CN102810690A - High-voltage ionic liquid electrolyte for lithium ion battery and preparation method of high-voltage ionic liquid electrolyte - Google Patents
High-voltage ionic liquid electrolyte for lithium ion battery and preparation method of high-voltage ionic liquid electrolyte Download PDFInfo
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- CN102810690A CN102810690A CN2012102652922A CN201210265292A CN102810690A CN 102810690 A CN102810690 A CN 102810690A CN 2012102652922 A CN2012102652922 A CN 2012102652922A CN 201210265292 A CN201210265292 A CN 201210265292A CN 102810690 A CN102810690 A CN 102810690A
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Abstract
The invention relates to ionic liquid electrolyte for a high-voltage lithium ion battery, which effectively improves the circulating property and security performance of the high-voltage lithium ion battery. The ionic liquid in the lithium ion battery electrolyte is a series of imidazolium ionic liquid of unitary, binary or triple substitution; the battery composed of the ionic liquid electrolyte is charged and discharged at 0.1C multiplying power; the retention rate of the discharge capacity is 65%, and the charge and discharge efficiency is basically kept over 98%; and the circulating property of the high-voltage lithium ion battery is ensured, and the security of the battery is also improved by adding ionic liquid.
Description
Technical field
The present invention relates to a kind of il electrolyte that is used for high-voltage lithium ion batteries, more specifically, the present invention relates to high voltage and improve the il electrolyte of the lithium ion battery of battery performance.
Background technology
Because the high-tech electronics industrial expansion, it is littler and lighter that electronic equipment becomes, thus the increase that causes portable electronic instrument to use.Research to lithium secondary battery is carried out energetically, so that satisfy the needs to high energy density cells that increase day by day, said battery is as the power supply of these portable electronic instruments.
Present employed anode material for lithium-ion batteries is like LiCoO
2, LiMn
2O
4And the voltage platform of novel nickel-cobalt-manganese ternary material is approximately 4V, limited the power of battery, and lithium ion battery with cobalt be positive electrode because the cobalt resource rareness causes costing an arm and a leg, can not be widely used on the large-sized power instrument.Though LiMn2O4 is relatively cheap because of manganese aboundresources price, and safety non-pollution, its high temperature circulation poor stability and the serious problem of capacity attenuation also are not well solved, and its commercialization is restricted.
To LiMn
2O
4Find LiMn2O4 LiMn in the study on the modification by Transition metal substituted
2-XM
xO
4(M=Cr, Co, Ni, Cu, Fe, Mo, cycle performance V) obviously is superior to LiMn
2O
4, and along with the increase of transient metal doped amount, another discharge platform appears in material near 5V.At these spinelles LiMn
2-XM
xO
4In the material, LiMn
1.5Ni
0.5O
4Because of having better cycle performance and higher relatively capacity receives extensive concern.Its theoretical capacity is 147mAh/g, and energy density is 690Wh/Kg.
As the positive electrode in the exploitation, the key problem that the nickel LiMn2O4 exists mainly is: needing can be at the electrolyte of steady operation under the high voltage.Since historical reasons, present widely used LiPF
6The main application fields of electrolyte is to be positive pole with cobalt acid lithium; With graphite is the lithium ion battery of negative pole; The operating voltage of this type battery is the highest also can only to reach 4.2V; So the design of electrolyte system also generally can only guarantee in the scope below 4.5V stable the use, and the high charge cut-ff voltage of nickel LiMn2O4 can reach 5.2V, so conventional electrolysis liquid oxidation Decomposition problem with this understanding becomes obviously.The raising of anodal current potential means that also the reproducibility environment in negative pole zone strengthens; This has also caused the dynamics that surperficial SEI film (solid electrolyte interface film) forms behind the traditional graphite cathode of nickel LiMn2O4 coupling to change; Isolate electrolyte and material with carbon element and can not form effective SEI film, then the cycle life of negative material also reduces greatly.
Summary of the invention
In order to address the above problem, the purpose of this invention is to provide a kind of il electrolyte that is used for high-voltage lithium ion batteries, it can improve with the nickel LiMn2O4 is the fail safe and the chemical property of master's high-voltage lithium ion batteries.
In order to realize above-mentioned aspect, the present invention provides a kind of high-voltage lithium ion batteries electrolyte, and wherein this electrolyte comprises lithium salts, organic solvent, and ionic liquid, and this ionic liquid is a series of glyoxaline ion liquids, its anion can be PF
6 -, BF
4 -, TFSI
-, FSI
-, BOB
-Deng.
Ion liquid solvent provided by the invention is characterized in that: described ionic liquid cation has following structure, and this ionic liquid shared part by weight in lithium battery electrolytes is 0.1%-95%;
Be substituted by monobasic, binary or ternary in the said structure and replace, and, R
1, R
2, R
3Independently be selected from alkyl, alkoxyl, aromatic radical, carboxyl, hydroxyl, cyanic acid, nitro, ether oxygen base, the halogen of carbon atom between 0-20 respectively.Especially respectively independently be selected from following group: it is PF that methyl, ethyl, propyl group, butyl, vinyl, pi-allyl, cyclobutenyl, ethenylidene, phenyl, benzyl or benzyl, X can be selected from
6 -, BF
4 -, TFSI
-, FSI
-, BOB
-Deng.
Above-mentioned ion liquid cation preferentially is selected from least a in the following several kinds of materials: 1-vinyl-2-ethyl-3-methylimidazole cation, 1-vinyl-2-propyl group-3-methylimidazole cation, 1-pi-allyl-2-ethyl-3-ethyl imidazol(e) cation; 1-pi-allyl-2-propyl group-3-methylimidazole cation, 1-vinyl-2-pi-allyl-3-methylimidazole cation, 1-pi-allyl-2-pi-allyl-3-methylimidazole cation; 1-ethyl-2-vinyl imidazole cation, 1-propyl group-2-vinyl imidazole cation, 1-pi-allyl-2-ethyl imidazol(e) cation; 1-pi-allyl-2-propyl imidazole cation, 1-vinyl-2-allyl imidazole cation, 1-pi-allyl-2-allyl imidazole cation; 1-ethenylidene-2-pi-allyl-3-methylimidazole cation, 1-phenyl-2-pi-allyl-3-methylimidazole cation, 1-benzyl-2-pi-allyl-3-methylimidazole cation; 2-phenyl-1-methylimidazole cation, 2-ethenylidene-1-ethyl imidazol(e) cation, 2-vinyl-1-phenylimidazole cation; 2-phenylimidazole cation; 2-vinyl-3-methylimidazole cation, 2-pi-allyl-3-methylimidazole cation, 2-ethenylidene glyoxaline cation.
Said lithium salts is selected from LiPF
6, LiBF
4, LiTFSI, LiFSI, LiBOB etc.
In addition, preferred organic is selected from ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, ethyl acetate, at least a in the sulfolane, and their mixture.
The il electrolyte of described high-voltage lithium ion batteries, wherein the mass percent of lithium salts is 5～50%, and ion liquid mass percent is 0.1～95%, and the mass percent of organic solvent is 5～90%.
The invention has the beneficial effects as follows, in lithium-ion battery electrolytes, add described additive, can effectively promote the graphite cathode film forming, and then improve the cycle performance and the security performance of battery, have higher market popularization value.
Description of drawings
Fig. 1,2 is respectively the cycle discharge curve of the battery of the embodiment of the invention 4, with cyclic voltammogram.
Embodiment
The present invention explains with following embodiment, but is not limited to following embodiment, before and after not breaking away from, in the scope of said aim, changes and implements to be included within the technical scope of the present invention.
Embodiment 1:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) mass ratio with 1:1 is mixed, be made into mixed solvent.Get mixed solvent 99 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 1 part of additive 1-phenyl of the present invention-2-pi-allyl-3-methylimidazole, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-phenyl-2-pi-allyl-3-methylimidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-phenyl-2-pi-allyl-3-methylimidazole, 1wt.%.
Anodal preparation: with a certain amount of LiMn
1.5Ni
0.5O
4Be dispersed in by Kynoar (PVDF) with acetylene black and be dissolved in the solvent in the N-N-methyl-2-2-pyrrolidone N-(NMP), obtain uniform slurry, be coated on the aluminium foil in 80 ℃ of vacuum oven dry 12 hours, obtain anode pole piece after the calendering.
The preparation of negative pole: phase microballoon (CMS) in the middle of a certain amount of carbon and acetylene black is dispersed in by Kynoar (PVDF) is dissolved in the solvent in the N-N-methyl-2-2-pyrrolidone N-(NMP); Obtain uniform slurry; Be coated on the Copper Foil and in 80 ℃ of vacuum, dried 12 hours, obtain cathode pole piece after the calendering.
The preparation of lithium ion battery: above-mentioned positive pole and cathode pole piece and Celgand2400 barrier film are assembled into battery, simultaneously the resulting electrolyte in front are added in this battery, sealing makes lithium ion battery.
Embodiment 2:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) mass ratio with 1:1 is mixed, be made into mixed solvent.Get mixed solvent 97 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 3 parts of additive 1-phenyl of the present invention-2-pi-allyl-3-methylimidazoles, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-phenyl-2-pi-allyl-3-methylimidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-phenyl-2-pi-allyl-3-methylimidazole, 3wt.%.
Electrolyte according to the same procedure of embodiment 1 adopts present embodiment to obtain is prepared lithium ion battery.
Embodiment 3:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) mass ratio with 1:1 is mixed, be made into mixed solvent.Get mixed solvent 95 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 5 parts of additive 1-phenyl of the present invention-2-pi-allyl-3-methylimidazoles, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-phenyl-2-pi-allyl-3-methylimidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-phenyl-2-pi-allyl-3-methylimidazole, 5wt.%.
Electrolyte according to the same procedure of embodiment 1 adopts present embodiment to obtain is prepared lithium ion battery.
Embodiment 4:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) mass ratio with 1:1 is mixed, be made into mixed solvent.Get mixed solvent 99 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 1 part of additive 1-propyl group of the present invention-2-vinyl imidazole, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-propyl group-2-vinyl imidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-propyl group-2-vinyl imidazole, 1wt.%.
Electrolyte according to the same procedure of embodiment 1 adopts present embodiment to obtain is prepared lithium ion battery.
Embodiment 5:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) with the mixed of 1:1, are made into mixed solvent.Get mixed solvent 97 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 3 parts of additive 1-propyl group of the present invention-2-vinyl imidazoles, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-propyl group-2-vinyl imidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-propyl group-2-vinyl imidazole, 3wt.%.
Electrolyte according to the same procedure of embodiment 1 adopts present embodiment to obtain is prepared lithium ion battery.
Embodiment 6:
Ethylene carbonate (EC) and dimethyl carbonate (DMC) mass ratio with 1:1 is mixed, be made into mixed solvent.Get mixed solvent 95 parts, add two (trifluoromethyl sulphonyl) inferior amine salts of 5 parts of additive 1-propyl group of the present invention-2-vinyl imidazoles, add a certain amount of LiPF
6, make it be formulated as the electrolyte of 1M.
Configuration electrolyte carries out in glove box (water, oxygen content are all less than 1ppm); Two (trifluoromethyl sulphonyl) inferior amine salts of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and 1-propyl group-2-vinyl imidazole are mixed, add LiPF at last
6, make its solution that becomes 1M, prepare electrolyte of the present invention.
Weight with electrolyte is benchmark, and the composition of this additive is: two (trifluoromethyl sulphonyl) inferior amine salts of 1-pi-allyl-2-ethyl imidazol(e), 5wt.%.
Electrolyte according to the same procedure of embodiment 1 adopts present embodiment to obtain is prepared lithium ion battery.
Claims (5)
1. the il electrolyte of a high-voltage lithium ion batteries comprises: non-aqueous organic solvent, lithium salts, and ionic liquid, and described ionic liquid comprises zwitterion, cation has following structure,
Be substituted by monobasic, binary or ternary in the said structure and replace, and R1, R2, R3 independently are selected from carbon atom respectively
Alkyl between 0-20, alkoxyl, aromatic radical, carboxyl, hydroxyl, cyanic acid, nitro, ether oxygen base, halogen.
2. il electrolyte according to claim 1 is characterized in that: substituent R
1, R
2, R
3Independently be selected from following group respectively: methyl, ethyl, propyl group, butyl, vinyl, pi-allyl, cyclobutenyl, ethenylidene, phenyl, benzyl or benzyl.
3. il electrolyte according to claim 1 and 2 is characterized in that: described ionic liquid cation is selected from least a in the following several kinds of materials: 1-ethyl-2-vinyl-3-methylimidazole cation, 1-propyl group-2-vinyl-3-methylimidazole cation; 1-pi-allyl-2-ethyl-3-ethyl imidazol(e) cation, 1-pi-allyl-2-propyl group-3-methylimidazole cation, 1-vinyl-2-pi-allyl-3-methylimidazole cation; 1-pi-allyl-2-pi-allyl-3-methylimidazole cation, 1-ethyl-2-vinyl imidazole cation, 1-propyl group-2-vinyl imidazole cation; 1-pi-allyl-2-ethyl imidazol(e) cation, 1-pi-allyl-2-propyl imidazole cation, 1-vinyl-2-allyl imidazole cation; 1-pi-allyl-2-allyl imidazole cation, 1-ethenylidene-2-pi-allyl-3-methylimidazole cation, 1-phenyl-2-pi-allyl-3-methylimidazole cation; 1-benzyl-2-pi-allyl-3-methylimidazole cation; 2-phenyl-1-methylimidazole cation, 2-ethenylidene-1-ethyl imidazol(e) cation, 2-vinyl-1-phenylimidazole cation; 2-phenylimidazole cation; 2-vinyl-3-methylimidazole cation, 2-pi-allyl-3-methylimidazole cation, 2-ethenylidene glyoxaline cation.
4. the ionic liquid in the il electrolyte according to claim 1 and 2 is characterized in that: be selected from least a in following several kinds: PF with the anion of ionic liquid cation complexing
6 -, BF
4 -, TFSI
-, FSI
-, BOB
-
5. the il electrolyte of high-voltage lithium ion batteries according to claim 1, wherein the mass percent of lithium salts is 5～50%, and ion liquid mass percent is 0.1～95%, and the mass percent of organic solvent is 5～90%.
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103151560A (en) * | 2013-02-05 | 2013-06-12 | 东莞新能源科技有限公司 | Lithium ion battery electrolyte solution and its additive |
| CN104466237A (en) * | 2014-12-09 | 2015-03-25 | 上海交通大学 | Composite mesoporous silica (IL/SiO2) for encapsulating ionic liquid and preparation and application thereof |
| CN108336412A (en) * | 2018-01-16 | 2018-07-27 | 深圳大学 | A kind of lithium ion battery electrolyte and preparation method thereof and lithium ion battery |
| CN111477964A (en) * | 2020-04-14 | 2020-07-31 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device |
| CN112086683A (en) * | 2019-06-14 | 2020-12-15 | 比亚迪股份有限公司 | Lithium ion battery electrolyte, preparation method thereof, high-voltage lithium ion battery and battery module |
| CN113474932A (en) * | 2019-02-27 | 2021-10-01 | 大金工业株式会社 | Electrolyte solution, electrochemical device, lithium ion secondary battery, module, and compound |
| CN114725509A (en) * | 2022-04-25 | 2022-07-08 | 西安交通大学 | Sulfone-based lithium battery electrolyte and lithium battery |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103151560A (en) * | 2013-02-05 | 2013-06-12 | 东莞新能源科技有限公司 | Lithium ion battery electrolyte solution and its additive |
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| CN104466237A (en) * | 2014-12-09 | 2015-03-25 | 上海交通大学 | Composite mesoporous silica (IL/SiO2) for encapsulating ionic liquid and preparation and application thereof |
| CN108336412A (en) * | 2018-01-16 | 2018-07-27 | 深圳大学 | A kind of lithium ion battery electrolyte and preparation method thereof and lithium ion battery |
| CN113474932A (en) * | 2019-02-27 | 2021-10-01 | 大金工业株式会社 | Electrolyte solution, electrochemical device, lithium ion secondary battery, module, and compound |
| CN112086683A (en) * | 2019-06-14 | 2020-12-15 | 比亚迪股份有限公司 | Lithium ion battery electrolyte, preparation method thereof, high-voltage lithium ion battery and battery module |
| CN111477964A (en) * | 2020-04-14 | 2020-07-31 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device |
| CN111477964B (en) * | 2020-04-14 | 2021-06-25 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device |
| CN114725509A (en) * | 2022-04-25 | 2022-07-08 | 西安交通大学 | Sulfone-based lithium battery electrolyte and lithium battery |
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Application publication date: 20121205 |