CN103165897A - A cathode material for lithium-ion batteries, lithium-ion battery cathodes, and lithium-ion batteries - Google Patents
A cathode material for lithium-ion batteries, lithium-ion battery cathodes, and lithium-ion batteries Download PDFInfo
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- CN103165897A CN103165897A CN2011104162711A CN201110416271A CN103165897A CN 103165897 A CN103165897 A CN 103165897A CN 2011104162711 A CN2011104162711 A CN 2011104162711A CN 201110416271 A CN201110416271 A CN 201110416271A CN 103165897 A CN103165897 A CN 103165897A
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- ion batteries
- anode material
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- 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
Abstract
The present invention provides a cathode material for lithium-ion batteries, including a cathode active material and an additive, wherein the additive is Li[x]Ni[y]Mn[z]O[2], (0.8 =< x=<1.2, 0 <y <1, and 0 <z <1). Based on the percentage content of the cathode material of the lithium-ion battery, the content of the additive is not more than 15%. The present invention also provides lithium-ion battery cathodes made from the cathode material for lithium-ion batteries and lithium-ion batteries. Lithium ion batteries made from the cathode material for lithium-ion batteries provided in the invention can better solve the problem of the battery over discharge.
Description
Technical field
The present invention relates to the lithium ion battery field, relate in particular to a kind of anode material for lithium-ion batteries, lithium ion cell positive and lithium ion battery.
Background technology
Compare with other chemical power source, lithium ion battery has the performance of many excellences, as high in energy density, have extended cycle life, the advantages such as open circuit voltage is high, memory-less effect, safety non-pollution.Through the develop rapidly of recent two decades, lithium ion battery has been widely used in the fields such as mobile phone, notebook computer, digital camera.Along with the rise of global oil price and the enhancing of people's environmental consciousness, no matter be research institution or enterprise, all sight is concerned about in the exploitation of electric automobile.The researcher generally believes that lithium ion battery is a kind of most potential chemical power source that is applied on electric automobile.Compare with other mobile device, electric automobile proposes higher requirement to the performances such as cycle life, energy density, consistency of battery pack and large current discharging capability of battery.
In order to improve the security performance of lithium ion battery; the mistake that prevents lithium ion battery is put; usually adopt protective circuit that battery is protected in prior art; but adopt the cost of protective circuit higher; and adopt protective circuit the pressure limiting effect to be arranged to cell; cause whole PACK Capacity fading very fast, therefore, need to seek a kind of more suitable lithium ion battery that prevents and cross the technical scheme of putting.
Summary of the invention
The present invention prevented the dissatisfactory technical problem of the scheme of putting for solving existing lithium ion battery, and a kind of novel anode material for lithium-ion batteries is provided, and comprised positive electrode active materials and additive, and wherein, additive is Li
xNi
yMn
zO
2, 0.8≤x≤1.2,0＜y＜1,0＜z＜1; Take the percentage composition of anode material for lithium-ion batteries as benchmark, the content of additive is not higher than 15%.
The mistake that adopts the lithium ion battery of positive electrode provided by the present invention preparation can better solve battery is put problem.
The present invention provides a kind of lithium ion cell positive simultaneously, is coated on positive electrode collector after being mixed with slurry by anode material for lithium-ion batteries provided by the present invention together with conductive agent, binding agent and solvent, and drying, calendering prepare.
The present invention also provides lithium ion battery simultaneously, comprises battery container and is sealed in this battery container interior electrode group and electrolyte; The electrode group comprises positive pole, negative pole and the barrier film between positive pole and negative pole, wherein, and just very above-mentioned positive pole.
The present inventor is unexpected to be found, adds content not higher than 15% Li in anode material for lithium-ion batteries
xNi
yMn
zO
2, 0.8≤x≤1.2,0＜y＜1,0＜z＜1 wherein, the lithium ion battery that makes of positive electrode has and better prevented putting performance thus.Infer its former because: the additive in positive electrode is after initial charge discharges lithium, material structure partly caves in, the part of caving in can not be returned the embedding lithium again, and this part lithium has been stayed in negative pole because had more than needed out, and cross when putting when battery, because there is the lithium of this part reservation to exist, the negative pole current potential rises slowly (stable negative electrode potential), is unlikely to be raised to fast to analyse the copper current potential, cause short circuit, thereby play the effect that prevents or delayed to put.Additive used in the present invention, because its cycle performance is very poor, can not directly be used as the positive electrode active materials of lithium ion battery, normally by those skilled in the art gave up, and the invention such material has been applied in the positive electrode of lithium ion battery, and the content that adds is not high, just plays the effect of an additive, and the anti-mistake that just can obviously mention lithium ion battery is put performance.
Embodiment
In order to make technical problem solved by the invention, technical scheme and beneficial effect clearer, below in conjunction with embodiment, the present invention is further elaborated.Should be appreciated that specific embodiment described herein only in order to explain the present invention, is not intended to limit the present invention.
The invention provides a kind of anode material for lithium-ion batteries, comprise positive electrode active materials and additive, wherein, additive is Li
xNi
yMn
zO
2, 0.8≤x≤1.2,0＜y＜1,0＜z＜1; Take the percentage composition of anode material for lithium-ion batteries as benchmark, the content of additive is not higher than 15%.
In anode material for lithium-ion batteries provided by the invention, preferred, additive is Li
0.95Ni
0.84Mn
0.21O
2, LiNi
0.5Mn
0.5O
2, Li
1.01Ni
0.85Mn
0.15O
2, Li
1.01Ni
0.89Mn
0.1O
2, Li
1.076Ni
0.628Mn
0.624O
2Or Li
1.2Ni
0.2Mn
0.6O
2In one or more.
In anode material for lithium-ion batteries provided by the invention, preferred, the D of additive
50Not higher than 5 microns, D
maxNot higher than 9 microns; Further preferred, the D of additive
50At 0.5-2 micron, D
maxNot higher than 5 microns, material is mixed more even, lithium more than needed can be evenly distributed on negative plate.Wherein, D
50Refer to meso-position radius, D
maxRefer to maximum particle diameter.In anode material for lithium-ion batteries provided by the invention, preferred, take the percentage composition of anode material for lithium-ion batteries as benchmark, the content of additive is 5-8%, also improves the overall performance of battery when the mistake that improves lithium ion battery is put performance.
Positive electrode active materials of the present invention can be any positive active material that can be purchased in prior art, for example, can adopt all positive active materials that can be purchased, as LiFePO
4, Li
3V
2(PO
4)
3, LiMn
2O
4, LiMnO
2, LiNiO
2, LiCoO
2Or LiVPO
4In F one or more.Preferably, the grain diameter of positive electrode active materials is D
50Not higher than 15 microns, D
90Not higher than 30 microns; Further preferred, the D of positive electrode active materials
50Not higher than 2 microns, D
90Not higher than 10 microns.Wherein, D
50Refer to meso-position radius, D
90Corresponding particle diameter when referring to that the cumulative particle sizes distribution number reaches 90%.
in anode material for lithium-ion batteries provided by the invention, positive electrode active materials is preferably LiFePO4, because with LiFePO4 during as positive electrode active materials, in the lithium ion battery discharge process, the discharge curve of LiFePO4 is all different from the discharge curve of any positive electrode active materials, its plateau potential is the 3.45V left and right, this platform is very flat, almost can think a straight line that is parallel to X-axis, but arrived the discharge end, its curve is not slow decreasing like other positive electrode active materials like that, but almost be an angle of 90 degrees straight glide, like this at discharge voltage below 2.0V when the discharge voltage of the operated by rotary motion (limit), how many capacity LiFePO4 has remained hardly, be under identical discharging current condition, discharge time is very short, illustrate that at this time negative pole does not have lithium to deviate from substantially, to such an extent as to the negative pole current potential is easy to rise to reach analyse the copper current potential, the copper dendrite that forms like this is easy to pierce through barrier film and causes battery short circuit, produce safety problem, crossing and putting the probability that causes short circuit is almost 100%, therefore, adding additive during as positive electrode active materials with LiFePO4, can better alleviate this problem, play and better prevented the effect of putting.
The present invention provides a kind of lithium ion cell positive simultaneously, is coated on positive electrode collector after being mixed with slurry by anode material for lithium-ion batteries provided by the present invention together with conductive agent, binding agent and solvent, and drying, calendering prepare.When preparing anode sizing agent by anode material for lithium-ion batteries provided by the present invention, conductive agent used, binding agent and solvent etc. can be various material known in those skilled in the art, ratio the present invention of anodal activity, conductive agent, binding agent and solvent also is not particularly limited, can adjust flexibly material concentration according to the viscosity of the slurry coating of the composition of battery electrode positive electrode, binding agent and positive electrode to be prepared and the requirement of operability, mode is conventionally known to one of skill in the art.In general take the total amount of positive electrode as benchmark, the consumption of binding agent is 2%-9%, and the consumption of conductive agent is 2%-8%; The consumption of solvent is 60%-90%.
Wherein, positive electrode collector is positive electrode collector known in those skilled in the art, for example can be selected from aluminium foil, Copper Foil or various Punching steel strip.
Wherein, drying, the step of calendering, the same with prior art, namely drying usually under vacuum condition at 50-160 ℃, carry out under preferred 80-150 ℃, dry after dispersant can exist also in pole piece and can not exist.Calendering can be adopted this area rolling condition commonly used, such as the 0.5-3.0 MPa.
Anodal preparation can also comprise other steps, for example, the cut-parts of reprocessing, cut-parts are known to the skilled person, and after calendering is completed, cut according to the anodal size of prepared battery request, obtain anode pole piece.
The present invention provides lithium ion battery simultaneously, comprises battery container and is sealed in this battery container interior electrode group and electrolyte; The electrode group comprises positive pole, negative pole and the barrier film between positive pole and negative pole, wherein, and just very above-mentioned positive pole.Because the present invention only relates to improvement to the prior art lithium ion cell positive, therefore other the Nomenclature Composition and Structure of Complexes of lithium ion battery had no particular limits.
Wherein, membrane layer can be selected from and well known to a person skilled in the art various membrane layers used in lithium ion battery, for example polyolefin micro porous polyolefin membrane (PP), polyethylene felt (PE), glass mat or ultra-fine fibre glass paper or PP/PE/PP.As preferred embodiment a kind of, described barrier film is PP/PE/PP.
Wherein, negative pole can adopt this area negative pole in common knowledge, namely contains negative electrode collector and the negative material that is coated on this negative electrode collector.Collector body can adopt the various collector bodies that are used for lithium ion battery negative in prior art, as stamped metal, metal forming, net metal and foamed metal, and preferred Copper Foil.Anticathode material of the present invention has no particular limits, can be the same with prior art, and described negative material generally includes negative electrode active material and negative pole binding agent.
Negative electrode active material can adopt all negative electrode active materials that can be purchased, as graphite and lithium titanium oxygen compound.The kind of negative pole binding agent and content are conventionally known to one of skill in the art, for example one or more in fluorine resin and polyolefin compound such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), butadiene-styrene rubber (SBR) and sodium carboxymethylcellulose (CMC); In general, according to the difference of binding agent kind used, with respect to the negative electrode active material of 100 weight portions, the content of negative pole binding agent is the 0.005-8 weight portion, is preferably the 0.008-5 weight portion.The preparation method of negative pole is similar with anodal preparation method, is not described in detail in this.
Electrolyte contains lithium salts and nonaqueous solvents, and lithium salts can be one or more in lithium hexafluoro phosphate, LiBF4, hexafluoroarsenate lithium, lithium perchlorate, trifluoromethyl sulfonic acid lithium, perfluoro butyl Sulfonic Lithium, lithium aluminate, chlorine lithium aluminate, fluoro sulfimide lithium, lithium chloride and lithium iodide; Nonaqueous solvents can be for gamma-butyrolacton, methyl ethyl carbonate, methyl propyl carbonate, dipropyl carbonate, acid anhydrides, 1-METHYLPYRROLIDONE, N-METHYLFORMAMIDE, N-methylacetamide, acetonitrile, DMF, sulfolane, methyl-sulfoxide, dimethyl sulfite and other is fluorine-containing, sulfur-bearing or contain one or more in the ring-type organic ester of unsaturated bond.The concentration of lithium salts in electrolyte can be the 0.3-4 mol/L, is preferably the 0.5-2 mol/L.
The preparation method of lithium ion battery provided by the invention can be well known for the person skilled in the art method, in general, the method comprises anodal, negative pole and the barrier film between positive pole and the negative pole formation pole piece of reeling successively, pole piece is inserted in battery case, add electrolyte, then sealing, wherein, described positive pole comprises collector and the positive electrode that loads on collector.Wherein, the method for coiling and sealing is that those skilled in the art are known.The consumption of electrolyte is conventional amount used.
Unless stated otherwise, various solvent of the present invention and reagent are commercially available analytical reagent.
Below in conjunction with specific embodiment, the present invention is further described.
Embodiment 1
(1) anodal preparation:
With the iron phosphate serving as positive active material of 80g, the additive Li of 20g
1.01Ni
0.89Mn
0.1O
2, the binding agent Kynoar (PVDF) of 4g, the conductive agent SP of 5g, the polyethylene of dispersing agent pyrrolidones (PVP) of 0.5g and the 1-METHYLPYRROLIDONE of 120g join to stir in de-airing mixer and form uniform positive electrode.This positive electrode is uniformly coated on the both sides of the aluminium foil of 20 microns of thickness, the then lower oven dry of 150 degree.Again through roll-in, cut the positive plate that obtains size 453*40 millimeter.
(2) preparation of negative pole:
With the native graphite of 50g, the binding agent butadiene-styrene rubber of 1g breast (SBR), the binding agent carboxymethyl cellulose (CMC) of 0.5g, the deionized water of 125g join to stir in de-airing mixer and form uniform negative material.This negative material is coated on the both sides that thickness is the Copper Foil of 12 microns equably, then oven dry under 90 ℃.Again through roll-in, cut, make the negative plate that is of a size of the 455*41 millimeter.
(3) preparation of battery:
Respectively above-mentioned positive and negative electrode and polypropylene screen are wound into the pole piece of a square lithium ion battery, subsequently with LiPF
6Be dissolved in by the concentration of 1 mol/L in the mixed solvent of EC/EMC/DEC=1:1:1 and form nonaqueous electrolytic solution, this electrolyte is injected battery aluminum shell with the amount of 3.8g/Ah, sealing changes into, and makes lithium ion battery.
Embodiment 2
Adopt that the preparation of the method identical with embodiment 1 and step is anodal, negative pole and battery, the additive that different is in positive electrode is the Li of 5g
1.076Ni
0.628Mn
0.624O
2, positive electrode active materials is the LiFePO4 of 95g.
Embodiment 3
Adopt that the preparation of the method identical with embodiment 1 and step is anodal, negative pole and battery, the additive that different is in anode sizing agent is the Li of 10g
0.95Ni
0.84Mn
0.21O
2, positive electrode active materials is the LiFePO4 of 90g.
Embodiment 4
Adopt that the preparation of the method identical with embodiment 1 and step is anodal, negative pole and battery, the additive that different is in anode sizing agent is the Li of 8g
1.2Ni
0.2Mn
0.6O
2, positive electrode active materials is the LiFePO4 of 92g.
Embodiment 5
Adopt that the preparation of the method identical with embodiment 1 and step is anodal, negative pole and battery, the additive that different is in anode sizing agent is the LiNi of 10g
0.5Mn
0.5O
2, positive electrode active materials is the LiFePO4 of 90g.
Comparative Examples 1
(1) anodal preparation:
Iron phosphate serving as positive active material with 100g, the binding agent Kynoar (PVDF) of 4g, the conductive agent SP of 5g, the polyethylene of dispersing agent pyrrolidones (PVP) of 0.5g, the 1-METHYLPYRROLIDONE of 120g join to stir in de-airing mixer and form uniform positive electrode.This positive electrode is uniformly coated on the both sides of the aluminium foil of 20 microns of thickness, the then lower oven dry of 150 degree.Again through roll-in, cut the positive plate that obtains size 453*40 millimeter.
(2) preparation of negative pole:
With the native graphite of 50g, the binding agent butadiene-styrene rubber of 1g breast (SBR), the binding agent carboxymethyl cellulose (CMC) of 0.5g, the deionized water of 125g join to stir in de-airing mixer and form uniform negative material.This negative material is coated on the both sides that thickness is the Copper Foil of 12 microns equably, then oven dry under 90 ℃.Again through roll-in, cut and make the negative plate that is of a size of the 455*41 millimeter.
(3) preparation of battery:
Respectively above-mentioned positive and negative electrode and polypropylene screen are wound into the pole piece of a square lithium ion battery, subsequently with LiPF
6Be dissolved in by the concentration of 1 mol/L in the mixed solvent of EC/EMC/DEC=1:1:1 and form nonaqueous electrolytic solution, this electrolyte is injected battery aluminum shell with the amount of 3.8g/Ah, sealing changes into, and makes lithium ion battery.
Electrochemical property test:
The battery of embodiment 1-5 and Comparative Examples 1 preparation is placed on new Weir-3000 type electrochemical property test instrument, charges to 4.3V with 0.1C, shelved 10 minutes, then be discharged to 2.0V with 0.1C.Then this battery is prepared into three electrodes, charges to 3.6V with 0.5C, shelved 10 minutes, then be discharged to 2.0V with 0.5C, uninterrupted, then continue to discharge into 0V with 0.5C.Record discharge capacity and the battery discharge capacity when 2.0V above of battery under 2.0-1.0V, the ratio value of the discharge capacity of battery when the shared 2.0V of the discharge capacity under 2.0-1.0V is above is recorded in table 1.Simultaneously, when battery discharge was arrived 1.0V, the potential value of battery cathode was recorded in table 1.
Table 1
| Embodiment | 2.0V the discharge capacity (%) that discharge capacity/2.0V of ~ 1.0V is above | Battery discharge is during to 1.0V, the current potential of battery cathode (V) |
| Embodiment 1 | 8 | 0.25 |
| Embodiment 2 | 7.6 | 0.25 |
| Embodiment 3 | 5 | 0.36 |
| Embodiment 4 | 6.1 | 0.30 |
| Embodiment 5 | 3.5 | 0.45 |
| Comparative Examples 1 | 0.8 | 1.1 |
Can be found out by data in table 1, the battery of embodiment 1-5 in the discharge capacity under the 2.0-1.0V condition with respect to the discharge capacity of battery under the above condition of 2.0V, proportion is higher, and the capacity that Comparative Examples 1 can be emitted under the 2.0-1.0V condition is low-down, put under condition can the stable negative electrode potential crossing for the battery that embodiment 1-5 is described, make the negative pole current potential be unlikely to be raised to fast and analyse the copper current potential, cause short circuit, thereby play the effect that prevents or delayed to put; Simultaneously, when battery discharge arrives 1.0V, and in Comparative Examples the negative pole current potential higher than 0.6V, at the negative pole current potential during higher than 0.6V, the formed SEI film of negative pole, thus make battery performance obviously worsen, and easily cause safety problem, and in embodiment 1-5, all lower than 0.6V, can't there be this problem in the negative pole current potential, and battery is significantly improved in the security performance under condition to one's heart's content.
The above is only preferred embodiment of the present invention, not in order to limiting the present invention, all any modifications of doing within the spirit and principles in the present invention, is equal to and replaces and improvement etc., within all should being included in protection scope of the present invention.
Claims (10)
1. an anode material for lithium-ion batteries, comprise positive electrode active materials and additive, it is characterized in that, described additive is Li
xNi
yMn
zO
2, 0.8≤x≤1.2,0＜y＜1,0＜z＜1 wherein; Take the percentage composition of anode material for lithium-ion batteries as benchmark, the content of described additive is not higher than 15%.
2. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, take the percentage composition of anode material for lithium-ion batteries as benchmark, the content of described additive is 5-8%.
3. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, described additive is Li
0.95Ni
0.84Mn
0.21O
2, LiNi
0.5Mn
0.5O
2, Li
1.01Ni
0.85Mn
0.15O
2, Li
1.01Ni
0.89Mn
0.1O
2, Li
1.076Ni
0.628Mn
0.624O
2Or Li
1.2Ni
0.2Mn
0.6O
2In one or more.
4. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, the D of described additive
50Not higher than 5 microns, D
maxNot higher than 9 microns.
5. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, the D of described additive
50At 0.5-2 micron, D
maxNot higher than 5 microns.
6. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, described positive electrode active materials is LiFePO4.
7. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, the D of described positive electrode active materials
50Not higher than 15 microns, D
90Not higher than 30 microns.
8. anode material for lithium-ion batteries as claimed in claim 1, is characterized in that, the D of described positive electrode active materials
50Not higher than 2 microns, D
90Not higher than 10 microns.
9. lithium ion cell positive, it is characterized in that, described lithium ion cell positive is coated on positive electrode collector after being mixed with slurry by the described anode material for lithium-ion batteries of any one in claim 1-8 together with conductive agent, binding agent and solvent, and drying, calendering prepare.
10. a lithium ion battery, is characterized in that, comprises battery container and be sealed in this battery container interior electrode group and electrolyte; Described electrode group comprises positive pole, negative pole and the barrier film between positive pole and negative pole, wherein, and described lithium ion cell positive just very claimed in claim 9.
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| US20080008933A1 (en) * | 2005-12-23 | 2008-01-10 | Boston-Power, Inc. | Lithium-ion secondary battery |
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| CN101471441A (en) * | 2007-12-27 | 2009-07-01 | 比亚迪股份有限公司 | Active substance of lithium ion battery anode and preparation method thereof |
| CN101667658A (en) * | 2009-10-20 | 2010-03-10 | 梅岭化工厂 | Iron phosphate lithium-based blended anode material series lithium ion battery |
| CN101901892A (en) * | 2009-05-26 | 2010-12-01 | 上海比亚迪有限公司 | Lithium-ion secondary battery anode and lithium-ion secondary battery |
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2011
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| US5429890A (en) * | 1994-02-09 | 1995-07-04 | Valence Technology, Inc. | Cathode-active material blends of Lix Mn2 O4 |
| CN1700498A (en) * | 2004-05-22 | 2005-11-23 | 比亚迪股份有限公司 | A Li-ion secondary battery |
| US20080008933A1 (en) * | 2005-12-23 | 2008-01-10 | Boston-Power, Inc. | Lithium-ion secondary battery |
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| CN103165897B (en) | 2016-04-27 |
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