CN103730263A - Organic electrolytic solution for super capacitor and super capacitor - Google Patents
Organic electrolytic solution for super capacitor and super capacitor Download PDFInfo
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- CN103730263A CN103730263A CN201310739205.7A CN201310739205A CN103730263A CN 103730263 A CN103730263 A CN 103730263A CN 201310739205 A CN201310739205 A CN 201310739205A CN 103730263 A CN103730263 A CN 103730263A
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/13—Energy storage using capacitors
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Abstract
The invention discloses an organic electrolytic solution for a super capacitor. The organic electrolytic solution for the super capacitor comprises a proton inert solvent, an organic electrolyte and an additive. Preferably, the organic electrolyte and the proton inert solvent form a 0.5-2.0mol/L solution. The additive accounts for 0.05wt%-5wt% of the organic electrolytic solution. The organic electrolytic solution for the super capacitor has the advantages that appropriate proton inert solvent components and the appropriate additive are selected, the solution ability and the dissociation ability of the electrolyte in the proton inert solvent are improved, the ion conductivity of the electrolytic solution is improved, so that the internal resistance of the organic electrolytic solution is reduced, the electrochemical stability window of the electrolytic solution is improved, and therefore the super capacitor can be used at a high working voltage (over 2.7V) and is high in power density and energy density and long in cycle life.
Description
Technical field
The present invention relates to electrochemical field, relate in particular to a kind of for ultracapacitor organic electrolyte and apply the ultracapacitor of this organic electrolyte.
Background technology
Ultracapacitor, is also gold capacitor, electrochemical capacitor, adopts ionic adsorption (double electric layer capacitor) or surperficial Quick Oxidation reduction reaction (fake capacitance device) to carry out stored energy.Ultracapacitor is a kind of novel energy-storing device between battery and conventional electrostatic capacitor.The electric charge of ultracapacitor storage is the one-tenth hundred of conventional solid-state electrochemical capacitor or thousands of times, can within the several seconds, discharge and recharge completely, has the power higher than battery and inputs or outputs, and can within the shorter time, reach.Simultaneously, it is short that ultracapacitor has the time of discharging and recharging, storage life is long, stability is high, the advantages such as operating temperature range wide (40 ℃～70 ℃), thereby be widely used in consumer electronics product field, grid-connected power generation system field, distributed energy storage system field, intelligent distributed network system field, the field of traffic such as new-energy automobile, energy-conserving elevator crane even load field, the military equipment fields such as ELECTROMAGNETIC BOMB and motion control field etc., relate to generation of electricity by new energy, intelligent grid, new-energy automobile, energy saving building, the industry-by-industries such as industrial energy saving reduction of discharging, the complete series low-carbon economy core product that belongs to standard.
Ultracapacitor is as one of promising energy storage device of tool in new energy field, become the countries such as the U.S., Japan, Korea S and Russia at present at one of focus of the multidisciplinary crossing domain researchs such as material, electric power, physics, chemistry.Main goal in research is the good and low-cost electrode material of processability; The electrolyte based material of, chemistry high with conductivity and Heat stability is good, operating voltage high (electrochemical stability window is wide), and prepare on this basis high-energy-density, high power density and long service life can be used for the unify ultracapacitor energy storage device of the aspects such as back-up source of electronic equipment of various electronic hybrid vehicle hybrid power systems.
The energy density of ultracapacitor is lower than battery, and this has limited its some practical applications.Square being directly proportional of the energy of ultracapacitor storage and voltage, is shown below:
In formula, E represents energy, (J); C is electric capacity, (F); V is the operating voltage of capacitor, (V).If voltage increases by three times, the energy of same capacitance stores will increase approximately order of magnitude.Therefore, therefore improving operating voltage is to improve the highly effective means of super capacitor energy density.But under high voltage, electrolyte easily decomposes, cause that capacity is decayed fast and internal resistance sharply increases.Thereby to improve the operating voltage of ultracapacitor, key point is to improve the high voltage performance of electrolyte.With organic electrolyte, replace aqueous electrolyte, capacitor working is pressed can bring up to 2.5～2.7V from 0.9V.Because propene carbonate and acetonitrile have good electrochemistry and chemical stability and to the good dissolubility of organic quaternary ammonium salt class, be widely used in the electrolyte system of ultracapacitor.Because the viscosity of AN is significantly less than PC, adopt AN high more a lot of as the conductivity of the electrolyte of solvent than adopting PC as the electrolyte of solvent, the advantage of AN is more obvious especially at low temperatures.But AN has certain toxicity, be unfavorable for personal safety and environmental protection.Although the operating voltage of AN system is 2.7V, and the operating voltage of PC system is 2.5V.With respect to the operating voltage more than 3V expecting, also has no small distance.
Summary of the invention
In view of this, goal of the invention of the present invention is in order to explain above-mentioned technical problem, a kind of low viscosity, conductivity is high, decomposition voltage is high organic electrolyte is provided and applies the ultracapacitor of this organic electrolyte.
In order to realize foregoing invention object, the technical solution used in the present invention is:
For an organic electrolyte for ultracapacitor, comprise aprotic solvent, organic bath and additive, described additive is one or more combinations in shown in pyridine, pyridine derivate, pyrroles, azole derivatives or structural formula (1),
R wherein
1, R
2, R
3for carbon number be 1-6 alkyl or silylation.
Wherein, described structural formula (1) is triethylamine, tripropyl amine (TPA), tri-n-butylamine, triamylamine, three (trimethyl silicane) amine, 1-methyl nafoxidine, 1-ethyl nafoxidine.
Preferably, described organic bath and aprotic solvent form the solution of 0.5-2.0mol/L, and described additive accounts for the 0.05wt%-5wt% of organic electrolyte.
Wherein, described aprotic solvent is one or more the mixture in acetonitrile, propionitrile, methoxypropionitrile, gamma-butyrolacton, gamma-valerolactone, ethylene carbonate, propene carbonate, DMF, dimethylacetylamide, 1-Methyl-2-Pyrrolidone, dimethoxy-ethane, 2-methyl ethyl ether, oxolane, dioxolanes, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, sulfolane or dimethyl sulfoxide (DMSO).
Wherein, described organic bath is tetraethylammonium tetrafluoroborate, tetramethyl ammonium tetrafluoroborate, tetrapropyl ammonium tetrafluoroborate, tetrabutyl ammonium tetrafluoroborate, methyltriethylammonitetrafluoroborate tetrafluoroborate, diethyl-dimethyl ammonium tetrafluoroborate, trimethyl ethyl ammonium tetrafluoroborate, N, N-dimethyl pyrrolidine tetrafluoro boric acid amine, N-ethyl-N-crassitude tetrafluoro boric acid amine, N-propyl group-N-crassitude tetrafluoro boric acid amine, N-N-tetramethylene pyrrolidines tetrafluoro boric acid amine, volution-(1, 1 ')-bis-pyrrolidines tetrafluoro boric acid amine, N, N-lupetidine tetrafluoro boric acid amine, N, N-diethyl piperidines tetrafluoro boric acid amine, N, N-thebaine tetrafluoro boric acid amine, 1-ethyl-3-methylimidazole tetrafluoro boric acid amine etc., ammonium perchlorate class is as tetraethyl ammonium perchlorate, tetramethyl ammonium perchlorate, tetrapropyl ammonium perchlorate, tetrabutylammonium perchlorate, methyl triethyl group ammonium perchlorate, N-N-dimethyl pyrrolidine ammonium perchlorate, N-ethyl-N-crassitude perchlorate, N-propyl group-N-crassitude ammonium perchlorate, N-N-tetramethylene pyrrolidines perchlorate, 1-ethyl-3-methylimidazole perchlorate, ammonium hexafluorophosphate class is as one or more the mixture in tetraethyl ammonium hexafluorophosphate, tetramethyl ammonium hexafluorophosphate, tetrapropyl ammonium hexafluorophosphate, tetrabutyl ammonium hexafluorophosphate, methyl triethyl group ammonium hexafluorophosphate, triethyl group methyl ammonium hexafluorophosphate or diethyl-dimethyl ammonium hexafluorophosphate.
In order to realize foregoing invention object, another technical scheme that the present invention adopts is:
A ultracapacitor, comprising: positive pole, negative pole, the barrier film between between positive pole and negative pole and organic electrolyte;
Described organic electrolyte comprises aprotic solvent, organic bath and additive;
Described additive is one or more combinations in shown in pyridine, pyridine derivate, pyrroles, azole derivatives or structural formula (1),
R wherein
1, R
2, R
3for carbon number be 1-6 alkyl or silylation;
Described positive pole and negative pole are material with carbon element electrode, and described barrier film is fiber cloth diaphragm.
Preferably, described organic bath and aprotic solvent form the solution of 0.5-2.0mol/L, and described additive accounts for the 0.05wt%-5wt% of organic electrolyte.
Beneficial effect of the present invention is: select suitable aprotic solvent to form and additive, improve the dissolving of electrolyte in aprotic solvent and the ability of dissociating, improve the ionic conductance performance of electrolyte, to reduce the internal resistance of organic electrolyte, improve the electrochemical stability window of electrolyte, thereby ultracapacitor can be used under higher operating voltage (more than 2.7V), and there is high power density, energy density and good cycle life.
Embodiment
By describing technology contents of the present invention, structural feature in detail, being realized object and effect, below in conjunction with execution mode, be explained in detail.
The vertical ultracapacitor model of group in glove box: battery core comprises two collector electrodes, two work electrodes of being made by active carbon that aluminium foil is made and the fiber cloth diaphragm inserting betwixt.Battery core is immersed in the electrolyte in following examples, adopt the vertical sealing of aluminum hull and micelle group.Then in the scope of U/2 – U (U is more than 2.7V), under the condition of constant current (10 or 20mA/F), this model is carried out to cycle life test, at room temperature by charging and discharging curve, determine its capacity and ESR.
Embodiment 1
In glove box, the methyltriethylammonitetrafluoroborate tetrafluoroborate of certain mass is dissolved in aprotic solvent acetonitrile, the solution that formation concentration is 1.0mol/L, add again the triethylamine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 2
In glove box, the methyltriethylammonitetrafluoroborate tetrafluoroborate of certain mass is dissolved in aprotic solvent propene carbonate, the solution that formation concentration is 1.0mol/L, add again the pyridine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 3
In glove box, the tetraethylammonium tetrafluoroborate of certain mass is dissolved in aprotic solvent acetonitrile, the solution that formation concentration is 1.0mol/L, add again the triethylamine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 4
In glove box, the tetraethylammonium tetrafluoroborate of certain mass is dissolved in to aprotic solvent 80% acetonitrile, in 20% sulfolane, the solution that formation concentration is 1.5mol/L, add again the pyridine of counting 5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 5
In glove box, the diethyl-dimethyl ammonium tetrafluoroborate of certain mass is dissolved in aprotic solvent acetonitrile, the solution that formation concentration is 1.0mol/L, add again the triethylamine of counting 0.5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 6
In glove box, the diethyl-dimethyl ammonium tetrafluoroborate of certain mass is dissolved in aprotic solvent propene carbonate, the solution that formation concentration is 0.8mol/L, add again the pyridine of counting 0.5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 7
In glove box, the trimethyl ethyl ammonium tetrafluoroborate of certain mass is dissolved in aprotic solvent acetonitrile, the solution that formation concentration is 1.0mol/L, add again the triethylamine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 8
In glove box, the trimethyl ethyl ammonium tetrafluoroborate of certain mass is dissolved in to aprotic solvent 80% acetonitrile, in 20% sulfolane, the solution that formation concentration is 0.8mol/L, add again the pyridine of counting 0.5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 9
In glove box, by the N of certain mass, N-dimethyl pyrrolidine tetrafluoro boric acid amine solvent is in aprotic solvent acetonitrile, the solution that formation concentration is 2mol/L, add again the triethylamine of counting 5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 10
In glove box, by the N of certain mass, N-dimethyl pyrrolidine tetrafluoro boric acid amine solvent is in aprotic solvent propene carbonate, the solution that formation concentration is 1.5mol/L, add again the pyridine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 11
In glove box, by the volution of certain mass-(1,1 ')-bis-pyrrolidines tetrafluoro boric acid amine solvents are in aprotic solvent acetonitrile, the solution that formation concentration is 0.5mol/L, add again the triethylamine of counting 0.05% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Embodiment 12
In glove box, by the volution of certain mass-(1,1 ')-bis-pyrrolidines tetrafluoro boric acid amine solvents are in aprotic solvent propene carbonate, the solution that formation concentration is 2.0mol/L, add again the pyridine of counting 0.5% by gross mass, form uniform mixing material, thereby obtain can be used for the target organic electrolyte of ultracapacitor.
Comparative example 1
In glove box, the tetraethyl ammonium tetrafluoroborate of certain mass is dissolved in aprotic solvent acetonitrile, the solution that to form concentration be 1.0mol/L, thus obtain can be used for the target organic electrolyte of ultracapacitor.
Comparative example 2
In glove box, the tetraethyl ammonium tetrafluoroborate of certain mass is dissolved in to aprotic solvent 80% acetonitrile, in 20% sulfolane, the solution that to form concentration be 1.0mol/L, thus obtain can be used for the target organic electrolyte of ultracapacitor.
Comparative example 3
In glove box, the methyltriethylammonitetrafluoroborate tetrafluoroborate of certain mass is dissolved in aprotic solvent propene carbonate, the solution that to form concentration be 1.0mol/L, thus obtain can be used for the target organic electrolyte of ultracapacitor.
For the ultracapacitor that uses embodiment and comparative example organic electrolyte, 25 ℃, upper voltage limit 3.0V, constant current 1000mA charge, and by lower voltage limit U/2(U, are then more than 2.7V), constant current 1000mA discharges; By above-mentioned upper voltage limit U, constant current 1000mA charges again, and in 65 ℃ of high-temperature cabinets, constant voltage is placed one week.Afterwards, temperature retrieval to 25 ℃, by upper voltage limit U, lower voltage limit U/2, constant current 1000mA discharges and recharges.The capacity of test ultracapacitor, the results are shown in Table 1.
(table 1)
| ? | Voltage U (V) | The capacity of ultracapacitor (F) | The ESR of ultracapacitor (m Ω) |
| Embodiment 1 | 3.0 | 57.1 | 98.1 |
| Embodiment 3 | 3.0 | 74.1 | 76.3 |
| Embodiment 5 | 3.0 | 59.5 | 8.8 |
| Embodiment 7 | 3.0 | 67.2 | 80.3 |
| Embodiment 9 | 3.0 | 67.0 | 69.9 |
| Embodiment 11 | 3.0 | 80.3 | 78.8 |
| Comparative example 1 | 3.0 | 51.8 | 108.5 |
| Embodiment 4 | 2.8 | 55.3 | 98.1 |
| Embodiment 8 | 2.8 | 59.5 | 78.8 |
| Comparative example 2 | 2.8 | 48.9 | 120.3 |
| Embodiment 2 | 2.7 | 70.1 | 78.3 |
| Embodiment 6 | 2.7 | 74.1 | 76.3 |
| Embodiment 10 | 2.7 | 67.2 | 80.3 |
| Embodiment 12 | 2.7 | 68.0 | 84.6 |
| Comparative example 3 | 2.7 | 51 | 94 |
Have upper table known, the invention enables ultracapacitor under higher operating voltage (more than 2.7V), to use, obviously capacity is large, can obtain thus ultracapacitor of the present invention and have high power density, energy density and good cycle life.
The foregoing is only embodiments of the invention; not thereby limit the scope of the claims of the present invention; every equivalent structure or conversion of equivalent flow process that utilizes specification of the present invention to do, or be directly or indirectly used in other relevant technical fields, be all in like manner included in scope of patent protection of the present invention.
Claims (7)
1. the organic electrolyte for ultracapacitor, it is characterized in that: comprise aprotic solvent, organic bath and additive, described additive is one or more combinations in shown in pyridine, pyridine derivate, pyrroles, azole derivatives or structural formula (1)
R wherein
1, R
2, R
3for carbon number be 1-6 alkyl or silylation.
2. the organic electrolyte for ultracapacitor according to claim 1, is characterized in that: described structural formula (1) is triethylamine, tripropyl amine (TPA), tri-n-butylamine, triamylamine, three (trimethyl silicane) amine, 1-methyl nafoxidine, 1-ethyl nafoxidine.
3. the organic electrolyte for ultracapacitor according to claim 1 and 2, is characterized in that: described organic bath and aprotic solvent form the solution of 0.5-2.0mol/L, and described additive accounts for the 0.05wt%-5wt% of organic electrolyte.
4. the organic electrolyte for ultracapacitor according to claim 1 and 2, it is characterized in that: described aprotic solvent is one or more the mixture in acetonitrile, propionitrile, methoxypropionitrile, gamma-butyrolacton, gamma-valerolactone, ethylene carbonate, propene carbonate, DMF, dimethylacetylamide, 1-Methyl-2-Pyrrolidone, dimethoxy-ethane, 2-methyl ethyl ether, oxolane, dioxolanes, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, sulfolane or dimethyl sulfoxide (DMSO).
5. the organic electrolyte for ultracapacitor according to claim 1 and 2, it is characterized in that: described organic bath is tetraethylammonium tetrafluoroborate, tetramethyl ammonium tetrafluoroborate, tetrapropyl ammonium tetrafluoroborate, tetrabutyl ammonium tetrafluoroborate, methyltriethylammonitetrafluoroborate tetrafluoroborate, diethyl-dimethyl ammonium tetrafluoroborate, trimethyl ethyl ammonium tetrafluoroborate, N, N-dimethyl pyrrolidine tetrafluoro boric acid amine, N-ethyl-N-crassitude tetrafluoro boric acid amine, N-propyl group-N-crassitude tetrafluoro boric acid amine, N-N-tetramethylene pyrrolidines tetrafluoro boric acid amine, volution-(1, 1 ')-bis-pyrrolidines tetrafluoro boric acid amine, N, N-lupetidine tetrafluoro boric acid amine, N, N-diethyl piperidines tetrafluoro boric acid amine, N, N-thebaine tetrafluoro boric acid amine, 1-ethyl-3-methylimidazole tetrafluoro boric acid amine etc., ammonium perchlorate class is as tetraethyl ammonium perchlorate, tetramethyl ammonium perchlorate, tetrapropyl ammonium perchlorate, tetrabutylammonium perchlorate, methyl triethyl group ammonium perchlorate, N-N-dimethyl pyrrolidine ammonium perchlorate, N-ethyl-N-crassitude perchlorate, N-propyl group-N-crassitude ammonium perchlorate, N-N-tetramethylene pyrrolidines perchlorate, 1-ethyl-3-methylimidazole perchlorate, ammonium hexafluorophosphate class is as one or more the mixture in tetraethyl ammonium hexafluorophosphate, tetramethyl ammonium hexafluorophosphate, tetrapropyl ammonium hexafluorophosphate, tetrabutyl ammonium hexafluorophosphate, methyl triethyl group ammonium hexafluorophosphate, triethyl group methyl ammonium hexafluorophosphate or diethyl-dimethyl ammonium hexafluorophosphate.
6. a ultracapacitor, is characterized in that, comprising: positive pole, negative pole, the barrier film between between positive pole and negative pole and organic electrolyte;
Described organic electrolyte comprises aprotic solvent, organic bath and additive;
Described additive is one or more combinations in shown in pyridine, pyridine derivate, pyrroles, azole derivatives or structural formula (1),
R wherein
1, R
2, R
3for carbon number be 1-6 alkyl or silylation;
Described positive pole and negative pole are material with carbon element electrode, and described barrier film is fiber cloth diaphragm.
7. ultracapacitor according to claim 6, is characterized in that, described organic bath and aprotic solvent form the solution of 0.5-2.0mol/L, and described additive accounts for the 0.05wt%-5wt% of organic electrolyte.
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| CN103956268A (en) * | 2014-05-15 | 2014-07-30 | 深圳新宙邦科技股份有限公司 | Electrolyte solute, electrolyte and high-voltage supercapacitor |
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| WO2018058837A1 (en) * | 2016-09-29 | 2018-04-05 | 深圳新宙邦科技股份有限公司 | Organic electrolyte solution for super capacitor, and super capacitor |
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| CN107845506A (en) * | 2017-10-26 | 2018-03-27 | 中国科学院福建物质结构研究所 | A kind of reinforced stone mertenyl ultracapacitor and preparation method thereof |
| CN110310842A (en) * | 2018-03-20 | 2019-10-08 | 中天储能科技有限公司 | Electrolyte of high voltage capacitor and preparation method thereof and capacitor element |
| CN110310842B (en) * | 2018-03-20 | 2022-03-18 | 中天超容科技有限公司 | Electrolyte of high-voltage capacitor, preparation method thereof and capacitor device |
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