CN105226292B - Lithium battery and its negative plate, CNT Cu composites as negative current collector application - Google Patents
Lithium battery and its negative plate, CNT Cu composites as negative current collector application Download PDFInfo
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Abstract
Lithium battery and its negative plate, CNT Cu composites as negative current collector application.The invention discloses a kind of lithium ion battery and its negative plate, negative plate includes negative current collector and the negative electrode active material coating being coated on negative current collector；Negative current collector is CNT Cu composites, and CNT therein arranges and formed the tectosome of horizontal direction matching along collector in-plane, and copper is then covered in carbon nanotube architecture body surface face and forms island structure.Lithium ion battery of the present invention is the lithium ion battery using above-mentioned negative plate.Compared with prior art, anode plate for lithium ionic cell of the present invention can substantially reduce the polarization in battery charging process, realize quick charge, fully meet requirement of the small-sized energy storage device such as smart electronicses product, portable power source to battery charging rate.
Description
Technical field
The invention belongs to field of lithium ion battery, it is more particularly related to a kind of lithium ion of quickly-chargeable
Battery and its negative plate.
Background technology
At present, lithium ion battery has been widely used for smart electronicses product, portable power source, electric automobile and large-scale storage
The fields such as energy.But, with the continuous progress of technology, these products are to the property such as the energy density of lithium ion battery and quick charge
The requirement of energy index is also more and more stricter；Wherein, requirement of the smart electronicses product to battery charging rate has even more turned into small-sized
One severe challenge of soft bag lithium ionic cell.
In view of this, it is necessory to provide the lithium ion battery and its negative plate of a kind of quickly-chargeable.
The content of the invention
It is an object of the invention to：The lithium ion battery and its negative plate of a kind of quickly-chargeable are provided, to meet intelligence
Requirement of the electronic product to battery charging rate.
In order to realize foregoing invention purpose, inventor has found that lithium ion battery is not quick charged by concentrating on studies
Reason essentially consist in its own internal resistance it is too high caused by polarize excessive, this causes cell voltage rapidly to be raised in charging transient
And quickly reach blanking voltage and the electricity that is filled with of battery is diminished.Due to lithium ion battery internal resistance essentially from negative plate,
The impedance of positive plate, barrier film and electrolyte intermediate ion and electronics, therefore can be by improving the ion and electricity of battery main material
Sub- conducting power improves the charging rate of battery.
Theoretical more than, the invention provides a kind of anode plate for lithium ionic cell, it includes negative current collector and coating
Negative electrode active material coating on negative current collector；The negative current collector is CNT-Cu composites, carbon nanometer therein
Pipe arranges and formed the tectosome of horizontal direction matching along collector in-plane, and copper is covered in carbon nanotube architecture body surface face and formed
Island structure.
Because above-mentioned CNT-Cu composites have high current-carrying capacity, therefore its temperature rise when big multiplying power charges is smaller,
And itself internal resistance is little with temperature change, so this collector can be reduced substantially in the big multiplying power charging process of battery
Polarization, meets lithium ion battery high power charging-discharging ability；Meanwhile, the CNT in above-mentioned CNT-Cu composites is added
Contact of the collector with active material, and then the electron exchange ability of collector and active material is improved, therefore, it is possible to effective
Reduce the resistance of cathode membrane, hence it is evident that increase the electronic conduction ability in battery and greatly reduce the physical impedance of battery, this has
Because the caused voltage of polarization rapidly increases when reducing to effect battery charging, raising battery charge window reached, improved electricity
The purpose of pond high rate performance.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the CNT-Cu composites are containing Cu ions
Water or organic solvent in use 1-5mA/cm2Current density to CNT carry out electroplating processes and be made.Select 1-5mA/cm2
Current density be because current density can influence the size and distributing homogeneity on Cu islands, and then to influence electric current on a current collector
Distribution；Current density is bigger, and the Cu islands size of formation is bigger, therefore needs to select the current density of suitable size during plating.
Improved as one kind of anode plate for lithium ionic cell of the present invention, copper plating is on the surface of CNT tectosomes and interior
Portion, copper is not distributed only over CNT tectosomes surface and forms island structure, is also at least partly present in what is formed between CNT
In hole.Wherein, CNT in collector equivalent to electric current carrier and passage, and Cu mainly be responsible for by carrier electronics pass
The negative electrode active material on surface is passed, therefore mainly the copper of surface plating works to electronics conduction, and Cu island structure
Its contact point with active material is added, advantageously in the conduction of electronics.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the negative electrode active material coating is with grain diameter
D50 is used as negative electrode active material for 8-22 μm of carbonaceous material.Because small-particulate materials can increase the ratio of active material
Surface area, increases the contact area of its island collector formed with CNT-Cu composites, and then is conducive to the biography of electronics
Lead and pass through with ion, reach the purpose that reduction charging polarization and voltage increase.
Improve, lived in the negative electrode active material coating containing negative pole as one kind of anode plate for lithium ionic cell of the present invention
Property material, cathode conductive agent and negative electrode binder.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the surface density of the negative electrode active material is 5-
30mg/cm3。
Improved as one kind of anode plate for lithium ionic cell of the present invention, the negative electrode active material is Delanium, naturally
One or more of mixtures in graphite, LTO, carbonaceous mesophase spherules.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the cathode conductive agent is electrically conductive graphite, conductive charcoal
The mixture of one or both of black, carbon fiber, CNT.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the negative electrode binder is butadiene-styrene rubber, poly- inclined two
The mixture of one or two kinds of in vinyl chloride, sodium carboxymethylcellulose, polytetrafluoroethylene (PTFE).
Improved as one kind of anode plate for lithium ionic cell of the present invention, the negative electrode active material, cathode conductive agent and negative
Binding agent mass percent shared in negative electrode active material coating in pole is respectively 88%-98%, 1%-8% and 0.5%-
8%.
Improved as one kind of anode plate for lithium ionic cell of the present invention, the quality of the cathode conductive agent and negative electrode binder
Ratio is 0.8-2.0.
In order to realize foregoing invention purpose, present invention also offers a kind of lithium ion battery, it includes positive plate, negative pole
Piece, electrolyte and the barrier film being interval between adjacent positive piece and negative plate, the negative plate are described in any of the above-described paragraph
Anode plate for lithium ionic cell.
Improved as one kind of lithium ion battery of the present invention, the positive plate includes plus plate current-collecting body and is coated in positive pole collection
Positive-active coating layer of active substance on fluid.
Improved as one kind of lithium ion battery of the present invention, contain positive electrode active material in the positive active material coating
Matter, positive conductive agent and positive electrode binder.
Improved as one kind of lithium ion battery of the present invention, the positive active material is LCO, NCM or both mixing
Thing.
Improved as one kind of lithium ion battery of the present invention, the grain diameter D50 of the positive electrode active material metallic substance is 6-
20μm。
Improved as one kind of lithium ion battery of the present invention, the positive conductive agent is electrically conductive graphite, conductive black, carbon fibre
The mixture of one or both of dimension, CNT.
As lithium ion battery of the present invention one kind improve, the positive electrode binder be butadiene-styrene rubber, polyvinylidene chloride,
The mixture of one or two kinds of in sodium carboxymethylcellulose, polytetrafluoroethylene (PTFE).
Improved as one kind of lithium ion battery of the present invention, the positive active material, positive conductive agent and positive pole are bonded
Agent mass percent shared in positive active material coating is respectively 88%-98%, 1%-8% and 0.5%-8%.
Improved as one kind of lithium ion battery of the present invention, the mass values of the positive conductive agent and positive electrode binder are
1.0-2.0。
Improved as one kind of lithium ion battery of the present invention, the barrier film is polyethylene individual layer polymer separators or poly- second
Tri- layers of composite diaphragms of PP/PE/PP that alkene (PE) is constituted with polypropylene (PP).
Improved as one kind of lithium ion battery of the present invention, the porosity of the barrier film is 25-50%, and thickness is 7-30 μ
m。
Improved as one kind of lithium ion battery of the present invention, the solvent of the electrolyte includes ol ester and cyclic ester.
Improved as one kind of lithium ion battery of the present invention, the ol ester is dimethyl carbonate, diethyl carbonate and carbon
It is one or more in sour methyl ethyl ester.
Improved as one kind of lithium ion battery of the present invention, the cyclic ester is in ethylene carbonate, propene carbonate
It is one or two kinds of.
Improved as one kind of lithium ion battery of the present invention, the mass ratio of the ol ester and ring-type fat is 0.8-2.0.
Improved as one kind of lithium ion battery of the present invention, the solvent of the electrolyte is LiPF6、LiAsF6Deng.
Compared with prior art, lithium ion battery of the present invention at least has the following advantages that：
1) there is excellent rapid charging performance, 60% electricity can be filled with 3min time；
2) there is excellent charging ability, charged under the conditions of 25 DEG C, 10C and do not analyse lithium.
Therefore, charge slow defect present invention efficiently solves current small-scale lithium ion cell high magnification, can be abundant
Meet requirement of the small-sized energy storage device such as smart electronicses product, portable power source to battery charging rate.
In order to realize foregoing invention purpose, negative electrode of lithium ion battery collection is used as present invention also offers CNT-Cu composites
The application of fluid.
Improved as CNT-Cu composites of the present invention as one kind of the application of negative electrode of lithium ion battery collector, it is described
CNT genesis analysis in CNT-Cu composites forms the CNT tectosomes of horizontal direction matching on a horizontal plane；Copper
Then it is covered in carbon nanotube architecture body surface face and forms island structure.
Improved as CNT-Cu composites of the present invention as one kind of the application of negative electrode of lithium ion battery collector, it is described
Cu in CNT-Cu composites is also at least partly present in the hole formed between CNT.
Brief description of the drawings
With reference to the accompanying drawings and detailed description, lithium ion battery of the present invention, negative plate and its advantage are carried out
Describe in detail.
Fig. 1 is the CNT tectosomes of horizontal direction matching.
Fig. 2 is the micro-structure diagram of the Cu-CNT composite current collectors of island structure made from embodiment 1.
Fig. 3 is the 15C charging curve comparison diagrams of comparative example 1 and the lithium ion battery obtained by embodiment 1.
Circulations of the Fig. 4 for the lithium ion battery obtained by comparative example 1 and embodiment 1 under the conditions of 50 DEG C, 3C/1C discharge and recharges
Life curve figure.
Fig. 5 is the conductivity versus temperature graph of a relation of comparative example 1 and the lithium ion battery obtained by embodiment 1.
Embodiment
In order that goal of the invention, technical scheme and the technique effect of the present invention become apparent from, below in conjunction with accompanying drawing and implementation
Example, the present invention will be described in further detail.It should be appreciated that the embodiment described in this specification is merely to explain
The present invention, is not intended to limit the present invention.
Comparative example 1
The preparation of negative plate：By native graphite, conductive black, butadiene-styrene rubber, sodium carboxymethylcellulose in mass ratio 90:5:
4:1 is mixed into slurry, is coated uniformly on by extruding on Cu collectors, and the surface density of negative electrode active material is 10mg/cm3, warp
Cross drying, cold pressing, slitting, cut-parts etc. and obtain negative plate.
The preparation of positive plate：By LCO, conductive black, polyvinylidene chloride in mass ratio 90:5:5 are mixed into slurry, pass through
Transfer or fashion of extrusion are coated uniformly on aluminium collector, and the surface density of positive electrode active materials is 20mg/cm3, by drying,
Cold pressing, slitting, cut-parts etc. obtain positive plate.
The preparation of barrier film：Barrier film is used as by the PE that 40%, thickness is 12 μm of porosity.
The preparation of electrolyte：By solvent component DMC in mass ratio:EMC:EC:PC=1:1:1:1 is made electrolyte solvent,
With LiPF61M/L electrolyte is made for solute.
The preparation of lithium ion battery：Obtained positive plate, negative plate are separated with barrier film and make naked according to winding process
Battery core, loads aluminum foil sack；Electrolyte is injected, battery core is activated using 0.02C-0.1C electric current, pumping is prepared into battery.
Embodiment 1
The preparation of negative current collector：CNT genesis analysis after purification is made level and matched somebody with somebody on a horizontal plane
To CNT tectosomes, as shown in Figure 1；CNT tectosomes are placed in the organic solvent copper ammon solution of the ion containing Cu, using 2mA/
cm2Current density to CNT tectosomes carry out electroplating processes, Cu is covered on CNT tectosomes surface and is formed island structure
Cu-CNT composite current collectors, as shown in Figure 2.
The preparation of negative plate：D50 is pressed for 22 μm of native graphite, conductive black, butadiene-styrene rubber, sodium carboxymethylcellulose
Mass ratio 90:5:4:1 is mixed into slurry, is coated uniformly on by fashion of extrusion on Cu-CNT composite current collectors, negative electrode active material
The surface density of matter is 10mg/cm3, negative plate is obtained by drying, cold pressing, slitting, cut-parts etc..
The preparation of positive plate：By LCO, conductive black, polyvinylidene chloride in mass ratio 90:5:5 are mixed into slurry, pass through
Transfer or fashion of extrusion are coated uniformly on aluminium collector, and the surface density of positive electrode active materials is 20mg/cm3, by drying,
Cold pressing, slitting, cut-parts etc. obtain positive plate.
The preparation of barrier film：Barrier film is used as by the PE that 40%, thickness is 12 μm of porosity.
The preparation of electrolyte：By solvent component DMC in mass ratio:EMC:EC:PC=1:1:1:1 is made electrolyte solvent,
With LiPF61M/L electrolyte is made for solute.
The preparation of lithium ion battery：Obtained positive plate, negative plate are separated with barrier film and make naked according to winding process
Battery core, loads aluminum foil sack；Electrolyte is injected, battery core is activated using 0.02C-0.1C electric current, pumping is prepared into battery.
Embodiment 2
The preparation of negative current collector：CNT genesis analysis after purification is made level and matched somebody with somebody on a horizontal plane
To CNT tectosomes；CNT tectosomes are placed in the organic solvent copper ammon solution of the ion containing Cu, using 1mA/cm2Electric current it is close
Degree carries out electroplating processes to CNT tectosomes, Cu is covered in the Cu-CNT for forming island structure on CNT tectosomes surface and is combined
Collector.
The preparation of negative plate：D50 is pressed for 15 μm of native graphite, conductive black, butadiene-styrene rubber, sodium carboxymethylcellulose
Mass ratio 92:4:3:1 is mixed into slurry, is coated uniformly on by transfer or fashion of extrusion on Cu-CNT composite current collectors, bears
The surface density of pole active material is 7mg/cm3, negative plate is obtained by drying, cold pressing, slitting, cut-parts etc..
The preparation of positive plate：By LCO, conductive black, polyvinylidene chloride in mass ratio 88:7:5 are mixed into slurry, pass through
Transfer or fashion of extrusion are coated uniformly on aluminium collector, and the surface density of positive electrode active materials is 15mg/cm3, by drying,
Cold pressing, slitting, cut-parts etc. obtain positive plate.
The preparation of barrier film：Barrier film is used as by the PE that 50%, thickness is 20 μm of porosity.
The preparation of electrolyte：By solvent component DMC in mass ratio:EMC:EC:PC=0.5:1.5:1:1 that electrolyte is made is molten
Agent, with LiPF61M/L electrolyte is made for solute.
The preparation of lithium ion battery：Obtained positive plate, negative plate are separated with barrier film and make naked according to winding process
Battery core, loads aluminum foil sack；Electrolyte is injected, battery core is activated using 0.02C-0.1C electric current, pumping is prepared into battery.
Embodiment 3
The preparation of negative current collector：CNT genesis analysis after purification is made level and matched somebody with somebody on a horizontal plane
To CNT tectosomes；CNT tectosomes are placed in the organic solvent copper ammon solution of the ion containing Cu, using 2mA/cm2Electric current it is close
Degree carries out electroplating processes to CNT tectosomes, Cu is covered in the Cu-CNT for forming island structure on CNT tectosomes surface and is combined
Collector.
The preparation of negative plate：D50 is pressed for 8 μm of Delanium, conductive black, butadiene-styrene rubber, sodium carboxymethylcellulose
Mass ratio 95:2.5:1.5:1 is mixed into slurry, and Cu-CNT composite current collectors are coated uniformly on by transfer or fashion of extrusion
On, the surface density of negative electrode active material is 18mg/cm3, negative plate is obtained by drying, cold pressing, slitting, cut-parts etc..
Subsequently the preparation of positive plate, barrier film, electrolyte and lithium ion battery is same as Example 1, has simply used this
The negative plate of embodiment, therefore here is omitted.
Battery performance test
Rate of charge test is carried out to the lithium ion battery obtained by comparative example 1 and embodiment 1, rate of charge is set to
15C (4.35V blanking voltages), obtains the charging curve shown in Fig. 3.From figure 3, it can be seen that the Cu collector batteries of comparative example 1
Blanking voltage is reached quickly, and the constant current time is short, and ability is filled soon；And the CNT-Cu composite current collector batteries of the embodiment of the present invention 1
Reach blanking voltage slow, the constant current time is long, therefore it is strong to fill ability soon.
Rate of charge test is carried out to the lithium ion battery obtained by comparative example 1 and embodiment 1-3, rate of charge is set to
3C/5C/10C/15C (using 1C constant current constant voltages as reference, continuous current is 500mA, and constant-voltage is 4.35V), test result is such as
Shown in table 1.
The rate of charge contrast table of table 1, comparative example and battery obtained by embodiment
| Rate of charge | 1C | 3C | 5C | 10C | 15C |
| Comparative example 1 | 96% | 50% | 20% | 9% | 3% |
| Embodiment 1 | 100% | 96% | 90% | 60% | 50% |
| Embodiment 2 | 100% | 95% | 89% | 61% | 46% |
| Embodiment 3 | 100% | 95% | 85% | 57% | 45% |
From table 1 it follows that 1-3 of embodiment of the present invention battery has good high rate performance, it is in constant current constant current
The electricity that stage can be filled with is much larger than comparative example 1.
Following analysis lithium test is carried out to the lithium ion battery obtained by comparative example 1 and embodiment 1-3：At room temperature, constant current
4.35V is charged to, rate of charge is as shown in the table；Then constant-voltage charge is until rate of charge is less than 0.05C；Then it will charge
Into battery standing 1 hour after constant current 0.5C be discharged to 3.0V.The battery for completing above-mentioned test is disassembled, observation battery is born
Analysis lithium situation at pole, test result is as shown in table 2.
The analysis lithium statistics of table 2, comparative example and battery obtained by embodiment
| Rate of charge | 1C | 3C | 5C | 10C | 15C |
| Comparative example 1 | 0/5 | 5/5 | 5/5 | 5/5 | 5/5 |
| Embodiment 1 | 0/5 | 0/5 | 0/5 | 0/5 | 5/5 |
| Embodiment 2 | 0/5 | 0/5 | 0/5 | 0/5 | 5/5 |
| Embodiment 3 | 0/5 | 0/5 | 0/5 | 0/5 | 5/5 |
From Table 2, it can be seen that 1-3 of embodiment of the present invention battery has good charging performance, it is in below 10C bars
Charged under part and do not analyse lithium, but the battery of comparative example 1 just all analyses lithium when 3C charges.
Cycle life test is carried out to the lithium ion battery obtained by comparative example 1 and embodiment 1, testing process is set to 3C
Charging, 1C electric discharges, test result are as shown in Figure 4.Figure 4, it is seen that the embodiment of the present invention 1 is circulated under the conditions of 50 DEG C
95% capacity is remained in that at 1000 times, hence it is evident that higher than comparative example 1.
Electrical conductivity test is carried out to the lithium ion battery obtained by comparative example 1 and embodiment 1：Conductance is used at different temperatures
Rate tester (the laboratory conductivity meter of the model BEC-510 types produced by Bel Analytical Instrument Co., Ltd) is tested respectively
The electrical conductivity of Cu collectors and Cu-CNT collectors, test result is as shown in Figure 5.From figure 5 it can be seen that with the liter of temperature
Height, the conductivity variations of the embodiment of the present invention 1 are little, but the electrical conductivity of comparative example 1 is substantially reduced.
In summary, the present invention is carried by using the island Cu-CNT composites of horizontal direction matching as negative current collector
The high current-carrying capacity of negative current collector so that battery can keep relatively low temperature rise under big multiplying power, so as to significantly reduce
Internal resistance in charging process increases.
The announcement and teaching of book according to the above description, those skilled in the art in the invention can also be to above-mentioned embodiment party
Formula carries out appropriate change and modification.Therefore, the invention is not limited in embodiment disclosed and described above, to this
Some modifications and changes of invention should also be as falling into the scope of the claims of the present invention.Although in addition, this specification
In used some specific terms, but these terms are merely for convenience of description, do not constitute any limitation to the present invention.
Claims (7)
1. a kind of anode plate for lithium ionic cell, including negative current collector are applied with the negative electrode active material being coated on negative current collector
Layer, it is characterised in that：The negative current collector is CNT-Cu composites, and CNT therein is arranged along collector in-plane
Cloth and the tectosome for forming horizontal direction matching, copper are covered in carbon nanotube architecture body surface face and form island structure.
2. anode plate for lithium ionic cell according to claim 1, it is characterised in that：The CNT-Cu composites be containing
Have and 1-5mA/cm is used in the water or organic solvent of Cu ions2Current density to CNT carry out electroplating processes and be made.
3. anode plate for lithium ionic cell according to claim 1, it is characterised in that：Copper in the CNT-Cu composites
It is also present in the hole that is formed between CNT.
4. anode plate for lithium ionic cell according to claim 1, it is characterised in that：The negative electrode active material coating with
Grain particle diameter D50 is used as negative electrode active material for 8-22 μm of carbonaceous material.
5. a kind of lithium ion battery, including positive plate, negative plate, electrolyte and it is interval between adjacent positive piece and negative plate
Barrier film, it is characterised in that：The negative plate is the anode plate for lithium ionic cell any one of Claims 1-4.
6.CNT-Cu composites as negative electrode of lithium ion battery collector application, it is characterised in that：The CNT-Cu is combined
CNT genesis analysis in material forms the CNT tectosomes of horizontal direction matching on a horizontal plane；Copper is covered in carbon and received
Mitron tectosome surface and form island structure.
7. CNT-Cu composites according to claim 6 are used as the application of negative electrode of lithium ion battery collector, its feature
It is：Cu in the CNT-Cu composites is also at least partly present in the hole formed between CNT.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106571458B (en) * | 2016-11-14 | 2019-05-31 | 赛福纳米科技(徐州)有限公司 | A kind of anode composite material and preparation method |
| KR102145493B1 (en) * | 2017-11-14 | 2020-08-18 | 주식회사 엘지화학 | Electrode assembly, rechargeable battery comprising the same and rechargeable battery manufacturing method |
| CN108134093A (en) * | 2017-12-28 | 2018-06-08 | 上海应用技术大学 | A kind of carbon nanotube paper-metal or alloy composite current collector and preparation method thereof |
| CN108539153B (en) * | 2018-03-27 | 2022-10-14 | 电子科技大学 | Metal lithium composite negative electrode material and preparation method thereof |
| CN113228353A (en) * | 2018-06-13 | 2021-08-06 | 托塔克纳米纤维有限公司 | Carbon Nanotube (CNT) -metal composite product and method for producing same |
| CN111430721A (en) * | 2020-02-25 | 2020-07-17 | 蜂巢能源科技有限公司 | Composite electrode and preparation method and application thereof |
| CN114497569B (en) * | 2022-01-10 | 2024-05-07 | 湖南大晶新材料有限公司 | Polymer current collector for lithium ion battery and preparation method thereof |
| WO2024071438A1 (en) * | 2022-09-30 | 2024-04-04 | 高圧ガス工業株式会社 | Electrode, and battery with electrode |
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