CN102315422B - A kind of lithium ion battery - Google Patents
A kind of lithium ion battery Download PDFInfo
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- CN102315422B CN102315422B CN201110268072.0A CN201110268072A CN102315422B CN 102315422 B CN102315422 B CN 102315422B CN 201110268072 A CN201110268072 A CN 201110268072A CN 102315422 B CN102315422 B CN 102315422B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention is intended to provide lithium ion compensator alloy anode to the loss of cell cathode capacity with benefit lithium negative electrode.Characteristic due to silicon anode causes the efficiency first of the lithium ion battery of this system low, and target capacity loss is large, and employing the loss of mending the lithium ion compensation target capacity that lithium negative electrode provides can highlight the advantage of silicon anode cell high-energy-density.In the mode of mending lithium, twice benefit lithium is carried out respectively to anode and cathode, effectively can improve capacity and the performance of battery.
Description
Technical field
The present invention relates to technical field of lithium ion, particularly relate to silicon anode architectures lithium ion battery and compensate for the capacity of cathode wear with external lithium source.
Background technology
Along with the raising that electronic product and electric motor car require energy density, energy density can not meet the demands gradually close to the lithium ion battery of the graphite anode system of the limit, and the silica-based anode with high power capacity becomes a focus of research at present as the possible replacer of graphite.For silicon anode architectures, its irreversible capacity is except forming the irreversible capacity of SEI consumption, more importantly because properties of materials makes the lithium ion when full battery discharge end in anode be trapped in inside and can not form effective capacity, cathode capacities is caused to be depleted, many about 20% of loss ratio graphite system, the advantage of the high-energy-density of silicon anode will be cancelled.Therefore, compensating the cathode capacities loss of silicon anode architectures battery, is the problem that silicon anode architectures lithium ion battery applications road must solve.
From the source of capacity loss, it is best approach that anode material improves.But because the current preparation to silicon anode material is also not overripened, the method that improvement material promotes efficiency first does not also have effect.
Another kind method compensates silicon anode irreversible lithium ion in charge and discharge process by adding lithium metal.FMC Corp. repeatedly describes the effect introducing its product SLMP (stabled lithium metal powder) in lithium ion battery.But because the use of SLMP requires harsh to the humidity of environment and oxygen content, use the unstable result of SLMP under existing environment, therefore, the industrialization of SLMP uses the problem also needing to solve storage and environment for use.Patent CN1279648C, CN102148401A, the method that before CN101459262A describes assembled battery, anode surface first forms SEI film compensates irreversible capacity first, but the anode after film forming needs humidity and the atmosphere of strictly controlled environment when assembled battery, so be inconvenient to operate.
In view of the foregoing, compensate the loss of silica-based anode lithium ion battery cathodes capacity, and find a kind ofly be easy to operation, low to environmental requirement, effective method is a kind of required.
Summary of the invention
The object of the invention is to, for the existing silicon anode low shortcoming causing cathode capacities loss of efficiency first, provide a kind of method of easy and simple to handle, low to environmental requirement, electrode compensation capacity that implementation result is good.
Object of the present invention is achieved by following technical solution:
A kind of lithium ion battery, comprise negative electrode, anode, be interval in barrier film between anode and cathode and electrolyte thereof, described anode and cathode and barrier film form battery core by lamination, and described anode is silica-based anode.The anode active material of the lithium ion battery of current commercialization mostly is graphite material, and the theoretical capacity of graphite is 372mAh/g, now reaches 365mAh/g, close to the limit with graphite material capacity.Along with the raising that electronic product and electric motor car require energy density, the lithium ion battery of graphite anode system can not meet the demands gradually.And silicon becomes research focus with the theoretical capacity of 4200mAh/g.By silicon anode with being also the necessity meeting energy density requirement in the battery.
Also comprise and mend lithium negative electrode, described benefit lithium negative electrode is arranged on battery core side.Because the present invention is that middle lithium ion needs to enter into anode and cathode inside from the benefit lithium negative electrode beyond battery core main body, battery core prepared by lamination process is compared to winding process, and both sides have more passage to be convenient to lithium ion to enter battery core main body between layers.Mend the lateral location that lithium negative electrode is placed on battery core, lithium ion can enter into battery core main body smoothly, and lithium ion diffusion length on width is short, is easy to reach the equally distributed state of lithium ion.Separately, from mending the interpolation of lithium negative electrode and taking out operation and consider, being placed on side ratio, to be placed on bottom desirable.
Described benefit lithium negative electrode target carries out twice benefit lithium.After battery core activation and 50% charged state (SOC) time target carry out first time and mend lithium, it mends lithium amount is mend lithium ion total amount on lithium negative electrode 10 ~ 40%, after first time mends lithium complete circulation, target carries out second time and mends lithium, its mend that lithium amount is lithium ion total amount on benefit lithium negative electrode 10 ~ 40%;
Described benefit lithium negative electrode antianode carries out twice benefit lithium, and time 50% charged state (SOC), antianode carries out first time and mends lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 5 ~ 20%; After first time mends lithium complete circulation, antianode carries out second time and mends lithium, its mend that lithium amount is lithium ion total amount on benefit lithium negative electrode 5 ~ 20%.
Before activation, negative electrode is in fully charged state, cannot supplement lithium ion to its charging.If lithium is mended in antianode precharge before activation, at lithium ion from the edge-diffusion of anode to the process of zone line, anode interior size of current skewness, forms uneven SEI film, unfavorable to battery performance.Therefore, first time mends lithium ion and should select after formation SEI, and selects to carry out in the 50%SOC state that charge and discharge platform is stable.
Then battery is after the process of a circulation, the lithium ion that first time supplements is uniformly distributed in anode and cathode inside, and now anode is in de-lithium state, because part lithium ion is detained in the anode, form irreversible capacity, negative electrode is also in lithium and is discontented with embedding state.Therefore, second time mend lithium select through one circulation after expire the state of putting.
Further, differing little situation in order to avoid mending current potential between lithium negative electrode and negative electrode, when charging benefit lithium, selecting first to mend lithium to negative electrode, then mending lithium to anode.
Capacity is made two bites at a cherry supplementary, just can well avoid the problem of external lithium ion skewness in anode and cathode, also reduce anode edge and to expand the irregular probability of battery core caused greatly.
What described benefit lithium negative electrode target carried out mends lithium twice, and each benefit lithium amount is equal, is and mends 1/3 of lithium ion total amount on lithium negative electrode.
What described benefit lithium negative electrode antianode carried out mends lithium twice, and each benefit lithium amount is equal, is and mends 1/6 of lithium amount.
The characteristic of silicon anode material makes the delay of the lithium ion when full battery discharge end in anode can not form effective capacity therein, causes cathode capacities to be depleted.The efficiency (i.e. anode efficiency) supposing full battery is 67%, if target is promoted to 85%, needs the capacity supplemented to be about 1/3 of full battery capacity.If all told is all replenished anode, external lithium ion can not be uniformly distributed in anode interior, then the serious even demoulding of the silicon anode expansion of edge fully charged state.And a part of capacity is replenished diffusion coefficient high, expand on little negative electrode, the risk of anode edge demoulding can be reduced.And anode diffusion is slow, expand large easily demoulding, and negative electrode diffusion is fast, expands little of demoulding, all supplements 1/3 of total capacity to negative electrode when therefore mending lithium at every turn, supplements 1/6 of total capacity for good to anode.
Described benefit lithium electric current is 0.01C ~ 0.05C.Because the lithium ion that supplements is from the inside of mending lithium negative electrode and enter into battery core, not only lithium ion diffusion length increases, and when mending lithium, the contact-making surface of two electrodes is little, and surface current density increases, and in order to reduce polarization, mending lithium electric current and should control to be less than 0.05C; Simultaneously too small electric current reduces production efficiency when obtaining the result of mending lithium, and therefore electric current should control to be greater than 0.01C.
Described benefit lithium negative electrode is arranged on the distance that battery core side is less than 40mm.When mending the distance of lithium negative electrode to nearest anode and being greater than 40mm, lithium ion is just difficult to diffuse into anode from benefit lithium negative electrode.Therefore mend lithium negative electrode to be placed on battery core side and to be less than in the scope of 40mm, be preferably not more than the distance of 20mm.
The active material that described silica-based anode comprises be in Si-C, SiOx, SiOx-C, silicon alloy any one or multiple.The anode of described lithium ion battery, be made up of collector and active material layer attached thereto, active material layer comprises silicon active material, conductive carbon and binding agent, and binding agent can be the combination of one or more of PVDF, CMC, SBR, PI, PAI.
Described benefit lithium active material of cathode be LiMn2O4, cobalt acid lithium, LiFePO4, lithium nickelate and cobalt nickel ion doped in any one or multiple.Benefit lithium negative electrode in this patent, effect supplements lithium ion to battery core main body, and then the cathode capacities of electrode compensation.So, as long as the material of lithium ion can be provided, the active material mending lithium negative electrode all can be used to.
Relative to prior art, tool of the present invention has the following advantages: one, mends lithium negative electrode and is placed on battery core side, during encapsulation and battery core main body encapsulate in the lump, easy and simple to handle, and follow-uply to charge in open environment, not high to environmental requirement.Two, prepared by battery core lamination process, and side layer structure is convenient to lithium ion and is entered battery core from benefit lithium negative electrode.Three, all lithium is mended to anode and cathode, can avoid capacity all being replenished the problem that the anode edge that anode causes completely fills demoulding; And replenish on negative electrode by 2/3 of capacity to be compensated, remaining 1/3 replenishes on anode, can the capacity of effective compensation cathode wear.Four, anode and cathode charging supplements lithium source and all completes with twice, can avoid carrying out supplementary lithium ion by disposable, cause lithium ion to spread the edge brought, middle lithium ion problem pockety.Five, mend lithium negative electrode after lithium source is provided, take out from battery, while not increasing battery volume, improve capacity, therefore effectively can promote the energy density of battery.
Embodiment
Below in conjunction with embodiment, the present invention is described in further detail, but embodiments of the present invention are not limited thereto.
Embodiment 1
A kind of lithium ion battery, comprise negative electrode, anode, be interval in barrier film between anode and cathode and electrolyte thereof, anode and cathode and barrier film prepare battery core 363173 (long is 73mm, and wide is 31mm, and thick is 3.6mm) by lamination.Anode is silica-based anode, and 9um Copper Foil does collector, and the formula of slurry is: Si active material: SP: CMC: SBR=90: 2: 4: 4.Cathodic Composition is: cobalt acid lithium: SP: PDVF=97: 1.6: 1.4.
The active material mending lithium negative electrode is cobalt acid lithium, mends lithium negative electrode and is of a size of long 69mm, wide 30mm, placed its adjacent battery core side.Described benefit lithium negative electrode is arranged in the distance that battery core side is 30mm, is the width being less than and mending lithium negative electrode.
Mend lithium negative electrode and respectively twice benefit lithium is carried out to anode and cathode.First time after battery core activation and 50% charged state (SOC) time, first target carries out benefits lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 1/3, and then antianode carries out benefit lithium, and benefit lithium amount is 1/6; After the circulation that benefit lithium completes for the first time, carry out second time mend lithium, successively target, anode supplement the capacity of 1/3,1/6 respectively.Benefit lithium electric current used is 0.001C.
Test the battery made, capacity is 1750mAh.Circulation volume conservation rate is: 97%@50 circulation (50cls) acquired results is shown in table 1.
Comparative example 1
Compared to embodiment 1, be that 363173 naked battery cores prepare battery according to a conventional method by model, do not mend lithium negative electrode and follow-up lithium up process.
Test gained battery, capacity is 1450mAh.Circulation volume conservation rate 94%@50cls.Acquired results is shown in table 1.
Embodiment 2
Battery core in the same manner as in Example 1.The active material mending lithium negative electrode is nickel manganese cobalt acid lithium, mends lithium negative electrode and is of a size of long 69mm, wide 20mm, placed its adjacent battery core side.Described benefit lithium negative electrode is arranged in the distance that battery core side is 20mm, is the width being less than and mending lithium negative electrode.
Mend lithium negative electrode and respectively twice benefit lithium is carried out to anode and cathode.First time after battery core activation and 50% charged state (SOC) time, first target carries out benefits lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 1/3, and then antianode carries out benefit lithium, and benefit lithium amount is 1/6; After the circulation that benefit lithium completes for the first time, carry out second time mend lithium, successively target, anode supplement the capacity of 1/3,1/6 respectively.Benefit lithium electric current used is 0.02C.
The battery obtained is tested, and capacity is 1790mAh, and circulation conservation rate is 95%@50cls, the speed of drift bolt security performance 2mm/s, battery energy safety.Acquired results is shown in table 1.
Comparative example 2
Compared to embodiment 2, battery is identical.Twice benefit lithium is carried out unlike a benefit lithium negative electrode antianode.First time battery core activation after and 50% charged state (SOC) time, second time be one circulation after.Mend lithium capacity twice identical.
The battery obtained is tested.Capacity is 1380mAh, and circulation conservation rate is 60%@50cls, drift bolt poor safety performance, and the speed battery of 5mm/s is all burnt.Acquired results is shown in table 1.
Embodiment 3
Battery core in the same manner as in Example 1.The active material mending lithium negative electrode is LiMn2O4, mends lithium negative electrode and is of a size of long 69mm, wide 10mm, and placed its adjacent battery core side, described benefit lithium negative electrode is arranged in the distance that battery core side is 10mm, is the width being less than and mending lithium negative electrode.
Mend lithium negative electrode and respectively twice benefit lithium is carried out to anode and cathode.First time after battery core activation and 50% charged state (SOC) time, first target carries out benefits lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 1/3, and then antianode carries out benefit lithium, and benefit lithium amount is 1/6; After the circulation that benefit lithium completes for the first time, carry out second time mend lithium, successively target, anode supplement the capacity of 1/3,1/6 respectively.Benefit lithium electric current used is 0.02C.
The battery obtained is tested.Capacity is 1760mAh, and circulation conservation rate is 96%@50cls, the speed of drift bolt security performance 2mm/s, battery energy safety.Acquired results is shown in table 1.
Comparative example 3
Battery core in the same manner as in Example 1.The active material mending lithium negative electrode is LiMn2O4, mends lithium negative electrode and is of a size of long 69mm, wide 20mm, is placed its adjacent battery core side.Described benefit lithium negative electrode is arranged in the distance that battery core side is 20mm, is the width being less than and mending lithium negative electrode.
Mend lithium negative electrode and twice benefit lithium is carried out to anode and cathode.First time after battery core activation and 50% charged state (SOC) time, first target carries out benefits lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 1/4, and then antianode carries out benefit lithium, and benefit lithium amount is 1/4; After the circulation that benefit lithium completes for the first time, carry out second time mend lithium, successively target, anode supplement the capacity of 1/4,1/4 respectively.Benefit lithium electric current used is 0.02C.
The battery obtained is tested.Capacity is 1510mAh, and circulation conservation rate is 68%@50cls, and the speed of drift bolt security performance 2mm/s, battery is burnt.Acquired results is shown in table 1.
Embodiment 4
Battery core in the same manner as in Example 1.The active material mending lithium negative electrode is the mixture of cobalt acid lithium and nickle cobalt lithium manganate, mend lithium negative electrode and be of a size of long 69mm, wide 10mm, its adjacent battery core side is placed, described benefit lithium negative electrode is arranged in the distance that battery core side is 10mm, is the width being less than and mending lithium negative electrode.
Mend lithium negative electrode and respectively twice benefit lithium is carried out to anode and cathode.First time after battery core activation and 50% charged state (SOC) time, first target carries out benefits lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 1/3, and then antianode carries out benefit lithium, and benefit lithium amount is 1/6; After the circulation that benefit lithium completes for the first time, carry out second time mend lithium, successively target, anode supplement the capacity of 1/3,1/6 respectively.Benefit lithium electric current used is 0.05C.
The battery obtained is tested.Capacity is 1740mAh, and circulation conservation rate is 95%@50cls, the speed of drift bolt security performance 2mm/s, battery energy safety.Acquired results is shown in table 1.
Comparative example 4
Compared to embodiment 4, adopt winding process to prepare the battery core of same size, under equal state, twice benefit lithium is carried out respectively to anode and cathode, benefit lithium electric current is increased to 0.07C.The test result of mending lithium capacity and battery is as shown in table 1.
The efficiency first of table 1 embodiment and comparative example gained battery and volume test value
Data display in table 1, comparative example 1 is compared with embodiment 1, do not mend the capacity that lithium negative electrode carrys out compensated cathode loss, the capacity of battery is low, lower than embodiment 1 by about 20%, can draw thus, under the capacity situation not having compensated cathode to consume, the advantage of silicon anode high power capacity can be given by the efficiency first that anode is low and be offset.Embodiment 2 mends lithium respectively by the two step anode and cathode optimized, and comparative example 2 is all replenished on anode by capacity, because the capacity supplemented is many, the diffusion of lithium ion in anode is slow, occur that edge reaches fully charged state, problem that inner SOC is very low, and then the anode that completely fills of edge occurs analysing lithium and expands and causes greatly diaphragm to come off, have a strong impact on the capacity of battery, cycle performance and security performance.Used LiMn2O4 as the active material mending lithium negative electrode in embodiment 3, lithium is mended to anode and cathode according to the benefit lithium mode optimized, and comparative example 3 is evenly distributed in anode and cathode by benefit lithium capacity on the basis of embodiment 3, from capacity and circulation result, when anode has shared 1/2 capacity, battery performance is just obvious worsens.Embodiment 4 has used the mixture of cobalt acid lithium and nickel manganese cobalt acid lithium as the active material mending lithium negative electrode, lithium is mended twice respectively to anode and cathode by optimal way, electric current used is 0.05C, comparative example 4 is battery cores that the battery core prepared by lamination process changes winding process into and prepares, because lithium ion admission passage is few, the evolving path is long, mends lithium difficulty, adopt and carry out benefit lithium in a like fashion, mending lithium capacity can reduce; Benefit lithium electric current is increased to 0.07C, and result is in the comparative example 4 that electric current is large, large owing to polarizing, and mend lithium capacity just for needing about 1/2 of compensation capacity, the capacity of battery does not get a promotion, and cycle performance also has variation.
Therefore, in order to the loss of the cathode capacities of silicon anode architectures lithium ion battery effectively can be compensated, the method for benefit lithium of the present invention should be applied.
The benefit lithium negative electrode mentioned in this patent, refers to the negative electrode be placed on outside inside battery, battery core main body, plays the effect supplementing lithium ion to battery core main body.Mending lithium, is under the condition of charging, mending the lithium ion transfer of lithium negative electrode in the negative electrode or anode of battery core main body, namely mending lithium negative electrode and supplementing capacity to battery core main body.
It should be noted that, according to the above description the announcement of book and elaboration, those skilled in the art in the invention can also change above-mentioned execution mode and revise.Therefore, the present invention is not limited to embodiment disclosed and described above, also should in the protection range of claim of the present invention to equivalent modifications more of the present invention and change.In addition, although employ some specific terms in this specification, these terms just for convenience of description, do not form any restriction to the present invention.
Claims (5)
1. a lithium ion battery, comprise negative electrode, anode, be interval in barrier film between anode and cathode and electrolyte thereof, described anode and cathode and barrier film form battery core by lamination, it is characterized in that,
Described anode is silica-based anode;
Also comprise and mend lithium negative electrode, described benefit lithium negative electrode is arranged on battery core side;
Described benefit lithium negative electrode target carries out twice benefit lithium, described benefit lithium negative electrode after battery core activation and 50% charged state SOC time target carry out first time and mend lithium, it mends lithium amount is mend lithium ion total amount on lithium negative electrode 10 ~ 40%, after first time mends lithium complete circulation, target carries out second time and mends lithium, its mend that lithium amount is lithium ion total amount on benefit lithium negative electrode 10 ~ 40%;
Described benefit lithium negative electrode antianode carries out twice benefit lithium, and during 50% charged state SOC, antianode carries out first time and mends lithium, and it mends lithium amount is mend lithium ion total amount on lithium negative electrode 5 ~ 20%; After first time mends lithium complete circulation, antianode carries out second time and mends lithium, its mend that lithium amount is lithium ion total amount on benefit lithium negative electrode 5 ~ 20%;
Benefit lithium negative electrode is arranged on the distance that battery core side is less than 40mm, and this distance is less than the width mending lithium negative electrode;
The active material of described benefit lithium negative electrode be in LiMn2O4, cobalt acid lithium, LiFePO4, lithium nickelate and cobalt nickel ion doped any one or multiple.
2. a kind of lithium ion battery according to claim 1, is characterized in that: it is mend lithium ion total amount on lithium negative electrode 1/3 that the first time that described benefit lithium negative electrode target carries out mends lithium amount; It is mend lithium ion total amount on lithium negative electrode 1/3 that the second time that described benefit lithium negative electrode target carries out mends lithium amount.
3. a kind of lithium ion battery according to claim 1, is characterized in that: the benefit lithium amount that described benefit lithium negative electrode antianode carries out first time benefit lithium is mend lithium ion total amount on lithium negative electrode 1/6; The benefit lithium amount that described benefit lithium negative electrode antianode carries out second time benefit lithium is 1/6.
4. a kind of lithium ion battery according to claim 1, is characterized in that: described benefit lithium electric current is 0.01C ~ 0.05C.
5. a kind of lithium ion battery according to claim 1, is characterized in that: the active material that described silica-based anode comprises is containing Si-C, SiO
x, SiO
xin-C, silicon alloy any one or multiple.
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| CN104733784B (en) * | 2015-04-01 | 2017-03-29 | 广东烛光新能源科技有限公司 | The preparation method of lithium ion battery |
| WO2017022734A1 (en) * | 2015-08-04 | 2017-02-09 | 三井化学株式会社 | Negative electrode for lithium ion secondary battery, lithium ion secondary battery comprising same, and method for producing negative electrode for lithium ion secondary battery |
| CN107768743A (en) * | 2016-08-18 | 2018-03-06 | 中信国安盟固利动力科技有限公司 | A kind of lithium ion battery mends lithium method |
| CN106909716B (en) * | 2017-01-19 | 2020-03-24 | 东北电力大学 | Lithium iron phosphate battery modeling and SOC estimation method considering capacity loss |
| CN108539124B (en) * | 2017-03-01 | 2021-07-20 | 北京卫蓝新能源科技有限公司 | Secondary battery with lithium-supplement electrode and preparation method thereof |
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| CN1909274A (en) * | 2005-08-05 | 2007-02-07 | 赖正义 | Energy-multiplying power lithium battery |
| CN101295783A (en) * | 2007-04-27 | 2008-10-29 | 松下电器产业株式会社 | Electrochemical element and electrode thereof, method and apparatus for manufacturing the electrode, method and apparatus for lithiation treatment |
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| CN1909274A (en) * | 2005-08-05 | 2007-02-07 | 赖正义 | Energy-multiplying power lithium battery |
| CN101295783A (en) * | 2007-04-27 | 2008-10-29 | 松下电器产业株式会社 | Electrochemical element and electrode thereof, method and apparatus for manufacturing the electrode, method and apparatus for lithiation treatment |
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