CN104347846A - Preparation method for safety-improved nickel-cobalt lithium manganate positive electrode sheet - Google Patents
Preparation method for safety-improved nickel-cobalt lithium manganate positive electrode sheet Download PDFInfo
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- 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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Abstract
The present invention discloses a safety-improved nickel-cobalt lithium manganate battery, which comprises a positive electrode sheet, a negative electrode sheet, separation membrane paper and an electrolyte. A purpose of the present invention is to improve the safety performance of the nickel-cobalt lithium manganate battery and ensure the use safety of the nickel-cobalt lithium manganate battery under the improper state. According to the present invention, the positive electrode active material adopting the nickel-cobalt lithium manganate as the main material is added with a small amount of lithium iron phosphate and lithium manganate materials with the good safety so as to improve the safety of the positive electrode sheet and the battery.
Description
Technical field
The present invention relates to field of lithium ion battery, more particularly, the positive plate that the present invention relates to a kind of higher economic usability and fail safe and the secondary lithium battery prepared by this positive plate.
Background technology
Current, compared with ni-mh, nickel-cadmium cell, lithium ion battery maintains the leading position with absolute predominance in 3C (computer, communication, consumption electronic product) field; Meanwhile, in order to adapt to energy-conserving and environment-protective requirement, electric motor car (comprising electric bicycle and electric automobile) has wide market prospects.As the power source of electric motor car, lithium ion battery has very large competitiveness.No matter be 3C consumer electronics field or electric motor car application, parallel connection and series connection use must be carried out in a certain way owing to making battery to the high request of power supply energy.This battery cell of instructions for use in groups of battery must have good consistency.But, due to the restriction of current battery manufacturing process, equipment and the difference of raw material supplied materials performance, cause the consistency of lithium ion battery (especially high-capacity battery) to be improved; In addition, battery is when using in groups, and often because placement location is different, the environment of heat radiation is not equal, makes the actual performance capacity difference to some extent of battery.Such battery is very easy to overcharge or cross put in actual use, causes the potential safety hazard that battery is serious.
As the positive electrode that a class is novel, nickle cobalt lithium manganate possesses higher energy density, cheap price and good cycle performance, and nickle cobalt lithium manganate has become the competitive material of 3C Product and the automobile-used lithium ion battery of electrical salf-walking.But because the ratio shared by nickel is higher, the layer structure formed in process manufactured by material is not very complete to the nickel-cobalt lithium manganate material of existing market routine (as: nickel: cobalt: manganese=5: 2: 3,4: 4: 2 etc.).When battery makes when the tight or improper use of environmental Kuznets Curves, the structural imperfection of nickle cobalt lithium manganate easily causes the cycle performance of battery to decay the series of problems such as large, poor safety performance (especially acupuncture, overcharge).When combo uses, this defect is more remarkable, amplificationization.
In view of this, be necessary to provide a kind of modification, have higher-security can nickle cobalt lithium manganate positive plate and the lithium rechargeable battery prepared thus.
Summary of the invention
The object of the invention is to: for the deficiencies in the prior art, a kind of positive plate with higher-security and the lithium rechargeable battery prepared thus are provided.
A kind of lithium-ion secondary battery positive plate, comprise plus plate current-collecting body and be coated in the positive pole diaphragm on plus plate current-collecting body, described positive pole diaphragm comprises positive active material, conductive agent and binding agent, described positive active material is the mixture of LiFePO4, nickle cobalt lithium manganate and LiMn2O4, and the weight ratio of described nickle cobalt lithium manganate, LiFePO4 and LiMn2O4 is 60: 20: 20 ~ 98: 1: 1.
Relative to existing nickle cobalt lithium manganate battery technology, containing nickle cobalt lithium manganate, LiMn2O4 and LiFePO4 in the positive plate of lithium rechargeable battery of the present invention; Nickle cobalt lithium manganate has higher gram specific volume capacity, nominal platform voltage 3.7V.But the structural imperfection of this material easily causes the poor heat stability of gained battery, anti-over-charging poor performance, be especially embodied in its poor acupuncture performance and almost become a difficult problem for industry; LiFePO4 Stability Analysis of Structures, Heat stability is good, security performance is excellent, and shortcoming is that platform voltage and tap density are lower; LiMn2O4 ore resources is abundanter, cheap, and platform voltage is up to 3.8V, and security performance is excellent, and overcharging resisting superior performance, shortcoming is that gram volume is low, and the gram volume as high temperature modification LiMn2O4 is only 100 ~ 105mAh/g.Therefore, the present invention proposes the LiFePO4 of nickle cobalt lithium manganate and security performance excellence and LiMn2O4 to mix, and prepares the high security nickel-cobalt lithium manganate cathode material of modified version.In the positive electrode of gained, the raising that the having of high voltage composition (i.e. LiMn2O4) is beneficial to composite material charging/discharging voltage platform and by nickle cobalt lithium manganate larger with particle diameter for LiFePO4 (D50:1 ~ 3 micron) less for particle diameter and LiMn2O4 (D50:10 ~ 14 micron) by the tap density that can improve gained composite material that mixes of different quality ratio, be conducive to the raising of battery capacity.And then LiFePO4 and the lower cost of LiMn2O4 have established the higher economic usability of blended anode material of the present invention.
In composite material, the combination property of weight ratio to resulting materials of nickle cobalt lithium manganate, LiFePO4, LiMn2O4 gets critical effect.On the one hand, the blended anode material capacitance of nickle cobalt lithium manganate content less (such as, lower than 60%) is less; On the other hand, if positive active material is not containing LiFePO4 and the complementation of LiMn2O4 capacity, easily causes when improper use overcharging, cause potential safety hazard.
One as lithium-ion secondary battery positive plate of the present invention is improved, and the weight ratio of described nickle cobalt lithium manganate, LiFePO4, LiMn2O4 is 60: 20: 20 ~ 98: 1: 1.
One as lithium-ion secondary battery positive plate of the present invention is improved, and described conductive agent is at least one in carbon black, the carbon fiber of vapor phase growth, superconduction carbon black and electrically conductive graphite.
One as the positive plate of lithium rechargeable battery of the present invention is improved, and described binding agent is polyvinylidene fluoride (PVDF).
Another object of the present invention is to provide a kind of lithium ion battery, comprises positive plate, negative plate, is interval in diaphragm paper between both positive and negative polarity, and electrolyte.Described positive plate is above-described composite material positive plate, because the active material in this positive plate uses the mixture of nickle cobalt lithium manganate, LiFePO4, LiMn2O4, makes this lithium ion battery have higher fail safe and economic use value.
The present invention adds LiFePO4 and LiMn2O4 in nickel-cobalt lithium manganate material, without the need to preparing new material, just being carried out mixing by these three kinds of materials, therefore not only reducing material cost, also improve material safety, and simple to operate.
Embodiment
Below in conjunction with specific embodiment, the present invention is described in further detail.But embodiments of the invention are not limited thereto.
Comparative example
The preparation of positive plate: take nickle cobalt lithium manganate as positive active material, its weight content (relative to powder weight, below roughly the same) is 94%; With polyvinylidene fluoride (PVDF) for binding agent, its weight content is 2.0%; With carbon black and electrically conductive graphite for conductive agent, its weight content is respectively 3.0% and 1.0%.Above-mentioned material is stirred by the mode be dry mixed, add solvent methyl pyrrole slightly alkane ketone (NMP) stir and make anode sizing agent.Be uniformly coated on by anode sizing agent on plus plate current-collecting body aluminium foil, through cutting after oven dry compacting, welding anode ear, sticks high tempreture tape and obtains positive plate.
The preparation of negative plate: take Delanium as negative active core-shell material, its weight content is 94%; With sodium cellulose glycolate (CMC) for thickener, its weight content is 1.7%; With carbon black (S-P) for conductive agent, its weight content is respectively 2%.Add deionized water after being stirred by the mode be dry mixed by above-mentioned material and carry out Keep agitation, add SBR emulsion (SBR) (weight content is 2.3%) evenly and stir and make cathode size.Cathode size is uniformly coated on negative current collector Copper Foil, through cut-parts, welding negative lug after oven dry compacting, sticks high tempreture tape and obtain negative plate.
The preparation of barrier film: take polyethene microporous membrane as barrier film.
The preparation of electrolyte: take lithium hexafluoro phosphate as lithium salts, with the mixture of propene carbonate (PC), ethylene carbonate (EC) and dimethyl carbonate (DMC) for solvent, the weight ratio of propene carbonate, ethylene carbonate and dimethyl carbonate is PC: EC: DMC=1: 1: 1.After being dissolved in mixed solvent by lithium hexafluoro phosphate (concentration is 1.0M), then add the electrolysis additive vinylene carbonate (VC) of 1%.
The preparation of lithium ion battery: after negative plate obtained for previous process, positive plate, barrier film are superposed successively, battery core is obtained by winding process, battery core is proceeded in battery packages shell, inwardly inject electrolyte, obtained comparative example lithium rechargeable battery after the operation such as changing into.
Embodiment one
The preparation of positive plate: with the mixture of nickle cobalt lithium manganate, LiFePO4, LiMn2O4 (weight ratio is for 60: 20: 20) for positive active material, its weight content is 93.2%; With polyvinylidene fluoride (PVDF) for binding agent, its weight content is 2.80%; With carbon black and electrically conductive graphite for conductive agent, its weight content is respectively 3% and 1%.Above-mentioned material is stirred by the mode be dry mixed, add solvent methyl pyrrole slightly alkane ketone (NMP) stir and make anode sizing agent.Be uniformly coated on by anode sizing agent on plus plate current-collecting body aluminium foil, through cutting after oven dry compacting, welding anode ear, sticks high tempreture tape and obtains positive plate.
The preparation of negative plate: take Delanium as negative active core-shell material, its weight content is 94%; With sodium cellulose glycolate (CMC) for thickener, its weight content is 1.7%; With carbon black (S-P) for conductive agent, its weight content is respectively 2%.Add deionized water after being stirred by the mode be dry mixed by above-mentioned material and carry out Keep agitation, add SBR emulsion (SBR) (weight content is 2.3%) evenly and stir and make cathode size.Cathode size is uniformly coated on negative current collector Copper Foil, through cut-parts, welding negative lug after oven dry compacting, sticks high tempreture tape and obtain negative plate.
The preparation of barrier film: take polyethene microporous membrane as barrier film.
The preparation of electrolyte: take lithium hexafluoro phosphate as lithium salts, with the mixture of propene carbonate (PC), ethylene carbonate (EC) and dimethyl carbonate (DMC) for solvent, the weight ratio of propene carbonate, ethylene carbonate and dimethyl carbonate is PC: EC: DMC=1: 1: 1.After being dissolved in mixed solvent by lithium hexafluoro phosphate (concentration is 1.0M), then add the electrolysis additive vinylene carbonate (VC) of 1%.
The preparation of lithium ion battery: after negative plate obtained for previous process, positive plate, barrier film are superposed successively, battery core is obtained by winding process, battery core is proceeded in battery packages shell, inwardly inject electrolyte, obtained embodiment one lithium rechargeable battery after the operation such as changing into.
Embodiment two
The preparation of positive plate: with the mixture of nickle cobalt lithium manganate, LiFePO4, LiMn2O4 (weight ratio is for 80: 10: 10) for positive active material, its weight content is 93.2%; With polyvinylidene fluoride (PVDF) for binding agent, its weight content is 2.80%; With carbon black and electrically conductive graphite for conductive agent, its weight content is respectively 3% and 1%.Above-mentioned material is stirred by the mode be dry mixed, add solvent methyl pyrrole slightly alkane ketone (NMP) stir and make anode sizing agent.Be uniformly coated on by anode sizing agent on plus plate current-collecting body aluminium foil, through cutting after oven dry compacting, welding anode ear, sticks high tempreture tape and obtains positive plate.
The preparation of negative plate: take Delanium as negative active core-shell material, its weight content is 94%; With sodium cellulose glycolate (CMC) for thickener, its weight content is 1.7%; With carbon black (S-P) for conductive agent, its weight content is respectively 2%.Add deionized water after being stirred by the mode be dry mixed by above-mentioned material and carry out Keep agitation, add SBR emulsion (SBR) (weight content is 2.3%) evenly and stir and make cathode size.Cathode size is uniformly coated on negative current collector Copper Foil, through cut-parts, welding negative lug after oven dry compacting, sticks high tempreture tape and obtain negative plate.
The preparation of barrier film: take polyethene microporous membrane as barrier film.
The preparation of electrolyte: take lithium hexafluoro phosphate as lithium salts, with the mixture of propene carbonate, ethylene carbonate and dimethyl carbonate for solvent, the weight ratio of propene carbonate, ethylene carbonate and dimethyl carbonate is 1: 1: 1.After being dissolved in mixed solvent by lithium hexafluoro phosphate (concentration is 1.0M), then add the electrolysis additive vinylene carbonate (VC) of 1%.
The preparation of lithium ion battery: after negative plate obtained for previous process, positive plate, barrier film are superposed successively, battery core is obtained by winding process, battery core is proceeded in battery packages shell, inwardly inject electrolyte, obtained embodiment two lithium rechargeable battery after the operation such as changing into.
Embodiment three
The preparation of positive plate: with the mixture of nickle cobalt lithium manganate, LiFePO4, LiMn2O4 (weight ratio is for 90: 5: 5) for positive active material, its weight content is 93.2%; With polyvinylidene fluoride (PVDF) for binding agent, its weight content is 2.80%; With carbon black and electrically conductive graphite for conductive agent, its weight content is respectively 3% and 1%.Above-mentioned material is stirred by the mode be dry mixed, add solvent methyl pyrrole slightly alkane ketone (NMP) stir and make anode sizing agent.Be uniformly coated on by anode sizing agent on plus plate current-collecting body aluminium foil, through cutting after oven dry compacting, welding anode ear, sticks high tempreture tape and obtains positive plate.
The preparation of negative plate: take Delanium as negative active core-shell material, its weight content is 94%; With sodium cellulose glycolate (CMC) for thickener, its weight content is 1.7%; With carbon black (S-P) for conductive agent, its weight content is respectively 2%.Add deionized water after being stirred by the mode be dry mixed by above-mentioned material and carry out Keep agitation; Add SBR emulsion (SBR) (weight content is 2.3%) evenly to stir and make cathode size.Cathode size is uniformly coated on negative current collector Copper Foil, through cut-parts, welding negative lug after oven dry compacting, sticks high tempreture tape and obtain negative plate.
The preparation of barrier film: take polyethene microporous membrane as barrier film.
The preparation of electrolyte: take lithium hexafluoro phosphate as lithium salts, with the mixture of propene carbonate, ethylene carbonate and dimethyl carbonate for solvent, the weight ratio of propene carbonate, ethylene carbonate and dimethyl carbonate is 1: 1: 1.After being dissolved in mixed solvent by lithium hexafluoro phosphate (concentration is 1.0M), then add the electrolysis additive vinylene carbonate (VC) of 1%.
The preparation of lithium ion battery: after negative plate obtained for previous process, positive plate, barrier film are superposed successively, by the battery core that winding process is obtained, battery core is proceeded in battery packages shell, inwardly inject electrolyte, obtained embodiment three lithium rechargeable battery after the operation such as changing into.
By the lithium rechargeable battery of comparative example, embodiment one, embodiment two and embodiment three at 25 DEG C with 0.5C constant-current constant-voltage charging to 4.2V, cut-off current 0.02C, shelves 5 minutes, with 0.5C constant-current discharge to 2.75V, shelves 5 minutes.Loop test like this is after five weeks, and with 0.5C constant-current constant-voltage charging to 4.2V, cut-off current 0.02C, shelves 24 hours, carries out safety test and compares.Every test carries out parallel testing with three batteries (3PCS).
As shown in the table, draw to draw a conclusion by contrast:
Be the single lithium battery that pure nickel-cobalt lithium manganate cathode material obtains described in comparative example, volume energy density is 560WH/L, in security testing process, acupuncture 3PCS explode, on fire, overcharge (3C10V) 1PCS to pass through, 2PCS blast, on fire, security performance is poor.Nickel-cobalt lithium manganate cathode material doped iron lithium phosphate described in embodiment three and LiMn2O4, ratio is 90: 5: 5, obtained single lithium battery volume energy density is 545WH/L, in security testing process, acupuncture 2PCS passes through, 1PCS is on fire, blast, overcharges (3C10V) 3PCS and all passes through.Illustrate by doping fail safe is further improved, especially in overcharging.The volume energy density of embodiment two, embodiment one is respectively 540WH/L and 530WH/L, and all safety tests are all passed through.Illustrating that doped scheme not only maintains the advantage of nickle cobalt lithium manganate higher volumes energy density, fundamentally solve again the safety issue of battery, is a kind of simple to operate, the Ways to improve that cost performance is higher.
The present invention is not limited in embodiment disclosed and described above, allly to modify based on basic thought of the present invention or in all belonging to of changing, protection of the present invention enclosed.
Claims (5)
1. a lithium-ion secondary battery positive plate, comprise plus plate current-collecting body and be coated in the positive pole diaphragm on plus plate current-collecting body, described positive pole diaphragm comprises positive active material, conductive agent and caking property, it is characterized in that: described positive active material is the mixture of nickle cobalt lithium manganate, LiFePO4, LiMn2O4.
2. press the lithium-ion secondary battery positive plate described in claim 1, it is characterized in that: in described positive active material, the weight ratio of nickle cobalt lithium manganate, LiFePO4, LiMn2O4 is 60: 20: 20 ~ 98: 1: 1.
3. press the lithium-ion secondary battery positive plate described in claim 1, it is characterized in that: described conductive agent is at least one in carbon black, gas-phase growth of carbon fibre, superconduction carbon black and electrically conductive graphite.
4. press the lithium-ion secondary battery positive plate described in claim 1, it is characterized in that: described binding agent is polyvinylidene fluoride (PVDF).
5. a lithium ion battery, comprises positive plate, negative plate, is interval in the diaphragm paper between positive plate negative plate, and electrolyte, it is characterized in that: the positive plate of described positive plate according to any one of Claims 1-4.
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105449269A (en) * | 2016-01-08 | 2016-03-30 | 深圳市沃特玛电池有限公司 | Lithium ion battery |
| CN105932222A (en) * | 2016-05-11 | 2016-09-07 | 东莞市久森新能源有限公司 | Conductive slurry and preparation method thereof, electrode plate coated with conductive slurry, and lithium ion battery |
| CN107204463A (en) * | 2017-06-16 | 2017-09-26 | 河南福森新能源科技有限公司 | A kind of based lithium-ion battery positive plate |
| CN107394124A (en) * | 2017-06-07 | 2017-11-24 | 天津中科先进技术研究院有限公司 | Lithium iron phosphate trace-doped ternary positive electrode material positive plate, preparation method thereof and power lithium ion battery |
| CN107528050A (en) * | 2017-08-08 | 2017-12-29 | 上海华普汽车有限公司 | Active substance of lithium ion battery anode, positive electrode, positive electrode slurry, positive plate, its preparation method and lithium ion battery |
| CN108232174A (en) * | 2018-01-31 | 2018-06-29 | 北京国能电池科技股份有限公司 | Positive electrode active materials, lithium ion battery and preparation method thereof |
| CN111883771A (en) * | 2020-09-14 | 2020-11-03 | 天津斯科兰德科技有限公司 | Lithium ion battery positive electrode material, positive plate and lithium ion battery |
| CN112290011A (en) * | 2020-09-28 | 2021-01-29 | 广西卓能新能源科技有限公司 | Preparation method of water-based lithium ion battery positive active material slurry and positive plate |
| CN112335089A (en) * | 2020-03-31 | 2021-02-05 | 宁德新能源科技有限公司 | Electrochemical device and battery pack |
| CN114686058A (en) * | 2020-12-31 | 2022-07-01 | 北京卫国创芯科技有限公司 | Single-layer or multi-layer polymer protective film, preparation method thereof and application thereof in lithium metal battery |
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