CN114597340A - Silicon-carbon negative plate and application thereof - Google Patents
Silicon-carbon negative plate and application thereof Download PDFInfo
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- CN114597340A CN114597340A CN202210255728.3A CN202210255728A CN114597340A CN 114597340 A CN114597340 A CN 114597340A CN 202210255728 A CN202210255728 A CN 202210255728A CN 114597340 A CN114597340 A CN 114597340A
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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Abstract
The invention provides a silicon-carbon negative plate and application thereof. According to the invention, the graphite layer, the silicon-carbon composite layer and the graphite layer are arranged on the two sides of the current collector, and the graphite layer is arranged to avoid side reactions caused by contact between the silicon-carbon composite layer and the electrolyte, so that the direct current internal resistance of the battery is effectively reduced, the large current damage caused by contact between the silicon-carbon composite layer and the current collector is avoided, and the storage capacity retention rate and the long-term stability of the battery are improved.
Description
Technical Field
The invention belongs to the field of batteries, relates to a negative plate, and particularly relates to a silicon-carbon negative plate and application thereof.
Background
Sub-silicon oxide material (SiO)x) The lithium ion battery has higher theoretical specific capacity and lower reaction potential, so that the lithium ion battery is applied to a power battery system with high energy density. However, the charged volume expansion of the silicon monoxide reaches 150%, and the huge volume expansion and shrinkage cause the silicon monoxide to generate particle cracks and pulverization in the charging and discharging process, new surface consumption lithium ions are continuously generated, particles are separated from a conductive agent or a current collector, and the cycle stability of the silicon monoxide negative electrode is reduced.
Although C-SiO is obtained by blending a silica with graphitexMaterial of SiOxThe volume expansion of (a) is borne by the graphite. However, SiOxBlending with graphite to form SiOxThe distribution of the lithium ion battery cathode in the cathode is random, and when the lithium ion battery cathode is distributed on the surface of the cathode, the lithium ion battery cathode and the electrolyte generate side reaction, so that the active lithium is excessively consumed, the impedance of the battery is increased, and the capacity of the battery is reduced; when the current collector is distributed on the surface of the current collector, local structural damage is caused by overlarge local current, and the impedance of the battery is increased.
Based on the above research, it is necessary to provide a silicon-carbon negative electrode plate, in which the silicon-oxygen material is not directly corroded by the electrolyte and damaged by large current, so as to reduce the direct current internal resistance of the battery and improve the capacity of the battery, which is a problem to be solved urgently at present.
Disclosure of Invention
The invention aims to provide a silicon-carbon negative plate and application thereof, and C-SiO of the silicon-carbon negative platexCan be protected and not directly contacted with electrolyte and negative current collector, thereby avoiding SiOxThe electrolyte reacts with the electrolyte, and the large current is destroyed, so that the capacity of the battery is improved, and the direct current internal resistance is reduced.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the invention provides a silicon-carbon negative plate, which comprises a current collector, and a graphite layer, a silicon-carbon composite layer and a graphite layer which are sequentially arranged on two sides of the current collector.
The graphite layers are arranged on the two sides of the silicon-carbon composite layer, namely, the graphite layers, the silicon-carbon composite layer and the graphite layers are arranged on the two sides of the negative current collector, so that the silicon-carbon composite layer is prevented from being directly contacted with the electrolyte and the negative current collector; compared with a silicon-carbon negative plate obtained by direct mixing, the battery with the three-layer structure design has smaller direct current internal resistance value and better storage capacity retention rate, and the long-term stability of the battery is effectively improved.
The silicon-carbon negative plate is structurally characterized by comprising a graphite layer, a silicon-carbon composite layer, a graphite layer, a current collector, a graphite layer, a silicon-carbon composite layer and a graphite layer which are sequentially stacked.
Preferably, the thickness of the silicon-carbon composite layer is 20 μm to 80 μm, and may be, for example, 20 μm, 30 μm, 40 μm, 50 μm, 60 μm, 70 μm or 80 μm, but is not limited to the enumerated values, and other values not enumerated within the numerical range are also applicable.
Preferably, the graphite layer has a thickness of 10 μm to 40 μm, and may be, for example, 10 μm, 15 μm, 20 μm, 25 μm, 30 μm, 35 μm or 40 μm, but is not limited to the values recited, and other values not recited within the range of values are equally applicable.
The thickness of the graphite layer is in a reasonable range, so that the contact between the silicon-carbon negative electrode plate and the electrolyte and the current collector can be effectively prevented, and the capacity of the silicon-carbon composite layer can be effectively exerted to the maximum extent.
Preferably, the silicon-carbon composite layer comprises a silicon-oxygen material, and the particle diameter D of the silicon-oxygen material50Is 4 μm to 10 μm, and may be, for example, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm or 10 μm, but is not limited to the values recited, and other values not recited in the numerical range are also applicable.
Preferably, the silicon-carbon composite layer further comprises graphite, a conductive agent and a binder.
The silicon-oxygen material is coated by carbon, so that the volume expansion of the silicon-oxygen material is shared by the carbon, the influence of the volume expansion of the silicon-oxygen material on the performance of the battery is reduced, and the reasonable carbon coating amount can increase the integral capacity of the negative plate while reducing the influence of the volume expansion on the battery.
Preferably, the graphite layer includes a graphite material, a conductive agent, and a binder.
Preferably, the mass ratio of the graphite material, the conductive agent and the binder is (90 to 99):1:3, for example 90:1:3, 95:1:3 or 99:1:3, but is not limited to the values listed, and other values not listed within the range of values are equally applicable.
The graphite layer of the present invention also includes a conductive agent and a binder, i.e., the graphite layer can not only serve as a buffer layer, but also serve as an active material layer.
Preferably, the particle size D of the graphite material508 μm to 18 μm, for example 8 μm, 10 μm, 12 μm, 14 μm, 16 μm or 18 μm, but is not limited to the values listed, and other values not listed in the numerical range are also applicable.
Preferably, the particle type of the graphite material includes single particles and/or secondary particles.
The graphite material is single particles and/or secondary particles, and the secondary particles are particles formed by agglomeration of the single particles.
Preferably, the graphite material comprises any one of or a combination of at least two of artificial graphite, natural graphite, or hard carbon, and typical but non-limiting combinations include a combination of artificial graphite and natural graphite, a combination of natural graphite and hard carbon, or a combination of artificial graphite and hard carbon.
Preferably, the current collector includes an aluminum foil or a copper foil.
The preparation method of the silicon-carbon negative plate comprises the step of coating the silicon-carbon composite layer slurry and the graphite layer slurry according to the structure of the silicon-carbon negative plate according to the formula amount to obtain the silicon-carbon negative plate.
Preferably, the coating manner includes one extrusion coating, two extrusion coating or three extrusion coating.
In a second aspect, the invention provides a lithium ion battery comprising the silicon-carbon negative electrode sheet according to the first aspect.
Compared with the prior art, the invention has the following beneficial effects:
according to the invention, the graphite layer, the silicon-carbon composite layer and the graphite layer are arranged on the two sides of the current collector, and the buffering of the graphite layer is utilized to avoid side reactions caused by the contact of the silicon-carbon composite layer and the electrolyte, so that the direct current internal resistance of the battery is effectively reduced, the large current damage caused by the contact of the silicon-carbon composite layer and the current collector is avoided, and the storage capacity retention rate and the long-term stability of the battery are improved.
Drawings
Fig. 1 is a schematic structural view of the silicon-carbon negative electrode sheet according to examples 1 to 3;
fig. 2 is a graph of capacity retention rate versus storage time for batteries prepared from the silicon-carbon negative electrode sheets described in example 1 and comparative example 1;
fig. 3 is a graph of resistance versus state of charge for batteries prepared from the silicon-carbon negative electrode sheets described in example 1 and comparative example 1;
the device comprises a current collector 1, a silicon-carbon composite layer 2 and a graphite layer 3.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
Example 1
The embodiment provides a silicon-carbon negative electrode sheet as shown in fig. 1, which includes a graphite layer 3, a silicon-carbon composite layer 2, a graphite layer 3, a current collector 1, a graphite layer 3, a silicon-carbon composite layer 2, and a graphite layer 3, which are sequentially stacked;
the thickness of the silicon-carbon composite layer 2 is 50 micrometers, and the thickness of the graphite layer 3 is 15 micrometers;
the silicon-carbon composite layer 2 comprises a silica material, graphite, conductive carbon black, conductive carbon nanotubes, styrene butadiene rubber and sodium carboxymethyl cellulose in a mass ratio of 27:63:1:0.5:1: 0.5;
the graphite layer 3 comprises artificial graphite, conductive carbon black, styrene butadiene rubber and sodium carboxymethylcellulose in a mass ratio of 95:1:2: 1;
particle diameter D of the silicon oxide material50Is 7 μm; particle diameter D of the artificial graphite50Is 8 μm; the current collector 1 is a copper foil;
the preparation method of the silicon-carbon negative plate comprises the following steps: coating the slurry of the silicon-carbon composite layer 2 and the slurry of the graphite layer 3 according to the structure of the silicon-carbon negative plate according to the formula amount to obtain the silicon-carbon negative plate;
the coating mode is secondary extrusion coating;
the change graph of the capacity retention rate of the battery prepared from the silicon-carbon negative electrode sheet along with the storage time is shown in fig. 2, and the change graph of the resistance along with the charge state is shown in fig. 3.
Example 2
The embodiment provides a silicon-carbon negative electrode sheet as shown in fig. 1, which includes a graphite layer 3, a silicon-carbon composite layer 2, a graphite layer 3, a current collector 1, a graphite layer 3, a silicon-carbon composite layer 2, and a graphite layer 3, which are sequentially stacked;
the thickness of the silicon-carbon composite layer 2 is 20 micrometers, and the thickness of the graphite layer 3 is 10 micrometers;
the silicon-carbon composite layer 2 comprises a silica material, graphite, conductive carbon black, conductive carbon nanotubes, styrene butadiene rubber and sodium carboxymethyl cellulose in a mass ratio of 30:60:1:0.5:1: 0.5;
the graphite layer 3 comprises artificial graphite, conductive carbon black, styrene butadiene rubber and sodium carboxymethylcellulose in a mass ratio of 99:1:2: 1;
particle diameter D of the silicon oxide material50Is 4 μm; particle diameter D of the artificial graphite50Is 8 μm; the current collector 1 is a copper foil;
the preparation method of the silicon-carbon negative plate comprises the following steps: coating the slurry of the silicon-carbon composite layer 2 and the slurry of the graphite layer 3 according to the structure of the silicon-carbon negative plate according to the formula amount to obtain the silicon-carbon negative plate;
the coating mode is one-time extrusion coating.
Example 3
The embodiment provides a silicon-carbon negative electrode sheet as shown in fig. 1, which includes a graphite layer 3, a silicon-carbon composite layer 2, a graphite layer 3, a current collector 1, a graphite layer 3, a silicon-carbon composite layer 2, and a graphite layer 3, which are sequentially stacked;
the thickness of the silicon-carbon composite layer 2 is 80 micrometers, and the thickness of the graphite layer 3 is 40 micrometers;
the silicon-carbon composite layer 2 comprises a silica material, conductive carbon black, conductive carbon nano tubes, styrene butadiene rubber and sodium carboxymethyl cellulose in a mass ratio of 28:62:1:0.5:1: 0.5;
the graphite layer 3 comprises artificial graphite, conductive carbon black, styrene butadiene rubber and sodium carboxymethylcellulose in a mass ratio of 90:1:2: 1;
particle diameter D of the silicon oxide material50Is 10 μm; particle diameter D of the artificial graphite50Is 18 μm; the current collector 1 is a copper foil;
the preparation method of the silicon-carbon negative plate comprises the following steps: coating the slurry of the silicon-carbon composite layer 2 and the slurry of the graphite layer 3 according to the structure of the silicon-carbon negative plate according to the formula amount to obtain the silicon-carbon negative plate;
the coating mode is three times of extrusion coating.
In examples 4 and 5, as shown in table 2, the thickness of the graphite layer was changed, and the ratio of the silica material to graphite in the silicon-carbon composite layer was changed, so that the content of the silica material in comparison with the negative electrode sheet was the same as in example 1, and the other conditions were the same as in example 1.
Comparative example 1 as shown in table 3, except that no graphite layer was provided, the ratio of the silica material to graphite in the silicon-carbon composite layer was changed accordingly, so that the content of the silica material in comparison with the negative electrode sheet was the same as in example 1, and the rest was the same as in example 1; the change graph of the capacity retention rate of the battery prepared from the obtained silicon-carbon negative electrode sheet along with the storage time is shown in fig. 2, and the change graph of the resistance along with the charge state is shown in fig. 3.
Comparative examples 2 and 3 as shown in table 3, the same as example 1 except that the position where the graphite layer was disposed was changed.
And (3) performance testing:
the thickness of the graphite layer and the silicon-carbon composite layer is obtained by testing with a reference microscope method (GB/T6462-; when the layers are embedded into each other, in addition to testing at the middle and both ends, testing is also required at the embedded part and both ends of the embedded part, and the average value is taken as the thickness of the final test layer.
According to the invention, the difference between the silicon-carbon composite layer and the graphite layer is distinguished through the difference of the section contrast of the graphite layer and the silicon-carbon composite layer, and the thickness of each layer is tested by referring to the microscope method.
The silicon-carbon negative plate obtained in the above examples and comparative examples, lithium iron phosphate positive plate, polyethylene diaphragm and 1mol/L LiPF6The method comprises the following steps of (1) assembling a/EC + DMC + EMC electrolyte into a 1Ah soft package battery according to a general process for preparing the lithium ion battery; forming and aging the soft package battery, defining the actual capacity of the battery after one-time charging and discharging with the current density of 0.33C and the voltage window of 2.0-3.65V, and then adjusting the state of charge of the battery to 100% SOC; and storing the battery in a constant-temperature oven at 60 ℃, taking the battery out of the oven every 15 days, standing to room temperature, testing the discharge capacity of the battery at 0.33C rate, and charging the battery to 4.2V voltage at 0.33C current to obtain the capacity retention rate of the battery.
After the state of charge of the battery is adjusted to 70% SOC, the battery is discharged for 30s at a current density of 4C, and the voltage difference value before and after the discharge is divided by the current density to obtain a direct current resistance value (DCR) at the state of charge (SOC); the DCR values of 50% SOC and 30% SOC can be measured by the method.
The test results are shown in tables 1 to 3:
TABLE 1
TABLE 2
TABLE 3
From tables 1 to 3, the following points can be seen:
(1) as can be seen from embodiments 1 to 5, the graphite layers are arranged on the two sides of the silicon-carbon composite layer, so that the silicon-carbon composite layer can be prevented from being directly contacted with the electrolyte and the negative current collector, the direct current internal resistance of the battery is effectively reduced, and the storage stability of the battery is improved; as is clear from examples 1, 4 and 5, when the content of the silicon oxide material in the negative electrode sheet was not changed, the thickness of the graphite layer was changed, which affected the performance of the battery.
(2) As can be seen from example 1 and comparative example 1, in comparative example 1, the graphite layer is not provided, which causes a side reaction between the silicon-carbon composite layer and the electrolyte, and increases the internal resistance of the battery, that is, the battery performance provided in comparative example 1 is inferior to that of example 1; as can be seen from example 1, comparative example 2, and comparative example 3, comparative example 2 provided the graphite layer only on the side of the silicon-carbon composite layer close to the current collector, which slightly improved the internal resistance of the battery, but did not significantly improve the storage performance, and comparative example 3 provided the graphite layer only on the side of the silicon-carbon composite layer far from the current collector, which slightly improved the storage performance, but did not significantly improve the battery, that is, the structure provided in example 1 gave the best overall performance of the battery.
In summary, the invention provides a silicon-carbon negative plate, and the graphite layer is arranged to prevent the silicon-carbon composite layer from directly contacting with the electrolyte and the negative current collector, and compared with the silicon-carbon negative plate obtained by direct blending, the battery with the three-layer structure design has a smaller direct current internal resistance value and a better storage capacity retention rate, and the long-term stability of the battery is effectively improved.
The above description is only for the specific embodiment of the present invention, but the protection scope of the present invention is not limited thereto, and it should be understood by those skilled in the art that any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are within the protection scope and the disclosure of the present invention.
Claims (10)
1. The silicon-carbon negative plate is characterized by comprising a current collector, and a graphite layer, a silicon-carbon composite layer and a graphite layer which are sequentially arranged on two sides of the current collector respectively.
2. The silicon-carbon negative electrode sheet according to claim 1, wherein the thickness of the silicon-carbon composite layer is 20 μm to 80 μm.
3. The silicon-carbon negative electrode sheet according to claim 1 or 2, wherein the graphite layer has a thickness of 10 μm to 40 μm.
4. The silicon-carbon negative electrode sheet according to claim 1, wherein the silicon-carbon composite layer comprises a silicon-oxygen material, and the particle diameter D of the silicon-oxygen material50Is 4 μm to 10 μm.
5. The silicon-carbon negative electrode sheet according to claim 4, wherein the silicon-carbon composite layer further comprises graphite, a conductive agent and a binder.
6. The silicon-carbon negative electrode sheet according to claim 1, wherein the graphite layer comprises a graphite material, a conductive agent, and a binder.
7. The silicon-carbon negative electrode sheet according to claim 6, wherein the mass ratio of the graphite material to the conductive agent to the binder is (90 to 99):1: 3.
8. The silicon-carbon negative electrode sheet according to claim 7, wherein the negative electrode sheet comprisesThe particle diameter D of the graphite material508 to 18 μm.
9. The silicon-carbon negative electrode sheet according to claim 7, wherein the graphite material comprises any one of or a combination of at least two of artificial graphite, natural graphite, or hard carbon.
10. A lithium ion battery, characterized in that the lithium ion battery comprises the silicon-carbon negative electrode sheet according to any one of claims 1 to 9.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115172652A (en) * | 2022-07-15 | 2022-10-11 | 惠州市豪鹏科技有限公司 | Silicon-based negative plate and battery thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107528044A (en) * | 2017-07-25 | 2017-12-29 | 深圳市沃特玛电池有限公司 | A kind of lithium ion battery negative electrode and preparation method thereof |
| CN111540882A (en) * | 2020-06-04 | 2020-08-14 | 湖北亿纬动力有限公司 | A kind of negative pole piece, its preparation method and use |
| CN213093250U (en) * | 2020-07-23 | 2021-04-30 | 常州赛得能源科技有限公司 | Lithium ion battery with composite structure negative electrode |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107528044A (en) * | 2017-07-25 | 2017-12-29 | 深圳市沃特玛电池有限公司 | A kind of lithium ion battery negative electrode and preparation method thereof |
| CN111540882A (en) * | 2020-06-04 | 2020-08-14 | 湖北亿纬动力有限公司 | A kind of negative pole piece, its preparation method and use |
| CN213093250U (en) * | 2020-07-23 | 2021-04-30 | 常州赛得能源科技有限公司 | Lithium ion battery with composite structure negative electrode |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115172652A (en) * | 2022-07-15 | 2022-10-11 | 惠州市豪鹏科技有限公司 | Silicon-based negative plate and battery thereof |
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