CN101162773A - Preparation method of battery positive plate, positive plate and lithium ionic cell - Google Patents
Preparation method of battery positive plate, positive plate and lithium ionic cell Download PDFInfo
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- CN101162773A CN101162773A CNA2006101496461A CN200610149646A CN101162773A CN 101162773 A CN101162773 A CN 101162773A CN A2006101496461 A CNA2006101496461 A CN A2006101496461A CN 200610149646 A CN200610149646 A CN 200610149646A CN 101162773 A CN101162773 A CN 101162773A
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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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Abstract
The present invention relates to a method for preparing a lithium-ion battery positive plate, comprising the following procedures: a caking agent is added into the water for dissolution; then an anode active substance is added to the prepared caking agent to mix and prepare a sizing agent; the prepared sizing agent is coated on a collecting fluid; then the lithium-ion battery positive plate is achieved through baking, preforming and slitting; the caking agent is chose from one kind or a plurality of kinds of sodium carboxymethyl cellulose, methylcellulose, hydroxypropyl methylcellulose, carboxymethyl hydroxyethyl cellulose or hydroxypropyl cellulose; the dosage of the caking agent is 0.8 weight percent to 3 weight percent of the battery active substance. The invention also relates to the positive plate made by the method and comprises a lithium-ion battery of the positive plate. The battery achieved by using the positive plate made by the preparation method of the invention has stable electrical property and good cycle performance.
Description
Technical field
The present invention relates to a kind of manufacture method of anode slice of lithium ion battery, and the anode pole piece that uses this method to make, and the lithium ion battery that comprises this anode pole piece.
Background technology
Lithium ion battery is divided into liquid lithium ion battery (LIB) and polymer Li-ion battery (PLIB), liquid lithium ionic cell is since nineteen ninety succeeds in developing, because it has the specific energy height, has high-energy-density, the operating voltage height, temperature limit is wide, self-discharge rate is low, have extended cycle life, pollution-free, in light weight, special advantages such as security performance is good, the use field is extremely extensive, as mobile phone, wireless device, notebook, instrument and meter, report to the police, toy, shake control, space flight, aviation, navigation, video camera, computer, communication, electrical equipment, game machine, household electrical appliance or the like.
Need in the manufacturing process of lithium rechargeable battery to use suitable binding agent to finish the manufacturing of electrode, binding agent in battery mainly in order to active material and electrode current collecting body is together bonded to each other.At present, lithium ion secondary battery electrode mostly adopts polyvinylidene fluoride (PVDF) as adhesive, with the solvent as PVDF such as organic solvent such as N-dimethyl pyrrolidone (NMP), dimethyl formamide (DMF), dimethyl sulfoxide (DMSO) (DMSO), adopt organic system slurry film-making technology to make the anode pole piece of battery.Need to use costliness and have corrosive organic solvent such as NMP, DMP, DMSO etc. in binding agent, use amount is big, the production cost height, and heating removes when desolvating, and air is polluted.
A kind of method for preparing lithium rechargeable battery is disclosed among the CN1532984A, this method has adopted water-soluble binder and tackifier with active material, conductive agent and electrode current collecting body are bonded together, the composition of this water-soluble binder is wherein a kind of or its mixture of polytetrafluoroethylene PTFE or styrene butadiene rubber sbr, consumption is the 0.5-15 weight % of active material, these tackifier are methylcellulose (MC), sodium carboxymethylcellulose (CMC-Na), hydroxypropyl methylcellulose (HPMC), one of them of carboxymethyl hydroxyethyl cellulose (CMHEC) and hydroxypropyl cellulose (HPC) or its mixture, consumption are the 0.2-10 weight % of active material.Use this water-soluble binder and tackifier that the manufacturing cost of lithium rechargeable battery is reduced, and pollution-free.But after this water system binding agent water that contains PTFE becomes mixed emulsion, when pole piece is dried, water wherein can not be removed totally fully, cause these moisture in the battery cyclic process slowly with battery in electrolyte carry out generated reactive gas, cause the battery swell, influence the serviceability of battery.Oxidation can take place in the SBR in this water system binding agent under high voltage, also can influence the serviceability of battery.
Summary of the invention
The objective of the invention is to overcome the shortcoming that above-mentioned binding agent causes the battery swell, influences the battery serviceability, provide a kind of method of making the anode pole piece can make strong, the good electrical property of stability test therefrom.Another object of the present invention is the anode pole piece that adopts this manufacture method to make.A further object of the invention provides a kind of battery that comprises above-mentioned anode pole piece.
The invention provides a kind of manufacture method of anode slice of lithium ion battery, this manufacture method comprises: (1) adds binding agent in the entry and dissolves; (2) positive active material is joined in the above-mentioned binding agent for preparing then and mix, be made into slurry; (3) the described slurry for preparing is applied on the collector, obtain the anode pole piece of lithium ion battery then through baking sheet, compressing tablet, cut-parts, wherein, described binding agent is selected from one or more in sodium carboxymethylcellulose, methylcellulose, hydroxypropyl methylcellulose, carboxymethyl hydroxyethyl cellulose or the hydroxypropyl cellulose, and the consumption of this binding agent is the 0.8-3 weight % of positive active material.
The present invention also provides a kind of anode pole piece by above-mentioned manufacture method made.
The present invention also provides a kind of lithium rechargeable battery that comprises above-mentioned anode pole piece.
Anode pole piece by method making of the present invention, and stability test therefrom is good, distortion is less after long-term the use, be difficult for the generation swell and influence battery performance, have high safety and good cycle characteristics, make the comprehensive electrochemical properties excellence of battery, reduced cost simultaneously, environment is not polluted.
Embodiment
The manufacture method of anode slice of lithium ion battery provided by the invention comprises: (1) adds binding agent in the entry and dissolves; (2) positive active material is joined in the above-mentioned binding agent for preparing then and mix, be made into slurry; (3) the described slurry for preparing is applied on the collector, obtain the anode pole piece of lithium ion battery then through baking sheet, compressing tablet, cut-parts, described binding agent is selected from one or more in sodium carboxymethylcellulose, methylcellulose, hydroxypropyl methylcellulose, carboxymethyl hydroxyethyl cellulose or the hydroxypropyl cellulose, and the consumption of this binding agent is the 0.8-3 weight % of positive active material.
In the preferred embodiment of the present invention, described binding agent is a sodium carboxymethylcellulose, and this sodium carboxymethylcellulose is a kind of cationic linear polymeric material, and structural formula is expressed from the next:
The molecular weight of this sodium carboxymethylcellulose is 50,000-1, and 000,000, be preferably 100,000-700,000.
Described cell active materials can be selected any active material that is used for lithium rechargeable battery for use, is preferably nickel, cobalt and manganese oxide, the preferred LiCoxNiyMnzO of described nickel, cobalt and manganese oxide
2(0＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1), LiCoxNiyMnzO
2-kFk (wherein 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z=1,0＜k＜2), LiCoxNiyMnzM1-x-y-zO
2(wherein 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z＜1) or LiCoxNiyMnzM1-x-y-zO
2-kFk (wherein, 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z＜1,0＜k＜2).Wherein, more preferably LiCoxNiyMnzO
2, its 4.2 volts of theoretical capacities are 140 Milliampere Hour/grams, 4.4 volts of theoretical capacities are 170 Milliampere Hour/grams, apparent density (gram per centimeter
3)＞1.0, tap density (gram per centimeter
3)＞2.1, granularity (micron) is 5-15, specific area (rice
2/ gram) be 0.2-0.5.Owing to select above-mentioned cell active materials for use, can reduce battery cost, use with aqueous binders of the present invention, battery cost can be reduced greatly, thereby the still good battery product of price low performance can be obtained.
In described slurry, also contain conductive agent, described conductive agent is preferably one or more in carbon black, acetylene black and the electrically conductive graphite, weight with battery positive electrode active material is benchmark, the consumption of preferred conductive agent is 0.8-10 weight %, wherein, the consumption of preferred described carbon black is that the consumption of 0.8-3 weight %, described acetylene black is that the consumption of 3-6 weight %, described electrically conductive graphite is 2-10 weight %.
In the step (2) of the manufacture method of anode slice of lithium ion battery provided by the invention, battery positive electrode active material added in the binding agent for preparing mix, be made into slurry.Can adopt the method for prior art to carry out above-mentioned mixing and stirring, it is mixed.Can also add conductive agent, conductive agent can be before adding positive active material, add simultaneously afterwards or with positive active material, preferably is mixed into dry mixture with positive active material earlier and adds in the binding agent for preparing again and mix.
In the step (3) of the manufacture method of anode slice of lithium ion battery provided by the invention, the described slurry for preparing is applied on the collector, obtain anode slice of lithium ion battery through baking sheet, compressing tablet, cut-parts then.Can adopt existing slurry mode to be applied on the collector in the slurry for preparing, for example, can adopt the method for artificial coating, perhaps adopt the method that on tensile pulp machine, applies, the method that preferably on tensile pulp machine, applies.The drying condition of baking sheet is conventionally known to one of skill in the art, and bake out temperature is generally 50-160 ℃, preferred 80-150 ℃.Compressing tablet be meant will be coated with the active material that is covered with form fine and close coating, the degree of active material densification makes the density of active material meet the requirement of battery, the degree of active material densification is conventionally known to one of skill in the art.According to the difference of battery, the thickness that is coated with the collector that is covered with active material that obtains behind the compressing tablet can in very large range change, and for existing small-scale lithium ion cell, this thickness is generally the 0.08-0.15 millimeter.Described tabletting method can adopt existing tabletting method arbitrarily, as carry out the method for compressing tablet with rolling mill.Cut-parts refer to be covered with the collector for preparing slurry and cut being coated with, and the width that cuts makes the width of collector be suitable as electrodes of lithium-ion batteries.In general, the width that cuts can in very large range change according to the size of battery, as the width that cuts to make the width of the collector that applies spreading mass be the 10-200 millimeter, and along with the development of technology, can be wideer or narrower.The described method that cuts can adopt existing cutting method arbitrarily, as the method for aritificial cut-off or the method that cuts with cutting machine.Be not particularly limited forming anodal collector, can be plus plate current-collecting body conventional in the lithium ion battery, in specific embodiments of the present invention, use aluminium foil as plus plate current-collecting body.
The present invention will be described below in conjunction with embodiment.
The manufacture method of anode pole piece is made in the following examples explanation of binding agent of the present invention.
Embodiment 1
Take by weighing mean particle diameter D respectively
50Be 9 microns positive electrode active material LiCoxNiyMnzO
296 grams, binding agent sodium carboxymethylcellulose (CMC-Na) 0.96 gram, conductive agent graphite 2.88 grams, this graphite mean particle diameter D
50Be that 0.2 micron, resistivity are 5 * 10
-5Ohmcm, specific surface are 350 meters squared per gram.Above-mentioned sodium carboxymethylcellulose (CMC-Na) is added in the 48 gram deionized waters, use de-airing mixer stirring and dissolving 0.5 hour, mixing speed is 500 rev/mins, and CMC-Na is dissolved in the deionized water fully.
After above-mentioned conductive agent and positive electrode active material be mixed into dry mixture, add in the CMC-Na binding agent that has prepared, stirred 2 hours with de-airing mixer, mixing speed is 800 rev/mins, obtains mixed uniformly slurry.
It is on 14 microns electrode current collecting body aluminium foils that resulting electrode material slurry is coated to thickness with the tensile pulp machine slurry, and it is dry in 150 ℃ baking oven, and then dried anode pole piece rolled by roll squeezer, obtain thickness and be 60 microns anode pole piece, to obtain diameter be that 1 centimetre, thickness are 60 microns positive plate through cutting.
Embodiment 2
Positive electrode active material LiCoxNiyMnzO
296 grams, sodium carboxymethylcellulose (CMC-Na) 2.88 grams, conductive agent acetylene black 5.76 grams, deionized water 57.6 grams adopt the method for embodiment 1 to make the anode pole piece.
Embodiment 3
Positive electrode active material LiCoxNiyMnzO
298 grams, sodium carboxymethylcellulose (CMC-Na) 1.96 grams, conductive agent carbon black 0.98 gram, deionized water 49 grams adopt the method for embodiment 1 to make the anode pole piece.
Embodiment 4
Positive electrode active material LiCoxNiyMnzO
296 grams, sodium carboxymethylcellulose (CMC-Na) 2.88 grams, conductive agent acetylene black 2.88 grams, electrically conductive graphite 6.72 grams, deionized water 38.4 grams adopt the method for embodiment 1 to make the anode pole piece.
Embodiment 5
Adopt the method for embodiment 1 to make the anode pole piece, that different is positive electrode active material LiCoxNiyMnzO
2Consumption be 97.5 the gram, the consumption of CMC-Na be 1.46 the gram, conductive agent is a carbon black, consumption be 0.98 the gram.
Embodiment 6
Adopt the method for embodiment 1 to make the anode pole piece, that different is positive electrode active material LiCoxNiyMnzO
2Consumption be 95.5 the gram, the consumption of CMC-Na be 1.43 the gram, conductive agent is an acetylene black, consumption be 2.87 the gram.
Embodiment 7
Adopt the method for embodiment 1 to make the anode pole piece, that different is positive electrode active material LiCoxNiyMnzO
2Consumption be 95.5 grams, adopt methylcellulose (MC) as binding agent, consumption is 1.43 grams, conductive agent is a graphite, consumption is 2.87 grams.
Comparative example 1
Being averaged particle diameter respectively is D
50Be 9 microns positive electrode active material LiCoxNiyMnzO
293 grams, binding agent sodium carboxymethylcellulose (CMC-Na) 0.93 gram, conductive agent graphite 2.79 grams, this graphite mean particle diameter D
50Be that 0.2 micron, resistivity are 5 * 10
-5Ohmcm, specific surface are 350 meters squared per gram.Above-mentioned sodium carboxymethylcellulose (CMC-Na) dissolving is added in the 46.5 gram deionized waters, stirred 0.5 hour with de-airing mixer, mixing speed is 500 rev/mins, and CMC-Na is dissolved in the deionized water fully.
After above-mentioned conductive agent and positive electrode active material be mixed into dry mixture, add in the CMC-Na binding agent that has prepared, stirred 2 hours with de-airing mixer, mixing speed is 800 rev/mins, add polytetrafluoroethylene (PTFE) 2.79 grams (for 3 weight % of battery active matter) again, vacuum stirring 0.5 hour obtains mixed uniformly slurry.
The method of following making anode pole piece is identical with embodiment 1.
Comparative example 2
Adopt the method for comparative example 1 to make the anode pole piece, different is that polytetrafluoroethylene is replaced with butadiene-styrene rubber (SBR).
Embodiment 1-7 and comparative example 1-2 are carried out electric performance test, the results are shown in table 1.
Electric performance test
Making the lithium ion battery model is LP043048A, with 0.2C constant-current constant-voltage charging 4.4V, again with 0.2C constant-current discharge 3.0V.
Table 1
Above test result shows, the resultant battery of anode pole piece of embodiment of the invention 1-7 is very little in the increase of 500 circulation back cell thickness, only between 0.31-0.37, and the battery that the anode pole piece of comparative example 1-2 obtains is very big in the increase of 500 circulation back cell thickness, be 0.64 and 0.77, be about 2 times of the present invention.When therefore the anode pole piece of the inventive method making is used for battery, have highly stable electrical property, and good cycle.
The anode of the present invention manufacture method of binding agent and anode pole piece, make lithium rechargeable battery that good cycle performance, self discharge, high-temperature behavior, cryogenic property, security performance and its comprehensive electrochemical properties be arranged, the present invention is used on other size battery also can obtain same effect.
Claims (10)
1. the manufacture method of an anode slice of lithium ion battery, this manufacture method comprises: (1) adds binding agent in the entry and dissolves; (2) positive active material is joined in the above-mentioned binding agent for preparing then and mix, be made into slurry; (3) the described slurry for preparing is applied on the collector, obtain the anode pole piece of lithium ion battery then through baking sheet, compressing tablet, cut-parts, it is characterized in that, described binding agent is selected from one or more in sodium carboxymethylcellulose, methylcellulose, hydroxypropyl methylcellulose, carboxymethyl hydroxyethyl cellulose or the hydroxypropyl cellulose, and the consumption of this binding agent is the 0.8-3 weight % of positive active material weight.
2. manufacture method according to claim 1, described binding agent are sodium carboxymethylcellulose, and the molecular weight of this sodium carboxymethylcellulose is 50,000-1,000,000.
3. manufacture method according to claim 2, the molecular weight of described sodium carboxymethylcellulose are 100,000-700,000.
4. method according to claim 1 is characterized in that, the employed water yield is the 40-80 weight % of described positive active material in the step (1).
5. according to claim 1 or described method, it is characterized in that described positive active material is the oxide of nickel cobalt manganese.
6. method according to claim 5 is characterized in that, described positive active material is LiCoxNiyMnzO
2, 0＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1; LiCoxNiyMnzO
2-kFk, wherein 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z=1,0＜k＜2; LiCoxNiyMnzM1-x-y-zO
2, wherein 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z＜1; Perhaps LiCoxNiyMnzM1-x-y-zO
2-kFk, wherein, 0＜x＜1,0＜y＜1,0＜z＜1, and x+y+z＜1,0＜k＜2.
7. method according to claim 6 is characterized in that, described positive active material is LiCoxNiyMnzO
2, its tap density＞2.1 gram per centimeters
3, granularity is the 5-15 micron, specific area is a 0.2-0.5 rice
2/ gram.
8. method according to claim 1, it is characterized in that, comprise also in the described slurry that conductive agent, described conductive agent are one or more in carbon black, acetylene black and the electrically conductive graphite, weight with positive active material is benchmark, and the consumption of described conductive agent is 0.8-10 weight %.
9. anode slice of lithium ion battery of making by each described manufacture method of claim 1-8.
10. lithium rechargeable battery, this battery comprises the described anode pole piece of claim 8.
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|---|---|---|---|
| CNA2006101496461A CN101162773A (en) | 2006-10-13 | 2006-10-13 | Preparation method of battery positive plate, positive plate and lithium ionic cell |
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|---|---|---|---|
| CNA2006101496461A CN101162773A (en) | 2006-10-13 | 2006-10-13 | Preparation method of battery positive plate, positive plate and lithium ionic cell |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102088098A (en) * | 2011-01-10 | 2011-06-08 | 南京大学 | Preparation method of membrane electrode support layer of fuel cell |
| CN102569733A (en) * | 2010-12-21 | 2012-07-11 | 比克国际(天津)有限公司 | Preparation method for lithium ion battery slurry, as well as battery slurry and lithium ion battery |
| CN102916197A (en) * | 2012-10-29 | 2013-02-06 | 清华大学深圳研究生院 | Current collector, preparation method of current collector, lithium-ion battery electrode sheet and lithium-ion battery |
| CN103151494A (en) * | 2012-07-09 | 2013-06-12 | 深圳市海太阳实业有限公司 | Preparation method of battery pole piece, the battery pole piece and battery |
| CN103515647A (en) * | 2012-06-29 | 2014-01-15 | 丰田自动车株式会社 | Non-aqueous electrolyte secondary battery pack and method for manufacturing the same |
| CN103682257A (en) * | 2013-12-27 | 2014-03-26 | 安徽亿诺新能源有限责任公司 | Preparation process for anode and cathode of lithium secondary battery |
| CN105762353A (en) * | 2016-04-08 | 2016-07-13 | 远东福斯特新能源有限公司 | Lithium-ion battery with high-nickel ternary aqueous positive electrode and preparation method thereof |
| CN108232152A (en) * | 2017-12-29 | 2018-06-29 | 银隆新能源股份有限公司 | A kind of battery anode slurry, anode and battery |
| CN109728350A (en) * | 2018-12-20 | 2019-05-07 | 福建师范大学 | The preparation method of the monolithic cell battery core of aqueous systems hydroxypropyl methyl cellulose |
| CN114792804A (en) * | 2022-04-28 | 2022-07-26 | 北京理工大学重庆创新中心 | 3D printing positive electrode ink, and positive electrode forming method and application applying same |
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| CN102569733A (en) * | 2010-12-21 | 2012-07-11 | 比克国际(天津)有限公司 | Preparation method for lithium ion battery slurry, as well as battery slurry and lithium ion battery |
| CN102569733B (en) * | 2010-12-21 | 2016-03-09 | 比克国际(天津)有限公司 | The preparation method of pulp of lithium ion battery, cell size and lithium ion battery |
| CN102088098A (en) * | 2011-01-10 | 2011-06-08 | 南京大学 | Preparation method of membrane electrode support layer of fuel cell |
| CN103515647A (en) * | 2012-06-29 | 2014-01-15 | 丰田自动车株式会社 | Non-aqueous electrolyte secondary battery pack and method for manufacturing the same |
| CN103151494B (en) * | 2012-07-09 | 2015-08-19 | 深圳市海太阳实业有限公司 | A kind of preparation method of battery pole piece and battery pole piece, battery |
| CN103151494A (en) * | 2012-07-09 | 2013-06-12 | 深圳市海太阳实业有限公司 | Preparation method of battery pole piece, the battery pole piece and battery |
| CN102916197A (en) * | 2012-10-29 | 2013-02-06 | 清华大学深圳研究生院 | Current collector, preparation method of current collector, lithium-ion battery electrode sheet and lithium-ion battery |
| CN103682257A (en) * | 2013-12-27 | 2014-03-26 | 安徽亿诺新能源有限责任公司 | Preparation process for anode and cathode of lithium secondary battery |
| CN105762353A (en) * | 2016-04-08 | 2016-07-13 | 远东福斯特新能源有限公司 | Lithium-ion battery with high-nickel ternary aqueous positive electrode and preparation method thereof |
| CN108232152A (en) * | 2017-12-29 | 2018-06-29 | 银隆新能源股份有限公司 | A kind of battery anode slurry, anode and battery |
| CN109728350A (en) * | 2018-12-20 | 2019-05-07 | 福建师范大学 | The preparation method of the monolithic cell battery core of aqueous systems hydroxypropyl methyl cellulose |
| CN114792804A (en) * | 2022-04-28 | 2022-07-26 | 北京理工大学重庆创新中心 | 3D printing positive electrode ink, and positive electrode forming method and application applying same |
| CN114920853A (en) * | 2022-06-29 | 2022-08-19 | 重庆力宏精细化工有限公司 | Flexible carboxymethyl cellulose ether and preparation method and application thereof |
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