CN115360424A - Electrolyte and lithium ion battery containing same - Google Patents
Electrolyte and lithium ion battery containing same Download PDFInfo
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- CN115360424A CN115360424A CN202211218811.XA CN202211218811A CN115360424A CN 115360424 A CN115360424 A CN 115360424A CN 202211218811 A CN202211218811 A CN 202211218811A CN 115360424 A CN115360424 A CN 115360424A
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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
- H01M10/056—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
- H01M10/0567—Liquid materials characterised by the additives
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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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 discloses an electrolyte and a lithium ion battery containing the same, wherein the electrolyte comprises lithium salt, an organic solvent and an additive, and the additive is selected from at least one of compounds shown in a structural formula I:
wherein R is 1 ～R 4 Each independently selected from one of hydrogen atom, substituted or unsubstituted C1-C6 alkyl, substituted or unsubstituted C1-C6 unsaturated alkyl, substituted or unsubstituted C2-C20 alkenyl, cyano, and a group formed by substituting aryl with 6-18 carbon atoms by carbonyl, cyano, halogen atom, nitro, carboxyl and sulfonic group, wherein the halogen atom is F, cl or Br; x is one selected from C, O, NH. The electrolyte of the invention can makeThe obtained lithium ion battery has better high-temperature storage and cycle performance under high voltage and better low-temperature performance.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to an electrolyte and a lithium ion battery containing the electrolyte.
Background
The lithium ion battery has the advantages of high specific energy, no memory effect, long cycle life and the like, and is widely applied to the fields of 3C digital products, electric tools, aerospace, energy storage, power automobiles and the like. The nickel-cobalt-manganese ternary positive electrode material (NCM material) is a preferred material for the positive electrode active material of the lithium ion battery due to good safety and low price, but the electrical performance requirement of the lithium ion battery is higher and higher with the development and popularization of the lithium ion battery with a higher voltage system.
At present, the irreversible phase change of H2-H3 is easy to occur in the ternary cathode material under high voltage and high temperature, so that oxygen is separated out, the interface of electrolyte and an electrode is unstable, and the battery has the problems of poor high-temperature storage and serious cycle gas generation. Meanwhile, the conventional electrolyte containing carboxylic ester has high conductivity, but is oxidized and decomposed on the surface of the battery anode at a high voltage of 4.4V, and particularly under a high temperature condition, the oxidative decomposition of the electrolyte is accelerated, and the deterioration reaction of the anode material is promoted.
Therefore, it is necessary to develop an electrolyte capable of withstanding a high voltage of 4.4V, and further achieve excellent performance of the lithium ion Chi Dianxing, so as to solve the problems of the prior art.
Disclosure of Invention
The invention aims to provide an electrolyte, which can enable a lithium ion battery to have better high-temperature storage and cycle performance under high voltage (such as 4.4V) and better low-temperature performance.
Another object of the present invention is to provide a lithium ion battery containing the electrolyte, which has better high temperature storage and cycle performance at high voltage (such as 4.4V), and better low temperature performance.
To achieve the above object, the present invention provides an electrolyte comprising a lithium salt, an organic solvent, and an additive selected from at least one of compounds represented by structural formula I:
wherein R is 1 ～R 4 Each independently selected from one of hydrogen atom, substituted or unsubstituted C1-C6 alkyl, substituted or unsubstituted C1-C6 unsaturated alkyl, substituted or unsubstituted C2-C20 alkenyl, cyano, and a group formed by substituting aryl with 6-18 carbon atoms by carbonyl, cyano, halogen atom, nitro, carboxyl and sulfonic group, wherein the halogen atom is F, cl and Br, and is preferably F, cl;
x is one selected from C, O, NH.
Compared with the prior art, in the electrolyte, the additive is at least one selected from the compounds shown in the structural formula I, the additive is a positive electrode protection additive, specifically, the compound shown in the structural formula I contains cyclic C = C unsaturated double bonds, and is reduced into a tougher interfacial film (SEI film) at the positive electrode/electrolyte interface, and the SEI film has good conductive lithium ion channels, so that the collapse of the lithium ion channels is not generated in the circulation process, and the high-temperature circulation and low-temperature performance of the battery can be well improved. Particularly, the five-membered heterocyclic compound is introduced, so that the stability of the SEI film can be improved, elements such as nitrogen and oxygen can enrich the components of the electrode/electrolyte interface film, the structural stability of the interface film is further improved, and the high-temperature storage performance of the lithium ion battery is greatly improved.
Wherein C1-C6 alkyl represents an alkyl group having 1-6 carbon atoms, the alkyl group may be a chain alkyl group or a cycloalkyl group, and hydrogen on the ring of the cycloalkyl group may be substituted with an alkyl group, and the alkyl group may specifically be, but not limited to, a methyl group, an ethyl group, a propyl group, a butyl group, a pentyl group, and a cyclohexyl group.
Wherein the C1-C6 unsaturated hydrocarbon group represents a hydrocarbon group having 1-6 carbon atoms.
Wherein C2-C20 alkenyl represents alkenyl having 2-20 carbon atoms, and may be cyclic alkenyl or chain alkenyl. Further, the alkenyl group is selected from those having 2 to 5 carbon atoms. Specifically, it may be, but not limited to, an ethylene group, a propylene group, and the like.
Wherein aryl may be, but is not limited to, phenyl and the like.
Preferably, the compound shown in the structural formula I is selected from at least one of a compound 1 to a compound 8:
preferably, the mass of the additive accounts for 0.1-5% of the total mass of the electrolyte, and specifically, but not limited to, 0.1%, 0.3%, 0.5%, 0.8%, 1.2%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.2%, 4.5%, 4.8%, 5%. Furthermore, the mass of the additive accounts for 0.2-3% of the total mass of the electrolyte.
Preferably, the lithium salt is selected from lithium hexafluorophosphate (LiPF) 6 ) Lithium perchlorate (LiClO) 4 ) Lithium tetrafluoroborate (LiBF) 4 ) Lithium methylsulfonate (LiCH) 3 SO 3 ) Lithium trifluoromethanesulfonate (LiCF) 3 SO 3 ) Lithium bistrifluoromethylsulfonyl imide (LiN (CF) 3 SO 2 ) 2 ) Lithium bis (oxalato) borate (C) 4 BLiO 8 ) Lithium difluorooxalato borate (C) 2 BF 2 LiO 4 ) Lithium difluorophosphate (LiPO) 2 F 2 ) Lithium difluorobis (oxalato) phosphate (LiDFBP), lithium bis (fluorosulfonylimide) (LiFSI), and lithium bis (trifluoromethylsulfonyl) imide (LiTFSI).
Preferably, the amount of the lithium salt is 5 to 25% by mass of the total mass of the electrolyte, and specifically, may be 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, but is not limited to the enumerated values, and other non-enumerated values within the numerical range are also applicable. Further, the mass of the lithium salt accounts for 6-20% of the total mass of the electrolyte.
Preferably, the organic solvent is at least one selected from the group consisting of chain carbonates, cyclic carbonates, carboxylic acid esters, ethers, and heterocyclic compounds. More specifically, the organic solvent of the present invention may be selected from at least one of Ethylene Carbonate (EC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl Methyl Carbonate (EMC), propylene Carbonate (PC), butyl acetate (n-Ba), γ -butyrolactone (γ -Bt), propyl propionate (n-PP), ethyl Propionate (EP) and ethyl butyrate (Eb). Further, the mass of the organic solvent is 60% or more, preferably 70% or more, more preferably 75% or more, of the total mass of the electrolyte, and may be, for example, but not limited to, 78%, 80%, 82%, 85%, and the like.
Preferably, the electrolyte of the present invention further comprises an auxiliary agent, wherein the auxiliary agent is at least one selected from Vinylene Carbonate (VC), vinylene vinyl carbonate (VEC), fluoroethylene carbonate (FEC), ethylene Sulfite (ES), 1,3 Propane Sultone (PS), and vinyl sulfate (DTD). The mass of the auxiliary agent is 0.1-6.0% of the total mass of the electrolyte, and specifically, but not limited to, 0.1%, 0.5%, 1.5%, 2%, 2.5%, 3%, 4%, 4.5%, 5%, 5.5%, 6.0%. The addition of the auxiliary agent can further improve the cycle performance and the high-temperature storage performance of the lithium ion battery.
Correspondingly, the invention also provides a lithium ion battery which comprises a positive electrode, a negative electrode and the electrolyte, wherein the positive electrode is made of a nickel-cobalt-manganese oxide material. The lithium ion battery adopts the electrolyte, and can still realize better high and low temperature discharge performance when the highest charging voltage is 4.4V, and the cycle life of the battery is obviously prolonged.
Preferably, the nickel-cobalt-manganese oxide material adopts high nickel-cobalt-manganese oxide, liNi x Co y Mn (1-x-y) M z O 2 Wherein x is more than or equal to 0.6<0.9，x+y<1，0≤z<0.08, M is at least one of Al, mg, zr and Ti.
Preferably, the negative electrode of the present invention is made of a carbon negative electrode material, a silicon negative electrode material or a silicon-carbon negative electrode material. The negative electrode is preferably a silicon carbon negative electrode material, wherein the mass ratio of carbon to silicon is 90.
Detailed Description
To better illustrate the objects, technical solutions and advantages of the present invention, the present invention will be further described with reference to specific examples. It should be noted that the following implementation of the method is a further explanation of the present invention, and should not be taken as a limitation of the present invention.
Example 1
(1) Preparing an electrolyte:
ethylene Carbonate (EC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) were mixed at a mass ratio of EC: DEC: EMC =1 6 ) After the lithium salt was completely dissolved, 1g of Vinylene Carbonate (VC) and 5g of fluoroethylene carbonate (FEC) and 0.5g of positive electrode protection additive compound 1 were added.
(2) Preparing a positive plate:
LiNi prepared from nickel cobalt lithium manganate ternary material 0.6 Co 0.2 Mn 0.2 Zr 0.03 O 2 And uniformly mixing the conductive agent SuperP, the adhesive PVDF and the Carbon Nano Tubes (CNT) according to a mass ratio of 97.5.
(3) Preparing a negative plate:
mixing artificial graphite and silicon according to a mass ratio of 90 to 10, preparing slurry with a conductive agent SuperP, a thickening agent CMC and a binder SBR (styrene butadiene rubber emulsion) according to a mass ratio of 95.5.
(4) Preparing a lithium ion battery:
and preparing the positive electrode, the diaphragm and the negative electrode into a square battery cell in a lamination mode, packaging by adopting a polymer, filling the prepared non-aqueous electrolyte of the lithium ion battery, and preparing the lithium ion battery with the capacity of 1000mAh through the working procedures of formation, capacity grading and the like.
The electrolyte compositions of examples 2 to 10 and comparative example 1 are shown in table 1, and the procedure for preparing the electrolyte and the lithium ion battery was the same as in example 1.
TABLE 1 electrolyte composition of examples and comparative examples
The lithium ion batteries manufactured in examples 1 to 10 and comparative example 1 were subjected to a normal temperature cycle test, a high temperature storage test, and a low temperature discharge test, respectively, under the following test conditions, and the test results are shown in table 2.
Normal temperature cycle test：
Under the condition of normal temperature (25 ℃), the lithium ion battery is charged and discharged at 1.0C/1.0C once (the battery discharge capacity is C) 0 ) The upper limit voltage was 4.4V, and then 1.0C/1.0C charging and discharging were performed under normal temperature conditions for 500 weeks (the battery discharge capacity was C) 1 )；
Capacity retention rate = (C) 1 /C 0 )*100％
High temperature cycle test：
Under the condition of over-high temperature (45 ℃), the lithium ion battery is charged and discharged at 1.0C/1.0C once (the battery discharge capacity is C) 0 ) The upper limit voltage was 4.4V, and then 1.0C/1.0C charging and discharging were performed under normal temperature conditions for 300 weeks (the battery discharge capacity was C) 1 )；
Capacity retention rate = (C) 1 /C 0 )*100％
High temperature storage test：
Under the condition of normal temperature (25 ℃), the lithium ion battery is charged and discharged once at 0.3C/0.3C (the discharge capacity of the battery is recorded as C) 0 ) The upper limit voltage is 4.4V; placing the battery in a 60 ℃ oven for 15 days, taking out the battery, placing the battery in an environment at 25 ℃, discharging at 0.3C, and recording the discharge capacity as C 1 (ii) a Then the lithium ion battery is charged once at 0.3C/0.3CAnd discharge (battery discharge capacity recorded as C) 2 )；
Capacity retention rate = (C) 1 /C 0 )*100％
Capacity recovery rate = (C) 2 /C 0 )*100％
Low temperature discharge test：
The lithium ion battery was charged and discharged at one time at normal temperature (25 ℃) at 0.3C/0.3C (battery discharge capacity is recorded as C) 0 ) The upper limit voltage is 4.4V; placing the battery in an oven at-20 deg.C for 4h, discharging the battery at 0.3C, and recording the discharge capacity as C 1 The cut-off voltage is 3.0V,
capacity retention rate = (C) 1 /C 0 )*100％
Table 2 results of performance test of lithium ion batteries of examples and comparative examples
As can be seen from table 2, the batteries using the electrolytes of the present invention were significantly improved in normal temperature cycle, high temperature storage performance, high temperature cycle performance, and low temperature discharge performance, as compared to comparative example 1. This is because the additive is selected from at least one of the compounds of formula I, which is a positive electrode protection additive, specifically, the compound of formula I contains cyclic C = C unsaturated double bonds, which are reduced to a tougher interfacial film (SEI film) at the positive electrode/electrolyte interface, and the film has good lithium ion conduction channels, does not cause collapse of lithium ion channels during cycling, and can improve the high temperature cycling and low temperature performance of the battery well. Particularly, the five-membered heterocyclic compound is introduced, so that the stability of the SEI film can be improved, elements such as nitrogen and oxygen can enrich the components of an electrode/electrolyte interface film, the lithium ion conduction characteristic of the interface film is further improved, and the low-temperature performance of the lithium ion battery is greatly improved.
As can be seen from the data of example 6, it has relatively superior high temperature performance, which may be that compound 6 has a completely symmetrical structure that improves the stability of compound 6 in a high voltage battery, and at the same time, compound 6 forms a thicker SEI after electropolymerization, thus resulting in a greater improvement in the high temperature performance of the battery.
It can be further understood from the data of examples 7-8 that the low temperature performance of the battery using compounds 7-8 as additives is more advantageous than that of compounds 1-6, probably because compounds 7-8 add O and N to the heterocyclic ring, lithium carboxylate and lithium nitride can be formed, and the SEI film is denser, which is beneficial to further reducing the transmission path of lithium ions in the SEI film, thereby effectively improving the low temperature performance of the battery.
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention and not for limiting the protection scope of the present invention, and although the present invention is described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions can be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention.
Claims (10)
1. An electrolyte comprising a lithium salt, an organic solvent and an additive, wherein the additive is at least one selected from the group consisting of compounds represented by formula I:
wherein R is 1 ～R 4 Each independently selected from one of hydrogen atom, substituted or unsubstituted C1-C6 alkyl, substituted or unsubstituted C1-C6 unsaturated alkyl, substituted or unsubstituted C2-C20 alkenyl, cyano, and a group formed by substituting aryl with 6-18 carbon atoms by carbonyl, cyano, halogen atom, nitro, carboxyl and sulfonic group, wherein the halogen atom is F, cl or Br;
x is one selected from C, O, NH.
2. The electrolyte of claim 1, wherein the compound of formula I is at least one compound selected from the group consisting of compounds 1 to 8:
3. the electrolyte of claim 1, wherein the additive comprises 0.1% to 5% by mass of the total mass of the electrolyte.
4. The electrolyte of claim 3, wherein the additive is present in an amount of 0.2% to 3% by weight of the total electrolyte.
5. The electrolyte of claim 1, wherein the lithium salt is selected from at least one of lithium hexafluorophosphate, lithium perchlorate, lithium tetrafluoroborate, lithium methanesulfonate, lithium trifluoromethanesulfonate, lithium bistrifluoromethylsulfonimide, lithium dioxalate borate, lithium difluorooxalato borate, lithium difluorophosphate, lithium difluorobisoxalato phosphate, lithium difluorosulfonimide, lithium bistrifluoromethylsulfonyl imide.
6. The electrolyte of claim 1, wherein the lithium salt is present in an amount of 5 to 25% by mass based on the total mass of the electrolyte.
7. The electrolyte according to claim 1, wherein the organic solvent is at least one selected from the group consisting of chain carbonates, cyclic carbonates, carboxylic acid esters, and ethers.
8. The electrolyte of claim 1, further comprising an additive selected from at least one of vinylene carbonate, vinylene ethylene carbonate, fluoroethylene carbonate, ethylene sulfite, 1,3 propane sultone, and ethylene sulfate.
9. A lithium ion battery comprising a positive electrode and a negative electrode, characterized by further comprising the electrolyte of any one of claims 1 to 8, wherein the positive electrode is made of a nickel-cobalt-manganese oxide material.
10. The lithium ion battery of claim 9, wherein the nickel cobalt manganese oxide material is LiNi x Co y Mn (1-x-y) M z O 2 Wherein x is more than or equal to 0.6<0.9，x+y<1，0≤z<0.08, M is at least one of Al, mg, zr and Ti.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN118099531A (en) * | 2024-04-29 | 2024-05-28 | 广州天赐高新材料股份有限公司 | Electrolyte and battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN118099531A (en) * | 2024-04-29 | 2024-05-28 | 广州天赐高新材料股份有限公司 | Electrolyte and battery |
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