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WO2025218178A1 - Batterie rechargeable et dispositif - Google Patents

Batterie rechargeable et dispositif

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Publication number
WO2025218178A1
WO2025218178A1 PCT/CN2024/135180 CN2024135180W WO2025218178A1 WO 2025218178 A1 WO2025218178 A1 WO 2025218178A1 CN 2024135180 W CN2024135180 W CN 2024135180W WO 2025218178 A1 WO2025218178 A1 WO 2025218178A1
Authority
WO
WIPO (PCT)
Prior art keywords
secondary battery
lithium
silicon
battery according
negative electrode
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.)
Pending
Application number
PCT/CN2024/135180
Other languages
English (en)
Chinese (zh)
Inventor
马娟
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
NIO Technology Anhui Co Ltd
Original Assignee
NIO Technology Anhui Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by NIO Technology Anhui Co Ltd filed Critical NIO Technology Anhui Co Ltd
Publication of WO2025218178A1 publication Critical patent/WO2025218178A1/fr
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0088—Composites
    • H01M2300/0091—Composites in the form of mixtures
    • 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

Definitions

  • the present application relates to the field of energy storage, and in particular to a secondary battery and a device.
  • lithium-ion secondary batteries have been increasingly used in mobile phones, computers, energy storage, power tools, and electric vehicles.
  • Faster charging speeds have long been a goal for lithium-ion secondary batteries, and the development of fast-charging technology can alleviate the anxiety of electric vehicle users about recharging.
  • Lithium-ion transmission speed is an important reference indicator for fast-charging performance.
  • the electrolyte is one of the key factors affecting the transmission speed of lithium-ion charging and discharging. This is because the electrolyte is an important medium connecting the positive and negative electrodes and is a key location for lithium-ion transmission. Therefore, the research on fast-charging electrolytes is an important development direction for fast-charging batteries.
  • electrolyte additives will form a solid electrolyte interface film at the interface of the positive and negative electrodes.
  • This interface film is one of the greater resistances in the lithium ion transfer process, thereby affecting the fast charging performance of the secondary battery.
  • the electrolyte body is an important place for lithium ion transmission, and the type and content of its electrolyte additives will also affect the fast charging speed of the battery.
  • the present application provides a secondary battery and a device to solve the technical problem of slow charging speed in the prior art.
  • the secondary battery includes a fast-charging electrolyte, wherein the fast-charging electrolyte includes nitrogen-containing additives, silicon-containing and phosphorus-containing additives, thereby enabling lithium ions to be quickly transmitted in the electrolyte body, and a special solid electrolyte interface film with less resistance can be formed at the interface of the negative electrode plate, so that lithium ions can also be quickly transmitted in the interface film, thereby significantly improving the fast charging speed of the battery.
  • the fast-charging electrolyte includes nitrogen-containing additives, silicon-containing and phosphorus-containing additives, thereby enabling lithium ions to be quickly transmitted in the electrolyte body, and a special solid electrolyte interface film with less resistance can be formed at the interface of the negative electrode plate, so that lithium ions can also be quickly transmitted in the interface film, thereby significantly improving the fast charging speed of the battery.
  • the present application provides a secondary battery, which includes a positive electrode plate, a negative electrode plate and an electrolyte; the electrolyte includes a nitrogen-containing additive, a silicon-containing additive and a phosphorus-containing additive; the negative electrode plate includes a negative electrode active material layer and a solid electrolyte interface film located on the surface of the negative electrode active material layer; using an X-ray photoelectron spectrometer to test at a sputtering etching time of 0 seconds, the mass percentage content of nitrogen in the solid electrolyte interface film is a%, the mass percentage content of silicon in the solid electrolyte interface film is b%, and the mass percentage content of phosphorus in the solid electrolyte interface film is c%; wherein 6 ⁇ 0.25a+b+0.5c ⁇ 10.
  • Another aspect of the present application provides a device, which includes the secondary battery described above.
  • the secondary battery of the present application adds nitrogen-containing additives, silicon-containing and phosphorus-containing additives to the electrolyte, and controls the content of nitrogen, silicon and phosphorus in the solid electrolyte interface film (SEI film) on the surface of the negative electrode active material layer.
  • SEI film solid electrolyte interface film
  • the fast-charging electrolyte can enable lithium ions to be quickly transmitted in the electrolyte, thereby improving the fast-charging speed;
  • the control of the content of nitrogen, silicon and phosphorus in the above-mentioned SEI film improves the inorganic component ratio and structural uniformity of the SEI film, significantly reduces the transfer resistance of the SEI film to lithium ions, and thus significantly reduces the impedance of the SEI film, achieving rapid transmission of lithium ions in the SEI film, thereby significantly improving the fast-charging speed of the battery and improving the rate performance of the battery.
  • the secondary battery of the present application has at least one of the following advantages: excellent cycle performance, fast-charging performance and rate performance.
  • FIG1 is a peak spectrum of nitrogen elements in an XPS spectrum of a SEI film of a negative electrode according to one embodiment of the present application.
  • FIG2 is a peak spectrum of silicon element in the XPS spectrum of the SEI film of the negative electrode according to one embodiment of the present application.
  • FIG3 is a peak spectrum of phosphorus element in the XPS spectrum of the SEI film of the negative electrode according to one embodiment of the present application.
  • any lower limit may be combined with any upper limit to form an unspecified range; and any lower limit may be combined with other lower limits to form an unspecified range, and similarly, any upper limit may be combined with any other upper limit to form an unspecified range.
  • each individually disclosed point or single value may itself serve as a lower limit or upper limit and be combined with any other point or single value, or with other lower limits or upper limits, to form an unspecified range.
  • a list of items connected by the terms “at least one of,” “at least one of,” “at least one of,” or other similar terms may mean any combination of the listed items. For example, if items A and B are listed, the phrase “at least one of A and B” means only A; only B; or A and B. In another example, if items A, B, and C are listed, the phrase “at least one of A, B, and C” means only A; or only B; only C; A and B (excluding C); A and C (excluding B); B and C (excluding A); or all of A, B, and C.
  • Item A may contain a single component or multiple components.
  • Item B may contain a single component or multiple components.
  • Item C may contain a single component or multiple components.
  • C1-C3 alkyl includes, but is not limited to, methyl, ethyl, n-propyl, isopropyl, cyclopropyl, and the like.
  • C3-C6 alkylsilyl refers to a silicon group having 3 to 6 carbon atoms, including but not limited to trimethylsilyl and the like.
  • C2-C3 alkenyl includes, but is not limited to, ethenyl, propenyl, and the like.
  • C6-C12 aryl includes, but is not limited to, phenyl or naphthyl.
  • substituted or unsubstituted means that the functional group described after the term may or may not have a substituent.
  • substituted or unsubstituted C1-C3 alkyl refers to a C1-C3 alkyl group with a substituent or an unsubstituted C1-C3 alkyl group.
  • the number of substituents may be 1 or more, and the substituents include at least one of a halogen (e.g., fluorine), an alkyl group, or an aryl group. It should be understood that when the number of substituents is greater than 1, the substituents may be the same or different.
  • the secondary battery provided in the present application includes a positive electrode plate, a negative electrode plate and an electrolyte; the electrolyte includes a nitrogen-containing additive, a silicon-containing additive and a phosphorus-containing additive; the negative electrode plate includes a negative electrode active material layer and a solid electrolyte interface film located on the surface of the negative electrode active material layer; using an X-ray photoelectron spectrometer to test at a sputtering etching time of 0 seconds, the mass percentage content of nitrogen element in the solid electrolyte interface film is a%, the mass percentage content of silicon element in the solid electrolyte interface film is b%, and the mass percentage content of phosphorus element in the solid electrolyte interface film is c%; wherein, 6 ⁇ 0.25a+b+0.5c ⁇ 10.
  • the secondary battery of the present application adds nitrogen-containing additives, silicon-containing and phosphorus-containing additives to the electrolyte, and controls the content of nitrogen, silicon and phosphorus in the solid electrolyte interface film (SEI film) on the surface of the negative electrode active material layer.
  • SEI film solid electrolyte interface film
  • the fast-charging electrolyte can enable lithium ions to be quickly transmitted in the electrolyte, thereby improving the fast-charging speed;
  • the control of the content of nitrogen, silicon and phosphorus in the above-mentioned SEI film improves the inorganic component ratio and structural uniformity of the SEI film, significantly reduces the transfer resistance of the SEI film to lithium ions, and thus significantly reduces the impedance of the SEI film, achieving rapid transmission of lithium ions in the SEI film, thereby significantly improving the fast-charging speed of the battery and improving the rate performance of the battery.
  • the secondary battery of the present application has at least one of the following advantages: excellent cycle performance, fast-charging performance and rate performance.
  • the mass percentage content of nitrogen in the solid electrolyte interface film is a%
  • the mass percentage content of silicon in the solid electrolyte interface film is b%
  • the mass percentage content of phosphorus in the solid electrolyte interface film is c%; wherein, 6 ⁇ 0.25a+b+0.5c ⁇ 10.
  • 0.25a+b+0.5c is 6, 6.5, 7, 7.5, 8, 8.5, 9, 9.5, 10, or any value therebetween.
  • the proportions of organic and inorganic components in the SEI film can be reasonable, and while ensuring the stability of the mechanical strength of the SEI film, the SEI film can have a loose and porous structure, allowing lithium ions to quickly transport through the interface, thereby achieving rapid lithium ion transport in the SEI film.
  • the value of 0.25a+b+0.5c is too large, it will make it difficult for the SEI film to maintain a stable state, causing the electrolyte to continue to undergo side reactions, and large solid byproducts to accumulate at the SEI film interface, increasing the transmission resistance of lithium ions and thus reducing fast charging performance.
  • the value of 0.25a+b+0.5c is too small, the SEI film will be denser, and the transmission resistance of lithium ions will also increase, which will also reduce fast charging performance.
  • the mass percentage content of nitrogen element in the solid electrolyte interface film is a%, 2 ⁇ a ⁇ 13.
  • a is 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13 or any value therebetween.
  • 4 ⁇ a ⁇ 8 is a loose, porous and stable SEI membrane interface structure.
  • a value is too large (for example, more LiFSI)
  • it will induce more side reactions in the current collector, forming by-product accumulation, which hinders the transfer of lithium ions.
  • the a value is too small (for example, less LiFSI)
  • the transmission resistance of lithium ions in the electrolyte body will increase, reducing the fast charging speed.
  • the mass percentage content of silicon element in the solid electrolyte interface film is b%, and 0.01 ⁇ b ⁇ 4.
  • b is 0.01, 0.1, 0.5, 1, 2, 3, 4 or any value therebetween.
  • the mass percentage content of phosphorus element in the solid electrolyte interface membrane is c%, and 0.01 ⁇ c ⁇ 15.
  • c is 0.01, 0.1, 0.5, 1, 2, 3, 4, 6, 8, 10, 12, 15 or any value therebetween.
  • the nitrogen-containing additive includes a fluorinated lithium sulfonyl imide
  • the fluorinated lithium sulfonyl imide includes at least one of lithium bis(fluorosulfonyl)imide (LiFSI), lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), lithium (fluorosulfonyl)(trifluoromethylsulfonyl)imide, lithium (fluorosulfonyl)(perfluorobutylsulfonyl)imide, lithium (trifluoromethylsulfonyl)(perfluorobutylsulfonyl)imide (LiFNFSI), and lithium bis(pentafluoroethylsulfonyl)imide (LiBETI).
  • the fluorinated lithium sulfonyl imide is a lithium imide salt with nitrogen as the central atom, which can improve the fast charging performance
  • the nitrogen-containing additive includes lithium bis(fluorosulfonyl)imide (LiFSI). Due to the large anionic radius of LiFSI, it is easier to dissociate into lithium ions, which can significantly improve the conductivity of the battery, thereby improving the fast charging performance of the battery, and at the same time, it can also improve the rate performance, safety, and high-temperature cycling stability of the secondary battery.
  • LiFSI lithium bis(fluorosulfonyl)imide
  • the weight percentage of the nitrogen-containing additive is 3% to 15% based on the weight of the electrolyte. In some embodiments, the weight percentage of the nitrogen-containing additive is 3%, 4%, 5%, 7%, 9%, 10%, 12%, 15%, or any value therebetween. In some embodiments, the weight percentage of the nitrogen-containing additive is 5% to 10%.
  • the silicon-containing and phosphorus-containing additives include at least one of the compounds represented by Formula I and Formula II:
  • R 3 , R 4 , R 5 , R 6 , R 7 , and R 8 are each independently selected from a substituted or unsubstituted C1-C3 alkyl group, a substituted or unsubstituted C3-C6 alkylsilyl group, a substituted or unsubstituted C2-C3 alkenyl group, or a substituted or unsubstituted C6-C12 aryl group; wherein Formula I contains at least one substituted or unsubstituted C3-C6 alkylsilyl group, and Formula II contains at least one substituted or unsubstituted C3-C6 alkylsilyl group, and the substituents are each independently selected from fluorine.
  • Formula I represents a silicon-containing phosphate additive
  • Formula II represents a silicon-containing phosphite additive.
  • the phosphorus-containing additive can reduce the interfacial impedance between the positive and negative electrodes, thereby improving battery power performance.
  • using a nitrogen-containing additive in conjunction with the silicon- and phosphorus-containing additives can further enhance the stability of the SEI film, improving the cycle performance and rate capability of the secondary battery.
  • the silicon- and phosphorus-containing additive includes at least one of tris(trimethylsilyl)phosphate (TMSP) and tris(trimethylsilyl)phosphite (TMSPi). In some embodiments, the silicon- and phosphorus-containing additive includes tris(trimethylsilyl)phosphate (TMSP). This can further enhance the stability of the SEI film and improve the cycling performance of the battery.
  • TMSP tris(trimethylsilyl)phosphate
  • TMSPi tris(trimethylsilyl)phosphite
  • the weight percentage of the silicon-containing and phosphorus-containing additives is 0.01% to 2% based on the weight of the electrolyte. In some embodiments, the weight percentage of the silicon-containing and phosphorus-containing additives is 0.01%, 0.1%, 0.3%, 0.5%, 0.7%, 0.9%, 1%, 1.1%, 1.3%, 1.5%, 1.7%, 1.9%, 2%, or any value therebetween. In some embodiments, the weight percentage of the phosphorus-containing additive is 0.5% to 2%.
  • the solid electrolyte interface film is a non-artificial film.
  • the solid electrolyte interface film (SEI film) is formed by a solid product generated by a reaction of specific components in the electrolyte at a specific voltage.
  • the nitrogen in the solid electrolyte interface film comes from a nitrogen-containing additive, and the silicon and phosphorus in the solid electrolyte interface film come from silicon- and phosphorus-containing additives.
  • the mass percentage contents of nitrogen, silicon, and phosphorus in the solid electrolyte interface film refer to the mass percentage contents of the corresponding elements measured on the surface of the negative electrode active material layer using an X-ray photoelectron spectrometer at a sputtering etching time of 0 seconds.
  • the electrolyte further comprises a first additive comprising at least one of a cyclic carbonate containing a carbon-carbon double bond, a fluorine-containing cyclic carbonate, a fluorine-containing phosphate, and an oxalate borate.
  • the first additive comprises at least one of vinylene carbonate (VC), fluoroethylene carbonate (FEC), lithium difluorophosphate (LiDFP), lithium difluorooxalatoborate (LiDFOB), and lithium dioxalatoborate (LiBOB).
  • the weight percentage of the first additive is 0.05% to 10% based on the weight of the electrolyte. In some embodiments, the weight percentage of the first additive is 0.05%, 0.5%, 1%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 7%, 8%, 9%, 10%, or any value therebetween. In some embodiments, the weight percentage of the first additive is 0.1% to 5%.
  • the electrolyte further includes a lithium salt
  • the lithium salt includes at least one of lithium hexafluorophosphate (LiPF 6 ), lithium tetrafluoroborate (LiBF 4 ), lithium trifluorosulfonyl (LiTf), and lithium bis(fluoromalonate)borate (LiBFMB).
  • the weight percentage content of the lithium salt is 0.05% to 20% based on the weight of the electrolyte. In some embodiments, the weight percentage content of the lithium salt is 0.05%, 0.5%, 1%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, or any value therebetween. In some embodiments, the weight percentage content of the lithium salt is 1% to 15%.
  • the electrolyte further includes a solvent
  • the solvent includes at least one of a linear carbonate, a cyclic carbonate, and a carboxylate.
  • the linear carbonate is selected from at least one of dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), diethyl carbonate, dipropyl carbonate, methylpropyl carbonate, ethylpropyl carbonate and fluorinated linear carbonate.
  • the cyclic carbonate includes at least one of ethylene carbonate (EC), propylene carbonate and butylene carbonate.
  • the carboxylate is selected from at least one of methyl formate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, gamma-butyrolactone and fluorinated carboxylate.
  • the mass percentage content of the solvent is 0.05% to 80% based on the mass of the electrolyte. In some embodiments, the mass percentage content of the solvent is 0.05%, 0.5%, 1%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80% or any value therebetween. In some embodiments, the mass percentage content of the solvent is 20% to 70%.
  • the positive electrode sheet includes a positive electrode active material layer, the positive electrode active material layer includes a positive electrode active material, and the positive electrode active material includes lithium nickel transition metal oxide.
  • the lithium nickel transition metal oxide includes at least one of LiNi x M 1-x O 2 , where M includes at least one of cobalt, manganese, iron, chromium, titanium, zinc, vanadium, aluminum, zirconium, cerium, magnesium, calcium, molybdenum, strontium, tungsten, yttrium, lanthanum, silver, niobium, copper, and barium, and 0.7 ⁇ x ⁇ 0.98.
  • all transition metal elements in the positive electrode active material include transition element nickel (Ni) and other transition elements M.
  • the molar percentage content of nickel is based on the total molar amount of all transition metal elements (including transition element Ni and other transition elements M) in the positive electrode active material.
  • x is 0.7, 0.72, 0.74, 0.76, 0.78, 0.8, 0.82, 0.84, 0.86, 0.88, 0.9, 0.92, 0.94, 0.96, 0.98, or any value therebetween.
  • the positive electrode active material includes at least one of lithium nickel oxide, lithium nickel cobalt aluminum oxide, lithium nickel cobalt manganese oxide, lithium nickel manganese cobalt magnesium oxide, and lithium nickel manganese oxide.
  • the positive electrode active material layer further includes a binder, and optionally a conductive material.
  • the binder improves the bonding between the positive electrode active material particles and also improves the bonding between the positive electrode active material and the current collector.
  • the binder includes: polyvinylidene fluoride (PVDF), polyacrylonitrile (PAN), polyacrylic acid (PAA), polymethyl methacrylate (PMMA), polyimide (PI), polyvinyl alcohol, hydroxypropyl cellulose, diacetyl cellulose, polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, polymers containing ethylene oxide, polyvinyl pyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene 1,1-difluoride, polyethylene, polypropylene, styrene-butadiene rubber, acrylated styrene-butadiene rubber, epoxy resin or nylon, etc.
  • PVDF polyvinylidene fluoride
  • PAN polyacrylonitrile
  • PAA polyacrylic acid
  • PMMA polymethyl methacrylate
  • PI polyimide
  • polyvinyl alcohol hydroxypropyl cellulose
  • the conductive material includes: a carbon-based material, a metal-based material, a conductive polymer, and mixtures thereof.
  • the carbon-based material is selected from natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, carbon fiber, or any combination thereof.
  • the metal-based material is selected from metal powder, metal fiber, copper, nickel, aluminum, or silver.
  • the conductive polymer is a polyphenylene derivative.
  • the positive electrode sheet further includes a positive electrode current collector, which can be a metal foil or a composite current collector.
  • a positive electrode current collector can be a metal foil or a composite current collector.
  • aluminum foil can be used.
  • the composite current collector can be obtained by forming a metal material (copper, copper alloy, nickel, nickel alloy, titanium, titanium alloy, silver, silver alloy, etc.) on a polymer substrate.
  • the negative electrode sheet includes a negative electrode active material layer and a solid electrolyte interface film located on a surface of the negative electrode active material layer.
  • the negative electrode active material layer includes a negative electrode active material
  • the negative electrode active material includes a mixture of a silicon-based material and at least one material selected from a carbon-based material, a tin-based material, a phosphorus-based material, and metallic lithium.
  • the silicon-based material comprises at least one of silicon, a silicon alloy, a silicon oxide, and a silicon carbon compound.
  • the carbon-based material comprises at least one of graphite, soft carbon, hard carbon, carbon nanotubes, and graphene.
  • the tin-based material comprises at least one of tin, a tin oxide, and a tin alloy.
  • the phosphorus-based material comprises phosphorus and/or a phosphorus complex.
  • the mass percentage of the silicon-based material is 3% to 40% based on the mass of the negative electrode active material. In some embodiments, the mass percentage of the silicon-based material is 3%, 5%, 8%, 10%, 12%, 15%, 18%, 20%, 25%, 30%, 35%, 40%, or any value therebetween.
  • the negative electrode active material layer further comprises a binder and a conductive agent.
  • the binder comprises styrene-butadiene rubber (SBR), sodium carboxymethyl cellulose (CMC), polyacrylic acid (PAA), polyvinyl alcohol, hydroxypropyl cellulose, diacetyl cellulose, polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, polymers containing ethylene oxide, polyvinyl pyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, acrylated styrene-butadiene rubber, epoxy resin, or nylon.
  • SBR styrene-butadiene rubber
  • CMC sodium carboxymethyl cellulose
  • PAA polyacrylic acid
  • polyvinyl alcohol hydroxypropyl cellulose
  • diacetyl cellulose polyvinyl chloride
  • the conductive agent includes: a carbon-based material, a metal-based material, a conductive polymer, and mixtures thereof.
  • the carbon-based material is selected from natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, carbon fiber, or any combination thereof.
  • the metal-based material is selected from metal powder, metal fiber, copper, nickel, aluminum, or silver.
  • the conductive polymer is a polyphenylene derivative.
  • the negative electrode plate further includes a negative electrode current collector
  • the negative electrode current collector includes: copper foil, nickel foil, stainless steel foil, titanium foil, nickel foam, copper foam, a polymer substrate coated with a conductive metal, or any combination thereof.
  • a separator is provided between the positive and negative electrode plates to prevent short circuits.
  • the material and shape of the separator that can be used in the embodiments of the present application are not particularly limited and can be any known prior art material.
  • the separator comprises a polymer or inorganic material that is stable with the electrolyte of the present application.
  • the separator may include a substrate layer and a surface treatment layer.
  • the substrate layer is a non-woven fabric, film, or composite film having a porous structure
  • the material of the substrate layer includes at least one of polyethylene, polypropylene, polyethylene terephthalate, or polyimide.
  • polypropylene porous film, polyethylene porous film, polypropylene non-woven fabric, polyethylene non-woven fabric, or polypropylene-polyethylene-polypropylene porous composite film can be used.
  • a surface treatment layer is provided on at least one surface of the substrate layer.
  • the surface treatment layer may be a polymer layer or an inorganic layer, or a layer formed by mixing a polymer and an inorganic layer.
  • the inorganic layer includes inorganic particles and a binder, wherein the inorganic particles include at least one of aluminum oxide, silicon oxide, magnesium oxide, titanium oxide, hafnium dioxide, tin oxide, cerium dioxide, nickel oxide, zinc oxide, calcium oxide, zirconium oxide, yttrium oxide, silicon carbide, boehmite, aluminum hydroxide, magnesium hydroxide, calcium hydroxide, or barium sulfate.
  • the binder includes at least one of polyvinylidene fluoride, a copolymer of vinylidene fluoride and hexafluoropropylene, polyamide, polyacrylonitrile, polyacrylate, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polymethyl methacrylate, polytetrafluoroethylene, or polyhexafluoropropylene.
  • the polymer layer includes a polymer, and the polymer material includes at least one of polyamide, polyacrylonitrile, acrylate polymer, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polyvinylidene fluoride or poly(vinylidene fluoride-hexafluoropropylene).
  • the method for preparing the secondary battery includes providing an electrode assembly, injecting liquid, packaging, and forming.
  • the forming temperature is 40° C. to 50° C., for example, 41° C., 42° C., 43° C., 44° C., 45° C., 46° C., 47° C., 48° C., or 49° C.
  • the formation comprises: charging to 4.25V at 0.05C current and standing for 60min, then charging to 4.25V at 0.1C current, and then discharging to 3.0V at 0.2C current under the conditions of a temperature of 40°C-50°C, for example, 45°C, and a pressure of 150kgf-250kgf, for example, 210kgf.
  • the secondary battery is formed.
  • the solid electrolyte interface membrane is formed after the secondary battery is formed.
  • nitrogen-containing additives, silicon-containing additives, and phosphorus-containing additives are reduced on the surface of the negative electrode active material to form an SEI film.
  • the absolute content of nitrogen, silicon, and phosphorus in the SEI film will be different from the absolute content of nitrogen, silicon, and phosphorus in the SEI film after formation, but the relative content, that is, the mass percentage of nitrogen, silicon, and phosphorus in the SEI film, will still be between 2% and 12%, between 0.01% and 4%, and between 0.01% and 15%, respectively.
  • the secondary battery is a lithium secondary battery or a sodium secondary battery.
  • the lithium secondary battery includes: a lithium metal secondary battery, a lithium ion secondary battery, a lithium polymer secondary battery, or a lithium ion polymer secondary battery.
  • the secondary battery may include an outer packaging, which may be a hard shell, such as a hard plastic shell, an aluminum shell, a steel shell, etc.
  • the outer packaging of the secondary battery may also be a soft package, such as a bag-type soft package.
  • the material of the soft package may be plastic, such as one or more of polypropylene (PP), polybutylene terephthalate (PBT), polybutylene succinate (PBS), etc.
  • the shape of the secondary battery is not particularly limited, and it can be cylindrical, square, or any other shape.
  • the present application also provides a battery module.
  • the battery module includes the aforementioned secondary battery.
  • the battery module of the present application utilizes the aforementioned secondary battery and therefore has at least the same advantages as the aforementioned secondary battery.
  • the battery module of the present application may include multiple secondary batteries, the specific number of which can be adjusted based on the application and capacity of the battery module.
  • the present application further provides a battery pack comprising the above-mentioned battery module.
  • the number of battery modules contained in the battery pack can be adjusted according to the application and capacity of the battery pack.
  • the present application also provides a device, which includes the secondary battery.
  • the device includes an electric vehicle, a hybrid electric vehicle, a plug-in hybrid electric vehicle, a power storage system, etc.
  • a battery pack or battery module may be used.
  • the device may be a mobile phone, a tablet computer, a laptop computer, etc.
  • the device is generally required to be lightweight and thin, and may use a secondary battery as a power source.
  • conductive agent acetylene black binder styrene-butadiene rubber SBR
  • thickener sodium carboxymethyl cellulose CMCNa thickener sodium carboxymethyl cellulose CMCNa
  • PAA polyacryl
  • Diaphragm PP/PE/PP (polypropylene/polyethylene/polypropylene) three-layer composite diaphragm.
  • Preparation of lithium-ion secondary batteries The positive electrode sheet, separator (PP/PE/PP three-layer composite film), and negative electrode sheet prepared above are overlapped in sequence, with the separator located between the positive electrode sheet and the negative electrode sheet, and wound to obtain a bare cell. After the bare cell is fully dried, it is placed in a cylindrical (e.g., 18650 cylindrical) steel shell, and then the electrolyte prepared above is injected and sealed.
  • a cylindrical e.g., 18650 cylindrical
  • the battery undergoes pre-charging, high-temperature infiltration, formation (formation conditions are: temperature 45°C, 0.05C current charging to 3V and then standing for 5 minutes, then 0.1C charging to 3.5V and standing for 5 minutes, and then 0.33C charging to 4.0V) and high-temperature aging, and then regular capacity distribution is performed.
  • Examples 2 to 7 and Comparative Examples 1 to 3 are achieved by adjusting the types and contents of lithium salts, solvents, and additives in the electrolyte on the basis of Example 1. Specific adjustment measures and detailed data are shown in Table 1.
  • XPS X-ray photoelectron spectrometer
  • the lithium-ion battery was discharged at a current of 0.1C to 2.5V.
  • the battery was then disassembled in an argon-filled glove box to obtain the electrode sheets.
  • the resulting electrode sheets were cut into 8mm x 8mm test samples and soaked and cleaned in a low-boiling-point dimethyl carbonate (DMC) solvent for half an hour. After complete drying, they were attached to the XPS sample stage with the surface of the negative electrode active material layer facing away from the current collector facing upward. Measurements were performed without exposure to the atmosphere.
  • DMC dimethyl carbonate
  • the mass percentage content of nitrogen, silicon, and phosphorus in the negative electrode SEI film can be obtained by the above-mentioned test method. More specifically, Figures 1 to 3 are the XPS spectra of nitrogen, silicon, and phosphorus obtained by testing the negative electrode SEI film in Example 1. The peak areas in the spectra are integrated to obtain the peak area of each element, and the mass percentage content of the corresponding element is obtained by normalizing the peak area of each element.
  • this fast-charging electrolyte enables rapid lithium ion transport within the electrolyte, thereby increasing the fast-charging speed. Furthermore, by controlling the content of nitrogen, silicon, and phosphorus in the SEI film, the inorganic component ratio and structural uniformity of the SEI film are increased, significantly reducing the SEI film's resistance to lithium ion transfer, and thus significantly reducing the SEI film's impedance, enabling rapid lithium ion transport within the SEI film, thereby significantly increasing the battery's fast-charging speed and improving the battery's rate performance. Based on the above improvements, the secondary battery of the present application has at least one of the following advantages: excellent fast-charging performance and rate performance.

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Abstract

La présente demande se rapporte à une batterie rechargeable et à un dispositif. La batterie rechargeable de la présente demande comprend une feuille d'électrode positive, une feuille d'électrode négative et une solution électrolytique ; la solution électrolytique comprend un additif contenant de l'azote et un additif contenant du silicium et contenant du phosphore ; la feuille d'électrode négative comprend une couche de matériau actif d'électrode négative et un film d'interface d'électrolyte solide situé sur la surface de la couche de matériau actif d'électrode négative ; par test à un temps de gravure par pulvérisation de 0 seconde à l'aide d'un spectromètre photoélectronique à rayons X, la teneur en pourcentage en masse d'un élément azote dans le film d'interface d'électrolyte solide est a %, la teneur en pourcentage en masse d'un élément de silicium dans le film d'interface d'électrolyte solide est b %, et la teneur en pourcentage en masse d'un élément de phosphore dans le film d'interface d'électrolyte solide est c %, 5,5 ≤ 0,25 a + b + 0,5 c ≤ 10. Ainsi, la batterie rechargeable de la présente demande présente d'excellentes performance de cycle, performance de charge rapide et performance de vitesse.
PCT/CN2024/135180 2024-04-18 2024-11-28 Batterie rechargeable et dispositif Pending WO2025218178A1 (fr)

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CN118539005A (zh) * 2024-04-18 2024-08-23 蔚来汽车科技(安徽)有限公司 二次电池和装置
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CN110265717A (zh) * 2019-06-15 2019-09-20 松山湖材料实验室 高压锂离子电池电解液及其电池
CN116487706A (zh) * 2023-06-19 2023-07-25 蔚来电池科技(安徽)有限公司 二次电池和装置
CN118539005A (zh) * 2024-04-18 2024-08-23 蔚来汽车科技(安徽)有限公司 二次电池和装置

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CN110265717A (zh) * 2019-06-15 2019-09-20 松山湖材料实验室 高压锂离子电池电解液及其电池
CN116487706A (zh) * 2023-06-19 2023-07-25 蔚来电池科技(安徽)有限公司 二次电池和装置
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