CN113140411A - Electrolyte of high-voltage lithium ion capacitor - Google Patents
Electrolyte of high-voltage lithium ion capacitor Download PDFInfo
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- CN113140411A CN113140411A CN202110622375.1A CN202110622375A CN113140411A CN 113140411 A CN113140411 A CN 113140411A CN 202110622375 A CN202110622375 A CN 202110622375A CN 113140411 A CN113140411 A CN 113140411A
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- Prior art keywords
- electrolyte
- lithium ion
- ion capacitor
- carbonate
- lithium
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 51
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 51
- 239000003990 capacitor Substances 0.000 title claims abstract description 50
- 239000003792 electrolyte Substances 0.000 title claims abstract description 43
- 239000002904 solvent Substances 0.000 claims abstract description 23
- ZTOMUSMDRMJOTH-UHFFFAOYSA-N glutaronitrile Chemical group N#CCCCC#N ZTOMUSMDRMJOTH-UHFFFAOYSA-N 0.000 claims abstract description 21
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 18
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 18
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims abstract description 14
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000000654 additive Substances 0.000 claims abstract description 13
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims abstract description 8
- 230000000996 additive effect Effects 0.000 claims abstract description 8
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910001290 LiPF6 Inorganic materials 0.000 claims abstract description 3
- 238000004146 energy storage Methods 0.000 abstract description 3
- 239000002931 mesocarbon microbead Substances 0.000 description 9
- 238000002156 mixing Methods 0.000 description 9
- 229910013872 LiPF Inorganic materials 0.000 description 8
- 101150058243 Lipf gene Proteins 0.000 description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 8
- 239000000203 mixture Substances 0.000 description 8
- 239000003960 organic solvent Substances 0.000 description 8
- 229910052760 oxygen Inorganic materials 0.000 description 8
- 239000001301 oxygen Substances 0.000 description 8
- 238000003756 stirring Methods 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 230000001351 cycling effect Effects 0.000 description 4
- 238000006138 lithiation reaction Methods 0.000 description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 229910052744 lithium Inorganic materials 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000002033 PVDF binder Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- 235000012431 wafers Nutrition 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000012983 electrochemical energy storage Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000013112 stability test Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/58—Liquid electrolytes
- H01G11/64—Liquid electrolytes characterised by additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/04—Hybrid capacitors
- H01G11/06—Hybrid capacitors with one of the electrodes allowing ions to be reversibly doped thereinto, e.g. lithium ion capacitors [LIC]
-
- 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
- Y02E60/13—Energy storage using capacitors
Landscapes
- Engineering & Computer Science (AREA)
- Power Engineering (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Materials Engineering (AREA)
- Electric Double-Layer Capacitors Or The Like (AREA)
Abstract
The invention belongs to the technical field of energy storage devices, and particularly discloses an electrolyte of a high-voltage lithium ion capacitor. The electrolyte consists of the following components: additives, lithium salts, carbonate solvents; the additive is glutaronitrile and/or fluoroethylene carbonate, and the lithium salt is LiPF6The carbonate solvent consists of ethylene carbonate and methyl ethyl carbonate. The invention creatively discovers that the electrochemical performance of the lithium ion capacitor can be comprehensively improved after a small amount of glutaronitrile and/or fluoroethylene carbonate is added into an organic solution of lithium salt. The electrolyte disclosed by the invention is simple in components and low in cost.
Description
Technical Field
The invention belongs to the technical field of energy storage devices, and particularly relates to an electrolyte of a high-voltage lithium ion capacitor.
Background
In the past decades, the large consumption of fossil energy such as coal and petroleum causes serious environmental pollution and resource shortage, so people urgently need to develop renewable clean energy with abundant reserves and environmental friendliness. At present, clean energy sources such as solar energy, wind energy and tidal energy are widely used, but the energy sources have the defects of uneven spatial distribution, instability and the like, so that the development of electrochemical energy storage devices such as super capacitors, lithium ion batteries and the like with excellent performance is necessary. The lithium ion battery has the advantages of high energy density, long cycle life and the like, and is widely applied to the fields of electronic products and electric automobiles; the super capacitor has excellent large-current charging and discharging capacity and is mainly applied to the fields of mobile standby power supplies, starting power supplies and the like. Despite the many advantages of lithium ion batteries and supercapacitors, there is also a low power density of (<1000 w kg-1) And has low energy density (<10 wh kg-1) And the like, and can not meet the requirements of specific fields. To achieve this, it is proposed that a hybrid energy storage device, a lithium ion capacitor, can be assembled by combining the negative electrode of a lithium ion battery and the positive electrode of a supercapacitor.
When the lithium ion capacitor works, reversible ion adsorption and desorption reaction occurs on the positive electrode interface, and reversible electrochemical reaction occurs on the negative electrode interface, so that the lithium ion capacitor has the double characteristics of a lithium ion battery and a super capacitor. Compared with a lithium ion battery, the anode adopts a carbon material with a high specific surface area, so that the rate capability of the lithium ion capacitor can be improved, and the energy density is reduced. Compared with a super capacitor, the negative electrode is made of materials such as graphite and mesocarbon microbeads, so that the energy density of the lithium ion capacitor is improved, and rapid charging and discharging are not facilitated. Therefore, the electrochemical performance of the lithium ion capacitor is intermediate between that of the supercapacitor and the lithium ion battery.
The lithium ion capacitor adopts carbonate electrolyte similar to the lithium ion battery, the electrolyte is easy to oxidize and decompose under high voltage, the energy density of the lithium ion capacitor is linearly related to the square of working voltage, and the working voltage mainly depends on the electrochemical window of the electrolyte, so that the development of the electrolyte suitable for the high-voltage lithium ion capacitor has important significance.
Disclosure of Invention
Aiming at the problems in the prior art, the invention mainly aims to provide the electrolyte of the high-voltage lithium ion capacitor, which improves the specific capacity of the lithium ion capacitor and improves the cycle performance and the rate characteristic of a device under high voltage under the condition of basically not increasing economic cost.
In order to achieve the purpose, the invention adopts the following technical scheme:
the electrolyte of the high-voltage lithium ion capacitor comprises the following components: additive, lithium salt and carbonate solvent.
The additive is Glutaronitrile (GLN) and/or fluoroethylene carbonate (FEC), and the mass fraction of the additive in the electrolyte is 1% -5%.
The lithium salt is LiPF6The molar concentration in the electrolyte is 1-1.5 mol/L.
The carbonate solvent is preferably composed of Ethylene Carbonate (EC) and Ethyl Methyl Carbonate (EMC), wherein the mass ratio of the ethylene carbonate to the ethyl methyl carbonate is 3/7-1.
The invention creatively discovers that GLN as a typical dinitrile compound has good oxidation stability, can widen the electrochemical window of electrolyte when used as an additive, and is beneficial to active carbon and other materials to exert larger specific capacity. The molecules have fluorine atoms with strong electronegativity, so that the oxidation voltage of FEC is high, and meanwhile, FEC is a common negative electrode film forming additive and is commonly used for reducing the first capacity loss of a negative electrode material and improving the cycle performance.
The invention further creatively discovers that a small amount of fluoroethylene carbonate and glutaronitrile are added into the organic solution of lithium salt as additives, so that the specific capacitance of the anode material can be greatly increased, the cycling stability of the MCMB (mesocarbon microbeads) cathode can be improved and the electrochemical performance of the lithium ion capacitor can be comprehensively improved under the condition that the economic cost is hardly increased.
The more important discovery of the invention is that the comprehensive electrochemical performance of the lithium ion capacitor is further improved by simultaneously adding a small amount of GLN and FEC in the electrolyte compared with the independent addition of GLN or FEC.
Compared with the prior art, the electrolyte of the lithium ion capacitor provided by the invention has the advantages of simple components and low cost, and can effectively improve the specific capacity, the cycle performance and the rate capability of the lithium ion capacitor.
Detailed Description
The invention is described in detail below, and the description in this section is merely exemplary and explanatory and should not be construed as limiting the scope of the invention in any way. Furthermore, those skilled in the art can combine features from the embodiments of this document and from different embodiments accordingly based on the description of this document.
Example 1:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and adding 1% of FEC (forward error correction) into the solvent and the lithium salt according to the mass sum of 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 2:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and (3) adding 1% of GLN into the solvent and the lithium salt according to the mass sum of 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 3:
in this embodiment, a lithium ion capacitor electrolyte is provided, whichThe preparation steps are as follows: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and adding 5% of FEC (forward error correction) into the solvent and the lithium salt according to the mass sum of 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 4:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and adding 5% GLN into the solvent and the lithium salt according to the mass sum of 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 5:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6The concentration is 1 mol/l, and the mixture is vibrated evenly by a magnetic stirrer; and adding 1% of FEC and 5% of GLN into the solvent and the lithium salt according to the mass sum of the solvent and the lithium salt being 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 6:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and adding 1% of FEC and 1% of GLN into the solvent and the lithium salt according to the mass sum of 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Example 7:
in this embodiment, an electrolyte for a lithium ion capacitor is provided, which is prepared by the following steps: low in both moisture and oxygen contentMixing 30% of EC and 70% of EMC in a glove box with the mass percent of 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6Adjusting the concentration to 1 mol/l, and shaking uniformly by a magnetic stirrer; and adding 5% of FEC and 1% of GLN into the solvent and the lithium salt according to the mass sum of the solvent and the lithium salt being 100%, and uniformly stirring to obtain the lithium ion capacitor electrolyte.
Comparative example 1:
in this case, a lithium ion capacitor base electrolyte is provided, which is prepared by the following steps: mixing 30% of EC and 70% of EMC by mass percent in a glove box with the moisture and oxygen content lower than 0.1 ppm to obtain an organic solvent; adding LiPF to the solvent6The concentration is 1 mol/l, and the mixture is shaken evenly by a magnetic stirrer.
Manufacturing a positive plate:
the positive electrode is prepared from the following active carbon: uniformly mixing PVDF and Super P in a mass ratio of 8:1:1, coating the mixture on an aluminum foil, drying the mixture for 6 hours in a vacuum oven, and cutting the mixture into small wafers with the diameter of 12 mm.
And (3) manufacturing a negative plate:
the cathode is prepared by the following steps of: uniformly mixing PVDF and Super P in a mass ratio of 8:1:1, coating the mixture on a copper foil, drying the mixture in a vacuum oven for 6 hours, and cutting the mixture into small wafers with the diameter of 12 mm.
Pre-lithiation of the negative electrode:
assembling the MCMB/Li half cell by the prepared electrolyte in a glove box, and pre-lithiating the cell after standing for 8 hours. And (3) carrying out pre-lithiation within the voltage range of 2-0.01V and at the multiplying power of 0.1C, discharging and then charging during testing, and stopping testing when the third discharge capacity is 200 mAh/g.
Manufacturing a lithium ion capacitor:
and disassembling the battery after the pre-lithiation in a glove box, and assembling the AC/MCMB full battery by using an active carbon positive plate and an MCMB negative plate after the pre-lithiation.
The AC/MCMB lithium ion capacitor is subjected to constant-current charge-discharge tests under the conditions of 2-4V, 1A/g, 2-4.3V and 1A/g, and the test results are shown in tables 1 and 2:
TABLE 1 test results of cycle performance of AC/MCMB in 2-4V voltage interval
TABLE 2 test results of the cycle performance of AC/MCMB in the voltage range of 2-4.3V
Comparing the capacity test results of the comparative example 1 and the examples 1 to 7, it can be seen that the specific capacity of the lithium capacitor can be obviously improved when 1% of FEC or GLN with the content not exceeding 5% is added into the electrolyte, the specific capacity of the lithium capacitor is further improved by the synergistic effect between GLN and FEC when the GLN and FEC are simultaneously used as additives, and the voltage range of 2-4.4V reaches 65 mAh/g. Comparing the cycling stability test results of comparative example 1 and examples 1-7, it can be seen that the cycling performance of the lithium capacitor can be improved by adding a small amount of FEC or GLN into the electrolyte, 1% is the preferred addition amount, and 1% of FEC and 1% of GLN are added into the electrolyte at the same time, so that the cycling stability of the device can be further improved by the synergistic effect between the two, and the best electrochemical performance can be realized.
The above description is only an embodiment of the present invention and should not be taken as limiting the invention, and all changes, substitutions and alterations that come within the spirit and scope of the invention are therefore intended to be embraced therein.
Claims (5)
1. The electrolyte of the high-voltage lithium ion capacitor is characterized by comprising the following components: additives, lithium salts, carbonate solvents; the additive is glutaronitrile and/or fluoroethylene carbonate, and the lithium salt is LiPF6The carbonate solvent consists of ethylene carbonate and methyl ethyl carbonate.
2. The electrolyte for the high-voltage lithium ion capacitor according to claim 1, wherein the mass fraction of the additive in the electrolyte is 1% to 10%.
3. The electrolyte of the high-voltage lithium ion capacitor according to claim 2, wherein when the additives are glutaronitrile and fluoroethylene carbonate, the mass fraction ratio of glutaronitrile to fluoroethylene carbonate is 1/5-5.
4. The electrolyte for a high voltage lithium ion capacitor according to claim 1, wherein the molar concentration of the lithium salt in the electrolyte is 1 to 1.5 mol/L.
5. The electrolyte of the high-voltage lithium ion capacitor according to claim 1, wherein the mass ratio of the ethylene carbonate to the ethyl methyl carbonate in the carbonate solution is 3/7-1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202110622375.1A CN113140411A (en) | 2021-06-04 | 2021-06-04 | Electrolyte of high-voltage lithium ion capacitor |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202110622375.1A CN113140411A (en) | 2021-06-04 | 2021-06-04 | Electrolyte of high-voltage lithium ion capacitor |
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| Publication Number | Publication Date |
|---|---|
| CN113140411A true CN113140411A (en) | 2021-07-20 |
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Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
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| CN202110622375.1A Pending CN113140411A (en) | 2021-06-04 | 2021-06-04 | Electrolyte of high-voltage lithium ion capacitor |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113707939A (en) * | 2021-08-27 | 2021-11-26 | 河南省法恩莱特新能源科技有限公司 | Low-impedance high-rate electrolyte |
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