CN110783632A - Formation method of lithium ion battery with mixed electrode - Google Patents
Formation method of lithium ion battery with mixed electrode Download PDFInfo
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- CN110783632A CN110783632A CN201911080773.4A CN201911080773A CN110783632A CN 110783632 A CN110783632 A CN 110783632A CN 201911080773 A CN201911080773 A CN 201911080773A CN 110783632 A CN110783632 A CN 110783632A
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- 238000000034 method Methods 0.000 title claims abstract description 26
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 24
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 15
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 15
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims abstract description 19
- HFCVPDYCRZVZDF-UHFFFAOYSA-N [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O Chemical compound [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O HFCVPDYCRZVZDF-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 claims abstract description 5
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229910015243 LiMg Inorganic materials 0.000 claims abstract description 4
- 229910012888 LiNi0.6Co0.1Mn0.3O2 Inorganic materials 0.000 claims abstract description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000013543 active substance Substances 0.000 claims abstract description 3
- 238000007600 charging Methods 0.000 claims description 51
- 238000007599 discharging Methods 0.000 claims description 29
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- 229910002804 graphite Inorganic materials 0.000 claims description 2
- 239000010439 graphite Substances 0.000 claims description 2
- 239000000463 material Substances 0.000 description 12
- 239000003792 electrolyte Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 238000010277 constant-current charging Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- -1 lithium hexafluorophosphate Chemical compound 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- CQDGTJPVBWZJAZ-UHFFFAOYSA-N monoethyl carbonate Chemical compound CCOC(O)=O CQDGTJPVBWZJAZ-UHFFFAOYSA-N 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 238000004904 shortening Methods 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
Classifications
-
- 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
- H01M10/058—Construction or manufacture
-
- 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
-
- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention provides a formation method of a lithium ion battery with a mixed electrode, wherein active substances of the mixed electrode comprise nickel cobalt lithium manganate and lithium iron phosphate, and the nickel cobalt lithium manganate is LiNi
0.6Co
0.1Mn
0.3O
2The lithium iron phosphate is LiMg
0.02Fe
0.98PO
4. Wherein the lithium nickel cobalt manganese oxide: the mass ratio of the lithium iron phosphate is 75:25-80:20, and the formation method comprises a charge-discharge cycle within a range of 3.55-3.65V and a charge-discharge cycle within a range of 3.70-3.90V in the charge-discharge process.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries with mixed electrodes, in particular to a formation method of a lithium ion battery with a mixed electrode.
Background
In the power battery, the energy density, the safety and the manufacturing cost of the battery are higher, the ternary material and the lithium iron phosphate battery have good high temperature resistance and safety performance, and are the first choice as the active material of the power battery, and the mixed electrodes of different materials are beneficial to improving the energy density of the lithium ion battery, however, because the working voltage of the ternary material is different from the working voltage of the lithium iron phosphate, two working platforms can appear in the charging and discharging process, the working platform of the lithium iron phosphate is under the action of 3.6V, the starting voltage and the ending voltage of the platform are closer, the working platform is more gentle, the ternary material has three different transition metals, the inclination of the working platform is larger and is generally about 3.8V, and for the mixed material of the ternary material and the lithium iron phosphate, the common formation mode is difficult to fully activate and form two different materials at the same time, and SEI film formation is insufficient, and thus lithium ions are irreversibly intercalated during cycling in many cases, resulting in a decrease in durability of the battery.
Disclosure of Invention
Aiming at the problems, the invention provides a formation method of a lithium ion battery with a mixed electrode, which comprises a pre-lithium-embedding formation step a of a carbon negative electrode and a formation step b of the lithium ion battery after the battery is assembled, and through the formation steps, the quantity of transferred lithium between a positive electrode and a negative electrode can be increased, and the quantity of lithium ions lost by an SEI film can be compensated, so that the rate capability of the battery is improved; in addition, through the formation step b of the present invention, a stable SEI film can be formed by controlling the formation process, thereby improving the cyclicity of the lithium ion battery.
The specific scheme is as follows:
a formation method of a lithium ion battery with a mixed electrode is provided, wherein active substances of the mixed electrode comprise nickel cobalt lithium manganate and lithium iron phosphate, and the nickel cobalt lithium manganate is LiNi
0.6Co
0.1Mn
0.3O
2The lithium iron phosphate is LiMg
0.02Fe
0.98PO
4The formation method comprises the following steps: during the charging and discharging process, the charging and discharging cycle is carried out for a plurality of times within the range of 3.55-3.65V, and the charging and discharging cycle is carried out for a plurality of times within the range of 3.70-3.90V.
Further, the formation method comprises the following steps:
1) pre-charging the battery, and charging the battery to 2.9-3.0V at a constant current of 0.01-0.02C;
2) adjusting current, and charging to 3.55V at constant current of 0.02-0.05C;
3) performing constant current charge and discharge at 0.05-0.1C for several times within the range of 3.55-3.65V;
4) charging to 3.7V with a constant current of 0.05-0.1C;
5) performing constant current charge and discharge at 0.02-0.05C for several times within the range of 3.70-3.90V;
6) charging to a charge cut-off voltage by a constant current of 0.05-0.1C, wherein the charge cut-off voltage is 4.2-4.3V;
7) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
8) discharging to 3.7V with constant current of 0.05-0.1C;
9) performing constant current charge and discharge at 0.05-0.1C for several times within the range of 3.70-3.90V;
10) discharging to 3.55V with constant current of 0.05-0.1C;
11) performing constant current charge and discharge at 0.1-0.2C within the range of 3.55-3.65V for several times;
12) discharging with a constant current of 0.05-0.1C to a discharge cut-off voltage of 2.7-2.8V;
13) charging to 3.3-3.55V with 0.1-0.2C current.
Further, the negative electrode of the battery is a graphite negative electrode.
Further, the current of the step 2 is larger than that of the step 1.
Further, the current of the step 3 is 2-3 times of the current of the step 5.
Further, the current of the step 11 is 2-3 times of the current of the step 9.
Further, wherein the lithium nickel cobalt manganese oxide: the mass ratio of the lithium iron phosphate is 70:30-90: 10.
Further, wherein the lithium nickel cobalt manganese oxide: the mass ratio of the lithium iron phosphate is 83: 17.
The invention has the following beneficial effects:
1) the initial voltage interval and the final voltage interval of the discharging platform of the lithium iron phosphate and the nickel cobalt lithium manganate used in the invention are respectively 3.55-3.65V and 3.70-3.90V, in the interval, a large amount of lithium ions are inserted or removed, the voltage change is not large, and a certain amount of charging and discharging circulation is carried out in the interval, so that the battery material is activated;
2) performing charge and discharge cycles in a specific operating voltage interval of the specific material, wherein a stable SEI film can be formed because a voltage change rate is small although a large amount of lithium ions are inserted and extracted in the interval;
3) the current is gradually increased in the initial pre-formation process, which is beneficial to gradually activating the anode material of the battery;
4) and because the working voltage of the lithium iron phosphate is more stable than that of the ternary material, the circulating current of the working voltage platform of the ternary material is lower than that of the working voltage platform of the lithium iron phosphate, so that the voltage change rates of the two platforms during charging and discharging are as close as possible, an SEI film with good consistency is formed, and the stability of the battery is improved, preferably, the circulating current near the working platform of the lithium iron phosphate is about 2-3 times of the circulating current near the working voltage of the ternary material.
5) The invention has short formation time, only carries out charge-discharge circulation in a specific voltage interval and only needs to charge and discharge once in a complete voltage interval, thereby greatly shortening the formation time and improving the stability and the production efficiency of products.
Detailed Description
The present invention will be described in more detail below with reference to specific examples, but the scope of the present invention is not limited to these examples.
The positive electrode of the battery adopted by the invention is a mixed electrode comprising LiNi
0.6Co
0.1Mn
0.3O
2And LiMg
0.02Fe
0.98PO
4The negative electrode is 2:1 of natural graphite and artificial graphite; the electrolyte consists of electrolyte salt and electrolyte solvent, wherein the electrolyte salt is 1M lithium hexafluorophosphate, and the electrolyte solvent is a mixed solvent of ethyl carbonate and dimethyl carbonate in a volume ratio of 1: 2.
Example 1
1) Charging to 2.9V with a current of 0.01C;
2) charging to 3.55V with a current of 0.02C;
3) performing constant current charge and discharge at 0.05C for 4 times within the range of 3.55-3.65V;
4) charging to 3.7V with a current of 0.05C;
5) performing constant current charging and discharging at 0.02C in the range of 3.70-3.90V for 4 times;
6) charging to a charge cut-off voltage with a constant current of 0.05C, wherein the charge cut-off voltage is 4.2V;
7) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
8) discharging to 3.7V at constant current of 0.05C;
9) performing constant current charge and discharge at 0.05C for 4 times within the range of 3.70-3.90V;
10) discharging to 3.55V at constant current of 0.05C;
11) performing constant current charge and discharge at 0.1C within the range of 3.55-3.65V for 4 times;
12) discharging at constant current of 0.05C to discharge cut-off voltage, wherein the discharge cut-off voltage is 2.7V;
13) the battery was charged to 3.3V with a constant current of 0.1C.
Example 2
1) Charging to 3.0V with a current of 0.02C;
2) charging to 3.55V with a current of 0.05C;
3) performing constant current charge and discharge at 0.1C within the range of 3.55-3.65V for 4 times;
4) charging to 3.7V with a current of 0.1C;
5) performing constant current charge and discharge at 0.05C for 4 times within the range of 3.70-3.90V;
6) charging to a charge cut-off voltage with a constant current of 0.1C, wherein the charge cut-off voltage is 4.3V;
7) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
8) discharging to 3.7V with a constant current of 0.1C;
9) performing constant current charge and discharge at 0.1C for 4 times within the range of 3.70-3.90V;
10) discharging to 3.55V with a constant current of 0.1C;
11) performing constant current charge and discharge at 0.2C within the range of 3.55-3.65V for 4 times;
12) discharging at constant current of 0.1C to discharge cut-off voltage, wherein the discharge cut-off voltage is 2.8V;
13) the battery was charged to 3.55V with a constant current of 0.2C.
Example 3
1) Charging to 3.0V with a current of 0.01C;
2) charging to 3.55V with a constant current of 0.03C;
3) performing constant current charging and discharging at 0.06C within the range of 3.55-3.65V for 4 times;
4) charging to 3.7V with a constant current of 0.06C;
5) performing constant current charging and discharging at 0.02C in the range of 3.70-3.90V for 4 times;
6) charging to a charge cut-off voltage with a constant current of 0.06C, wherein the charge cut-off voltage is 4.25V;
7) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
8) discharging to 3.7V with a constant current of 0.06C;
9) performing constant current charge and discharge at 0.05C for 4 times within the range of 3.70-3.90V;
10) discharging to 3.55V with a constant current of 0.1C;
11) performing constant current charge and discharge at 0.15C within the range of 3.55-3.65V for 4 times;
12) discharging at a constant current of 0.1C to a discharge cut-off voltage, wherein the discharge cut-off voltage is 2.75V;
13) the battery was charged to 3.4V with a constant current of 0.1C.
Comparative example 1
The battery of example 1 was used
1) Charging to 2.9-3.0V with a current of 0.01C;
2) charging to 3.55V with a current of 0.02C;
3) charging to 3.7V with a current of 0.05C;
4) charging to a charge cut-off voltage with a constant current of 0.1C, wherein the charge cut-off voltage is 4.2V;
5) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
6) discharging at constant current of 0.1C to discharge cut-off voltage, wherein the discharge cut-off voltage is 2.7V;
7) the charge and discharge were performed 5 times at a constant current between the charge cut-off voltage and the discharge cut-off voltage at a current of 0.1C.
Comparative example 2
The battery of example 2 was used
1) Charging to 2.9-3.0V with a current of 0.01C;
2) charging to 3.55V with a current of 0.02C;
3) charging to 3.7V with a current of 0.05C;
4) charging to a charge cut-off voltage with a constant current of 0.1C, wherein the charge cut-off voltage is 4.2V;
5) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
6) discharging at constant current of 0.1C to discharge cut-off voltage, wherein the discharge cut-off voltage is 2.7V;
7) the charge and discharge were performed 5 times at a constant current between the charge cut-off voltage and the discharge cut-off voltage at a current of 0.1C.
Comparative example 3
The battery of example 3 was used
1) Charging to 2.9-3.0V with a current of 0.01C;
2) charging to 3.55V with a current of 0.02C;
3) charging to 3.7V with a current of 0.05C;
4) charging to a charge cut-off voltage with a constant current of 0.1C, wherein the charge cut-off voltage is 4.2V;
5) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
6) discharging at constant current of 0.1C to discharge cut-off voltage, wherein the discharge cut-off voltage is 2.7V;
7) the charge and discharge were performed 5 times at a constant current between the charge cut-off voltage and the discharge cut-off voltage at a current of 0.1C.
Experiment and data
The batteries obtained according to the methods of examples 1 to 3 and comparative examples 1 to 3 were subjected to charge and discharge cycles at 1C for 50 times and 100 times, respectively, and the results are shown in the following table. As can be seen from the following table, although the cycle performance of the battery is not much different within 50 cycles, after 100 cycles, the difference of the capacity retention performance is obvious, and the formation method of the invention occupies shorter time, thereby effectively improving the stability of the product and the formation efficiency.
TABLE 1
While the present invention has been described in detail with reference to the preferred embodiments, it should be understood that the above description should not be taken as limiting the invention.
Claims (8)
1. A formation method of a lithium ion battery with a mixed electrode is provided, wherein active substances of the mixed electrode comprise nickel cobalt lithium manganate and lithium iron phosphate, and the nickel cobalt lithium manganate is LiNi
0.6Co
0.1Mn
0.3O
2The lithium iron phosphate is LiMg
0.02Fe
0.98PO
4The formation method comprises the following steps: in the process of charging and discharging, the voltage is in the range of 3.55-3.65VSeveral times of charge-discharge cycles in the range, and several times of charge-discharge cycles in the interval of 3.70-3.90V.
2. The formation method according to claim 1, which consists of the following steps:
1) pre-charging the battery, and charging the battery to 2.9-3.0V at a constant current of 0.01-0.02C;
2) adjusting current, and charging to 3.55V at constant current of 0.02-0.05C;
3) performing constant current charge and discharge at 0.05-0.1C for several times within the range of 3.55-3.65V;
4) charging to 3.7V with a constant current of 0.05-0.1C;
5) performing constant current charge and discharge at 0.02-0.05C for several times within the range of 3.70-3.90V;
6) charging to a charge cut-off voltage by a constant current of 0.05-0.1C, wherein the charge cut-off voltage is 4.2-4.3V;
7) charging at constant voltage with a charge cut-off voltage until the charge current is lower than 0.01C;
8) discharging to 3.7V with constant current of 0.05-0.1C;
9) performing constant current charge and discharge at 0.05-0.1C for several times within the range of 3.70-3.90V;
10) discharging to 3.55V with constant current of 0.05-0.1C;
11) performing constant current charge and discharge at 0.1-0.2C within the range of 3.55-3.65V for several times;
12) discharging with a constant current of 0.05-0.1C to a discharge cut-off voltage of 2.7-2.8V;
13) charging to 3.3-3.55V with 0.1-0.2C current.
3. The method of the preceding claim, the negative electrode of the battery being a graphite negative electrode.
4. The method of claims 2-3, wherein the current of step 2 is greater than the current of step 1.
5. The method of claims 2-4, wherein the current of step 3 is 2-3 times the magnitude of the current of step 5.
6. The method of claims 2-5, wherein the current of step 11 is 2-3 times the magnitude of the current of step 9.
7. The method of claim wherein the lithium nickel cobalt manganese oxide: the mass ratio of the lithium iron phosphate is 70:30-90: 10.
8. The method of claim wherein the lithium nickel cobalt manganese oxide: the mass ratio of the lithium iron phosphate is 83: 17.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111342028A (en) * | 2020-03-20 | 2020-06-26 | 金妍 | Formation method of lithium ion battery with graphite-based cathode |
| CN111430694A (en) * | 2020-04-09 | 2020-07-17 | 盛蕾 | Mixing method of composite anode slurry |
| WO2024098271A1 (en) * | 2022-11-09 | 2024-05-16 | 广州丰江电池新技术股份有限公司 | Charging method for battery made of mixed system material of lithium iron phosphate and ternary |
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