CN110323435A - Organic material/graphite composite negative pole, preparation method and lithium ion battery - Google Patents
Organic material/graphite composite negative pole, preparation method and lithium ion battery Download PDFInfo
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- CN110323435A CN110323435A CN201910625608.6A CN201910625608A CN110323435A CN 110323435 A CN110323435 A CN 110323435A CN 201910625608 A CN201910625608 A CN 201910625608A CN 110323435 A CN110323435 A CN 110323435A
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- composite negative
- negative pole
- organic material
- acid
- graphite
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/20—Graphite
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/60—Selection of substances as active materials, active masses, active liquids of organic compounds
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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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 invention discloses a kind of organic material/graphite composite negative poles, the composite negative pole is prepared by organic material, graphitic carbon material and auxiliary material, and organic material is selected from one of organic acid/acid anhydrides with conjugation carbonyl structure or a variety of mixtures.The present invention also provides the preparation method of the composite negative pole and the lithium ion batteries manufactured with the composite negative pole.Organic material/graphite composite negative pole of the invention, has the characteristics that high capacity, high power and long-life, is with a wide range of applications.
Description
Technical field
The present invention relates to technical field of lithium batteries, and in particular to a kind of organic with high capacity, high power and long-life
Material/graphite composite negative pole, preparation method and the lithium ion battery manufactured with the composite negative pole.
Background technique
Develop high capacity and high-performance negative electrode material is to improve performance of lithium ion battery, enhancing circulating battery stability and peace
One important channel of full property.The graphite negative electrode material important as commercial lithium-ion batteries, there is many advantages, electricity
Subconductivity is high, and embedding de- lithium current potential is low, at low cost, also relatively small to the harm of environment.However as lithium ion battery in electricity
The problem of extensive use in electrical automobile and scale energy storage technology, graphite cathode exposure is also increasingly prominent, one of main problem
Show that its theoretical specific capacity is low, only 372mAh/g, energy density and power density are very limited, in addition its large current density
Electrical property and long-term cycle performance are also not good enough.It says, improve the reversible capacity of graphite cathode and high rate performance, follows in terms of these
Ring performance is most important to development high capacity and high power lithium ion cell.
Although people do a lot of work in the aspect of performance for improving graphite material in recent years, previous work is mainly concentrated
Optimize graphite cathode surface nature, binder system and in terms of, although these researchs achieve
Effect, but limited by its theoretical capacity, the theoretical capacity of its 372mAh/g can not be broken through.In order to significantly improve graphite material
Specific capacity and specific energy, silicon/graphite composite negative pole has received widespread attention, because the theoretical specific capacity of silicon is up to 4200mAh/
G, silicon is compound with graphite material, the specific capacity of graphite cathode can be significantly improved, although it is to be noted that this compound
The specific capacity and energy density of electrode are obviously improved, but the bulk effect of silicon materials super large, lead to the amount of its compound silicon materials
Cannot be too high, generally 10% hereinafter, and combination electrode cycle performance it is not good enough, especially by 100-200 times circulation after, easily
It causes the dusting of electrode material and falls off from collector, the embedding de- lithium performance of silicon materials just can not persistently play a role, to lead
Cause the rapid decaying of capacity in cyclic process.
Organic material can use carbonyl and the reversible storage lithium ion of conjugation, and not only lithium storage content is reachable
2000mAh/g, and organic material itself has elasticity and flexibility well, and the bulk effect during embedding de- lithium is small,
And have the characteristics that green and reproducible.But its electron conduction is poor, generally requires a large amount of electronic conductive material.It will be organic
Matter energy storage material and graphite material carry out it is compound can in conjunction with organic material high lithium storage content property and graphite it is highly conductive
Property develops next-generation high capacity, high power, long-life novel anode material, and manufacture has high-performance long on this basis
The lithium-ion battery systems in service life are an important development directions of lithium ion battery from now on.
Summary of the invention
The technical problem to be solved by the present invention is to overcome the deficiencies in the prior art, provide a kind of with high capacity, high power
With organic material/graphite composite negative pole of long-life.
It is an object of that present invention to provide a kind of organic material/graphite composite negative poles, and the composite negative pole is by organic matter
What material, graphitic carbon material and auxiliary material were prepared, organic material be selected from conjugation carbonyl structure organic acid/
One of acid anhydrides or a variety of mixtures.
Further, the chemical general formula of organic material are as follows:Formula
Middle R1, R2, R3, R4For hydrogen, C1~C8Alkyl, hydroxyl, carboxyl, ester group, aryl, acid anhydrides are either containing alkenyl or/and carboxyl
Alkyl chain.Wherein, alkyl includes alkyl, alkenyl etc..
Further, organic material is selected from maleic acid, fumaric acid, itaconic acid, mesaconic acid, citraconic acid, vinyl
One of benzoic acid, terephthalic acid (TPA), trimesic acid, Pyromellitic Acid, pyromellitic dianhydride or a variety of mixtures.
In the present invention, the graphitic carbon material is a kind of commercialization graphitic carbon material with carbonization structure, including day
Right graphite and electrographite.
Further, the auxiliary material includes binder and conductive agent.
Further, the binder is aqueous binders or oiliness binder, and the aqueous binders are selected from carboxymethyl
One of cellulose (CMC), polyacrylic acid (PAA), polyvinyl alcohol (PVA), alginate, carragheen, butadiene-styrene rubber (SBR)
Or a variety of mixtures, the oiliness binder are selected from one of Kynoar (PVDF), polyvinyl fluoride (PVF) or a variety of
Mixture.Preferably, the binder is polyacrylic acid (PAA), and dosage is 5~10wt.%.
Further, the conductive agent is selected from one of conductive black, acetylene black, carbon fiber, carbon nanotube, graphene
Or a variety of mixture.Preferably, the conductive agent be acetylene black and carbon nanotube compound, dosage be 5~
15wt.%.
Further, the mass ratio of organic material, graphitic carbon material, conductive agent and binder be 1~5:3~
5:1~3:1~2；Wherein, the mass ratio of organic material and graphitic carbon material is 0.2~1.
Another aspect of the present invention additionally provides the preparation method of the composite negative pole, comprising the following steps:
S1: organic material, graphitic carbon material and auxiliary material are mixed in dispersing agent, obtain electrode slurry；
S2: the electrode slurry is coated on electrode current collecting body, is suppressed, cuts and is dried after dry, obtains described multiple
Composite electrode.
Further, in step S1, the dispersing agent is selected from water, N-Methyl pyrrolidone (NMP), N, N dimethyl formyl
One of amine (DMF), dimethyl sulfoxide (DMSO) or a variety of mixtures.Preferably, the dispersing agent is ultrapure water.
Further, in step S2, the temperature of the drying is 90~150 DEG C.
The present invention also provides a kind of lithium ion batteries, including composite negative pole above-mentioned.
The beneficial effects of the present invention are:
Have organic acid/acid anhydrides of conjugation carbonyl structure compound with graphitic carbon material 1. the present invention selects, on the one hand utilizes
The lithium storage content property of organic material superelevation (one there is the molecule of conjugation carbonyl structure can store 8~14 lithium ions)
Increase substantially the specific capacity of graphite electrode；On the other hand, organic material is improved using the highly conductive property of graphite material
Electric conductivity；In addition, the elasticity and flexibility excellent based on organic material, can liquidate graphite material in charge and discharge process
Expansion and contraction, reduce the bulk effect of electrode.After tested, organic material/graphite composite negative pole reversible specific capacity can be with
Reach 500~1000mAh/g, be 1.4~3 times of existing graphite cathode theoretical specific capacity 372mAh/g, it is aobvious to realize the field
The technological break-through of work.After advanced optimizing electrode composition, this organic/inorganic combination electrode recycles 500~1000 times without obvious
Inducing capacity fading；Reversible capacity under the conditions of 50A/g under the current density of (135C for being equivalent to graphite cathode) is still up to
500mAh/g breaches the multiplying power limitation of conventional graphite cathode 10C, is a kind of negative electrode material with high power nature, simultaneously
With excellent long-term cycle performance.
2. organic/graphite composite negative pole of the invention has many advantages, such as that abundance, price are low and renewable, with graphite material
The compound cathode that not only may be implemented of material has the characteristics that high capacity, high power and long-life, also reduces electrochmical power source to future
Cost and cost it is significant, be to develop following high specific energy, high power, the Green Chemistry power supply of long-life and low cost
Important selection.
Detailed description of the invention
Fig. 1 is the preceding charging and discharging curve three times of fumaric acid/graphite combination electrode in embodiment 1；
Fig. 2 is fumaric acid/graphite combination electrode multiplying power property in embodiment 1；
Fig. 3 is the long-term cycle performance of fumaric acid/graphite combination electrode in embodiment 1；
Fig. 4 is fumaric acid in embodiment 1/graphite compound electric pole piece circulation front and back SEM figure.
Specific embodiment
The present invention will be further explained below with reference to the attached drawings and specific examples, so that those skilled in the art can be with
It more fully understands the present invention and can be practiced, but illustrated embodiment is not as a limitation of the invention.
Examples 1 to 24: organic material/graphite combination electrode is prepared
The present embodiment provides a kind of organic material/graphite combination electrode materials, specific to walk for making cathode of lithium battery
Suddenly are as follows:
(a) it is formulated according to shown in table 1, by organic lithium storage materials, graphite, conductive agent, binder, dispersing agent in deionization
It is sufficiently mixed in water (commercially available) and electrode slurry is uniformly made；
(b) electrode slurry is coated on copper foil current collector (commercially available), uses 2MPa/cm after dry2Pressure pressed
System dries 16h under 120 DEG C, vacuum condition to get the combination electrode after cutting.
In 1 Examples 1 to 24 of table high capacity it is organic/the formula rate table of graphite composite negative pole and reversible capacity for the first time
Fumaric acid made from embodiment 1/graphite combination electrode is made according to existing battery production method with lithium metal
To carry out charge-discharge test at battery to electrode assembling, result is as shown in Figure 1 to Figure 3.
As seen from Figure 1, the electrode nearly 530mAh/g of reversible capacity for the first time, coulombic efficiency is 80% for the first time.It is followed by 3 times
The reversible capacity of electrode is stablized in 537mAh/g after ring, and coulombic efficiency reaches 96%.It remains to obviously observe the three of graphite simultaneously
Rank charge and discharge platform illustrates that this composite negative pole effectively maintains the activity of graphite.
The multiplying power discharging property of the electrode is shown in Fig. 2, it can be seen that this material has very excellent high rate performance,
100mA/g charge when, as discharge-rate increases to 50A/g from 250mA/g, electrode reversible specific capacity almost without decaying, and
It discharging under the conditions of the super-large current of 50A/g (135C for being equivalent to graphite cathode), reversible capacity is still up to 500mAh/g,
This property is that pure graphite cathode is incomparable, shows excellent power nature.Pass through 500 charge and discharges at 500mA/g
After electricity circulation, the capacity of electrode shows that this organic/graphite composite negative pole has very almost without any decaying (see Fig. 3)
Excellent long-term recursive nature.
Fig. 4 is the scanning electron microscope (SEM) photograph of 500 circle front and back of this combination electrode circulation, it can be seen that graphite clearly may be used before recycling
See, acetylene black is uniform with graphene dispersion.It remains to see graphite block body after 500 circle circulations, but it is formd more than one layer above
Hole reticular structure, this is not only conducive to the transmission of lithium ion, can also alleviate the Volumetric expansion of graphite.Therefore this Compound Negative
Pole presents high capacity, high power and the excellent electrochemical performance of long-life.
Embodiment described above is only to absolutely prove preferred embodiment that is of the invention and being lifted, protection model of the invention
It encloses without being limited thereto.Those skilled in the art's made equivalent substitute or transformation on the basis of the present invention, in the present invention
Protection scope within.Protection scope of the present invention is subject to claims.
Claims (12)
1. a kind of organic material/graphite composite negative pole, which is characterized in that the composite negative pole is by organic material, graphite
What carbon material and auxiliary material were prepared, organic material is in the organic acid/acid anhydrides with conjugation carbonyl structure
One or more mixtures.
2. organic material/graphite composite negative pole as described in claim 1, which is characterized in that the change of organic material
Learn general formula are as follows:R in formula1, R2, R3, R4Selected from hydrogen, C1~C8Alkyl, hydroxyl,
One of carboxyl, ester group, aryl, acid anhydrides, alkyl chain containing alkenyl and/or carboxyl.
3. organic material/graphite composite negative pole as described in claim 1, which is characterized in that organic material is selected from
Maleic acid, fumaric acid, itaconic acid, mesaconic acid, citraconic acid, vinyl benzoic acid, terephthalic acid (TPA), trimesic acid, equal benzene four
One of formic acid, pyromellitic dianhydride or a variety of mixtures.
4. organic material/graphite composite negative pole as described in claim 1, which is characterized in that the graphitic carbon material includes
Natural graphite and electrographite.
5. organic material/graphite composite negative pole as described in claim 1, which is characterized in that the auxiliary material includes binder
And conductive agent.
6. organic material/graphite composite negative pole as claimed in claim 5, which is characterized in that the binder is aqueous viscous
Agent or oiliness binder are tied, the aqueous binders are selected from carboxymethyl cellulose, polyacrylic acid, polyvinyl alcohol, alginate, card
One of glue, butadiene-styrene rubber or a variety of mixtures are drawn, the oiliness binder is in Kynoar, polyvinyl fluoride
One or more mixtures.
7. organic material/graphite composite negative pole as claimed in claim 5, which is characterized in that the conductive agent is selected from conduction
One of carbon black, acetylene black, carbon fiber, carbon nanotube, graphene or a variety of mixtures.
8. such as the described in any item organic material/graphite composite negative poles of claim 5~7, which is characterized in that the organic matter
Material, graphitic carbon material, conductive agent and binder mass ratio be 1~5:3~5:1~3:1~2；Wherein, the organic matter
The mass ratio of material and graphitic carbon material is 0.2~1.
9. the preparation method of composite negative pole according to claim 1, which comprises the following steps:
S1: organic material, graphitic carbon material and auxiliary material are mixed in dispersing agent, obtain electrode slurry；
S2: the electrode slurry is coated on electrode current collecting body, is suppressed, cuts and is dried after dry, obtains the compound electric
Pole.
10. the preparation method of composite negative pole as claimed in claim 9, which is characterized in that in step S1, the dispersing agent is selected from
Water, N-Methyl pyrrolidone, N, one of N-dimethylformamide, dimethyl sulfoxide or a variety of mixtures.
11. the preparation method of composite negative pole as claimed in claim 10, which is characterized in that in step S2, the temperature of the drying
Degree is 90~150 DEG C.
12. a kind of lithium ion battery, which is characterized in that including composite negative pole as described in any one of claims 1 to 7.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111725481A (en) * | 2020-07-17 | 2020-09-29 | 苏州大学 | Preparation method of organic material/graphite composite negative electrode, composite negative electrode and application of composite negative electrode |
| CN112382763A (en) * | 2020-11-11 | 2021-02-19 | 苏州华赢新能源材料科技有限公司 | Organic matter/silicon composite material, battery cathode obtained from organic matter/silicon composite material and preparation method of battery cathode |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111725481A (en) * | 2020-07-17 | 2020-09-29 | 苏州大学 | Preparation method of organic material/graphite composite negative electrode, composite negative electrode and application of composite negative electrode |
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| CN112382763A (en) * | 2020-11-11 | 2021-02-19 | 苏州华赢新能源材料科技有限公司 | Organic matter/silicon composite material, battery cathode obtained from organic matter/silicon composite material and preparation method of battery cathode |
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Application publication date: 20191011 |