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WO2018120787A1 - Électrolyte et batterie rechargeable - Google Patents

Électrolyte et batterie rechargeable Download PDF

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Publication number
WO2018120787A1
WO2018120787A1 PCT/CN2017/093744 CN2017093744W WO2018120787A1 WO 2018120787 A1 WO2018120787 A1 WO 2018120787A1 CN 2017093744 W CN2017093744 W CN 2017093744W WO 2018120787 A1 WO2018120787 A1 WO 2018120787A1
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WO
WIPO (PCT)
Prior art keywords
chloro
group
electrolyte
ethyl
secondary battery
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.)
Ceased
Application number
PCT/CN2017/093744
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English (en)
Chinese (zh)
Inventor
王小梅
付成华
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.)
Contemporary Amperex Technology Co Ltd
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Contemporary Amperex Technology Co Ltd
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Filing date
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Publication of WO2018120787A1 publication Critical patent/WO2018120787A1/fr
Anticipated expiration legal-status Critical
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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
    • H01M10/056—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
    • H01M10/05—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
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • 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 invention relates to the field of battery technologies, and in particular, to an electrolyte and a secondary battery.
  • a widely used electrolyte for a lithium ion secondary battery includes a lithium hexafluorophosphate as a conductive lithium salt and a mixture of a cyclic carbonate and a chain carbonate as an organic solvent, but the above electrolyte still has many disadvantages, particularly At high voltages, lithium ion secondary batteries have poor performance, such as poor high temperature cycle performance, poor high temperature storage performance, and poor rate performance.
  • an object of the present invention is to provide an electrolyte and a secondary battery, which can simultaneously improve the rate performance of a secondary battery at a high temperature and a high voltage when the electrolyte is applied to a secondary battery. , loop performance and storage performance.
  • the present invention provides an electrolyte comprising an electrolyte salt, an organic solvent, and an additive.
  • the organic solvent includes a carboxylate compound.
  • the additives include cyclic sulfates and triphenyl phosphite.
  • the invention provides a secondary battery comprising an electrolyte according to an aspect of the invention.
  • the electrolyte of the present invention includes a carboxylate compound, a cyclic sulfate, and a triphenyl phosphite.
  • a carboxylate compound When applied to a secondary battery, the synergistic action of the three can simultaneously increase the secondary battery at a high temperature. Rate performance, cycle performance, and storage performance at voltage.
  • the electrolytic solution according to the first aspect of the invention includes: an electrolyte salt, an organic solvent, and an additive.
  • the organic solvent includes a carboxylate compound.
  • the additives include cyclic sulfates and triphenyl phosphite.
  • the carboxylate compound is used for improving the rate performance of the secondary battery, but when the carboxylate compound is applied to a secondary battery of a high voltage system, it is easily oxidized.
  • the secondary battery using the carboxylic acid ester compound is decomposed and used in a high-temperature environment, the capacity loss after repeated cycles of the secondary battery is severe, and the high-temperature storage performance of the secondary battery is seriously deteriorated.
  • the cyclic sulfate has a high reduction potential, and can preferentially form a film on the surface of the negative electrode to suppress reduction of the carboxylate compound, thereby improving the cycle performance of the secondary battery.
  • Triphenyl phosphite can react with HF to reduce the HF, thereby improving the high-temperature storage performance of the secondary battery.
  • the electrolyte includes three substances at the same time, under the synergistic action of the three, the rate performance, cycle performance and storage performance of the secondary battery at high temperature and high voltage can be simultaneously improved.
  • the carboxylic acid ester compound is selected from one or more of the compounds represented by the formula I.
  • R 1 and R 2 are each independently selected from the group consisting of an alkane group having 1 to 10 carbon atoms and a halogenated alkane group having 1 to 10 carbon atoms; and the halogen atom in the halogenated alkane group is selected from the group consisting of F and Cl.
  • the alkane group having 1 to 10 carbon atoms may be a chain alkane group or a cyclic alkane group.
  • the chain alkane group further includes a linear alkane group and a branched alkane group.
  • the cyclic alkane group may have a substituent or may not contain a substituent.
  • a preferred lower limit of the number of carbon atoms may be 1, 2, and 3, and a preferred upper limit of the number of carbon atoms may be 4, 5, 6, 7, 8, or 10.
  • R 1 and R 2 are each independently selected from a chain alkane group having 1 to 6 carbon atoms or a cyclic alkane group having 3 to 8 carbon atoms. Still more preferably, R 1 and R 2 are each independently selected from a chain alkane group having 1 to 4 carbon atoms or a cyclic alkane group having 5 to 7 carbon atoms.
  • the alkane group having 1 to 10 carbon atoms may be selected from the group consisting of methyl, ethyl, n-propyl, isopropyl, cyclopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, Cyclobutyl, n-pentyl, isopentyl, tert-amyl, neopentyl, cyclopentyl, 2,2 dimethylpropyl, 1-ethylpropyl, 1-methylbutyl, 2-methyl Butyl, n-hexyl, isohexyl, 2-hexyl, 3-hexyl, cyclohexyl, 2-methylpentyl, 3-methylpentyl, 1,1,2-trimethylpropyl, 3,3 - dimethylbutyl, n-heptyl, 2-heptyl, 3-heptyl, 2-methylhexyl, 3-methylhexyl,
  • the number of substitution of the halogen atom in the halogenated alkane group having 1 to 10 carbon atoms and the position of substitution thereof are not particularly limited, and may be selected according to actual needs.
  • the number of halogen atoms may be one, two, three or four.
  • the types of the halogen atoms may be the same, or they may be completely different or partially the same.
  • the haloalkane group may be a chain haloalkane group or a cyclic haloalkane group.
  • the chain haloalkane group in turn includes a linear haloalkane group and a branched haloalkane group.
  • the cyclic haloalkane group may or may not have a substituent.
  • a preferred lower limit of the number of carbon atoms may be 1, 2, and 3, and a preferred upper limit of the number of carbon atoms may be 4, 5, 6, 7, 8, or 10.
  • R 1 and R 2 are each independently selected from a chain halogenated alkane group having 1 to 6 carbon atoms or a cyclic halogenated alkane group having 3 to 8 carbon atoms. Still more preferably, each of R 1 and R 2 is independently selected from a chain halogenated alkane group having 1 to 4 carbon atoms or a cyclic halogenated alkane group having 5 to 7 carbon atoms.
  • the halogenated alkane group having 1 to 10 carbon atoms is selected from the group consisting of chloromethyl, dichloromethyl, trichloromethyl, 1-chloroethyl, 1,2-dichloroethyl, 2-chloro-n-propyl , 2,2-dichloro-n-propyl, 1-chloroisopropyl, monochlorocyclopropyl, 1-chloro-n-butyl, 2-chloroisobutyl, monochlorocyclobutyl, 1-chloro-n-pentane Base, 2-chloro-n-pentyl, 1-chloroisopentyl, 2,2-dichloromethylpropyl, monochlorocyclopentyl, 3-chloro-2,2-dimethylpropyl, 1-chloro 1-ethylpropyl, 1-chloro-1-methylbutyl, 2-chloro-2-methylbutyl, 2-chloro-n-hexy
  • the carboxylic acid ester compound may be selected from the group consisting of methyl formate, ethyl formate, ethyl acetate, ethyl propionate, ethyl valerate, and ethyl isovalerate.
  • the cyclic sulfate is selected from one or more of the compounds represented by the formula II.
  • n is an integer within 1 to 3; and R 3 , R 4 , R 5 and R 6 are each independently selected from the group consisting of H, F, Cl, Br, I, an alkyl group having 1 to 10 carbon atoms, and a carbon atom.
  • One of the alkoxy groups having 1 to 10, wherein the H on the alkyl group or the alkoxy group may be substituted with one or more of F, Cl, Br, and I.
  • the cyclic sulfate is selected from one or more of the following compounds;
  • the triphenyl phosphite structure is as follows:
  • the volume of the carboxylate compound is 5% to 50% of the total volume of the organic solvent.
  • the volume of the carboxylic acid ester compound is from 10% to 40% of the total volume of the organic solvent.
  • the volume of the carboxylate compound is from 20% to 35% of the total volume of the organic solvent.
  • the content of the cyclic sulfate is 0.5% to 10% of the total weight of the electrolytic solution.
  • the cyclic sulfate is present in an amount of from 1% to 5% by weight based on the total weight of the electrolyte.
  • the content of the triphenyl phosphite is 0.03% to 1% of the total weight of the electrolytic solution.
  • the content of the triphenyl phosphite is from 0.1% to 0.3% of the total weight of the electrolyte.
  • the specific kind of the organic solvent is not particularly limited and may be selected according to actual needs.
  • a non-aqueous organic solvent is used.
  • the organic solvent may also include halogenated compounds of any kind of carbonates and carbonates.
  • the carbonate includes a cyclic carbonate and a chain carbonate.
  • the organic solvent may further include ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate, pentylene carbonate, fluoroethylene carbonate, dimethyl carbonate, and diethyl carbonate.
  • EC ethylene carbonate
  • PC propylene carbonate
  • butylene carbonate pentylene carbonate
  • fluoroethylene carbonate dimethyl carbonate
  • diethyl carbonate diethyl carbonate
  • ester DEC
  • dipropyl carbonate dipropyl carbonate
  • ethyl methyl carbonate ⁇ -butyrolactone
  • tetrahydrofuran tetrahydrofuran.
  • the electrolyte salt may be selected from a lithium salt, a sodium salt or a zinc salt, which varies depending on the secondary battery to which the electrolyte is applied.
  • the content of the electrolyte salt is 6.2% to 25% of the total weight of the electrolytic solution.
  • the content of the electrolyte salt is 6.25% to 18.8% of the total weight of the electrolyte.
  • the content of the electrolyte salt is 10% to 15% of the total weight of the electrolyte.
  • the electrolyte in the present application can be prepared by a conventional method, that is, the materials in the electrolyte are uniformly mixed.
  • a secondary battery according to a second aspect of the invention includes the electrolytic solution according to the first aspect of the invention.
  • the secondary battery further includes a positive electrode sheet, a negative electrode sheet, and a separator.
  • the positive electrode sheet includes a positive electrode current collector and a positive electrode active slurry layer on the positive electrode current collector, wherein the positive electrode active slurry layer includes a positive electrode active layer material.
  • the specific type of the positive electrode active material is not particularly limited and can be selected according to requirements.
  • the negative electrode sheet includes a negative electrode current collector and a negative electrode active slurry layer on the negative electrode current collector.
  • the negative active slurry layer includes a negative active material.
  • the specific type of the negative active material is not particularly limited and can be selected according to requirements.
  • the specific type of the separator is not affected
  • a specific limitation may be any separator material used in the existing secondary battery, such as polyethylene, polypropylene, polyvinylidene fluoride, and a multilayer composite film thereof, but is not limited thereto.
  • the secondary battery may be a lithium ion secondary battery, a sodium ion secondary battery, or a zinc ion secondary battery.
  • the positive electrode active material is selected from lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), olivine-type lithium iron phosphate (LiFePO 4 ), Olivine-type LiMPO 4 , spinel-type LiMn 2 O 4 , ternary cathode material LiNi x A y B (1-xy) O 2 and Li 1-x' (A' y' B' z' C 1 -y'-z' ) One or several of O 2 .
  • M is selected from one or more of Co, Ni, Fe, Mn, V; A and B are each independently selected from one of Co, Al, and Mn, and A and B are not the same; 0 ⁇ x ⁇ 1,0 ⁇ y ⁇ 1 and x+y ⁇ 1;0 ⁇ x' ⁇ 1,0 ⁇ y' ⁇ 1,0 ⁇ z' ⁇ 1 and y'+z' ⁇ 1;A',B', C is each independently selected from one of Co, Ni, Fe, and Mn, and A', B', and C are different.
  • the negative active material may be selected from metallic lithium, and the negative active material may also be selected from materials capable of intercalating lithium when the electrode potential of the Li/Li + equilibrium potential is ⁇ 2V.
  • the anode active material is selected from the group consisting of natural graphite, artificial graphite, mesophase micro carbon spheres (abbreviated as MCMB), hard carbon, soft carbon, silicon, silicon-carbon composite, Li-Sn alloy, Li-Sn- One or more of an O alloy, Sn, SnO, SnO 2 , a lithiated lithiated TiO 2 -Li 4 Ti 5 O 12 , Li-Al alloy.
  • the electrolyte salt may be a lithium salt, and the lithium salt may be selected from LiPF 6 , LiBF 4 , LiN(SO 2 F) 2 (abbreviated as LiFSi), LiN(CF 3 SO 2 ) 2 (abbreviated as LiTFSi), LiClO. 4 , one or more of LiAsF 6 , LiB(C 2 O 4 ) 2 (abbreviated as LiBOB), LiBF 2 C 2 O 4 (abbreviated as LiDFOB), and LiPO 2 F 2 .
  • LiPF 6 LiBF 4
  • LiN(SO 2 F) 2 abbreviated as LiFSi
  • LiTFSi LiN(CF 3 SO 2 ) 2
  • LiClO. 4 LiClO. 4
  • LiAsF 6 LiB(C 2 O 4 ) 2
  • LiBOB LiBF 2 C 2 O 4
  • LiDFOB LiBF 2 C 2 O 4
  • the lithium ion secondary batteries of Examples 1 to 11 and Comparative Examples 1 to 7 were each prepared in the following manner.
  • the positive electrode active material lithium cobaltate (LiCoO 2 ), the binder polyvinylidene fluoride, and the conductive agent acetylene black were mixed at a weight ratio of 98:1:1, and N-methylpyrrolidone (NMP) was added thereto under the action of a vacuum mixer.
  • NMP N-methylpyrrolidone
  • the negative electrode active material artificial graphite, thickener sodium carboxymethyl cellulose (CMC), binder styrene-butadiene rubber were mixed at a weight ratio of 98:1:1, deionized water was added, and the negative electrode slurry was obtained under the action of a vacuum mixer.
  • the negative electrode slurry was uniformly coated on a negative electrode current collector copper foil having a thickness of 8 ⁇ m; the copper foil was air-dried at room temperature, transferred to an oven at 120 ° C for 1 hour, and then subjected to cold pressing and slitting to obtain a negative electrode sheet.
  • the content of the carboxylate compound is a volume percentage calculated based on the total volume of the organic solvent
  • the content of the cyclic sulfate and the triphenyl phosphite is a weight percentage calculated based on the total weight of the electrolyte.
  • a 16 ⁇ m thick polypropylene separator (model A273, supplied by Celgard) was used.
  • the positive electrode sheet, the separator film and the negative electrode sheet are stacked in order, so that the separator is in a role of isolation between the positive and negative electrode sheets, and then wound to obtain a bare cell; the bare cell is placed in the outer packaging foil, The prepared electrolyte solution is injected into the dried bare cell, and subjected to vacuum encapsulation, standing, formation, shaping, and the like to obtain a lithium ion secondary battery.
  • the lithium ion secondary battery was charged at a constant current of 1 C (nominal capacity) to a voltage of 4.4 V at 25 ° C, and then charged at a constant voltage of 4.4 V until the current was less than or equal to 0.05 C. After leaving for 5 minutes, the constant current was discharged at 0.2 C. The electric current is up to the voltage of 3V, and the discharge capacity at this time is recorded as D0.
  • the lithium ion secondary battery is charged at a constant current of 1 C to a voltage of 4.4 V, and then charged at a constant voltage of 4.4 V until the current is less than or equal to 0.05 C. After being left for 5 minutes, the battery is discharged at a constant current of 2 C to a voltage of 3 V, and the discharge is performed at this time. The capacity is recorded as D1.
  • Lithium ion secondary battery 2C/0.2C rate performance D1/D0 ⁇ 100%.
  • the lithium ion secondary battery is first charged at a constant current of 1 C to a voltage of 4.4 V, further charged at a constant voltage of 4.4 V until the current is 0.05 C, and then discharged at a constant current of 1 C to a voltage of 3.0 V, which is A charge and discharge cycle, this discharge capacity is the discharge capacity of the first cycle.
  • the lithium ion secondary battery was subjected to 300 cycles of charge/discharge test in accordance with the above method, and the discharge capacity at the 300th cycle was detected.
  • the capacity retention ratio (%) of the lithium ion secondary battery after 300 cycles (discharge capacity of 300 cycles of lithium ion secondary battery / discharge capacity of the first cycle of lithium ion secondary battery) ⁇ 100%.
  • the lithium ion secondary battery was charged at a constant current of 0.5 C to a voltage of 4.4 V at 85 ° C, and then charged at a constant voltage of 4.4 V until the current was 0.05 C. At this time, the thickness of the lithium ion secondary battery was tested and recorded as h. 0 ; After that, the lithium ion secondary battery was placed in an oven at 85 ° C, and stored for 24 hours, and then taken out, and the thickness of the lithium ion secondary battery at this time was measured and recorded as h 1 .
  • the thickness expansion ratio (%) of the lithium ion secondary battery after 24 hours of storage [(h 1 -h 0 ) / h 0 ] ⁇ 100%.
  • Table 1 gives the parameters and performance test results of Examples 1-11 and Comparative Examples 1-7.
  • the lithium ion secondary battery has better rate performance, and has better high temperature cycle performance and high temperature storage performance.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention porte sur un électrolyte et sur une batterie rechargeable. L'électrolyte comprend un sel d'électrolyte, un solvant organique et un additif. Le solvant organique comprend un composé carboxylate. L'additif comprend du sulfate cyclique et du phosphite de triphényle. Lorsque l'électrolyte est appliqué dans la batterie rechargeable, les performances de vitesse, les performances de circulation et les performances de stockage de la batterie rechargeable à haute température et à haute tension peuvent être simultanément améliorées sous la synergie des trois.
PCT/CN2017/093744 2016-12-26 2017-07-20 Électrolyte et batterie rechargeable Ceased WO2018120787A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN201611218760.5 2016-12-26
CN201611218760.5A CN108242566A (zh) 2016-12-26 2016-12-26 电解液及二次电池

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20220190389A1 (en) * 2020-12-11 2022-06-16 Sila Nanotechnologies Inc. Electrolytes for lithium-ion battery cells with volume-changing anode particles
CN116435601A (zh) * 2023-06-14 2023-07-14 广州天赐高新材料股份有限公司 一种电解液及其应用
EP4435920A4 (fr) * 2021-11-20 2025-11-12 Jiujiang Tinci Advanced Mat Co Ltd Composition d'additif de solution d'électrolyte, solution d'électrolyte et batterie secondaire au lithium

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CN109037779A (zh) * 2018-09-19 2018-12-18 南通海嘉智能科技有限公司 新能源电池电解液负极成膜添加剂
CN111244541B (zh) * 2020-01-20 2024-04-05 宁德新能源科技有限公司 电解液和使用其的电化学装置
US12095035B2 (en) * 2020-01-20 2024-09-17 Ningde Amperex Technology Limited Electrolytic solution, and electrochemical device using the same
CN113363584A (zh) * 2021-07-19 2021-09-07 河源市联懋新材料有限公司 一种锂离子电池及其电解液、电极的制造方法
CN113707941A (zh) * 2021-09-01 2021-11-26 河源市联懋新材料有限公司 一种改善锂离子电池产气电解液及其制造方法

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CN102593517A (zh) * 2012-04-09 2012-07-18 山东鸿正电池材料科技有限公司 一种用于磷酸铁锂电池的非水电解液
CN103682442A (zh) * 2013-12-18 2014-03-26 张家港市国泰华荣化工新材料有限公司 一种非水电解液及其应用
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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20220190389A1 (en) * 2020-12-11 2022-06-16 Sila Nanotechnologies Inc. Electrolytes for lithium-ion battery cells with volume-changing anode particles
EP4435920A4 (fr) * 2021-11-20 2025-11-12 Jiujiang Tinci Advanced Mat Co Ltd Composition d'additif de solution d'électrolyte, solution d'électrolyte et batterie secondaire au lithium
CN116435601A (zh) * 2023-06-14 2023-07-14 广州天赐高新材料股份有限公司 一种电解液及其应用
CN116435601B (zh) * 2023-06-14 2024-03-22 广州天赐高新材料股份有限公司 一种电解液及其应用

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