CN102237513A - Negative active material and preparation method thereof as well as negative electrode and lithium battery using negative active material - Google Patents
Negative active material and preparation method thereof as well as negative electrode and lithium battery using negative active material Download PDFInfo
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- CN102237513A CN102237513A CN2010101661450A CN201010166145A CN102237513A CN 102237513 A CN102237513 A CN 102237513A CN 2010101661450 A CN2010101661450 A CN 2010101661450A CN 201010166145 A CN201010166145 A CN 201010166145A CN 102237513 A CN102237513 A CN 102237513A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a negative active material which is formed by compounding artificial graphite and natural graphite. The negative active material is characterized in that the compound percentage ratio of artificial graphite to natural graphite is between 71:29 and 92:8. The compound negative active material prepared by the method disclosed by the invention has the low cost and the high compaction density; a negative electrode prepared by the negative active material has high processing performance and is not easy to fall off; when the negative electrode is applied to a lithium battery, the obtained lithium battery can acquire higher energy density per unit volume and the cycle performance is improved.
Description
Technical field
The present invention relates to its negative pole and lithium battery of a kind of negative active core-shell material, its preparation method and use.More specifically, the present invention relates to the negative active core-shell material and the lithium battery of the high energy density per unit volume metric density of a kind of high power capacity, this negative active core-shell material is composited by Delanium and two kinds of negative active core-shell materials of native graphite.
Background technology
Since nineteen ninety Sony invention lithium ion battery, along with the development of lithium-ion electric pool technology and the reduction of battery material cost, lithium ion battery is widely used in mobile electronic device at present, as bluetooth, mobile phone, MP3/MP4, digital camera and notebook computer etc.Along with the development of electronic product technology with and more and more widely application, the electronic product flying power requires more and more higher.
In recent years, along with the development of mobile communication, 3G mobile is come quietly, and is presenting the trend of high speed development.Because 3G mobile is more and more higher to the requirement of multimedia function, and function such as color screen, camera, bluetooth, recreation and Streaming Media or to use power consumption higher, the profile of 3G mobile is more and smaller and more exquisite, frivolous in addition, the volume of battery of mobile phone is more and more littler, it is little to cause most of 3G mobile all to be faced with battery capacity, problems such as standby, operating time weak point.Therefore the capacity of battery is had higher requirement, need design the more thin polymer lithium secondary battery of high power capacity, satisfy the instructions for use of more areas.
Selecting rational high power capacity graphite cathode material is one of method that improves battery capacity.Lithium battery commonly used at present is many about 330～350mAh/g with the graphite cathode material gram volume, and compacted density is many at 1.50g/cm
3Below.And lithium battery mainly divides two classes with the high power capacity graphite cathode material: a class is spherical modified natural graphite or the cladded type native graphite of gram volume more than 350mAh/g, and this type of native graphite part gram volume can reach more than the 360mAh/g; Another kind of is to adopt rhombus Delanium or the erose Delanium of gram volume more than 350mAh/g.The former mostly is sphere or ellipsoidal particle owing to shape, good processability when it makes pole piece; But owing to be that native graphite forms through modification or surface coating, its compacted density is not high, often at 1.50g/cm
3Below, so the volume energy density of this type of material is not high.Can destroy its modification or surperficial clad structure if compacted density is too high, cause cycle performance of battery sharply to descend.The latter can obtain to be higher than the compacted density of 1.50g/cm3, but because its shape mostly is rhombus or irregularly shaped, and specific area is bigger, and difficulty of processing is big when being made into pole piece, pole piece often falls material easily or comes off.Fall material or come off in order to overcome pole piece, usually need to add more binding agent, so just limited the raising of its compacted density to a large extent, thereby also be difficult to obtain very high volume energy density.
Therefore, prior art awaits improving and development.
Summary of the invention
Purpose of the present invention is intended to solve the technical problem that exists in the existing high power capacity graphite cathode material application, provides a kind of being composited by Delanium and two kinds of negative active core-shell materials of native graphite to reach the composite anode active material and the lithium battery thereof of the high energy density per unit volume metric density of high power capacity.
In order to solve the problems of the technologies described above, technical scheme of the present invention is as follows:
A kind of negative active core-shell material is composited by Delanium and native graphite, and wherein, the composite quality ratio of Delanium and native graphite is between 71: 29～92: 8.
Described negative active core-shell material, wherein, the composite quality ratio of Delanium and native graphite is between 75: 25～85: 15.
Described negative active core-shell material, wherein, described Delanium, its gram volume are more than 350mAh/g, and meso-position radius is shaped as rhombus or irregularly shaped particles between 10～22 μ m, and its specific area is at 2.5～4.0m
2Between/the g.
Described negative active core-shell material, wherein, described native graphite is that its gram volume is more than 355mAh/g through modification or surface coated native graphite, and meso-position radius is shaped as sphere or ellipsoidal particle between 10～22 μ m, and its specific area is at 1.5～2.5m
2Between/the g.
Described negative active core-shell material, its meso-position radius are between 10～22 μ m, and its tap density is 0.65～0.95g/ml, and specific area is 2.3～3.3m
2/ g.
A kind of preparation method of negative active core-shell material may further comprise the steps:
(1) do Delanium and native graphite mixed with 71: 29～92: 8 mass ratio;
(2) solvent, binding agent are mixed, make binding agent in solvent, after the abundant dissolving, add conductive agent again and fully stir;
(3) dry powder that step (1) is obtained joins in the mixture of step (2).
A kind of preparation method of negative active core-shell material may further comprise the steps:
(1) solvent, binding agent are mixed, make binding agent in solvent, after the abundant dissolving, add conductive agent again and fully stir;
(2) add native graphite, after fully stirring, add Delanium again, fully stir, wherein the composite quality ratio of Delanium and native graphite is between 71: 29～92: 8.
A kind of negative pole comprises negative current collector and the negative active core-shell material that is coated on the negative current collector, and wherein, described negative active core-shell material is above-mentioned negative active core-shell material.
Described negative pole, wherein, the negative plate compacted density is at 1.55～1.75g/cm
3Between.
A kind of lithium battery comprises negative pole, positive pole and electrolyte, and wherein, described negative pole contains above-mentioned negative active core-shell material.
Adopt such scheme, the composite anode active material cost that the present invention obtains is low, compacted density is high, the negative pole of making by this negative active core-shell material, the processing characteristics height, difficult drop-off, be used for lithium battery, the lithium battery that obtains can obtain higher energy density per unit volume metric density, and cycle performance is improved.
Description of drawings
Fig. 1 is for using the 041230125mAh battery cyclic curve figure of negative active core-shell material of the present invention;
Fig. 2 is for using the 4250801850mAh battery cyclic curve figure of negative active core-shell material of the present invention.
Embodiment
Below in conjunction with accompanying drawing, preferred embodiment of the present invention is described in further detail.
According to technology implementation scheme of the present invention, provide a kind of composite anode active material that is composited and obtains by Delanium and two kinds of negative active core-shell materials of native graphite.
Described Delanium is meant its gram volume more than 350mAh/g, and D50 (meso-position radius) is shaped as rhombus or irregularly shaped particles between 10～22 μ m, and its specific area is at 2.5～4.0m
2Between/the g.
Described native graphite is that its gram volume is more than 355mAh/g through modification or surface coated native graphite, and D50 is shaped as sphere or ellipsoidal particle between 10～22 μ m, and its specific area is at 1.5～2.5m
2Between/the g.
The composite quality ratio of described two kinds of negative active core-shell materials is between 71: 29～92: 8, more preferably between 75: 25～85: 15.If the ratio of native graphite surpasses 30%, the negative pole that composite anode active material is made is difficult to obtain higher compacted density; And if the ratio of native graphite is improved not quite the processing characteristics of pole piece less than 8%, pole piece still falls material easily or comes off.This composite anode active material D50 still maintains between 10～22 μ m, and its tap density is 0.65～0.95g/ml, and specific area is 2.3～3.3m
2/ g.
The complex method of described two kinds of negative active core-shell materials divides two classes: method one is in advance two kinds of negative active core-shell materials to be carried out mechanical dry to mix, and carries out the preparation of composite anode active material slurry again; Method two is in the preparation process of slurry, with two kinds of negative active core-shell materials feed in raw material step by step realize compound.
Cathode size is realized by following steps in the described method one:
(1), two kinds of negative active core-shell materials are done mixed by mixer according to predetermined mass ratio, obtain well-mixed negative active core-shell material dry powder.Described mixer includes but not limited to cone-type mixer, three mixers, V-Mixer etc.;
(2), solvent, binding agent are mixed 3～15h, guarantee that binding agent fully dissolves at solvent; Add conductive agent again and fully stir 1～3h;
(3), the negative active core-shell material dry powder that mixes is joined in the above-mentioned mixture, fully stir 3～15h and make cathode size.
Cathode size is realized by following steps in the described method two:
(1), solvent, binding agent are mixed 3～15h, guarantee that binding agent fully dissolves at solvent; Add conductive agent again and fully stir 1～3h;
(2), add the negative active core-shell material native graphite, fully stir 2～6h, add the negative active core-shell material Delanium again, fully stir 3～13h and make cathode size.
Add the back at negative active core-shell material graphite in said method one and the method two and stir 10min～1h with the slower speed of 300r/min～600r/min earlier, the remaining time of back stirs with the higher speed of 1000r/min～2000r/min again, to guarantee abundant mixing.
According to another embodiment of the present invention, a kind of negative pole that comprises negative current collector and be coated in the negative active core-shell material on the negative current collector is provided, this negative pole is when making, and the negative plate compacted density that is rolled into is at 1.55～1.75g/cm
3Between, wherein this negative active core-shell material is above-mentioned composite anode active material.
The preparation of described negative plate realizes by the following method:
As collector, the slurry that method one or method two are made is dried to pole piece being applied on the coating machine on the Copper Foil with the thick Copper Foil of 9～12 μ m, through roll-in, cut and be made into negative plate.This negative plate compacted density is at 1.55～1.75g/cm
3Between.
According to an embodiment more of the present invention, a kind of lithium battery that comprises negative pole, positive pole and electrolyte is provided, wherein this negative pole comprises above-mentioned composite anode active material.
The preparation of described lithium battery realizes by the following method:
(1), preparation positive plate;
The manufacture method of positive plate is to be that 93.0%～97.0% cobalt acid lithium, 1.5%～3.0% conductive additive, 2.0%～6.0% binding agent mix with mass percent, with solvent furnishing paste, the thick aluminium foil of 14～20 μ m is as collector, be dried to pole piece on the aluminium foil on the coating machine creme being applied to, through roll-in, cut and be made into positive plate.
(2), lug is gone up in each welding of negative plate that positive plate, above-mentioned composite anode active material are prepared, be wound into electric core together with barrier film, seal with three limits of plastic-aluminum packaging film electric core, injection electrolyte also seals, bleed after changing into and seal the 4th limit, carry out the battery capacity screening again and form polymer Li-ion battery; Or the electric core that is rolled into changes in the metal-back, and metal-back can be square or circle etc., injects electrolyte and also seals, change into reprocessing and the liquid metal case lithium ion battery.
Characteristics and advantage that the technical solution used in the present invention has are:
Adopt this composite anode active material to make the lithium battery negative pole, can keep the characteristics of two kinds of negative material high power capacity, can obtain higher compacted density, the negative plate compacted density that is rolled into is at 1.55～1.75g/cm
3Between.Simultaneously composite anode active material is because the introducing of spherical modification or surface coated native graphite, and specific area reduces relatively, can improve the processing characteristics of pole piece well, shortcoming such as avoid pole piece to fall material easily or to come off.
Use the lithium battery of this high power capacity high compacted density composite anode active material, the lifting that capacity can be by a relatively large margin, battery can obtain higher energy density per unit volume metric density.According to the size of battery size, capacity can promote 3.0%～15.0% on the original basis and not wait.
So that generally the 041230110mAh and the 4250801750mAh polymer Li-ion battery of production are example in the market, after adopting said method, the capacity of 041230 lithium ion battery can promote 5.0%～15.0%, 425080 lithium ion batteries on original basis capacity can promote 3.0%～8.0% on original basis.By adopting suitable function electrolyte to improve the stability of whole electrochemical system, can guarantee that the battery of above preparation has excellent cycle performance, the 300 all capacity that circulate can maintain more than 80% even 90%.
Adopt negative active core-shell material of the present invention to prepare the 041230110mAh polymer Li-ion battery, obtain embodiment 1, embodiment 2, and simultaneously prepare 041230110mAh polymer Li-ion battery example 1 in contrast with on the market common negative active core-shell material.Following table 1 is the contrast that several embodiment of 041230 battery and reference examples capacity promote:
Table 1
| Example | Design minimum capacity/mAh | Actual average capacity/mAh | Design capacity promotes ratio |
| Embodiment 1 | 120 | 126 | 9.1％ |
| Embodiment 2 | 125 | 131 | 13.6％ |
| Reference examples 1 | 110 | 115 | - |
Adopt negative active core-shell material of the present invention to prepare the 4250801750mAh polymer Li-ion battery, obtain embodiment 3, embodiment 4, and simultaneously prepare 4250801750mAh polymer Li-ion battery example 2 in contrast with on the market common negative active core-shell material.Following table 2 is contrasts that several embodiment of 425080 batteries and reference examples capacity promote:
Table 2
| Example | Design minimum capacity/mAh | Actual average capacity/mAh | Design capacity promotes ratio |
| Embodiment 3 | 1810 | 1906 | 3.4％ |
| Embodiment 4 | 1850 | 1951 | 5.7％ |
| Reference examples 2 | 1750 | 1835 | - |
The a plurality of batteries that use the technology of the present invention preparation are charged and discharged the cycle life test, obtain cyclic curve as shown in Figure 1 and Figure 2.As shown in Figure 1, capability retention maintains more than 85% after the 300 week circulation of 041230125mAh battery.As shown in Figure 2, capability retention maintains more than 90% after the 300 week circulation of 4250801850mAh battery.
The high-capacity polymer secondary cell of this exploitation can be widely used in most 3C electronic product on the present market, as bluetooth earphone, MP3/MP4, mobile phone, media player, digital camera, Portable DVD and notebook computer etc.
Should be understood that, for those of ordinary skills, can be improved according to the above description or conversion, and all these improvement and conversion all should belong to the protection range of claims of the present invention.
Claims (10)
1. a negative active core-shell material is composited by Delanium and native graphite, it is characterized in that, the composite quality ratio of Delanium and native graphite is between 71: 29～92: 8.
2. negative active core-shell material according to claim 1 is characterized in that, the composite quality ratio of Delanium and native graphite is between 75: 25～85: 15.
3. negative active core-shell material according to claim 1 is characterized in that, the gram volume of described Delanium is more than 350mAh/g, and meso-position radius is between 10～22 μ m, and specific area is at 2.5～4.0m
2Between/the g.
4. negative active core-shell material according to claim 1 is characterized in that, described native graphite is that its gram volume is more than 355mAh/g through modification or surface coated native graphite, and meso-position radius is between 10～22 μ m, and its specific area is at 1.5～2.5m
2Between/the g.
5. negative active core-shell material according to claim 1 is characterized in that, the meso-position radius of described negative active core-shell material is between 10～22 μ m, and its tap density is 0.65～0.95g/ml, and specific area is 2.3～3.3m
2/ g.
6. the preparation method of a negative active core-shell material may further comprise the steps:
Step (1), Delanium and native graphite done with 71: 29～92: 8 mass ratio mix;
Step (2), solvent, binding agent are mixed, make binding agent in solvent, fully after the dissolving, add conductive agent again and fully stir;
Step (3), the dry powder that step (1) is obtained join in the mixture of step (2).
7. the preparation method of a negative active core-shell material may further comprise the steps:
Step (1), solvent, binding agent are mixed, make binding agent in solvent, fully after the dissolving, add conductive agent again and fully stir;
Step (2), adding native graphite after fully stirring, add Delanium again, fully stir, and wherein the composite quality ratio of Delanium and native graphite is between 71: 29～92: 8.
8. a negative pole comprises negative current collector and the negative active core-shell material that is coated on the negative current collector, it is characterized in that described negative active core-shell material is according to the arbitrary described negative active core-shell material of claim 1～5.
9. negative pole according to claim 8 is characterized in that the negative plate compacted density is at 1.55～1.75g/cm
3Between.
10. a lithium battery comprises negative pole, positive pole and electrolyte, it is characterized in that, described negative pole contains the arbitrary described negative active core-shell material of with good grounds claim 1～5.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102386384A (en) * | 2011-11-28 | 2012-03-21 | 深圳市贝特瑞新能源材料股份有限公司 | Spherical hard carbon lithium ion battery cathode material and preparation method thereof |
| CN110148714A (en) * | 2018-02-13 | 2019-08-20 | 宁德时代新能源科技股份有限公司 | Secondary battery |
| CN110931855A (en) * | 2018-09-19 | 2020-03-27 | 三星Sdi株式会社 | Lithium battery |
| US11251432B2 (en) | 2016-02-12 | 2022-02-15 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11264644B2 (en) | 2016-02-12 | 2022-03-01 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11264645B2 (en) | 2016-02-12 | 2022-03-01 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11335952B2 (en) | 2016-02-12 | 2022-05-17 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11637322B2 (en) | 2016-02-12 | 2023-04-25 | Samsung Sdi Co., Ltd. | Lithium battery |
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| CN101459237A (en) * | 2007-12-10 | 2009-06-17 | 深圳市比克电池有限公司 | Battery cathode slurry, preparation and battery produced by the cathode slurry |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102386384A (en) * | 2011-11-28 | 2012-03-21 | 深圳市贝特瑞新能源材料股份有限公司 | Spherical hard carbon lithium ion battery cathode material and preparation method thereof |
| CN102386384B (en) * | 2011-11-28 | 2013-07-10 | 深圳市贝特瑞新能源材料股份有限公司 | Spherical hard carbon lithium ion battery cathode material and preparation method thereof |
| US11251432B2 (en) | 2016-02-12 | 2022-02-15 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11264644B2 (en) | 2016-02-12 | 2022-03-01 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11264645B2 (en) | 2016-02-12 | 2022-03-01 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11335952B2 (en) | 2016-02-12 | 2022-05-17 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11637322B2 (en) | 2016-02-12 | 2023-04-25 | Samsung Sdi Co., Ltd. | Lithium battery |
| CN110148714A (en) * | 2018-02-13 | 2019-08-20 | 宁德时代新能源科技股份有限公司 | Secondary battery |
| CN110931855A (en) * | 2018-09-19 | 2020-03-27 | 三星Sdi株式会社 | Lithium battery |
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Application publication date: 20111109 |