KR101647405B1 - Binder for lithium-ion battery and lithium-ion battery having the binder - Google Patents

Binder for lithium-ion battery and lithium-ion battery having the binder Download PDF

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Publication number
KR101647405B1
KR101647405B1 KR1020150032190A KR20150032190A KR101647405B1 KR 101647405 B1 KR101647405 B1 KR 101647405B1 KR 1020150032190 A KR1020150032190 A KR 1020150032190A KR 20150032190 A KR20150032190 A KR 20150032190A KR 101647405 B1 KR101647405 B1 KR 101647405B1
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KR
South Korea
Prior art keywords
binder
negative electrode
secondary battery
ion secondary
alginate
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KR1020150032190A
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Korean (ko)
Inventor
임태은
김영준
조용남
최수정
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전자부품연구원
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    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00Electrodes
    • H01M4/02Electrodes composed of or comprising active material
    • H01M4/62Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/052Li-accumulators
    • H01M10/0525Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00Electrodes
    • H01M4/02Electrodes composed of or comprising active material
    • H01M4/62Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621Binders
    • H01M4/622Binders being polymers
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies or technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage
    • Y02E60/12Battery technologies with an indirect contribution to GHG emissions mitigation
    • Y02E60/122Lithium-ion batteries

Abstract

Provided are a binder for a lithium-ion secondary battery and a lithium-ion secondary battery having the same. The binder for a lithium-ion secondary battery has strength and adhesion force to respond to external stress and has abundant elasticity to respond to the volume expansion of a silicon-based material, for preventing the decline in a lifespan caused by the shrinkage and the expansion of the volume with respect to the use in the silicon-based material during charging and discharging. The binder for a lithium-ion secondary battery comprises a synthetic binder with reinforced elasticity and strength by chemically synthesizing a first binder including a carboxylic group (-COOH) and a second binder including alginate.

Description

BACKGROUND OF THE INVENTION 1. Field of the Invention [0001] The present invention relates to a binder for a lithium ion secondary battery, and a lithium ion secondary battery having the binder.

The present invention relates to a binder for a lithium ion secondary battery and a lithium ion secondary battery having the same.

Lithium ion secondary batteries are one of the energy storage devices that store energy.

The lithium ion secondary battery has a higher energy density than the nickel cadmium battery, has no memory effect, is environmentally friendly, has a long life cycle, can output a high voltage, and can be miniaturized Recently, it is widely used in small portable electronic products such as mobile phones, tablet PCs and camcorders.

Conventional lithium ion secondary batteries include a positive electrode, a negative electrode, a separator, and an electrolytic solution as main components.

Conventionally, a cathode of a lithium ion secondary battery includes lithium oxide, and a cathode includes a carbon compound such as graphite capable of storing lithium ions. The separator prevents direct contact between the anode and the cathode, And serves as a medium for allowing lithium ions to move.

Recently, a technique for increasing the reversible capacity and increasing the energy density of the lithium ion secondary battery by changing the anode material of the lithium ion secondary battery from a carbon-based material to a silicon-based material has been studied.

However, when the anode material of the lithium ion secondary battery is changed from the carbon material to the silicon material, the reversible capacity and the energy density of the lithium ion secondary battery having the silicon-based cathode can be increased. On the other hand, The binder and the active material of the silicon base material are separated from the cathode due to the expansion of the silicon base material by about 400% or more, thereby significantly reducing the lifetime of the lithium ion secondary battery.

In order to solve the problem caused by employing a silicon material in the anode of such a lithium ion secondary battery, Korean Patent Publication No. 2007-0110569, published on Nov. 20, 2007, "Poly Discloses a binder in which polyurethane is physically mixed with polyacrylic acid (PAA), and an electrode mixture containing acrylic acid and a lithium secondary battery based thereon.

When a negative electrode material mixture is produced using a binder, a silicon-based active material, a conductive material, and a solvent having polyacrylic acid (PAA) as a binder of a silicon-based negative electrode of a lithium ion secondary battery, a solid content And there is a problem that the electrode density of the negative electrode becomes uneven when the negative electrode mixture having the settling phenomenon is applied to the negative electrode.

Korean Patent Publication No. 2007-0110569, an electrode mixture containing polyacrylic acid physically mixed with polyurethane as a binder, and a lithium secondary battery based thereon (2007. 11. 20)

In order to prevent reduction in life due to volume expansion and shrinkage caused by the use of a silicone-based material during charging and discharging, the present invention provides a battery pack having sufficient elasticity capable of coping with volume expansion of a silicon crab material, And a lithium ion secondary battery having the binder.

In one embodiment, the binder for a lithium ion secondary battery includes a synthetic binder chemically synthesized by a first binder containing a carboxyl group (-COOH) and a second binder containing alginate to enhance rigidity and elasticity.

The first binder of the binder for a lithium ion secondary battery includes polyacrylic acid (PAA).

In the binder for a lithium ion secondary battery, the synthetic binder of the lithium ion secondary battery includes a carbonyl group (C = O) as a functional group.

In one embodiment, the lithium ion secondary battery includes a positive electrode coated with a positive electrode mixture containing a positive electrode active material, a conductive agent, and a positive electrode binder on a positive electrode, a negative electrode active material, a conductive agent, and a negative electrode binder mixed with the negative electrode, A negative electrode coated with a negative electrode mixture, a separator for separating the positive electrode and the negative electrode, and an electrolyte for ion transfer between the positive electrode and the negative electrode, wherein the negative electrode binder contained in the negative electrode mixture contains a carboxyl group (-COOH) 1 binder, and a synthetic binder chemically synthesized by a second binder containing alginate to enhance rigidity and elasticity.

The first binder of the lithium ion secondary battery includes polyacrylic acid (PAA).

The synthetic binder of the lithium ion secondary battery contains a carbonyl group (C = O) as a functional group.

The binder for a lithium ion secondary battery and the lithium ion secondary battery having the same according to the present invention have sufficient elasticity, rigidity and binding force in response to volume expansion and contraction during charging and discharging caused by using a negative electrode mixture containing silicon, Ion secondary battery is prevented from being degraded, and sedimentation of solids generated when polyacrylic acid (PAA) is used as a binder is prevented, uniform distribution of the anode mixture is uniformly distributed on the electrode, uniform formation of the electrode density, , And has excellent rigidity, thereby greatly improving the performance of the lithium ion secondary battery.

BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a view showing a synthetic binder obtained by synthesizing a first binder, a second binder, and first and second binders constituting a synthetic binder according to an embodiment of the present invention.
2 is a graph showing functional groups of a synthetic binder by FT-IR analysis of the synthetic binder shown in Fig.
3 is a graph showing 13 C-NMR (nuclear magnetic resonance) analysis of the synthetic binder shown in Fig.
4 is a graph showing tensile test results of polyacrylic acid, alginate and synthetic binders according to one embodiment of the present invention.
5 is a graph showing the recovery rate and the stiffness after forming a negative electrode mixture containing polyacrylic acid (PAA), alginate and a synthetic binder on the electrode, respectively.
6 is a graph showing peeling test of polyacrylic acid (PAA), alginate and synthetic binder.
7 is a graph showing settling characteristics of polyacrylic acid (PAA), alginate and synthetic binder.
8 is a cross-sectional view conceptually showing a lithium ion secondary battery including a negative electrode coated with a negative electrode mixture containing the synthetic binder shown in FIG.
FIG. 9 is a graph showing a result of evaluating a battery for each binder after applying a polyacrylic acid binder, an alginate binder, and a synthetic binder to the negative electrode of the lithium ion secondary battery of FIG.

In the following description, only parts necessary for understanding the embodiments of the present invention will be described, and the description of other parts will be omitted so as not to obscure the gist of the present invention.

The terms and words used in the present specification and claims should not be construed as limited to ordinary or dictionary meanings and the inventor is not limited to the meaning of the terms in order to describe his invention in the best way. It should be interpreted as meaning and concept consistent with the technical idea of the present invention. Therefore, the embodiments described in the present specification and the configurations shown in the drawings are merely preferred embodiments of the present invention, and are not intended to represent all of the technical ideas of the present invention, so that various equivalents And variations are possible.

BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a view showing a synthetic binder obtained by synthesizing a first binder, a second binder, and first and second binders constituting a synthetic binder according to an embodiment of the present invention.

Referring to FIG. 1, a synthetic binder (PAA-Alginate) 300 is formed by chemically synthesizing a first binder 100 and a second binder 200.

The first binder 100 for forming the composite binder 300 may be, for example, a material containing a carboxyl group (-COOH).

In one embodiment of the present invention, the material that can be used as the first binder 100 may comprise, for example, poly (acrylic acid) (PAA).

Polyacrylic acid (PAA), which is the first binder 100 constituting the synthetic binder 300, provides sufficient rigidity to overcome the external stress applied to the anode material of the lithium ion secondary battery.

However, the polyacrylic acid (PAA), which is the first binder 100, has an advantage of providing strength to overcome the external stress applied to the negative electrode material of the lithium ion secondary battery, while the first binder 100 is a lithium ion When used as a single binder to be applied to a negative electrode material of a secondary battery, the active material or the conductive agent may separate due to sedimentation over time, and a low binding force, resulting in volume expansion and desorption due to shrinkage.

That is, the first binder 100 has an advantage of providing a rigidity corresponding to an external stress, but may cause a settling problem, a tearing problem, and the like.

The second binder 200 of the composite binder 300 may comprise, for example, alginate.

Alginate is a material mainly extracted from algae, brown algae, etc., and has elasticity-rich characteristics.

Since alginate is rich in elasticity, it has an advantage in that it can actively cope with volume expansion and contraction generated by forming a negative electrode of a lithium ion secondary battery from a silicon material, but has an advantage that it does not have a rigidity suitable for externally applied stress .

In one embodiment of the present invention, polyacrylic acid (PAA), which is the first binder 100 having the disadvantage of being capable of providing sufficient stiffness corresponding to external stress, And alginate, which is a second binder 200 having the disadvantage that it has a sufficient strength to cope with external stress but lacks rigidity, is chemically synthesized to produce the synthetic binder 300.

The synthetic binder 300 formed by synthesizing the first binder 100 and the second binder 200 has sufficient rigidity against external stress which is an advantage of the first binder 100 and is advantageous to the second binder 200 A lithium ion secondary battery including a negative electrode of a silicon material has sufficient elasticity so that it can prevent detachment due to volume expansion and contraction during charging and discharging, has sufficient rigidity and binding force, and has a variety of properties that do not cause sedimentation over time And these advantages can greatly improve the lifetime and characteristics of the lithium ion secondary battery.

In one embodiment of the present invention, the synthetic binder 300 formed by synthesizing polyacrylic acid (PAA) as the first binder 100 and alginate as the second binder 200 includes a carbonyl group (C = O) as a functional group .

In one embodiment of the present invention, in order to synthesize the synthetic binder 300 shown in FIG. 1, for example, polyacrylic acid (PAA) of about 5 g, which is the first binder 100, Dissolve.

Subsequently, about 5 [g] of alginate is provided in a solution of polyacrylic acid (PAA) dissolved therein.

In addition to polyacrylic acid (PAA) and alginate, an additional acid catalyst is added in an amount of about 0.1 [h], which serves to induce dehydration between polyacrylic acid (PAA) and alginate in solution.

In one embodiment of the present invention, the ratio of the first binder 100, the second binder 200, and the reaction inducing agent may be 1: 1: 0.02.

The solution containing polyacrylic acid (PAA), alginate and acid catalyst is stirred for about 24 hours under reflux conditions.

After stirring for about 24 hours, the remaining filtrate is removed through a distillation apparatus.

Then, a mixture of ethyl acetate and diethyl ether is added so that a trace amount of impurities, which may be produced during synthesis of the first and second binders 100 and 200, is not contained in the synthetic binder 300, Decantation is performed to remove impurities.

Thereafter, the unreacted first and second binders 100 and 200, and the synthetic binder remaining after the removal of water and impurities are dried under vacuum for 24 hours to obtain a synthetic binder 300 (polyacrylic acid (PAA) and alginate) chemically synthesized ).

Hereinafter, the function and characteristics of the synthetic binder 300 obtained by synthesizing polyacrylic acid (PAA) and alginate will be described.

2 is a graph showing functional groups of a synthetic binder by FT-IR analysis of the synthetic binder shown in Fig.

1 and 2, FT-IR analysis of a synthetic binder 300 synthesizing polyacrylic acid (PAA) as the first binder 100 and alginate as the second binder 200, As a result of the chemical structure analysis of the binder 300, the synthetic binder 300 was found to have a molecular weight of about 1700 cm < RTI ID = 0.0 > (cm) < / RTI & It was confirmed that a specific absorbance peak related to the ester newly introduced in the formula ( 1 ) appears.

The absorption peak observed at about 1700 cm -1 in the analysis graph of the synthetic binder 300 is an absorption peak not observed in the first binder 100 and the second binder 200, (C = O), which is a functional group generated in the compound of formula (I).

3 is a graph showing 13 C-NMR (nuclear magnetic resonance) analysis of the synthetic binder shown in Fig.

1 and 3, 13 C-NMR (nuclear magnetic resonance) analysis of the synthetic binder 300 shows that the carboxyl groups (-COOH) contained in the conventional polyacrylic acid (PAA) and alginate are shifted As a result, it can be confirmed that a carbonyl group (C = O) is successfully formed on the synthesized binder 300 synthesized by polymerizing the first binder 100 and the second binder 200.

4 is a graph showing tensile test results of polyacrylic acid, alginate and synthetic binders according to one embodiment of the present invention.

1 and 4, when polyacrylic acid (PAA), alginate and synthetic binder (PAA-Alginate, 300) were respectively subjected to tensile tests under the same conditions, the alginate had the lowest tensile strength, Acrylic acid (PAA) has the highest tensile strength. On the other hand, the synthetic binder 300 has a tensile strength lower than polyacrylic acid (PAA) as shown in Fig. 4, but higher than alginate.

According to FIG. 4, the composite binder 300 has been analyzed to have a rigidity suitable for external stress.

5 is a graph showing the recovery rate and the stiffness after forming a negative electrode mixture containing polyacrylic acid (PAA), alginate and a synthetic binder on the electrode, respectively.

Referring to FIG. 5, a negative electrode mixture containing polyacrylic acid (PAA), alginate, and a synthetic binder was prepared on each electrode, and recovery and stiffness were evaluated using a microindentor. As a result, a force of about 10 mN Measure the rigidity, which is the depth at which the electrodes are pressed.

Then, the recovery rate and the stiffness of the electrode according to the binder were analyzed by measuring the recovery rate, which was recovered after removing the force of about 10 mN.

The binder containing polyacrylic acid (PAA) has a high rigidity with a relatively small depth at which the electrode is pressed, but has a low recovery rate, while the alginate has a relatively low rigidity and a high recovery rate.

The synthetic binder 300 synthesized with polyacrylic acid (PAA) and alginate has a higher recovery rate and higher rigidity than the binder containing only polyacrylic acid (PAA) or alginate, and the recovery rate of the synthetic binder 300 is higher than that of polyacrylic acid (PAA) And intermediate of alginate, indicating that the synthetic binder 300 is superior in elasticity to polyacrylic acid (PAA).

6 is a graph showing peeling test of polyacrylic acid (PAA), alginate and synthetic binder.

According to the graph of Fig. 6, an electrode is formed using a polyacrylic acid binder in the current collector, an electrode is formed in the current collector using an alginate binder, and electrodes are formed in the current collector using a synthetic binder, (PAA) in the case of synthetic binders. The results showed that the binding strength of polyacrylic acid (PAA) improves.

7 is a graph showing settling characteristics of polyacrylic acid (PAA), alginate and synthetic binder.

Referring to FIG. 7, when a slurry is formed by mixing polyacrylic acid, alginate, and a synthetic binder with an active material and a conductive agent, it is confirmed whether or not the slurry has settled after one week has elapsed. , About 20% sedimentation occurred. However, in the case of the synthetic binder, about 2% sedimentation occurred. As a result, the dispersion stability of the synthetic binder was further improved as compared with that of polyacrylic acid.

8 is a cross-sectional view conceptually showing a lithium ion secondary battery including a negative electrode coated with a negative electrode mixture containing the synthetic binder shown in FIG.

1 and 8, a lithium ion secondary battery 500 includes a cathode 510, a cathode 520, a separator 530, and an electrolyte 540.

The anode 510 includes an anode electrode 511 and a cathode mixture 515.

The positive electrode mixture 515 includes a positive electrode active material containing lithium oxide, a conductive agent for improving the conductivity of the positive electrode active material, and a binder, and the positive electrode mixture 515 is applied or formed on the surface of the positive electrode 511.

The cathode 520 includes a cathode electrode 521 and a cathode mixture 525.

The anode electrode 521 is disposed apart from the anode electrode 511. The anode mixture 525 is an anode active material in which silicon and graphite are mixed in a ratio of 3: And a synthetic binder 300 shown in Fig.

In one embodiment of the present invention, the active material contained in the negative electrode material mixture 525, the synthetic binder 300 and the conductive agent are produced at a ratio of, for example, 8: 1: 1. The cathode mixture 525 is applied and formed on the surface of the cathode electrode 511. [

The separation membrane 530 has a structure having pores through which the electrolytic solution passes. For example, PE (poly (ethylene) is used as the separation membrane.

The electrolyte solution 540 contains EC: EMC in a ratio of 1: 2, and the electrolyte solution 540 includes 1 mole (M) of LiPF 6 and 10% of F-EC.

In one embodiment of the present invention, the synthetic binder contained in the anode mix 525 comprises a first binder 100 comprising a polyacrylic acid (PAA) comprising a carboxylic acid and an alginate ), And the synthetic binder 300 includes a carbonyl group (C = O) as a functional group.

FIG. 9 is a graph showing a result of evaluating a battery for each binder after applying a polyacrylic acid binder, an alginate binder, and a synthetic binder to the negative electrode of the lithium ion secondary battery of FIG.

Referring to FIGS. 1 and 9, the configuration of the lithium ion secondary battery is manufactured in the same manner as in FIG. 8, and the evaluation voltage condition is 1.5 [V] to 0.01 [V] The discharge was evaluated about 300 times.

As a result of evaluation, the lithium ion secondary battery including the synthesized binder 300 was higher than the lithium ion secondary battery including the binder containing polyacrylic acid in the first charging in terms of the storage capacity.

On the other hand, even in the case of the lithium ion secondary battery including the synthetic binder 300 after repeatedly performing 300 times of charge and discharge, it includes a lithium ion secondary battery and alginate including a binder containing polyacrylic acid in terms of storage capacity Which is higher than that of a lithium ion secondary battery containing a binder.

As described above in detail, since the negative electrode mixture containing silicon has sufficient elasticity, rigidity and binding force in correspondence with the volume expansion and contraction during charging and discharging, the lifetime of the lithium ion secondary battery can be prevented , And polyacrylic acid (PAA) as binders, uniform distribution of the anode mixture to the electrodes to uniformly form the electrode density, excellent adhesion, excellent recovery rate, and excellent rigidity, Thereby greatly improving the performance of the battery.

It should be noted that the embodiments disclosed in the drawings are merely examples of specific examples for the purpose of understanding, and are not intended to limit the scope of the present invention. It will be apparent to those skilled in the art that other modifications based on the technical idea of the present invention are possible in addition to the embodiments disclosed herein.

510 ... anode 520 ... cathode
530 ... Membrane 540 ... Electrolyte

Claims (6)

  1. A negative electrode active material containing silicon, a negative electrode active material mixed with a conductive agent and a negative electrode binder,
    Wherein the negative electrode binder comprises a synthetic binder chemically synthesized from polyacrylic acid (PAA) and alginate to enhance rigidity and elasticity.
  2. delete
  3. The method according to claim 1,
    Wherein the synthetic binder comprises a carbonyl group (C = O) as a functional group.
  4. A positive electrode coated with a positive electrode mixture including a positive electrode active material, a conductive agent, and a positive electrode binder on the positive electrode;
    A negative electrode coated with a negative electrode mixture mixed with a negative electrode active material, a conductive agent and a negative electrode binder, the negative electrode being spaced apart from the positive electrode;
    A separator separating the anode and the cathode; And
    And an electrolyte solution for ion movement between the anode and the cathode,
    Wherein the negative electrode binder included in the negative electrode mixture includes a synthetic binder chemically synthesized with polyacrylic acid (PAA) and alginate to enhance rigidity and elasticity.
  5. delete
  6. 5. The method of claim 4,
    Wherein the synthetic binder comprises a carbonyl group (C = O) as a functional group.
KR1020150032190A 2015-03-09 2015-03-09 Binder for lithium-ion battery and lithium-ion battery having the binder KR101647405B1 (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20070110569A (en) 2006-05-15 2007-11-20 주식회사 엘지화학 Electrode material containing polyacrylic acid physically mixed with polyurethane as binder and lithium secondary battery employed with the same
US20120088155A1 (en) * 2010-05-03 2012-04-12 Gleb Yushin Alginate-containing compositions for use in battery applications
KR20140039244A (en) * 2011-06-29 2014-04-01 닛토덴코 가부시키가이샤 Nonaqueous electrolyte secondary battery and cathode sheet therefor

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR101378046B1 (en) * 2012-05-04 2014-03-27 한국과학기술원 Electrode binder for lithium secondary battery, manufacturing method for the same, and electrode for lithium secondary battery
KR101428246B1 (en) * 2012-12-05 2014-08-08 한국과학기술원 Active material for suppressing metal ion migration in lithium secondary battery and ithium secondary battery comprising the same

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20070110569A (en) 2006-05-15 2007-11-20 주식회사 엘지화학 Electrode material containing polyacrylic acid physically mixed with polyurethane as binder and lithium secondary battery employed with the same
US20120088155A1 (en) * 2010-05-03 2012-04-12 Gleb Yushin Alginate-containing compositions for use in battery applications
KR20140039244A (en) * 2011-06-29 2014-04-01 닛토덴코 가부시키가이샤 Nonaqueous electrolyte secondary battery and cathode sheet therefor

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