CN101640269A - Material for lithium-ion secondary battery cathode, cathode pole piece and lithium-ion secondary battery - Google Patents
Material for lithium-ion secondary battery cathode, cathode pole piece and lithium-ion secondary battery Download PDFInfo
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- CN101640269A CN101640269A CN200810117583A CN200810117583A CN101640269A CN 101640269 A CN101640269 A CN 101640269A CN 200810117583 A CN200810117583 A CN 200810117583A CN 200810117583 A CN200810117583 A CN 200810117583A CN 101640269 A CN101640269 A CN 101640269A
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- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses a material used for a lithium-ion secondary battery cathode, which comprises active material silicon or tin. The active material is also doped with carbon element and hydrogenelement. The material used for the lithium-ion secondary battery cathode has the advantages that a cathode pole piece prepared by the cathode material provided by the invention has extremely high volume ratio capacity and excellent cycle performance, and also has high-magnification charge/discharge capacity. Batteries prepared by the pole piece can be widely applied in the fields of electric tools, electric automobiles, energy storage equipment and the like, and have good market prospect.
Description
Technical field
The present invention relates to lithium rechargeable battery, particularly can be used for making the material of lithium ion secondary battery negative pole and contain the cathode pole piece of this material with high-rate charge-discharge capability, and the lithium rechargeable battery that uses this cathode pole piece.
Background technology
Since the beginning of the nineties, Japan Sony Corporation succeeded in developing lithium rechargeable battery, as battery of new generation, lithium rechargeable battery had been obtained swift and violent development, is widely used in a plurality of fields such as civilian and military.Recently, along with the size and the weight of portable electric appts constantly reduces, and the development of electric automobile, space flight and energy storage device, require lithium battery to have higher capacity density, power density and fail safe.Especially the field of attracting attention for this whole world of electric automobile, improving large current discharging capability will be the key of the comprehensive commercial applications of lithium rechargeable battery.The negative material that uses in the lithium battery mainly is a material with carbon element at present, yet the current potential of carbon negative pole and lithium metal are approaching, and big electric current may cause electrode surface to form Li dendrite, has very big potential safety hazard.The theoretical capacity of material with carbon element has only 372mAh/g in addition, and capacity and cycle performance all descend very soon during high-multiplying power discharge, can't satisfy the practical requirement to lithium secondary battery of electric automobile, electric tool.
Defective for material with carbon element, but patent CN200410066489.9 discloses electrode composite material of a kind of high power charging-discharging and preparation method thereof, be characterised in that this composite material constitutes by possessing otide containing lighium thing and the argent that lithium ion takes off the embedding ability, wherein argent is dispersed on the material crystal boundary mutually as second, has played the conductive agent effect.And patent CN200510026685.8 discloses a kind of based on the second mutually compound high multiplying power lithium ion secondary battery cathode material, is characterised in that with the lithium titanate to be matrix, and the oxide of introducing metallic copper or copper can carry out the high power charging-discharging circulation as second phase.But the electrode material of oxide system all is the electronics non-conductor usually, even add second phase material as conductive agent, can not tackle the problem at its root.The theoretical capacity of oxide material lithium titanate own has only 175mAh/g in addition, and discharge capacity is lower under the big electric current, can't satisfy the requirement of lithium battery height ratio capacity.
Summary of the invention
Therefore, task of the present invention is the defective that overcomes prior art, thereby a kind of material that is used to make lithium ion secondary electrode cathode pole piece is provided.
Another task of the present invention provides a kind of cathode pole piece that uses above-mentioned material to make.
Another task of the present invention provides a kind of lithium rechargeable battery that uses above-mentioned cathode pole piece.
On the one hand, the invention provides a kind of material that is used for lithium ion secondary battery negative pole, comprise active material silicon or tin, also be doped with carbon and protium in this active material.
In the above-mentioned material, described two kinds of doped chemicals are uniformly distributed in the described active material, and the atomic ratio of active material and carbon preferred 10: 1-100: 1, and the atomic ratio of active material and protium preferred 50: 1-100: 1.
In the above-mentioned material, described active material preferably exists with the form of film.
In the above-mentioned material, the structure optimization nano microcrystalline structure or the non crystalline structure of described active material.
In the above-mentioned material, the preferred 1-20 μ of the thickness of described active material m.
In the above-mentioned material, also preferably be doped with in aluminium, boron, iron, copper and the silver element one or more in the described active material.
On the other hand, the present invention also provides a kind of cathode pole piece, comprises above-mentioned negative material, carries the collector of this negative material and covers the lip-deep resilient coating of described negative material.
In the above-mentioned cathode pole piece, the preferred carbon of described cushioning layer material, aluminium, boron, iron, copper or silver element, the preferred 10-500nm of described buffer layer thickness.
Another aspect, the present invention also provides a kind of lithium rechargeable battery, comprises above-mentioned cathode pole piece, also comprise anode pole piece and be located at anode pole piece and cathode pole piece between be used to transmit the electrolyte of lithium ion.
The invention has the advantages that and utilize the cathode pole piece of negative material preparation provided by the invention to possess high volume and capacity ratio, excellent cycle performance possesses high power charging-discharging ability simultaneously.Utilize the battery of this pole piece preparation can be widely used in fields such as electric tool, electric automobile and energy storage device, have market prospects preferably.
Description of drawings
Below, describe embodiments of the invention in conjunction with the accompanying drawings in detail, wherein:
Fig. 1 is the active material layer for preparing and the cathode pole piece of lithium ion secondary battery cross sectional representation of resilient coating on collector.
Fig. 2 is the XRD figure of the negative active core-shell material of embodiment 1 preparation.
Fig. 3 is the electrochemical properties resolution chart of corresponding cathode pole piece among the embodiment 1 in the embodiment of the present invention.
Fig. 4 is a cathode pole piece cycle performance curve chart corresponding among the embodiment 1.
Fig. 5 is the electrochemical properties resolution chart of corresponding cathode pole piece among the embodiment 2 in the embodiment of the present invention.
Fig. 6 is the electrochemical properties resolution chart of corresponding cathode pole piece among the embodiment 3 in the embodiment of the present invention.
Fig. 7 is a cathode pole piece cycle performance curve chart corresponding among the embodiment 5.
Embodiment
Cathode pole piece structure of the present invention and manufacture method are as follows: the active material layer 2 and the resilient coating 5 (preferred thickness 10-500nm) that deposit certain thickness (preferred 1-20 μ m) on the collector of making such as metals such as copper 1 by magnetron sputtering successively, as shown in Figure 1, described active material is for embedding active material silicon or the tin with the removal lithium embedded ion, and also be doped with carbon 4 and protium 3 in this active material layer 2, these two kinds of doped chemicals preferably are uniformly distributed in the described active material layer 2, and the atomic ratio of active material and carbon is 10: 1-100: 1, and the atomic ratio of active material and protium is 50: 1-100: 1.
Now, with reference to embodiment technical scheme of the present invention is described further.
Prepare cathode pole piece according to following steps:
At first prepare active material layer: utilize magnetically controlled DC sputtering, piecing together target (silicon-carbon target ratio is 1: 1) with high-purity silicon-carbon is sputtering source, and sputtering power is 500W, at thickness is to deposit active material layer on the copper collector of 15 μ m, and thickness is 3 μ m.Working gas is argon gas and hydrogen, and wherein argon flow amount is 58sccm, and hydrogen flowing quantity is 10sccm, and operating air pressure remains on 0.1Pa.
Prepare resilient coating then: with the high purity graphite target is sputtering source, and sputtering power is 800W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 5 * 10
-1Pa.
The XRD of resulting negative material as shown in Figure 2, therefore the diffraction maximum that marks among the figure is the characteristic peak of collector copper, illustrates that active material is nano microcrystalline structure or non crystalline structure.
The cathode pole piece that above-mentioned preparation process obtains is measured, can be obtained that the atomic ratio of silicon and carbon is 10: 1 in the active material, the atomic ratio of silicon and hydrogen is 50: 1.
Resulting cathode pole piece and metal Li composition button half-cell are carried out electrochemical property test, and the discharging current multiplying power is 0.5C-10C, and the charging/discharging voltage scope is at 0～2.0V.Test result is as shown in table 1:
Table 1
| Discharge-rate | ??0.5C | ??1C | ??1.5C | ??2.5C | ??5C | ??10C | ??1C |
| Discharge capacity (mAh/g) | ??1076 | ??1042 | ??1028 | ??1071 | ??1073 | ??1072 | ??1123 |
Can see that the discharge capacity of the cell of present embodiment is bigger from table, under the discharging current multiplying power of 0.5C-10C, significant change does not take place all the time greater than 1000mAh/g in discharge capacity, demonstrates very superior multiplying power discharging property.After discharging current was reduced to 1C, discharge capacity slightly increased, and was 1123mAh/g.
The charge discharge curve of half-cell as shown in Figure 3, the discharge platform of material and traditional negative material graphite are approaching, plateau potential is between 0.1V-0.4V, voltage platform is more smooth.Along with the increase of discharging current, plateau potential does not almost change.The electrochemistry cycle performance as shown in Figure 4, test result shows, even under the 10C discharging current, the capacity of battery is not obviously decay also, demonstrates very superior multiplying power discharging property.
Prepare cathode pole piece according to following steps:
At first, the preparation active material layer: utilizing magnetically controlled DC sputtering, is sputtering source with high-purity silicon target, and sputtering power is 500W, is to deposit active material layer on the copper collector of 15 μ m at thickness, and thickness is 3 μ m.Working gas is acetylene and hydrogen, and wherein the acetylene flow is 10sccm, and hydrogen flowing quantity is 20sccm, and operating air pressure remains on 8 * 10
-1Pa.
Then, preparation resilient coating: with the high purity graphite target is sputtering source, and sputtering power is 800W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 5 * 10
-1Pa.
The cathode pole piece that above-mentioned preparation process obtains is measured, can be obtained that the atomic ratio of silicon and carbon is 20: 1 in the active material, the atomic ratio of silicon and hydrogen is 60: 1.
The positive electrode pole piece that lithium ion battery uses in the embodiment of the invention can prepare according to following method: utilize solvent such as N-first class-2-Pyrrolidone (NMP), disperse the mixture LiMO of composite oxides
2(wherein M is at least a transition metal) is as LixCoO
2, LixNiO
2, LiMn
2O
4, LixMnO
3Deng, use electric conducting material such as carbon black and binding agent such as Kynoar (PVDF) simultaneously, adopt the mixture that forms to apply such as above the aluminum foil current collector.
The method step of conventional manufacturing lithium ion battery is as follows:
In the air ambient or inert gas environment of drying, lamination cathode pole piece and anode pole piece are placed how empty film as barrier film between cathode pole piece and anode pole piece.Many empty films can be by polyolefin, for example polypropylene or polyethylene etc.With negative pole, barrier film, anodal laminated construction, be placed in the battery container.The electrolyte that is fit to comprises the lithium salts that is dissolved in the solvent, and solvent comprises polypropylene carbonate fat, ethylene carbonate, butylene carbonate etc.And can utilize solid polymer electrolyte to replace above-mentioned liquid electrolyte.Electrolyte also can be for gel state.
Present embodiment is assembled into battery in the mode of lamination equally, changes into aluminum plastic film encapsulation and fluid injection.Can change pole piece size and lamination sheet number as requested, obtain the polymer lithium ion secondary battery of different rated capacities.
When positive plate is of a size of 100 * 60mm, when the anodal lamination number of plies was 6 layers, the gained battery carried out the discharge performance test, and the discharging current multiplying power is 0.25-5C, and charging/discharging voltage is 3-4.2V, and test result is as shown in table 2.
Table 2
| Discharge-rate | ??0.25C | ??0.5C | ??1C | ??2C | ??3C | ??5C |
| Discharge capacity (mAh) | ??746 | ??729 | ??702 | ??669 | ??644 | ??587 |
When as seen, the discharge capacity of the lithium rechargeable battery of present embodiment when 3C reaches 0.5C 88.3%; When the discharge capacity during 5C reaches 0.5C 80.5%, charging and discharging curve as shown in Figure 5, along with discharging current increases, plateau potential decreases, discharge capacity remains on more than 80%.
Prepare cathode pole piece according to following steps:
At first, the preparation active material layer: utilize magnetically controlled DC sputtering, piecing together target (ratio of sial target is 10: 1) with high-purity sial is sputtering source, and sputtering power is 500W, at thickness is to deposit active material layer on the copper collector of 15 μ m, and thickness is 3 μ m.Working gas is acetylene and hydrogen, and wherein the acetylene flow is 10sccm, and hydrogen flowing quantity is 20sccm, and operating air pressure remains on 8 * 10
-1Pa.
Then, preparation resilient coating: with the high purity graphite target is sputtering source, and sputtering power is 800W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 3Pa.
The cathode pole piece that above-mentioned preparation process obtains is measured, can be obtained that the atomic ratio of silicon and aluminium is 5: 1 in the active material, the atomic ratio of silicon and carbon is 40: 1, and the atomic ratio of silicon and hydrogen is 70: 1.
The positive electrode pole piece that lithium ion battery uses in the embodiment of the invention is identical with embodiment 2 with the preparation method of lithium ion battery.
When positive plate is of a size of 100 * 60mm, when the anodal lamination number of plies was 4 layers, the gained battery carried out the discharge performance test, and the charging current multiplying power is 0.25-5C, and charging/discharging voltage is 3-4.2V, and test result is as shown in table 3.
Table 3
| Discharge-rate | ??0.5C | ??1C | ??2C | ??5C | ??10C | ??15C |
| Charging capacity (mAh) | ??369.2 | ??345 | ??366 | ??345 | ??309 | ??288 |
As known from Table 3, record battery when the 5C charging capacity reaches 0.5C 93.4%; When the 10C charging capacity reaches 0.5C 83.7%, 78% when the 15C charging capacity reaches 0.5C, charging and discharging curve as shown in Figure 6, along with charging current increases, the charging voltage platform increases to some extent, the corresponding reduction of charging capacity.
Use sial to piece together target in the present embodiment, a certain amount of aluminium that in negative material, mixed, those skilled in the art should be appreciated that and can also use various doped chemicals commonly used, as in boron, iron, copper and/or the silver element one or more.
Comparative example 1
Prepare cathode pole piece according to technical process among the embodiment 1 and condition, sputtering source is used pure silicon target instead, and active material does not add any doped chemical in the preparation process.
At first prepare active material layer: utilizing magnetically controlled DC sputtering, is sputtering source with high-purity silicon target, and sputtering power is 500W, at thickness is to deposit active material layer on the copper collector of 15 μ m, and thickness is 3 μ m.Working gas is an argon gas, and wherein argon flow amount is 58sccm, and operating air pressure remains on 0.1Pa.
Prepare resilient coating then: with the high purity graphite target is sputtering source, and sputtering power is 800W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 5 * 10
-1Pa.
Resulting cathode pole piece and metal Li composition button half-cell are carried out electrochemical property test, and the discharging current multiplying power is 0.5C-10C, and the charging/discharging voltage scope is at 0～2.0V.The material property of preparation is compared as follows among the test result of gained and the embodiment 1.
Table 4
| Discharge-rate | ??0.5C | ??1C | ??1.5C | ??2.5C | ??5C | ??10C | ?? |
| Embodiment | |||||||
| 1 | ??1076 | ??1042 | ??1028 | ??1071 | ??1073 | ??1072 | ??1123 |
| Middle material discharging capacity (mAh/g) | |||||||
| Material discharging capacity (mAh/g) in the comparative example 1 | ??1500 | ??1320 | ??1214 | ??1031 | ??983 | ??792 | ??1438 |
From table comparative result as can be seen, though the pure silicon sample of preparation possesses higher discharge capacity in the comparative example 1, along with discharging current increases, the decline of the capacity of material is very fast.When discharging current was 10C, 52.8% when discharge capacity has only 0.5C was far below the cathode pole piece of embodiment 1 preparation.Yi Qian experimental result shows in addition, and the pure silicon material can't suppress volumetric expansion, and cycle performance is also very poor.
Embodiment 4
Prepare cathode pole piece according to following steps:
At first prepare active material layer: utilize magnetically controlled DC sputtering, piecing together target (tin carbon target ratio is 2: 1) with high purity tin carbon is sputtering source, and sputtering power is 500W, at thickness is to deposit active material layer on the copper collector of 15 μ m, and thickness is 3 μ m.Working gas is argon gas and hydrogen, and wherein argon flow amount is 58sccm, and hydrogen flowing quantity is 10sccm, and operating air pressure remains on 7Pa.
Prepare resilient coating then: with the high purity graphite target is sputtering source, and sputtering power is 800W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 5 * 10
-1Pa.
The cathode pole piece that above-mentioned preparation process obtains is measured, can be obtained that the atomic ratio of tin and carbon is 60: 1 in the active material, the atomic ratio of tin and hydrogen is 80: 1.
Resulting cathode pole piece and metal Li composition button half-cell are carried out electrochemical property test, and the discharging current multiplying power is 0.5C-10C, and the charging/discharging voltage scope is at 0～2.0V.Test result is as shown in table 1:
Table 5
| Discharge-rate | ??0.5C | ??1C | ??1.5C | ??2.5C | ??5C | ??10C | ??1C |
| Discharge capacity (mAh/g) | ??783 | ??742 | ??728 | ??681 | ??673 | ??652 | ??739 |
Can see that the discharge capacity of the cell of present embodiment is more lower slightly than silicon-based anode battery from table, under the discharging current multiplying power of 10C, discharge capacity remains on 652mAh/g, is 83% of 0.2C discharge capacity, demonstrates comparatively superior multiplying power discharging property.After discharging current was reduced to 1C, discharge capacity returned to 739mAh/g.
Prepare cathode pole piece according to following steps:
At first prepare active material layer: utilize magnetically controlled DC sputtering, piecing together target (silicon-carbon target ratio is 1: 1) with high-purity silicon-carbon is sputtering source, and sputtering power is 500W, at thickness is to deposit active material layer on the copper collector of 15 μ m, and thickness is 3 μ m.Working gas is argon gas and hydrogen, and wherein argon flow amount is 58sccm, and hydrogen flowing quantity is 10sccm, and operating air pressure remains on 9Pa.
Prepare resilient coating then: with the rafifinal target is sputtering source, and sputtering power is 300W, deposits resilient coating on active material layer, and thickness is 1 μ m.Working gas is an argon gas, and flow is 50sccm, and operating air pressure remains on 5 * 10
-1Pa.
The cathode pole piece that above-mentioned preparation process obtains is measured, can be obtained that the atomic ratio of silicon and carbon is 100: 1 in the active material, the atomic ratio of silicon and hydrogen is 100: 1.
Resulting cathode pole piece and metal Li are formed the button half-cell carry out electrochemical property test, test result as shown in Figure 7, the discharging current multiplying power is 0.5C-10C, the charging/discharging voltage scope is at 0～2.0V.
Aluminium is as resilient coating, and the gram specific capacity of negative material decreases, and the 0.5C discharge-rate is 780mAh/g down.Along with the increase of discharging current, battery capacity changes little, remains on 735mAh/g under the 10C multiplying power, is 94% of capacity under the 0.5C discharge-rate.When discharging current drops to 0.5C, the capacity performance is 755mAh/g.Experimental result shows that cathode pole piece possesses multiplying power discharging property preferably.In addition, present embodiment can also use materials such as boron, iron, copper or silver as resilient coating.
At last, it will be appreciated by those skilled in the art that the foregoing description just is used for technical scheme of the present invention is described, and unrestricted.For a person skilled in the art, various technical scheme of the present invention can be carried out various combinations, changes and be equal to replacement.Therefore, all any combinations of being done within the spirit and principles in the present invention, revise, be equal to replacement, improve and upgrade or the like, all should be included within protection scope of the present invention.
Claims (14)
1. a negative material that is used for lithium ion secondary battery negative pole is characterized in that,
Comprise active material silicon or tin, also be doped with carbon and protium in this active material.
2. negative material according to claim 1, it is characterized in that, described two kinds of doped chemicals are uniformly distributed in the described active material, and the atomic ratio of active material and carbon is 10: 1-100: 1, and the atomic ratio of active material and protium is 50: 1-100: 1.
3. negative material according to claim 1 is characterized in that described active material exists with the form of film.
4. negative material according to claim 3 is characterized in that, the structure of described active material is nano microcrystalline structure or non crystalline structure.
5. negative material according to claim 3 is characterized in that, the thickness of described active material is 1-20 μ m.
6. negative material according to claim 1 is characterized in that, also is doped with in aluminium, boron, iron, copper and the silver element one or more in the described active material.
7. be used for the preparation method of the negative material of lithium rechargeable battery, may further comprise the steps:
(a) provide collector;
(b) use physical gas-phase deposite method, by the gas phase doping mode, dopant deposition has the active material layer of protium and carbon on described collector, and wherein, described active material is silicon or tin.
8. preparation method according to claim 7 is characterized in that, described physical gas-phase deposite method is a dc magnetron sputtering method.
9. preparation method according to claim 7, it is characterized in that, the employed gas of described gas phase doping is the mist of hydrogen and carbonaceous gas, and described carbonaceous gas is selected from alkanes, alkynes class and alkene class gas, and the operating air pressure of mist is 0.1Pa-10Pa.
10. preparation method according to claim 9, it is characterized in that, in preparation process, control the flow separately of described hydrogen and carbonaceous gas, make in the negative material, the atomic ratio of described active material and carbon is 10: 1-100: 1, and the atomic ratio of active material and protium is 50: 1-100: 1.
11. a cathode pole piece comprises the described negative material of claim 1, carries the collector of this negative material and covers the lip-deep resilient coating of described negative material.
12. cathode pole piece according to claim 11 is characterized in that, described cushioning layer material is carbon, aluminium, boron, iron, copper or silver element.
13. cathode pole piece according to claim 11 is characterized in that, described buffer layer thickness is 10-500nm.
14. a lithium rechargeable battery comprises the described cathode pole piece of claim 11, also comprise anode pole piece and be located at anode pole piece and cathode pole piece between be used to transmit the electrolyte of lithium ion.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102054981A (en) * | 2010-07-22 | 2011-05-11 | 中信国安盟固利动力科技有限公司 | Anode material doped with hydrogen and carbon elements and preparation method thereof |
| CN102054961A (en) * | 2010-07-22 | 2011-05-11 | 中信国安盟固利动力科技有限公司 | Active negative pole piece and preparation method thereof |
| CN102315445A (en) * | 2010-07-07 | 2012-01-11 | 三星Sdi株式会社 | Be used for secondary lithium battery cathode active material and serondary lithium battery |
| CN108559961A (en) * | 2017-12-19 | 2018-09-21 | 成都亦道科技合伙企业（有限合伙） | A kind of method and device of polynary magnetron sputtering prepares the method for lithium metal combination electrode, prepares the equipment of electrode |
-
2008
- 2008-08-01 CN CN200810117583A patent/CN101640269A/en not_active Withdrawn
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102315445A (en) * | 2010-07-07 | 2012-01-11 | 三星Sdi株式会社 | Be used for secondary lithium battery cathode active material and serondary lithium battery |
| US8551655B2 (en) | 2010-07-07 | 2013-10-08 | Samsung Sdi Co., Ltd. | Negative active material for secondary lithium battery and secondary lithium battery |
| CN102315445B (en) * | 2010-07-07 | 2015-02-11 | 三星Sdi株式会社 | Negative active material for rechargeable lithium battery and rechargeable lithium battery |
| CN102054981A (en) * | 2010-07-22 | 2011-05-11 | 中信国安盟固利动力科技有限公司 | Anode material doped with hydrogen and carbon elements and preparation method thereof |
| CN102054961A (en) * | 2010-07-22 | 2011-05-11 | 中信国安盟固利动力科技有限公司 | Active negative pole piece and preparation method thereof |
| CN108559961A (en) * | 2017-12-19 | 2018-09-21 | 成都亦道科技合伙企业（有限合伙） | A kind of method and device of polynary magnetron sputtering prepares the method for lithium metal combination electrode, prepares the equipment of electrode |
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Open date: 20100203 |