CN114583240A - Lithium ion battery - Google Patents
Lithium ion battery Download PDFInfo
- Publication number
- CN114583240A CN114583240A CN202011370485.5A CN202011370485A CN114583240A CN 114583240 A CN114583240 A CN 114583240A CN 202011370485 A CN202011370485 A CN 202011370485A CN 114583240 A CN114583240 A CN 114583240A
- Authority
- CN
- China
- Prior art keywords
- positive electrode
- lithium ion
- ion battery
- carbonate
- coo
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 80
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 80
- 239000007774 positive electrode material Substances 0.000 claims abstract description 65
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 43
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 43
- 150000001875 compounds Chemical class 0.000 claims abstract description 40
- 239000008151 electrolyte solution Substances 0.000 claims abstract description 29
- 239000011247 coating layer Substances 0.000 claims abstract description 28
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 20
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 20
- 229910003063 Li1−xCoO2 Inorganic materials 0.000 claims abstract description 13
- 239000003960 organic solvent Substances 0.000 claims abstract description 12
- 125000003118 aryl group Chemical group 0.000 claims abstract description 7
- 125000004432 carbon atom Chemical group C* 0.000 claims abstract description 7
- -1 cyclic carbonate compound Chemical class 0.000 claims description 27
- 239000011255 nonaqueous electrolyte Substances 0.000 claims description 19
- 239000000654 additive Substances 0.000 claims description 15
- 239000010405 anode material Substances 0.000 claims description 14
- 239000007773 negative electrode material Substances 0.000 claims description 11
- 230000000996 additive effect Effects 0.000 claims description 10
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 9
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 9
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 8
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 7
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 7
- 239000000395 magnesium oxide Substances 0.000 claims description 7
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- CREMABGTGYGIQB-UHFFFAOYSA-N carbon carbon Chemical compound C.C CREMABGTGYGIQB-UHFFFAOYSA-N 0.000 claims description 6
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- 150000005676 cyclic carbonates Chemical class 0.000 claims description 6
- 150000002170 ethers Chemical class 0.000 claims description 6
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 6
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- 125000001153 fluoro group Chemical group F* 0.000 claims description 6
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- DFJYZCUIKPGCSG-UHFFFAOYSA-N decanedinitrile Chemical compound N#CCCCCCCCCC#N DFJYZCUIKPGCSG-UHFFFAOYSA-N 0.000 claims description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 3
- HHEIMYAXCOIQCJ-UHFFFAOYSA-N ethyl 2,2-dimethylpropanoate Chemical compound CCOC(=O)C(C)(C)C HHEIMYAXCOIQCJ-UHFFFAOYSA-N 0.000 claims description 3
- LLEVMYXEJUDBTA-UHFFFAOYSA-N heptanedinitrile Chemical compound N#CCCCCCC#N LLEVMYXEJUDBTA-UHFFFAOYSA-N 0.000 claims description 3
- 229910003437 indium oxide Inorganic materials 0.000 claims description 3
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 14
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Classifications
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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- H—ELECTRICITY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
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- H01M4/366—Composites as layered products
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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Abstract
The invention relates to the technical field of new energy, and discloses a lithium ion battery which comprises a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode, and a non-aqueous electrolyteA positive electrode containing a positive electrode material, wherein a positive electrode active material of the positive electrode material contains Li1‑xCoO2(0≤x<1) And Li1‑xCoO2The surface is provided with a metal oxide coating layer; the nonaqueous electrolytic solution comprises an organic solvent, a lithium salt and a compound represented by formula (1), wherein in the formula (1), R1Is one or more of chain, ring and aromatic groups with 2-20 carbon atoms, and the charge cut-off voltage of the lithium ion battery is more than 4.35V. The lithium ion battery has the advantages of good cycle and storage performance at high temperature, and can remarkably improve the phenomenon of lithium separation after long-term cycle and inhibit the increase of internal resistance.
Description
Technical Field
The invention relates to the technical field of new energy, in particular to a lithium ion battery.
Background
The lithium ion battery has the advantages of high working voltage, wide working temperature range, large energy density and power density, no memory effect, long cycle life and the like, and is widely applied to the field of 3C digital products such as mobile phones, notebook computers and the like and new energy automobiles. In recent years, with the continuous development of thinning and thinning of 3C digital products, the demand for energy density of lithium ion batteries is also increasing. Therefore, it is highly desirable to increase the energy density of lithium ion batteries.
At present, two methods for improving the energy density of the battery are mainly used, namely, the charge cut-off voltage of a positive electrode is improved, and the active material layer of the electrode is pressurized to realize high density. However, when the charge cut-off voltage of the positive electrode is increased, the activity of the positive electrode is further increased, and a side reaction between the positive electrode and the electrolyte is also increased, whereby the transition metal ions in the positive electrode are eluted, and the high-temperature performance of the battery is deteriorated. In addition, when a high-compaction electrode is adopted, the porosity of the high-compaction electrode is low, the liquid retention amount of the battery is also reduced, the electrolyte is difficult to permeate at the interface of the low-porosity pole piece, the contact internal resistance between the electrolyte and the electrode is increased, and the charge-discharge polarization is increased in the long-term circulation process, so that the situation of sudden water jump caused by lithium precipitation can be caused. Therefore, how to improve the long-term cycle performance of high-voltage and high-compaction lithium ion batteries is an industrial problem, and improvement needs to be carried out from various aspects of electrode materials, electrolyte and the like.
In the aspect of anode materials, surface coating modification is an important means for improving the performance of the anode materials of the lithium ion batteries. The surface coating material can effectively reduce the corrosion of the electrolyte to the anode and reduce the dissolution of metal ions. Meanwhile, the surface coating material can also isolate the contact between the electrolyte and the surface active material of the positive electrode from the physical space. However, in the case of using a coating material such as alumina or the like on the surface of the positive electrode, there is a problem in that the coated metal oxide having no electrochemical activity suppresses the transport of lithium ions at the interface of the positive electrode, resulting in an increase in impedance, which is disadvantageous for long-term cycling of the lithium ion battery.
At present, no good solution exists in the aspect of electrolyte. Therefore, the long-term cycle performance of the battery is ensured from the perspective of the electrolyte, the high-temperature performance of the battery is also considered, and no lithium precipitation in the later cycle period is ensured, which is a great problem of high-voltage high-compaction lithium ion batteries.
Disclosure of Invention
The invention aims to solve the problems of poor long-term cycle performance, increased internal resistance, serious lithium separation and the like of a high-compaction lithium ion battery in the prior art, and provides a lithium ion battery which has the advantages of good cycle and storage performance at high temperature, can obviously improve the lithium separation phenomenon after long-term cycle and inhibit the increase of internal resistance.
In order to achieve the above object, the present invention provides a lithium ion battery comprising a positive electrode, a negative electrode, a separator interposed between the positive electrode and the negative electrode, and a nonaqueous electrolytic solution,
the positive electrode contains a positive electrode material, and a positive electrode active material of the positive electrode material contains Li1-xCoO2(0≤x<1) And Li1-xCoO2The surface is provided with a metal oxide coating layer;
the nonaqueous electrolytic solution includes an organic solvent, a lithium salt, and a compound represented by formula (1),
in the formula (1), R1Is one or more of chain, ring and aromatic groups with 2-20 carbon atoms, and the charge cut-off voltage of the lithium ion battery is more than 4.35V.
Preferably, in formula (1), R is1Is one or more of chain, ring and aromatic groups with 3-18 carbon atoms; more preferably, said R1One or more selected from the following structures, wherein denotes the position of binding:
preferably, the compound represented by the formula (1) is selected from one or more of the following compounds:
preferably, the content of the compound represented by the formula (1) in the nonaqueous electrolytic solution is 0.001 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution; more preferably, the content of the compound represented by formula (1) in the nonaqueous electrolytic solution is 0.1 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution.
Preferably, the charge cut-off voltage of the lithium ion battery is 4.45-4.60V.
Preferably, Li in the positive electrode active material1-xCoO2Has a specific surface area of 0.02-0.85m2(iv)/g, D50 is 4-20 μm; more preferably, Li in the positive electrode active material1-xCoO2Has a specific surface area of 0.06-0.65m2The D50 is 9-15 μm.
Preferably, Li in the positive electrode active material is based on the total weight of the positive electrode active material1-xCoO2The content of (B) is 50% by weight or more; more preferably, Li in the positive electrode active material is based on the total weight of the positive electrode active material1-xCoO2The content of (B) is 80-100 wt%.
Preferably, the metal oxide of the metal oxide coating layer is one or more of aluminum oxide, magnesium oxide, titanium oxide, tungsten oxide, tin oxide, zinc oxide, indium oxide, zirconium oxide, lanthanum oxide, molybdenum oxide, and chromium oxide; more preferably, the metal oxide of the metal oxide coating layer is one or more of magnesium oxide, tungsten oxide and aluminum oxide.
Preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1-xCoO20.01-3 wt% of the weight; more preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1-xCoO20.5-3% by weight.
Preferably, the organic solvent is one or more of cyclic carbonates, linear carbonates, carboxylic esters and ethers.
Preferably, the cyclic carbonate includes one or more of vinylene carbonate, propylene carbonate and ethylene carbonate.
Preferably, the linear carbonate comprises one or more of dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate.
Preferably, the carboxylic acid ester comprises one or more of methyl acetate, ethyl acetate, methyl propionate, ethyl propionate, methyl butyrate, methyl isobutyrate, methyl pivalate, and ethyl pivalate.
Preferably, the ethers include one or more of ethylene glycol dimethyl ether, 1, 3-dioxolane, and 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether.
Preferably, the lithium salt is LiPF6、LiPO2F2、LiBF4、LiBOB、LiClO4、LiCF3SO3、LiDFOB、LiN(SO2CF3)2And LiN (SO)2F)2One or more of; more preferably, the lithium salt is LiPF6。
Preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.5 to 3.5 mol/L; more preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.8 to 2 mol/L.
Preferably, the nonaqueous electrolytic solution further contains an additive, and the additive is one or more of a cyclic carbonate compound having a fluorine atom, a cyclic carbonate compound having a carbon-carbon unsaturated bond, a cyclic sulfonate compound, and a nitrile compound.
Preferably, the cyclic carbonate compound having a fluorine atom is fluoroethylene carbonate and/or difluoroethylene carbonate.
Preferably, the cyclic carbonate compound having a carbon-carbon unsaturated bond is one or more of vinylene carbonate, vinyl ethylene carbonate and methyl vinylene carbonate.
Preferably, the cyclic sulfonate compound is 1, 3-propane sultone and/or propylene sulfite.
Preferably, the nitrile compound is one or more of succinonitrile, adiponitrile, ethylene glycol bis (propionitrile) ether, hexanetrinitrile, adiponitrile, pimelonitrile, suberonitrile, nonadinitrile and decanedinitrile.
Preferably, the compacted density of the cathode material is 3.5g/cm3The above; more preferably, the positive electrode material has a compacted density of 3.6 to 4.13g/cm3。
Preferably, the compacted density of the anode material is 1.5g/cm3The above; more preferably, the compacted density of the anode material is 1.55 to 1.8g/cm3。
Preferably, the positive electrode material and the negative electrode material have a porosity of 50% or less; more preferably, the positive electrode material and the negative electrode material have a porosity of 10% to 35%.
By the technical scheme, the positive active material contains Li1-xCoO2(0≤x<1) And Li1-xCoO2In the lithium ion battery with the metal oxide coating layer on the surface, in the charge cut-off voltage range limited by the invention, the compound represented by the formula (1) is added into the electrolyte, so that the capacity retention rate and the capacity recovery rate of the high-compaction lithium ion battery after long-term circulation can be obviously improved, the thickness expansion rate of the battery can be obviously inhibited, in addition, the occurrence of a lithium precipitation phenomenon can be effectively inhibited, the increase of internal resistance is inhibited, and the risk of capacity water-jumping occurring in the later cycle period of the high-compaction battery is greatly reduced.
Detailed Description
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For ranges of values, between the endpoints of each of the ranges and the individual points, and between the individual points may be combined with each other to give one or more new ranges of values, and these ranges of values should be considered as specifically disclosed herein.
The invention provides a lithium ion battery, which comprises a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode and a non-aqueous electrolyte,
the positive electrode contains a positive electrode material, and a positive electrode active material of the positive electrode material contains Li1-xCoO2(0≤x<1) And Li1-xCoO2The surface of the non-aqueous electrolyte is provided with a metal oxide coating layer, the non-aqueous electrolyte comprises an organic solvent, a lithium salt and a compound represented by a formula (1),
in the formula (1), R1Is one or more of chain, ring and aromatic groups with 2-20 carbon atoms, and the charge cut-off voltage of the lithium ion battery is more than 4.35V.
Through a great deal of research and experiments, the inventor of the invention finally and unexpectedly discovers that when the charging of the lithium ion battery is cut offThe lithium ion battery has a cut-off voltage of 4.35V or more, and the positive electrode active material contains Li having a metal oxide coating layer on the surface thereof1-xCoO2(0≤x<1) In the process, the compound represented by the formula (1) is added into the non-aqueous electrolyte of the lithium ion battery, so that the side reaction of the electrolyte solution can be effectively inhibited, good cycle performance and high-temperature storage performance can be realized even if the compaction density of the anode and the cathode of the lithium ion battery is improved, the lithium precipitation risk of the high-pressure solid battery in the later cycle stage can be effectively reduced, and the problem of water jump possibly occurring in the later cycle stage of the battery is solved.
The mechanism of action of the compound represented by the formula (1) is not clear at present, and the inventors of the present invention speculate that the specific group contained in the compound represented by the formula (1) may react with Li after the compound represented by the formula (1) is added to the nonaqueous electrolyte solution for a lithium ion battery of the present invention1-xCoO2Co element in the anode material is complexed to stabilize the position of Co in crystal lattices, thereby effectively inhibiting the dissolution of Co and improving the high-temperature performance of the battery. At present, although the performance of the anode material can be improved by coating the metal oxide, the metal oxide can cause the problem of high anode impedance while improving the stability of the anode, and a specific group of the compound represented by the formula (1) can react with the metal oxide coating to change the space structure of the metal oxide and introduce lattice defects, so that the ion conductivity can be improved and the anode impedance can be reduced by increasing the concentration of the lattice defects. Meanwhile, specific groups contained in the compound represented by the formula (1) can react with the negative electrode, the interface of the negative electrode and electrolyte is regulated and controlled, and the impedance growth speed of the negative electrode in the circulating process is reduced. Therefore, the battery containing the compound represented by the formula (1) greatly reduces the risk of lithium deposition due to an increase in charge polarization caused by an excessive internal resistance in the latter stage of the cycle by suppressing the impedance of the positive and negative electrodes.
According to the present invention, preferably, in formula (1), R is1Is one or more of chain, ring and aromatic groups with 3-18 carbon atoms; more preferably, said R1One or more selected from the following structures, wherein denotes the position of binding (i.e., the atom attached to the N atom in formula (1)):
in the present invention, preferably, the compound represented by the formula (1) is selected from one or more of the following compounds:
in the present invention, the content of the compound represented by formula (1) in the nonaqueous electrolytic solution may vary widely, and for example, may be 0.001 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution; preferably, the content of the compound represented by formula (1) in the nonaqueous electrolytic solution is 0.1 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution.
In the nonaqueous electrolytic solution for a lithium ion battery of the present invention, the improvement of the battery performance can be remarkably achieved as long as the compound represented by formula (1) is contained in a very small amount, and for further improvement of the effect, the content of the compound represented by formula (1) may be appropriately increased, but it is not preferable to exceed 3.5% by weight because, when the content of the compound represented by formula (1) in the nonaqueous electrolytic solution is higher than 3.5% by weight, the improvement effect on the lithium ion battery performance is not further improved, and moreover, the electrolyte turbidity is easily caused by the compound represented by formula (1) in a high content, and the lithium ion battery performance may be rather lowered.
According to the present invention, the positive electrode active material contains Li1-xCoO2(0≤x<1) And Li1-xCoO2The surface is provided with a metal oxide coating layer. Preferably, with a positive electrodeLi in the positive electrode active material based on the total weight of the active material1-xCoO2The content of (B) is 50% by weight or more; more preferably, LiCoO in the positive electrode active material is based on the total weight of the positive electrode active material2The content of (B) is 80-100 wt%. For example, LiCoO in the positive electrode active material based on the total weight of the positive electrode active material2The content of (b) may be 80% by weight, may be 85% by weight, may be 90% by weight, may be 95% by weight, or may be 100% by weight. Particularly preferably, LiCoO in the positive electrode active material is based on the total weight of the positive electrode active material2Is 100 wt%. When Li is contained in the positive electrode active material1-xCoO2When the content of (b) is within the above range, the volumetric energy density of the battery can be effectively improved.
The value of x may be, for example, 0, 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, or the like.
In the present invention, LiCoO in the positive electrode active material2Has a specific surface area of 0.02-0.85m2(ii)/g, D50 (median particle size) is 4-20 μm; preferably, LiCoO in the positive electrode active material2Has a specific surface area of 0.06-0.65m2(iv)/g, D50 is 9-15 μm; further preferably, Li in the positive electrode active material1-xCoO2Has a specific surface area of 0.1 to 0.2m2D50 is 12-15 μm. When LiCoO is used2When the specific surface area and the D50 are within the range, a proper positive electrode can be prepared by coating, compacting and other processes; if LiCoO2If the specific surface area of (2) and the D50 are outside this range, high-pressure electrode production is difficult, and the yield is lowered.
According to the present invention, the metal oxide of the metal oxide coating layer may be LiCoO coated commonly used in the art2The various metal oxides of (a) are not particularly limited, and for example, may be one or more of alumina, magnesia, titania, tungsten oxide, tin oxide, zinc oxide, indium oxide, zirconia, lanthanum oxide, molybdenum oxide, and chromium oxide; preferably, the metal oxide of the metal oxide coating layer is one or more of magnesium oxide, tungsten oxide and aluminum oxideA variety of.
In the present invention, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1-xCoO2The weight ratio may also vary within a wide range, for example, the weight of the metal oxide coating layer may account for Li in the positive electrode active material1- xCoO20.01-3 wt% of the weight; preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1- xCoO20.5-3 wt% of the weight; more preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1- xCoO21.5-2.5 wt% of the weight. When the weight of the metal oxide coating layer is less than Li in the positive electrode active material1-xCoO2When the weight is 0.01 wt%, the positive active material still has large-area contact with the electrolyte, and cannot play a sufficient protection role; when the weight of the metal oxide coating layer is higher than that of Li in the positive electrode active material1-xCoO2At 3 wt%, the metal oxide coating layer is too thick, resulting in the failure to smoothly conduct lithium ions, and further resulting in the rapid decrease in the rate capability of the battery.
In the present invention, the charge cut-off voltage of the lithium ion battery is 4.35V or more, and preferably, the charge cut-off voltage of the lithium ion battery is 4.45 to 4.60V. As long as it is within this range, for example, the charge cut-off voltage of the lithium ion battery may be 4.4V, 4.5V, 4.55V, 4.6V, and the like, without particular limitation. As long as the lithium ion battery positive electrode active material and the compound represented by formula (1) added to the nonaqueous electrolyte solution provided by the invention are combined within the above range, the high-temperature cycle and storage performance of the lithium ion battery can be remarkably improved under high compaction density, the increase of internal resistance can be reduced, and the occurrence of lithium precipitation can be inhibited.
According to the present invention, the organic solvent is not particularly limited, and may be various organic solvents commonly used in the art for preparing a nonaqueous electrolyte for a lithium ion battery, and for example, one or more of cyclic carbonates, linear carbonates, carboxylates, and ethers may be selected.
The cyclic carbonate as a nonaqueous electrolyte for a lithium ion battery may include: one or more of vinylene carbonate, propylene carbonate and ethylene carbonate.
The linear carbonate as a non-aqueous electrolyte of a lithium ion battery may include one or more of dimethyl carbonate, diethyl carbonate, and ethyl methyl carbonate.
The carboxylic acid ester as a non-aqueous electrolyte of the lithium ion battery may include one or more of methyl acetate, ethyl acetate, methyl propionate, ethyl propionate, methyl butyrate, methyl isobutyrate, methyl pivalate, and ethyl pivalate.
The ethers as the non-aqueous electrolyte of the lithium ion battery may include one or more of ethylene glycol dimethyl ether, 1, 3-dioxolane, and 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether.
In a particularly preferred embodiment of the present invention, the organic solvent is selected from a mixture of ethylene carbonate, diethyl carbonate and ethyl methyl carbonate, and the ratio of the three is 1:1: by using the three compounds in the proportion range as organic solvents, the conductivity, viscosity and safety of the electrolyte can be balanced, and the electrolyte can achieve better comprehensive performance.
According to the present invention, various lithium salts commonly used in the art for preparing lithium ion batteries can be used as the lithium salt in the nonaqueous electrolyte of the lithium ion battery, and are not particularly limited, and for example, LiPF can be selected6、LiPO2F2、LiBF4、LiBOB、LiClO4、LiCF3SO3、LiDFOB、LiN(SO2CF3)2And LiN (SO)2F)2Preferably, the lithium salt is LiPF6。
In the present invention, the content of the lithium salt may be a content generally used in lithium ion batteries in the art, and is not particularly limited. For example, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.5 to 3.5 mol/L; preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.8 to 2 mol/L; more preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.8 to 1.2 mol/L. When the content of the lithium salt is within this range, not only can good battery performance be achieved, but also the cost of the electrolyte can be effectively controlled.
According to the present invention, the lithium ion battery may further contain various additives commonly used in the art for improving the performance of lithium ion batteries, such as: the additive may be one or more of a cyclic carbonate compound having a fluorine atom, a cyclic carbonate compound having a carbon-carbon unsaturated bond, a cyclic sulfonate compound, and a nitrile compound.
Preferably, the cyclic carbonate compound having a fluorine atom is fluoroethylene carbonate and/or difluoroethylene carbonate; the cyclic carbonate compound with carbon-carbon unsaturated bonds is one or more of vinylene carbonate, vinyl ethylene carbonate, ethylene carbonate and methyl vinylene carbonate; the cyclic sulfonate compound is 1, 3-propane sultone and/or propylene sulfite; the nitrile compound is one or more of succinonitrile, adiponitrile, ethylene glycol bis (propionitrile) ether, hexanetricarbonitrile, adiponitrile, pimelonitrile, suberonitrile, nonadinitrile and sebaconitrile.
In a preferred embodiment of the present invention, an additive, fluoroethylene carbonate (FEC) and/or Succinonitrile (SN), is further added to the lithium ion nonaqueous electrolyte. Based on the above-described studies, the inventors of the present invention have found that when the compound represented by formula (1) is contained in the nonaqueous electrolyte solution for a lithium ion battery of the present invention and the additive is added, the cycle performance of the battery can be further improved.
According to the present invention, in the lithium ion battery nonaqueous electrolyte, the content of the additive may be a content conventionally used in lithium ion batteries for various additives in the art. For example, the content of the additive can be 0.1-5 wt% of the total mass of the lithium ion battery nonaqueous electrolyte; preferably, the content of the additive can be 2-5 wt% of the total mass of the lithium ion battery nonaqueous electrolyte.
According to the present invention, the active material of the anode may be selected from various materials commonly used in the art for anode active materials of lithium ion batteries, without particular limitation, and the anode active material may be selected from one or more of metallic lithium, carbon-based anode materials, and non-carbon-based anode materials. Preferably, the carbon-based negative electrode material is one or more of a graphite-based carbon material, hard carbon and soft carbon; the non-carbon negative electrode material is one or more of silicon base, tin base, antimony base, aluminum base and transition metal compound. More preferably, the negative active material is one or more of artificial graphite, natural graphite, and silicon.
In the present invention, the preparation of the positive electrode and the negative electrode of the lithium ion battery may be performed according to a method commonly used in the art for preparing the positive electrode and the negative electrode of the lithium ion battery, and is not particularly limited. For example, the active materials of the positive and negative electrodes may be mixed with a conductive agent and a binder, and the mixture may be dispersed in an organic solvent to prepare a slurry, and then the obtained slurry may be coated on a current collector and subjected to drying, calendaring, and the like. The conductive agent, binder, organic solvent and current collector can be materials and substances commonly used in the art, and are not described in detail herein.
According to the invention, in order to improve the energy density of the battery, the compacted density of the anode and cathode materials of the battery is improved, and specifically, the compacted density of the anode material is 3.5g/cm3The compacted density of the anode material is 1.5g/cm3As described above, the positive electrode material and the negative electrode material have a porosity of 50% or less; preferably, the compacted density of the cathode material is 3.6-4.13g/cm3The compacted density of the negative electrode material is 1.55-1.8g/cm3The porosity of the anode material and the cathode material is 10% -35%. Since the inventors of the present invention have overcome the above-described problems of poor performance inherent in the high-compaction lithium ion battery in the prior art in the charge cut-off voltage range defined in the present invention by adding the compound represented by the formula (1) or the like, the positive and negative pressures of the lithium ion battery in the present invention are compacted to the above-described range.
According to the present invention, the separator disposed between the positive electrode and the negative electrode may be any of various materials commonly used as separators in the art, and is not particularly limited, and may be, for example, one or more of a polyolefin-based separator, a polyamide-based separator, a polysulfone-based separator, a polyphosphazene-based separator, a polyethersulfone-based separator, a polyetherketoneketone-based separator, a polyetheramide-based separator, and a polyacrylonitrile-based separator; preferably, the separator is selected from one or more of a polyolefin separator, a polyamide separator, and a polyacrylonitrile separator.
In the invention, the lithium ion battery can be prepared by a sandwich method commonly used in the field, for example, a diaphragm is arranged between a positive plate and a negative plate coated with an active material, then the whole is coiled, a coiled body is flattened and then placed into a packaging bag for vacuum baking and drying to obtain a battery cell, then electrolyte is injected into the battery cell, and the battery cell is formed after vacuum packaging and standing. This method is well known in the art and will not be described further herein.
The present invention will be described in detail below by way of examples. In the following examples, all materials used are commercially available unless otherwise specified.
In the following examples and comparative examples, compounds 1-6 were obtained from Shanghai Allantin Biotech Co., Ltd.
Positive electrode active material LiCoO2Has a specific surface area of 0.16m2D50 is 14.69 μm. When the coating layer of metal oxide is provided, the metal oxide in the coating layer of metal oxide is MgO and Al2O3(the mass ratio of the two is 1:2, the model is LC95X, purchased from Hu nan fir Technique Co., Ltd.), and the weight of the metal oxide coating layer accounts for the weight of the positive electrode active material LiCoO22% by weight of the total weight.
The following test examples and comparative examples were conducted in accordance with the methods for testing the respective properties.
Test example 1: high temperature cycle performance test
The lithium ion batteries prepared in the following examples and comparative examples were placed in an oven at a constant temperature of 45 ℃, and were charged to 4.45V (or 4.5V, 4.55V) at a constant current of 1C, further charged at a constant voltage until the current decreased to 0.03C, and then discharged to 3.0V at a constant current of 1C, and the discharge capacity and the termination internal resistance were recorded for the 1 st and 400 th cycles, and the capacity retention rate and the internal resistance increase rate for the high-temperature cycle were calculated according to the following formulas:
capacity retention (%) — 400 th cycle discharge capacity/1 st cycle discharge capacity × 100%.
The internal resistance increase rate (%) (internal resistance of the battery after the 400 th cycle-internal resistance of the battery after the 1 st cycle)/internal resistance of the battery after the 1 st cycle × 100%.
Test example 2: 60 ℃ high temperature storage Performance test
The lithium ion batteries prepared in the following examples and comparative examples were charged to 4.45V (or 4.5V, 4.55V) at a constant current and a constant voltage of 1C at room temperature, with a cutoff current of 0.03C, the initial discharge capacity, the initial battery thickness and the initial internal resistance of the batteries were measured, and then stored in an environment of 60 ℃ for 30 days, respectively, discharged to 3V at 1C, the retention capacity and recovery capacity of the batteries at that time and the battery thickness and internal resistance after storage were measured, and the battery capacity retention rate, capacity recovery rate, thickness expansion rate and internal resistance increase rate were calculated as follows:
battery capacity retention (%) — retention capacity/initial discharge capacity × 100%;
battery capacity recovery (%) — recovery capacity/initial discharge capacity × 100%;
thickness expansion (%) (battery thickness after storage-initial battery thickness)/initial battery thickness × 100%;
the internal resistance increase rate (%) (internal resistance of battery after storage-initial internal resistance of battery)/initial internal resistance of battery × 100%.
Test example 3: negative pole lithium precipitation condition and metal ion dissolution test after 45 ℃ circulation for 400 times
The formed battery is circulated for 400 times under the conditions of 45 ℃, 3.0V-4.45V (or 4.5V and 4.55V) and 1C/1C, the battery is charged to 4.45V (or 4.5V and 4.55V) at constant current, then the battery is disassembled in a glove box, a negative plate is taken to observe the condition of lithium precipitation of the negative electrode, and then the negative plate is placed in HNO3(concentration: 14.5mol/L) and H2Soaking the O mixed solution (mixed according to the mass ratio of 1: 1) for 12 hours, and taking the soaked liquid for ICP test.
Example 1
1) Preparation of the electrolyte
Ethylene Carbonate (EC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) were mixed in a mass ratio of EC: DEC: EMC ═ 1:1:1, and then lithium hexafluorophosphate (LiPF) was added to the resultant mixture6) To a molar concentration of 1mol/L, compound 1 (note: compound 1 here is compound 1 in the specification, the same applies below);
2) preparation of positive plate
LiCoO as positive electrode active material2(surface with a coating layer of Metal oxide, LiCoO in Positive electrode active Material2The content of the conductive carbon black is 100 percent), the conductive carbon black Super-P and the adhesive polyvinylidene fluoride (PVDF) are uniformly mixed according to the weight ratio of 93:4:3, and then the mixture is dispersed in N-methyl-2-pyrrolidone (NMP) to obtain anode slurry; uniformly coating the positive electrode slurry on two surfaces of an aluminum foil, drying, rolling (the compacted density is shown in table 1) and vacuum drying, and welding an aluminum outgoing line by using an ultrasonic welding machine to obtain a positive electrode plate, wherein the thickness of the positive electrode plate is 100 +/-2 mu m;
3) preparation of negative plate
Uniformly mixing artificial graphite serving as a negative electrode active material, conductive carbon black Super-P serving as a conductive agent, Styrene Butadiene Rubber (SBR) serving as a binder and carboxymethyl cellulose (CMC) according to a weight ratio of 94:1:2.5:2.5, and dispersing the mixture in deionized water to obtain negative electrode slurry; coating the negative electrode slurry on two sides of a copper foil, drying, rolling (the compacted density is shown in table 1) and vacuum drying, and welding a nickel outgoing line by using an ultrasonic welding machine to obtain a negative plate, wherein the thickness of the negative plate is 120 +/-2 microns;
4) preparation of cell
Placing three layers of isolating films with the thickness of 20 mu m between the positive plate and the negative plate, then winding a sandwich structure consisting of the positive plate, the negative plate and the diaphragm, flattening the wound body, then placing the flattened wound body into an aluminum foil packaging bag, and baking the flattened wound body in vacuum at 75 ℃ for 48 hours to obtain a battery cell to be injected with liquid;
5) liquid injection and formation of battery core
In a glove box with the water oxygen content of less than 10ppm, injecting the electrolyte prepared in the step 1) into the battery cell prepared in the step 4), and standing for 24 hours after vacuum packaging;
then the first charge is normalized according to the following steps: charging at 0.1C for 45min, charging at 0.2C for 30min, charging at 0.5C for 75min, vacuum sealing for the second time, constant-current charging to 4.45V (or 4.5V, 4.55V) at 0.2C, stopping current at 0.3C, standing at room temperature for 24hr, and constant-current discharging at 0.2C to 3.0V.
Examples 2 to 22 and comparative examples 1 to 5
The procedure of example 1 was followed except that the positive electrode active material (whether or not there was a metal oxide coating layer), the compacted density of the positive and negative electrode materials, the kind and content of the compound represented by formula (1) added to the electrolyte, the kind and content of other additives, and the charge cut-off voltage of the lithium ion battery were varied, and the specific contents are shown in table 1.
TABLE 1
The relevant properties of the lithium ion batteries prepared in examples 1 to 22 and comparative examples 1 to 5 are shown in table 2.
TABLE 2
From the results of examples 1 to 3 and comparative examples 1 to 3, it can be seen that the high-temperature storage performance and the high-temperature cycle performance of the battery can be significantly improved by adding the compound represented by formula 1 as the compacted density of the positive and negative electrodes increases within the charge cut-off voltage range defined in the present invention. After the circulation is carried out for 400 circles at the temperature of 45 ℃, the dissolving-out amount of the metal cobalt is obviously reduced, and the lithium precipitation phenomenon and the internal resistance increase can be obviously inhibited.
It can be seen from the combination of examples 3 to 5 and comparative example 3 that, even at a relatively high positive and negative electrode compacted density, the addition of the compound represented by formula (1) provided by the present invention to the electrolyte can effectively improve the high-temperature storage performance and high-temperature cycle performance of the battery, suppress the dissolution of metallic cobalt and the occurrence of lithium precipitation, and reduce the increase rate of internal resistance, within the charge cut-off voltage range defined by the present invention.
Combining the results of examples 6-10 and comparative example 3, it can be seen that the compounds represented by formula 1 provided by the present invention all have the same function as compound 1, and when added to the nonaqueous electrolyte of a lithium ion battery, the high temperature cycle and storage performance of the lithium ion battery can be improved to different degrees.
As can be seen from examples 3, 11 to 19 and comparative example 3, in the range of 0.001 to 3% by weight, the increase in resistance during high-temperature cycling at 45 ℃ of the battery can be further improved with the increase in the amount of compound 1 added, while further suppressing elution of metal ions; when the amount of addition is increased from 3% by weight to 3.5% by weight, the effect of improving the battery performance is reduced.
As can be seen from examples 3 and 20 to 22 and comparative examples 1 and 4, the addition of other additives to the compound represented by formula (1) provided by the present invention helps to further improve the high-temperature storage and cycle performance of the lithium ion battery, but if the compound represented by formula (1) provided by the present invention is not added, the addition of other additives alone has a very limited effect of improving various performances of the lithium ion battery.
From the results of example 3 and comparative example 5, it can be seen that the addition of the compound represented by formula (1) to the nonaqueous electrolytic solution and the coating of the metal oxide on the surface of the positive electrode material at the charge cut-off voltage defined in the present invention can effectively improve the high-temperature cycle and storage performance of the lithium ion battery and reduce the increase rate of the internal resistance of the battery.
The preferred embodiments of the present invention have been described above in detail, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, many simple modifications can be made to the technical solution of the invention, including combinations of various technical features in any other suitable way, and these simple modifications and combinations should also be regarded as the disclosure of the invention, and all fall within the scope of the invention.
Claims (10)
1. A lithium ion battery is characterized by comprising a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode and a non-aqueous electrolyte,
the positive electrode contains a positive electrode material, and a positive electrode active material of the positive electrode material contains Li1-xCoO2And Li1-xCoO2Having a coating layer of a metal oxide on the surface, Li1-xCoO2X is more than or equal to 0<1；
The nonaqueous electrolytic solution includes an organic solvent, a lithium salt, and a compound represented by formula (1),
in the formula (1), R1Is one or more of chain, ring and aromatic groups with 2-20 carbon atoms,
the charge cut-off voltage of the lithium ion battery is more than 4.35V.
2. The lithium ion battery according to claim 1, wherein in formula (1), the R is1Is one or more of chain, ring and aromatic groups with 3-18 carbon atoms;
preferably, said R is1One or more selected from the following structures, wherein denotes the position of binding:
3. the lithium ion battery according to any one of claims 1 or 2, wherein the compound represented by formula (1) is selected from one or more of the following compounds:
4. the lithium ion battery according to any one of claims 1 to 3, wherein the content of the compound represented by formula (1) in the nonaqueous electrolytic solution is 0.001 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution;
preferably, the content of the compound represented by formula (1) in the nonaqueous electrolytic solution is 0.1 to 3.5% by weight based on the total weight of the nonaqueous electrolytic solution;
preferably, the charge cut-off voltage of the lithium ion battery is 4.45-4.60V.
5. The lithium ion battery of any of claims 1-3, wherein Li in the positive electrode active material1- xCoO2Has a specific surface area of 0.02-0.85m2(iv)/g, D50 is 4-20 μm;
preferably, Li in the positive electrode active material1-xCoO2Has a specific surface area of 0.06-0.65m2(iv)/g, D50 is 9-15 μm;
preferably, Li in the positive electrode active material is based on the total weight of the positive electrode active material1-xCoO2The content of (B) is 50% by weight or more;
more preferably, Li in the positive electrode active material is based on the total weight of the positive electrode active material1-xCoO2The content of (B) is 80-100 wt%.
6. The lithium ion battery of any of claims 1-3, wherein the metal oxide of the metal oxide cladding layer is one or more of aluminum oxide, magnesium oxide, titanium oxide, tungsten oxide, tin oxide, zinc oxide, indium oxide, zirconium oxide, lanthanum oxide, molybdenum oxide, and chromium oxide;
preferably, the metal oxide of the metal oxide coating layer is one or more of magnesium oxide, tungsten oxide and aluminum oxide;
preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1-xCoO20.01-3 wt% of the weight;
preferably, the weight of the metal oxide coating layer accounts for Li in the positive electrode active material1-xCoO20.5-3% by weight.
7. The lithium ion battery according to any one of claims 1 to 3, wherein the organic solvent is one or more of cyclic carbonates, linear carbonates, carboxylates, and ethers;
preferably, the cyclic carbonate includes one or more of vinylene carbonate, propylene carbonate and ethylene carbonate;
preferably, the linear carbonate comprises one or more of dimethyl carbonate, diethyl carbonate and ethyl methyl carbonate;
preferably, the carboxylic acid ester comprises one or more of methyl acetate, ethyl acetate, methyl propionate, ethyl propionate, methyl butyrate, methyl isobutyrate, methyl pivalate, and ethyl pivalate;
preferably, the ethers include one or more of ethylene glycol dimethyl ether, 1, 3-dioxolane, and 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether.
8. The lithium ion battery of any of claims 1-3, wherein the lithium salt is LiPF6、LiPO2F2、LiBF4、LiBOB、LiClO4、LiCF3SO3、LiDFOB、LiN(SO2CF3)2And LiN (SO)2F)2One or more of (a) or (b),
preferably, the lithium salt is LiPF6；
Preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.5 to 3.5 mol/L;
more preferably, the concentration of the lithium salt in the nonaqueous electrolytic solution is 0.8 to 2 mol/L.
9. The lithium ion battery according to any one of claims 1 to 3, wherein the nonaqueous electrolytic solution further contains an additive, and the additive is one or more of a cyclic carbonate compound having a fluorine atom, a cyclic carbonate compound having a carbon-carbon unsaturated bond, a cyclic sulfonate compound, and a nitrile compound;
preferably, the cyclic carbonate compound having a fluorine atom is fluoroethylene carbonate and/or difluoroethylene carbonate;
preferably, the cyclic carbonate compound having a carbon-carbon unsaturated bond is one or more of vinylene carbonate, vinyl ethylene carbonate and methyl vinylene carbonate;
preferably, the cyclic sulfonate compound is 1, 3-propane sultone and/or propylene sulfite;
preferably, the nitrile compound is one or more of succinonitrile, adiponitrile, ethylene glycol bis (propionitrile) ether, hexanetrinitrile, adiponitrile, pimelonitrile, suberonitrile, nonadinitrile and decanedinitrile.
10. The lithium ion battery of any of claims 1-3, wherein the positive electrode material has a compacted density of 3.5g/cm3In the above-mentioned manner,
preferably, the positive electrode material has a compacted density of 3.6 to 4.13g/cm3；
Preferably, the compacted density of the anode material is 1.5g/cm3The above;
more preferably, the anode material has a compacted density of 1.55 to 1.8g/cm3；
Preferably, the positive electrode material and the negative electrode material have a porosity of 50% or less;
more preferably, the porosity of the positive electrode material and the negative electrode material is 10% to 35%.
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