CN1925191A - Lithium secondary anode, its preparing method and lithium secondary anode using same - Google Patents
Lithium secondary anode, its preparing method and lithium secondary anode using same Download PDFInfo
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- CN1925191A CN1925191A CNA2005100370211A CN200510037021A CN1925191A CN 1925191 A CN1925191 A CN 1925191A CN A2005100370211 A CNA2005100370211 A CN A2005100370211A CN 200510037021 A CN200510037021 A CN 200510037021A CN 1925191 A CN1925191 A CN 1925191A
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- lithium secondary
- secondary battery
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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
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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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
This invention provides one lithium secondary battery anode and its process method, which comprises secondary anode composed of one base and two different compounds coating on different areas. The process method comprises the following steps: coating one compound onto anode base surface area different to basic materials; coating other compound different to basic materials on other part of the base surface to get lithium secondary battery anode of different basic material two compounds. This invention provides one lithium secondary battery composed of one anode, one cathode and one transmission isolation film.
Description
[technical field]
The present invention relates to a kind of lithium secondary battery, relate in particular to a kind of cathode plate for lithium secondary battery, its preparation method and adopt this anodal lithium secondary battery.
[background technology]
Lithium secondary battery is meant by lithium ion as conductive medium in the electrolyte, and the electro-chemical systems that can repeat to discharge and recharge.Along with the electronic product trend is compact, and environmental protection cry day is high, and lithium secondary battery is because of having high-energy-density, high-output power, quickly-chargeable, in light weight, volume is little and characteristic such as pollution-free, has become one of optimal selection of Portable 3C Product power supply supply.
Generally speaking, lithium secondary battery comprises a positive pole, a negative pole and connects anodal with negative pole and with the two separated osmotic isolating film.Above-mentioned positive pole, negative pole and osmotic isolating film place in the metal can, and inject the electrolyte in the metal can, soak anodal, negative pole, so that electrochemical reaction to take place, electric energy and chemical energy are changed mutually.
Wherein, osmotic isolating film is a loose structure, and ion is passed through, and but to electronic isolation, is generally polyethylene, polypropylene or polystyrene.Positive pole is the electronics provider, and the atom of positive electrode becomes ion in oxidizing process, and discharges electronics, and ion reduces at negative pole by osmotic isolating film, and electronics then transfers to and forms electric current in the external circuit.But negative material is generally lithium intercalation compound, comprises graphite, carbon fiber and metal oxide etc. as various material with carbon elements.
At present the positive electrode material of lithium secondary cell research emphasis is the positive electrode of Li-M-O (M is any one or two kinds of above compound of Co, Mn, Ni, Cr) system.Wherein, spinel-type LiMn
2O
4With its aboundresources, cheap, the advantage such as pollution-free and synthetic method is simple becomes the focus of research, is considered to the positive electrode of tool potentiality in the lithium secondary battery.But, spinel-type LiMn
2O
4Cycle performance poor, charge/discharge capacity decay was serious when capacity attenuation, particularly temperature were higher than 55 ℃.Therefore, the research emphasis of Li-M-O compound positive electrode is to improve aspects such as charge/discharge capacity and cycle characteristics at present.
In order to improve the characteristic of positive electrode material of lithium secondary cell, the technology that is adopted mainly is that anodal material surface is carried out modification in recent years, thereby overcomes its capacity attenuation and improve chemical property.
But, all only adopt the unification compound that positive electrode is carried out finishing at present, though these class methods have been stablized the cycle performance of positive electrode, often be attended by the defective that initial capacity descends.
In view of this, a kind of cycle characteristics that can improve positive electrode material of lithium secondary cell is provided, can effectively stops simultaneously cathode plate for lithium secondary battery that initial capacity descends and preparation method thereof again and have a good lithium secondary battery of high-capacitance, high-temperature cycle life real for necessary.
[summary of the invention]
Below will a kind of cycle characteristics that can improve positive electrode material of lithium secondary cell be described with embodiment, and can effectively stop again cathode plate for lithium secondary battery of initial capacity decline and preparation method thereof simultaneously.
And, provide a kind of have high power capacity, the good lithium secondary battery of high-temperature cycle life by these embodiment.
This kind cathode plate for lithium secondary battery comprises a base material, and the two kinds of different compounds that are different from substrate material that apply in this substrate surface zones of different respectively; These two kinds of compound molecule formulas are respectively LiMO
2And A
xO
y, wherein, M is a kind of in Co, Ni, Mn, the Cr transition metal, and A is any in Mg, Sn, Al, the Si element, and x is 0＜x≤2, and y is 0＜y≤3.
The preparation method of this kind cathode plate for lithium secondary battery, its step comprises:
Apply a compound that is different from substrate material on cathode plate for lithium secondary battery base material part surf zone, this compound molecule formula is LiMO
2, M is a kind of in Co, Ni, Mn, the Cr transition metal in the formula, obtains the base material part surf zone and is coated with LiMO
2Cathode plate for lithium secondary battery;
Apply another compound that is different from substrate material in the other subregion of cathode plate for lithium secondary battery substrate surface, this compound molecule formula is A
xO
y, A is any in Mg, Sn, Al, the Si element in the formula, and x is 0＜x≤2, and y is 0＜y≤3, obtains the substrate surface zones of different and is coated with respectively the compound L iMO that is different from substrate material
2And A
xO
yCathode plate for lithium secondary battery.
This kind lithium secondary battery comprises a positive pole, a negative pole and an osmotic isolating film, and this osmotic isolating film connects positive pole and separates with negative pole and with the two; This anodal substrate surface zones of different is coated with two kinds of different compounds that are different from substrate material; These two kinds of compound molecule formulas are respectively LiMO
2And A
xO
yWherein M is a kind of in Co, Ni, Mn, the Cr transition metal, and A is any in Mg, Sn, Al, the Si element, and the span of x, y is respectively 0＜x≤2,0＜y≤3.
Compared with prior art, cathode plate for lithium secondary battery of the embodiment of the invention and preparation method thereof, its advantage is: owing to be coated with two kinds of different compound L iMO that are different from substrate material in positive-pole base material surface zones of different
2And A
xO
y, wherein, LiMO
2Can between positive-pole base material and electrolyte, form one deck passivation layer, can reduce electrolytical decomposition, thereby make positive pole show good cyclic reversibility; A
xO
yCan form the high concentration metal atomic layer on the positive-pole base material surface, can reduce the dissolving of anodal crystal defect and minimizing cathode metal ion, thereby anodal high temperature cyclic performance is stablized, can also suppress the decay of anodal initial capacity.Thereby the cathode plate for lithium secondary battery of gained not only improves the charge/discharge cycle characteristics of positive electrode, can also effectively stop the decay of capacitance simultaneously.
Adopt the advantage of this anodal lithium secondary battery to be: cathode plate for lithium secondary battery substrate surface zones of different is coated with two kinds of different compound L iMO that are different from substrate material
2And A
xO
y, can improve the charge/discharge cycle characteristics of positive electrode, improve battery capacity and high-temperature cycle.
[description of drawings]
Fig. 1 be in the embodiment of the invention base material part surf zone by cathode plate for lithium secondary battery structural representation that lithium and cobalt oxides coated.
Fig. 2 is the cathode plate for lithium secondary battery structural representation that is coated on the substrate surface zones of different in the embodiment of the invention by cobalt lithium oxide and two kinds of compounds of magnesium oxide respectively.
Fig. 3 is a lithium secondary battery structural representation in the embodiment of the invention.
[embodiment]
The cathode plate for lithium secondary battery that the embodiment of the invention provides comprises a base material, and the two kinds of different compounds that are different from substrate material that apply in this substrate surface zones of different respectively; These two kinds of compound molecule formulas are respectively LiMO
2And A
xO
yWherein M is a kind of in Co, Ni, Mn, the Cr transition metal, and A is any in Mg, Sn, Al, the Si element, and the span of x, y is respectively 0＜x≤2,0＜y≤3.
In the present embodiment, M is Co; A is Mg.
Wherein said base material is a kind of of cobalt acid lithium, lithium nickelate, LiMn2O4 and their modified compound, and present embodiment adopts LiMn2O4 (LiMn
2O
4).
The preparation method of this kind cathode plate for lithium secondary battery that the embodiment of the invention provided, it may further comprise the steps:
Apply a compound that is different from substrate material on cathode plate for lithium secondary battery base material part surf zone, this compound molecule formula is LiMO
2, M is a kind of in Co, Ni, Mn, the Cr transition metal in the formula, obtains the base material part surf zone and is coated with LiMO
2Cathode plate for lithium secondary battery;
Apply another compound that is different from substrate material in the other subregion of cathode plate for lithium secondary battery substrate surface, this compound molecule formula is A
xO
y, A is any in Mg, Sn, Al, the Si element in the formula, and x is 0＜x≤2, and y is 0＜y≤3, obtains the substrate surface zones of different and is coated with respectively the compound L iMO that is different from substrate material
2And A
xO
yCathode plate for lithium secondary battery.
Wherein, coating compound LiMO
2And A
xO
yThe time, all can adopt solid-phase synthesis, gel-sol method or utilize K
3Fe (CN)
6The method that adsorption capacity applies, present embodiment applies LiMO
2Shi Liyong K
3Fe (CN)
6Adsorption capacity apply; Apply A
xO
yThe Shi Caiyong sol-gel process applies.
The present embodiment first step is with Spinel LiMn
2O
4Powder is positive-pole base material, utilizes K
3Fe (CN)
6Chemical adsorption capacity, with Co (NO
3)
2Solution slowly mixes the formation cobalt complex, controls reactant consumption and concentration therebetween, guarantees the cobalt complex precipitation and covers LiMn
2O
4On the positive pole powder part surface zone, obtain the positive pole that the base material part surf zone is coated by the cobalt oxidate for lithium through heat treatment;
Second step was to utilize the product of sol-gel process with first step gained, with Mg (OH)
2Solution mixes, heat this mixture at a certain temperature, make the magnesium oxide of generation be coated on the zone that anodal substrate surface is not coated by cobalt lithium oxide, heat-treat the cathode plate for lithium secondary battery that obtains being coated on respectively the substrate surface zones of different afterwards again by cobalt lithiated compound and magnesium oxide.
The concrete steps of present embodiment are as follows:
(1) with the 10g particle diameter is 25 μ m base material powder LiMn
2O
4With 40mL concentration be the K of 0.1mol/L
3Fe (CN)
6Aqueous solution obtains solution A; With 2mL/min speed is the Co (NO of 0.05mol/L with 100mL concentration
3)
2Solution splashes into and obtains solution B in the solution A; Filtering solution B removes unnecessary K
3Fe (CN)
6With KNO
3Solution; With filtering gains and 100mL concentration is that the LiOH solution of 0.05mol/L fully mixes, and stirs 0.5 hour, obtains solution C; Refilter solution C, remove unnecessary LiOH solution; Wet mash after filtering was placed 90～100 ℃ of baking ovens dry 12 hours; Take out the material of oven dry, be placed under the oxygen state,, be calcined to 500 ℃, be incubated 10 hours, reduce to room temperature with the rate of temperature fall of 5 ℃ of per minutes again, obtain the positive pole that anodal base material part surf zone is coated by cobalt lithium oxide with the rate of heat addition of 5 ℃ of per minutes;
(2) anodal base material part surf zone is coated with the positive pole of cobalt lithium oxide and the Mg (OH) that 60mL concentration is 0.1mol/L
2Solution mixes; 200～300 ℃ of heating, make by Mg (OH)
2The magnesium oxide that decomposes gained is coated on the zone that described substrate surface is not coated by cobalt lithium oxide; Carry out calcination at 750 ℃ and handled 12 hours, obtain being coated on respectively the positive pole of substrate surface zones of different by cobalt lithium oxide and two kinds of compounds of magnesium oxide.
Fig. 1 be in the present embodiment base material part surf zone by cathode plate for lithium secondary battery structural representation that lithium and cobalt oxides coated, wherein, lithium and cobalt oxides 14 is coated on base material 12 part surface zones, forms to have only a kind of compound local surfaces to modify cathode plate for lithium secondary battery structure 10.
Fig. 2 is the cathode plate for lithium secondary battery structural representation that is coated on the substrate surface zones of different in the present embodiment by cobalt lithium oxide and two kinds of compounds of magnesium oxide respectively, wherein, lithium and cobalt oxides 14 and magnesium oxide 21 are coated on the zones of different of substrate surface respectively, form two kinds of different compound finishing cathode plate for lithium secondary battery structures 20.
See also Fig. 3, the lithium secondary battery 100 of present embodiment comprises a positive pole 110, a negative pole 120 and connects anodal 110 with negative pole 120 and with the two separated osmotic isolating film 130.This osmotic isolating film 130 is loose structures, and ion is passed through, and but to electronic isolation, is generally polyethylene, polypropylene or polystyrene, adopts polyethylene in the present embodiment.But the material of negative pole 120 is lithium intercalation compound, comprises graphite, carbon fiber and metal oxide etc. such as various material with carbon elements, adopts graphite in the present embodiment.The substrate surface zones of different of present embodiment cathode plate for lithium secondary battery 110 is coated with two kinds of different compound cobalt lithium oxides and the magnesium oxide that is different from substrate material.
The operation principle of present embodiment lithium secondary battery 100 is: the atom of cathode plate for lithium secondary battery 110 becomes ion in oxidizing process, and discharges electronics, and in another electrode reduction, electronics then transfers to and forms electric current in the external circuit ion by osmotic isolating film 130.
Present embodiment cathode plate for lithium secondary battery and preparation method thereof provides a kind of cathode plate for lithium secondary battery by cobalt lithium oxide and two kinds of compound finishinges of magnesium oxide, because lithium and cobalt oxides can form one deck passivation layer between anodal base material and electrolyte, can reduce electrolytical decomposition, thereby make positive pole show good cyclic reversibility; Magnesium oxide can form the high concentration metal atomic layer at anodal substrate surface, can reduce the dissolving of anodal crystal defect and minimizing cathode metal ion, thereby anodal high temperature cyclic performance is stablized, and can also suppress the decay of anodal initial capacity.Thereby the cathode plate for lithium secondary battery of gained not only improves the charge/discharge cycle characteristics of positive electrode, can also effectively stop the decay of capacitance simultaneously.Adopt this anodal lithium secondary battery to have high-capacitance, the good advantage of high-temperature cycle life.
Claims (16)
1. a cathode plate for lithium secondary battery comprises a base material, it is characterized in that this cathode plate for lithium secondary battery also comprises two kinds of different compounds that are different from substrate material, and it is coated in respectively this substrate surface zones of different, and these two kinds of compound molecule formulas are respectively LiMO
2And A
xO
y, wherein M is a kind of in Co, Ni, Mn, the Cr transition metal, A is any in Mg, Sn, Al, the Si element, and the span of x, y is respectively 0＜x≤2,0＜y≤3.
2. cathode plate for lithium secondary battery as claimed in claim 1 is characterized in that described base material is a kind of of cobalt acid lithium, lithium nickelate, LiMn2O4 and their modified compound.
3. the preparation method of a cathode plate for lithium secondary battery, its step comprises:
Apply a compound that is different from substrate material on cathode plate for lithium secondary battery base material part surf zone, this compound molecule formula is LiMO
2, M is a kind of in Co, Ni, Mn, the Cr transition metal in the formula, obtains the base material part surf zone and is coated with LiMO
2Cathode plate for lithium secondary battery;
Apply another compound that is different from substrate material in the other subregion of cathode plate for lithium secondary battery substrate surface, this compound molecule formula is A
xO
y, A is any in Mg, Sn, Al, the Si element in the formula, and the span of x, y is respectively 0＜x≤2,0＜y≤3, obtains the substrate surface zones of different and is coated with respectively the compound L iMO that is different from substrate material
2And A
xO
yCathode plate for lithium secondary battery.
4. as the preparation method of cathode plate for lithium secondary battery as described in the claim 3, it is characterized in that described base material is a kind of of cobalt acid lithium, lithium nickelate, LiMn2O4 and their modified compound.
5. as the preparation method of cathode plate for lithium secondary battery as described in the claim 3, it is characterized in that coating compound LiMO
2The time, can adopt solid-phase synthesis, gel-sol method or utilize K
3Fe (CN)
6The method that applies of adsorption capacity.
6. the preparation method of cathode plate for lithium secondary battery as claimed in claim 3 is characterized in that coating compound A
xO
yThe time, can adopt solid-phase synthesis, gel-sol method or utilize K
3Fe (CN)
6The method that applies of adsorption capacity.
7. as the preparation method of cathode plate for lithium secondary battery as described in the claim 3, it is characterized in that coating compound LiMO
2The time, with base material by weight percentage 1-10% add in the solution that molar concentration is 0.01-0.05mol/L and react, make LiMO
2Cover cathode plate for lithium secondary battery base material part surf zone.
8. as the preparation method of cathode plate for lithium secondary battery as described in the claim 7, it is characterized in that described base material part surface coverage is had LiMO
2Cathode plate for lithium secondary battery hour get final product to such an extent that anodal base material part surface-coated has LiMO at 150-600 ℃, calcination 10-12
2Cathode plate for lithium secondary battery.
9. such as the preparation method of cathode plate for lithium secondary battery as described in claim 3 or 7, it is characterized in that the positive-pole base material part surface is coated with LiMO
2Cathode plate for lithium secondary battery by weight percentage 2-20% add in the other solution that molar concentration rate is 0.05-0.1mol/L and react, make the A that generates
xO
yCover the other subregion of substrate surface.
10. the preparation method of cathode plate for lithium secondary battery as claimed in claim 9 is characterized in that the other subregion of substrate surface is coated with A
xO
yCathode plate for lithium secondary battery at 700～800 ℃ of calcination 10-12 hours, obtain the substrate surface zones of different and be coated with respectively the compound L iMO that is different from substrate material
2And A
xO
yCathode plate for lithium secondary battery.
11. lithium secondary battery, comprise a positive pole, a negative pole and an osmotic isolating film, this osmotic isolating film connects positive pole and separates with negative pole and with the two, and it is characterized in that: this cathode plate for lithium secondary battery substrate surface zones of different is coated with two kinds of different compounds that are different from substrate material; These two kinds of compound molecule formulas are respectively LiMO
2And A
xO
yWherein M is a kind of in Co, Ni, Mn, the Cr transition metal, and A is any in Mg, Sn, Al, the Si element, and the span of x, y is respectively 0＜x≤2,0＜y≤3.
12. lithium secondary battery as claimed in claim 11 is characterized in that described base material is a kind of of cobalt acid lithium, lithium nickelate, LiMn2O4 and their modified compound.
13. lithium secondary battery as claimed in claim 11 is characterized in that described osmotic isolating film is a loose structure.
14. lithium secondary battery as claimed in claim 11, the material that it is characterized in that described osmotic isolating film is polyethylene, polypropylene or polystyrene.
15. lithium secondary battery as claimed in claim 11, but it is characterized in that the material of described anode is lithium intercalation compound.
16. lithium secondary battery as claimed in claim 11, but it is characterized in that described lithium intercalation compound is graphite, carbon fiber or metal oxide.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100370211A CN100502100C (en) | 2005-09-02 | 2005-09-02 | Lithium secondary anode, its preparing method and lithium secondary anode using same |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100370211A CN100502100C (en) | 2005-09-02 | 2005-09-02 | Lithium secondary anode, its preparing method and lithium secondary anode using same |
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| Publication Number | Publication Date |
|---|---|
| CN1925191A true CN1925191A (en) | 2007-03-07 |
| CN100502100C CN100502100C (en) | 2009-06-17 |
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ID=37817731
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|---|---|---|---|
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|---|---|
| CN (1) | CN100502100C (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101882679A (en) * | 2009-05-07 | 2010-11-10 | 索尼公司 | Active material, battery and the method that is used to make electrode |
| CN104078655A (en) * | 2014-06-30 | 2014-10-01 | 天津巴莫科技股份有限公司 | Preparation method of cladding type titanium oxide compound |
| CN109911946A (en) * | 2017-12-13 | 2019-06-21 | 中国科学院过程工程研究所 | The method of saggar recovery processing is discarded in a kind of cobalt acid lithium battery material preparation process |
Family Cites Families (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6737195B2 (en) * | 2000-03-13 | 2004-05-18 | Samsung Sdi Co., Ltd. | Positive active material for rechargeable lithium battery and method of preparing same |
| KR100369445B1 (en) * | 2000-04-17 | 2003-01-24 | 한국과학기술원 | Coating materials and method of lithium manganese oxide for positive electr odes in the Lithium secondary batteries |
| CN1208866C (en) * | 2001-11-02 | 2005-06-29 | 中国科学院物理研究所 | Lithium secondary battery by use of composite material covered with nano surface as active material of positive polar |
| CN1627550A (en) * | 2003-12-11 | 2005-06-15 | 比亚迪股份有限公司 | Anode material of lithium ion cell and preparation method |
| CN1585161A (en) * | 2004-05-25 | 2005-02-23 | 惠州Tcl金能电池有限公司 | Potassium manganate modifying technology of secondary lithium ion battery |
-
2005
- 2005-09-02 CN CNB2005100370211A patent/CN100502100C/en not_active Expired - Fee Related
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101882679A (en) * | 2009-05-07 | 2010-11-10 | 索尼公司 | Active material, battery and the method that is used to make electrode |
| CN101882679B (en) * | 2009-05-07 | 2015-07-01 | 索尼公司 | Active material, battery, and method for manufacturing electrode |
| CN104078655A (en) * | 2014-06-30 | 2014-10-01 | 天津巴莫科技股份有限公司 | Preparation method of cladding type titanium oxide compound |
| CN104078655B (en) * | 2014-06-30 | 2016-03-09 | 天津巴莫科技股份有限公司 | A kind of preparation method of cladded type titanium oxygen compound |
| CN109911946A (en) * | 2017-12-13 | 2019-06-21 | 中国科学院过程工程研究所 | The method of saggar recovery processing is discarded in a kind of cobalt acid lithium battery material preparation process |
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| Publication number | Publication date |
|---|---|
| CN100502100C (en) | 2009-06-17 |
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