WO2018112801A1 - Batterie lithium-ion et son procédé de production - Google Patents

Batterie lithium-ion et son procédé de production Download PDF

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Publication number
WO2018112801A1
WO2018112801A1 PCT/CN2016/111329 CN2016111329W WO2018112801A1 WO 2018112801 A1 WO2018112801 A1 WO 2018112801A1 CN 2016111329 W CN2016111329 W CN 2016111329W WO 2018112801 A1 WO2018112801 A1 WO 2018112801A1
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Prior art keywords
lithium
cathode
ion battery
lithium ion
anode
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PCT/CN2016/111329
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English (en)
Inventor
Jun Yang
Yitian BIE
Jingjing Zhang
Yuqian DOU
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Robert Bosch Gmbh
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Priority to PCT/CN2016/111329 priority Critical patent/WO2018112801A1/fr
Priority to DE112016007530.8T priority patent/DE112016007530T5/de
Priority to CN201680091755.4A priority patent/CN110100335A/zh
Priority to KR1020197017721A priority patent/KR20190095928A/ko
Publication of WO2018112801A1 publication Critical patent/WO2018112801A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • 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
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    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
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    • 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
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    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/44—Methods for charging or discharging
    • H01M10/446—Initial charging measures
    • H—ELECTRICITY
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    • H01M4/04—Processes of manufacture in general
    • H01M4/0438—Processes of manufacture in general by electrochemical processing
    • H01M4/044—Activating, forming or electrochemical attack of the supporting material
    • H01M4/0445—Forming after manufacture of the electrode, e.g. first charge, cycling
    • H01M4/0447—Forming after manufacture of the electrode, e.g. first charge, cycling of complete cells or cells stacks
    • H—ELECTRICITY
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    • H01M4/0459—Electrochemical doping, intercalation, occlusion or alloying
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    • 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
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
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    • H01M4/134—Electrodes based on metals, Si or alloys
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    • 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
    • H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
    • H—ELECTRICITY
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    • 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
    • H01M4/139—Processes of manufacture
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    • 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
    • H01M4/139—Processes of manufacture
    • H01M4/1397—Processes of manufacture of electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
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    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • H01M4/364—Composites as mixtures
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    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • H—ELECTRICITY
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    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • H—ELECTRICITY
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    • 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
    • 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 lithium ion batteries and methods for preparing the same.
  • Lithium ion batteries have now been widely used in energy storage systems and electric vehicles.
  • lithium ion batteries which comprise lithium-containing cathode materials (such as LiCoO 2 or LiNiO 2 ) , lithium-free anode materials (such as graphite) and electrolytes
  • lithium ions move from cathodes to anodes when charging.
  • the moving lithium ions inevitably and continuously react with the electrolytes.
  • lithium is undesirably consumed and solid electrolyte interfaces (SEI) are formed on the anodes. The consumed lithium does not return to the cathodes during subsequent discharges, causing fast capacity fading for the lithium ion batteries.
  • SEI solid electrolyte interfaces
  • the inventors After intensive study, the inventors have developed a novel lithium ion battery, comprising a cathode, an anode and an electrolyte, wherein the cathode comprises a cathode active material and lithium peroxide.
  • the lithium ion battery is prelithiated or unprelithiated, and the content of lithium peroxide is from more than 0 to about 20%by weight, preferably from more than 0 to less than 20%by weight, more preferably from about 0.01%to about 5%by weight, still further preferably from about 0.01%to about 1%, based on the total dry weight of cathode composition.
  • the content of the lithium peroxide in the prelithiated battery or unprelithiated battery is from more than 0 to about 20%by weight, preferably from more than 0 to less than 20%by weight, more preferably from about 0.01%to about 5%by weight, still further preferably from about 0.01%to about 1%, based on the total dry weight of cathode composition.
  • a lithium ion battery comprising a cathode, an anode and an electrolyte, wherein the electrolyte comprises lithium salt, a non-aqueous solvent and lithium peroxide.
  • lithium peroxide Li 2 O 2
  • the inventors found that lithium peroxide (Li 2 O 2 ) can be advantageously used in a cathode or an electrolyte of lithium ion battery as a lithium source for prelithiating the anode.
  • the capacity fading may be compensated, and the battery performances (such as irreversible capacity and cycling stability) may be significantly improved.
  • lithium powders or lithium nitride As for the proposal of coating lithium powders or lithium nitride onto anodes to prelithiate the anodes in the prior art, on the one hand, lithium powders have high activity with moisture in the atmosphere and release hydrogen gas upon reaction with water, thus, there is a risk of explosion when employing lithium powders in batteries. Likewise, lithium nitride also reacts with moisture in the air and generates sparks. On the other hand, lithium powders are coated onto the anodes by an additional step of spraying, sputtering or deposition. In order to meet the requirements of carrying out such additional step, other components of the anode composition, such as binder and solvent, need to be modified.
  • lithium peroxide which is employed in the present disclosure is relatively steady against moisture. Even if lithium peroxide reacts with moisture, no gas is generated and thus there is no risk of explosion, which greatly improves production safety and reduces manufacturing cost. Furthermore, the introduction of lithium peroxide may be integrated with the addition of other components of the cathode composition or electrolyte composition, and does not additionally need a separate step or requires a special condition, which means considerable cost saving and labor saving for industrial production.
  • Figure 1 compares discharge/charge profiles of cells prepared according to Examples of the present disclosure and a Comparative Example.
  • Figure 2 compares cycling performances of cells prepared according to Examples of the present disclosure and a Comparative Example.
  • Figure 3 compares discharge/charge profiles of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 4 compares cycling performances of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 5 shows discharge/charge profiles of cells prepared according to an Example of the present disclosure.
  • Figure 6 shows cycling performances of cells prepared according to an Example of the present disclosure.
  • Figure 7 compares discharge/charge profiles of a cell prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 8 compares cycling performances of a cell prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 9 shows discharge/charge profiles of a cell prepared according to an Example of the present disclosure.
  • Figure 10 shows cycling performances of a cell prepared according to an Example of the present disclosure.
  • Figure 11 compares discharge/charge profiles of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 12 compares cycling performances of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 13 compares discharge/charge profiles of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • Figure 14 compares cycling performances of cells prepared according to an Example of the present disclosure and a Comparative Example.
  • cell and “battery” may be interchangeably used.
  • lithium ion cell (or battery) may also be abbreviated to “cell” or “battery” .
  • the term “comprising” means that other ingredients or other steps which do not affect the final effect can be included. This term encompasses the terms “consisting of” and “consisting essentially of” .
  • the product and process according to the present disclosure can comprise, consist of, and consist essentially of the essential technical features and/or limitations of the present disclosure described herein, as well as any additional and/or optional ingredients, components, steps, or limitations described herein.
  • cathode composition or “anode composition” intends to mean the composition used to form the cathode slurry or the anode slurry.
  • the cathode slurry or the anode slurry may be subsequently applied onto the corresponding current collector and dried to from the cathode or anode.
  • a lithium ion battery which comprises a cathode, an anode and an electrolyte, wherein the cathode comprises a cathode active material and lithium peroxide.
  • the lithium ion battery is prelithiated or unprelithiated, and the content of lithium peroxide is from more than 0 to about 20%by weight, preferably from more than 0 to less than 20%by weight, more preferably from about 0.01%to about 5%by weight, still further preferably from about 0.01%to about 1%by weight, based on the total dry weight of cathode composition.
  • the method of preparing the lithium ion battery according to the present disclosure comprises:
  • the content of the lithium peroxide in the prelithiated battery or unprelithiated battery is from more than 0 to about 20%by weight, preferably from more than 0 to less than 20%by weight, more preferably from about 0.01%to about 5%by weight, still further preferably from about 0.01%to about 1%, based on the total dry weight of cathode composition.
  • a lithium ion battery which comprises a cathode, an anode and an electrolyte, wherein the electrolyte comprises lithium salt, a non-aqueous solvent and lithium peroxide.
  • the method of preparing the lithium ion battery according to the present disclosure comprises:
  • Lithium peroxide which is employed in the present disclosure is relatively steady against moisture. Even if lithium peroxide reacts with moisture, no gas is generated and thus there is no risk of explosion, which greatly improves production safety and reduces manufacturing cost.
  • lithium peroxide is provided to the cathode or the electrolyte. Since lithium peroxide is compatible with other components contained in the cathode or the electrolyte, there is no need to change the composition of the cathode or the electrolyte. In contrast, if lithium peroxide is directly provided to the anode, the solvent and adhesive contained in the anode need to be correspondingly modified.
  • the cathode active material and lithium peroxide may be employed to form a cathode slurry, and subsequently the cathode slurry may be applied onto a cathode current collector.
  • lithium peroxide may be mixed with other components of the cathode composition (such as the cathode active material, a carbon material, a binder, a solvent, and/or optional additive (s) ) to prepare a cathode slurry.
  • the cathode slurry may be applied onto a current collector, for example by coating, so as to form a cathode containing lithium peroxide.
  • a current collector for example by coating
  • the introduction of lithium peroxide is integrated with the addition of other components of the cathode composition, and does not additionally need a separate step or requires a special condition, which means considerable cost saving and labor saving for industrial production.
  • the cathode active material may be applied onto a cathode collector to form an active material layer, and then lithium peroxide may be applied onto the active material layer to form a lithium peroxide layer.
  • Providing lithium peroxide in this way is also easy to be conducted.
  • lithium ions are extracted from the lithium peroxide in the cathode or in the electrolyte. Meanwhile, the peroxide anions (O 2 2- ) in the lithium peroxide lose electrons and convert into oxygen gas. The extracted lithium ions insert into and store in the anode. The anode is thus prelithiated.
  • the first several charges during which the anode is prelithiated are also referred to as “formation charges” .
  • the lithium stored in the anode in the formation charges may take part in lithium ion transference, compensate lithium loss due to the formation of SEI layer, stabilize the SEI layer and reduce the capacity fading.
  • the formation charges may be conducted within a voltage range, i.e., a cut-off voltage range.
  • the upper limit of the cut-off voltage may be no less than about 3.8V but no more than about 5V, preferably no less than about 4.2V but no more than about 5V.
  • the upper limit of cut-off voltage during the formation charges may depend on the cathode active material contained in the lithium ion battery. The cathode active material will be described hereinafter.
  • the upper limit of the cut-off voltage during formation charges may be no less than about 4.2V but no more than about 5V.
  • the cathode contains lithium nickel cobalt manganese oxide/Li 2 MnO 3 composite (also referred to as “lithium-riched NCM” ) as active material
  • the upper limit of the cut-off voltage during the formation charges may be no less than about 4.35V but no more than about 5.0V.
  • the anode may be partially prelithiated, so as to not only compensate the lithium loss due to the formation of SEI, but also retain desirable lithium transference between the cathode and the anode.
  • the irreversible capacity (unit: mAh/cm 2 ) of the anode that is available for lithium insertion is from about 1 to about 1.2 times, e.g. from about 1 to 1.1 times of the irreversible capacity (unit: mAh/cm 2 ) of the cathode.
  • the ratio of the irreversible capacity of the anode to the irreversible capacity of the cathode may be 1. However, considering that there are inevitable operation errors during preparing the battery, said ratio may be larger than 1.
  • the ratio of the irreversible capacity of the anode to the irreversible capacity of the cathode is less than 1, excessive lithium metal may aggregate around the anode, undesirably forming lithium dendrites and causing short circuit. If the ratio of the irreversible capacity of the anode to the irreversible capacity of the cathode is more than 1.2, the anode capacity is too large and it excessively consumes anode irreversible capacity.
  • the lithium ion batteries according to the present disclosure may be used in energy storage systems and electric vehicles.
  • the cathode composition may comprise lithium peroxide as a lithium source for prelithiating the anode.
  • the cathode composition may retain a trace amount of lithium peroxide, e.g., from about 0.01%to about 1%by weight, based on the total dry weight of cathode composition.
  • the cathode may comprise a cathode active material.
  • the cathode active material may be a material that reversibly deserts and inserts lithium ions during charge/discharge cycles. In discharge cycles, the lithium ions originated from the cathode active material can transfer from the anode back to the cathode to form the cathode active material again.
  • lithium peroxide may be referred to as an “additional lithium source” or “supplemental lithium source” .
  • the cathode active material there is no specific limitation to the cathode active material, and those cathode active materials commonly used in lithium ion cells may be used.
  • the cathode active material may be different from lithium peroxide.
  • the cathode active material may be a lithium-based active material.
  • the cathode active material may be selected from the group consisting of lithium metal oxides, lithium metal phosphates, lithium metal silicates, sulfides and any combination thereof, preferably lithium-transition metal composite oxides, lithium-transition metal phosphates, lithium metal silicates, metal sulfides and any combination thereof.
  • the cathode active material may be selected from the group consisting of lithium iron phosphate, lithium manganese phosphate, lithium manganese iron phosphate and any combination thereof.
  • the lithium-transition metal composite oxide may be lithium nickel oxide, lithium cobalt oxide, lithium manganese oxide, lithium nickel cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide (NCM) , lithium nickel cobalt aluminum oxide (NCA) , lithium nickel cobalt manganese oxide/Li 2 MnO 3 composite (also referred to as “lithium-riched NCM” ) , or any combination thereof.
  • the metal sulfide may be iron sulfide.
  • the cathode active material may have a size of from 1 micrometer to several tens micrometers.
  • the cathode may additionally comprise fine particles having a particle size less than that of the cathode active material.
  • the fine particles may have a size less than 1 micrometer (i.e., nano scale) .
  • the fine particles may be selected from the group consisting of transition metal compounds, noble metals, carbon materials and any combination thereof.
  • the fine particles may be commercially available, or be obtained by grinding relatively larger particles into small sizes, for example, by using a mill ball. These fine particles may advantageously catalyze the decomposition of lithium peroxide into lithium ions during the formation charges.
  • Transition metal compounds may include compounds of any transitional metals in group 3 through group 12 of the period table, such as titanium oxide, zinc oxide, copper oxide, nickel oxide, molybdenum oxide.
  • Noble metals include gold, silver, and platinum-group metals (i.e., ruthenium, rhodium, palladium, osmium, iridium and platinum) .
  • Fine particles of carbon materials may be carbon nanotube, hard carbon, spherical carbon, etc.
  • the cathode may simultaneously comprise cathode active materials of two different sizes. In some examples, the cathode may simultaneously comprise a cathode active material having a size from 1 micrometer to several tens micrometers, and fine particles of the identical cathode active material having a size less than 1 micrometer.
  • the cathode composition may further comprise a carbon material.
  • Carbon material may be a material containing carbon element. The carbon material may increase the electrical conductivity and/or dispersibility of the cathode composition. There is no specific limitation to the carbon material, and those which are known for use in lithium ion batteries may be used.
  • the carbon material may include but is not limited to carbon black, super P, acetylene black, Ketjen black, graphite, graphene, carbon nanotubes, carbon fibers, vapour grown carbon fibers, and combination thereof.
  • the cathode may contain a mixture of two or different types of carbon materials.
  • the cathode may simultaneously comprise carbon materials of two different sizes, i.e., a carbon material of no less than 1 micrometer, and fine particles of the identical or a different carbon material of less than 1 micrometer.
  • the cathode composition may further comprise a binder.
  • the binder may hold the components of the cathode composition together and attach the cathode composition to the cathode current collector, help to retain good stability and integrity of the cathode when volume change occurs during repeated charge/discharge cycles, and thus improve the electrochemical properties of the final cells, including cycling performances and rate performances.
  • the binder may be polyvinylidene fluoride (PVDF) , polyacrylic acid (PAA) , sodium carboxymethyl cellulose (CMC) , preferably PVDF.
  • the cathode compositions may further comprise a solvent.
  • the solvent may dissolve other components of the cathode composition to provide a cathode slurry.
  • the resultant cathode slurry may be subsequently applied onto the cathode current collector.
  • the cathode current collector having the cathode slurry applied thereon may be dried to obtain a cathode.
  • the solvent contained in the cathode composition and those which are known for use in lithium ion batteries may be used.
  • the solvent in the cathode composition may be N-methyl-2-pyrrolidone (NMP) .
  • the cathode composition comprises lithium peroxide, a cathode active material, a carbon material, a binder and a solvent.
  • other additives commonly known for use in lithium ion batteries may be optionally used, so long as they do not adversely impair the desired performances of the battery.
  • cathode current collector there is no specific limitation to the cathode current collector.
  • aluminum foil may be used as the cathode current collector.
  • the anode compositions according to the present disclosure may comprise an anode active material.
  • anode active material There is no specific limitation to the anode active material, and those anode active materials commonly known in lithium ion cells may be used.
  • the anode active material may be selected from the group consisting of silicon-based active materials, graphite-based active materials and any combination thereof.
  • Silicon-based active material may be an active material containing silicon element.
  • suitable silicon-based active material may include but is not limited to silicon, silicon alloys, silicon oxides, silicon/carbon composites, silicon oxide/carbon composites and any combination thereof.
  • the silicon alloy may comprise silicon and one or more metals selected from the group consisting of Ti, Sn, Al, Sb, Bi, As, Ge and Pb.
  • the silicon oxide may be a mixture of more than one oxides of silicon.
  • the silicon oxide may be represented as SiO x , where the average value of x may be from about 0.5 to about 2.
  • Carbon-based active material may be an active material containing carbon element.
  • the carbon-based active material in the anode may be identical or different from the carbon material contained in the cathode.
  • suitable carbon-based active material may include but is not limited to graphite, graphene, hard carbon, carbon black and carbon nanotubes.
  • the anode composition may further comprise a carbon material, a binder and/or a solvent.
  • the carbon material, binder and solvent in the anode may be identical or different from those contained in the cathode, respectively.
  • other additives commonly known for use in lithium ion batteries may be optionally used, so long as they do not adversely impair the desired performances of the battery.
  • anode current collector there is no specific limitation to the anode current collector.
  • nickel foil, a nickel net, copper foil or copper net may be used as the anode current collector.
  • the lithium ion batteries according to the present disclosure may comprise an electrolyte.
  • the electrolyte may comprise a lithium salt and a non-aqueous solvent.
  • the lithium salt in the electrolyte may be different from the lithium peroxide and the cathode active material in the cathode.
  • the lithium salts may include but are not limited to lithium hexafluorophosphate (LiPF 6 ) , lithium tetrafluoroborate (LiBF 4 ) , lithium arsenate (LiAsO 4 ) , LiSbO 4 , Lithium perchlorate (LiC1O 4 ) , LiAlO 4 , LiGaO 4 , lithium bis (oxalate) borate (LiBOB) and any combination thereof, with preference being given to LiPF 6 .
  • LiPF 6 lithium hexafluorophosphate
  • LiBF 4 lithium tetrafluoroborate
  • LiAsO 4 lithium arsenate
  • LiSbO 4 Lithium perchlorate
  • LiAlO 4 LiAlO 4
  • LiGaO 4 LiGaO 4
  • LiBOB lithium bis (oxalate) borate
  • the non-aqueous solvents may be carbonates (i.e., non-fluorinated carbonates) and fluorinated carbonates.
  • the carbonates may include but are not limited to cyclic carbonates, such as ethylene carbonate (EC) , propylene carbonate (PC) , butylene carbonate (BC) ; linear carbonates, such as dimethyl carbonate (DMC) , diethyl carbonate (DEC) , dipropyl carbonate (DPC) , ethyl methyl carbonate (EMC) , methylpropyl carbonate (MPC) , ethylpropyl carbonate (EPC) ; and any combination of the aforementioned carbonates.
  • cyclic carbonates such as ethylene carbonate (EC) , propylene carbonate (PC) , butylene carbonate (BC) ; linear carbonates, such as dimethyl carbonate (DMC) , diethyl carbonate (DEC) , dipropyl carbonate (DPC
  • the fluorinated carbonates may be fluorinated derivatives of the aforementioned carbonates, such as fluoroethylene carbonate (FEC) and difluoroethylene carbonate, difluorinated dimethyl carbonate (DFDMC) .
  • FEC fluoroethylene carbonate
  • DMDMC difluorinated dimethyl carbonate
  • a mixture of non-fluorinated carbonate and fluorinated carbonate may be referred to “partially fluorinated carbonate” .
  • a fluorinated carbonate may be referred to “fully fluorinated carbonate” , relative to non-fluorinated carbonate and partially fluorinated carbonate.
  • the electrolyte may further comprise a boron-based anion acceptor.
  • a boron-based anion acceptor there is no specific limitation to the boron-based anion acceptor, and the boranes and borates which have Lewis acid centers on boron atoms and can form complexes with the peroxide ion (O 2 2- , a Lewis base center) may be used.
  • the solubility of the lithium peroxide into the electrolyte may be increased, and the kinetics for the delithiation of lithium peroxide may be improved which facilitates the release of lithium ion from lithium peroxide.
  • the boranes or borates may also stabilize the anion (such as PF 6 5- ) and mitigate the decomposition of the lithium salt (such as LiPF 6 ) which would otherwise cause capacity fading and increase the impedance during charge/discharge cycling.
  • borates represented by formula (fluorinated alkyl-O) 3 -B borates represented by formula (fluorinated aryl-O) 3 -B, and boranes represented by general formula (fluorinated aryl) 3 -B described by H. S. Lee, etc. (J. Electochem. Soc., 145 (1998) , pp 2813-2818, which is incorporated herein by reference in its entirety) may be used according to the present disclosure.
  • Exemplified borates may include but are not limited to tris (2H-hexafluoroisopropyl) borate (THFPB, [ (CF 3 ) 2 CHO] 3 B) and tris (2, 4-difluoroethyl) borate (F 2 C 6 H 3 O) 3 B, and exemplified boranes may include but are not limited to tris (pentafluorophenyl) borane (TPFPB, (C 6 F 5 ) 3 B) .
  • R is a fluorine bearing moiety (ies) .
  • a non-limiting example of the fluorinated arylboron oxalates may include but are not limited to pentafluorophenylboron oxalate (PFPBO) .
  • LiBOB Lithium bis (oxalato) borate
  • boron-based anion acceptor in the electrolyte.
  • LiODFB lithium oxaltodifluoroborate
  • the fluorinated arylboron oxalates e.g., PFPBO
  • LiBOB and LIODFB may also help to form a more stable SEI layer on the surface of the anode, which decreases the lithium consumption and improves the battery performances.
  • NCM-111 lithium nickel cobalt manganese oxide, active material of the cathode, D50: 12 ⁇ m, available from BASF.
  • Si/C composite active material of the anode, homemade by mixing silicon nanoparticles (diameter: 50 nm, available from Alfa Aesar) and graphite (available from Shenzhen Kejingstar Technology Ltd. ) in a weight ratio of 1: 1.
  • KS6L graphite flake, carbon material, about 6 ⁇ m, available from Timcal.
  • Lithium peroxide lithium source for anode prelithiation, available from Alfa Aesar.
  • PVDF polyvinylidene fluoride, binder, available from Sovey.
  • NMP N-methyl-2-pyrrolidone, solvent, available from Guoyao.
  • Celgard 2325 PP/PE/PP membrane, separator, available from Celgard.
  • NCM-111 938.6 mg NCM-111, 26.4 mg lithium peroxide, 10 mg Super P, 5 mg KS6L, 20 mg PVDF were added into 450 mL NMP in an Argon-filled glovebox (MB-10 compact, MBraun) . After stirring for 3 h, the resultant uniformly-dispersed slurry was coated onto an aluminum foil, then dried at 80°C in vacuum for 6 h. The coated Al foil was taken out from the glovebox and cut into several ⁇ 12 mm cathodes (abbreviated to NCM-Li 2 O 2 cathodes) .
  • Coin cells (CR2016) was assembled in an Argon-filled glovebox (MB-10 compact, MBraun) by using the cathodes obtained above. A pure Li metal foil was used as a counter electrode. 1M LiPF 6 in FEC + EMC (3: 7 by volume, partially fluorinated carbonate electrolyte) was used as an electrolyte. Celgard 2325 was employed as a separator.
  • NCM-Li 2 O 2 -catalyst cathodes were prepared in the same way as described above for Example 1, except that 10 mg fine particles of NCM-111 as catalyst were added to prepare the cathode slurry, and 928.6 mg NCM-111 were used instead of 938.6 mg NCM-111.
  • the fine particles of NCM-111 have a particle size of less than 1 ⁇ m.
  • Cathodes (abbreviated to NCM-Li 2 O 2 -catalyst cathodes) were prepared in the same way as described above for Example 2, except that 24.1 mg lithium peroxide was used instead of 26.4 mg lithium peroxide.
  • Cathodes (abbreviated to NCM-Li 2 O 2 -catalyst cathodes) were prepared in the same way as described above for Example 2, except that 50 mg lithium peroxide was used instead of 26.4 mg lithium peroxide.
  • a cell was prepared in the same way as described above for Example 4, except that 1M LiPF 6 in EC + DMC (1: 1 by volume, non-fluorinated carbonate electrolyte) was used as an electrolyte.
  • a cell was prepared in the same way as described above for Example 4, except that 1M LiPF 6 in fully fluorinated carbonate electrolyte (containing 30 vol%of FEC) was used as an electrolyte.
  • a cell was prepared in the same way as described above for Example 2, except that Si/C composite was used as anode.
  • a cell was prepared in the same way as described above for Example 7, except that 1M LiPF 6 in fully fluorinated carbonate electrolyte (containing 30 vol%of FEC) was used as an electrolyte.
  • NCM cathodes were prepared in the same way as described above for Example 1, except that no lithium peroxide was employed, and 965 mg NCM- 111 was employed instead of 938.6 mg NCM-111.
  • a cell was prepared in the same way as described above for Comparative Example 1, except that Si/C composite was used as anode.
  • a cell was prepared in the same way as described above for Comparative Example 2, except that 1M LiPF 6 in fully fluorinated carbonate electrolyte (containing 30 vol%of FEC) was used as an electrolyte.
  • Figure 1 compares discharge/charge profiles of the cells prepared according to Example 1, Example 2 and Comparative Example 1 for the first charge/discharge cycle.
  • each cell was charged/discharged within a voltage range of 3 to 4.6 V (vs Li/Li + ) .
  • the mass loading of NCM in each cathode of the cells is about 10 mg/cm 2 .
  • the specific capacities were calculated on the basis of the weight of NCM. Comparing with the NCM cathode in Comparative Example 1, the NCM-Li 2 O 2 cathode in Example 1 improved the charge capacity in the 1 st charge.
  • the NCM-Li 2 O 2 -catalyst cathode in Example 2 Comparing with the NCM-Li 2 O 2 cathode in Example 1, the NCM-Li 2 O 2 -catalyst cathode in Example 2 further improved the charge capacity in the 1 st charge. This was attributed to the fine particles of NCM which catalyzed the decomposition of lithium peroxide, thereby more lithium ions were provided to the anodes.
  • Figure 2 compares cycling performances of the cells prepared according to Example 1, Example 2 and Comparative Example 1. Each cell was discharged/charged within a voltage range of 3 to 4.6 V (vs Li/Li + ) for the 1 st charge cycle, and then charged/discharged at normal voltage range of 3 to 4.3V.
  • the mass loading of NCM in each cathode of the cells is about 10 mg/cm 2 .
  • the specific capacities were calculated on the basis of the weight of NCM.
  • Figure 3 compares discharge/charge profiles of the cells prepared according to Example 3 and Comparative Example 1 for the first charge/discharge cycle.
  • Figure 4 compares cycling performances of the cells prepared according to Example 3 and Comparative Example 1.
  • Figure 5 shows discharge/charge profiles of the cells prepared according to Example 4 for the first charge/discharge cycle.
  • Figure 6 shows cycling performances of the cells prepared according to Example 4.
  • Each cell was discharged/charged within a voltage range of 3 to 4.6 V (vs Li/Li + ) for the 1 st charge cycle, and then charged/discharged at normal voltage range of 3 to 4.3V.
  • the mass loading of NCM in each cathode of the cells is about 10 mg/cm 2 .
  • the specific capacities were calculated on the basis of the weight of NCM.
  • Figures 3 to 6 demonstrated that NCM-Li 2 O 2 -catalyst cathodes significantly improves the capacities and stabilities of the cells than NCM cathodes.
  • Figure 7 compares the discharge/charge profile of the cell prepared according to Example 5 and Comparative Example 1 for the first charge/discharge cycle.
  • Figure 8 compares the cycling performance of the cell prepared according to Example 5 and Comparative Example 1.
  • Figure 9 shows the discharge/charge profile of the cell prepared according to Example 6 for the first charge/discharge cycle.
  • Figure 10 shows the cycling performance of the cell prepared according to Example 6.
  • Each cell was discharged/charged within a voltage range of 3 to 4.6 V (vs Li/Li + ) for the 1 st charge cycle, and then charged/discharged at normal voltage range of 3 to 4.3V.
  • the mass loading of NCM in each cathode of the cells is about 10 mg/cm 2 .
  • the specific capacities were calculated on the basis of the weight of NCM.
  • Figures 7-10 demonstrated that non-fluorinated carbonates, fully fluorinated carbonates and partially fluorinated carbonates are all suitable for the prelithiation method, and significantly improve the capacities and stabilities of the
  • Figure 11 compares discharge/charge profiles of the cells prepared according to Example 7 and Comparative Example 2 for the first charge/discharge cycle.
  • Figure 12 compares cycling performances of the cells prepared according to Example 7 and Comparative Example 2. Each cell was charged within a voltage range of 2.5 to 4.6 V (vs Li/Li + ) for the 1 st charge cycle, and then charged/discharged at normal voltage range of 2.5 to 4.2V. The mass loading of NCM in each cathode of the cells is about 18 mg/cm 2 . Comparing with the cell in Comparative Example 2, the NCM-Li 2 O 2 -catalyst cathode in Example 7 exhibits more charge capacity in the 1 st charge, and shows better capacity retention during charge/discharge cycles.
  • Figure 13 compares discharge/charge profiles of the cells prepared according to Example 8 and Comparative Example 3 for the first charge/discharge cycle.
  • Figure 14 compares cycling performances of the cells prepared according to Example 8 and Comparative Example 3. Comparing with the cell in Comparative Example 3, the NCM-Li 2 O 2 -catalyst cathode in Example 8 exhibits more charge capacity in the 1 st charge, and shows better capacity retention during charge/discharge cycles.

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Abstract

L'invention concerne une nouvelle batterie lithium-ion, qui comprend une cathode, une anode et un électrolyte, la cathode contenant un matériau actif cathodique et du peroxyde de lithium. L'invention concerne également un procédé de préparation de la batterie lithium-ion.
PCT/CN2016/111329 2016-12-21 2016-12-21 Batterie lithium-ion et son procédé de production WO2018112801A1 (fr)

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DE112016007530.8T DE112016007530T5 (de) 2016-12-21 2016-12-21 Lithium-ionen-batterie und herstellungsverfahren dafür
CN201680091755.4A CN110100335A (zh) 2016-12-21 2016-12-21 锂离子电池及其制备方法
KR1020197017721A KR20190095928A (ko) 2016-12-21 2016-12-21 리튬 이온 배터리 및 그 제조 방법

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CN110896143A (zh) * 2018-09-13 2020-03-20 宁德时代新能源科技股份有限公司 锂离子电池
WO2020091428A1 (fr) * 2018-10-30 2020-05-07 주식회사 엘지화학 Accumulateur au lithium
WO2020233799A1 (fr) 2019-05-21 2020-11-26 Wacker Chemie Ag Batteries lithium-ion
CN114207876A (zh) * 2019-07-22 2022-03-18 宝马股份公司 具有过氧化锂的阴极活性材料、用于锂离子电池的阴极、锂离子电池以及被涂层的过氧化锂在锂离子电池中的应用
WO2022262981A1 (fr) 2021-06-17 2022-12-22 Wacker Chemie Ag Procédé de prélithiation d'anode contenant du silicium dans une batterie au lithium-ion

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CN112615043A (zh) * 2020-08-26 2021-04-06 清陶（昆山）能源发展有限公司 一种全固态锂离子电池
CN112271281B (zh) * 2020-10-22 2023-01-13 欣旺达电动汽车电池有限公司 复合正极材料及其制备方法、应用和锂离子电池

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Cited By (9)

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Publication number Priority date Publication date Assignee Title
CN110896143A (zh) * 2018-09-13 2020-03-20 宁德时代新能源科技股份有限公司 锂离子电池
EP3624237A3 (fr) * 2018-09-13 2020-04-15 Contemporary Amperex Technology Co., Limited Batterie au lithium-ion
CN110896143B (zh) * 2018-09-13 2021-08-06 宁德时代新能源科技股份有限公司 锂离子电池
US11239501B2 (en) 2018-09-13 2022-02-01 Contemporary Amperex Technology Co., Limited Lithium-ion battery
WO2020091428A1 (fr) * 2018-10-30 2020-05-07 주식회사 엘지화학 Accumulateur au lithium
WO2020233799A1 (fr) 2019-05-21 2020-11-26 Wacker Chemie Ag Batteries lithium-ion
CN114207876A (zh) * 2019-07-22 2022-03-18 宝马股份公司 具有过氧化锂的阴极活性材料、用于锂离子电池的阴极、锂离子电池以及被涂层的过氧化锂在锂离子电池中的应用
CN114207876B (zh) * 2019-07-22 2024-05-24 宝马股份公司 具有过氧化锂的阴极活性材料、用于锂离子电池的阴极、锂离子电池以及被涂层的过氧化锂在锂离子电池中的应用
WO2022262981A1 (fr) 2021-06-17 2022-12-22 Wacker Chemie Ag Procédé de prélithiation d'anode contenant du silicium dans une batterie au lithium-ion

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