CN101841064A - High capacity and Coulomb-efficiency lithium-ion capacitance battery anode system - Google Patents
High capacity and Coulomb-efficiency lithium-ion capacitance battery anode system Download PDFInfo
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- CN101841064A CN101841064A CN201010177428A CN201010177428A CN101841064A CN 101841064 A CN101841064 A CN 101841064A CN 201010177428 A CN201010177428 A CN 201010177428A CN 201010177428 A CN201010177428 A CN 201010177428A CN 101841064 A CN101841064 A CN 101841064A
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Abstract
The invention relates to a high capacity and Coulomb-efficiency lithium-ion capacitance battery anode system, belonging to the field of electrochemistry. The lithium-ion capacitance battery anode material comprises graphite-base anode material and activated carbon, and the electrolyte solution comprises ionic liquid and lithium salt, wherein the lithium salt is LiPF6 or LiN(CF3SO2)2, and the ionic liquid is 1-ethyl-3-methylimidazolium bis((trifluoromethyl)sulfonyl)imide salt or N-methyl, propyl piperidinium bis((trifluoromethyl)sulfonyl)imide which is used as solvent. The organic solvent of propylene carbonate, ethylene carbonate, dimethyl carbonate or ethyl methyl carbonate can be added into the electrolyte solution to be used as the functional additive. The capacity and the Coulomb efficiency of the lithium-ion capacitance battery anode material can be markedly improved in the electrolyte solution.
Description
Technical field
The present invention relates to improving one's methods of lithium ion capacitor battery cathode material capacity and coulombic efficiency, belong to electrochemical field.
Technical background
Lithium-ion capacitor battery is a development in recent years novel green energy storage device rapidly, it combines lithium ion cell high-capacity and the powerful advantage of ultracapacitor, these two kinds of energy storage system combinations of lithium ion battery and ultracapacitor have two kinds in the lithium-ion capacitor battery, and a kind of is " outer combination " formula (monomer that is about to both is combined into an energy storage component or system by power-supply management system); Another kind is " interior combination " formula (being about to both organically is combined in the same monomer).There are some researches show, can obtain good electrochemical by the capacitor batteries that " interior combination " constitutes based on active carbon electrode material ultracapacitor and lithium ion battery.
Lithium-ion capacitor battery has the energy storage device of the characteristics of lithium ion battery and ultracapacitor concurrently, promptly in a kind of device, have high energy density and power density simultaneously, shortcoming that power density is not high when overcoming lithium ion battery separately as electrical source of power and ultracapacitor be the not high shortcoming of energy density during separately as electrical source of power, is a kind of novel energy-storing device that development potentiality is relatively arranged.
At present, the negative material of lithium-ion capacitor battery mainly is lithium ion battery carbon base negative material and the compound system that has than the electrode material for super capacitor of bigger serface.In business-like lithium ion battery organic electrolysis plastidome, owing to provide the electrode material of electric double layer capacity to have very big specific area, in the charge and discharge process of capacitor batteries, form the SEI film and cause the reversible capacity of battery and first charge-discharge efficiency obviously to reduce, limited giving full play to of lithium-ion capacitor battery capacity.At present, the reversible capacity of lithium ion capacitor battery cathode material is lower than the theoretical capacity (372mAh/g) of graphite-based negative material, and coulombic efficiency is lower than 50% first.Therefore, improve the lithium-ion capacitor battery system, whether the reversible capacity and the first charge-discharge efficiency that improve its negative material can practical application have crucial effects for lithium-ion capacitor battery.
Reversible capacity and the low shortcoming of first charge-discharge efficiency at capacitor batteries, certain methods is used to improve lithium ion battery carbon base negative material reversible capacity and first charge-discharge efficiency, as adopt higher lithium ion battery negative material of removal lithium embedded current potential (as lithium titanate) and electrode material for super capacitor compound, mainly utilize lithium titanate to discharge and recharge the characteristics of current potential height (about 1.5V), avoided forming the SEI film in electrode material surface, therefore, reversible capacity and first charge-discharge efficiency have been improved.But the negative material that adopts in this method discharges and recharges the current potential height, can reduce the energy density of capacitor batteries.Therefore, exploitation a kind of can improve capacitor batteries reversible capacity and first charge-discharge efficiency and don't influence the method for other performance necessary.
The advantage that ionic liquid has that conductance height, steam force down, electrochemical window is wide, chemistry and electrochemical stability is good, pollution-free and easy recovery etc. are given prominence to is described as green solvent.Not only can widen the operating temperature range of battery as lithium ion battery electrolyte, and can improve the fail safe of battery under high power density, eliminate the potential safety hazard of lithium ion battery.
The present invention is a kind of have the lithium ion capacitor battery cathode material capacity of development potentiality and improving one's methods of coulombic efficiency to contain ion liquid electrolyte as the electrolyte of lithium-ion capacitor battery, constitute reversible capacity and the coulombic efficiency that electrode system improves lithium ion capacitor battery cathode material with the mixture of graphite-based material and active carbon as lithium ion capacitor battery cathode material.
Summary of the invention
The object of the invention is to provide a kind of lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency, constitute lithium ion capacitor battery cathode material with graphite-based material and active carbon, the mass ratio of graphite-based material and active carbon is 1: 0.1～1, it is characterized in that, to contain the ion-conducting material of ion liquid electrolyte solution as lithium-ion capacitor battery, constitute the electrode system of lithium ion capacitor battery cathode, contain ion liquid electrolyte solution by ionic liquid with contain lithium electrolyte salt and constitute, ionic liquid wherein is the two fluoroform sulfimide salt of 1-ethyl-3-methylimidazole, in the two fluoroform sulfimide salt of N-methyl-propyl piperidines one or both, containing lithium electrolyte salt is LiPF
6And LiN (CF
3SO
2)
2In one or both, containing the molar concentration of lithium electrolyte salt in electrolyte solution is 0.5～1.4mol/L.
A kind of lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency, described graphite-based material is one or both in MCMB, the Delanium.
A kind of lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency, also contain organic solvent in the described electrolyte solution, the quality of organic solvent is smaller or equal to 50% of the electrolyte solution quality, and organic solvent is one or more in propene carbonate, ethylene carbonate, dimethyl carbonate and the methyl ethyl carbonate.
The present invention has the following advantages and good effect:
The present invention is directed to the lithium ion capacitor battery cathode material that graphite-based material and active carbon constitute, employing contains ion liquid electrolyte solution, can significantly improve the reversible capacity of lithium ion capacitor battery cathode material and coulombic efficiency first, reversible capacity can be up to 600mAh/g, and coulombic efficiency is greater than 90% first; And in conventional electrolysis matter solution, the reversible capacity of lithium ion capacitor battery cathode material is less than 372mAh/g, and coulombic efficiency is less than 50% first.So this invention has solved in conventional electrolysis matter solution a lithium ion capacitor battery cathode material reversible capacity and the low difficult problem of coulombic efficiency first effectively.
Description of drawings
Fig. 1: the first charge-discharge curve (0.1C) of lithium ion capacitor battery cathode material in its corresponding electrolyte solution among the embodiment of the invention 1 and the embodiment 2; 1-embodiment 1; 2-embodiment 2.
Fig. 2: the first charge-discharge curve (0.1C) of lithium ion capacitor battery cathode material in its corresponding electrolyte solution in the embodiment of the invention 3.
Embodiment
The invention will be further described below in conjunction with the drawings and specific embodiments, but the present invention is not subjected to any qualification of these embodiment, can carry out suitable change and implement in the scope that does not change feature of the present invention.
Embodiment 1:
Select for use MCMB and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 0.25; With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with LiN (CF
3SO
2)
2Constitute electrolyte solution for containing lithium electrolyte salt, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 0.8mol/L.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
Among Fig. 1, curve 1 is the first charge-discharge curve of embodiment 1 lithium ion capacitor battery cathode material in the electrolyte solution of embodiment 1, as can be seen from the figure, in this electrolyte solution, the first reversible capacity of lithium ion capacitor battery cathode material in the 0.1C charge and discharge process is 638.1mAh/g, and coulombic efficiency is 93% first.
Embodiment 2:
Select for use Delanium and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of Delanium and active carbon is 1: 0.25; With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with propene carbonate as organic solvent, with LiN (CF
3SO
2)
2For containing lithium electrolyte salt, constitute electrolyte solution, and the concentration that contains lithium electrolyte salt is 0.8mol/L, the quality of organic solvent equals 30% of electrolyte solution quality.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
Among Fig. 1, curve 2 is the first charge-discharge curves of embodiment 2 lithium ion capacitor battery cathode materials at the electrolyte solution of embodiment 2, as can be seen from the figure, in this electrolyte solution, the first reversible capacity of lithium ion capacitor battery cathode material in the 0.1C charge and discharge process is 511mAh/g, and first charge-discharge efficiency is 92.07%.
Embodiment 3:
Select for use MCMB and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 0.25; With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with LiN (CF
3S O
2)
2For containing lithium electrolyte salt, constitute electrolyte solution, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 0.8mol/L.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
Fig. 2 is the first charge-discharge curves of middle embodiment 3 lithium ion capacitor battery cathode materials in the electrolyte solution of embodiment 3, as can be seen from the figure, in this electrolyte solution, the first reversible capacity of lithium ion capacitor battery cathode material in the 0.1C charge and discharge process is 382mAh/g, and coulombic efficiency is 99.8% first.
Embodiment 4:
Select for use MCMB and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 0.1; With the N-methyl, the two fluoroform sulfimide salt ion liquid of propyl group piperidines are as solvent, with LiN (CF
3SO
2)
2For containing lithium electrolyte salt, constitute electrolyte solution, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 0.5mol/L.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
After tested, in this electrolyte solution, the first reversible capacity of embodiment 4 lithium ion capacitor battery cathode materials in the 0.1C charge and discharge process is 380.1mAh/g, and coulombic efficiency is 99.6% first.
Embodiment 5:
Select for use MCMB and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 1; With the N-methyl, the two fluoroform sulfimide salt ion liquid of propyl group piperidines are as solvent, with LiPF
6For containing lithium electrolyte salt, constitute electrolyte solution, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 1.4mol/L.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
After tested, in this electrolyte solution, the first reversible capacity of embodiment 5 lithium ion capacitor battery cathode materials in the 0.1C charge and discharge process is 495.6mAh/g, and coulombic efficiency is 97.1% first.
Embodiment 6:
Select for use two kinds of silicon/carbon/graphite in lithium ion batteries based composites of MCMB and Delanium and active carbon as lithium ion capacitor battery cathode material, and the quality of graphite-base composite material and active carbon is 1: 0.5; With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with propene carbonate as organic solvent, with LiN (CF
3SO
2)
2For containing lithium electrolyte salt, constitute electrolyte solution, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 0.8mol/L, the quality of organic solvent equals 1% of electrolyte solution quality.Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
After tested, in this electrolyte solution, the first reversible capacity of embodiment 6 lithium ion capacitor battery cathode materials in the 0.1C charge and discharge process is 511.2mAh/g, and coulombic efficiency is 92.7% first.
Embodiment 7:
Select for use MCMB and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 0.2; With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with propene carbonate as organic solvent, with LiPF
6For containing lithium electrolyte salt, constitute electrolyte solution, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 1mol/L, the quality of organic solvent equals 50% of electrolyte solution quality; Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
After tested, in this electrolyte solution, the first reversible capacity of embodiment 7 lithium ion capacitor battery cathode materials in the 0.1C charge and discharge process is 426.6mAh/g, and coulombic efficiency is 98.9% first.
Embodiment 8:
Select for use Delanium and active carbon as lithium ion capacitor battery cathode material, and the mass ratio of MCMB and active carbon is 1: 0.6.With the two fluoroform sulfimide salt ion liquid of 1-ethyl-3-methylimidazole as solvent, with ethylene carbonate, dimethyl carbonate and methyl ethyl carbonate as organic solvent, with LiPF
6And LiN (CF
3SO
2)
2For containing lithium electrolyte salt, constitute electrolyte solvent, and to contain the concentration of lithium electrolyte salt in electrolyte solution be 1mol/L, the gross mass of organic solvent equals 30% of electrolyte solution quality; Constitute the lithium ion capacitor battery cathode system of test by above-mentioned lithium ion capacitor battery cathode material and electrolyte solution.
After tested, in this electrolyte solution system, the first reversible capacity of embodiment 8 lithium ion capacitor battery cathode materials in the 0.1C charge and discharge process is 391.6mAh/g, and coulombic efficiency is 99.2% first.
Claims (4)
1. lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency, constitute lithium ion capacitor battery cathode material with graphite-based material and active carbon, the mass ratio of graphite-based material and active carbon is 1: 0.1～1, it is characterized in that: to contain the ion-conducting material of ion liquid electrolyte solution as lithium-ion capacitor battery, constitute the electrode system of lithium ion capacitor battery cathode, contain ion liquid electrolyte solution by ionic liquid with contain lithium electrolyte salt and constitute, described ionic liquid is the two fluoroform sulfimide salt of 1-ethyl-3-methylimidazole, in the two fluoroform sulfimide salt of N-methyl-propyl piperidines one or both, containing lithium electrolyte salt is LiPF
6And LiN (CF
3SO
2)
2In one or both, containing the molar concentration of lithium electrolyte salt in electrolyte solution is 0.5～1.4mol/L.
2. the lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency according to claim 1 is characterized in that: described graphite-based material is one or both in MCMB, the Delanium.
3. the lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency according to claim 1 also contains organic solvent in the described electrolyte solution, the quality of organic solvent is smaller or equal to 50% of the electrolyte solution quality.
4. the lithium ion capacitor battery cathode system with high power capacity and coulombic efficiency according to claim 3 is characterized in that: described organic solvent is one or more in propene carbonate, ethylene carbonate, dimethyl carbonate and the methyl ethyl carbonate.
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102127782A (en) * | 2011-01-18 | 2011-07-20 | 上海交通大学 | Method for preparing super-hydrophobic indium antimonide film by deposition in ionic liquid |
| CN102544634A (en) * | 2011-09-02 | 2012-07-04 | 渤海大学 | Mixed electrolyte and preparation method and application thereof |
| CN102719863A (en) * | 2011-01-18 | 2012-10-10 | 上海交通大学 | Method for depositing and preparing super-hydrophobic indium antimonide thin film from ionic liquid |
| CN103367708A (en) * | 2012-03-29 | 2013-10-23 | 海洋王照明科技股份有限公司 | Battery positive pole and preparation method thereof, battery negative pole and preparation method thereof, and capacitor battery |
| CN103833675A (en) * | 2012-11-26 | 2014-06-04 | 海洋王照明科技股份有限公司 | Piperidine ionic liquid, and preparation method and application thereof |
| CN103833661A (en) * | 2012-11-26 | 2014-06-04 | 海洋王照明科技股份有限公司 | Oxazolidine ionic liquid, and preparation method and application thereof |
| CN105190810A (en) * | 2013-03-19 | 2015-12-23 | 住友电气工业株式会社 | Lithium ion capacitor and method for charging and discharging same |
| CN105706202A (en) * | 2013-11-08 | 2016-06-22 | 住友电气工业株式会社 | Alkali metal ion capacitor, method for manufacturing same, and method for charging/discharging same |
| CN106504912A (en) * | 2015-09-04 | 2017-03-15 | 罗伯特·博世有限公司 | hybrid super capacitor |
| CN109560320A (en) * | 2011-12-06 | 2019-04-02 | 阿克马法国公司 | Purposes of the lithium salt mixture as lithium ion battery electrolyte |
| CN112952194A (en) * | 2021-04-14 | 2021-06-11 | 苏州大学张家港工业技术研究院 | Low-temperature battery electrolyte based on ionic liquid and preparation method and application thereof |
| CN113823838A (en) * | 2021-10-27 | 2021-12-21 | 湖南法恩莱特新能源科技有限公司 | Composite lithium ion electrolyte and battery containing same |
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Cited By (15)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102127782A (en) * | 2011-01-18 | 2011-07-20 | 上海交通大学 | Method for preparing super-hydrophobic indium antimonide film by deposition in ionic liquid |
| CN102719863A (en) * | 2011-01-18 | 2012-10-10 | 上海交通大学 | Method for depositing and preparing super-hydrophobic indium antimonide thin film from ionic liquid |
| CN102544634A (en) * | 2011-09-02 | 2012-07-04 | 渤海大学 | Mixed electrolyte and preparation method and application thereof |
| CN102544634B (en) * | 2011-09-02 | 2013-10-23 | 渤海大学 | Mixed electrolyte and preparation method and application thereof |
| CN109560320A (en) * | 2011-12-06 | 2019-04-02 | 阿克马法国公司 | Purposes of the lithium salt mixture as lithium ion battery electrolyte |
| CN103367708A (en) * | 2012-03-29 | 2013-10-23 | 海洋王照明科技股份有限公司 | Battery positive pole and preparation method thereof, battery negative pole and preparation method thereof, and capacitor battery |
| CN103833661A (en) * | 2012-11-26 | 2014-06-04 | 海洋王照明科技股份有限公司 | Oxazolidine ionic liquid, and preparation method and application thereof |
| CN103833661B (en) * | 2012-11-26 | 2016-04-20 | 海洋王照明科技股份有限公司 | Azoles alkanes ionic liquid and its preparation method and application |
| CN103833675B (en) * | 2012-11-26 | 2016-04-27 | 海洋王照明科技股份有限公司 | Piperidines ionic liquid and its preparation method and application |
| CN103833675A (en) * | 2012-11-26 | 2014-06-04 | 海洋王照明科技股份有限公司 | Piperidine ionic liquid, and preparation method and application thereof |
| CN105190810A (en) * | 2013-03-19 | 2015-12-23 | 住友电气工业株式会社 | Lithium ion capacitor and method for charging and discharging same |
| CN105706202A (en) * | 2013-11-08 | 2016-06-22 | 住友电气工业株式会社 | Alkali metal ion capacitor, method for manufacturing same, and method for charging/discharging same |
| CN106504912A (en) * | 2015-09-04 | 2017-03-15 | 罗伯特·博世有限公司 | hybrid super capacitor |
| CN112952194A (en) * | 2021-04-14 | 2021-06-11 | 苏州大学张家港工业技术研究院 | Low-temperature battery electrolyte based on ionic liquid and preparation method and application thereof |
| CN113823838A (en) * | 2021-10-27 | 2021-12-21 | 湖南法恩莱特新能源科技有限公司 | Composite lithium ion electrolyte and battery containing same |
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Open date: 20100922 |