WO2011105348A1 - Procédé de séchage de film de revêtement d'électrode pour batterie au lithium-ion - Google Patents

Procédé de séchage de film de revêtement d'électrode pour batterie au lithium-ion Download PDF

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Publication number
WO2011105348A1
WO2011105348A1 PCT/JP2011/053776 JP2011053776W WO2011105348A1 WO 2011105348 A1 WO2011105348 A1 WO 2011105348A1 JP 2011053776 W JP2011053776 W JP 2011053776W WO 2011105348 A1 WO2011105348 A1 WO 2011105348A1
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WO
WIPO (PCT)
Prior art keywords
coating film
drying
electrode
binder
temperature
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Application number
PCT/JP2011/053776
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English (en)
Japanese (ja)
Inventor
道郎 青木
良夫 近藤
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日本碍子株式会社
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Publication date
Application filed by 日本碍子株式会社 filed Critical 日本碍子株式会社
Priority to JP2011522715A priority Critical patent/JP4801233B1/ja
Publication of WO2011105348A1 publication Critical patent/WO2011105348A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • 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

Definitions

  • the present invention relates to a method for drying an electrode coating film for a lithium ion battery in the production process of the lithium ion battery.
  • an active material powder which is a positive electrode material or a negative electrode material
  • a metal sheet such as aluminium or copper
  • a coating film having a thickness of about 100 ⁇ m is formed and then dried.
  • the electrode material is generally lithium cobaltate as a positive electrode material, PVDF as a binder, carbon as a conductive material, and NMP as a solvent.
  • the binder has a role of bonding the electrode material and the conductive material in the dried electrode. For this reason, in order to improve the performance of the lithium ion battery, it is desirable that the distribution in the thickness direction of the binder in the electrode after drying is as uniform as possible.
  • the solvent concentration decreased only in the surface layer portion at a relatively early stage of drying, and the binder was fixed there.
  • the drying speed and the uniform distribution of the binder after drying are also in conflict, and there is an inherent dilemma between productivity and quality improvement. It was.
  • the binder concentration is relatively high in the lower layer in direct contact with the aluminum sheet. As described above, the binder concentration of the surface layer increases as the solvent evaporates. On the other hand, since the binder concentration is low in the middle layer, the bonding strength of the intermediate layer is reduced. As a result, the surface of the electrode after drying is easily peeled off from the aluminum sheet, and there is a risk of peeling or cracking during the winding operation of the aluminum sheet performed during battery assembly. In order to avoid this problem, if the binder concentration is increased, the amount of the electrode material is relatively reduced, which causes a decrease in battery output.
  • Patent Document 1 proposes a method in which the drying process is divided into a plurality of processes having different coating film temperatures.
  • the heating means for drying may be an infrared heater, hot air, or dielectric heating.
  • drying by an infrared heater is performed relatively uniformly in the entire coating film because infrared rays reach the inside of the coating film, but drying by hot air is performed only from the surface layer, and the inside is mainly heated. Since it is heated by conduction, the behavior of the solvent and binder during the drying process is greatly different. For this reason, the method of Patent Document 1 focusing only on the drying temperature of the coating film still cannot sufficiently equalize the distribution in the thickness direction of the binder in the electrode.
  • the object of the present invention is to solve the above-mentioned conventional problems, and by appropriately using the drying means, the binder distribution in the thickness direction in the electrode after drying is made more uniform than in the past, and the peeling of the electrode and the occurrence of cracks are caused. It is providing the drying method of the electrode coating film for lithium ion batteries which can be prevented.
  • the method for drying an electrode coating film for a lithium ion battery according to the present invention made to solve the above-described problems is obtained by applying an electrode material paste containing an electrode agent, a binder, a conductive material, and a solvent on a metal sheet.
  • a method for drying an electrode coating film for a battery comprising an initial stage in which the coating film temperature is quickly raised, and an intermediate stage in which the entire coating film is heated by hot air and infrared irradiation at a temperature lower than the sheet temperature.
  • the boundary between the stage and the middle stage is a period when the electrode agent is exposed on the surface.
  • the electrode material is lithium cobalt oxide as a positive electrode material
  • the binder is PVDF
  • the conductive material is carbon powder
  • the solvent is NMP.
  • the aim of the method for drying an electrode coating film for a lithium ion battery in the present invention is to maintain a liquid phase inside the coating film at a high concentration and a high temperature as much as possible while ensuring the necessary solvent evaporation rate, particularly from the initial stage to the middle stage of drying. It is to secure a long time and to reversely diffuse the binder from the surface layer to the middle layer or lower during that period.
  • the binder is initially dissolved in a solvent, and electrode agent particles exist in the mixed solution. Since the evaporation of the solvent that occupies the main part of the mixture proceeds in order from the surface layer, the mixture liquid mass fraction based on the electrode agent mass in the surface layer decreases early, and between the mixture liquid mass fraction in the lower layer Differences occur.
  • This difference is a kind of concentration difference, which becomes a driving force, and the liquid mixture sequentially moves from the lower layer to the upper layer by diffusion. Therefore, the binder dissolved in this also inevitably gathers on the surface layer.
  • the binder cannot evaporate, the result is that the binder concentration has a distribution with the surface layer as the apex within the coating thickness.
  • the concentration difference becomes a driving force, and this time, the binder is diffused from the surface layer to the lower layer, that is, in the direction opposite to the diffusion of the whole liquid mixture.
  • This phenomenon is called despreading in the present invention.
  • the above two types of diffusion are considered to occur almost simultaneously. In particular, controlling the latter despreading is the key to realizing uniform binder concentration.
  • the coating film temperature is quickly raised by hot air spraying and infrared heating.
  • the above-mentioned period is extended ahead.
  • the entire coating film is heated by infrared irradiation while controlling the sheet temperature to be below the allowable temperature with hot air lower than the sheet temperature. To do. This makes it possible to ensure a long period during which the evaporation rate is constant and the coating film temperature is maintained at a relatively high temperature without excessively rising. During that period, binder despreading is promoted.
  • the absorption of the infrared rays inside the coating film does not form a continuous film due to the binder deposited on the surface, and the evaporation of the solvent can proceed from the inside of the coating film through the surface electrode materials.
  • the present invention is a method for drying an electrode coating film for a lithium ion battery in which an electrode material paste containing an electrode material, a binder, a conductive material, and a solvent is applied onto a metal sheet such as an aluminum sheet.
  • a metal sheet such as an aluminum sheet.
  • lithium cobaltate is used as the electrode material for the positive electrode, but lithium nickelate or lithium manganate may be used.
  • the electrode material for the negative electrode is, for example, graphite. These are all fine powders.
  • the binder is a component for adhering the electrode material and the carbon powder as the conductive material as described above.
  • the binder is PVDF (polyvinylidene fluoride).
  • the solvent in this embodiment is NMP (N-methyl-pyrrolidone).
  • the kind of the binder and the solvent is not limited to this, and various known substances can be used as the constituent material of the electrode coating film for the lithium ion battery.
  • FIG. 1 is a schematic diagram showing the state, in which 1 is a metal sheet, 2 is a coating film, 3 is an electrode material, 4 is a conductive material, and 5 is a solvent. In this state, the binder is dissolved in the solvent.
  • hot air is blown onto the surface of the coating film 2 and infrared heating is performed.
  • a general infrared heater can be used as the heating means. Since the thickness of the coating film 2 is about 200 ⁇ m at the maximum, the infrared rays reach the inside thereof, and the coating film 2 is also heated from the inside.
  • the temperature of the infrared heating is about 250 to 330 ° C., and the internal temperature of the coating film 2 is raised at an early stage.
  • the temperature of the hot air is preferably a medium temperature of about 110 to 120 ° C., and it is a weak wind.
  • the solvent starts to evaporate from the surface of the coating film 2, and the solvent and the binder flow from the inside of the coating film 2 toward the surface layer, so that the binder concentration in the surface layer inevitably increases.
  • the solvent starts to evaporate from the surface of the coating film 2, and the electrode material 3 appears on the surface and shifts from the initial stage of drying to the middle stage of drying.
  • the entire coating film is heated by infrared heating while preventing overheating of the surface layer with hot air lower than the sheet temperature.
  • This period overlaps with the main period of solvent evaporation, and is also the main period during which binder reverse diffusion is possible because the difference in the binder concentration between the surface layer and the middle layer increases.
  • the factor governing the binder reverse diffusion rate other than the concentration difference is the diffusion coefficient, which depends on the temperature. The higher the coating temperature, the larger the diffusion coefficient, and the higher the diffusion rate.
  • the effective reverse diffusion period can be kept longer and further as high as possible by a combination of infrared heating and convection cooling. Can be realized.
  • the temperature of the hot air may be a low temperature of about 90 to 100 ° C., and the wind speed may be stronger than the initial stage of drying. As shown in FIG. 7, the wind speed contributes to the constant evaporation rate, and can be appropriately changed depending on the coating film physical properties of the sheet.
  • the infrared heating temperature is preferably a high temperature of the initial set temperature ⁇ 20 ° C.
  • the surface layer side binder is changed to the middle layer side by utilizing the binder concentration difference inside the coating film 2.
  • the surface layer of the coating film 2 is controlled in evaporation speed by low temperature and strong air blowing, but even if the solvent concentration is lowered, the solvent is evaporated through the surface electrode materials 3 and 3 by the internal absorption of infrared rays. It progresses from the inside of the coating film. The evaporated solvent is quickly removed by the wind.
  • the concentration of the solvent is below the allowable value, it may be cooled as it is, but in order to improve the quality, the infrared heating is relaxed. It is preferable to add an end of drying in which the hot air temperature is further lowered.
  • a preferable infrared heating temperature at the end of drying is a low temperature of 200 to 250 ° C.
  • a hot air temperature is a low temperature of 80 to 90 ° C.
  • a wind speed is a strong wind. This completes evaporation of the solvent from the interior of the coating film 2 and prevents overheating of the surface.
  • the binder distribution in the thickness direction is made more uniform than before, and it is possible to prevent electrode peeling and cracking even in the step of winding an aluminum sheet.
  • the infrared heater is not used in the third zone. In such a case, it is effective to increase the hot air temperature to about 120 to 130 ° C.
  • FIGS. 4 and 5 show graphs of the temperature of the coating film when the drying is performed only with hot air and the amount of solvent transfer to the surface layer
  • FIGS. 6 and 7 show the coating film when the drying is performed according to the present invention.
  • the graph of the temperature of this and the amount of solvent movement to the surface layer is shown.
  • Each horizontal axis is time (s).
  • the heating with only hot air causes a gradual rise in temperature, and the period during which the solvent movement to the surface layer is accelerated, which is correlated with the surface layer evaporation promotion period and the binder reverse diffusion period, is short-pointed.
  • an electrode coating film for a lithium ion battery was prepared by applying an electrode material paste containing an electrode material, a binder, a conductive material, and a solvent on an aluminum sheet having a thickness of 20 ⁇ m and a width of 200 mm to a thickness of 80 ⁇ m.
  • an extrusion type nozzle was used as in Patent Document 1.
  • an apparatus including an infrared heater 10 and a hot air chamber 11 for sending hot air to a roll-to-roll roll apparatus having a furnace length of 12 m as shown in FIG. 8 was used. Moreover, from the hot air chamber 11, the apparatus which can control the hot air of the upper direction and the downward hot air which are shown in figure was used.
  • the temperature of the infrared heater 10 was set to the same temperature in the coating width direction, and the following conditions were used in the coating film transport direction.
  • the hot air the upper hot air was defined as the upper hot air
  • the lower hot air was defined as the lower hot air.
  • Table 1 shows the method of the present invention
  • Table 2 shows a comparative example using only hot air. Note Table 1, the air volume 19.5 m 3 / min in Table 2, 12m 3 / min, respectively correspond to the air speed of about 6.5m / s and about 4m / s.
  • 1 zone was the initial state
  • 2 zones were in the mid-term state
  • 3 zones, and 4 zones were in the final state.
  • the medium-term state is a stage where the electrode material appears on the surface.
  • the detection method the reflectivity of the surface changes as the coating film becomes thinner, and the reflectivity hardly changes after the electrode material appears on the surface. Transition to state control.
  • the transition to the final state is intended to promote evaporation in consideration of mass productivity and the like, and can be appropriately set as long as the reverse diffusion state in the intermediate state can be secured for a certain period.
  • Table 3 shows the results of measuring the residual amount of the solvent and the mass fraction of the binder for the surface layer, middle layer and lower layer of the electrode obtained by drying the coating film by the method of the present invention and the method of the comparative example as described above. Summarized. The defect rate was indicated by the number of peeling or cracking that occurred during the 200 m electrode winding operation.
  • the binder distribution in the thickness direction in the electrode after drying is made more uniform than before by properly using a drying means, There is an advantage that electrode peeling and cracking can be prevented.

Abstract

L'invention concerne un procédé de séchage de film de revêtement d'électrode pour batterie au lithium-ion dans lequel une pâte de matière d'électrode contenant une matière d'électrode (3), un liant, une matière conductrice (4), et un solvant (5), est appliquée sur une feuille métallique (1), puis séchée. En début de séchage, un air chaud est soufflé sur la surface du film de revêtement et un chauffage par infrarouge est effectué, élevant ainsi de manière rapide la température du film de revêtement. En milieu de séchage, lorsque la matière d'électrode (3) commence à apparaître en surface, tout en régulant la température de la feuille au moyen d'un air chaud de température plus basse que celle de la feuille, l'ensemble du film de revêtement est chauffé par irradiation d'infrarouge, et tout en rétrodiffusant côté couche intermédiaire le liant situé côté couche de surface à l'aide de la différence de concentration de liant dans la partie interne du film de revêtement, l'évaporation du solvant continue à partir de la partie interne du film de revêtement principalement à travers la matière d'électrode située côté surface.
PCT/JP2011/053776 2010-02-26 2011-02-22 Procédé de séchage de film de revêtement d'électrode pour batterie au lithium-ion WO2011105348A1 (fr)

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JP2010-041218 2010-02-26

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JP2013219012A (ja) * 2012-03-15 2013-10-24 Hitachi Ltd 非水二次電池用電極の製造方法、非水二次電池および乾燥装置
WO2014083950A1 (fr) * 2012-11-29 2014-06-05 株式会社日立製作所 Batterie secondaire au lithium-ion et procédé de production associé
JP2016152181A (ja) * 2015-02-19 2016-08-22 日立マクセル株式会社 非水二次電池用負極の製造方法、および非水二次電池の製造方法
CN107438914A (zh) * 2015-04-07 2017-12-05 株式会社Lg 化学 电极及其制造方法
JP2019012709A (ja) * 2018-10-30 2019-01-24 マクセルホールディングス株式会社 非水二次電池用負極の製造方法、および非水二次電池の製造方法
JP2021018964A (ja) * 2019-07-24 2021-02-15 トヨタ自動車株式会社 電極塗膜の乾燥方法

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JP5282148B2 (ja) * 2011-03-18 2013-09-04 株式会社日立製作所 電極及びその製造方法
CN102607240B (zh) * 2012-03-06 2014-07-23 宁德新能源科技有限公司 一种锂离子电池极片的干燥设备及方法
JP5325332B1 (ja) * 2012-12-28 2013-10-23 日本碍子株式会社 電池用電極塗膜の乾燥方法及び乾燥炉
KR101769186B1 (ko) * 2014-12-23 2017-08-17 주식회사 엘지화학 리튬 이차전지용 양극의 제조방법, 이를 이용하여 제조한 양극, 및 이를 포함하는 리튬 이차전지
KR102245127B1 (ko) 2018-01-08 2021-04-28 주식회사 엘지화학 전극기재의 건조 상태를 모니터링하는 방법 및 장치
DE102019210865B3 (de) * 2019-07-23 2020-12-31 Vitesco Technologies Germany Gmbh Verfahren zur Herstellung einer Polymerschicht auf einer Komposit-Elektrodenschicht

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Publication number Priority date Publication date Assignee Title
JP2013219012A (ja) * 2012-03-15 2013-10-24 Hitachi Ltd 非水二次電池用電極の製造方法、非水二次電池および乾燥装置
WO2014083950A1 (fr) * 2012-11-29 2014-06-05 株式会社日立製作所 Batterie secondaire au lithium-ion et procédé de production associé
JP2014107182A (ja) * 2012-11-29 2014-06-09 Hitachi Ltd リチウムイオン二次電池及びその製造方法
JP2016152181A (ja) * 2015-02-19 2016-08-22 日立マクセル株式会社 非水二次電池用負極の製造方法、および非水二次電池の製造方法
CN107438914A (zh) * 2015-04-07 2017-12-05 株式会社Lg 化学 电极及其制造方法
CN107438914B (zh) * 2015-04-07 2020-11-13 株式会社Lg 化学 电极及其制造方法
JP2019012709A (ja) * 2018-10-30 2019-01-24 マクセルホールディングス株式会社 非水二次電池用負極の製造方法、および非水二次電池の製造方法
JP2021018964A (ja) * 2019-07-24 2021-02-15 トヨタ自動車株式会社 電極塗膜の乾燥方法
JP7157912B2 (ja) 2019-07-24 2022-10-21 トヨタ自動車株式会社 電極塗膜の乾燥方法

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TW201205932A (en) 2012-02-01
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