CN111477841A - Lithium battery pole piece and preparation method thereof - Google Patents
Lithium battery pole piece and preparation method thereof Download PDFInfo
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- CN111477841A CN111477841A CN202010457167.6A CN202010457167A CN111477841A CN 111477841 A CN111477841 A CN 111477841A CN 202010457167 A CN202010457167 A CN 202010457167A CN 111477841 A CN111477841 A CN 111477841A
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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
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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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
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0419—Methods of deposition of the material involving spraying
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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
- H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
Abstract
The application provides a lithium battery pole piece and a preparation method thereof, wherein the lithium battery pole piece comprises a current collector and a coating layer positioned on the surface of the current collector, the coating layer comprises active metal ions, and the mole percentage content of the active metal ions is increased or reduced in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector. The lithium battery pole piece of the technical scheme has high capacity, high stability and high safety.
Description
Technical Field
The application relates to the field of lithium batteries, in particular to a lithium battery pole piece and a preparation method thereof.
Background
The pole piece of the lithium battery is an important component of the lithium battery, and the service life and the safety performance of the lithium battery are influenced. At present, a wet pulping process is generally adopted to prepare the pole piece, and although the method has the advantages of short time consumption, good slurry fluidity, less bubbles, high production efficiency and the like, the method also has the problems of high energy consumption, large internal resistance of the pole piece, poor high-temperature performance, pollution and the like. Meanwhile, the surface area of the conductive agent is large, so that the conductive agent can absorb the solvent easily, the mobility of the solvent is poor, and the added active substances are not easy to disperse uniformly. In addition, the solvent and the binder form a binder layer to coat the surface of the active material particles, which hinders the contact between the active material particles and the conductive agent, so that the electrode plate has poor conductivity, and the residual solvent in the electrode plate can generate side reaction with the electrolyte, which causes the performance reduction of the battery cell, such as capacity reduction, gas generation, life decay and the like.
In recent years, novel lithium ion ternary materials are applied to the preparation of lithium battery pole pieces, wherein the industrialization of high nickel materials is basically realized due to the remarkable characteristics of high capacity and the like, but the problems exist, such as serious cation mixed discharge phenomenon, poor interface stability and storage performance, L iOH on the surface of the materials can react with electrolyte to generate corrosive HF which corrodes the inside of a battery and damages an SEI film, transition metals enter a lithium ion layer through adjacent vacancies in the charging and discharging process to cause the crystal phase transformation of the material structure, so that the particle volume shrinkage change of the materials is large, cracks are generated on the surface and inside of the materials, the cracks can contact with the electrolyte to generate more side reactions, and the stability, the cycle performance and the like of the whole battery are influenced.
Disclosure of Invention
The technical problem to be solved by the application is to provide a lithium battery pole piece and a preparation method thereof, which can improve the capacity, stability and safety of the lithium battery pole piece.
In order to solve the technical problem, the application provides a lithium battery pole piece, which comprises a current collector and a coating layer located on the surface of the current collector, wherein the coating layer comprises active metal ions, and the mole percentage content of the active metal ions is increased or reduced in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector.
In an embodiment of the present application, the coating layer includes at least two sub-coating layers, the sub-coating layers include active materials, and the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in the active materials included in the sub-coating layers is.
In an embodiment of the present application, the active species comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, magnesium ions, titanium ions, tungsten ions, iron ions, and copper ions.
In an embodiment of the present application, the active material includes at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, lithium manganese rich.
In an embodiment of the application, the active material includes lithium nickel cobalt manganese oxide, and the closer to the current collector, the larger the mole percentage content of nickel ions is, the smaller the mole percentage content of cobalt ions and manganese ions is in the lithium nickel cobalt manganese oxide contained in the sub-coating layer.
In an embodiment of the application, the sub-coating layer further includes a binder and a conductive agent, wherein the active material is 88-97% by mass, the binder is 1-6% by mass, and the conductive agent is 1-6% by mass.
In embodiments of the present application, the binder comprises at least one of polyvinylidene fluoride, polytetrafluoroethylene, and polymethacrylic polymer.
In an embodiment of the present application, the conductive agent includes at least one of acetylene black, conductive graphite, graphene, carbon black, a single-arm carbon tube, a multi-arm carbon tube, and a carbon fiber, and the material of the current collector includes at least one of aluminum, nickel, copper, a carbon-coated aluminum foil, an aluminum alloy, and polyethylene terephthalate.
The application also provides a preparation method of the lithium battery pole piece, which comprises the following steps: mixing an active material, a binder and a conductive agent to form a mixed material; coating the mixed material on a current collector to form a coating layer, wherein the molar percentage content of active metal ions in the coating layer is increased or decreased in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector; and rolling the coating layer on the current collector to form a pole piece.
In an embodiment of the present application, the active material, binder and conductive agent are mixed to form at least two sub-mixes, and each sub-mix comprises a different mole percent content of active metal ions.
In an embodiment of the present application, the mixture is coated on a current collector to form a coating layer, including: and coating each sub-mixture on the current collector to form at least two sub-coating layers, wherein the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in active substances contained in the sub-coating layers is.
In the embodiments of the present application, after each formation of one sub-coating layer, the formed sub-coating layer is rolled on the current collector.
In an embodiment of the present application, the active species comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, magnesium ions, titanium ions, tungsten ions, iron ions, and copper ions.
In an embodiment of the present application, the active material includes at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, lithium manganese rich.
In an embodiment of the application, the active material includes lithium nickel cobalt manganese oxide, and the closer to the current collector, the larger the mole percentage content of nickel ions is, the smaller the mole percentage content of cobalt ions and manganese ions is in the lithium nickel cobalt manganese oxide contained in the sub-coating layer.
In the embodiment of the application, in the mixed material, the mass fraction of the active substance is 88-97%, the mass fraction of the binder is 1-6%, and the mass fraction of the conductive agent is 1-6%.
In embodiments of the present application, the binder comprises at least one of polyvinylidene fluoride, polytetrafluoroethylene, and polymethacrylic polymer.
Compared with the prior art, the technical scheme of the application has the following beneficial effects:
according to the lithium battery pole piece in the technical scheme, the distribution mode that the mol percentage content of active metal ions contained in the coating layer is designed to be increased or reduced in a gradient mode from the surface of the current collector to the direction far away from the surface of the current collector can be ensured, and the high capacity, the high safety and the stability of the pole piece can be realized under the condition that components in the coating layer are homogeneous.
Further, by designing the coating layer to be a laminated structure including at least two sub-coating layers, and the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in the active material contained in the sub-coating layers is, the larger or smaller the molar percentage content of active metal ions in the entire coating layer is, so that the gradient increase or decrease in the molar percentage content of active metal ions in the entire coating layer is realized, and further, the high capacity, high safety and stability of the pole piece are realized.
Common ternary or quaternary materials can be used as the active material in the technical scheme of the application, and the specific capacity, safety and stability of the pole piece can be improved only by adjusting the molar percentage content of the active metal ions of the active material in each sub-coating layer, so that the problem that the active material cannot be distributed in a gradient manner in the industry at present is effectively solved.
As the ternary or quaternary material is doped with metal elements (such as Mg, Al, Ti, Zr, Cu, W and the like), microcracks generated by volume expansion of the material in the charging and discharging process due to different excessive element concentration distributions of interfaces among the sub-coating layers can be effectively reduced, and the cycle stability and the thermal stability of the pole piece are further improved.
Furthermore, the active material comprises nickel cobalt lithium manganate, the closer to the current collector, the higher the mole percentage content of nickel ions in the nickel cobalt lithium manganate contained in the sub-coating layer is, the smaller the mole percentage content of cobalt ions and manganese ions is, so that the nickel content in the inner layer of the pole piece is higher, and high capacity can be provided; the nickel content of the outer layer of the pole piece is low, and the cobalt and manganese content is high, so that the decomposition of electrolyte on the surface of the electrode can be effectively inhibited, and the stability of an electrode/electrolyte interface and the long cycle performance of the battery are improved.
According to the preparation method of the lithium battery pole piece, dry materials are mixed, an organic solvent is not required to be added, and the conditions that the fluidity of the solvent is poor and the active substances are not uniformly dispersed due to the fact that the conductive agent absorbs the solvent are avoided; the problem that in the prior art, the solvent is easy to form an adhesive layer with the adhesive to prevent the contact between the active material particles and the conductive agent particles, so that the conductivity of the electrode plate is poor is solved; meanwhile, the problem that the performance of the battery cell is reduced due to the side reaction of residual solvent in the pole piece and electrolyte is avoided. Compared with the existing wet process, the dry process does not need the steps of dissolving the organic solvent and drying again, namely, drying equipment and solvent recovery equipment are saved in the production process.
The coating layer with the laminated structure is formed by adopting a mode of multiple coating and rolling, so that the thickness of the pole piece is obviously increased, the contact among the active substance, the binder and the conductive agent is tighter, and the prepared pole piece has high density, good conductivity and high capacity. Meanwhile, the toughness of the pole piece is good, the carbon powder is not easy to fall off, and the cycle life is long.
Because the binder adopted by the technical scheme of the application comprises at least one of polyvinylidene fluoride, polytetrafluoroethylene and polymethacrylic acid polymers, and the binders have no bonding property or weak bonding property at normal temperature, active substances, the binder and the conductive agent can be easily and uniformly mixed during dry mixing, and the binder can exert excellent bonding property during subsequent hot rolling and calendering operation on the coating layer.
The dry method is used for spraying the mixed material of ternary materials (NMC or NCA) containing active metal ions (such as nickel ions, cobalt ions, manganese ions or aluminum ions) with different mole percentage contents on a current collector in sequence, and then calendering to form a pole piece with concentration gradient, thereby effectively solving the problem that the gradient distribution of active substances cannot be realized in the current industry.
Drawings
The following drawings describe in detail exemplary embodiments disclosed in the present application. Wherein like reference numerals represent similar structures throughout the several views of the drawings. Those of ordinary skill in the art will understand that the present embodiments are non-limiting, exemplary embodiments and that the accompanying drawings are for illustrative and descriptive purposes only and are not intended to limit the scope of the present application, as other embodiments may equally fulfill the inventive intent of the present application. It should be understood that the drawings are not to scale. Wherein:
fig. 1 is a schematic cross-sectional structure diagram of a lithium battery pole piece according to an embodiment of the present application;
fig. 2 is a schematic view of a preparation process of a lithium battery pole piece according to an embodiment of the present application.
Detailed Description
The following description is presented to enable any person skilled in the art to make and use the present disclosure, and is provided in the context of a particular application and its requirements. Various modifications to the disclosed embodiments will be readily apparent to those skilled in the art, and the general principles defined herein may be applied to other embodiments and applications without departing from the spirit and scope of the present application. Thus, the present application is not limited to the embodiments shown, but is to be accorded the widest scope consistent with the claims.
The technical solution of the present application will be described in detail below with reference to the embodiments and the accompanying drawings.
As shown in fig. 1, the embodiment of the present application provides a lithium battery pole piece, the lithium battery pole piece includes a current collector 1 and a coating layer 2 located on the surface of the current collector 1, the coating layer 2 includes active metal ions, and the mole percentage content of the active metal ions increases or decreases in a gradient manner from the surface of the current collector 1 to a direction away from the surface of the current collector 1. By designing the distribution mode of the active metal ions in the coating layer, the high capacity, the high safety and the stability of the pole piece can be realized under the condition of ensuring the homogeneity of components in the coating layer 2.
In some embodiments, the coating layer 2 may include at least two sub-coating layers, where the sub-coating layers include active materials, and the closer to the current collector 1, the larger or smaller the molar percentage content of active metal ions in the active materials included in the sub-coating layers is, the larger or smaller the molar percentage content of active metal ions in the entire coating layer is, the more or smaller the molar percentage content of active metal ions in the entire coating layer is, and thus, the high capacity, the high safety and the stability of the pole piece are achieved. Fig. 1 shows a case where the coating layer 2 comprises three sub-coating layers. In other embodiments, the coating layer 2 may further include two sub-coating layers, four sub-coating layers, or more sub-coating layers, etc.
The active substance can be a common ternary or quaternary material, and the specific capacity, safety and stability of the pole piece can be improved only by adjusting the molar percentage content of the active metal ions of the active substance in each sub-coating layer, so that the problem that the active substance cannot be distributed in a gradient manner in the industry at present is effectively solved. And common ternary or quaternary materials are doped with metal elements (such as Mg, Al, Ti, Zr, Cu, W and the like), so that microcracks generated by volume expansion of materials in the charging and discharging process due to different excessive element concentration distributions of interfaces among all sub-coating layers can be effectively reduced, and the cycle stability and the thermal stability of the pole piece are further improved.
In some embodiments, the active species comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, magnesium ions, titanium ions, tungsten ions, iron ions, and copper ions. The active metal ions may be provided by common ternary or quaternary materials, such as at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, lithium rich manganese.
In some embodiments, the active may be encapsulatedLithium nickel cobalt manganese (NMCx)1y1z1) And the closer to the current collector 1, the greater the molar percentage content of nickel ions (Ni) in the sub-coating layer, and the smaller the molar percentage content of cobalt ions (Co) and manganese ions (Mn). The closer to the current collector 1, the greater the molar percentage content of nickel ions, the higher the capacity can be provided; the farther away from the current collector 1, the smaller the mole percentage content of nickel ions, and the larger the mole percentage content of manganese ions and cobalt ions, the higher the safety and stability of the pole piece.
In the examples of the present application, the formula NMCx1y1z1X in (2)1y1z1The approximate molar ratio of Ni, Co and Mn elements in the nickel cobalt lithium manganate is represented. For example, NMC811 refers to the approximate molar ratio of Ni, Co and Mn elements in nickel cobalt lithium manganate of 8: 1, NMC523 refers to the approximate molar ratio of Ni, Co and Mn elements in nickel cobalt lithium manganate of 5: 2: 3, and NMC111 refers to the approximate molar ratio of Ni, Co and Mn elements in nickel cobalt lithium manganate of 1: 1.
With continued reference to fig. 1, the coating layer 2 may have a three-layer structure, for example, including a first sub-coating layer 21 on the surface of the current collector 1, a second sub-coating layer 22 on the surface of the first sub-coating layer 21, and a third sub-coating layer 23 on the surface of the second sub-coating layer 22. Wherein the first sub-coating layer 21 includes an active material NMC811, the second sub-coating layer 22 includes an active material NMC523, and the third sub-coating layer 23 includes an active material NMC 111. From the first sub-coating layer 21 to the third sub-coating layer 23 (i.e. in a direction away from the surface of the current collector 1), the mole percentage content of nickel ions is gradually reduced, and the mole percentage content of cobalt ions and manganese ions is gradually increased, which is beneficial to improving the capacity of the pole piece, and the safety and stability of the pole piece.
In some embodiments, the coating layer 2 may also include four sub-coating layers, namely, a first sub-coating layer located on the surface of the current collector, a second sub-coating layer located on the surface of the first sub-coating layer, a third sub-coating layer located on the surface of the second sub-coating layer, and a fourth sub-coating layer located on the surface of the third sub-coating layer, where the material of the first sub-coating layer includes NCM811, the material of the second sub-coating layer includes NCM622, the material of the third sub-coating layer includes NCM523, and the material of the fourth sub-coating layer includes NCM111, where from the first sub-coating layer to the fourth sub-coating layer (i.e., in a direction away from the surface of the current collector), the mole percentage content of nickel ions gradually decreases, and the mole fraction content of cobalt ions and manganese ions gradually increases.
In other embodiments, the coating layer 2 may also be a two-layer structure, for example, including a first sub-coating layer on the surface of the current collector and a second sub-coating layer on the surface of the first sub-coating layer, the first sub-coating layer including NCM811, the second sub-coating layer including NCM 622; alternatively, the first sub-coating layer includes NCM811, and the second sub-coating layer includes NCM 523; or the first sub-coating layer comprises NCM622 and the second sub-coating layer comprises NCM 523; alternatively, the first sub-coating layer includes the NCM523, the second sub-coating layer includes the NCM111, and the like.
Of course, in other embodiments, the active material may also be other common ternary or quaternary materials, such as at least one of nickel manganese aluminum acid, nickel cobalt manganese aluminum acid, lithium cobaltate, lithium manganate, lithium iron phosphate, and lithium-rich manganese, and the gradient distribution of the mole percentage content of nickel ions, cobalt ions, manganese ions, aluminum ions, or iron ions in the active material in the coating layer may also be adjusted to improve the capacity of the pole piece and the safety and stability of the pole piece.
The sub-coating layer 21 further includes a binder and a conductive agent, wherein the mass fraction of the active material may be 88% to 97%, the mass fraction of the binder may be 1% to 6%, and the mass fraction of the conductive agent may be 1% to 6%.
In some embodiments, the binder may include at least one of polyvinylidene fluoride, polytetrafluoroethylene, and polymethacrylic polymer. Furthermore, the molecular weight of the polyvinylidene fluoride, the polytetrafluoroethylene and the polymethacrylic acid polymer is 50-800 ten thousand. The adopted binder has no bonding performance or weaker bonding capability at normal temperature, as long as the binder, the active substance and the conductive agent are not prevented from being uniformly mixed, and meanwhile, the binder needs to have better bonding performance during the rolling operation (such as hot rolling or hot pressing) of the coating layer.
In some embodiments, the conductive agent may include at least one of acetylene black, conductive graphite, graphene, carbon black, single-arm carbon tubes, multi-arm carbon tubes, carbon fibers. The material of the current collector may include at least one of aluminum, nickel, copper, carbon-coated aluminum foil, aluminum alloy, polyethylene terephthalate.
Correspondingly, the embodiment of the application also provides a preparation method of the lithium battery pole piece, which comprises the following steps:
step S1: mixing an active material, a binder and a conductive agent to form a mixed material;
step S2: coating the mixed material on a current collector to form a coating layer, wherein the molar percentage content of active metal ions in the coating layer is increased or decreased in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector;
step S3: and rolling the coating layer on the current collector to form a pole piece.
In some embodiments, the step S1 includes: mixing the active substance, the binder and the conductive agent to form at least two groups of sub-mixed materials, wherein the sub-mixed materials contain different active metal ions by mass percentage. Wherein the mass fraction of the active material is 88-97%, the mass fraction of the binder is 1-6%, and the mass fraction of the conductive agent is 1-6%.
The adhesive has no viscosity or weaker adhesive capacity when mixed at normal temperature, has better adhesive performance when being subjected to calendering operation, can ensure that active substances, the adhesive and a conductive agent can be fully mixed at normal temperature, and can show excellent adhesive performance when being subjected to calendering operation under the conditions of hot pressing or hot rollers, so that the pole piece prepared by the method has better cohesive force and adhesive force performance under the condition of high temperature. In some embodiments, the binder may include at least one of polyvinylidene fluoride, polytetrafluoroethylene, and polymethacrylic polymer.
The active material comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, and iron ions. For example, the active material may include at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, and lithium manganese rich. In some embodiments, the active material may also include some dopant metal ions such as Mg, Al, Ti, Zr, Cu, W, and the like.
The resulting sub-mixes contain different mole percent levels of active metal ions in preparation for the formation of a gradient distribution of active metal ions below. In some embodiments, different active materials may be used to form sub-mixes with the binder and conductive agent, such that each sub-mix contains a different mole percent level of active metal ions. For example, the types of the binder and the conductive agent are determined such that when the active material includes NMC811, a first sub-mix is formed, when the active material includes NMC523, a second sub-mix is formed, and when the active material includes NMC111, a third sub-mix is formed, the molar percentage contents of the active metal ions contained in the first sub-mix, the second sub-mix, and the third sub-mix being significantly different.
In some embodiments, the active material, binder, and conductive agent may be uniformly mixed by high pressure air flow shearing, mechanical shearing, milling, and the like. According to the embodiment of the application, dry materials are mixed, an organic solvent is not required to be added, and the conditions that the fluidity of the solvent is poor and the active substances are not uniformly dispersed due to the fact that the conductive agent absorbs the solvent are avoided; the problem that in the prior art, the solvent is easy to form an adhesive layer with the adhesive to prevent the contact between the active material particles and the conductive agent particles, so that the conductivity of the electrode plate is poor is solved; meanwhile, the problem that the performance of the battery cell is reduced due to the side reaction of residual solvent in the pole piece and electrolyte is avoided.
Proceeding to step S2, including: and coating each sub-mixture on the current collector to form at least two sub-coating layers, wherein the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in active substances contained in the sub-coating layers is.
In some embodiments, the active material of the sub-coating layer may include lithium nickel cobalt manganese oxide, and the closer to the current collector, the higher the mole percentage content of nickel ions in the lithium nickel cobalt manganese oxide contained in the sub-coating layer, the lower the mole percentage content of cobalt ions and manganese ions. The mass percentage content of the nickel ions near the current collector is higher, so that the pole piece has higher capacity; the farther away from the current collector, the mole percentage content of nickel ions is reduced, while the mole percentage content of cobalt ions and manganese ions is increased, so that the safety and the stability of the pole piece are improved.
After the coating is completed, a calendering operation is performed. In one embodiment, the calendering can be concentrated after all the sub-mixes have been coated. In another embodiment, after each sub-coating layer is formed, the formed sub-coating layer may be rolled on the current collector, and the coating-rolling operation may be cycled until all sub-mixes form a sub-coating layer and are rolled onto the current collector. Compared with a centralized rolling mode, the method adopts a circulating coating-rolling mode, so that the contact among the active substance, the binder and the conductive agent is tighter, and the prepared pole piece has high density, good conductivity and high capacity. In some embodiments, the calendering operation can be performed by hot rolling or hot pressing, among others.
The embodiment of the application adopts the dry process to prepare the lithium battery pole piece, and compared with the wet process, the steps of dissolving the organic solvent and drying the organic solvent are not needed, namely, the drying equipment and the solvent recovery equipment are saved in the production process, and the prepared pole piece has good toughness, the carbon powder is not easy to fall off, and the cycle life is long. Because the pole piece is prepared at high temperature in the embodiment of the application, the pole piece has better cohesive force and adhesive force performance under the high-temperature condition.
The dry process is adopted to spray the mixed material of ternary materials (NMC or NCA) containing active metal ions (such as nickel ions, cobalt ions, manganese ions or aluminum ions) with different mole percentage contents on a current collector in sequence, and then the mixed material is calendered to form a pole piece with concentration gradient, so that the problem that the gradient distribution of active substances cannot be realized in the current industry can be effectively solved.
The following description will specifically discuss a positive electrode sheet having a concentration gradient prepared by a cyclic coating-rolling method.
Example 1
Mixing NCM811, polyvinylidene fluoride and carbon black to form a mixed material 1; mixing NMC523, polyvinylidene fluoride and carbon black to form a mixed material 2; NCM111, polyvinylidene fluoride and carbon black were mixed to form blend 3. In each mixed material, the mass fraction of the active material is 90%, the mass fraction of the polyvinylidene fluoride is 6% and the mass fraction of the carbon black is 4%.
As shown in fig. 2, the mixed materials 1, 2 and 3 are respectively put into the mixing chamber 1, the mixing chamber 2 and the mixing chamber 3, and different substances in the mixed materials are uniformly mixed under the action of the shearing force generated by the high-speed operation of the blade stirrer and the airflow shearing force generated by high-pressure nitrogen.
And then feeding the mixed material 1 into a spraying system with 16KV, wherein the pressure of a carrier gas inlet is 1.2bar, and the linear distance between a nozzle and a current collector is 3.5 cm. By utilizing the principle of a high-voltage electrostatic electric field, a stronger electrostatic field is formed between the spray gun and the active substance, when the mixed powder is conveyed to the spray gun from the mixing chamber through the powder conveying pipe by the carrier gas, dense charges are generated around the mixed powder, and the powder is uniformly adsorbed on the aluminum foil (a current collector is grounded) under the action of the electrostatic field.
With reference to fig. 1 and 2, the current collector with the mixture 1 passes through an upper hot roller press and a lower hot roller press, so that the mixture is melted (or plasticized) and rolled into a uniform, continuous and flat first sub-coating layer 21;
then, according to the same coating method as the mixed material 1, the mixed material 2 is uniformly sprayed on the first sub-coating layer 21, and then is melted (or plasticized) and rolled into a uniform, continuous and flat second sub-coating layer 22 through an upper hot rolling press and a lower hot rolling press;
and continuously spraying the mixed material 3 on the second sub-coating layer 22 uniformly according to the same coating method as the mixed material 1, and then performing melting (or plasticizing) and calendering on the mixed material by an upper hot roller press and a lower hot roller press to form a uniform, continuous and flat third sub-coating layer 23.
Example 2
Mixing NCM811, polyvinylidene fluoride and carbon black to form a mixed material 1; NMC622, polyvinylidene fluoride and carbon black were mixed to form blend 2. In each mixed material, the mass fraction of the active material is 90%, the mass fraction of the polyvinylidene fluoride is 6% and the mass fraction of the carbon black is 4%.
The mixes 1 and 2 were then coated and calendered onto a current collector, in a similar process to example 1. The finally obtained pole piece comprises two sub-coating layers, wherein an active substance in a first sub-coating layer on the surface of the current collector is NCM811, and an active substance in a second sub-coating layer on the surface of the first sub-coating layer is NMC 622.
Example 3
Mixing NCM811, polyvinylidene fluoride and carbon black to form a mixed material 1; NMC523, polyvinylidene fluoride and carbon black were mixed to form blend 2. In each mixed material, the mass fraction of the active material is 90%, the mass fraction of the polyvinylidene fluoride is 6% and the mass fraction of the carbon black is 4%.
The mixes 1 and 2 were then coated and calendered onto a current collector, in a similar process to example 1. The finally obtained pole piece comprises two sub-coating layers, wherein an active substance in a first sub-coating layer positioned on the surface of the current collector is NCM811, and an active substance in a second sub-coating layer positioned on the surface of the first sub-coating layer is NMC 523.
Comparative example 1
NCM811, PVDF and carbon black are prepared into slurry according to the proportion of example 1 by a traditional wet process, and then rolled to prepare the pole piece.
Comparative example 2
NCM622, PVDF and carbon black are prepared into slurry according to the proportion of example 1 by a traditional wet process, and then the slurry is rolled to prepare the pole piece.
Comparative example 3
Preparing slurry by using NCM523, PVDF and carbon black according to the proportion of example 1 through a traditional wet process, and then rolling to prepare the pole piece.
The pole pieces prepared in the examples 1 to 3 and the comparative examples 1 to 3 were subjected to slitting and die cutting to obtain positive pole pieces, graphite as negative pole pieces and a negative pole piece containing 1L iPF6(1M) EC/EMC/DMC system as electrolyte, and is filledPreparing a soft package battery, and testing the capacity retention rate (voltage range is 2.8-4.3) of the soft package battery after the soft package battery is cycled for 2000 times at room temperature at 0.33 ℃. The test results are shown in table 1.
Table 1 gram capacity of active material and battery capacity retention rate test results
As can be seen from table 1, the active material gram capacities of examples 1 to 3 of the present application are higher than those of the comparative examples as a whole in terms of capacity, and although the active material gram capacity of comparative example 1 is the highest, the capacity retention rate is much lower than that of the examples of the present application, and the performance of the electrode sheet prepared in the examples of the present application is better than that of the comparative examples in terms of both capacity and cycle stability. Therefore, by designing the molar percentage content of the active metal ions contained in the coating layer to be in a distribution mode of increasing or decreasing in a gradient manner from the surface of the current collector to a direction far away from the surface of the current collector, the prepared pole piece can have higher gram capacity, and the prepared lithium battery has excellent stability.
The technical scheme of the application can be applied to a negative plate prepared by taking an alloy material as an active substance, and the gram capacity of the plate and the stability of a battery are improved by controlling the mole percentage content of active metal ions in the coating layer to be increased or decreased in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector.
In view of the above, it will be apparent to those skilled in the art upon reading the present application that the foregoing application content may be presented by way of example only, and may not be limiting. Those skilled in the art will appreciate that the present application is intended to cover various reasonable variations, adaptations, and modifications of the embodiments described herein, although not explicitly described herein. Such alterations, modifications, and variations are intended to be within the spirit and scope of the exemplary embodiments of this application.
It is to be understood that the term "and/or" as used herein in this embodiment includes any and all combinations of one or more of the associated listed items. It will be understood that when an element is referred to as being "connected" or "coupled" to another element, it can be directly connected or coupled to the other element or intervening elements may also be present.
Similarly, it will be understood that when an element such as a layer, region or substrate is referred to as being "on" another element, it can be directly on the other element or intervening elements may also be present. In contrast, the term "directly" means that there are no intervening elements. It will be further understood that the terms "comprises," "comprising," "includes" or "including," when used in this specification, specify the presence of stated features, integers, steps, operations, elements, and/or components, but do not preclude the presence or addition of one or more other features, integers, steps, operations, elements, components, and/or groups thereof.
It will be further understood that, although the terms first, second, third, etc. may be used herein to describe various elements, these elements should not be limited by these terms. These terms are only used to distinguish one element from another. Thus, a first element in some embodiments may be termed a second element in other embodiments without departing from the teachings of the present application. The same reference numerals or the same reference characters denote the same elements throughout the specification.
Further, the present specification describes example embodiments with reference to idealized example cross-sectional and/or plan and/or perspective views. Accordingly, variations from the shapes of the illustrations as a result, for example, of manufacturing techniques and/or tolerances, are to be expected. Thus, example embodiments should not be construed as limited to the shapes of regions illustrated herein but are to include deviations in shapes that result, for example, from manufacturing. For example, an etched region shown as a rectangle will typically have rounded or curved features. Thus, the regions illustrated in the figures are schematic in nature and their shapes are not intended to illustrate the actual shape of a region of a device and are not intended to limit the scope of exemplary embodiments.
Claims (17)
1. The lithium battery pole piece is characterized by comprising a current collector and a coating layer positioned on the surface of the current collector, wherein the coating layer comprises active metal ions, and the mole percentage content of the active metal ions is increased or decreased in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector.
2. The lithium battery pole piece according to claim 1, wherein the coating layer comprises at least two sub-coating layers, the sub-coating layers comprise active materials, and the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in the active materials contained in the sub-coating layers is.
3. The lithium battery pole piece of claim 2, wherein the active material comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, magnesium ions, titanium ions, tungsten ions, iron ions, and copper ions.
4. The lithium battery pole piece of claim 3, wherein the active material comprises at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, and lithium rich manganese.
5. The lithium battery pole piece of claim 4, wherein the active material comprises nickel cobalt lithium manganate, and the closer to the current collector, the more molar percentage content of nickel ions in the nickel cobalt lithium manganate the sub-coating layer contains, the less molar percentage content of cobalt ions and manganese ions.
6. The lithium battery pole piece of claim 2, wherein the sub-coating layer further comprises a binder and a conductive agent, wherein the mass fraction of the active material is 88-97%, the mass fraction of the binder is 1-6%, and the mass fraction of the conductive agent is 1-6%.
7. The lithium battery pole piece of claim 6, wherein the binder comprises at least one of polyvinylidene fluoride, polytetrafluoroethylene, and polymethacrylic polymer.
8. The lithium battery pole piece of claim 6, wherein the conductive agent comprises at least one of acetylene black, conductive graphite, graphene, carbon black, single-arm carbon tubes, multi-arm carbon tubes and carbon fibers, and the material of the current collector comprises at least one of aluminum, nickel, copper, carbon-coated aluminum foil, aluminum alloy and polyethylene terephthalate.
9. A preparation method of a lithium battery pole piece is characterized by comprising the following steps:
mixing an active material, a binder and a conductive agent to form a mixed material;
coating the mixed material on a current collector to form a coating layer, wherein the molar percentage content of active metal ions in the coating layer is increased or decreased in a gradient manner from the surface of the current collector to the direction far away from the surface of the current collector;
and rolling the coating layer on the current collector to form a pole piece.
10. The method of claim 9, wherein the active material, the binder, and the conductive agent are mixed to form at least two sub-mixes, and each sub-mix contains different mole percent amounts of active metal ions.
11. The method for preparing the lithium battery pole piece according to claim 10, wherein the step of coating the mixture on a current collector to form a coating layer comprises the following steps: and coating each sub-mixture on the current collector to form at least two sub-coating layers, wherein the closer to the current collector, the larger or smaller the molar percentage content of active metal ions in active substances contained in the sub-coating layers is.
12. The method of manufacturing a lithium battery electrode sheet according to claim 11, wherein after each sub-coating layer is formed, the formed sub-coating layer is rolled on the current collector.
13. The method for preparing a lithium battery pole piece according to claim 11 or 12, wherein the active material comprises at least one of the following active metal ions: nickel ions, cobalt ions, manganese ions, aluminum ions, magnesium ions, titanium ions, tungsten ions, iron ions, and copper ions.
14. The method of claim 13, wherein the active material comprises at least one of lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminate, lithium nickel manganese aluminate, lithium nickel cobalt manganese aluminate, lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, and lithium rich manganese.
15. The method of claim 14, wherein the active material comprises nickel cobalt lithium manganate, and the closer to the current collector, the greater the mole percentage content of nickel ions in the nickel cobalt lithium manganate contained in the sub-coating layer, the smaller the mole percentage content of cobalt ions and manganese ions.
16. The method for preparing the lithium battery pole piece as claimed in claim 9, wherein the mass fraction of the active material is 88-97%, the mass fraction of the binder is 1-6%, and the mass fraction of the conductive agent is 1-6%.
17. The method for manufacturing a lithium battery pole piece according to claim 9, wherein the binder comprises at least one of polyvinylidene fluoride, polytetrafluoroethylene and polymethacrylic acid polymer.
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Application publication date: 20200731 |