CN109830645A - Battery anode slice and its manufacturing method and lithium battery and its manufacturing method - Google Patents
Battery anode slice and its manufacturing method and lithium battery and its manufacturing method Download PDFInfo
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Abstract
The invention discloses battery anode slice and its manufacturing method and lithium battery and its manufacturing methods, wherein, battery anode slice include cathode metal substrate and coated on cathode metal substrate outside positive coating, positive coating includes the component of following parts by weight: the positive active material of 96%-98%；The positive conductive agent A of 0.5%-0.8%；The positive conductive agent B of 0.1%-0.4%；The positive electrode binder of 1.3%-1.8%；Positive active material is by LiNixCoyAl1‑x‑ yO2、LiNi0.5Co0.2Mn0.3O2And LiNi0.6Co0.2Mn0.2O2It is mixed to form.In the present invention, three kinds of active materials have complementary advantages, and can obtain more balanced chemical property, so that the capacity retention ratio after 0.5C charge/discharge 200 weeks circulations of the lithium battery made of the battery anode slice is greater than 90%, cost performance is high, can satisfy the demand in market.
Description
Technical Field
The invention relates to the field of lithium batteries, in particular to a battery positive plate and a manufacturing method thereof, and a lithium battery and a manufacturing method thereof.
Background
With the continuous development of the lithium battery industry, 18650 lithium batteries (the diameter of the battery is 18mm, the height of the battery is 65mm) become the preferred model in the field of battery packaging due to the standardized size and flexible grouping mode. However, in the prior art, due to the technical limit of lithium battery raw materials, the capacity retention rate of the prior 18650 type lithium battery after charge and discharge cycles is low, and the requirement of the market on the battery capacity is difficult to meet.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention discloses a battery positive plate which is used for solving the problems that the existing lithium battery is low in capacity retention rate after cyclic charge and discharge and is difficult to meet the market requirement.
In order to achieve the purpose, the invention adopts the technical scheme that:
the battery positive plate comprises a positive metal substrate, a positive lug in conductive connection with the positive metal substrate and a positive coating coated outside the positive metal substrate, wherein the positive coating comprises the following components in parts by weight:
the positive active material comprises a positive active material D, a positive active material E and a positive electrodeActive material F is formed by mixing, and the positive active material D is LiNixCoyAl1-x-yO2Wherein x is more than or equal to 0.7 and less than or equal to 0.9, y is more than or equal to 0.1 and less than or equal to 0.3, and the positive active material E is LiNi0.5Co0.2Mn0.3O2The positive active material F is LiNi0.6Co0.2Mn0.2O2。
Preferably, the weight parts of the positive electrode active material D, the positive electrode active material E and the positive electrode active material F in the positive electrode active substance are (3-5): (1-3): (3-5).
Preferably, the positive coating comprises the following components in parts by weight: 97.5% of positive electrode active substance, 0.7% of positive electrode conductive agent A, 0.3% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 2: 4; or,
the anode coating comprises the following components in parts by weight: 97.3% of positive electrode active substance, 0.6% of positive electrode conductive agent A, 0.4% of positive electrode conductive agent B and 1.7% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 1: 5; or,
the anode coating comprises the following components in parts by weight: 97.8% of positive electrode active substance, 0.5% of positive electrode conductive agent A, 0.2% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 5: 1: 4.
preferably, the median particle diameter of the positive electrode active material D is 10-12 μm, the median particle diameter of the positive electrode active material E is 9-11 μm, and the median particle diameter of the positive electrode active material F is 11-13 μm; and/or the presence of a gas in the atmosphere,
the tap density of the positive electrode active material D is 2.3-2.6g/cm3Said positive electrode being activeThe tap density of the material E is 2.4-2.6g/cm3The tap density of the positive electrode active material F is 2.3-2.5g/cm3(ii) a And/or the specific surface area of the positive electrode active material D is 2-2.5m2(ii)/g, the specific surface area of the positive electrode active material E is 0.3 to 0.5m2(ii)/g, the specific surface area of the positive electrode active material F is 0.25 to 0.4m2(ii)/g; and/or the presence of a gas in the atmosphere,
the gram capacity of the positive active material D is 175-195mAh/g, the gram capacity of the positive active material E is 150-160mAh/g, and the gram capacity of the positive active material F is 155-170 mAh/g; and/or the positive electrode conductive agent A is a carbon nanotube or a carbon fiber or a combination of the carbon nanotube and graphene; and/or the presence of a gas in the atmosphere,
the positive conductive agent B is conductive graphite or conductive carbon black; and/or the presence of a gas in the atmosphere,
the positive adhesive is polyvinylidene fluoride or polyvinyl alcohol; and/or the presence of a gas in the atmosphere,
the thickness of the positive electrode metal substrate is 12 microns +/-2 microns, and the thickness of the battery positive electrode sheet is 145 microns +/-5 microns; and/or the presence of a gas in the atmosphere,
the positive electrode metal substrate is an aluminum foil.
The second purpose of the invention is to disclose a method for manufacturing the battery positive plate, which comprises the following steps:
a step of preparing anode slurry, in which the anode active material, the anode conductive agent A, the anode conductive agent B and the anode binder are uniformly mixed with a nitrogen-methyl pyrrolidone solvent according to the weight part ratio in the anode coating to prepare the anode slurry;
coating the positive electrode slurry on the positive electrode metal substrate to obtain a positive electrode coating intermediate product;
drying and curing the anode slurry, namely placing the anode coating intermediate product in an environment of 80-120 ℃ for drying and curing so as to dry and cure the anode slurry into the anode coating and prepare an anode cured intermediate product;
a positive plate processing step, namely sequentially rolling and cutting the positive solidified intermediate product to obtain a positive plate semi-finished product;
and a positive tab welding step, namely welding a positive tab on the semi-finished product of the positive plate to obtain the battery positive plate.
Preferably, the positive electrode slurry coating step is performed by: coating the anode slurry on the top surface and the bottom surface of the anode metal substrate at intervals respectively so as to form two anode top coating layers arranged at intervals on the top surface of the anode metal substrate, forming two anode bottom coating layers arranged at intervals on the bottom surface of the anode metal substrate, wherein a gap between the two anode top coating layers and a gap between the two anode bottom coating layers are arranged in a vertically aligned manner; in the step of welding the positive lugs, the positive lugs are welded in a gap between two positive top coating layers of the semi-finished positive plate.
The third purpose of the invention is to disclose a lithium battery, which comprises a battery shell, a battery negative plate, a first diaphragm, a second diaphragm, electrolyte and the battery positive plate, the battery positive plate, the battery negative plate, the first diaphragm, the second diaphragm and the electrolyte are all arranged in the battery shell, and the battery positive plate, the battery negative plate, the first diaphragm and the second diaphragm are all immersed in the electrolyte, the battery negative plate is positioned between the battery positive plate and the battery shell, the first diaphragm is arranged between the battery positive plate and the battery negative plate, the second diaphragm is arranged between the battery shell and the battery negative plate, the battery negative plate comprises a negative metal substrate and a negative coating coated outside the negative metal substrate, and the negative coating comprises the following components in parts by weight:
the negative active material is composite graphite powder.
Preferably, the negative electrode coating comprises the following components in parts by weight: 95% of negative electrode active material, 1.5% of negative electrode conductive agent, 1.3% of suspending agent and 2.2% of negative electrode binder; or,
the negative coating comprises the following components in parts by weight: 95.2% of negative electrode active material, 1.3% of negative electrode conductive agent, 1.4% of suspending agent and 2.1% of negative electrode binder; or,
the negative coating comprises the following components in parts by weight: 95.5% of negative electrode active material, 1% of negative electrode conductive agent, 1.5% of suspending agent and 2% of negative electrode binder.
Preferably, the composite graphite powder is formed by compounding natural graphite powder and artificial stone toner; and/or the presence of a gas in the atmosphere,
the median particle diameter of the composite graphite powder A is 15-19 mu m, and the tap density of the composite graphite powder is 1-1.2g/cm3The specific surface area of the composite graphite powder is 1.2-3.0m2The gram capacity of the composite graphite powder is 340-380 mAh/g; and/or the presence of a gas in the atmosphere,
the negative conductive agent is conductive carbon black or conductive graphite or carbon nano tubes; and/or the presence of a gas in the atmosphere,
the negative electrode binder is sodium carboxymethylcellulose or styrene butadiene rubber or polyacrylic acid or sodium alginate; and/or the presence of a gas in the atmosphere,
the suspending agent is sodium carboxymethyl cellulose; and/or the presence of a gas in the atmosphere,
the thickness of the negative electrode metal substrate is 8 microns +/-2 microns, and the thickness of the battery negative electrode sheet is 160 microns +/-5 microns; and/or the presence of a gas in the atmosphere,
the negative metal substrate is a copper foil; and/or the presence of a gas in the atmosphere,
the first diaphragm and the second diaphragm are both three-layer polypropylene diaphragms manufactured by adopting a dry process; and/or the presence of a gas in the atmosphere,
the thickness of the first separator and the thickness of the second separator are both 22 μm ± 2 μm.
A fourth object of the present invention is to disclose a method for manufacturing the lithium battery, including the steps of:
assembling the battery shell, the battery positive plate, the battery negative plate, the first diaphragm and the second diaphragm, baking and injecting the electrolyte, wherein the battery positive plate is prepared by the method for manufacturing the battery positive plate;
the battery negative plate is prepared by the following steps:
a step of preparing cathode slurry, in which the cathode active material, the cathode conductive agent, the suspending agent and the cathode binder are uniformly mixed with deionized water according to the weight part ratio in the cathode coating to prepare cathode slurry;
coating the negative electrode slurry on the negative electrode metal substrate to dry and solidify the negative electrode slurry into a negative electrode coating to obtain a negative electrode coating intermediate product;
a step of drying and curing the cathode slurry, which is to place the cathode coating intermediate product in an environment of 80-120 ℃ for drying and curing to prepare a cathode curing intermediate product;
a negative plate processing step, namely sequentially rolling and cutting the negative solidified intermediate product to obtain a negative plate semi-finished product;
and a negative electrode tab welding step, wherein a negative electrode tab is welded on the semi-finished product of the negative electrode sheet to prepare the battery negative electrode sheet.
Compared with the prior art, the invention has the beneficial effects that:
according to the battery positive plate and the manufacturing method thereof, as well as the lithium battery and the manufacturing method thereof, the battery positive plate is formed by mixing the active substances including the three active materials with different performances, the advantages of the three active materials are complementary, and more balanced electrochemical performances can be obtained, so that the capacity retention rate of the lithium battery manufactured by the battery positive plate is more than 90% after the lithium battery is charged/discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
Drawings
FIG. 1 is a schematic diagram of a first view angle of a positive plate of a battery disclosed in an embodiment of the invention;
fig. 2 is a schematic diagram of a second view angle structure of a positive plate of a battery disclosed in the embodiment of the invention.
Detailed Description
The present invention will be further described with reference to the accompanying drawings and the detailed description, and it should be noted that any combination of the embodiments or technical features described below can be used to form a new embodiment without conflict.
Referring to fig. 1 and fig. 2, a battery positive plate 10 disclosed in an embodiment of the present invention includes a positive metal substrate 11, a positive tab 12 conductively connected to the positive metal substrate 11, and a positive coating 13 coated outside the positive metal substrate 11, where the positive coating 13 includes the following components in parts by weight:
the positive electrode active material is formed by mixing a positive electrode active material D, a positive electrode active material E and a positive electrode active material F, wherein the positive electrode active material D is LiNixCoyAl1-x-yO2Wherein x is more than or equal to 0.7 and less than or equal to 0.9, y is more than or equal to 0.1 and less than or equal to 0.3, and the positive active material E is LiNi0.5Co0.2Mn0.3O2The positive electrode active material F is LiNi0.6Co0.2Mn0.2O2。
According to the battery positive plate 10 disclosed by the invention, the active substance is formed by mixing three active materials with different performances, the advantages of the three active materials are complementary, and more balanced electrochemical performances can be obtained, so that the capacity retention rate of a lithium battery made of the battery positive plate is more than 90% after the lithium battery is charged/discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
Preferably, the weight parts of the positive electrode active material D, the positive electrode active material E and the positive electrode active material F in the positive electrode active substance are (3-5): (1-3): (3-5).
Preferably, the positive electrode coating comprises the following components in parts by weight: 97.5% of positive electrode active substance, 0.7% of positive electrode conductive agent A, 0.3% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 2: 4; or the positive coating comprises the following components in parts by weight: 97.3% of positive electrode active substance, 0.6% of positive electrode conductive agent A, 0.4% of positive electrode conductive agent B and 1.7% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 1: 5; or the positive coating comprises the following components in parts by weight: 97.8% of positive electrode active substance, 0.5% of positive electrode conductive agent A, 0.2% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 5: 1: 4. according to test tests, the positive coating adopts the components in parts by weight, and the effects of improving the cycle performance of the positive plate of the battery and improving the safety performance of the lithium battery are obvious.
Preferably, the median particle diameter of the positive electrode active material D is 10 to 12 μm, the median particle diameter of the positive electrode active material E is 9 to 11 μm, and the median particle diameter of the positive electrode active material F is 11 to 13 μm. Through setting three kinds of positive active material to have different particle diameters for the space between the material granule obtains abundant utilization thereby improves the compaction density of battery positive plate, thereby makes better electrochemical performance, makes the lithium cell of making by this battery positive plate charge/discharge capacity retention ratio after 200 cycles of 0.5C and is greater than 90%, and the sexual valence relative altitude can satisfy the demand in market.
Preferably, the tap density of the positive electrode active material D is 2.3 to 2.6g/cm3The tap density of the positive electrode active material E is 2.4-2.6g/cm3The tap density of the positive electrode active material F is 2.3-2.5g/cm3. Through setting three positive active materials to have different tap densities, gaps among material particles are fully utilized, so that the compaction density of the positive plate of the battery is improved, the electrochemical performance is better, the capacity retention rate of a lithium battery made of the positive plate of the battery is more than or equal to 90% after the lithium battery is charged/discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
Preferably, the specific surface area of the cathode active material D is 2 to 2.5m2(ii)/g, the specific surface area of the positive electrode active material E is 0.3 to 0.5m2(ii)/g, the specific surface area of the positive electrode active material F is 0.25 to 0.4m2(ii) in terms of/g. Through the arrangement that the three positive active materials have different specific surface areas, gaps among material particles are fully utilized, so that the compaction density of the positive plate of the battery is improved, the electrochemical performance is better, the capacity retention rate of a lithium battery made of the positive plate of the battery is more than 90% after the lithium battery is charged/discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
Preferably, the gram capacity of the positive electrode active material D is 175-195mAh/g, the gram capacity of the positive electrode active material E is 150-160mAh/g, and the gram capacity of the positive electrode active material F is 155-170 mAh/g. By arranging the three positive active materials to have different gram capacities, compared with the single positive active material, the electrochemical performance is better balanced, so that the capacity retention rate of the lithium battery made of the battery positive plate is more than 90 percent after the lithium battery is charged/discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
Preferably, the positive electrode conductive agent a is a Carbon Nanotube (CNT) or a carbon fiber (VGCF) or a combination of a carbon nanotube and graphene. The material of the fibrous positive electrode conductive agent is optimally designed, so that the fibrous positive electrode conductive agent is favorably matched with the granular positive electrode conductive agent, and the internal resistance of the battery is effectively reduced.
Preferably, the positive electrode conductive agent B is conductive graphite or conductive carbon black. The material of the granular positive electrode conductive agent is optimally designed, so that the granular positive electrode conductive agent is favorably matched with the fibrous positive electrode conductive agent, the internal resistance of the battery is effectively reduced, and the flexibility of the pole piece is improved.
More preferably, the granular positive electrode conductive agent is any one of conductive carbon black 350G, SP-Li, acetylene black, Ketjen black, conductive graphite KS-6, conductive graphite KS-15, conductive graphite SFG-6 and conductive graphite SFG-15. .
Preferably, the positive binder is polyvinylidene fluoride (PVDF) or polyvinyl alcohol (PVA), and the positive binder adopts any one of the two binders, so that the positive coating and the positive metal substrate can have good adhesive property.
Preferably, the thickness t of the positive electrode metal substrate 11112 μm + -2 μm, the thickness t of the positive electrode sheet 10 of the battery2The thickness was 145 μm. + -. 5 μm. Thus, the battery positive electrode sheet 10 is advantageous for exhibiting the best performance of the positive electrode active material while ensuring a small size.
Preferably, the positive electrode metal substrate 11 is an aluminum foil. The conductive sheet can meet the conductive performance requirement of the battery positive plate 10, and has light weight and low cost.
The embodiment of the invention discloses a manufacturing method of the battery positive plate 10, which comprises the following steps:
a step of preparing anode slurry, which is to uniformly mix an anode active substance, an anode conductive agent A, an anode conductive agent B and an anode binder with a nitrogen-methyl pyrrolidone solvent according to the weight part ratio in the anode coating to prepare the anode slurry;
coating the positive electrode slurry on a positive electrode metal substrate to obtain a positive electrode coating intermediate product;
drying and curing the anode slurry, namely placing the anode coating intermediate product in an environment of 80-120 ℃ for drying and curing so as to dry and cure the anode slurry into an anode coating and prepare an anode cured intermediate product;
a positive plate processing step, namely sequentially rolling and cutting the positive solidified intermediate product to obtain a positive plate semi-finished product;
and a positive tab welding step, namely welding a positive tab on the semi-finished product of the positive tab to obtain the battery positive tab.
In the manufacturing method of the battery positive plate disclosed by the embodiment of the invention, the solvent is a nitrogen-methyl pyrrolidone solvent, the solid content of the positive slurry is 40-75%, and the positive slurry is dried and cured into the positive coating 13 in an environment of 80-120 ℃, so that the coating operation of the positive slurry on the positive metal substrate 11 is facilitated, and the drying and curing efficiency of the positive slurry is ensured to be higher. The manufacturing method of the battery positive plate 10 disclosed by the embodiment of the invention has the advantages that the manufacturing process is simple, the production efficiency is high, the capacity of the battery positive plate 10 is high in the manufactured battery positive plate 10, the adhesive force of the positive coating 13 on the positive metal substrate 11 is strong, the resistance of the battery positive plate 10 is low, and the capacity, the cycle performance and the safety performance of a lithium battery are favorably improved.
Preferably, the positive electrode slurry coating step is performed by: coating positive electrode slurry on the top surface and the bottom surface of the positive electrode metal substrate 11 at intervals respectively so as to form two positive electrode top coating layers 131 arranged at intervals on the top surface of the positive electrode metal substrate 11, form two positive electrode bottom coating layers 132 arranged at intervals on the bottom surface of the positive electrode metal substrate 11, and form a gap between the two positive electrode top coating layers 131 and a gap between the two positive electrode bottom coating layers 132 in a vertically and positively aligned manner; in the positive tab welding step, the positive tab 12 is welded in the gap between the two positive top coating layers 131 of the positive plate semi-finished product.
The embodiment of the invention discloses a lithium battery, which comprises a battery shell, a battery negative plate, a first diaphragm, a second diaphragm, electrolyte and the battery positive plate, wherein the battery positive plate, the battery negative plate, the first diaphragm, the second diaphragm and the electrolyte are all arranged in the battery shell, the battery positive plate, the battery negative plate, the first diaphragm and the second diaphragm are all immersed in the electrolyte, the battery negative plate is positioned between the battery positive plate and the battery shell, the first diaphragm is arranged between the battery positive plate and the battery negative plate, the second diaphragm is arranged between the battery shell and the battery negative plate, the battery negative plate comprises a negative metal substrate and a negative coating coated outside the negative metal substrate, and the negative coating comprises the following components in parts by weight:
the negative active material is composite graphite powder.
The components of the negative electrode coating are optimally designed, so that the capacity of the battery negative electrode piece and the adhesive force of the negative electrode coating on the negative electrode metal substrate are improved, the resistance of the battery negative electrode piece is reduced, and the capacity, the cycle performance and the safety performance of the lithium battery are further improved. In addition, the setting of the suspending agent can ensure that the cathode conductive agent and the cathode active substance are well dispersed and in a suspended state in the prepared cathode slurry, ensure the stability of the subsequent processing process (coating process) of the cathode slurry, avoid the agglomeration of the cathode conductive agent and avoid the sedimentation of the cathode active substance.
Preferably, the negative electrode coating comprises the following components in parts by weight: 95% of negative electrode active material, 1.5% of negative electrode conductive agent, 1.3% of suspending agent and 2.2% of negative electrode binder; or the negative coating comprises the following components in parts by weight: 95.2% of negative electrode active material, 1.3% of negative electrode conductive agent, 1.4% of suspending agent and 2.1% of negative electrode binder; or the negative coating comprises the following components in parts by weight: 95.5% of negative electrode active material, 1% of negative electrode conductive agent, 1.5% of suspending agent and 2% of negative electrode binder. According to test tests, the negative electrode coating adopts the components in parts by weight, and the effects of improving the capacity of the battery negative electrode sheet, improving the adhesive force of the negative electrode coating on the negative electrode metal substrate and reducing the resistance of the battery negative electrode sheet are obvious.
Preferably, the composite graphite powder is formed by compounding natural graphite powder and artificial stone toner. The composite graphite powder formed by compounding the natural graphite powder and the artificial graphite powder can overcome the defects of pure natural graphite powder or pure artificial graphite powder and obtain more balanced electrochemical performance.
The median particle diameter of the composite graphite powder A is 15-19 mu m, and the tap density of the composite graphite powder is 1-1.2g/cm3The specific surface area of the composite graphite powder is 1.2-3.0m2And the gram capacity of the composite graphite powder is 340-380 mAh/g.
Preferably, the negative electrode conductive agent is any one of conductive carbon black, conductive graphite or carbon nanotubes. Here, the material of the negative electrode conductive agent is optimally designed, which is beneficial to reducing the internal resistance of the battery.
More preferably, the negative electrode conductive agent is any one of conductive carbon black 350G, SP-Li, conductive graphite KS-6, conductive graphite SFG-6, Ketjen black ECP-600JD and carbon nanotube CNT.
Preferably, the negative electrode binder is any one of sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR), polyacrylic acid (PAA) and sodium alginate. The material of the cathode binder is optimally designed, so that the cathode coating and the cathode metal substrate are favorably ensured to have good bonding performance.
Preferably, the suspending agent is sodium carboxymethylcellulose (CMC). The suspending agent is sodium carboxymethyl cellulose, so that the cathode conductive agent and the cathode active substance can be suspended in the prepared cathode slurry, and the adhesive force between components of the cathode coating and between the cathode coating and the cathode metal substrate after the battery cathode sheet is dried can be improved by utilizing the adhesive capacity of the sodium carboxymethyl cellulose and the synergistic effect of the cathode adhesive.
Preferably, the thickness of the negative electrode metal substrate is 8 μm + -2 μm, and the thickness of the battery negative electrode sheet is 160 μm + -5 μm. Therefore, the best performance of the negative active material is favorably exerted on the premise of ensuring that the size of the battery negative plate is smaller.
Preferably, the negative electrode metal substrate is a copper foil. The conductive performance is good, and the conductive performance requirement of the battery negative plate can be met.
Preferably, the first membrane and the second membrane are both three-layer polypropylene material membranes manufactured by a dry process.
Preferably, the thickness of the first separator and the thickness of the second separator are both 22 μm ± 2 μm.
The embodiment of the invention discloses a manufacturing method of the lithium battery, which comprises the following steps:
assembling a battery shell, a battery positive plate, a battery negative plate, a first diaphragm and a second diaphragm, baking and injecting electrolyte, wherein the battery positive plate is prepared by the above manufacturing method of the battery positive plate;
the battery negative plate is prepared by the following steps:
a step of preparing cathode slurry, which is to uniformly mix a cathode active substance, a cathode conductive agent, a suspending agent and a cathode binder with deionized water according to the weight part ratio in the cathode coating to prepare cathode slurry;
coating the negative electrode slurry on a negative electrode metal substrate to dry and solidify the negative electrode slurry into a negative electrode coating to obtain a negative electrode coating intermediate product;
a step of drying and curing the cathode slurry, which is to place the cathode coating intermediate product in an environment of 80-120 ℃ for drying and curing to prepare a cathode curing intermediate product;
a negative plate processing step, namely sequentially rolling and cutting the negative solidified intermediate product to obtain a negative plate semi-finished product;
and a negative electrode tab welding step, namely welding a negative electrode tab on the semi-finished product of the negative electrode sheet to prepare the battery negative electrode sheet.
In the method for manufacturing the battery negative plate, the solvent adopts deionized water, the solid content of the negative slurry is set to be 45-55%, and the negative slurry is dried and cured into the negative coating in the environment of 80-120 ℃, so that the coating operation of the negative slurry on the negative metal substrate is facilitated, and the drying and curing efficiency of the negative slurry is ensured to be higher. The manufacturing method of the battery negative plate disclosed by the embodiment of the invention has the advantages that the manufacturing process is simple, the production efficiency is high, the capacity of the battery negative plate is high, the adhesive force of the negative coating on the negative metal substrate is strong, the resistance of the battery negative plate is low, and the capacity, the cycle performance and the safety performance of a lithium battery can be favorably improved.
Preferably, the battery case, the battery positive plate, the battery negative plate, the first diaphragm, the second diaphragm and the electrolyte are assembled in the following manner: stacking a battery positive plate, a battery negative plate, a first diaphragm and a second diaphragm in the order of a second diaphragm, a battery negative plate, a first diaphragm and a battery positive plate, then winding the stacked plates into a cylindrical winding core, assembling the winding core in a battery shell to prepare a semi-finished product battery cell, and baking the semi-finished product battery cell for 16-22 hours; injecting electrolyte into the semi-finished product battery cell, and then sealing the semi-finished product battery cell to obtain a semi-finished product battery; and (3) infiltrating and activating the semi-finished product battery for 33-40 hours in a manner of first inversely infiltrating and then positively infiltrating at the constant temperature of 30-45 ℃, and then charging the semi-finished product battery to form the lithium battery.
The following describes the manufacturing method and testing process of lithium batteries by three preferred embodiments:
example 1:
preparing a battery positive plate: 97.5 percent of positive active material (LiNi in the positive active material) by weight partxCoyAl1-x- yO2、LiNi0.5Co0.2Mn0.3O2And LiNi0.6Co0.2Mn0.2O2The weight part ratio of the positive active material is 4: 2: 4) 0.7 percent of carbon nano tube conductive agent, 0.3 percent of conductive graphite and 1.5 percent of polyvinylidene fluoride, nitrogen-methyl pyrrolidone solvent accounting for about 70 percent of solid is added and uniformly mixed to prepare anode slurry, the anode slurry is coated on a metal aluminum foil with the thickness of 12 mu m, and after the anode slurry is dried at the temperature of 80-120 ℃, the anode slurry is rolled into a battery anode sheet with the thickness of about 145 mu m.
Preparing a battery negative plate: adding deionized water accounting for 50% of solid into 95% of natural/artificial composite graphite powder, 1.5% of SuperP, 2.2% of SBR and 1.3% of CMC in parts by weight, uniformly mixing to prepare negative electrode slurry, coating the negative electrode slurry on a metal copper foil with the thickness of 8 microns, drying at the temperature of 80-120 ℃, and rolling to form a battery negative electrode sheet with the thickness of about 160 microns.
Assembling the lithium battery: cutting a battery positive plate and a battery negative plate into long strips, reserving a metal aluminum foil at the battery positive plate for welding a positive tab, reserving a metal copper foil piece at one end of the battery negative plate for welding a negative tab, winding the battery positive plate/polypropylene film diaphragm/battery negative plate/polypropylene film diaphragm into a cylindrical winding core, welding the positive tab led out from the battery positive plate at a cap aluminum sheet connecting piece by laser welding, spot-welding the negative tab led out from the battery negative plate at the bottom of a steel shell, fully baking the battery core, injecting electrolyte, and sealing to assemble the 18650-plus 2500mAh lithium battery.
Testing of the lithium battery: the limit voltage of the lithium battery is 2.75V-4.2V, the lithium battery is subjected to charge-discharge cycle test in a 0.5C constant-current constant-voltage charge and 0.5C constant-current discharge mode, and the capacity retention ratio of the battery in the 200 th week is 90.8%.
Example 2:
preparing a battery positive plate: 97.3 percent of positive active material (LiNi, whereinxCoyAl1-x-yO2、LiNi0.5Co0.2Mn0.3O2And LiNi0.6Co0.2Mn0.2O2The weight part ratio of the positive active material is 4: 1: 5) 0.6 percent of carbon nano tube conductive agent A, 0.4 percent of conductive graphite B and 1.7 percent of polyvinylidene fluoride, nitrogen-methyl pyrrolidone solvent accounting for about 70 percent of solid is added and uniformly mixed to prepare anode slurry, the anode slurry is coated on a metal aluminum foil with the thickness of 12 mu m, and after drying at the temperature of 80-120 ℃, the anode slurry is rolled into a battery anode sheet with the thickness of about 145 mu m.
Preparing a battery negative plate: adding deionized water accounting for 50% of solid into 95.2% of natural/artificial composite graphite powder, 1.3% of Super P, 2.1% of SBR and 1.4% of CMC in percentage by weight, uniformly mixing to prepare negative electrode slurry, coating the negative electrode slurry on a metal copper foil with the thickness of 8 microns, drying at the temperature of 80-120 ℃, and rolling to form a battery negative electrode sheet with the thickness of about 160 microns.
Assembling the lithium battery: cutting a battery positive plate and a battery negative plate into long strips, reserving a metal aluminum foil at the battery positive plate for welding a positive tab, reserving a metal copper foil piece at one end of the battery negative plate for welding a negative tab, winding the battery positive plate/polypropylene film diaphragm/battery negative plate/polypropylene film diaphragm into a cylindrical winding core, welding the positive tab led out from the battery positive plate at a cap aluminum sheet connecting piece by laser welding, spot-welding the negative tab led out from the battery negative plate at the bottom of a steel shell, fully baking the battery core, injecting electrolyte, and sealing to assemble the 18650-plus 2500mAh lithium battery.
Testing of the lithium battery: the charge-discharge limiting voltage of the lithium battery is 2.75V-4.2V, the charge-discharge cycle test of the lithium battery is carried out in a 0.5C constant-current constant-voltage charge and 0.5C constant-current discharge mode, and the capacity retention ratio of the battery in the 200 th week is 91.3%.
Experimental example 3:
preparing a battery positive plate: 97.8 percent of positive active material (LiNi, whereinxCoyAl1-x-yO2、LiNi0.5Co0.2Mn0.3O2And LiNi0.6Co0.2Mn0.2O2The weight part ratio of the positive active material is 5: 1: 4) 0.5 percent of carbon nano tube conductive agent A, 0.2 percent of conductive graphite B and 1.5 percent of polyvinylidene fluoride, N-methyl pyrrolidone solvent accounting for about 70 percent of solid is added and uniformly mixed to prepare anode slurry, the anode slurry is coated on a metal aluminum foil with the thickness of 12 mu m, and after drying at the temperature of 80-120 ℃, the anode slurry is rolled into a battery anode sheet with the thickness of about 145 mu m.
Preparing a battery negative plate: adding deionized water accounting for 50% of solid in percentage by weight into 95.5% of natural/artificial composite graphite powder, 1% of SuperP, 2% of SBR and 1.5% of CMC in percentage by weight, uniformly mixing to prepare negative electrode slurry, coating the negative electrode slurry on a metal copper foil with the thickness of 8 microns, drying at the temperature of 80-120 ℃, and rolling to form a battery negative electrode sheet with the thickness of about 160 microns.
Assembling the lithium battery: cutting a battery positive plate and a battery negative plate into long strips, reserving a metal aluminum foil at the battery positive plate for welding a positive tab, reserving a metal copper foil piece at one end of the battery negative plate for welding a negative tab, winding the battery positive plate/polypropylene film diaphragm/battery negative plate/polypropylene film diaphragm into a cylindrical winding core, welding the positive tab led out from the battery positive plate at a cap aluminum sheet connecting piece by laser welding, spot-welding the negative tab led out from the battery negative plate at the bottom of a steel shell, fully baking the battery core, injecting electrolyte, and sealing to assemble the 18650-plus 2500mAh lithium battery.
Testing of the lithium battery: the limit voltage of the lithium battery is 2.75V-4.2V, the lithium battery is subjected to charge-discharge cycle test in a 0.5C constant-current constant-voltage charge and 0.5C constant-current discharge mode, and the capacity retention ratio of the battery in the 200 th week is 92.8%.
Comparative example:
preparing a battery negative plate: mixing 2 wt% of suspending agent CMC dry powder with deionized water to prepare suspending agent glue solution with solid content of 1.8%, adding 94.5 wt% of graphite powder, 1.5 wt% of conductive graphite and 2 wt% of SBR, mixing, adding deionized water, and uniformly mixing to prepare negative electrode slurry with solid content of 46%. Coating the negative electrode slurry on a metal copper foil with the thickness of 8 mu m in a clearance manner, drying at the temperature of 100-130 ℃, rolling into a sheet body with the thickness of about 154 mu m, designing the compaction density of the sheet body to be not higher than 1.65g/cm3, cutting the sheet body into a strip shape, welding a negative electrode lug at the position of the clearance foil to prepare the battery negative electrode sheet, wherein the width of the cut sheet body is 58.5 mm.
Preparing a battery positive plate: firstly, 2 wt% of binder PVDF dry powder, 0.7 wt% of conductive agent Ks-6 and 0.5 wt% of carbon nano tube oily slurry are mixed, a proper amount of solvent nitrogen-methyl pyrrolidone (NMP) is added for mixing to prepare conductive agent glue solution, 96.8 wt% of active material nickel cobalt lithium manganate ternary material and a proper amount of NMP are added for mixing to prepare positive electrode slurry with solid content of 72%. Coating the positive slurry on a metal aluminum foil with the thickness of 14 mu m in a clearance way, drying at the temperature of 120-150 ℃, rolling into a sheet body with the thickness of about 158 mu m in a rolling way, cutting the sheet body into a strip shape, wherein the compaction density of the sheet body is not higher than 3.56g/cm3, the width of the cut sheet body is 56.5mm, and welding a positive lug at the position of the clearance foil to prepare the battery positive plate.
Assembling the lithium battery: the positive plate, the negative plate and the diaphragm of the battery are overlapped according to the sequence of 'diaphragm/negative plate/diaphragm/positive plate' and then wound into a cylindrical pole group, and the diaphragm is a polypropylene film with the width of 60.5mm and the thickness of 19 mu m. Sleeving the nickel-plated steel shell, spot-welding the negative electrode lug at the bottom of the steel shell, and rolling a groove; and welding the positive lug at the position of the cap bus sheet by laser welding to prepare a semi-finished product battery cell. After baking the semi-finished product battery cell, injecting 5.4g of electrolyte, and sealing; activating to make the electrolyte fully infiltrate the anode material, the cathode material and the diaphragm; after the battery is charged and formed, the conventional 18650 lithium battery is assembled.
Testing of the lithium battery: the limit voltage of the lithium battery is 2.75V-4.2V, the lithium battery is subjected to charge-discharge cycle test in a 0.5C constant-current constant-voltage charge and 0.5C constant-current discharge mode, and the capacity retention ratio of the battery in the 200 th week is 85.2%.
The test results are shown in Table 1:
| examples | Cycle performance: capacity retention ratio of battery in 0.5C charge-discharge cycle for 200 weeks |
| Example 1 | 90.8％ |
| Example 2 | 91.3％ |
| Example 3 | 92.8％ |
| Comparative example | 85.2％ |
Table 1 shows the test results in comparative example (existing 18650 type lithium battery), example 1, example 2, and example 3. As can be seen from table 1, the capacity retention rates of the lithium batteries disclosed in embodiments 1, 2 and 3 of the present invention are greater than 90% at 0.5C cycle of charge and discharge 200 cycles compared to the conventional 18650 type lithium battery.
The lithium battery disclosed by the embodiment of the invention can be applied to the market fields of digital codes, energy storage and the like, and the positive active material adopts three positive active materials with different performances, different particle sizes and different gram capacities, so that gaps among material particles are fully utilized, and the compaction density of an electrode positive plate is improved; compared with a single positive electrode material, the electrochemical performance more balanced on the mixing of three positive electrode active materials is obtained, the advantages of different materials are complementary, the electrochemical performance of the lithium battery is improved, the capacity retention rate of the battery is more than 90% after the battery is charged and discharged for 200 cycles at 0.5C, the cost performance is high, and the market requirements can be met.
The above embodiments are only preferred embodiments of the present invention, and the protection scope of the present invention is not limited thereby, and any insubstantial changes and substitutions made by those skilled in the art based on the present invention are within the protection scope of the present invention.
Claims (10)
1. The battery positive plate is characterized by comprising a positive metal substrate, a positive lug in conductive connection with the positive metal substrate and a positive coating coated outside the positive metal substrate, wherein the positive coating comprises the following components in parts by weight:
the positive active material comprises a positive active material D and a positive active materialE and a positive electrode active material F, wherein the positive electrode active material D is LiNixCoyAl1-x-yO2Wherein x is more than or equal to 0.7 and less than or equal to 0.9, y is more than or equal to 0.1 and less than or equal to 0.3, and the positive active material E is LiNi0.5Co0.2Mn0.3O2The positive active material F is LiNi0.6Co0.2Mn0.2O2。
2. The positive electrode sheet according to claim 1, wherein the weight parts ratio of the positive electrode active material D, the positive electrode active material E and the positive electrode active material F in the positive electrode active material is (3-5): (1-3): (3-5).
3. The positive plate of the battery according to claim 1, wherein the positive coating comprises the following components in parts by weight: 97.5% of positive electrode active substance, 0.7% of positive electrode conductive agent A, 0.3% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 2: 4; or,
the anode coating comprises the following components in parts by weight: 97.3% of positive electrode active substance, 0.6% of positive electrode conductive agent A, 0.4% of positive electrode conductive agent B and 1.7% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 4: 1: 5; or,
the anode coating comprises the following components in parts by weight: 97.8% of positive electrode active substance, 0.5% of positive electrode conductive agent A, 0.2% of positive electrode conductive agent B and 1.5% of positive electrode binder, wherein the weight parts of positive electrode active material D, positive electrode active material E and positive electrode active material F in the positive electrode active substance are 5: 1: 4.
4. the positive electrode sheet for batteries according to any one of claims 1 to 3, wherein the median particle diameter of the positive electrode active material D is 10 to 12 μm, the median particle diameter of the positive electrode active material E is 9 to 11 μm, and the median particle diameter of the positive electrode active material F is 11 to 13 μm; and/or the presence of a gas in the atmosphere,
the tap density of the positive electrode active material D is 2.3-2.6g/cm3The tap density of the positive electrode active material E is 2.4-2.6g/cm3The tap density of the positive electrode active material F is 2.3-2.5g/cm3(ii) a And/or the presence of a gas in the atmosphere,
the specific surface area of the positive electrode active material D is 2-2.5m2(ii)/g, the specific surface area of the positive electrode active material E is 0.3 to 0.5m2(ii)/g, the specific surface area of the positive electrode active material F is 0.25 to 0.4m2(ii)/g; and/or the presence of a gas in the atmosphere,
the gram capacity of the positive active material D is 175-195mAh/g, the gram capacity of the positive active material E is 150-160mAh/g, and the gram capacity of the positive active material F is 155-170 mAh/g; and/or the presence of a gas in the atmosphere,
the positive electrode conductive agent A is a carbon nano tube or a carbon fiber or a combination of the carbon nano tube and graphene; and/or the presence of a gas in the atmosphere,
the positive conductive agent B is conductive graphite or conductive carbon black; and/or the presence of a gas in the atmosphere,
the positive adhesive is polyvinylidene fluoride or polyvinyl alcohol; and/or the presence of a gas in the atmosphere,
the thickness of the positive electrode metal substrate is 12 microns +/-2 microns, and the thickness of the battery positive electrode sheet is 145 microns +/-5 microns; and/or the presence of a gas in the atmosphere,
the positive electrode metal substrate is an aluminum foil.
5. The method for manufacturing a positive electrode sheet for a battery according to any one of claims 1 to 4, comprising the steps of:
a step of preparing anode slurry, in which the anode active material, the anode conductive agent A, the anode conductive agent B and the anode binder are uniformly mixed with a nitrogen-methyl pyrrolidone solvent according to the weight part ratio in the anode coating to prepare the anode slurry;
coating the positive electrode slurry on the positive electrode metal substrate to obtain a positive electrode coating intermediate product;
drying and curing the anode slurry, namely placing the anode coating intermediate product in an environment of 80-120 ℃ for drying and curing so as to dry and cure the anode slurry into the anode coating and prepare an anode cured intermediate product;
a positive plate processing step, namely sequentially rolling and cutting the positive solidified intermediate product to obtain a positive plate semi-finished product;
and a positive tab welding step, namely welding a positive tab on the semi-finished product of the positive plate to obtain the battery positive plate.
6. The method for manufacturing a positive electrode sheet for a battery according to claim 5, wherein the positive electrode slurry coating step is carried out by: coating the anode slurry on the top surface and the bottom surface of the anode metal substrate at intervals respectively so as to form two anode top coating layers arranged at intervals on the top surface of the anode metal substrate, forming two anode bottom coating layers arranged at intervals on the bottom surface of the anode metal substrate, wherein a gap between the two anode top coating layers and a gap between the two anode bottom coating layers are arranged in a vertically aligned manner; in the step of welding the positive lugs, the positive lugs are welded in a gap between two positive top coating layers of the semi-finished positive plate.
7. A lithium battery, comprising a battery case, a negative electrode plate, a first diaphragm, a second diaphragm, an electrolyte and the positive electrode plate according to any one of claims 1 to 4, wherein the positive electrode plate, the negative electrode plate, the first diaphragm, the second diaphragm and the electrolyte are all disposed in the battery case, the positive electrode plate, the negative electrode plate, the first diaphragm and the second diaphragm are all immersed in the electrolyte, the negative electrode plate is disposed between the positive electrode plate and the battery case, the first diaphragm is disposed between the positive electrode plate and the negative electrode plate, the second diaphragm is disposed between the battery case and the negative electrode plate, the negative electrode plate comprises a negative metal substrate and a negative coating coated outside the negative metal substrate, the negative coating comprises the following components in parts by weight:
the negative active material is composite graphite powder.
8. The lithium battery as claimed in claim 7, wherein the negative electrode coating comprises the following components in parts by weight: 95% of negative electrode active material, 1.5% of negative electrode conductive agent, 1.3% of suspending agent and 2.2% of negative electrode binder; or,
the negative coating comprises the following components in parts by weight: 95.2% of negative electrode active material, 1.3% of negative electrode conductive agent, 1.4% of suspending agent and 2.1% of negative electrode binder; or,
the negative coating comprises the following components in parts by weight: 95.5% of negative electrode active material, 1% of negative electrode conductive agent, 1.5% of suspending agent and 2% of negative electrode binder.
9. The lithium battery of claim 7, wherein the composite graphite powder is formed by compounding natural graphite powder and artificial stone toner; and/or the presence of a gas in the atmosphere,
the median particle diameter of the composite graphite powder A is 15-19 mu m, and the tap density of the composite graphite powder is 1-1.2g/cm3The specific surface area of the composite graphite powder is 1.2-3.0m2The gram capacity of the composite graphite powder is 340-380 mAh/g; and/or the presence of a gas in the atmosphere,
the negative conductive agent is conductive carbon black or conductive graphite or carbon nano tubes; and/or the presence of a gas in the atmosphere,
the negative electrode binder is sodium carboxymethylcellulose or styrene butadiene rubber or polyacrylic acid or sodium alginate; and/or the presence of a gas in the atmosphere,
the suspending agent is sodium carboxymethyl cellulose; and/or the presence of a gas in the atmosphere,
the thickness of the negative electrode metal substrate is 8 microns +/-2 microns, and the thickness of the battery negative electrode sheet is 160 microns +/-5 microns; and/or the presence of a gas in the atmosphere,
the negative metal substrate is a copper foil; and/or the presence of a gas in the atmosphere,
the first diaphragm and the second diaphragm are both three-layer polypropylene diaphragms manufactured by adopting a dry process; and/or the presence of a gas in the atmosphere,
the thickness of the first separator and the thickness of the second separator are both 22 μm ± 2 μm.
10. A method of manufacturing a lithium battery as claimed in any one of claims 7 to 9, comprising the steps of:
assembling the battery case, the battery positive plate, the battery negative plate, the first diaphragm and the second diaphragm, baking and injecting the electrolyte, wherein the battery positive plate is prepared by the method for manufacturing the battery positive plate according to claim 5 or 6;
the battery negative plate is prepared by the following steps:
a step of preparing cathode slurry, in which the cathode active material, the cathode conductive agent, the suspending agent and the cathode binder are uniformly mixed with deionized water according to the weight part ratio in the cathode coating to prepare cathode slurry;
coating the negative electrode slurry on the negative electrode metal substrate to dry and solidify the negative electrode slurry into a negative electrode coating to obtain a negative electrode coating intermediate product;
a step of drying and curing the cathode slurry, which is to place the cathode coating intermediate product in an environment of 80-120 ℃ for drying and curing to prepare a cathode curing intermediate product;
a negative plate processing step, namely sequentially rolling and cutting the negative solidified intermediate product to obtain a negative plate semi-finished product;
and a negative electrode tab welding step, wherein a negative electrode tab is welded on the semi-finished product of the negative electrode sheet to prepare the battery negative electrode sheet.
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