CN115498258A - Electrolyte additive, lithium ion battery electrolyte and lithium ion battery - Google Patents

Electrolyte additive, lithium ion battery electrolyte and lithium ion battery Download PDF

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Publication number
CN115498258A
CN115498258A CN202210979196.8A CN202210979196A CN115498258A CN 115498258 A CN115498258 A CN 115498258A CN 202210979196 A CN202210979196 A CN 202210979196A CN 115498258 A CN115498258 A CN 115498258A
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electrolyte
lithium ion
oxygen
ion battery
additive
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Inventor
钟泽钦
万远鑫
谭旗清
孔令涌
赵中可
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Shenzhen Dynanonic Innovazone New Energy Technology Co Ltd
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Shenzhen Dynanonic Innovazone New Energy Technology Co Ltd
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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
    • 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
    • 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
    • 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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  • Chemical & Material Sciences (AREA)
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  • Manufacturing & Machinery (AREA)
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  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

The application relates to the technical field of lithium ion batteries, in particular to an electrolyte additive, a lithium ion battery electrolyte and a lithium ion battery. An electrolyte additive is provided, which includes at least one of a metal oxide containing an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses the generation of oxygen; the electrolyte additive can react with oxygen or inhibit the generation of oxygen, so that the problem that oxygen is easily generated after a positive electrode lithium supplement material is added into a lithium ion battery is solved, the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.

Description

Electrolyte additive, lithium ion battery electrolyte and lithium ion battery
Technical Field
The application belongs to the technical field of lithium ion batteries, and particularly relates to an electrolyte additive, a lithium ion battery electrolyte and a lithium ion battery.
Background
A lithium ion battery is a secondary battery (rechargeable battery) that mainly operates by movement of lithium ions between a positive electrode and a negative electrode. During charging and discharging, li + Intercalation and deintercalation to and from two electrodes: upon charging, li + The lithium ion battery is extracted from the positive electrode and is inserted into the negative electrode through the electrolyte, and the negative electrode is in a lithium-rich state; the opposite is true during discharge. Because the charge and discharge processes of the lithium ion battery are the insertion and extraction processes of lithium ions, lithium loss is caused in the charge and discharge processes of the lithium ion battery, and a lithium supplement additive is usually added for use.
Most of the common positive electrode lithium supplement additives at present are Li 2 The O form is decomposed to form active lithium, which can exert higher theoretical capacity, but is accompanied with the generation of a large amount of active oxygen, so that the lithium supplement materials easily cause the gas generation problem of the lithium ion battery in the formation stage in the use process, thereby causing the gas expansion phenomenon in the sealed battery system, generating more gas in the formation process, influencing the intercalation of lithium ions in a negative plate and the formation of a normal SEI film, causing the negative plate to be incapable of forming a uniform SEI film after the formation is finished, being accompanied with the defects of black spots, lithium precipitation and the like, seriously influencing the safety performance and the cycle performance of the lithium battery, and being incapable of being normally used. The existing solution is to pump gas away in the formation stage, but the existing lithium supplement material is not necessarily completely decomposed into oxygen gas in the first cycle of charging, and a small amount of oxygen is also available in the later stage, and the existence of the gas generated in the later stage can cause the performance deterioration of the battery and generate great potential safety hazard.
Li due to the influence of other factors such as kinetics during the formation process 2 The O composite material is not completely decomposed, and the rest Li although the partial decomposed oxygen can be pumped away in time 2 The O composite material can still be continuously decomposed to generate oxygen in the later charging process, and the continuous generation of the oxygen can cause the performance deterioration of the battery and the problem of potential safety hazard, so that the long-term use of the battery is not facilitated.
Disclosure of Invention
The application aims to provide an electrolyte additive, a lithium ion battery electrolyte and a lithium ion battery, and aims to solve the problems that in the prior art, a positive electrode lithium supplement material is still decomposed to generate oxygen in the later charging process, so that the battery is deteriorated and potential safety hazards are easy to occur.
In order to achieve the purpose of the application, the technical scheme adopted by the application is as follows:
in a first aspect, the present application provides an electrolyte additive comprising at least one of a metal oxide containing an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses the generation of oxygen.
In a second aspect, the present application provides a lithium ion battery electrolyte, which includes a lithium salt, an organic solvent, and an electrolyte additive, wherein the electrolyte additive includes the above electrolyte additive.
In a third aspect, the present application provides a lithium ion battery, where the assembly process of the lithium ion battery includes: and assembling the anode, the cathode, the diaphragm and the first electrolyte, carrying out formation treatment, pumping away oxygen after the formation treatment, and adding an electrolyte additive into the first electrolyte, wherein the electrolyte additive is selected from the electrolyte additives.
The electrolyte additive provided by the first aspect of the application comprises at least one of metal oxide containing oxygen defects, organic matter carrying groups capable of reacting with oxygen, and organic matter carrying groups for inhibiting oxygen generation; on one hand, the provided metal oxide containing oxygen defects has a certain physical adsorption effect on oxygen, and the internal crystal structure of the metal oxide containing oxygen defects can store oxygen generated by a lithium supplement agent; on the other hand, the metal oxide containing oxygen defects can react with oxygen chemically to change the metal element into a positive valence state, so as to obtain a stable product; the organic matter carrying the group capable of reacting with oxygen can directly react with oxygen, consumes peroxide generated by the lithium supplement additive and is converted into a stable inactive product; the organic matter carrying the group for inhibiting the generation of oxygen can well reduce the effect of gas generation and inhibit the generation of oxygen; therefore, the electrolyte additive comprises at least one of metal oxide containing oxygen defects, organic matter carrying groups capable of reacting with oxygen and organic matter carrying groups for inhibiting oxygen generation, and can control the generation of active oxygen in the electrolyte, so that the problem that oxygen is easily generated after a positive electrode lithium supplement material is added into a lithium ion battery is solved, the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.
The lithium ion battery electrolyte that this application second aspect provided, the lithium ion battery electrolyte that provides includes the electrolyte additive in, the electrolyte that contains the electrolyte additive can avoid owing to mend the incomplete later stage oxygen problem that leads to of lithium material decomposition in the formation process, has solved and has mended the problem of battery performance deterioration and potential safety hazard that the oxygen leads to of lithium material oxygen production after the formation is finished.
In the lithium ion battery provided by the third aspect of the present application, the lithium ion battery includes an anode, a cathode, a separator, a first electrolyte, and an electrolyte additive, and the battery is assembled first, and then a formation treatment is performed, and oxygen is pumped away after the formation treatment, and the electrolyte additive is added into the first electrolyte; the electrolyte additive is supplemented into the electrolyte, so that oxygen generated by the anode lithium supplement additive can be effectively consumed, and the problem that oxygen is easily generated after the anode lithium supplement material is added into the lithium ion battery is solved; the electrolyte additive provided by the application is added after formation treatment, so that the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present application more clearly apparent, the present application is further described in detail below with reference to the embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the present application and are not intended to limit the present application.
In this application, the term "and/or" describes an association relationship of associated objects, meaning that there may be three relationships, e.g., a and/or B, which may mean: a alone, A and B together, and B alone. Wherein A and B can be singular or plural. The character "/" generally indicates that the former and latter associated objects are in an "or" relationship.
In the present application, "at least one" means one or more, "a plurality" means two or more. "at least one of the following" or similar expressions refer to any combination of these items, including any combination of the singular or plural items. For example, "at least one (one) of a, b, or c," or "at least one (one) of a, b, and c," may each represent: a, b, c, a-b (i.e., a and b), a-c, b-c, or a-b-c, wherein a, b, and c may be single or plural, respectively.
It should be understood that, in various embodiments of the present application, the sequence numbers of the above-mentioned processes do not mean the execution sequence, some or all of the steps may be executed in parallel or executed sequentially, and the execution sequence of each process should be determined by its function and inherent logic, and should not constitute any limitation to the implementation process of the embodiments of the present application.
The terminology used in the embodiments of the present application is for the purpose of describing particular embodiments only and is not intended to be limiting of the application. As used in the examples of this application and the appended claims, the singular forms "a", "an", and "the" are intended to include the plural forms as well, unless the context clearly indicates otherwise.
The weight of the related components mentioned in the description of the embodiments of the present application may not only refer to the specific content of each component, but also represent the proportional relationship of the weight among the components, and therefore, the content of the related components is scaled up or down within the scope disclosed in the description of the embodiments of the present application as long as it is scaled up or down according to the description of the embodiments of the present application. Specifically, the mass in the description of the embodiments of the present application may be in units of mass known in the chemical industry, such as μ g, mg, g, and kg.
The terms "first" and "second" are used for descriptive purposes only and are used for distinguishing purposes such as substances from one another and are not to be construed as indicating or implying relative importance or to implicitly indicate the number of technical features indicated. For example, a first XX may also be referred to as a second XX, and similarly, a second XX may also be referred to as a first XX, without departing from the scope of embodiments of the present application. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature.
In a first aspect of the embodiments, there is provided an electrolyte additive including at least one of a metal oxide including an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses generation of oxygen.
In the electrolyte additive provided by the first aspect of the embodiments of the present application, the electrolyte additive includes at least one of a metal oxide containing an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses the generation of oxygen; on one hand, the provided metal oxide containing oxygen defects has a certain physical adsorption effect on oxygen, and the internal crystal structure of the metal oxide containing oxygen defects can store oxygen generated by a lithium supplement agent; on the other hand, the metal oxide containing oxygen defects can chemically react with oxygen to change the metal element into a positive valence state, so that a stable product is obtained; the organic matter carrying the group capable of reacting with oxygen can directly react with oxygen, consume peroxide generated by the lithium supplement additive, and be converted into a stable inactive product; the organic matter carrying the group for inhibiting the generation of oxygen can well reduce the effect of gas generation and inhibit the generation of oxygen; therefore, the electrolyte additive comprises at least one of metal oxide containing oxygen defects, organic matter carrying groups capable of reacting with oxygen and organic matter carrying groups for inhibiting oxygen generation, and can control the generation of active oxygen in the electrolyte, so that the problem that oxygen is easy to generate after a positive electrode lithium supplement material is added into the lithium ion battery is solved, the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.
The electrolyte additive selects metal oxide containing oxygen defects, on one hand, the electrolyte additive has certain physical adsorption effect on oxygen, and the crystal structure in the metal oxide containing oxygen defects can store oxygen generated by the lithium supplement agent; on the other hand, the metal oxide containing oxygen defects can react with oxygen chemically to change the metal element into a positive valence state, so that a stable product is obtained.
In some embodiments, the metal oxide containing oxygen defects has the formula MO x M is a metal element and satisfies: when the valence state of M is a, x is more than 0 and less than a/2; wherein M is at least one selected from Ce, ti, mn, sn, zr, W, al, mo, fe, zn, cu, co, ni and Cr. Wherein, in the selected metal oxide, the valence states of the metal element are unsaturated valence states, which ensures that the metal element is added into the electrolyte and can generate chemical reaction with redundant oxygen, after the metal element is reacted with oxygen, the metal element M is changed into a positive valence state, namely x = a/2, oxygen is supplemented for the metal oxide, the metal element with the positive valence state is obtained, and a stable product is obtained.
In some embodiments, the metal oxide containing oxygen defects is selected from TiO x 、CeO x Wherein 1.2 < x < 2, and TiO when x is selected to be 1.2 < x < 2 x And CeO x The compound is a sub-oxidation state compound with oxygen defects or oxygen vacancies, and can chemically react with redundant oxygen to supplement oxygen for the metal oxide to obtain the metal element with a positive valence state and obtain a stable product.
In a specific embodiment, the metal oxide TiO containing oxygen defects x Including but not limited to TiO 1.3 、TiO 1.5 、TiO 1.8 . When TiO is present x When the lithium ion battery electrolyte is used as an electrolyte additive, on one hand, the internal crystal structure can store oxygen generated by a lithium supplement agent; on the other hand, tiO x And reacting with excessive oxygen to obtain stable product.
In a specific embodiment, the oxygen deficient metal oxide CeO x Including but not limited to CeO 1.2 、CeO 1.6 、CeO 1.8 . When CeO is present x When the lithium ion battery electrolyte is used as an electrolyte additive, on one hand, the internal crystal structure can store oxygen generated by a lithium supplement agent; on the other hand, ceO x And the reaction product reacts with the redundant oxygen to obtain a stable product.
In some embodiments, the electrolyte additive is selected to be an organic species that carries groups capable of reacting with oxygen, which can react directly with oxygen, consuming the peroxide generated by the lithium supplement additive and converting to a stable inactive product.
In some embodiments, the organic species carrying a group capable of reacting with oxygen is selected from, but not limited to, at least one of phosphate organic species, phosphite organic species, phenolic antioxidants, alcoholic antioxidants.
The organic matter carrying the group capable of reacting with oxygen is selected from phosphate organic matter, and the phosphoric acid group in the provided phosphate organic matter can be combined with the generated oxygen, namely peroxide generated by the lithium supplement agent is consumed, and a stable inactive product is generated.
In some embodiments, the phosphate-based organic includes, but is not limited to, at least one of a-bis (diphenyl phosphate), resorcinol-bis (diphenyl phosphate), triethyl phosphate.
The organic matter carrying the group capable of reacting with oxygen is selected from phosphite organic matter, and the provided phosphite organic matter can directly react with oxygen to form a diphosphorous oxygen functional group so as to consume peroxide generated by the lithium supplement agent and generate a stable inactive product.
In some embodiments, the phosphite organic includes, but is not limited to, at least one of tris (2, 4-di-t-butylphenyl) phosphite, tetrakis (2, 4-di-t-butylphenyl-4, 4' -biphenylyl) bisphosphite, bis (2, 4-di-t-butylphenyl) pentaerythritol bisphosphite, bis (octadecyl) pentaerythritol bisphosphite.
The organic matter carrying the group capable of reacting with oxygen is selected from phenolic antioxidants, the provided phenolic antioxidants prevent or inhibit chain initiation reaction and chain growth reaction by capturing peroxy radicals of oxygen generated by the positive electrode lithium supplement additive, so that the free radical chain reaction is terminated, namely the peroxide free radicals capture hydrogen from phenol to generate hydroperoxide and phenoxy free radicals, and the generated phenoxy free radicals react with other peroxy free radicals in different ways to generate relatively stable products.
In some embodiments, the phenolic antioxidant includes, but is not limited to, at least one of 2, 6-di-tert-butyl-p-cresol, 2, 6-di-tert-butyl-4-methylphenol, 2' -methylenebis (4-methyl-6-tert-butylphenol). The phenolic antioxidant also comprises thiophenol compounds with S-H group and tea polyphenols. In addition, the alcoholic antioxidant includes thiol compounds having S-H groups.
In some embodiments, the organic bearing oxygen production inhibiting groups is selected from sulfonate-based organics. The organic matter carrying the group for inhibiting the generation of oxygen can better reduce the function of gas generation and inhibit the generation of oxygen.
In some embodiments, the provided sulfonate organic compound can better reduce the effect of oxygen generation, and has the effects of improving the high-temperature cycle retention rate and the capacity recovery rate.
In some embodiments, the sulfonate-based organic compound includes, but is not limited to, at least one of 1, 3-propane sultone, 1, 3-propene sultone, 1, 4-butane sultone,
In a second aspect, the embodiment of the present application provides a lithium ion battery electrolyte, where the lithium ion battery electrolyte includes a lithium salt, an organic solvent, and an electrolyte additive, and the electrolyte additive includes the above electrolyte additive.
The lithium ion battery electrolyte that the second aspect of the embodiment of this application provided includes the electrolyte additive in the lithium ion battery electrolyte that provides, and the electrolyte that contains the electrolyte additive can avoid owing to mend the incomplete later stage oxygen problem that leads to of lithium material decomposition in the formation process, has solved and has mended the problem that the battery performance worsens and the potential safety hazard that the oxygen leads to is produced to the lithium material after the formation is finished.
In some embodiments, the electrolyte additive is present in the lithium ion battery electrolyte in an amount of 1wt% to 10wt%. If the additive is added in too much amount, the additive cannot be completely dissolved in the electrolyte, and the mobility of lithium ions is reduced, so that the performance of the lithium ion battery is reduced; if the additive amount of the electrolyte is too small, the electrolyte does not play a corresponding role in consuming oxygen.
In some embodiments, the percentage by mass of the electrolyte additive in the lithium ion battery electrolyte includes, but is not limited to, 1wt%, 1.5wt%, 2wt%, 2.5wt%, 3wt%, 3.5wt%, 4wt%, 4.5wt%, 5wt%, 5.5wt%, 6wt%, 6.5wt%, 7wt%, 7.5wt%, 8wt%, 8.5wt%, 9wt%, 9.5wt%, 10wt%.
In some embodiments, the lithium ion battery electrolyte comprises a lithium salt, wherein the lithium salt includes, but is not limited to, liPF 6 、LiBF 4 、LiFSI、LiB(C 2 O 4 ) 2 One kind of (1).
In some embodiments, the lithium salt is present in the lithium ion battery electrolyte in an amount of 10% to 30% by weight.
In some embodiments, the lithium salt is present in the lithium ion battery electrolyte in a mass percent amount including, but not limited to, 10wt%, 12wt%, 14wt%, 16wt%, 18wt%, 20wt%, 22wt%, 24wt%, 26wt%, 28wt%, 30wt%.
In some embodiments, the lithium ion battery electrolyte comprises an organic solvent, wherein the organic solvent comprises, but is not limited to, at least one of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, methyl acetate, methyl propionate, ethyl acetate, 1, 3-propane sultone, adiponitrile, succinonitrile.
In some embodiments, the lithium ion battery electrolyte contains 55% to 75% by mass of an organic solvent.
In some embodiments, the mass percent of organic solvent in the lithium ion battery electrolyte includes, but is not limited to, 55wt%, 57wt%, 59wt%, 60wt%, 62wt%, 65wt%, 67wt%, 70wt%, 72wt%, 75wt%.
A third aspect of the embodiments of the present application provides a lithium ion battery, where an assembly process of the lithium ion battery includes: and assembling the anode, the cathode, the diaphragm and the first electrolyte, carrying out formation treatment, pumping away oxygen after the formation treatment, and adding an electrolyte additive into the first electrolyte, wherein the electrolyte additive is selected from the electrolyte additives.
In the lithium ion battery provided by the third aspect of the present application, the lithium ion battery includes a positive electrode, a negative electrode, a diaphragm, a first electrolyte, and an electrolyte additive, and the battery is assembled first, then a formation treatment is performed, oxygen is pumped away after the formation treatment, and the electrolyte additive is added into the first electrolyte; the electrolyte additive is supplemented into the electrolyte, so that oxygen generated by the anode lithium supplement additive can be effectively consumed, the problem that oxygen is easily generated after the anode lithium supplement material is added into the lithium ion battery is solved, if the electrolyte additive is added before formation, the oxygen is easily consumed immediately, and the problem that oxygen is easily generated after the anode lithium supplement material is added into the lithium ion battery cannot be solved; the electrolyte additive provided by the application is added after formation treatment, so that the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.
In some embodiments, the positive electrode includes a positive active material, a lithium supplement material, a conductive agent, and a binder.
In some embodiments, the positive electrode active material includes, but is not limited to, at least one of lithium cobaltate, lithium iron phosphate, lithium iron manganese phosphate, lithium manganese oxide, lithium nickel cobalt manganese oxide, lithium nickel manganese oxide.
In some embodiments, the lithium supplement material is a lithium supplement material that is susceptible to oxygen generation. In some embodiments, the material comprising the lithium core comprises Li x M y O z Wherein x is more than 0 and less than or equal to 6, y is more than 0 and less than or equal to 3, z is more than 0 and less than or equal to 4, and M comprises at least one of Fe, co, ni, mn, V, cu, mo, al, ti, mg, zr, re and the like.
In some embodiments, the lithium-supplementing material includes, but is not limited to, li 2 NiO 2 、Li 5 FeO 4 、Li 2 MnO 3 、Li 6 CoO 4 、Li 6 MnO 4 、Li 5 ReO 6 At least one of (1). In some embodiments, the conductive agent includes at least one of graphite, carbon black, acetylene black, graphene, carbon fibers, and carbon nanotubes.
In some embodiments, the binder includes, but is not limited to, at least one of polyvinylidene chloride, soluble polytetrafluoroethylene, styrene butadiene rubber, hydroxypropylmethyl cellulose, methyl cellulose, carboxymethyl cellulose, polyvinyl alcohol, acrylonitrile copolymer, sodium alginate, chitosan, and chitosan derivatives.
In some embodiments, the positive current collector includes, but is not limited to, at least one of aluminum foil, carbon-coated aluminum foil, iron foil, tin foil, zinc foil, nickel foil, titanium foil, and manganese foil.
In a specific embodiment, the preparation process of the positive electrode is as follows: mixing the positive electrode active material, the lithium supplement additive, the conductive agent and the binder to obtain electrode slurry, coating the electrode slurry on a current collector, and drying, rolling, die-cutting and the like to prepare the positive electrode piece.
In some embodiments, the negative electrode is selected from, but not limited to, natural graphite.
In some embodiments, the membrane is selected from, but not limited to, polypropylene membranes.
In a particular embodiment, to enable elimination of Li 2 The positive electrode lithium supplement material with active lithium formed by decomposing O is still decomposed to generate oxygen in the later charging process, so that the battery is deteriorated and potential safety hazards are easy to occur; therefore, in the assembly process of the lithium ion battery, a secondary liquid supplementing method is adopted, in the first liquid injection and packaging process, electrolyte without an electrolyte additive is injected for formation treatment, and a part of oxygen is pumped away after treatment; then adding electrolyte containing electrolyte additive in the subsequent liquid supplementing process to eliminate Li in the electrolyte additive 2 The positive electrode lithium supplement material with O decomposed to form active lithium is still decomposed to generate oxygen in the later charging process.
In some embodiments, assembling the lithium ion battery comprises: and assembling the anode, the cathode, the diaphragm and the first electrolyte, performing formation treatment, pumping away oxygen after the formation treatment, and adding an electrolyte additive into the first electrolyte.
In some embodiments, the lithium ion battery further comprises a second electrolyte, wherein the electrolyte additive is added to the first electrolyte by mixing the electrolyte additive with the second electrolyte to obtain a mixed electrolyte, and the mixed electrolyte is subjected to solution supplementation and added to the lithium ion battery.
In some embodiments, assembling the lithium ion battery comprises:
s01, assembling the anode, the cathode, the diaphragm and the first electrolyte, performing chemical conversion treatment, and pumping away oxygen after the chemical conversion treatment;
s02, mixing the electrolyte additive with a second electrolyte to obtain a mixed electrolyte, and supplementing the mixed electrolyte to the lithium ion battery.
In step S01, the positive electrode, the negative electrode, and the separator are assembled and then baked, and the baked battery cell is subjected to vacuum injection with a first electrolyte and pre-packaging treatment; then high-temperature standing and primary high-temperature formation are carried out; after the formation treatment, vacuum pumping is carried out, and oxygen is pumped away.
In step S02, the electrolyte additive is mixed with the second electrolyte to obtain a mixed electrolyte, the mixed electrolyte is replenished and added to the lithium ion battery, and after high-temperature aging treatment, cooling and final sealing treatment are performed. Electrolyte containing electrolyte additive is added in the liquid supplementing stage, so that Li can be fully eliminated 2 The positive electrode lithium supplement material with active lithium formed by decomposing O is continuously decomposed to generate oxygen in the later charging process; if Li is introduced before the battery is packaged 2 The positive electrode lithium supplement material with active lithium formed by decomposing O is still decomposed to generate oxygen in the later charging process, so that the electrolyte additive and the oxygen generated by decomposition are consumed in advance in the formation process, and cannot play a role in the later cyclic charging and discharging process. This application is through becoming after the end, and the oxygenating agent is introduced in the fluid infusion stage and avoids producing the oxygen problem because the incomplete later stage that leads to of earlier stage decomposition to the problem of battery performance deterioration and potential safety hazard that the solution produced oxygen and leads to.
Reason and effect of please supplement fluid infusion method
The following description is given with reference to specific examples.
Example A1
Lithium ion battery electrolyte and preparation method thereof
The types and contents of the components contained in the lithium ion battery electrolyte are shown in table 1.
The preparation method comprises the following steps: respectively mixing Ethylene Carbonate (EC), ethyl Methyl Carbonate (EMC) and Propylene Carbonate (PC) which are basic components according to the mass ratio of EC: EMC: PC =1.5 6 ) And then, the mixture was stirred until it was completely dissolved, and then, an electrolyte additive in an amount of 5% by mass of the total electrolyte was added and sufficiently mixed and dissolved to obtain an electrolyte of example A1.
Example A2
Lithium ion battery electrolyte and preparation method thereof
The types and contents of the components contained in the lithium ion battery electrolyte are shown in table 1, and the preparation method is the same as that provided in example A1.
Example A3
Lithium ion battery electrolyte and preparation method thereof
The types and contents of the components contained in the lithium ion battery electrolyte are shown in table 1, and the preparation method is the same as that provided in example A1.
Example A4
Lithium ion battery electrolyte and preparation method thereof
The types and contents of the components contained in the lithium ion battery electrolyte are shown in table 1, and the preparation method is the same as that provided in example A1.
Comparative example A1
Battery electrolyte and preparation method thereof
The types and contents of the components contained in the battery electrolyte are shown in table 1.
The preparation method comprises the following steps: mixing basic components of Ethylene Carbonate (EC), ethyl Methyl Carbonate (EMC) and Propylene Carbonate (PC) according to a mass ratio of EC to EMC to PC =1.5 to 0.5, and adding lithium salt to prepare lithium hexafluorophosphate (LiPF) with a concentration of 1.0mol/L 6 ) And thoroughly mixed and dissolved to obtain the electrolyte of comparative example A1.
TABLE 1
Figure BDA0003799726380000121
Example B1
Lithium ion battery and preparation method thereof
The lithium ion batteries are assembled into the lithium ion batteries according to the following methods:
1) Positive plate: the anode active material LiFePO is added 4 Lithium-supplementing material LiFeO 2 ·2Li 2 O, a conductive agent Super P, a binder polyvinylidene fluoride (PVDF) and N-methyl pyrrolidone (NMP) are uniformly mixed to prepare anode slurry, wherein LiFePO 4 ：LiFeO 2 ·2Li 2 O: super P: the mass ratio of PVDF is 93. And coating the positive slurry on a current collector aluminum foil, and performing drying-rolling-secondary drying processes to obtain the positive plate.
2) And (3) negative plate: uniformly mixing negative active material graphite, a conductive agent Super P, a thickening agent carboxymethyl cellulose (CMC) and a binder Styrene Butadiene Rubber (SBR) in deionized water to prepare negative slurry, wherein the weight ratio of graphite: super P: CMC: the mass ratio of SBR is 95. And coating the negative electrode slurry on a current collector copper foil, and performing drying-rolling-secondary drying procedures to prepare a negative electrode pole piece.
3) Diaphragm: using Polyethylene (PE) separators
4) Assembling the secondary battery:
and assembling the positive plate, the negative plate, the electrolyte and the diaphragm into the lithium ion soft package battery according to the assembly requirements of the lithium ion battery.
The preparation method comprises the following steps:
(1) Vacuum liquid injection is carried out on the soft package battery (the electrolyte solvent is ethylene carbonate, the solute is LiPF6, and no electrolyte additive is contained); (2) pre-sealing; (3) standing at high temperature; (4) carrying out primary high-temperature formation; (5) vacuum pumping; (6) Electrolyte is replenished for the second time, namely the electrolyte provided in the embodiment A1 is used as the electrolyte replenished for the second time, (7) high-temperature aging is carried out; (8) cooling; and (9) finishing.
Example B2
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the lithium ion battery provided is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A1 are respectively used as the electrolytes to be replenished twice" is modified to "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A2 are used as the electrolytes to be replenished twice".
Example B3
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A1 were used as the respective twice-replenished electrolytes" was modified to "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A3 were used as the twice-replenished electrolytes".
Example B4
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A1 were used as the respective twice-replenished electrolytes" was modified to "(6) twice-replenishing electrolytes, that is, the electrolytes provided in example A4 were used as the twice-replenished electrolytes".
Comparative example B1
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the lithium ion battery provided is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(6) twice-replenishing electrolyte, that is, the electrolyte provided in the example A1 is respectively used as each twice-replenished electrolyte," is modified to "(6) twice-replenishing electrolyte, that is, the electrolyte provided in the comparative example A1 is used as the twice-replenished electrolyte," that is, no electrolyte additive is added to the electrolyte before and after formation.
Comparative example B2
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(1) vacuum liquid injection is carried out on the soft package battery (here, the electrolyte solvent is ethylene carbonate, and the solute is LiPF 6 The electrolyte additive is not contained) "modified to" (1) vacuum charging of the pouch cell (here, the electrolyte solvent is the electrolyte provided in example A1) "; and "(6) Secondary replenishment electrolyte," modification of "6 Secondary replenishment electrolyte" in which the electrolytes provided in example A1 were used as the electrolytes for respective Secondary replenishment "(6) Secondary replenishment electrolyte, (here, the electrolyte solvent was ethylene carbonate, and the solute was LiPF 6 "without electrolyte additive)", that is, the electrolyte additive was added to the electrolyte before formation (the electrolyte was the same as in example A1), and the electrolyte additive was not added after formation.
Comparative example B3
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(1) vacuum liquid injection is carried out on the soft package battery (here, the electrolyte solvent is ethylene carbonate, and the solute is LiPF 6 The "modification without an electrolyte additive" is "(1) vacuum injection of the pouch battery (the electrolyte solvent here is the electrolyte provided in example A2)"; and "(6) twice-replenishing electrolytes, namely, the electrolytes provided in example A2 are respectively used as the electrolytes to be replenished twice, so that the electrolytes are not modified (6) twice-replenishing electrolytes, (the solvent of the electrolytes is ethylene carbonate, and the solute is LiPF (lithium iron phosphate) 6 "without electrolyte additive)", that is, the electrolyte additive was added to the electrolyte before formation (the electrolyte was the same as in example A2), and the electrolyte additive was not added after formation.
Comparative example B4
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(1) vacuum liquid injection is carried out on the soft package battery (here, the electrolyte solvent is ethylene carbonate, and the solute is LiPF 6 The electrolyte additive was not included) "modified to" (1) vacuum charging the pouch cell (the electrolyte solvent here is the electrolyte provided in example A3) "; and "(6) twice-replenishing electrolytes, namely, the electrolytes provided in example A3 are respectively used as the electrolytes to be replenished twice, so that the electrolytes are not modified (6) twice-replenishing electrolytes, (the solvent of the electrolytes is ethylene carbonate, and the solute is LiPF (lithium iron phosphate) 6 "without electrolyte additive)", that is, the electrolyte additive was added to the electrolyte before formation (the electrolyte was the same as in example A3), and the electrolyte additive was not added after formation.
Comparative example B5
Lithium ion battery and preparation method thereof
The selection of the positive plate, the negative plate and the diaphragm of the provided lithium ion battery is consistent with that of the lithium ion battery provided in the embodiment B1;
in the preparation method, "(1) vacuum liquid injection is carried out on the soft package battery (here, the electrolyte solvent is ethylene carbonate, and the solute is LiPF 6 The electrolyte additive was not included) "modified to" (1) vacuum charging the pouch cell (the electrolyte solvent here is the electrolyte provided in example A4) "; and, "(6) Secondary replenishment electrolyte, that is," modified "(6) Secondary replenishment electrolyte using the electrolyte provided in example A4 as each of the secondary replenishment electrolytes, respectively, (here, the electrolyte solvent is ethylene carbonate, and the solute is LiPF 6 "without electrolyte additive)", that is, the electrolyte additive was added to the electrolyte before formation (the electrolyte was the same as in example A4), and the electrolyte additive was not added after formation.
Performance test
The lithium ion batteries that were assembled and sealed in examples B1 to B4 and comparative examples B1 to B5 were subjected to the following performance tests:
and (3) normal-temperature cycle test: the battery is placed at 25 ℃, and is subjected to charge-discharge circulation by using 1C current in a charge-discharge voltage interval of 3.0-4.4V, and the initial thickness is recorded as T 0 And an initial capacity ofQ 0 Thickness T recycled to 100cycles 1 And a capacity of Q 1 And calculating the thickness change rate and the capacity retention rate of the battery in normal temperature cycle of 100cycles according to the following formulas:
normal temperature cycle 100cycles thickness change rate (%) = (T) 1 -T 0 )/T 0 ×100％；
Capacity retention ratio (%) of 100cycles at normal temperature cycle = Q 1 /Q 0 ×100％。
High-temperature cycle testing: under the condition of high temperature of 60 ℃, using 1C current to carry out charge-discharge circulation in the charge-discharge voltage interval of 3.0-4.4V, and recording the initial thickness T 2 And an initial capacity of Q 2 Thickness T cycled to 100cycles 3 And a capacity of Q 3 The rate of change in thickness and capacity retention of 100cycles of high temperature (60 ℃) cycling of the battery were calculated from the following equations:
high temperature (60 ℃) cycle 100cycles thickness change rate (%) = (T) 3 -T 2 )/T 2 ×100％；
High temperature (60 ℃) cycle 100cycles capacity retention (%) = Q 3 /Q 2 ×100％。
Analysis of results
The analysis results of the performance test on the lithium ion batteries assembled and sealed in the examples B1 to B4 and the comparative examples B1 to B5 are shown in Table 2, and the test results in Table 2 show that: examples B1-B4 have a much lower thickness change rate than comparative example B1 when circulating 100cycles at room temperature, and the capacity retention rates are all above 93%, and even after circulating 100cycles at high temperature (60 ℃), the thickness change rates are all below 6%; further analysis, when the lithium ion battery obtained in example B1 was compared with the lithium ion battery obtained in comparative example B1, it was found that the lithium ion battery obtained in example B1 had a thickness change rate of 100cycles at room temperature and a capacity retention rate of 3.30% and 94.35%, respectively, and had a thickness change rate (%) of 100cycles at a high temperature (60 ℃) and a capacity retention rate of 5.43% and 88.47%, respectively; on the other hand, the lithium ion battery obtained in comparative example B1 (no electrolyte additive was added to the electrolyte before and after formation) had a cycle thickness change rate of 100cycles at room temperature and a capacity retention rate of 9.37% and 84.30%, respectively, and a cycle thickness change rate (%) of 100cycles at a high temperature (60 ℃) and a capacity retention rate of 13.72% and 75.41%, respectively; the overall performance is obviously inferior to that of the lithium ion battery obtained in the example B1, which shows that, compared with the battery (comparative example B1) assembled by the electrolyte without the electrolyte additive, the battery (example 1) assembled by the electrolyte with the electrolyte additive has a smaller thickness change rate and a higher capacity retention rate, and can effectively avoid the problem of late-stage oxygen production caused by incomplete decomposition of the lithium supplement material in the formation process.
Further, comparing the performances of the lithium ion batteries obtained in the embodiments B1 and B2, the lithium ion batteries obtained in the embodiments B2 and B3, the lithium ion batteries obtained in the embodiments B3 and B4, and the lithium ion batteries obtained in the embodiments B4 and B5 respectively, it can be seen that the lithium ion batteries obtained in the embodiments B1 to B4 have a thickness change rate of 3.19-3.30% and capacity retention rates of 93.81-94.40% under a normal temperature cycle of 100 cycles; the lithium ion batteries obtained by the comparative examples B2 to B5 have the thickness change rate of 7.18 to 8.54 percent and the capacity retention rate of 89.12 to 90.27 percent; under the condition of high-temperature (60 ℃) cycle of 100cycles, the thickness change rate of the lithium ion batteries obtained in the embodiments B1 to B4 is 5.25 to 5.67 percent, and the capacity retention rate is 87.98 to 89.25 percent; the lithium ion batteries obtained by the comparative examples B2 to B5 have the thickness change rate of 11.14 to 12.35 percent and the capacity retention rate of 79.23 to 81.99 percent; it can be seen that, under the condition of circulating for 100 circles at normal temperature or circulating for 100 circles at high temperature (60 ℃), the electrolyte is added with the electrolyte additive before formation, but the lithium ion battery obtained without adding the electrolyte additive after formation has obvious thickness change and rapid battery performance attenuation, which indicates that the lithium ion battery is easy to be immediately exhausted when the electrolyte additive is added before formation and cannot relieve the problem that oxygen is easy to generate after a positive electrode lithium supplement material is added into the lithium ion battery; the electrolyte additives provided by embodiments B1 to B4 of the present application are added after formation treatment, so that the amount of oxygen generated after formation of the lithium supplement material can be effectively reduced or eliminated, thereby reducing potential safety hazards in battery use, significantly reducing the rate of change of the battery thickness, improving the capacity retention rate, facilitating improvement of the overall properties of the battery, and enabling the application of the battery to be wider.
In conclusion, the electrochemical performance of the battery containing the electrolyte additive is superior to that of the battery without the electrolyte additive at normal temperature and high temperature, and the electrolyte additive provided by the application is added after formation treatment, so that the overall property of the battery is improved, and the potential safety hazard of the battery is reduced.
TABLE 2
Figure BDA0003799726380000181
In summary, the electrolyte additive provided in the present application includes at least one of a metal oxide containing an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses the generation of oxygen; on one hand, the provided metal oxide containing oxygen defects has a certain physical adsorption effect on oxygen, and the internal crystal structure of the metal oxide containing oxygen defects can store oxygen generated by a lithium supplement agent; on the other hand, the metal oxide containing oxygen defects can react with oxygen chemically to change the metal element into a positive valence state, so as to obtain a stable product; the organic matter carrying the group capable of reacting with oxygen can directly react with oxygen, consumes peroxide generated by the lithium supplement additive and is converted into a stable inactive product; the organic matter carrying the group for inhibiting the generation of oxygen can well reduce the effect of gas generation and inhibit the generation of oxygen; in addition, as for the addition mode of the electrolyte additive, the electrolyte additive is supplemented in the electrolyte after the formation treatment, so that oxygen generated by the anode lithium supplement additive can be effectively consumed, and the problem that oxygen is easily generated after the anode lithium supplement material is added in the lithium ion battery is solved. Therefore, the electrolyte additive comprises at least one of metal oxide containing oxygen defects, organic matter carrying groups capable of reacting with oxygen and organic matter carrying groups for inhibiting oxygen generation, and can control the generation of active oxygen in the electrolyte, so that the problem that oxygen is easily generated after a positive electrode lithium supplement material is added into a lithium ion battery is solved, the overall property of the battery is improved, the potential safety hazard of the battery is reduced, and the battery is more widely applied.
The above description is only exemplary of the present application and should not be taken as limiting the present application, as any modification, equivalent replacement, or improvement made within the spirit and principle of the present application should be included in the protection scope of the present application.

Claims (11)

1. An electrolyte additive, characterized in that the electrolyte additive comprises at least one of a metal oxide containing an oxygen defect, an organic substance carrying a group capable of reacting with oxygen, and an organic substance carrying a group that suppresses the generation of oxygen.
2. The electrolyte additive of claim 1 wherein the oxygen-deficient metal oxide has the formula MO x M is a metal element and satisfies: when the valence state of M is a, x is more than 0 and less than a/2; wherein M is at least one selected from Ce, ti, mn, sn, zr, W, al, mo, fe, zn, cu, co, ni and Cr.
3. The electrolyte additive of claim 2 wherein the oxygen-deficient metal oxide is selected from the group consisting of TiO x 、CeO x Wherein 1.2 < x < 2.
4. The electrolyte additive as claimed in claim 1, wherein the organic substance having a group capable of reacting with oxygen is selected from at least one of phosphate organic substances, phosphite organic substances, phenolic antioxidants, and alcohol antioxidants; and/or the presence of a gas in the gas,
the organic matter carrying the group for inhibiting the generation of oxygen is selected from sulfonate organic matters.
5. A lithium ion battery electrolyte, characterized in that the lithium ion battery electrolyte comprises a lithium salt, an organic solvent and an electrolyte additive, wherein the electrolyte additive comprises the electrolyte additive of any one of claims 1 to 4.
6. The lithium ion battery electrolyte of claim 5, wherein the electrolyte additive is present in the lithium ion battery electrolyte in an amount of 1 to 10wt%.
7. The lithium ion battery electrolyte of claim 5, wherein the organic solvent comprises at least one of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl formate, methyl acetate, methyl propionate, ethyl acetate, 1, 3-propane sultone, adiponitrile, succinonitrile; and/or the presence of a gas in the gas,
the lithium salt comprises LiPF 6 、LiBF 4 、LiFSI、LiB(C 2 O 4 ) 2 To (3) is provided.
8. The lithium ion battery electrolyte of claim 5, wherein the mass percent of the organic solvent in the lithium ion battery electrolyte is 55-75%; and/or the presence of a gas in the gas,
in the lithium ion battery electrolyte, the mass percentage of the lithium salt is 10-30%.
9. The lithium ion battery is characterized by comprising a positive electrode, a negative electrode, a diaphragm, a first electrolyte and an electrolyte additive, wherein the lithium ion battery comprises the following components in the assembling process: assembling a positive electrode, a negative electrode, a diaphragm and a first electrolyte, carrying out formation treatment, pumping away oxygen after the formation treatment, and adding the electrolyte additive into the first electrolyte, wherein the electrolyte additive is selected from the electrolyte additive disclosed in any one of claims 1 to 4.
10. The lithium ion battery of claim 9, further comprising a second electrolyte, wherein the adding of the electrolyte additive to the first electrolyte is to mix the electrolyte additive with the second electrolyte to obtain a mixed electrolyte, and to add the mixed electrolyte to the lithium ion battery.
11. The lithium ion battery according to any one of claims 9 or 10, wherein the positive electrode comprises a lithium supplement material, and the lithium supplement material is a lithium supplement material which is easy to generate oxygen.
CN202210979196.8A 2022-08-16 2022-08-16 Electrolyte additive, lithium ion battery electrolyte and lithium ion battery Pending CN115498258A (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023206921A1 (en) * 2022-04-26 2023-11-02 惠州市豪鹏科技有限公司 Lithium-ion battery
WO2024197461A1 (en) * 2023-03-24 2024-10-03 宁德时代新能源科技股份有限公司 Use of compound as electrolyte additive, electrolyte, battery and electrical apparatus
WO2024250149A1 (en) * 2023-06-05 2024-12-12 宁德时代新能源科技股份有限公司 Secondary battery and electric device

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2023206921A1 (en) * 2022-04-26 2023-11-02 惠州市豪鹏科技有限公司 Lithium-ion battery
WO2024197461A1 (en) * 2023-03-24 2024-10-03 宁德时代新能源科技股份有限公司 Use of compound as electrolyte additive, electrolyte, battery and electrical apparatus
WO2024250149A1 (en) * 2023-06-05 2024-12-12 宁德时代新能源科技股份有限公司 Secondary battery and electric device

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