WO2017084538A1 - 一种二次电池及其制备方法 - Google Patents
一种二次电池及其制备方法 Download PDFInfo
- Publication number
- WO2017084538A1 WO2017084538A1 PCT/CN2016/105533 CN2016105533W WO2017084538A1 WO 2017084538 A1 WO2017084538 A1 WO 2017084538A1 CN 2016105533 W CN2016105533 W CN 2016105533W WO 2017084538 A1 WO2017084538 A1 WO 2017084538A1
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- WIPO (PCT)
- Prior art keywords
- battery
- secondary battery
- active material
- electrolyte
- positive electrode
- Prior art date
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- C01—INORGANIC CHEMISTRY
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- C01B32/00—Carbon; Compounds thereof
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- H01M6/168—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by additives
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- 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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Definitions
- the invention belongs to the technical field of secondary batteries, and particularly relates to a secondary battery using a layered crystal structural material as a positive electrode active material and containing no negative electrode active material, and a preparation method thereof.
- a secondary battery also called a rechargeable battery, is a battery that can be repeatedly charged and discharged and used multiple times. Compared with a non-reusable primary battery, the secondary battery has the advantages of low cost of use and low environmental pollution.
- the main secondary battery technologies are lead-acid batteries, nickel-chromium batteries, nickel-hydrogen batteries, and lithium-ion batteries. Among them, lithium-ion batteries are the most widely used, and daily use of mobile phones, notebook computers, digital cameras, etc. are all powered by lithium-ion batteries.
- the core component of a lithium ion battery usually comprises a positive electrode, a negative electrode and an electrolyte, which realizes electrical energy storage and release by a redox reaction in which ion transport and electron transport phase separation occurs at the interface between the positive electrode, the negative electrode and the electrolyte.
- the commercial lithium ion battery mainly uses a transition metal oxide (LiCoO 2 , LiNiMnCoO 2 , LiMn 2 O 4 ) or a polyanionic metal compound (LiFePO 4 ) as a positive electrode active material, and graphite or other carbon materials as a negative electrode active material.
- the ester electrolyte or polymer gel is an electrolyte.
- lithium ions are extracted from the positive electrode active material and embedded in the negative electrode active material; during discharge, lithium ions are extracted from the negative electrode active material and embedded in the positive electrode active material.
- negative positive electrode
- the operating voltage of the conventional lithium ion battery is about 3.7V; and the theoretical capacity of the positive electrode material is limited, so that the energy density of the battery is relatively low, which is difficult to be greatly improved; in addition, the positive active material contains a transition metal element, which makes the material The cost of preparation increases, and on the other hand, the potential harm to the environment after the battery is discarded increases.
- 201410419495.1 also discloses a rechargeable aluminum ion battery and a preparation method thereof, wherein the positive electrode is a graphite structure carbon material, the negative electrode is high purity aluminum, and the ionic liquid containing an aluminum salt is used as an electrolyte.
- the current working mechanism of aluminum ion batteries is the redox reaction of aluminum ions between positive and negative electrodes.
- Al 2 Cl 7 - Al simple substance is formed in the negative electrode and AlCl 4 -, and AlCl 4 - moving to the positive electrode is embedded into the graphite intercalation compound is formed in C n (AlCl 4); the opposite discharge process.
- the aluminum ion battery Due to the different reaction mechanism, the aluminum ion battery has the advantages of fast charge and discharge speed, long cycle life and good safety. However, the battery operates at a low voltage of only about 2.2V, resulting in a lower energy density (only 40Wh/kg); in addition, the ionic liquid is expensive, leaving the battery at a distance from the actual energy storage application.
- the battery uses a graphite-based carbon material as a positive electrode and a negative electrode active material, and is completely free of transition metal elements.
- a graphite-based carbon material as a positive electrode and a negative electrode active material
- transition metal elements For example, Read and Xu of the US Army Laboratory (Energy Environ. Sci. 2014, 7, 617) have developed a double-graphite secondary battery that uses graphite as both a negative electrode and a positive electrode active material to fluorinate-modified esters.
- As the electrolyte solvent As the electrolyte solvent, reversible charge and discharge of the battery system was achieved. Rothermel and Placke et al. (Energy Environ. Sci.
- the reaction principle of the battery is that when charging, the anion in the electrolyte is embedded in the cathode graphite material, and the lithium ion is embedded in the cathode graphite material; when discharging, the anion is released from the cathode material, and lithium ions are separated from the anode material.
- the negative: positive electrode Although the double graphite battery improves the environmental impact of the battery, the preparation cost of the fluorinated modified ester electrolyte and the ionic liquid electrolyte used in the double graphite battery is very high, the production cost of the battery is still high, and the positive and negative electrodes
- the active materials are all made of graphite, which makes the quality and volume of the battery rise significantly, which reduces the energy density of the battery.
- the object of the present invention is to overcome the deficiencies of the prior art and provide a secondary battery using graphite or other layered crystal structure material as a positive electrode active material and containing no negative electrode active material to solve the environment of the existing secondary battery. Defects such as high pollution, high manufacturing cost, low energy density, and low operating voltage.
- the present invention provides a novel secondary battery comprising: a battery negative electrode, an electrolyte, a separator, a battery positive electrode, and a battery case for packaging; wherein,
- the negative electrode of the battery includes a negative current collector, and does not include a negative active material
- the electrolyte contains organic additives such as esters, sulfones, ethers, nitriles or olefins;
- the positive electrode of the battery includes a positive active material layer including a positive active material, wherein the positive active material includes a graphite-based material, a sulfide, a nitride, an oxide or a carbide having a layered crystal structure.
- the present invention also provides a novel secondary battery comprising: a battery negative electrode, an electrolyte, a separator, a battery positive electrode, and a battery case for packaging; wherein,
- the negative electrode of the battery includes a negative current collector, and does not include a negative active material
- the electrolyte contains organic additives such as esters, sulfones, ethers, nitriles or olefins;
- the positive electrode of the battery includes a positive active material layer including a positive active material, wherein the positive active material is composed of a graphite-based material, sulfide, nitride, oxide or carbide having a layered crystal structure.
- the invention provides a method for preparing the above secondary battery, comprising: preparing a battery negative electrode; preparing an electrolyte; preparing a separator; preparing a battery positive electrode; and using the battery negative electrode, the electrolyte, the separator, and the battery positive electrode to perform a novel secondary battery Assembly.
- the main active component of the positive electrode of the secondary battery proposed by the present invention is a material having a layered crystal structure, which is environmentally friendly and low in cost.
- the negative electrode current collector functions as an electrode to conduct electricity, and also serves as an electrode.
- the material which reacts with the cation in the electrolyte is equivalent to the action of the negative electrode active material of the secondary battery in the prior art. Therefore, the secondary battery provided by the embodiment of the present invention does not need to further contain the negative electrode active material, thereby significantly reducing the battery weight and cost.
- the battery energy density is improved;
- the secondary battery reaction principle proposed by the present invention is: when charging, the anion in the electrolyte is embedded in the cathode graphite layer, the cation in the electrolyte moves to the surface of the anode current collector to form an alloy, and the discharge is reversed.
- the reaction mechanism significantly increases the operating voltage of the battery (about 4.2V), further increasing the energy density.
- FIG. 1 is a schematic structural view of a novel secondary battery according to an embodiment of the present invention.
- FIG. 2 is a schematic view showing the working principle of a novel secondary battery using graphite as a positive electrode material and containing no negative electrode material according to an embodiment of the present invention
- FIG. 3 is a schematic view showing a new secondary battery in which graphite is used as a positive electrode material and does not contain a negative electrode material according to an embodiment of the present invention
- FIG. 4 is a schematic view showing a discharge of a novel secondary battery using graphite as a positive electrode material and containing no negative electrode material according to an embodiment of the present invention.
- the novel secondary battery includes a battery negative electrode 1, an electrolyte 2, a separator 3, a battery positive electrode 4, and a battery case (not shown) for packaging.
- the battery negative electrode 1 includes a negative electrode current collector and does not include a negative electrode active material;
- the electrolytic solution contains an ester, sulfone, ether, nitrile or olefin organic additive;
- the battery positive electrode 4 includes a positive electrode current collector 42 and a positive electrode active material layer 41.
- the positive electrode active material layer 41 includes a positive electrode active material, a conductive agent, and a binder, and the positive electrode active material includes a graphite-based material, a sulfide, a nitride, an oxide, or a carbide having a layered crystal structure.
- FIG. 2 is a schematic view showing the working principle of a secondary battery using graphite as a positive electrode material and containing no negative electrode material according to an embodiment of the present invention.
- FIG. 3 is a schematic view during charging
- FIG. 4 is a schematic view during discharging, and the present invention is implemented.
- the anode current collector in the secondary battery of the embodiment of the present invention functions as a material for reacting with the cation in the electrolyte in addition to the conductivity of the electrode, and is equivalent to the action of the anode active material of the secondary battery in the prior art.
- the battery structure not including the negative electrode active material provided by the embodiment of the present invention can realize a secondary battery capable of performing multiple charge and discharge.
- an operating voltage of about 4.2 V can be obtained, which significantly increases the operating voltage of the battery.
- the anode current collector is a conductive material capable of conducting and reversibly embedding or extracting cations.
- the anode current collector is one of aluminum, copper, iron, tin, zinc, nickel, titanium, manganese or an alloy of the foregoing.
- the anode current collector may include one substance, or may also contain various substances, for example, an alloy which may include one or more of aluminum, copper, iron, tin, zinc, nickel, titanium, and manganese described above.
- an alloy which may include one or more of aluminum, copper, iron, tin, zinc, nickel, titanium, and manganese described above. The invention is not limited.
- the anode active material is aluminum.
- the electrolyte comprises a solvent and an electrolyte.
- the solvent in the electrolyte can dissociate the electrolyte into cations and anions, and the cations and anions can freely migrate in the solvent.
- the solvent is an ester, sulfone or ether organic solvent, and diethyl carbonate, dimethyl carbonate, ethyl methyl carbonate, dimethyl sulfone or dimethyl ether may be used.
- the solvent may include a mixture of one or more of an ester, a sulfone or an ether organic solvent, and may include, for example, diethyl carbonate, dimethyl carbonate, ethyl methyl carbonate, dimethyl carbonate as described above.
- the mixing of one or more of the sulfone or dimethyl ether is not limited in the present invention.
- the solvent is ethyl methyl carbonate.
- the anion in the electrolyte is embedded in the positive electrode active material of the layered crystal structure to have a certain limit.
- the use of ethyl methyl carbonate as a solvent ensures that the anion in the electrolyte is sufficiently embedded in the positive electrode active material, thereby increasing the capacity of the secondary battery. .
- E the battery energy density
- C the battery capacity
- U the battery operating voltage
- E the increase of the battery capacity is beneficial to increase the energy density of the battery, so the ethyl methyl carbonate as the solvent of the second
- the secondary battery further increases the energy density of the battery by increasing the battery capacity.
- the electrolyte in the electrolyte can be dissociated into cations and anions.
- the electrolyte is a lithium salt, and lithium hexafluorophosphate, lithium tetrafluoroborate or lithium perchlorate may be used in a concentration ranging from 0.1 to 10 mol/L.
- the electrolyte may include a mixture of one or more of lithium hexafluorophosphate, lithium tetrafluoroborate or lithium perchlorate, which is not limited in the present invention.
- the electrolyte is lithium hexafluorophosphate; the electrolyte concentration is 4 mol/L.
- an additive is further included in the electrolyte, which is capable of forming a solid electrolyte membrane (SEI) on the surface of the anode current collector.
- SEI solid electrolyte membrane
- the secondary battery of the embodiment of the present invention can form a stable solid electrolyte membrane (SEI) on the surface of the anode current collector during charge and discharge to prevent the anode current collector from being displaced due to volume during charge and discharge.
- SEI solid electrolyte membrane
- the additive in the electrolyte can promote the formation of a solid electrolyte membrane (SEI) on the surface of the anode current collector.
- SEI solid electrolyte membrane
- the additive is an organic additive containing an ester, a sulfone, an ether, a nitrile or an olefin, and may be selected from vinylene carbonate, ethylene sulfite, propylene sulfite, ethylene sulfate, and cyclobutyl. Sulfone, 1,3-dioxocyclopentane, acetonitrile or long-chain olefin in an amount of from 0.1 to 20% by weight.
- the additive may include a mixture of one or more of an ester, a sulfone, an ether, a nitrile or an olefin organic additive, and may include, for example, the above-described vinylene carbonate, ethylene sulfite, or sub
- the mixing of one or more of propylene sulfate, ethylene sulfate, cyclobutyl sulfone, 1,3 dioxetane, acetonitrile or long-chain olefin is not limited in the present invention.
- the additive is vinylene carbonate.
- the vinylene carbonate is added in an amount of 2% by weight.
- the separator is not particularly limited, and it is generally used in the art.
- the separator 3 may be an insulating porous polymer film or an inorganic porous film, and a porous polypropylene film, a porous polyethylene film, a porous composite polymer film, a glass fiber paper or a porous ceramic separator may be used.
- the cathode current collector is a conductive material.
- the cathode current collector is one of aluminum, copper, iron, tin, zinc, nickel, titanium, manganese or an alloy of the foregoing.
- the cathode current collector may include one substance, or may also contain various substances, for example, an alloy which may include one or more of aluminum, copper, iron, tin, zinc, nickel, titanium, and manganese described above.
- an alloy which may include one or more of aluminum, copper, iron, tin, zinc, nickel, titanium, and manganese described above. The invention is not limited.
- the positive electrode active material in the positive electrode active material layer has a layered crystal structure capable of reversibly extracting or embedding an anion.
- the positive electrode active material includes a graphite-based material having a layered crystal structure, a sulfide, a nitride, an oxide, a carbide,
- graphite materials natural graphite, artificial graphite or graphite sheets
- Sulfide selected from molybdenum disulfide, tungsten disulfide or vanadium disulfide;
- Nitride hexagonal boron nitride or carbon doped hexagonal boron nitride
- molybdenum trioxide molybdenum trioxide, tungsten trioxide or vanadium pentoxide
- carbides use titanium carbide, tantalum carbide or molybdenum carbide.
- the positive electrode active material may include a mixture of one or more of a graphite-based material having a layered crystal structure, a sulfide, a nitride, an oxide, and a carbide, or may include different kinds of graphite-based materials, or different
- the mixing of one or more of the types of sulfides, nitrides, oxides, and carbides is not limited in the present invention.
- the positive active material is a graphite-based material.
- the conductive agent in the positive electrode active material layer is also not particularly limited, and it is conventionally used in the art.
- the conductive agent is one or more of conductive acetylene black, Super P conductive carbon sphere, conductive graphite KS6, carbon nanotube, graphene.
- the conductive agent may include only one substance, or may also contain a plurality of substances, for example, may include a mixture of one or more of various conductive agents commonly used in the art, and the invention is not limited thereto.
- the binder in the positive electrode active material layer is also not particularly limited, and it is conventionally used in the art.
- the binder is one or more of polyvinylidene fluoride, polytetrafluoroethylene, polyvinyl alcohol, carboxymethyl cellulose, SBR rubber, and polyolefin.
- the binder may include only one substance, or may also contain a plurality of substances, for example, may include a mixture of one or more of various binders commonly used in the art, and the invention is not limited thereto.
- the ratio of the active material in the positive electrode active material layer 41 to the conductive agent and the binder is not particularly limited, and it is generally used in the art.
- the amount of the positive electrode active material is 60 - 90% by weight
- the content of the conductive agent is 30 - 5% by weight
- the content of the binder is 10 - 5% by weight.
- the invention has prepared a button battery, which can be reversibly charged and discharged by the battery system test, and the battery preparation process is significantly simplified, the material cost can be reduced by 40%, and the energy density can be increased to 1.3-2 times of the existing commercial lithium ion battery. After the battery is cycled for 200 cycles, the capacity is attenuated by about 10%, and the battery cycle performance is improved.
- the form of the secondary battery is not particularly limited, and may be commonly used in the art, such as a button battery, a prism battery, a cylindrical battery, a soft battery, and the like.
- an embodiment of the present invention provides a method for preparing a secondary battery according to an embodiment of the present invention, including the following steps:
- Step 1 preparing a battery negative electrode
- the negative electrode of the battery comprises a negative current collector, and does not comprise a negative active material
- the preparation process is to cut metal foils such as copper, iron, tin, aluminum, etc. into a desired size, and clean the surface for use.
- Step 2 preparing an electrolyte
- Step 3 preparing a separator
- porous polymer film or the inorganic porous film is cut into a desired size, cleaned and used.
- Step 4 preparing a positive electrode of the battery
- the positive electrode of the battery is a positive electrode of a graphite battery, and includes a positive active material layer and a positive current collector.
- the preparation process is to weigh the active material, the conductive agent, and the binder in a certain ratio, and fully grind into a uniform slurry by adding a suitable solvent, and then uniformly apply to the surface of the cathode current collector, that is, formed on the surface of the cathode current collector.
- the positive electrode active material layer after the slurry is completely dried, it is cut to obtain a battery positive electrode of a desired size.
- steps 1 - 4 describe the operation of the preparation method of the present invention in a specific order, it is not required or implied that these operations must be performed in this particular order.
- the preparation of steps 1 - 4 can be carried out simultaneously or in any order.
- Step 5 assembling the new secondary battery by using the battery negative electrode, the electrolyte, the separator, and the battery positive electrode;
- the battery is assembled in an inert gas or waterless environment, and the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the battery case to complete the battery. Assembly.
- the choice of the kind, the kind and the component of the electrolyte additive improve the stability of the anode current collector structure of the embodiment of the invention, the operating voltage of the battery and the battery capacity that can be achieved when the layered crystal structure material is used as the positive electrode, further improve The energy density of the secondary battery of the embodiment of the invention.
- Preparation of battery negative electrode Take aluminum foil with a thickness of 0.3 mm, cut into a 12 mm diameter disc, wash with ethanol, and dry it as a negative current collector for use.
- the glass fiber paper was cut into a 16 mm diameter disc, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 0.8g natural graphite, 0.1g carbon black, 0.1g polyvinylidene fluoride was added to 2ml of nitromethylpyrrolidone solution, fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil (ie , positive current collector) and vacuum dried.
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- the reaction principle of the secondary battery of Embodiment 1 of the present invention is: negative electrode: positive electrode:
- Electrochemical performance test of the battery The secondary battery prepared in the above secondary battery preparation method was charged at a current density of 100 mA/g until its voltage reached 4.8 V, and then discharged at the same current until the voltage reached 3 V. The battery specific capacity and energy density were measured, and the cycle stability was tested (in terms of the number of cycles, the number of cycles refers to the number of times the battery is charged and discharged when the battery capacity is attenuated to 85%).
- the electrochemical performance test of the battery of the secondary battery provided by the embodiment 1 of the present invention is compared with the performance of the conventional lithium ion battery, the aluminum ion battery and the double graphite battery mentioned in the background, and the results and comparisons are shown in the table. 1.
- Table 1 Electrochemical performance parameter table of secondary battery of Example 1 of the present invention and secondary battery of the background art
- the secondary battery of the first embodiment of the present invention which is different from the various battery reaction principles in the background art has a high operating voltage and a high energy density.
- the secondary battery positive electrode of the first embodiment of the present invention replaces the lithium-containing compound with graphite, is environmentally friendly, and does not pollute the environment;
- the negative electrode current collector of the secondary battery of the first embodiment of the present invention In addition to conducting electricity as an electrode, it also acts as a material that reacts with the cations in the electrolyte, and does not need to contain a negative electrode.
- the active material significantly reduces the battery weight and cost, and increases the energy density of the battery.
- the anion in the electrolyte is embedded in the cathode graphite layer, and the cation in the electrolyte moves to the surface of the anode current collector. Alloy, the opposite is the discharge, its working voltage is about 4.2V, which improves the working voltage of the battery and increases the energy density of the battery.
- the secondary battery electrolyte of Example 1 of the present invention is different from the aluminum ion battery in the background art, and thus the reaction mechanism and performance are different.
- an anion in the electrolytic solution is embedded in the positive electrode graphite layer, and the cation in the electrolyte moves to the surface of the negative electrode current collector to form an alloy, and the discharge is reversed.
- Its operating voltage is about 4.2V, which increases the operating voltage of the battery, which in turn increases the energy density of the battery.
- the negative electrode current collector of the secondary battery of the first embodiment of the present invention functions as a material for reacting with the cation in the electrolyte, and does not need to further contain the negative electrode active material. Significantly reduce battery weight and cost, and increase battery energy density.
- Example 2-11 The preparation process of the secondary battery of Example 2-11 and Example 1 was the same except that the materials used in the preparation of the battery negative electrode were the same, and all the other steps and materials used were the same, while the secondary battery of Example 2-11 was subjected to the battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the negative electrode materials used in Examples 2-11 and their electrochemical properties are shown in Table 2.
- Table 2 Electrochemical performance parameter table of the secondary battery of Example 1-11 of the present invention
- the anode current collector is preferably an aluminum foil, which has high specific capacity, good cycle performance and highest energy density.
- Example 12-34 and Example 1 The secondary battery preparation process of Example 12-34 and Example 1 was the same except that the positive electrode active material used in the preparation of the battery positive electrode was the same, and all the other steps and materials used were the same, and the secondary battery of Example 12-34 was simultaneously subjected.
- the electrochemical performance of the battery was tested and compared with the performance of Example 1 of the present invention.
- the positive electrode active materials used in Examples 12-34 and their electrochemical properties are detailed in Table 3.
- the positive electrode material is preferably a graphite material, and the specific capacity thereof is high. High energy density.
- Example 35-37 and Example 1 The production process of the secondary battery of Example 35-37 and Example 1 was the same except that the electrolyte material used in the preparation of the electrolytic solution was the same, and all the other steps and materials used were the same, and the secondary battery of Example 35-37 was subjected to the battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the electrolyte materials used in Examples 35-37 and their electrochemical properties are detailed in Table 4.
- the electrolyte is preferably lithium hexafluorophosphate, which has high specific capacity, good cycle stability, and high energy density.
- Example 38-42 The preparation process of the secondary battery of Example 38-42 and Example 1 was the same except that the electrolyte concentration used in the preparation of the electrolytic solution was the same, all other steps and materials used were the same, and the secondary battery of Example 38-42 was subjected to the battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the electrolyte concentrations and electrochemical properties used in Examples 38-42 are detailed in Table 5.
- the electrolyte concentration is preferably 4 M, which has a high specific capacity, good cycle stability, and high energy density.
- Example 43-52 The preparation process of the secondary battery of Example 43-52 and Example 1 was the same except that the solvent materials used in the preparation of the electrolyte were different, all other steps and materials used were the same, and the secondary battery of Example 43-52 was subjected to a battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the solvent materials used in Examples 43-52 and their electrochemical properties are detailed in Table 6.
- the solvent is preferably ethyl methyl carbonate, which has a high specific capacity and a high energy density.
- Example 53-60 The preparation process of the secondary battery of Example 53-60 and Example 1 was the same except that the type of the additive used in the preparation of the electrolytic solution was the same, and all the other steps and materials used were the same, and the secondary battery of Example 53-60 was subjected to the battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the solvent materials used in Examples 53-60 and their electrochemical properties are detailed in Table 7.
- Table 7 Electrochemical performance parameter table of the secondary battery of Example 53-60 of the present invention
- the additive is preferably vinylene carbonate, which has good cycle stability.
- Example 61-67 The preparation process of the secondary battery of Example 61-67 and Example 1 was the same except that the concentration of the additive used in the preparation of the electrolytic solution was different, all other steps and materials used were the same, and the secondary battery of Example 61-67 was subjected to a battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the concentration of the additive used in Examples 61-67 and its electrochemical performance are detailed in Table 8.
- Table 8 Electrochemical performance parameter table of the secondary battery of Example 61-67 of the present invention
- the additive concentration is preferably 2% by weight, and the cycle stability is good.
- Example 68-71 The preparation process of the secondary battery of Example 68-71 and Example 1 was the same except that the separator material used in the preparation of the separator was the same, and all the other steps and materials used were the same, and the secondary battery of Example 68-71 was subjected to the battery.
- the electrochemical performance test was compared with the performance of Example 1 of the present invention.
- the separator materials used in Examples 68-71 and their electrochemical properties are detailed in Table 9.
- Example 72 The preparation process of the secondary battery of Example 72-78 and Example 1 was the same except that the conductive agent, the binder type and the mass fraction used in the preparation of the battery positive electrode were the same, and all the other steps and materials used were the same, and at the same time, Example 72
- the secondary battery of ⁇ 78 was subjected to electrochemical performance test of the battery and compared with the performance of Example 1 of the present invention.
- the conductive agent, binder type and mass fraction used in Examples 72-78 are shown in Table 10.
- Preparation of battery negative electrode Take a copper foil with a thickness of 0.5 mm, cut into a 12 mm diameter disk, wash the copper piece with ethanol, and dry it as a negative electrode current collector for use.
- the Celgard 2400 porous polymer film was cut into a 16 mm diameter disc, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 0.8g artificial graphite, 0.1g carbon black, 0.1g polyvinylidene fluoride was added to 2ml of nitromethylpyrrolidone solution, fully ground to obtain a uniform slurry; then the slurry was uniformly applied to the surface of the aluminum foil (ie , positive current collector) and vacuum dried.
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- Preparation of battery negative electrode Take aluminum foil with a thickness of 0.3 mm, cut into a 12 mm diameter disk, wash the copper piece with ethanol, and dry it as a negative current collector for use.
- the glass fiber paper was cut into a 16 mm diameter disc, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 0.7g artificial graphite, 0.2g carbon black, 0.1g polyvinylidene fluoride was added to 2ml of nitromethylpyrrolidone solution, fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of aluminum foil and vacuum dry.
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- Preparation of battery negative electrode Take aluminum foil with a thickness of 0.3 mm, cut into a 12 mm diameter disk, wash the copper piece with ethanol, and dry it as a negative current collector for use.
- the glass fiber paper was cut into a 16 mm diameter disc, washed with acetone, dried and used as a separator.
- Formulation of electrolyte 2g of lithium tetrafluoroborate is added to 5ml of ethyl methyl carbonate, stirred until lithium tetrafluoroborate is completely dissolved, then ethylene carbonate of 3% by mass is added as an additive, fully stirred and then used as electrolysis Liquid spare.
- Preparation of battery positive electrode 0.8g artificial graphite, 0.15g carbon black, 0.05g polyvinylidene fluoride was added to 2ml of nitromethylpyrrolidone solution, fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil and vacuum dry.
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- Preparation of battery negative electrode Take an iron piece with a thickness of 0.3 mm, cut into a 12 mm diameter disk, wash the copper piece with ethanol, and dry it as a negative electrode current collector for use.
- the glass fiber paper was cut into a 16 mm diameter disc, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 1 g of titanium carbide, 0.15 g of carbon black, 0.05 g of polyvinylidene fluoride was added to 2 ml of nitromethylpyrrolidone solution, and fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil and vacuum dried. .
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- Preparation of battery negative electrode Take a copper foil with a thickness of 0.3mm, cut into a 12mm diameter disc, and clear with ethanol Wash the copper sheet and dry it as a negative current collector.
- the porous polypropylene film was cut into a 16 mm-diameter wafer, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 1 g of titanium carbide, 0.15 g of carbon black, 0.05 g of polyvinylidene fluoride was added to 2 ml of nitromethylpyrrolidone solution, and fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil and vacuum dried. .
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- the prepared negative electrode current collector, separator, and battery positive electrode are closely stacked in sequence, and the electrolyte is dripped to completely infiltrate the separator, and then the stacked portion is packaged into the button battery case. , complete battery assembly.
- Preparation of battery negative electrode Take aluminum foil with a thickness of 0.3 mm, cut into a 12 mm diameter disk, wash the copper piece with ethanol, and dry it as a negative current collector for use.
- the porous polypropylene film was cut into a 16 mm-diameter wafer, washed with acetone, dried and used as a separator.
- Preparation of battery positive electrode 1 g of molybdenum disulfide, 0.15 g of carbon black, 0.05 g of polyvinylidene fluoride was added to 2 ml of nitromethylpyrrolidone solution, and fully ground to obtain a uniform slurry; then the slurry was uniformly coated on the surface of the aluminum foil and vacuumed dry.
- the electrode sheet obtained by drying was cut into a disk having a diameter of 10 mm, and compacted as a battery positive electrode.
- Table 11 Electrochemical performance parameter tables of secondary batteries of Example 79-84 of the present invention
- Examples 80, 81, and 84 aluminum foil was used as the negative electrode material, and Examples 79, 82, and 83 which used other materials as the negative electrode material had higher specific capacity and higher energy density.
- Example 79 used a vinylene carbonate having a mass fraction of 2% as an additive, and the cycle stability was better than that of Examples 80-84 using other additives.
- Example 80 4 M lithium hexafluorophosphate was used as the electrolyte, and Examples 81 and 84, which used other materials as the electrolyte, had higher specific capacity and higher energy density.
- the form of the secondary battery according to the present invention is not limited to the button type battery, and may be designed in the form of a prismatic battery, a cylindrical battery, a soft pack battery or the like according to the core component.
- the main active component of the secondary battery proposed by the present invention is a graphite-like material having a layered crystal structure, which is environmentally friendly and low in cost.
- the secondary battery system of the present invention does not require a negative active material, thereby significantly reducing the battery weight and cost, and increasing the energy density of the battery.
- the reaction principle adopted by the secondary battery proposed by the invention can reach an operating voltage of about 4.2V, the battery operating voltage is high, and the battery energy density can be greatly improved.
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Abstract
Description
Claims (12)
- 一种二次电池,其特征在于,包括:电池负极、电解液、隔膜、电池正极以及用于封装的电池壳体;其中,电池负极包括负极集流体,不包含负极活性材料;电解液包含酯类、砜类、醚类、腈类或烯烃类有机添加剂;电池正极包括正极活性材料层,所述正极活性材料层包括正极活性材料,其中,所述正极活性材料包括具有层状晶体结构的石墨类材料、硫化物、氮化物、氧化物或碳化物。
- 一种二次电池,其特征在于,包括:电池负极、电解液、隔膜、电池正极以及用于封装的电池壳体;其中,电池负极包括负极集流体,不包含负极活性材料;电解液包含酯类、砜类、醚类、腈类或烯烃类有机添加剂;电池正极包括正极活性材料层,所述正极活性材料层包括正极活性材料,其中,所述正极活性材料由具有层状晶体结构的石墨类材料、硫化物、氮化物、氧化物或碳化物组成。
- 根据权利要求1或2所述的二次电池,其特征在于,所述负极集流体为导电材料,所述导电材料为铝、铜、铁、锡、锌、镍、钛、锰中的一种或前述的合金。
- 根据权利要求3所述的二次电池,其特征在于,所述负极集流体为铝。
- 根据权利要求1或2所述的二次电池,其特征在于,所述电解液的组分还包含溶剂、电解质;其中,所述溶剂为酯类、砜类或醚类有机溶剂;所述电解质为锂盐。
- 如权利要求5所述的二次电池,其特征在于,所述电解质选用六氟磷酸锂、四氟硼酸锂或高氯酸锂,且浓度范围为0.1–10mol/L。
- 如权利要求5所述的二次电池,其特征在于,所述溶剂选用碳酸二乙酯、碳酸二甲酯、碳酸甲乙酯、二甲基砜或二甲醚。
- 如权利要求7所述的二次电池,其特征在于,所述溶剂为碳酸甲乙酯。
- 如权利要求1或2所述的二次电池,其特征在于,所述酯类、砜类、醚类、腈类或烯烃类有机添加剂,选用碳酸亚乙烯酯、亚硫酸亚乙酯、亚硫酸丙烯酯、硫酸亚乙酯、环丁基砜、1,3‐二氧环戊烷、乙腈或长链烯烃,且添加量为0.1‐20%wt。
- 如权利要求9所述的二次电池,其特征在于,所述有机添加剂为碳酸亚乙烯酯,添加量为2%wt。
- 根据权利要求1或2所述的新型二次电池,其特征在于,在所述正极活性材料中的所述石墨类材料,选用天然石墨、人造石墨或石墨片;所述硫化物,选用二硫化钼、二硫化钨或二硫化钒;所述氮化物,选用六方氮化硼或碳掺杂六方氮化硼;所述氧化物,选用三氧化钼、三氧化钨或五氧化二钒;所述碳化物,选用碳化钛、碳化钽或碳化钼。
- 一种制备权利要求1至11中任一项所述的新型二次电池的方法,其特征在于,包括:制备电池负极;配制电解液;制备隔膜;制备电池正极;利用所述电池负极、电解液、隔膜、电池正极进行新型二次电池的组装。
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JP2018521962A JP7091242B2 (ja) | 2015-11-18 | 2016-11-12 | 二次電池及びその製造方法 |
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WO2017084128A1 (zh) | 2017-05-26 |
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