CN106058168A - Prelithiated positive electrode material for lithium ion secondary battery - Google Patents
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
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- 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
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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
- H01M4/36—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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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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
- H01M4/36—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
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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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
- H01M4/36—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
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- H—ELECTRICITY
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- H01M4/00—Electrodes
- 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
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention discloses a prelithiated positive electrode material for a lithium ion secondary battery. The prelithiated positive electrode material for the lithium ion secondary battery is prepared from, by weight, 88 to 95 parts of a positive electrode active substance, 0.5 to 3 parts of a conductive agent, 0.7 to 4 parts of a bonding agent and 2 to 10 parts of nanometer lithium fluoride. According to the invention, a formula for the positive electrode material is optimized, and in particular, nanometer lithium fluoride is added; so the whole positive electrode material is prelithiated, has good stability, and can improve the initial delithiation capacity, initial charge and discharge efficiency and energy density of the battery.
Description
Technical field
The present invention relates to a kind of anode material for lithium-ion batteries, especially relate to a kind of prelithiation lithium ion secondary electricity
Pond positive electrode.
Background technology
In recent years, the fast development in the fields such as portable type electronic product/electric automobile/energy-accumulating power station, energy is store
The technology of depositing is had higher requirement.Lithium ion battery becomes these fields due to its high energy density at present
Primary selection, but still its requirement to energy density can not be met.
Lithium ion battery generally includes following ingredient: can embed/deintercalation or alloying/remove alloy
Changing the both positive and negative polarity of lithium ion, both positive and negative polarity directly fills the electrolyte with lithium ion conduction effect, between both positive and negative polarity
There is the barrier film cutting off electronics conduction, and the adnexa such as collector/lug/outer package.Positive electrode carries
Medium-lithium ion for lithium ion battery energy storage；Electrolyte provides the conduction pathway of lithium ion；Negative pole is made
For the received vector of lithium ion, typically do not contain lithium ion.Lithium ion battery passes through lithium ion between both positive and negative polarity
Conduction and lithiumation/go physical and chemical reaction to realize storage and the release of energy, therefore lithium ion in lithium ion battery
Amount determines the energy density of battery.Owing to electrolyte occurs redox reaction on both positive and negative polarity surface, formed steady
Fixed solid electrolyte film (SEI), the composition of this film is alkylcarbonic acid esters organic lithium salt and other inorganic lithiums
Salt, consumes lithium ion, just reduces the utilization rate of lithium ion in positive electrode, reduces the capacity of lithium ion battery
And energy density.
For this present situation, every industry or trade and scientific research institution equal active development prelithiation technology, its principle is:
Lithium metal or other lithium-containing compounds is additionally added, for the lithium that the formation offer of SEI is enough when negative pole makes
Source, thus reduce the loss of the lithium ion in positive pole, improve capacity and the energy density of battery.Prelithiation at present
Technology mainly includes following two: one is the addition lithium powder when negative pole makes；Two is that negative plate is carried out electrochemistry
Lithiumation or chemistry lithiumation process, and form SEI in the outer system of battery.Both approaches all can effectively reduce
The loss of lithium ion in positive pole, improves capacity and the energy density of battery.Relevant main patent has: Zhejiang
University's patent 104993104A by metal-oxide/silica-base material/lithium hydride/CO2 gas is carried out spheroidal graphite,
Form prelithiation material；Chinese Academy of Sciences chemistry institute patent 104630575 A utilizes Al to become electricity with assembled metal
Chi Hou, forms the Al electrode of prelithiation；House journal of LG Corporation 104584278A utilizes by pole piece extremely
In reactive tank, the method for the charging of lithium metallic plate is utilized to carry out prelithiation；The Tianjin bar not science and technology limited public affairs of share
Department patent 104538591 A uses lithium metal anticathode to carry out prelithiation；The patent of Li Zhenqi/Liu Lijun
104538630 A then use lithium metal to react with chelating agent, and anticathode material carries out chemistry lithiumation, and needs
High temperature strengthens prelithiation reaction；Patent 102642024A of Ningde new forms of energy scientific & technical corporation then uses polymer bag
The lithium metal anticathode covered realizes prelithiation process.
But, all there is the problems such as complex process/preparation condition harshness in above two prelithiation method.Wherein lithium
Powder activity is relatively strong, needs to carry out polymer overmold or strictly controlled environment temperature and temperature and atmosphere, improves
Cost；Anticathode sheet carries out the technological means of electrochemistry lithiumation or chemistry lithiumation process then needs extra lithium
Changing the pole piece activity after technical matters, and prelithiation relatively strong, temperature/humidity and atmosphere to environment are wanted
Ask the most harsh.Therefore, there is complex process/environmental Kuznets Curves and require the shortcomings such as harsh in current prelithiation technology.
Summary of the invention
The present invention be in order to solve the lithium ion battery of prior art can reduce in use in positive electrode lithium from
The problem of the utilization rate of son, it is provided that a kind of compatibility is reasonable, can improve battery and take off lithium capacity, first charge and discharge first
The prelithiation lithium ion secondary battery anode material of electrical efficiency and energy density.
To achieve these goals, the present invention is by the following technical solutions:
A kind of prelithiation lithium ion secondary battery anode material, described prelithiation lithium ion secondary battery anode material
Being made up of the component of following weight portion: 88～95 parts of positive active materials, 0.5～3 part of conductive agent, 0.7～4 part is glued
Connect agent, 2～10 parts of nano-lithium fluorides.Optimal improvements of the present invention positive electrode formula, especially with the addition of nanometer
Lithium fluoride, nano-lithium fluoride is different from pre existing lithiation reagent, its stable chemical nature, be difficult to in air
Gas reacts, it is possible to stable existence in suitable environment, and storage technological requirement is low, can be directly as adding
Add agent to be added in anode sizing agent, prepare pole piece together with positive electrode, to existing process conditions without particular/special requirement,
Reducing technique manufacture and environmental Kuznets Curves cost, the Li-F key occurred under high voltages furthermore with lithium fluoride breaks
Split process, be possible not only to provide lithium ion into battery, moreover it is possible to provide F doping possible for positive electrode, improve
The stability of positive electrode.
As preferably, described positive active material is lithium nickel cobalt manganese ternary material or rich lithium manganese base solid solution material.
As preferably, described lithium nickel cobalt manganese ternary material formula is LiNixM(1-x)O2, wherein M=Co, Mn,
One or more in Al, 0.6≤x is less than 1.
As preferably, described rich lithium manganese base solid solution material formula is xLi2MnO3(1～x) LiYO2, wherein,
Y is the one in Co, Mn, Mg, Ni, Cr, Al, Ti, Mo, Nd, and 0 ＜ x ＜ 1.
As preferably, described conductive agent is the one or many in acetylene black, Ketjen black, Super P-Li, ECP
Kind.
As preferably, described binding agent is PVDF.
As preferably, described nano-lithium fluoride prepares by the following method: analytically pure lithium fluoride is placed in inertia
In the ball-grinding machine of atmosphere protection, spheroidal graphite 12～48h, i.e. obtain nano-lithium fluoride.Prepared by ball milling, no
Relating to harsh environmental Kuznets Curves, processing step is simple, and workable and prepared nano-lithium fluoride is not
There is spontaneous combustion probability, there is the advantages such as safety/cheap.
Therefore, there is advantages that Optimal improvements positive electrode formula, especially with the addition of
Nano-lithium fluoride so that whole positive electrode prelithiation, good stability, can improve battery take off first lithium capacity,
First charge-discharge efficiency and energy density.
Detailed description of the invention
Below by detailed description of the invention, the present invention will be further described.
Embodiment 1
(1) analytically pure lithium fluoride is placed in the ball-grinding machine of inert atmosphere protection, spheroidal graphite 12h, to obtain final product
To nano-lithium fluoride, stand-by；
(2) 88g positive electrode active material lithium-nickel-cobalt manganese ternary material LiNi is pressed0.5Co0.2Mn0.3O2, 0.5g conducts electricity
Agent acetylene black, 0.7g bonding agent PVDF, the proportioning of 2g nano-lithium fluoride weighs each component, each component is added
Organic solvent is made anode sizing agent.
Embodiment 2
(1) analytically pure lithium fluoride is placed in the ball-grinding machine of inert atmosphere protection, spheroidal graphite 20h, to obtain final product
To nano-lithium fluoride, stand-by；
(2) 90g positive electrode active material lithium-nickel-cobalt manganese ternary material LiNi0.4Co0.2Mn0.4O is pressed2, 2g leads
Electricity agent acetylene black and Ketjen black (mass ratio 1:1), 2g bonding agent PVDF, the proportioning of 5g nano-lithium fluoride claims
Take each component, each component is added in organic solvent and makes anode sizing agent.
Embodiment 3
(1) analytically pure lithium fluoride is placed in the ball-grinding machine of inert atmosphere protection, spheroidal graphite 48h, to obtain final product
To nano-lithium fluoride, stand-by；
(2) by 88～95 parts of positive active material rich lithium manganese base solid solution material 0.8Li2MnO3·0.8LiMoO2,
3g conductive agent Super P-Li, 4g bonding agent PVDF, the proportioning of 10g nano-lithium fluoride weighs each component, will
Each component adds in organic solvent makes anode sizing agent.
The slurry each embodiment made is coated, be dried, roll and make positive plate, uses graphite as negative pole
Sheet, is assembled into the full battery that model is 2025, and the full battery made carries out first week efficiency for charge-discharge test,
The result of test is as follows:
| Sample | Efficiency |
| Embodiment 1 | 85.4% |
| Embodiment 2 | 80.2% |
| Embodiment 3 | 84.3% |
From upper table it will be seen that the prelithiation lithium ion secondary battery anode material of the present invention can be effectively improved full electricity
The coulombic efficiency in pond, shows good chemical stability and active electrochemical stability, can be to secondary lithium
The electrode of ion battery carry out mend lithium, can be applicable to electric automobile, hybrid vehicle, mobile electronic device and
Other electronic products.
Embodiment described above is the one preferably scheme of the present invention, and the present invention not makees any form
On restriction, on the premise of without departing from the technical scheme described in claim, also have other variant and change
Type.
Claims (7)
1. a prelithiation lithium ion secondary battery anode material, it is characterised in that described prelithiation lithium ion secondary
Cell positive material is made up of the component of following weight portion: 88～95 parts of positive active materials, 0.5～3 part of conduction
Agent, 0.7～4 part of bonding agent, 2～10 parts of nano-lithium fluorides.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 1, it is characterised in that
Described positive active material is lithium nickel cobalt manganese ternary material or rich lithium manganese base solid solution material.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 2, it is characterised in that
Described lithium nickel cobalt manganese ternary material formula is LiNixM(1-x)O2, wherein the one in M=Co, Mn, Al or
Multiple, 0.6≤x is less than 1.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 2, it is characterised in that
Described rich lithium manganese base solid solution material formula is xLi2MnO3(1～x) LiYO2, wherein, Y is Co, Mn,
One in Mg, Ni, Cr, Al, Ti, Mo, Nd, and 0 ＜ x ＜ 1.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 1, it is characterised in that
Described conductive agent is one or more in acetylene black, Ketjen black, Super P-Li, ECP.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 1, it is characterised in that
Described binding agent is PVDF.
A kind of prelithiation lithium ion secondary battery anode material the most according to claim 1, it is characterised in that
Described nano-lithium fluoride prepares by the following method: analytically pure lithium fluoride is placed in the ball milling of inert atmosphere protection
In equipment, spheroidal graphite 12～48h, i.e. obtain nano-lithium fluoride.
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Cited By (21)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2018137169A1 (en) * | 2017-01-25 | 2018-08-02 | 罗伯特·博世有限公司 | Lithium ion battery and preparation method therefor |
| CN108365174A (en) * | 2018-03-23 | 2018-08-03 | 复旦大学 | A kind of prelithiation method of anode material for lithium-ion batteries |
| CN109473668A (en) * | 2018-10-26 | 2019-03-15 | 溧阳天目先导电池材料科技有限公司 | A kind of modified prelithiation material and preparation method thereof and lithium battery |
| CN109560257A (en) * | 2017-09-25 | 2019-04-02 | 银隆新能源股份有限公司 | A kind of lithium ion battery anode glue size and preparation method thereof |
| CN109638237A (en) * | 2018-11-26 | 2019-04-16 | 华南理工大学 | A kind of compound anode material for lithium-ion batteries and preparation method thereof |
| CN109888274A (en) * | 2018-12-24 | 2019-06-14 | 中国电子科技集团公司第十八研究所 | Pre-lithiated lithium ion battery positive electrode material and preparation method thereof |
| CN110061202A (en) * | 2019-03-18 | 2019-07-26 | 合肥国轩高科动力能源有限公司 | Preparation method of ternary battery positive pole piece and ternary battery |
| CN110176641A (en) * | 2019-06-03 | 2019-08-27 | 哈尔滨工业大学 | A kind of nanometer of LiF/Fe/ graphite anode mends the preparation method and applications of lithium slurry |
| CN110212184A (en) * | 2019-06-04 | 2019-09-06 | 安徽科达新材料有限公司 | A kind of prelithiation method of carbon negative electrode material of lithium ion cell |
| CN110233244A (en) * | 2019-06-28 | 2019-09-13 | 北京科技大学 | A kind of nickelic tertiary cathode material particle surface stabilization treatment method |
| EP3573143A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium anode and method for its manufacture |
| EP3573142A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Cathode assembly and method for its manufacture |
| EP3573144A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium ion cell and method of producing the same |
| EP3573141A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium anode and method for its manufacture |
| CN111600020A (en) * | 2020-05-27 | 2020-08-28 | 常州赛得能源科技有限公司 | Lithium ion battery and preparation method thereof |
| CN111799457A (en) * | 2020-07-30 | 2020-10-20 | 广东邦普循环科技有限公司 | Pre-lithiation-treated lithium ion positive electrode material and preparation method and application thereof |
| CN112271279A (en) * | 2020-10-22 | 2021-01-26 | 欣旺达电动汽车电池有限公司 | Composite cathode material, preparation method and application thereof, and lithium ion battery |
| CN113314699A (en) * | 2021-04-09 | 2021-08-27 | 上海工程技术大学 | Lithium ion battery anode material and preparation method thereof |
| CN113937255A (en) * | 2020-06-29 | 2022-01-14 | 北京卫蓝新能源科技有限公司 | Lithium ion battery composite positive electrode material and preparation method and application thereof |
| CN114586194A (en) * | 2019-12-19 | 2022-06-03 | 宝马股份公司 | Lithium ion battery and method for producing a lithium ion battery |
| WO2022156706A1 (en) * | 2021-01-21 | 2022-07-28 | 宁德新能源科技有限公司 | Positive electrode plate and electrochemical device and electronic device comprising positive electrode plate |
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| WO2018137169A1 (en) * | 2017-01-25 | 2018-08-02 | 罗伯特·博世有限公司 | Lithium ion battery and preparation method therefor |
| CN109560257A (en) * | 2017-09-25 | 2019-04-02 | 银隆新能源股份有限公司 | A kind of lithium ion battery anode glue size and preparation method thereof |
| CN108365174A (en) * | 2018-03-23 | 2018-08-03 | 复旦大学 | A kind of prelithiation method of anode material for lithium-ion batteries |
| EP3573141A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium anode and method for its manufacture |
| CN110534747B (en) * | 2018-05-25 | 2022-11-29 | 大众汽车有限公司 | Cathode arrangement and method for producing the same |
| US11276854B2 (en) | 2018-05-25 | 2022-03-15 | Volkswagen Aktiengesellschaft | Lithium anode and method for producing same |
| CN110534747A (en) * | 2018-05-25 | 2019-12-03 | 大众汽车有限公司 | Cathode assembly and method for manufacturing the cathode assembly |
| EP3573143A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium anode and method for its manufacture |
| EP3573142A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Cathode assembly and method for its manufacture |
| EP3573144A1 (en) | 2018-05-25 | 2019-11-27 | Volkswagen Aktiengesellschaft | Lithium ion cell and method of producing the same |
| CN109473668A (en) * | 2018-10-26 | 2019-03-15 | 溧阳天目先导电池材料科技有限公司 | A kind of modified prelithiation material and preparation method thereof and lithium battery |
| CN109638237A (en) * | 2018-11-26 | 2019-04-16 | 华南理工大学 | A kind of compound anode material for lithium-ion batteries and preparation method thereof |
| CN109888274A (en) * | 2018-12-24 | 2019-06-14 | 中国电子科技集团公司第十八研究所 | Pre-lithiated lithium ion battery positive electrode material and preparation method thereof |
| CN110061202A (en) * | 2019-03-18 | 2019-07-26 | 合肥国轩高科动力能源有限公司 | Preparation method of ternary battery positive pole piece and ternary battery |
| CN110176641A (en) * | 2019-06-03 | 2019-08-27 | 哈尔滨工业大学 | A kind of nanometer of LiF/Fe/ graphite anode mends the preparation method and applications of lithium slurry |
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| CN111600020A (en) * | 2020-05-27 | 2020-08-28 | 常州赛得能源科技有限公司 | Lithium ion battery and preparation method thereof |
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