CN1228624A - Lithium ion battery using high polymer pyrolytic carbon as negative pole - Google Patents
Lithium ion battery using high polymer pyrolytic carbon as negative pole Download PDFInfo
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- CN1228624A CN1228624A CN98100696A CN98100696A CN1228624A CN 1228624 A CN1228624 A CN 1228624A CN 98100696 A CN98100696 A CN 98100696A CN 98100696 A CN98100696 A CN 98100696A CN 1228624 A CN1228624 A CN 1228624A
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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
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Abstract
The present invention relates to a lithium ion cell. Its negative pole is a mixture body using high polymer pyrolytic carbon as main component. Said high polymer pyrolytic carbon is obtained by using a simple, safe and low-cost preparation method. Its positive pole is a lithium-inlayed transition metal oxide, and the lithium salt mixed organic solvent solution is its electrolyte, and the high-molecular polymer microporous membrane is used as its diaphragm. The capacity of said cell is between 350-454 mAh/g.
Description
The present invention relates to a kind of lithium ion battery, its negative pole is to be the mixture of main component with the high polymer pyrolytic carbon, and used high polymer pyrolytic carbon is to be raw material with the polyphenyl, makes with simple, safety and low cost method.The capacity of this battery (in the amount of negative electrode active material, as follows) is between 350-454mAh/g.
Lithium ion battery is being subjected to correlative study personnel and industrial circle personage's special concern in the last few years, but its key is the preparation and the premium properties thereof of positive and negative pole material, promptly makes every effort to obtain the specific capacity height, constitutionally stable both positive and negative polarity.Petroleum coke and the special processing of graphite process once were used as the negative material of lithium ion battery, but the specific capacity of the two is all not too high, and the former is that the latter is up to 350mAh/g about 180mAh/g.Subsequently, through further development, the carbonaceous material that adopts high polymer pyrolytic to obtain is made negative active core-shell material, has obtained effect preferably.According to Science1994 (264) 556 reports, in hydrogen atmosphere,, make negative pole with the RESEARCH OF PYROCARBON that so obtains in 700 ℃ of pyrolysis polyphenyl, specific capacity can reach 680mAh/g.But deal with atmosphere with hydrogen, the cost height is dangerous big, and according to J.Electrochem.Soc.1944 (11) L143 report, the specific capacity and the heat treatment temperature of the RESEARCH OF PYROCARBON that said method makes are closely related, simultaneously, in the charge and discharge process afterwards, capacity loses gradually.Therefore, use the negative pole of above polyphenyl RESEARCH OF PYROCARBON material, do not make the lithium ion battery product of realistic application as yet as battery.
The objective of the invention is, at above-described defective, provide a kind of suitable lithium ion battery, its negative pole is to be key component with the polyphenyl RESEARCH OF PYROCARBON, is equipped with formations such as conductive agent, stabilizer and bonding agent.Polyphenyl RESEARCH OF PYROCARBON wherein be with simple, safety and cheaply new method make.
Lithium ion battery of the present invention comprises:
1. negative pole: its composition comprises: polyphenyl RESEARCH OF PYROCARBON, conductive agent, stabilizer and bonding agent, their weight ratio is followed successively by: 99.4-35%: 0.5-16%: 0-40%: 0.1-10%.
Polyphenyl RESEARCH OF PYROCARBON is wherein made by following method: with the atomic ratio of hydrogen and carbon is polyphenyl pyrolysis in the nitrogen current that flow velocity rises for per minute 0.01-10 of 0.2-0.8, programming rate is per minute 2-40 ℃, keep 600-1100 ℃ heat treatment 0.5-48 hour, cooling is reduced to 15-25 ℃ with per minute 1-35 ℃ speed then.The RESEARCH OF PYROCARBON that so makes is disordered carbon and its weight 0, the mixture of the graphite microcrystal of 001-2%.
Conductive agent wherein is selected from graphite or carbon black, perhaps their mixture, and its mixed weight ratio is followed successively by (1-2): (2-3).
Stabilizer wherein is selected from and comprises: ammonium chloride, ammonium carbonate or carbonic hydroammonium, and perhaps their mixture, when any two in them mixed successively, its weight mixing ratio was (0.5-1): (1-2)); During three kinds of mixing, its weight mixing ratio is followed successively by (0.5-1): (1-2)): (2-5).
Bonding agent wherein is selected from polytetrafluoroethylene or Kynoar.
2. anodal: the transition metal oxide by the embedding lithium constitutes, and is selected to comprise: the transition metal oxide of embedding lithiums such as embedding lithium cobalt oxide, embedding lithium nickel oxide or embedding lithium manganese oxide.
3. electrolyte: be organic mixed solvent solution of lithium salts, concentration is one mole, and lithium salts is selected from and comprises; Lithium perchlorate, LiBF4 or lithium hexafluoro phosphate.
Organic solvent wherein is selected from: any two kinds combination in them of ethyl carbonate, diethyl carbonate, propene carbonate, glycol dimethyl ether, its volumetric mixture ratio is one to one.
4. barrier film: be the high molecular polymer microporous membrane, comprise: polypropylene microporous film etc.
As above behind the lithium ion cell charging of Gou Chenging, lithium ion embeds negative pole, forms working battery, discharges and recharges its capacity of mensuration continuously, and in the weight of negative electrode active material, the reversible specific capacity of different batteries is between 350-454mAh/g.This battery can cooperate with multiple electrolyte, and excellent cycle performance is arranged.
The preparation method of lithium ion battery of the present invention, it comprises:
(1). the preparation of negative pole:
A. prepare the polyphenyl RESEARCH OF PYROCARBON, with the atomic ratio of hydrogen and carbon is polyphenyl pyrolysis in the nitrogen current that flow velocity rises for per minute 0.01-10 of 0.2-0.8, programming rate is per minute 2-40 ℃, keep 600-1100 ℃ heat treatment 0.5-48 hour, cooling then, reduce to 15-25 ℃ with per minute 1-35 ℃ speed, can obtain required aforementioned RESEARCH OF PYROCARBON.
B. add the aforesaid stabilizer of its weight 0-20% in the RESEARCH OF PYROCARBON that more than a certain amount of, makes, add aforesaid conductive agent of its weight 0.5-20% and the aforesaid bonding agent of 0.1-15% more respectively, after the grinding evenly, make the carbon negative pole with known method.
(2). select the transition metal oxide of aforesaid embedding lithium to do anodal.
(3). preparation electrolyte mixed organic solvents solution, concentration is 1 mole, electrolyte is selected aforesaid lithium salts for use; Organic solvent is selected from any two kinds combination of aforementioned solvents, and their mixed volume ratio is one to one.
(4). select for use the high molecular polymer porous membrane to make barrier film.
Above-listed each material is assembled into the various model batteries that vary in size according to its functional requirement, is lithium ion battery of the present invention.
Advantage of the present invention is:
(1). make the polyphenyl RESEARCH OF PYROCARBON with low cost, safe method, and it is stable and reliable for performance.
(2). negative pole is mixed and made into the carbon negative pole by polyphenyl RESEARCH OF PYROCARBON and conductive agent, stabilizer and bonding agent, makes it that high reversibility be arranged.
(3). reversible specific capacity is between 350-454mAh/g.This battery can cooperate with multiple electrolyte, and excellent cycle performance is arranged.
The purposes of lithium ion battery of the present invention:
The purposes of such battery is very extensive, comprising: be used for mobile phone, notebook computer, take the photograph player, electric automobile etc., can be made into the different shape that varies in size because of it simultaneously, be suitable for using with electrical domain various.
In order to be illustrated more clearly in the present invention, enumerate following examples, but it there is not any restriction to the present invention.
Embodiment 1.
With 10 gram hydrogen-carbon ratios is 0.62 polyphenyl, under the nitrogen atmosphere that per minute 1-6 rises, rises to 700-800 ℃ with the speed of 20 ℃ of per minutes, keeps this temperature after 0.5-1.5 hour, and temperature is dropped to 15-20 ℃ by per minute 1-3 ℃ speed.The gained RESEARCH OF PYROCARBON prepares battery cathode as follows.
Take by weighing 10 gram RESEARCH OF PYROCARBON, in wherein adding 2 gram carbon black or graphite, 1 gram polytetrafluoroethylene after the grinding evenly, is made electrode by known method.With embedding lithium cobalt oxide is positive pole.1 mole lithium perchlorate is dissolved in 1 liter of ethyl carbonate and diethyl carbonate (volume ratio 1: the 1) mixed solvent, makes electrolyte.With the polypropylene microporous film is barrier film, is assembled into the model battery.Charge to 4.1 volts by the 25 milliamperes/speed of (gram carbon), be discharged to 2.0 volts, recording reversible specific capacity is 380mAh/g.
Embodiment 2.
Method according to embodiment 1 prepares RESEARCH OF PYROCARBON material and electrode, makes 1 mole lithium perchlorate electrolyte with propene carbonate and dimethylamino ethanol ether mixed solvent (volume ratio 1: 1).Measuring reversible specific capacity by the method for example 1 is 350mAh/g.
Embodiment 3.
Method according to embodiment 1 prepares the RESEARCH OF PYROCARBON material, prepares carbon electrode as follows: taking by weighing 10 gram RESEARCH OF PYROCARBON, is 1: 1 the 2 gram carbon blacks and the mixture of graphite in wherein adding mixing ratio, 1 gram polytetrafluoroethylene, and 5 gram carbonic hydroammonium, grind evenly after, make electrode by known method.After being assembled into battery by the method for embodiment 1, measure its reversible specific capacity, be 454mAh/g, after 20 charge and discharge cycles, capacity is 402mAh/g.
Embodiment 4.
Method according to embodiment 1 and 3 prepares RESEARCH OF PYROCARBON material and electrode respectively, is positive pole with embedding lithium manganese oxide, is assembled into the model battery according to the method for embodiment 1.Speed by 25 milliamperes/gram carbon charges to 4.3 volts, is discharged to 3.5 volts, and recording reversible specific capacity is 395mAh/g.
Embodiment 5.
Method according to embodiment 1 prepares the RESEARCH OF PYROCARBON material, prepare carbon electrode as follows: take by weighing 10 gram RESEARCH OF PYROCARBON, in wherein adding 2 gram carbon blacks, 1 gram Kynoar, and the mixture of 4 gram carbonic hydroammonium and ammonium chloride, its mixing ratio is 3: 1, after grinding evenly, make electrode by known method, the method by embodiment 1 is assembled into the model battery again, and measuring its reversible specific capacity is 412mAh/g.
Embodiment 6.
Method according to embodiment 5 prepares the carbon carbon electrode, with the embedding lithium nickel oxide is positive pole, make 1 mole electrolyte with ethyl carbonate and dimethyl carbonate mixed solvent (volume ratio 1: 1) with lithium hexafluoro phosphate, method by embodiment 1 is assembled into the model battery again, surveying its reversible specific capacity is 450mAh/g, discharge and recharge for 20 times, circulation back capacity is 410mAh/g.
Claims (9)
1. a lithium ion battery is characterized in that, described battery comprises:
(1). negative pole: its composition comprises: polyphenyl RESEARCH OF PYROCARBON, conductive agent, stabilizer and bonding agent, their weight ratio is followed successively by: 99.4-35%: 0.5-16%: 0-40%: 0.1-10%;
Polyphenyl RESEARCH OF PYROCARBON is wherein made by following method: with the atomic ratio of hydrogen and carbon is that the polyphenyl flow velocity of 0.2-0.8 is pyrolysis in the nitrogen current that rises of per minute 0.01-10, programming rate is per minute 2-40 ℃, keep 600-1100 ℃ heat treatment 0.5-48 hour, cooling then, reduce to 15-25 ℃ with per minute 1-35 ℃ speed, the RESEARCH OF PYROCARBON that so makes is the mixture of the graphite microcrystal of disordered carbon and its weight 0.001-2%;
Conductive agent wherein is selected from graphite or carbon black, perhaps their mixture, and its mixed weight ratio is followed successively by (1-2): (2-3);
Stabilizer wherein is selected from and comprises: ammonium chloride, ammonium carbonate or carbonic hydroammonium, and perhaps their mixture, when any two in them mixed successively, its weight mixing ratio was (0.5-1): (1-2)); During three kinds of mixing, its weight mixing ratio is followed successively by (0.5-1): (1-2)): (2-5);
Adhesive wherein is selected from polytetrafluoroethylene or Kynoar;
(2). positive pole: the transition metal oxide by the embedding lithium constitutes, and is selected to comprise: the transition metal oxide of embedding lithium cobalt oxide, embedding lithium nickel oxide or embedding lithium manganese oxide embedding lithium;
(3). electrolyte: be organic mixed solvent solution of lithium salts, concentration is one mole, and lithium salts is selected from and comprises: lithium chlorate, LiBF4 or lithium hexafluoro phosphate;
Organic solvent is selected from: any two kinds combination in them of ethyl carbonate, diethyl carbonate, propene carbonate, glycol dimethyl ether, and volumetric mixture ratio is one to one;
(4). barrier film: be the high molecular polymer microporous membrane, comprise: polypropylene microporous film;
Such battery discharges and recharges its capacity of measuring continuously, reversible specific capacity between 350-454mAh/g,
2. according to the described lithium ion battery of claim 1, it is characterized in that, described battery:
(1). negative pole: its composition comprises: polyphenyl RESEARCH OF PYROCARBON, carbon black, polytetrafluoroethylene, their weight ratio is followed successively by: 10: 2: 1;
Polyphenyl RESEARCH OF PYROCARBON is wherein made by following method: be that 0.6 polyphenyl is under the nitrogen atmosphere that flow velocity rises for per minute 1-6 with the atom of hydrogen and carbon, speed with 20 ℃ of per minutes rises to 700-800 ℃, keep this temperature after 0.5-1.5 hour, temperature is dropped to 15-25 ℃ by per minute 1-3 ℃ speed;
(2). positive pole: be embedding lithium cobalt oxide;
(3). electrolyte: be that mixing ratio is one to one the ethyl carbonate and the lithium perchlorate solution of diethyl carbonate mixed liquor, its concentration is one mole;
(4). barrier film: be polypropylene microporous film;
This battery charges to 4.1 volts by the 25 milliamperes/speed of (gram carbon), is discharged to 2.0 volts, and recording reversible specific capacity is 380mAh/g,
3. according to the described lithium ion battery of claim 1, it is characterized in that the electrolyte of described battery: be that mixing ratio is one to one the propene carbonate and the lithium perchlorate solution of glycol dimethyl ether mixed liquor, its concentration is one mole; The reversible specific capacity of this battery is 350mAh/g,
4. according to the described lithium ion battery of claim 1, it is characterized in that, the negative pole of described battery comprises: polyphenyl RESEARCH OF PYROCARBON, carbon black, polytetrafluoroethylene and carbonic hydroammonium, their weight ratio is followed successively by: 10: 2: 1: 5, the reversible specific capacity of this battery is 454mAh/g, after 20 charge and discharge cycles, capacity is 402mAh/g
5. according to the described lithium ion battery of claim 1, it is characterized in that the just very embedding lithium manganese oxide of described battery; This battery charges to 4.3 volts by the 25 milliamperes/speed of (gram carbon), is discharged to 3.5 volts, and recording reversible specific capacity is 395mAh/g,
6. according to the described lithium ion battery of claim 1, it is characterized in that the negative pole of described battery comprises: polyphenyl RESEARCH OF PYROCARBON, carbon black, Kynoar and carbonic hydroammonium, their weight ratio is followed successively by: 10: 2: 1: 4, the reversible specific capacity of this battery is 412mAh/g
7. according to the described lithium ion battery of claim 1, it is characterized in that the positive pole of described battery: be the embedding lithium nickel oxide; Electrolyte is: mixing ratio is one to one the ethyl carbonate and the lithium hexafluoro phosphate solution of dimethyl carbonate mixed liquor, and its concentration is one mole, and the reversible specific capacity of this battery is 450mAh/g, and after 20 charge and discharge cycles, capacity is 410mAh/g,
8. the preparation method of claim 1,2,3,4,5,6 or 7 described batteries is characterized in that, described method comprises:
(1). the preparation of negative pole:
A. prepare the polyphenyl RESEARCH OF PYROCARBON, with the atomic ratio of hydrogen and carbon is polyphenyl pyrolysis in the nitrogen current that flow velocity rises for per minute 0.01-10 of 0.2-0.8, programming rate is per minute 2-40 ℃, keep 600-1100 ℃ heat treatment 0.5-48 hour, cooling is reduced to 15-25 ℃ with per minute 1-35 ℃ speed then, can obtain required RESEARCH OF PYROCARBON, this RESEARCH OF PYROCARBON is disordered carbon and its weight 0, the mixture of the graphite microcrystal of 001-2%;
B. add the aforesaid stabilizer of its weight 0-40% in the RESEARCH OF PYROCARBON that more than a certain amount of, makes, add aforesaid conductive agent of its weight 0.5-16% and the aforesaid bonding agent of 0.1-10% more respectively, after the grinding evenly, make the carbon negative pole with known method;
(2). select the transition metal oxide of aforesaid embedding lithium to do anodal;
(3). preparation electrolyte mixed organic solvents solution: concentration is 1 mole, and electrolyte is selected aforesaid lithium salts for use; Organic solvent is selected from any two kinds combination of aforementioned solvents, and their mixed volume ratio is one to one;
(4). select for use the high molecular polymer porous membrane to make barrier film;
Above-listed each material is assembled into the various model batteries that vary in size according to its functional requirement, is lithium ion battery of the present invention,
9. the purposes of claim 1,2,3,4,5,6 or 7 described batteries, it is characterized in that, the purposes of such battery comprises: be used for mobile phone, notebook computer, take the photograph player, electric automobile, because of it can be made into the different shape that varies in size, be suitable for using with electrical domain various.
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| Application Number | Priority Date | Filing Date | Title |
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| CN98100696A CN1087877C (en) | 1998-03-11 | 1998-03-11 | Lithium ion battery using high polymer pyrolytic carbon as negative pole |
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| CN98100696A CN1087877C (en) | 1998-03-11 | 1998-03-11 | Lithium ion battery using high polymer pyrolytic carbon as negative pole |
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| CN1228624A true CN1228624A (en) | 1999-09-15 |
| CN1087877C CN1087877C (en) | 2002-07-17 |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100349985C (en) * | 2004-07-03 | 2007-11-21 | 三星电子株式会社 | Non-humidified polymer electrolyte |
| CN102456915A (en) * | 2010-10-26 | 2012-05-16 | 通用汽车环球科技运作有限责任公司 | Electrolytic cell and method of estimating a state of charge thereof |
| CN102610791A (en) * | 2012-02-27 | 2012-07-25 | 宁德新能源科技有限公司 | Lithium ion battery for plug-in type hybrid power automobile and cathode thereof |
| CN102683745A (en) * | 2012-03-01 | 2012-09-19 | 华瑞(新乡)化工有限公司 | Method for preparing electrolyte of novel 5V lithium ion battery |
| CN103367806A (en) * | 2012-03-27 | 2013-10-23 | 中国科学院宁波材料技术与工程研究所 | Novel electrolyte system of lithium ion battery |
| CN106158412A (en) * | 2015-03-25 | 2016-11-23 | 江苏集盛星泰新能源科技有限公司 | A kind of lithium-ion capacitor and preparation method thereof |
| US11769871B2 (en) | 2005-10-20 | 2023-09-26 | Mitsubishi Chemical Corporation | Lithium secondary batteries and nonaqueous electrolyte for use in the same |
-
1998
- 1998-03-11 CN CN98100696A patent/CN1087877C/en not_active Expired - Lifetime
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100349985C (en) * | 2004-07-03 | 2007-11-21 | 三星电子株式会社 | Non-humidified polymer electrolyte |
| US11769871B2 (en) | 2005-10-20 | 2023-09-26 | Mitsubishi Chemical Corporation | Lithium secondary batteries and nonaqueous electrolyte for use in the same |
| CN102456915A (en) * | 2010-10-26 | 2012-05-16 | 通用汽车环球科技运作有限责任公司 | Electrolytic cell and method of estimating a state of charge thereof |
| CN102610791A (en) * | 2012-02-27 | 2012-07-25 | 宁德新能源科技有限公司 | Lithium ion battery for plug-in type hybrid power automobile and cathode thereof |
| CN102683745A (en) * | 2012-03-01 | 2012-09-19 | 华瑞(新乡)化工有限公司 | Method for preparing electrolyte of novel 5V lithium ion battery |
| CN102683745B (en) * | 2012-03-01 | 2015-08-19 | 华瑞(新乡)化工有限公司 | Voltage is the preparation method of the electrolyte of the new type lithium ion battery of 5V |
| CN103367806A (en) * | 2012-03-27 | 2013-10-23 | 中国科学院宁波材料技术与工程研究所 | Novel electrolyte system of lithium ion battery |
| CN106158412A (en) * | 2015-03-25 | 2016-11-23 | 江苏集盛星泰新能源科技有限公司 | A kind of lithium-ion capacitor and preparation method thereof |
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| CN1087877C (en) | 2002-07-17 |
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