CN106099197A - All solid state metal ion battery and preparation method thereof, electric motor car - Google Patents
All solid state metal ion battery and preparation method thereof, electric motor car Download PDFInfo
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- CN106099197A CN106099197A CN201610542873.4A CN201610542873A CN106099197A CN 106099197 A CN106099197 A CN 106099197A CN 201610542873 A CN201610542873 A CN 201610542873A CN 106099197 A CN106099197 A CN 106099197A
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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
- H01M10/058—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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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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- 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
The present invention relates to the preparation method of a kind of all solid state metal ion battery, comprise the following steps: a substrate is provided；Forming at least two hierarchical element on substrate, described hierarchical element includes anode thin film, negative film and the inorganic solid electrolyte thin film being arranged between anode thin film and negative film；Hierarchical element described in superposition.The invention still further relates to a kind of at least two all solid state metal ion battery of the hierarchical element of superposition on substrate that includes, and a kind of electric motor car applying above-mentioned all solid state metal ion battery.The battery using the preparation method of described all solid state metal ion battery to prepare has that avirulence, high security, high energy storage density, battery capacity be big, charge/discharge capacity conservation rate high.
Description
[technical field]
The present invention relates to technical field of energy storage, particularly relate to a kind of all solid state metal ion battery and preparation method thereof, electricity
Motor-car.
[background technology]
Electric energy is the application form of the most universal the most most promotion prospect of clean energy resource.Energy storage technology is that energy resource structure is by passing
The key link that the fossil energy of system adjusts to the clean energy resource such as wind energy, solar energy and changes.In numerous electric energy memory technologies
In, the metal ion battery with lithium ion battery as representative is to have technology maturity and advanced preferred electric power storage skill at present concurrently
Art.
The growth requirement of metal ion battery technology be high safety, high-energy-density, high power density, long circulation life,
Low cost.Wherein, improving safety is the primary of the application form such as current power battery of electric vehicle, familial distribution of cases formula energy-storage system
Demand.Electrolyte solid state is that lithium ion battery security that is the most most potential and that be worth improves means.
The all-solid-state battery product of the solid polyelectrolyte exploitation of preparation at present is put on market in a small amount, capacity density
130-220Wh/kg.But, the heat stability of organic polymer solid electrolyte and electrochemical stability often cannot meet
The demand of complex working condition.
Inorganic solid electrolyte material technology is limited to inorganic material thick film coating critical process, it is difficult to support Large Copacity complete
The scale application of solid metallic ion battery.It is currently based on all-solid lithium-ion battery technical research, laboratory sample energy
Density is 200Wh/kg, at a temperature of 60 DEG C, after implementing the charging of 300 0.1C and the discharge cycles of 0.5C, and battery discharge
Capability retention is 80%.Although similar hull cell and the integrated preparation of microelectronic component, it is possible to resolve part microelectronic component
Energy supply problem, but its capacity constraint is in the size of battery device, therefore, it is difficult to meet power battery of electric vehicle, familial distribution of cases formula
The application demands such as energy-storage system.
[summary of the invention]
For overcoming the little technical problem of existing battery capacity, the present invention provides a kind of all solid state metal ion battery and preparation thereof
Method, electric motor car.
The present invention solves the technical scheme of technical problem and is to provide the preparation method of a kind of all solid state metal ion battery, bag
Include step S1, it is provided that a substrate；Step S2, forms at least two hierarchical element on substrate, and described hierarchical element includes positive pole
Thin film, negative film and the inorganic solid electrolyte thin film being arranged between anode thin film and negative film；And step S3, folded
Add described hierarchical element.
Preferably, described hierarchical element includes the first hierarchical element, the second hierarchical element；Described first hierarchical element includes
The anode thin film of lamination-inorganic solid electrolyte thin film-negative film successively, described second hierarchical element includes lamination successively
Negative film-inorganic solid electrolyte thin film-anode thin film.
Preferably, in step s 2, on substrate, anode collection body thin film, negative pole currect collecting body thin film are formed further；Institute
State anode collection body thin film to be arranged at anode thin film and be arranged at away from inorganic solid electrolyte film side, negative pole currect collecting body thin film
Negative film is away from inorganic solid electrolyte film side.
Preferably, in step s3, when the first hierarchical element, the second hierarchical element are disposed adjacent, at the first hierarchical element
And negative pole currect collecting body thin film or anode collection body thin film are set between the second hierarchical element.
Preferably, in step s 2, the air pressure of regulation vacuum vapor deposition is 0.2-3Pa, and holding substrate temperature is 200-
800 DEG C, on substrate, form barrier film further；
In step s3, when identical hierarchical element is disposed adjacent, described first hierarchical element is formed at the first lamination
On unit, negative pole currect collecting body thin film-barrier film-anode collection body thin film is set between hierarchical element；Or described second fold
Layer unit is formed on the second hierarchical element, arranges anode collection body thin film-barrier film-negative pole currect collecting between hierarchical element
Body thin film.
Preferably, in step s 2, the air pressure of regulation vacuum vapor deposition is 0.2-3Pa, and holding substrate temperature is 10-30
DEG C, substrate is formed anode collection body thin film；Substrate is warming up to 200-800 DEG C, sequentially forms on anode collection body thin film
Anode thin film, inorganic solid electrolyte thin film；Substrate is cooled to 10-30 DEG C, sequentially forms on inorganic solid electrolyte thin film
Negative film, negative pole currect collecting body thin film.
Preferably, described anode collection body thin film, anode thin film, inorganic solid electrolyte thin film, negative film, negative pole collection
The thickness of fluid film and barrier film is that 10 nanometers are to 2 microns；Described hierarchical element number is more than or equal to 2.
The present invention solves the technical scheme of technical problem and is to provide a kind of all solid state metal ion battery, including at least two
The hierarchical element of superposition on substrate；Described hierarchical element include anode thin film, negative film and be arranged on anode thin film with
Inorganic solid electrolyte thin film between negative film.
Preferably, described hierarchical element includes the first hierarchical element, the second hierarchical element；Described first hierarchical element includes
The anode thin film of lamination-inorganic solid electrolyte thin film-negative film successively, described second hierarchical element includes lamination successively
Negative film-inorganic solid electrolyte thin film-anode thin film.
The present invention solves the technical scheme of technical problem and is to provide all solid state metal ion cell electric vehicle of a kind of tool, its bag
Include all solid state metal ion battery as above.
Compared with prior art, a kind of all solid state metal ion battery of the present invention and preparation method thereof, electric motor car have with
Lower advantage:
(1) preparation method of all solid state metal ion battery provided by the present invention, deposits at least two hierarchical element, institute
State hierarchical element and include anode thin film, negative film and inorganic solid electrolyte thin film, and repeated deposition, form multiple lamination
Unit superposition, can arrange multiple hierarchical element in the case of cell device sizes is limited, and the energy storage improving unit volume is close
Degree, thus improve the capacity of battery, solve microelectronic component energy supply problem.
(2) described hierarchical element includes the first hierarchical element, the second hierarchical element, thus can arrange multiple superposition side
Formula, thus increase all solid state metal ion battery variety, make all solid state metal ion battery have wide applicability.
In the case of (3) first hierarchical elements, the second hierarchical element are disposed adjacent, the first hierarchical element and the second hierarchical element
Between an anode collection body thin film or negative pole currect collecting body thin film are set, in the case of cell device sizes is limited, one can be reduced
Hierarchical element takes up room, and can arrange more hierarchical element in cell device sizes one timing simultaneously, improves complete further
Solid metallic ion battery energy storage density, thus improve battery capacity.
(4) regulate air pressure and the substrate temperature of vacuum vapor deposition, can guarantee that the uniformity of vacuum vapor deposition film forming.
(5) anode collection body thin film, anode thin film, inorganic solid electrolyte thin film, negative film, negative pole currect collecting body thin film
With thickness and the number of hierarchical element superposition of barrier film, can select according to the capacity of all solid state metal ion battery
With, therefore can prepare the combination all solid state metal ion battery that laminate film thickness is different and hierarchical element number is different, because of
And substantially increase size range and the battery capacity of all solid state metal ion battery, there is wide applicability.
(6) preparation has all solid state metal ion battery of described hierarchical element superposition and has that battery capacity is big, discharge and recharge
The advantage that battery capacity conservation rate is high.
(7) electric motor car of all solid state metal ion battery with described hierarchical element superposition provided by the present invention, has
Service life length, security performance is high, charge/discharge capacity conservation rate high feature.
[accompanying drawing explanation]
Fig. 1 is that the preparation method of the present invention all solid state metal ion battery uses magnetic control sputtering device structural representation.
Fig. 2 is the detailed schematic of target position in magnetic control sputtering device shown in Fig. 1.
Fig. 3 is prepared by the preparation method of all solid state metal ion battery of the first embodiment of first embodiment of the invention
Battery device laminated construction schematic diagram.
Fig. 4 is prepared by the preparation method of all solid state metal ion battery of the second embodiment of first embodiment of the invention
Battery device laminated construction schematic diagram.
Fig. 5 is that all solid state metal ion battery structure prepared by the preparation method of the present invention all solid state metal ion battery shows
It is intended to.
[detailed description of the invention]
In order to make the purpose of the present invention, technical scheme and advantage are clearer, below in conjunction with accompanying drawing and embodiment,
The present invention is further elaborated.Should be appreciated that specific embodiment described herein only in order to explain the present invention,
It is not intended to limit the present invention.
The present invention uses vacuum vapor disposing technique to prepare all solid state metal ion battery.Vacuum vapor disposing technique includes
The technology such as sputtering, evaporation, molecular beam epitaxy, laser pulse, chemical vacuum vapour deposition.The embodiment that the present invention is more excellent has
Body can be: magnetron sputtered vacuum gas phase deposition technology.
First embodiment of the invention provides the preparation method of a kind of all solid state metal ion battery, and it includes following step
Rapid:
Step S1, material prepares；
Step S2, the preparation of hierarchical element and superposition；
And step S3, cell package.
Above-mentioned steps S1 comprise the following steps that target needed for all solid state metal ion battery is prepared in offer: plus plate current-collecting body
Target, positive pole target, inorganic solid electrolyte target, negative pole target, negative current collector target, barrier layer target.
In the present invention, in described all solid state metal ion battery, the kind of metal ion can include but not limited to lithium
One or more metal ions mixing in ion, sodium ion, potassium ion, magnesium ion or aluminium ion etc..Concrete all solid state metal
Ion battery, can include but not limited to lithium ion battery, sodium-ion battery, kalium ion battery, Magnesium ion battery or aluminium ion
The metal ion battery of one or more metal ions mixing in battery etc..Species of metal ion has multiformity, therefore expands
The scope of application of all solid state metal ion battery.
Described positive pole target, according to the kind of metal ion used, selecting can be real by the embedding of metal ion and deintercalation
The condensed state material of existing electric energy storage.Can be selected for but be just not limited to cobalt acid lithium, LiMn2O4, LiFePO4, nickel cobalt manganese, nickel cobalt aluminum etc.
The mixture of one or more in the material of pole.
Described inorganic solid electrolyte target, according to the kind of metal ion used, selection can conduct above-mentioned metal from
The inorganic solid-state ion conductor of son.Can be selected for but be not limited to following material: transition metal oxide, olivine structural oxide,
The mixture of one or more in polyanionic structure compound, quaternary system slaine etc..
Described negative pole target, according to the kind according to metal ion used, selecting can be by the embedding of metal ion and deintercalation
Realize the condensed state material of electric energy storage.Can be selected for but be not limited to following material: carbons negative material, lithium titanate, alloy type are negative
The mixture of one or more in pole material, transition metal oxide negative material etc..
The material selection good insulating of described barrier layer target, solid-state material without electro-chemical activity.
In some preferred embodiments of the present invention, when all solid state metal ion battery used is lithium ion battery, inorganic
Solid electrolyte target can be selected for but is not limited to Li7La3Ta2O13、Li7La3Zr2O13、Li7Y3Nb2O13、LiGePO4、Li-Ge-P-
S, Li-La-Ti-O quaternary system solid electrolyte or anti-perovskite structure solid electrolyte.
In some more excellent embodiments of the present invention, described barrier layer target concretely: titanium nitride, silicon nitride.
In some preferred embodiments of the present invention, when all solid state metal ion battery used is sodium-ion battery, inorganic
Solid electrolyte target can be selected for but is not limited to following material: Na-Mn-O solid electrolyte, Na-Co-O solid electrolyte, Na-
One or more mixed such as the fluorophosphate solid electrolytes such as olivine structural solid electrolyte, the Na-P-O-F such as Mn-Fe-P-O
Compound.
In some more excellent embodiments of the present invention, when all solid state metal ion battery used is lithium ion battery, described
Plus plate current-collecting body target, positive pole target, inorganic solid electrolyte target, negative pole target, negative current collector target specifically can be distinguished
For: aluminum simple substance target, LiFePO4 compound target, Li7Y3Nb2O13Solid electrolyte compound target, lithium simple substance target, copper
Simple substance target；Or molybdenum simple substance target, nickel cobalt manganese compound target, Li-La-Ti-O solid electrolyte compound target, lithium simple substance
Target and copper simple substance target.
Described plus plate current-collecting body target, positive pole target, inorganic solid electrolyte target, negative pole target, negative current collector target
Material, barrier layer target can be configured to different types of all solid state metal ion battery as required.
The preparation method of all solid state metal ion battery provided by the present invention specifically can use magnetron sputtering device 1
Carrying out the preparation of above-mentioned all solid state metal ion battery, its particular content is as described below.
Refer to Fig. 1, magnetic control sputtering device 1 of the present invention, including supporting mechanism 11, loading mechanism 13, rotating mechanism 15, crystalline substance
Governor motion (not shown) of shaking and vacuum chamber (not shown).Vacuum chamber houses supporting mechanism 11, loading mechanism 13, rotating mechanism
15, crystal oscillator governor motion.Parallel support mechanism of loading mechanism 13 11 is arranged.The corresponding supporting mechanism 11 of rotating mechanism 15 is arranged, and
Connect one end of loading mechanism 13.Crystal oscillator governor motion is used for monitoring vacuum vapor deposition film forming thickness.
Please also refer to Fig. 2, supporting mechanism 11 arranges at least one target position 111.Arrange electric power in target position 111 to supply
Answer mechanism 1111, magnetic field generation mechanisms 1113, target 1115.The corresponding target 1115 of magnetic field generation mechanisms 1113 is arranged, and electric power supplies
Mechanism 1111 is answered to connect target 1115.
Described magnetic field generation mechanisms 1113 includes multiple permanent magnet 1112.
At least one substrate 131 is fixed by described loading mechanism 13.Thin film is deposited thick on crystal oscillator governor motion monitoring substrate 131
Degree.
Close vacuum chamber, vacuum chamber is evacuated to vacuum higher than 10-4More than pa, is passed through argon as protective gas.
Loading mechanism 13 is moved away the target region completing sputtering, moves to substrate 131 corresponding to next target to be sputtered
1115 positions.Regulate supply of electric power mechanism 1111 power in target district, target 1115 place to be sputtered 111, and regulation permanent magnet
1112 distribution and density, continue spatter film forming.Repeat operation, prepare multiple material superposition thin film.
In above-mentioned steps S2 of the first detailed description of the invention of first embodiment of the invention, it is provided that a substrate 131, successively
Fixing plus plate current-collecting body target, positive pole target, inorganic solid electrolyte target, negative pole target, negative current collector target are in five
On target position 111.Described substrate 131 is fixed in loading mechanism 13 corresponding to plus plate current-collecting body target.Substrate 131 shape is with big
Little and prepared size of devices is consistent.Vacuum vapor deposition at least two the first hierarchical element.Described first hierarchical element includes
The anode thin film 102-inorganic solid electrolyte thin film 103-negative film 104 of lamination successively.Concrete acquisition the first hierarchical element
Step as follows:
Step T1, vacuum vapor deposition anode collection body thin film 101: arranging supply of electric power mechanism 1111 is DC source,
Regulation sputtering voltage is to the ignition phase of plus plate current-collecting body target.Regulation operating air pressure is to 0.2-3pa.Now substrate 131 is positioned at
Plus plate current-collecting body generated beneath, keeps the temperature of substrate 131 to be 10-30 DEG C.Start vacuum vapor deposition positive pole on substrate 131
Collector thin film 101, crystal oscillator governor motion records anode collection body thin film 101 vacuum vapor deposition thickness when being 10-2000nm,
Close DC source.Loading mechanism 13 is moved away plus plate current-collecting body target region.
Step T2, vacuum vapor deposition anode thin film 102: arranging supply of electric power mechanism 1111 is radio-frequency power supply, and regulation is spattered
Radio is depressed into the ignition phase of positive pole target.Loading mechanism 13, to 0.2-3pa, is moved to positive pole target by regulation operating air pressure
Side, now substrate 131 correspondence is positioned at positive pole generated beneath.Substrate is warming up to 200-800 DEG C, starts vacuum vapor deposition the most very thin
Film 102, crystal oscillator governor motion records anode thin film 102 vacuum vapor deposition thickness when being 10-2000nm, cuts out radio-frequency power supply.
Loading mechanism 13 is moved away positive pole target region.
Step T3, vacuum vapor deposition inorganic solid electrolyte thin film 103: supply of electric power mechanism 1111 is set for radio frequency electrical
Source, the ignition phase of regulation sputtering voltage to inorganic solid electrolyte target.Regulation operating air pressure is to 0.2-3pa, by material holder
Structure 13 moves to inorganic solid electrolyte generated beneath.Keep substrate 131 temperature 200-800 DEG C, start vacuum vapor deposition without
Machine solid electrolyte thin film 103, crystal oscillator governor motion records inorganic solid electrolyte thin film 103 vacuum vapor deposition thickness and is
During 10-2000nm, close radio-frequency power supply.Loading mechanism 13 is moved away inorganic solid electrolyte target region.
Step T4, vacuum vapor deposition negative film 104: arranging supply of electric power mechanism 1111 is DC source, and regulation is spattered
Radio is depressed into the ignition phase of negative pole target.Loading mechanism 13, to 0.2-3pa, is moved to negative pole target by regulation operating air pressure
Side, now substrate 131 correspondence is positioned at negative pole generated beneath.Substrate 131 is cooled to 10-30 DEG C, starts vacuum vapor deposition negative pole
Thin film 104, crystal oscillator governor motion records negative film 104 vacuum vapor deposition thickness when being 10-2000nm, cuts out unidirectional current
Source.Loading mechanism 13 is moved away negative pole target region.
Step T5, vacuum vapor deposition negative pole currect collecting body thin film 105: arranging supply of electric power mechanism 1111 is radio-frequency power supply,
Regulation sputtering voltage is to the ignition phase of negative current collector target.Loading mechanism 13, to 0.2-3pa, is moved by regulation operating air pressure
To negative current collector generated beneath, now substrate 131 correspondence is positioned at negative current collector generated beneath.Keep substrate 131 temperature 10-
30℃.Starting vacuum vapor deposition negative pole currect collecting body thin film 105, crystal oscillator governor motion records negative pole currect collecting body thin film 105 vacuum
When vapour deposition thickness is 10-2000nm, close radio-frequency power supply.Loading mechanism 13 is moved away negative current collector target district
Territory.
The second detailed description of the invention in first embodiment of the invention is with the difference of the first detailed description of the invention:
Five target positions 111 are fixed successively negative current collector target, negative pole target, inorganic solid electrolyte target,
Positive pole target and plus plate current-collecting body target.Vacuum vapor deposition at least one second hierarchical element successively.Described second hierarchical element
Negative film 104-inorganic solid electrolyte thin film 103-anode thin film 102 including lamination successively.
In the present invention first, second detailed description of the invention, described anode collection body thin film 101 is arranged at anode thin film
102 away from inorganic solid electrolyte thin film 103 side, and negative pole currect collecting body thin film 105 is arranged at negative film 104 away from inorganic solid
State electrolytic thin-membrane 103 side.
Repeat above-mentioned experimental procedure T1-step T5 of the present invention the first detailed description of the invention, vacuum vapor deposition at least two
Individual hierarchical element, hierarchical element described in superposition.Described hierarchical element includes the first hierarchical element and the second hierarchical element.
Step T6, vacuum vapor deposition barrier film 106: constant resistance layer target is in magnetic control sputtering device 1 target position
On 111.Arranging supply of electric power mechanism 1111 is radio-frequency power supply, the ignition phase of regulation sputtering voltage to barrier layer target.Change
Gas componant is that regulation operating air pressure is 0.2-3pa, by loading mechanism 13 containing 20% nitrogen, the mixed gas of 80% nitrogen
Mobile to barrier layer generated beneath, now substrate 131 correspondence is positioned at barrier layer generated beneath.Substrate 131 is warming up to 200-800
℃.Starting vacuum vapor deposition, it is 10-2000nm that crystal oscillator governor motion records barrier film 106 vacuum vapor deposition thickness
Time, close radio-frequency power supply.Recover only single argon shield gas, loading mechanism 13 is moved away target region, barrier layer.
The preparation method of the present invention all solid state metal ion battery some preferably in embodiment, superposition first can be combined
Hierarchical element, the second hierarchical element.Described first hierarchical element, the set-up mode of the second hierarchical element include identical lamination list
Unit is disposed adjacent and different hierarchical element is disposed adjacent.Described first hierarchical element, the second hierarchical element can combine superposition, because of
And multiple stacked system can be set, thus increase all solid state metal ion battery variety, make all solid state metal ion battery have
There is wide applicability.
The preparation method of the present invention all solid state metal ion battery some preferably in embodiment, can individually superposition identical
Hierarchical element, described identical hierarchical element is disposed adjacent.
The preparation method of the present invention all solid state metal ion battery some preferably in embodiment, superposition first can be replaced
Hierarchical element, the second hierarchical element, described different hierarchical elements are disposed adjacent.The plurality of first hierarchical element and multiple second
When hierarchical element replaces superposition, the first hierarchical element of the most adjacent superposition and the second hierarchical element, meet at negative current collector thin
Film 105 both sides are all arranged negative film 104 or all arrange anode thin film 102 in anode collection body thin film 101 both sides.Therefore at electricity
In the case of pool size is limited, space shared by a hierarchical element can be saved, can arrange more in battery size one timing simultaneously
Many hierarchical elements, thus further increase the energy storage density of the unit volume of described all solid state metal ion battery.Therefore
In the case of cell device sizes is limited, by increasing capacitance it is possible to increase battery capacity, solve microelectronic component energy supply problem.
Refer to Fig. 3, when identical hierarchical element is disposed adjacent, described first hierarchical element vacuum vapor deposition is in
On one hierarchical element, negative pole currect collecting body thin film 105-barrier film 106-anode collection body thin film is set between hierarchical element
101。
When identical hierarchical element is disposed adjacent, described second hierarchical element vacuum vapor deposition is in the second hierarchical element
On, anode collection body thin film 101-barrier film 106-negative pole currect collecting body thin film 105 is set between hierarchical element.
Refer to Fig. 4, when different hierarchical elements is disposed adjacent, described second hierarchical element vacuum vapor deposition is in
On one hierarchical element, a negative pole currect collecting body thin film 105 is set between the first hierarchical element and the second hierarchical element.
When different hierarchical elements is disposed adjacent, described first hierarchical element vacuum vapor deposition is in the second hierarchical element
On, an anode collection body thin film 101 is set between the first hierarchical element and the second hierarchical element.
When the first hierarchical element is disposed adjacent with substrate 131, at anode thin film 102 and the base of described first hierarchical element
Anode collection body thin film 101 is set between sheet 131.
When the second hierarchical element is disposed adjacent with substrate 131, at negative film 104 and the base of described second hierarchical element
Negative pole currect collecting body thin film 105 is set between sheet 131.
Preparing when completing whole hierarchical element superposition, the hierarchical element of last vacuum vapor deposition is the first hierarchical element
Time, at the negative film 104 of described first hierarchical element away from substrate 131 side vacuum vapor deposition negative pole currect collecting body thin film
105。
Preparing when completing whole hierarchical element superposition, the hierarchical element of last vacuum vapor deposition is the second hierarchical element
Time, at the anode thin film 102 of described second hierarchical element away from substrate 131 side vacuum vapor deposition anode collection body thin film
101。
In some preferred embodiments of the present invention first, second detailed description of the invention, described step T1, described step
In T4, described step T5, can be in following operating air pressure vacuum vapor deposition film forming: 0.2-0.3pa, 0.3-0.5pa, 0.35-
0.6pa, 0.5-0.6pa, 0.6-1.6pa, 1.6-1.8pa, 1.8-2pa, 2-3pa or 2.5-3pa.In the present invention, some are more excellent
Operating air pressure described in embodiment is concretely: 0.2pa, 0.25pa, 0.3pa, 0.35pa, 0.4pa, 0.45pa, 0.5pa,
0.55pa or 0.6pa.
In some preferred embodiments of the present invention first, second detailed description of the invention, described step T1, described step
In T4, described step T5, substrate 131 can be at following Temperature Vacuum vapor deposition film-formation: 10-15 DEG C, 15-20 DEG C, 20-25 DEG C
Or 25-30 DEG C.Described in some more excellent embodiments of the present invention, temperature is concretely: 10 DEG C, 15 DEG C, 20 DEG C or 25 DEG C.
In some preferred embodiments of the present invention first, second detailed description of the invention, described step T2, described step
In T3, described step T6, can be in following operating air pressure vacuum vapor deposition film forming: 0.2-0.6pa, 0.5-0.6pa, 0.6-
1.6pa, 1.6-1.8pa, 1.8-2pa, 2-3pa or 2.5-3pa.Operating air pressure described in some more excellent embodiments of the present invention
Concretely: 1pa, 1.2pa, 1.4pa, 1.5pa, 1.6pa, 1.7pa, 1.8pa, 1.9pa or 2pa.
In some preferred embodiments of the present invention first, second detailed description of the invention, described step T2, described step
In T3, described step T6, substrate 131 can be at following Temperature Vacuum vapor deposition film-formation: 200-300 DEG C, 300-500 DEG C,
500-600 DEG C or 600-800 DEG C.Described in some more excellent embodiments of the present invention, temperature is concretely: 300 DEG C, 400 DEG C,
500 DEG C, 600 DEG C, 700 DEG C or 800 DEG C.
In some preferred embodiments of the present invention first, second detailed description of the invention, in described step T1-T6, institute
State the anode collection body thin film 101 of vacuum vapor deposition, anode thin film 102, inorganic solid electrolyte thin film 103, negative film
104, negative pole currect collecting body thin film 105 and barrier film 106 thickness can be: 10-50nm, 10-100nm, 50-100nm, 80-
200nm、100-300nm、200-400nm、300-500nm、500-800nm、800-1000n m、1000-2000nm.At this
Described in brighter more excellent embodiment, thickness is concretely: 10nm, 50nm, 80nm, 100nm, 200nm, 300nm, 400nm,
500nm, 600nm, 700nm, 800nm, 900nm, 1000nm, 1200nm, 1500nm or 2000nm.
Hierarchical element number described in the present invention first, second detailed description of the invention is more than or equal to 2.The present invention first,
In some preferred embodiments of two detailed description of the invention, described hierarchical element number is 2-10,5-50,20-100,50-100,
80-150,100-200,200-400,300-500,200-500 or 500-2000.Described in some more excellent embodiments of the present invention
Hierarchical element number 10,20,50,100,150,200,300,500 or 1000.
The air pressure of described regulation vacuum vapor deposition and substrate 131 temperature, to suitable scope, can guarantee that vacuum gas-phase sinks
Amass into film uniformity.
The number of described hierarchical element, and the electrolysis of described anode collection body thin film 101, anode thin film 102, inorganic solid-state
Matter thin film 103, negative film 104, negative pole currect collecting body thin film 105 and barrier film 106 thickness can be according to all solid state metals
The capacity setting of ion battery.Therefore the combination that laminate film thickness is different and hierarchical element number is different can be prepared all solid state
Metal ion battery, thus substantially increase size range and the battery capacity of all solid state metal ion battery, have extensively
The suitability.
Refer to Fig. 5, at all solid state metal ion battery preparation method that first embodiment of the invention is provided, above-mentioned
In step S3, the preferred steps of concrete cell package is as follows:
Each anode collection body thin film 101 above-mentioned is electrically connected on the first lug 301, each plus plate current-collecting body described
Thin film 101 is parallel with one another.Each anode collection body thin film 101 described is connected with external circuit by the first lug 301, thus real
Existing each hierarchical element well turns on external circuit.
Each negative pole currect collecting body thin film 105 above-mentioned is electrically connected on the second lug 302, each negative current collector described
Thin film 105 is parallel with one another.Each negative pole currect collecting body thin film 105 described is connected with external circuit by the second lug 302, thus real
Existing each hierarchical element well turns on external circuit.
The operation such as the most sealed, shaping obtains all solid state metal ion battery.
Second embodiment of the invention provides a kind of all solid state metal ion battery, and described battery includes at least two present invention
Described in the first detailed description of the invention in first embodiment and the second detailed description of the invention on substrate 131 vacuum vapor deposition
Battery device prepared by hierarchical element superposition.The each thin film of described hierarchical element uses above-mentioned all solid state metal ion battery preparation side
Method prepares.Described hierarchical element includes the first hierarchical element, the second hierarchical element；Described first hierarchical element includes successively
The anode thin film 102-inorganic solid electrolyte thin film 103-negative film 104 of lamination, described second hierarchical element includes successively
The negative film 104-inorganic solid electrolyte thin film 103-anode thin film 102 of lamination.Described all solid state metal ion battery has
Have that avirulence, high security, high energy storage density, battery capacity be big, charge/discharge capacity conservation rate high.
In some preferred embodiments of the present invention, compared with the all-solid-state battery product of existing preparation, described employing is true
Vapor depos is prepared all solid state metal ion battery and can be improved energy storage density, charge/discharge capacity conservation rate, increase battery capacity
Deng.When all solid state metal ion battery stack unit is 50-100, all solid state metal ion battery energy storage density up to
More than 350Wh/Kg；After 1000-1500 circulation of 5C discharge and recharge, capacitance conservation rate is more than 90%；Battery capacity is up to 10Ah
Above.
Third embodiment of the invention provides the electric motor car of all solid state metal ion battery with described hierarchical element superposition,
Described electric motor car uses all solid state metal ion battery as described in second embodiment of the invention.Described electric motor car has to be made
By life-span length, the feature such as security performance is high, charge/discharge capacity holding capacity is strong.
Compared with prior art, a kind of all solid state metal ion battery of the present invention and preparation method thereof, electric motor car have with
Lower advantage:
(1) preparation method of all solid state metal ion battery provided by the present invention, deposits at least two hierarchical element, institute
State hierarchical element and include anode thin film, negative film and inorganic solid electrolyte thin film, and repeated deposition, form multiple lamination
Unit superposition, can arrange multiple hierarchical element in the case of cell device sizes is limited, and the energy storage improving unit volume is close
Degree, thus improve the capacity of battery, solve microelectronic component energy supply problem.
(2) described hierarchical element includes the first hierarchical element, the second hierarchical element, thus can arrange multiple superposition side
Formula, thus increase all solid state metal ion battery variety, make all solid state metal ion battery have wide applicability.
In the case of (3) first hierarchical elements, the second hierarchical element are disposed adjacent, the first hierarchical element and the second hierarchical element
Between an anode collection body thin film or negative pole currect collecting body thin film are set, in the case of cell device sizes is limited, one can be reduced
Hierarchical element takes up room, and can arrange more hierarchical element in cell device sizes one timing simultaneously, improves complete further
Solid metallic ion battery energy storage density, thus improve battery capacity.
(4) regulate air pressure and the substrate temperature of vacuum vapor deposition, can guarantee that the uniformity of vacuum vapor deposition film forming.
(5) anode collection body thin film, anode thin film, inorganic solid electrolyte thin film, negative film, negative pole currect collecting body thin film
With thickness and the number of hierarchical element superposition of barrier film, can select according to the capacity of all solid state metal ion battery
With, therefore can prepare the combination all solid state metal ion battery that laminate film thickness is different and hierarchical element number is different, because of
And substantially increase size range and the battery capacity of all solid state metal ion battery, there is wide applicability.
(6) preparation has all solid state metal ion battery of described hierarchical element superposition and has that battery capacity is big, discharge and recharge
The advantage that battery capacity conservation rate is high.
(7) electric motor car of all solid state metal ion battery with described hierarchical element superposition provided by the present invention, has
Service life length, security performance is high, charge/discharge capacity conservation rate high feature.
The foregoing is only present pre-ferred embodiments, not in order to limit the present invention, all principle of the present invention it
Interior made any amendment, within equivalent and improvement etc. all should comprise protection scope of the present invention.
Claims (10)
1. the preparation method of an all solid state metal ion battery, it is characterised in that: include
Step S1 a, it is provided that substrate；
Step S2, on substrate formed at least two hierarchical element, described hierarchical element include anode thin film, negative film and
The inorganic solid electrolyte thin film being arranged between anode thin film and negative film；
And step S3, hierarchical element described in superposition.
The preparation method of all solid state metal ion battery the most as claimed in claim 1, it is characterised in that: described hierarchical element bag
Include the first hierarchical element, the second hierarchical element；Described first hierarchical element includes the anode thin film-inorganic solid-state electricity of lamination successively
Solve matter thin film-negative film, described second hierarchical element include the negative film-inorganic solid electrolyte thin film of lamination successively-
Anode thin film.
The preparation method of all solid state metal ion battery the most as claimed in claim 2, it is characterised in that: in step s 2, enter
One step forms anode collection body thin film, negative pole currect collecting body thin film on substrate；Described anode collection body thin film is arranged at the most very thin
Film is away from inorganic solid electrolyte film side, and it is thin away from inorganic solid electrolyte that negative pole currect collecting body thin film is arranged at negative film
Film side.
The preparation method of all solid state metal ion battery the most as claimed in claim 3, it is characterised in that: in step s3, the
When one hierarchical element, the second hierarchical element are disposed adjacent, negative pole currect collecting is set between the first hierarchical element and the second hierarchical element
Body thin film or anode collection body thin film.
The preparation method of all solid state metal ion battery the most as claimed in claim 3, it is characterised in that: in step s 2, adjust
The air pressure of joint vacuum vapor deposition is 0.2-3Pa, keeps substrate temperature to be 200-800 DEG C, is formed further and stop on substrate
Layer film；
In step s3, when identical hierarchical element is disposed adjacent, described first hierarchical element is formed at the first hierarchical element
On, negative pole currect collecting body thin film-barrier film-anode collection body thin film is set between hierarchical element；Or described second lamination list
Unit is formed on the second hierarchical element, arranges anode collection body thin film-barrier film-negative current collector thin between hierarchical element
Film.
The preparation method of all solid state metal ion battery the most as claimed in claim 5, it is characterised in that: in step s 2, adjust
The air pressure of joint vacuum vapor deposition is 0.2-3Pa, keeps substrate temperature to be 10-30 DEG C, forms plus plate current-collecting body thin on substrate
Film；Substrate is warming up to 200-800 DEG C, sequentially forms anode thin film, inorganic solid electrolyte thin film on anode collection body thin film；
Substrate is cooled to 10-30 DEG C, sequentially forms negative film, negative pole currect collecting body thin film on inorganic solid electrolyte thin film.
The preparation method of all solid state metal ion battery the most as claimed in claim 5, it is characterised in that: described plus plate current-collecting body
The thickness of thin film, anode thin film, inorganic solid electrolyte thin film, negative film, negative pole currect collecting body thin film and barrier film is
10 nanometers are to 2 microns；Described hierarchical element number is more than or equal to 2.
8. an all solid state metal ion battery, it is characterised in that: include at least two hierarchical element of superposition on substrate；Institute
State hierarchical element and include anode thin film, negative film and the inorganic solid-state electrolysis being arranged between anode thin film and negative film
Matter thin film.
All solid state metal ion battery the most as claimed in claim 8, it is characterised in that: described hierarchical element includes the first lamination
Unit, the second hierarchical element；Described first hierarchical element include the anode thin film-inorganic solid electrolyte thin film of lamination successively-
Negative film, described second hierarchical element includes the negative film-inorganic solid electrolyte thin film-anode thin film of lamination successively.
10. have all solid state metal ion cell electric vehicle, it is characterised in that: include all solid state gold as claimed in claim 8 or 9
Belong to ion battery.
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