CN105609869A - High-specific-energy and high-safety lithium ion power battery based on high-nickel ternary material - Google Patents
High-specific-energy and high-safety lithium ion power battery based on high-nickel ternary material 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
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- 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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Abstract
The invention discloses a lithium ion power battery. The lithium ion power battery comprises a positive electrode pole piece, a negative electrode pole piece and a membrane, wherein a positive electrode material on the positive electrode pole piece is composed of a positive electrode active substance, a conducting agent, a binding agent and a safety addition agent; the positive electrode active substance is a high-nickel ternary material LiNixCoyMn1-x-yO2, wherein x is more than or equal to 0.8 and less than or equal to 0.9, y is more than or equal to 0.05 and the sum of the x and the y is smaller than or equal to 1; meanwhile, the safety addition agent is introduced and the high-temperature-resisting ceramic membrane is used, so that the safety of the battery is guaranteed when the high-energy-density lithium ion power battery is prepared; and compared with current commercial lithium ion power batteries, the energy density and the safety are remarkably improved.
Description
Technical field
The invention belongs to lithium battery field, relate to lithium-ion-power cell, relate in particular to a kind of based on nickelic ternaryPositive electrode, high-energy-density highly secure lithium ion dynamic battery.
Background technology
As the breach of cracking the energy, environmental problem and realizing new wave of economic growth, main state in the worldFamily is using new-energy automobile industry as national strategy new industry. Electrokinetic cell is zero of the core of new-energy automobilePart, directly determines the performance of car load. Lithium-ion-power cell has that energy density is high, the feature such as have extended cycle life,In electric automobile, have been used in a large scale. Based on the expection to lithium ion battery technological progress in industry, itsApplication scale is rapid growth, in following 10～20 years by dominate.
The energy density of vehicle lithium-ion power battery product is generally distributed within the scope of 120～180Wh/kg at present,For further meeting the long mileage demand of pure electric automobile, how promoting energy content of battery density becomes government and each grand dukeThe difficult problem that department faces. According to relevant high in China's " energy-conservation with new-energy automobile industrial development planning 2012～2020 "The planning of specific energy lithium ion battery product index, to 2015, cell energy density required to reach 200Wh/kg,To the year two thousand twenty, cell energy density requires to reach 350Wh/kg. China's automobile-used lithium ion power in earlier stageBattery mainly adopts ferric phosphate lithium cell, and theoretical gram volume only has 170mAh/g, and operating voltage is 3.20V, andLiNixCoyMn1-x-yO2The theoretical gram volume of ternary material can reach 278mAh/g, and operating voltage is 3.65V, phosphorusThe energy density of acid lithium iron battery the highlyest only can arrive 130Wh/kg, but ternary material battery can be accomplishedMore than 150Wh/kg. With LiNixCoyMn1-x-yO2Ternary material is example, the main dependence of its actual gram volume performanceWith the number of Ni content in material, as LiNi0.5Co0.2Mn0.3O2The about 170mAh/g of the actual gram volume of ternary material,And LiNi0.8Co0.1Mn0.1O2The actual gram volume of nickelic ternary material can reach 200mAh/g. But, withLiNixCoyMn1-x-yO2The increase of middle nickel content, can bring again multiple negative effect, as SunYang-Kook etc.Report (JournalofPowerSources, 2013,233,121-130), the thermally-stabilised of nickelic ternary material becomesPoorer, will bring the safety issue of battery thus. This has also limited nickelic tertiary cathode material at lithium-ion electricApplication in pond and the more exploitation of high energy density lithium ion electrokinetic cell.
And for automobile with for power source, the safety problem of electrokinetic cell is stood in the breach. If can be for nickelicThe safety problem that material brings at lithium-ion-power cell, finds a kind of reasonably solution, and this will be forHigh-energy-density ternary lithium-ion-power cell applying on electric automobile based on nickelic ternary material hasImportant meaning.
In the Chinese patent application of publication number CN102544436A, the people such as Wang Zongxiong disclose positive electrode knotStructure and preparation method thereof, positive electrode structure comprises positive electrode active materials main body and is coated containing containing skeleton on itNitrogen high molecular polymer and nanometer conductive material composite membrane, by dividing nanometer conductive material and positive electrode active materialsDo not add in the reaction solution containing skeleton nitrogen containing polymer polymer monomer and react, obtain upgrading type positive electrode,Thereafter prepare lithium ion battery by the known method assembling in this area, the battery preparing has wellSecurity performance. In the Chinese patent application of publication number CN103050706A, Zhu Zheng is first by cyanamide and threePoly cyanamid and maleimide pyroreaction in NMP obtains containing the maleimide additive of cyanamide modification moltenLiquid, joins this solution after thereafter conventional anode sizing agent being prepared again, and lithium ion battery, electricity are prepared in assemblingPond has good security performance. But above patent battery preparation process complexity, has increased the cost of battery greatly.
Therefore, in the urgent need to finding a kind of lithium-ion-power cell that has high security and high-energy-density concurrently.
Summary of the invention
The present invention seeks to a kind of high safe high-energy-density lithium-ion-power cell based on nickelic ternary material,To solve the demand of the high-energy-density lithium-ion-power cell of existing electric automobile to high safety.
For achieving the above object, the present invention is by the following technical solutions:
A kind of lithium-ion-power cell, comprises anode pole piece, cathode pole piece and barrier film, and anode pole piece is collected by positive poleFluid and the positive electrode being coated on plus plate current-collecting body form, and cathode pole piece is by negative current collector and be coated in negativeNegative material on utmost point collector forms. Positive electrode on anode pole piece by positive active material, conductive agent,Binding agent and safe additive composition, wherein, described positive active material is nickelic ternary materialLiNixCoyMn1-x-yO2, wherein 0.8≤x≤0.9, y >=0.05, x+y≤1; Preferably, 0.8≤x≤0.9,0.05≤y≤0.1,X+y≤1; More preferably, 0.85≤x≤0.9,0.05≤y≤0.1, x+y≤1; Most preferably, 0.85≤x≤0.9,0.05≤y≤0.1,x+y≤0.95。
Advantageously, nickelic ternary material LiNixCoyMn1-x-yO2D50Be 8～15 μ m, surface area is0.2～0.6m2/ g, tap density is >=2.0g/cm3；
According to aforesaid lithium-ion-power cell, wherein, described safe additive is bismaleimide amine polymerPowder, is formed by BMI and barbiturates or derivatives thereof polymerisation, and number-average molecular weight is100000-500000, preferably, number-average molecular weight is 200000-500000, more preferably, number-average molecular weight is300000-500000。
The example of described BMI includes, but not limited to N, N '-ethene-BMI, N, and N '-Butylene-BMI, N, N '-hexa-methylene-BMI, N, N '-penylene-BMI,N, N '-4,4 '-diphenyl methane-BMI, N, N '-4,4 '-diphenyl ether-BMI, N, N '-4,4 '-Diphenyl sulphone (DPS)-BMI, N, N '-4,4 '-dicyclohexyl methyl hydride-BMI, N, N '-benzene first two bases-BMI and N, N '-diphenyl cyclohexane-BMI. Described barbiturates or derivatives thereof asShown in following formula:
Wherein, R1And R2Be H, C independently of one another1-20Alkyl or C5-12Aryl. Work as R1And R2While being H,Be barbiturates.
Advantageously, polymer powder needs powder to be dissolved in the solution that forms 1-20% in NMP in use, makesUsed time, first positive electrode active materials is disperseed in solution, add again thereafter conductive agent, binding agent just to prepareUtmost point slurry.
According to aforesaid lithium-ion-power cell, wherein, the positive active material of described positive electrode, conductive agent,The weight proportion of binding agent and safe additive is (88～95): (1～4.5): (3～6): (0.5～4.5). Preferably,The weight proportion of positive active material, conductive agent, binding agent and the safe additive of described positive electrode is(90～95)：(1～4.5)：(3～4)：(3～4.5)。
According to aforesaid lithium-ion-power cell, wherein, the negative material on described cathode pole piece is by negative electrode activeMaterial, conductive agent, binding agent composition.
According to aforesaid lithium-ion-power cell, wherein, the negative electrode active material of described negative material, conductive agent,The weight proportion of binding agent is (90～96): (0.5～2): (3.5～8). Preferably, the negative pole of described negative material is livedThe weight proportion of property material, conductive agent, binding agent is (93～96): (0.5～2): (3.5～5).
According to aforesaid lithium-ion-power cell, wherein, described negative electrode active material is Delanium.
Advantageously, Delanium is high power capacity Delanium, D50For 15-25 μ m, surface area is 2～5m2/g，Tap density is 0.8～1.2g/cm3。
According to aforesaid lithium-ion-power cell, wherein, the conductive agent of described negative or positive electrode material is identical or notWith, be selected from one or more the combination in conductive black, electrically conductive graphite, VGCF, CNT, Graphene.
According to aforesaid lithium-ion-power cell, wherein, the binding agent of described negative or positive electrode material is PVDF.
According to aforesaid lithium-ion-power cell, wherein, described barrier film is refractory ceramics barrier film.
According to aforesaid lithium-ion-power cell, wherein, described refractory ceramics barrier film be 10～25 μ mPE orOn PP basement membrane, apply 2～5 μ m aluminum oxide coating layers of one or both sides.
Compared with prior art, the present invention is owing to adopting nickelic ternary material LiNixCoyMn1-x-yO2(0.8≤x≤0.9，Y >=0.05, x+y≤1) as positive electrode active materials, the gram volume of prepared lithium-ion-power cell reaches200mAh/g, energy content of battery density is greater than 200Wh/kg. Introducing by safe additive simultaneously and use resistance to heightThe ceramic diaphragm of temperature has ensured the peace of battery in preparing the lithium-ion-power cell of high-energy-densityQuan Xing.
Detailed description of the invention
Below in conjunction with detailed description of the invention, the present invention will be further described
In the present invention, if not refer in particular to, all percentage is unit of weight, and all devices and raw material all can be fromMarket is buied or the industry is conventional, and the method in following embodiment, if no special instructions, is this areaConventional method.
Embodiment 1
Synthesizing of BMI polymer powder: by N, N '-hexa-methylene-BMI and barbitalAcid, according to mol ratio 1:1 reaction, after centrifugal, washing, drying process, obtains above-mentioned BMI poly-Compound powder.
Make positive and negative electrode pole piece: the bismaleimide amine polymer that is 100000 by 0.5% number-average molecular weight peaceFull additive is dissolved in NMP, and forming containing safe additive is 1%NMP solution, then by 88% nickelic ternary materialMaterial LiNi0.8Co0.1Mn0.1O2Be dispersed in nmp solution, thereafter, (2% leads to add 4% conductive agentElectricity carbon black+2% electrically conductive graphite), 6% PVDF binding agent dispersed with stirring evenly prepares anode sizing agent, will be justAfter utmost point slurry is coated on plus plate current-collecting body by drying, roll-in, cut and obtain anode pole piece; By 90% peopleMake graphite, 2% conductive agent (1% conductive black+1% electrically conductive graphite), 8% PVDF binding agent is dispersedIn NMP, obtain cathode size, cathode size is coated on negative current collector after by drying, roll-in, sanctionCut and obtain cathode pole piece;
Battery core assembling: stack successively and make battery core, electricity by cathode pole piece, refractory ceramics barrier film, anode pole pieceCore both sides outermost layer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Embodiment 2
Make positive and negative electrode pole piece: the bismaleimide amine polymer that is 500000 by 4.5% number-average molecular weight peaceFull additive is dissolved in NMP, and forming containing safe additive is 20%NMP solution, then by 95% nickelic ternaryMaterial LiNi0.85Co0.1Mn0.05O2Be dispersed in nmp solution, thereafter, add 1% conductive agent (0.5%Conductive black+0.5%VGCF), 3% PVDF binding agent dispersed with stirring evenly prepares anode sizing agent, willAfter anode sizing agent is coated on plus plate current-collecting body by drying, roll-in, cut and obtain anode pole piece; By 96%Delanium, 0.5% conductive agent (0.5%CNT), 3.5% PVDF binding agent are dispersed in NMPObtain cathode size, cathode size is coated on negative current collector after by drying, roll-in, cut and bornUtmost point pole piece;
Battery core assembling: stack successively and make battery core, electricity by cathode pole piece, refractory ceramics barrier film, anode pole pieceCore both sides outermost layer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Embodiment 3
Make positive and negative electrode pole piece: the bismaleimide amine polymer that is 300000 by 3% number-average molecular weight peaceFull additive is dissolved in NMP, and forming containing safe additive is 10%NMP solution, then by 90% nickelic ternaryMaterial LiNi0.9Co0.05Mn0.05O2Be dispersed in nmp solution, thereafter, add 4.5% conductive agent (2%Conductive black+2%VGCF+0.5% Graphene), 4% PVDF binding agent dispersed with stirring just evenly preparingUtmost point slurry, anode sizing agent is coated on plus plate current-collecting body after by drying, roll-in, cut and obtain anode pole piece;By equal to 93% Delanium, 2% conductive agent (1% conductive black+1%CNT), 5% PVDF binding agentIn the even NMP of being scattered in, obtain cathode size, cathode size is coated on negative current collector after by drying, rollerPress, cut and obtain cathode pole piece;
Battery core assembling: stack successively and make battery core, electricity by cathode pole piece, refractory ceramics barrier film, anode pole pieceCore both sides outermost layer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Comparative example 1
Make positive and negative electrode pole piece: the bismaleimide amine polymer that is 300000 by 3% number-average molecular weight peaceFull additive is dissolved in NMP, and forming containing safe additive is 10%NMP solution, then by 90% ternary materialLiNi0.6Co0.2Mn0.2O2Be dispersed in nmp solution, thereafter, add 4.5% conductive agent (2% conductionCarbon black+2%VGCF+0.5% Graphene), 4% PVDF binding agent dispersed with stirring evenly prepares anodal slurryMaterial, anode sizing agent is coated on plus plate current-collecting body after by drying, roll-in, cut and obtain anode pole piece; Will93% Delanium, 2% conductive agent (1% conductive black+1%CNT), 5% PVDF binding agent are evenBe scattered in NMP and obtain cathode size, cathode size is coated on negative current collector after by drying, roll-in,Cut and obtain cathode pole piece;
Battery core assembling: stack successively and make battery core, electricity by cathode pole piece, refractory ceramics barrier film, anode pole pieceCore both sides outermost layer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Comparative example 2
Make positive and negative electrode pole piece: by 90% nickelic ternary material LiNi0.85Co0.1Mn0.05O2, 4.5% leadElectricity agent (2% conductive black+2%VGCF+0.5% Graphene), 4% PVDF binding agent are dispersed in containing peaceIn the NMP of full additive, obtain anode sizing agent, anode sizing agent is coated on plus plate current-collecting body after by drying,Roll-in, cut and obtain anode pole piece; By 93% Delanium, 2% conductive agent (1% conductive black+ 1%CNT), 5% PVDF binding agent is dispersed in NMP and obtains cathode size, cathode size is coated withAfter being overlying on negative current collector by drying, roll-in, cut and obtain cathode pole piece;
Battery core assembling: stack successively and make battery core by cathode pole piece, barrier film, anode pole piece, battery core both sides outermostLayer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Comparative example 3
Make positive and negative electrode pole piece: by 90% nickelic ternary material LiNi0.6Co0.2Mn0.2O2, 4.5% conductionAgent (2% conductive black+2%VGCF+0.5% Graphene), 4% PVDF binding agent are dispersed in containing safetyIn the NMP of additive, obtain anode sizing agent, anode sizing agent is coated on plus plate current-collecting body after by drying, rollerPress, cut and obtain anode pole piece; By 93% Delanium, 2% conductive agent (1% conductive black+1%CNT),5% PVDF binding agent is dispersed in NMP and obtains cathode size, and cathode size is coated on to negative pole collectionAfter on fluid by drying, roll-in, cut and obtain cathode pole piece;
Battery core assembling: stack successively and make battery core, electricity by cathode pole piece, refractory ceramics barrier film, anode pole pieceCore both sides outermost layer is cathode pole piece; ,, obtain the packaging battery core of one-sided opening through welding, heat-sealing thereafter;
Fluid injection with change into: electrolyte is injected to packaging battery core from a side of opening, then carries out vacuum-pumping and sealing;By battery shelve, preliminary filling, two envelopes, change into, after partial volume, the lithium ion power electricity that the capacity of obtaining is 22AhPond.
Energy density test
Energy density test is carried out according to GB/T31486-2015, at 25 ± 2 DEG C, by battery with 22A constant currentBe discharged to 2.8V, leave standstill after 1 hour, turn constant-voltage charge during to 4.2V with 22A electric current constant-current charge, to chargingWhen electric current is down to 1.1A, stop charging, leave standstill 1 hour, with 22Ah electric current constant-current discharge, to 2.8V, record is electricCapacity when tank discharge and electric weight; Repeat above-mentioned steps 5 times, when the extreme difference of continuous 3 result of the tests is less than 0.66Time, can finish in advance test, get the mean value of last 3 result of the tests. With the weight of electronic balance weighing batteryAmount. Calculate according to the following formula the energy density of battery
Energy content of battery density=battery discharge electric weight/battery weight
Each embodiment and comparative example are got three batteries and are carried out energy density test, and test result is as shown in table 1
Table 1 energy content of battery density measurement result
| Group | Battery average size/Ah | Battery average weight/g | Energy content of battery density/Wh/kg |
| Embodiment 1 | 23.5 | 377.9 | 227 |
| Embodiment 2 | 23.7 | 343.3 | 252 |
| Embodiment 3 | 23.6 | 354.5 | 243 |
| Comparative example 1 | 23.2 | 483.9 | 175 |
| Comparative example 2 | 23.5 | 366.6 | 234 |
| Comparative example 3 | 23.3 | 472.5 | 180 |
Security performance test
According to standard-required, security performance test comprises overdischarge test, overcharge test, short-circuit test, fallsTest, heating test, extruding test, lancing test, sea water immersion test, temperature cycling test, low gas fallPress test, wherein especially harsh with lancing test, for this reason, in this explanation, safety test is only done with lancing testFor battery safety evaluation index. Lancing test carries out according to GB/T31485-2015, at 25 ± 2 DEG C,By battery with 22A constant-current discharge to 2.8V, leave standstill after 1 hour, with 22A electric current constant-current charge during to 4.2VTurn constant-voltage charge, in the time that charging current is down to 1.1A, stop charging, leave standstill 1 hour, withDraw point with 25mm/sSpeed, from run through the center of battery perpendicular to the direction of battery, draw point rest in battery, observe 1 littleTime, battery is not on fire, not exploding is considered as battery by lancing test, and test result is as shown in table 2:
Table 2 lancing test result
| Group | Phenomenon | Whether pass through test |
| Embodiment 1 | Smolder but not on fire | Be |
| Embodiment 2 | Smolder but not on fire | Be |
| Embodiment 3 | Smolder but not on fire | Be |
| Comparative example 1 | Smolder but not on fire | Be |
| Comparative example 2 | Blast on fire | No |
| Comparative example 3 | On fire | No |
Can find out that from the result of table 1 and table 2 lithium-ion-power cell that adopts made of the present invention to obtain hasApparently higher than current business-like lithium-ion-power cell, meanwhile, battery has good security performance, and this alsoFor the use of battery on electric automobile provides Reliability Assurance.
The present invention also can have other various embodiments, in the situation that not deviating from the present invention and essence thereof, and this areaTechnical staff make corresponding change and distortion according to invention, but these corresponding change and distortion all should belong toThe protection domain of the claims in the present invention.
Claims (10)
1. a lithium-ion-power cell, comprises anode pole piece, cathode pole piece and barrier film, and on anode pole piece justUtmost point material is made up of positive active material, conductive agent, binding agent and safe additive, it is characterized in that instituteStating positive active material is nickelic ternary material LiNixCoyMn1-x-yO2, wherein 0.8≤x≤0.9, y >=0.05,x+y≤1。
2. lithium-ion-power cell according to claim 1, wherein, described safe additive is bismaleimideAmine polymer powder, is formed by BMI and barbiturates or derivatives thereof polymerisation, and number is divided equallySon amount 100000-500000.
3. lithium-ion-power cell according to claim 1 and 2, wherein, the positive pole activity of described positive electrodeThe weight proportion of material, conductive agent, binding agent and safe additive is (88～95): (1～4.5): (3～6):(0.5～4.5)。
4. lithium-ion-power cell according to claim 1, wherein, the negative material on described cathode pole piece byNegative electrode active material, conductive agent, binding agent composition.
5. lithium-ion-power cell according to claim 4, wherein, the negative electrode active material of described negative material,The weight proportion of conductive agent, binding agent is (90～96): (0.5～2): (3.5～8).
6. according to the lithium-ion-power cell described in claim 4 or 5, wherein, described negative electrode active material is artificialGraphite.
7. according to the lithium-ion-power cell described in claim 4 or 5, wherein, the leading of described negative or positive electrode materialElectricity agent is identical or different, is selected from the one in conductive black, electrically conductive graphite, VGCF, CNT, GrapheneOr several combination.
8. according to the lithium-ion-power cell described in claim 4 or 5, wherein, described negative or positive electrode material stickyKnot agent is PVDF.
9. lithium-ion-power cell according to claim 1, wherein, described barrier film is refractory ceramics barrier film.
10. lithium-ion-power cell according to claim 7, wherein, described refractory ceramics barrier film isOn 10～25 μ mPE or PP basement membrane, apply 2～5 μ m aluminum oxide coating layers of one or both sides.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108091927A (en) * | 2017-12-13 | 2018-05-29 | 桑顿新能源科技有限公司 | A kind of lithium ion battery and preparation method thereof of high safety, long circulation life |
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| CN112864379A (en) * | 2019-11-12 | 2021-05-28 | 王復民 | Preparation method of positive electrode material of lithium battery |
| US11848444B2 (en) | 2019-11-12 | 2023-12-19 | National Taiwan University Of Science And Technology | Preparation method of positive electrode material of lithium battery |
| CN115050961A (en) * | 2022-06-17 | 2022-09-13 | 苏州易来科得科技有限公司 | Lithium battery negative coating composition, preparation method of negative pole piece and lithium battery |
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