A CN 201010023027 A CN201010023027 A CN 201010023027A CN 101752627 B CN101752627 B CN 101752627B
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Abstract
The invention relates to a high-energy-density metal lithium-air battery and a production method thereof. The battery consists of a metal lithium anode compound, an electrolyte chamber and an air electrode compound, wherein the metal lithium anode compound consists of a lithium source provider, a lithium iron selective conduction membrane and an elastic supporting body; the electrolyte chamber consists of an electrolyte storage chamber and a capillary microchannel; and the air electrode compound is formed by compounding an air electrode and a ventilated membrane. The metal lithium-air battery produced by the method has strong environmental adaptation. The energy density of the battery is 2 to 10 times that of the conventional lithium iron battery. The high-energy-density metal lithium-air battery is suitable for application occasions with small current and long-term work.
Description
Technical field
The present invention relates to a kind of metal lithium-air battery, particularly disclose a kind of high-energy-density metal lithium-air and preparation method thereof, belong to chemical power source and association area.
Background technology
Along with the exhaustion day by day that with the oil is the fossil fuel of representative, chemical power source more and more comes important more in the mankind's social life, and particularly the chemical cell increasing demand to high-energy-density manifests.On the one hand, electric automobile requires very high to the energy density of energy-storage battery, the chemical cell that comprises lithium ion battery, Ni-MH battery etc. at present all fully battery satisfy the durability electricity consumption requirement of electric automobile.On the other hand, move consumer electronics product, increasing like power consumptions such as game machine such as 3G mobile, notebook computer, PS3/XBOX360 and high-grade digital cameras, existing chemical cell energy storage density deficiency has been brought great inconvenience to the consumer.
(Li-Air Battery, appearance LAB) is expected to break through the technical bottleneck of chemical cell to lithium-air battery, satisfies the long-time electricity consumption requirement of following electric motor car and other electronic product.This battery is from be lithium ion battery (Li-ion Battery in essence; LiB) technology and fuel cell (Fuel Cell; FC) combination of technology; It adopts the highest lithium metal of electrochemical equivalent and is not stored in the interior air of battery system is active material, and its theoretical specific energy is the several times of Ni-MH battery and lithium-ion battery system energy density up to 11140Wh/kg.
The notion of metal lithium-air battery takes the lead in being proposed in 1996 by the breadboard K Abraham of AUS research group.J Read and P Bruce have done deep research respectively to discharge mechanism subsequently, for fast progressive the development with practicability of technology of this battery indicated direction.In March, 2009, Japan energy technology research department of industrial technology comprehensive study institute (AIST) reported the new structure metal lithium-air battery laboratory prototype of their research; In air during with the discharge of the discharge rate of 0.1A/g; But continuous discharge 20 days, discharge capacity is about 50Ah/g.In May in the same year, Britain is holy. and P professor Bruce of Andrew university announces " STAIR " metal lithium-air battery that their group succeeds in developing again, and preliminary experimental result shows that its energy density is 5-10 a times of existing lithium ion battery.
Metal current lithium-air battery technical difficulty is bigger, and disclosed patented technology is less, and (US 7147967 mainly to concentrate on US Army Lab; 55102209,5411041), U.S. Oak Ridge NationalLab (US 5314765); The PolyPlus Battery Company (US 2007011707,20070051620, and 20060078790; 20050186469,20020055039,6025094) and Japan OHARA company (US 6030909).See from disclosed situation; The encapsulation technology of battery structure design, air electrode technology of preparing, barrier film technology of preparing, function electrolyte preparation technique and battery etc. is not effectively broken through yet; The metal lithium-air battery causes countries in the world researcher's attention just day by day, is expected to become the focus and emphasis of chemical cell research of future generation.
Summary of the invention
The present invention seeks to overcome the prior art difficulty, a kind of high-energy-density metal lithium-air and preparation method thereof is provided.This battery is made up of lithium metal anode complex, electrolyte liquor chamber, air electrode complex three parts.Wherein the lithium metal anode complex provides body, lithium ion selectivity conductive membranes and elastic support to constitute by the lithium source; Electrolyte liquor chamber is made up of liquid storage room and capillary microchannel; The air electrode complex is composited by air electrode and ventilated membrane.The metal lithium-air battery environmental suitability of making thus is strong, and its energy density is that existing lithium ion battery has 2-10 doubly, the application scenario that be fit to little electric current, works long hours.
Technical scheme of the present invention is: the active component of lithium anode complex is made up of lithium, and concrete physical configuration can be band shape, sheet, paper tinsel shape, bar-shaped, column and granular etc.It is to contact with the physics of slider in order to ensure lithium anode that elastic support is set.One or several constitute elastic support by nickel plating stainless steel, carbon spring steel, low manganese spring steel, silicon-manganese spring steel and chrome-vanadium steel etc.Lithium ion selectivity conductive membranes has the lithium ion conduction selectivity, and air molecule and hydrone can not penetrate, and can be LISICON film, LIPON film, Li
3The N film, or other has the inoranic membrane or the organic membrane of lithium ion conduction function through modification.Its main material is glass-ceramic material (GC), polymer-ceramic material (PC), LiPON and Li
3N etc. can be made by methods such as magnetron sputtering (MS) or chemical vapor deposition (CVD)s.Lithium ion conduction selective membrane thickness is 50-300 μ m.Electrolyte liquor chamber is made up of liquid storage room and capillary microchannel; The top of electrolyte liquor chamber or bottom are capillary channel; Capillary channel is of a size of 1-50 μ m; It is through MEMS (Micro Electro Mechanical System, MEMS) technology, laser ablation/engraving technology, mold or other machinery production fabrication techniques form, the basis material of electrolyte liquor chamber (or claim slider) is one or more in silicon, SOI silicon, pottery, polymethyl methacrylate, polytetrafluoroethylene, epoxy, Merlon, polyurethane, polyvinyl alcohol, polyvinyl chloride, the polyphenyl rubber; Wherein, the Main Ingredients and Appearance of silicon substrate surface electronic isolation property layer is SiO
2And Si
3N
4As when adopting insulating material such as pottery, polymethyl methacrylate, PTFE to be made into electrolyte liquor chamber then the surface need not make insulating barrier.The air electrode complex is composited by ventilated membrane and air electrode, and ventilated membrane waits one or more formations by polytetrafluoroethylene (PTFE), polyethylene (PE), polypropylene (PP), thermoplastic elastic rubber (TPU); Air electrode can be made by traditional fuel battery air method for making its electrode, also can be through the MEMS technology, and the combined with electrochemical fabrication techniques forms the composite air electrode in individual layer air electrode or double-deck different apertures; Wherein, catalyst can be Pt, Pt-Ru, Pd, PdCo, MnO
2, Co
3O
4, Fe
3O
4And Fe
2O
3Wait one or more, can be carbon and carry (Carbon Carried) or carbon-free year form.The above-mentioned parts that are made are encapsulated, can make the described high-energy-density metal lithium-air of Fig. 1 of the present invention.
Described electrolyte is for containing hexafluoroarsenate lithium (LiAsF
6), lithium hexafluoro phosphate (LiPF
6), trifluoromethyl sulfonic acid lithium (CF
3SO
3Li) lithium perchlorate (LiClO
4), LiBF4 (LiBF
4), one or more mixing of di-oxalate lithium borate (LiBOB), lithium hydroxide (LiOH), lithium chloride supporting electrolytes such as (LiCl), concentration is 0.1-3.0M.Organic solvent is one or more mixing of acetonitrile (AN), propene carbonate (PC), diethyl carbonate (DEC), methyl ethyl carbonate alkene ester (EMC), dimethyl carbonate (DMC), ethylene carbonate (EC), dimethoxy-ethane (DME), butyrolactone (GBL).Electrolyte liquid can contain functional additive, is typically chlorous acid (SOCl
2), sulfur dioxide (SO
2), carbon dioxide (CO
2), in vinylene carbonate (VC), propylene sulfite (PS), ethylene sulfite (ES), diethyl sulfite (DES) and the dimethyl sulfite (DMS) one or more.
In a word, high-energy-density metal lithium-air manufacture method provided by the invention is characterised in that uses the MEMS method to produce three parts earlier, then three component packages is formed.
Concrete manufacture method comprises:
A, electrolyte liquor chamber are made
1) with the basis material of electrolyte liquor chamber, produces electrolyte liquor chamber through MEMS dry method wet processing, and pour into electrolyte;
2) adopt MEMS technology, laser/engraving process, one or more methods in mold or the Machining Technology are produced the capillary microchannel respectively in the top and the bottom of the electrolyte that step 1) is made;
B, lithium metal anode complex are made
1) in the square frame body of the rectangle sky of the formation of the silicon on silicon or SOI elastic support is set earlier;
2) on elastic support, placing the active lithium source provides body to adopt magnetron sputtering or chemical gaseous phase depositing process to provide the body upper surface to make lithium ion selectivity conductive membranes in the active lithium source then;
The making of C, air electrode complex
1) air electrode is by the manufacture method of existing fuel battery air electrode or through the MEMS technology, the combined with electrochemical fabrication techniques forms the composite air electrode in individual layer air electrode or double-deck different apertures;
2) on the air electrode that step 1) is made, prepare ventilated membrane, described ventilated membrane is by one or more compound breath films formed in polytetrafluoroethylene, polyethylene, polypropylene, the thermoplastic elastic material;
D, the complex bonding that steps A, B, C are made.
With respect to disclosed patented technology, benefit of the present invention is: (1) has increased substantially the integrated level that battery is made, and has significantly reduced nonactive parts proportion in entire cell, thereby has effectively improved the energy density of battery; (2) strengthened the adaptability of battery, prolonged the useful life of battery in varying environment; (3) energy density of metal lithium-air battery provided by the invention is 300-700wh/kg, with the battery specific capacity of carbon metering up to 1000-2500mAh/g.
Description of drawings
Fig. 1 is a high-energy-density metal lithium-air structural representation provided by the invention.
Wherein, 1. lithium anode complex; 2. air electrode complex; 3. electrolyte liquor chamber; 11. lithium ion selectivity conductive membranes; 12. the lithium metal source provides body; 13. elastic support; 14. the square frame of silica-based sky; 21. ventilated membrane; 31. capillary microchannel; 32. liquid storage room.
Embodiment
With the silicon chip is base material, produces electrolyte liquor chamber 3 through the classical wet method/dry process of MEMS, and its top and bottom are capillary microchannel 31, and the centre is a liquid storage room 32.Electrolyte liquor chamber 32 top layers make it have electronic isolation property through MEMS heat treatment and nitrogen treatment, and the Main Ingredients and Appearance of its insulating barrier is SiO
2And Si
3N
4Effective electrolyte capacity of liquid storage room is 400 μ l, and wherein the capillary microchannel is of a size of 8 μ m.It is the source of the lithium sheet 12 of 2mm as lithium ion that the lithium metal anode complex adopts thickness, and the surface is with the LIPON film 11 of the about 120nm of magnetically controlled sputter method sputter.Above-mentioned parts are made physics by nickel plating stainless steel elastic support 13 and are supported, so that keep the lithium metal source to provide body lithium sheet to contact with the effective of capillary microchannel in the battery discharge procedure.Described lithium metal anode complex 1 is in the empty square frame body 14 of the rectangle of the silicon formation on silicon or SOI.Air electrode complex 2 adopts electrolysis MnO
2Air electrode and the PTFE/PE compound breath film 21 of making catalyst constitute.The effective area of the battery of made is 2cm
2, electrolyte is SO
2The 1M LiPF that handles
6/ PC organic solution.Under normal temperature, different air humidity conditions, with 0.1mA/cm
2Discharge, the battery specific capacity of measuring with carbon can reach more than the 1600mAh/g, and energy density is greater than 300Wh/kg.
Other condition only changes the manufacture method of air electrode with embodiment 1.The employing porous silicon is a base material, produces the air electrode that contains micro channel through MEMS porous silicon technology of preparing and electrochemical method.Battery is under normal temperature, different air humidity conditions, with 0.2mA/cm
2Discharge, the battery specific capacity of measuring with carbon can reach more than the 1800mAh/g, and energy density is greater than 350Wh/kg.
Other condition only substitutes the LIPON film with the LISICON film with embodiment 1.Battery is under normal temperature, different air humidity conditions, with 0.2mA/cm
2Discharge, the battery specific capacity of measuring with carbon can reach more than the 2200mAh/g, and energy density is greater than 400Wh/kg.
Embodiment 4
Other condition only changes the manufacture method of air electrode body with embodiment 1.Air electrode adopts traditional fuel battery air electrode, and catalyst uses Pt, Pt-Ru, Pd, PdCo, Co respectively
3O
4, Fe
3O
4And Fe
2O
3In one or more, can be carbon and carry (Carbon Carried) or carbon-free year form.Adopt the MEMS dry process to make the composite air electrode in double-deck different apertures.Battery is under normal temperature, different air humidity conditions, with 0.1mA/cm
2Discharge, the battery specific capacity of measuring with carbon is 1000-2400mAh/g, energy density is 280-600Wh/kg.
Need to prove, the invention is not restricted to the foregoing description, anyly be equal to or replace all in rights protection scope of the present invention of the present invention.
Claims (10)
1. high-energy-density metal lithium-air; It is characterized in that described battery is made up of lithium metal anode complex (1), electrolyte liquor chamber (3), air electrode complex (2) three parts successively, and electrolyte liquor chamber and lithium metal anode complex and air electrode complex electric insulation; Wherein, the lithium metal anode complex selects conductive membranes, lithium metal source to provide body and elastic support to constitute by lithium ion successively; Electrolyte liquor chamber is made up of liquid storage room and capillary microchannel, and the capillary microchannel is positioned at the top and the bottom of electrolyte liquor chamber, and the centre is a liquid storage room; The air electrode complex is composited by air electrode and ventilated membrane.
2. by the described high-energy-density metal lithium-air of claim 1, it is characterized in that:
1. the lithium metal source provides the physical configuration of body to be band shape, sheet, paper tinsel shape, bar-shaped, column or granular in the described lithium metal anode complex;
2. described lithium ion selectivity conductive membranes is LiPON film, LiSiCON film, Li
3N film or other have the inorganic or organic membrane of lithium ion conduction function through modification;
3. described elastic support is to be made up of any in nickel plating stainless steel, carbon spring steel, low manganese spring steel, silicon-manganese spring steel and the chrome-vanadium steel or several kinds;
4. described lithium metal anode complex is in the empty square frame body of the rectangle of the silicon chip formation on silicon or SOI.
3. by the described high-energy-density metal lithium-air of claim 1, the basis material that it is characterized in that described electrolyte liquor chamber is one or more in silicon, SOI silicon, pottery, polymethyl methacrylate, polytetrafluoroethylene, Merlon, polyurethane, polyvinyl alcohol, polyvinyl chloride, the polyphenyl rubber.
4. by the described high-energy-density metal lithium-air of claim 1, it is characterized in that the Main Ingredients and Appearance of the silicon substrate surface electronic isolation property layer on silicon or the SOI is SiO
2Or Si
3N
4, through it and lithium metal anode complex and the insulation of air electrode complex.
5. by the described high-energy-density metal lithium-air of claim 1, it is characterized in that the top of electrolyte liquor chamber and the capillary microchannel of bottom are of a size of 1-50 μ m.
6. by each described high-energy-density metal lithium-air among the claim 1-5, the energy density that it is characterized in that described metal lithium-air battery is 300-700wh/kg, and the battery specific capacity of measuring with carbon is 1000-2500mAh/g.
7. make method, it is characterized in that using the MEMS method to produce three parts earlier, then three component packages are formed like each described high-energy-density metal lithium-air among the claim 1-5.
8. by the manufacture method of the described high-energy-density metal lithium-air of claim 7, it is characterized in that comprising:
A, electrolyte liquor chamber are made
1) with the basis material of electrolyte liquor chamber, produces electrolyte liquor chamber through MEMS dry method wet processing, and pour into electrolyte;
2) adopt MEMS technology, laser ablation/engraving process, one or more methods in mold or the Machining Technology are produced the capillary microchannel respectively in the top and the bottom of the electrolyte liquor chamber that step 1) is made;
B, lithium metal anode complex are made
1) in the square frame body of the rectangle sky of the formation of the silicon on silicon or SOI elastic support is set earlier;
2) on elastic support, place the active lithium source body is provided, adopt magnetron sputtering or chemical gaseous phase depositing process to provide the body upper surface to make lithium ion selectivity conductive membranes in the active lithium source then;
The making of C, air electrode complex
1) air electrode is by the manufacture method of existing fuel battery air electrode or through the MEMS technology, the combined with electrochemical fabrication techniques forms the composite air electrode in individual layer air electrode or double-deck different apertures;
2) on the air electrode that step 1) is made, prepare ventilated membrane, described ventilated membrane is by one or more compound breath films formed in polytetrafluoroethylene, polyethylene, polypropylene, the thermoplastic elastic material;
D, the complex bonding that steps A, B, C are made.
9. by the manufacture method of the described high-energy-density metal lithium-air of claim 8, it is characterized in that:
The catalyst that uses when 1. making air electrode is Pt, Pt-Ru, Pd, PdCo, Co
3O
4, Fe
3O
4, MnO
2Or Fe
2O
3In any or several kinds;
2. catalyst is that carbon carries or carbon-free year form;
3. described air electrode is the air electrode that contains micro channel.
10. by the manufacture method of the described high-energy-density metal lithium-air of claim 8, it is characterized in that:
1. the electrolyte of described electrolyte liquor chamber is for containing hexafluoroarsenate lithium, lithium hexafluoro phosphate, trifluoromethyl sulfonic acid lithium or several kinds of mixing, and concentration is 0.1-3.0M;
2. the organic solvent of electrolyte is one or more the mixing in acetonitrile, propene carbonate, diethyl carbonate, methyl ethyl carbonate alkene ester, dimethyl carbonate, ethylene carbonate, dimethoxy-ethane, the butyrolactone;
3. electrolyte is one or more functional additives that contain in sulfur dioxide, carbon dioxide, vinylene carbonate, propylene sulfite, ethylene sulfite, diethyl sulfite and the dimethyl sulfite.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107634231A (en) * | 2017-09-07 | 2018-01-26 | 厦门大学 | The preparation method of one proton exchanging film fuel battery |
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|---|---|---|---|---|
| CN102034985B (en) * | 2010-11-15 | 2013-06-19 | 中国科学院青岛生物能源与过程研究所 | Oxygen electrode of lithium air battery as well as preparation method and application thereof |
| CN103579715A (en) * | 2012-07-31 | 2014-02-12 | 中国科学院上海微系统与信息技术研究所 | Button lithium air battery capable of working in air |
| RU2578196C2 (en) * | 2012-09-28 | 2016-03-27 | Общество с ограниченной ответственностью "ФМ Лаб" | Lithium-air accumulator and preparation method thereof |
| JP6155864B2 (en) * | 2013-06-07 | 2017-07-05 | スズキ株式会社 | Positive electrode structure of lithium air battery and positive electrode manufacturing method |
| CN103647089A (en) * | 2013-12-19 | 2014-03-19 | 济南开发区星火科学技术研究院 | Oxyhydrogen alkaline fuel cell |
| CN109075413B (en) * | 2016-04-25 | 2021-05-07 | 铃木株式会社 | Negative electrode composite structure of lithium air battery |
| CN107146926A (en) * | 2017-05-22 | 2017-09-08 | 深圳市航盛新材料技术有限公司 | The quick-replaceable negative pole end of air cell and air cell |
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Cited By (2)
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| CN107634231A (en) * | 2017-09-07 | 2018-01-26 | 厦门大学 | The preparation method of one proton exchanging film fuel battery |
| CN107634231B (en) * | 2017-09-07 | 2020-11-27 | 厦门大学 | Preparation method of proton exchange membrane fuel cell |
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