CN114865092A - Nonaqueous lithium ion battery electrolyte and lithium ion battery - Google Patents
Nonaqueous lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN114865092A CN114865092A CN202210560342.3A CN202210560342A CN114865092A CN 114865092 A CN114865092 A CN 114865092A CN 202210560342 A CN202210560342 A CN 202210560342A CN 114865092 A CN114865092 A CN 114865092A
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- ion battery
- lithium ion
- electrolyte
- carbonate
- lidfob
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 61
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 35
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 35
- 229910013870 LiPF 6 Inorganic materials 0.000 claims abstract description 15
- 239000003960 organic solvent Substances 0.000 claims abstract description 15
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 14
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 14
- 238000000034 method Methods 0.000 claims abstract description 6
- 239000000203 mixture Substances 0.000 claims abstract description 5
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims abstract description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims abstract description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims abstract description 4
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims abstract description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims abstract description 4
- 229910012851 LiCoO 2 Inorganic materials 0.000 claims description 5
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 4
- 229910052744 lithium Inorganic materials 0.000 claims description 4
- 239000007774 positive electrode material Substances 0.000 claims description 4
- 229910013716 LiNi Inorganic materials 0.000 claims description 3
- 229910013290 LiNiO 2 Inorganic materials 0.000 claims description 3
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 claims description 3
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 239000007773 negative electrode material Substances 0.000 claims description 3
- 238000002360 preparation method Methods 0.000 abstract description 3
- 230000001351 cycling effect Effects 0.000 abstract description 2
- 239000012046 mixed solvent Substances 0.000 abstract description 2
- 230000000052 comparative effect Effects 0.000 description 12
- 239000002904 solvent Substances 0.000 description 10
- 238000012360 testing method Methods 0.000 description 7
- 229910013872 LiPF Inorganic materials 0.000 description 5
- 101150058243 Lipf gene Proteins 0.000 description 5
- 239000002033 PVDF binder Substances 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 5
- 238000002156 mixing Methods 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 239000011888 foil Substances 0.000 description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 238000006864 oxidative decomposition reaction Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 238000007792 addition Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000000269 nucleophilic effect Effects 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 238000012552 review Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0568—Liquid materials characterised by the solutes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/0042—Four or more solvents
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses a non-aqueous lithium ion battery electrolyte and a lithium ion battery, and the non-aqueous lithium ion battery electrolyte comprises lithium salt and an organic solvent, wherein the lithium salt is LiPF 6 And LiDFOB, and the organic solvent is a mixture of ethylene carbonate EC, fluoroethylene carbonate FEC, propylene carbonate PC, ethyl methyl carbonate EMC, diethyl carbonate DEC. A lithium ion battery comprises a positive electrode, a negative electrode, a diaphragm and a nonaqueous lithium ion battery electrolyte. The electrolyte disclosed by the invention has the advantages that the electrochemical window of the electrolyte is improved by using various mixed solvents, and meanwhile, the use of LiDFOB can improve the interface of a positive electrode and the electrolyte and improve the cycling stability of a battery under high voltage. The electrolyte disclosed by the invention is simple in preparation method, mature in process, easy to operate and suitable for industrial application.
Description
Technical Field
The invention relates to a battery electrolyte and a lithium ion battery, in particular to a non-aqueous lithium ion battery electrolyte and a lithium ion battery, belonging to the field of lithium ion batteries.
Background
Lithium ion batteries are widely used in consumer electronics, power vehicles and energy storage applications due to their long cycle life, high operating voltage, low self-discharge rate, no memory effect and environmental friendliness. In the field of consumer electronics, with the development of information and network technologies and the pursuit of long endurance, there is an urgent need for higher energy density batteries. The energy density of the battery can be effectively improved by increasing the charging voltage of the cathode material, but the oxidation of the cathode material is also improved by the higher charging voltage, so that the oxidative decomposition of the electrolyte is aggravated. Common lithium ion battery electrolyte 1M LiPF 6 EC-DMC, which undergoes severe oxidation at voltages above 4.5V, especially with an excessively high EC content leading to nucleophilic/electronegative reactions and CO 2 Is released. By improving the electrochemical window of the electrolyte, a good anode-electrolyte interface layer is constructed, so that the catalytic activity of the high-voltage anode can be effectively reduced, the decomposition of the electrolyte is inhibited, and the high-voltage performance of the battery is improved.
Disclosure of Invention
In order to solve the defects of the prior art, the invention provides a nonaqueous lithium ion battery electrolyte and a lithium ion battery, wherein the oxidation resistance of the electrolyte is improved by adopting a mode of mixing and using various solvents, and a stable anode-electrolyte interface is constructed by using LiDFOB lithium salt, so that the high-voltage cycle performance of the battery is improved.
In order to solve the technical problems, the technical scheme adopted by the invention is as follows: a non-aqueous lithium ion battery electrolyte comprises lithium salt and organic solvent, wherein the lithium salt is LiPF 6 And LiDFOB, and the organic solvent is a mixture of ethylene carbonate EC, fluoroethylene carbonate FEC, propylene carbonate PC, ethyl methyl carbonate EMC, diethyl carbonate DEC.
Preferably, LiPF 6 The concentration of (B) is 0.5 to 0.9mol/L, and the concentration of LiDFOB is 0.1 to 0.5 mol/L.
Preferably, LiPF 6 The concentration of (b) is 0.5 to 0.8mol/L, and the concentration of LiDFOB is 0.2 to 0.5 mol/L.
Preferably, the content of the organic solvent is EC: 5-15%, FEC: 3-5%, PC: 20-30%, EMC: 35-45%, DEC: 15 to 25 percent.
Preferably, the content of the organic solvent is EC: 10-15%, FEC: 3-4%, PC: 20-25%, EMC: 40-45%, DEC: 15 to 20 percent.
A lithium ion battery comprises a positive electrode, a negative electrode, a diaphragm and a nonaqueous lithium ion battery electrolyte.
Preferably, the positive electrode material is selected from the group consisting of lithium transition metal oxide LiCoO 2 、LiNiO 2 、LiNi x Co y Mn 1-x-y O 2 In the method, the negative electrode material is metal lithium.
Compared with the prior art, the invention has the following beneficial effects:
(1) the electrolyte disclosed by the invention has the advantages that the electrochemical window of the electrolyte is improved by using various mixed solvents, and meanwhile, the use of LiDFOB can improve the interface of a positive electrode and the electrolyte and improve the cycling stability of a battery under high voltage.
(2) The electrolyte disclosed by the invention is simple in preparation method, mature in process, easy to operate and suitable for industrial application.
Drawings
FIG. 1 is a graph of cycle performance for example 1 and comparative examples 1-4.
FIG. 2 is a graph of linear voltammetric sweep tests of the inventive and comparative electrolytes.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and specific embodiments.
A non-aqueous lithium ion battery electrolyte comprises lithium salt and organic solvent, wherein the lithium salt is LiPF 6 And LiDFOB, and the organic solvent is a mixture of ethylene carbonate EC, fluoroethylene carbonate FEC, propylene carbonate PC, ethyl methyl carbonate EMC, diethyl carbonate DEC.
Wherein, LiPF 6 The concentration of (B) is 0.5 to 0.9mol/L, and the concentration of LiDFOB is 0.1 to 0.5 mol/L.
Preferably, LiPF 6 The concentration of (B) is 0.5 to 0.8mol/L, and the concentration of LiDFOB is 0.2 to 0.5 mol/L.
Wherein the content of the organic solvent is respectively EC: 5-15%, FEC: 3-5%, PC: 20-30%, EMC: 35-45%, DEC: 15 to 25 percent. (note: the contents of the organic solvents are volume fractions).
Preferably, the content of the organic solvent is EC: 10-15%, FEC: 3-4%, PC: 20-25%, EMC: 40-45%, DEC: 15 to 20 percent.
A lithium ion battery comprises a positive electrode, a negative electrode, a diaphragm and a nonaqueous lithium ion battery electrolyte.
Wherein the positive electrode material is selected from lithium transition metal oxide LiCoO 2 、LiNiO 2 、LiNi x Co y Mn 1-x-y O 2 In the method, the negative electrode material is metal lithium.
The present invention will be described in further detail with reference to examples.
Example 1
The nonaqueous lithium ion battery electrolyte is prepared by the following method: in a glove box, FEC, EC, PC, EMC and DEC were mixed in a volume ratio of 3.8:11.3:25:41.2:18.7, and then 0.6M LiPF was added 6 And 0.4M LiDFOB. The electrolyte is noted as 0.6M-0.4M.
LiCoO 2 The preparation method of the positive plate comprises the following steps: mixing an active material with acetylene black and polyvinylidene fluoride (PVDF) according to a mass ratio of 8:1:1, uniformly mixing a solvent N-methylpyrrolidone (NMP), coating the mixture on an aluminum foil after uniformly mixing slurry, drying the aluminum foil in a drying box at 70 ℃, cutting the aluminum foil into a pole piece with the thickness of 10mm after finishing the drying, wherein the positive active material is 2.8mg/cm 2 。
The prepared electrolyte is used for LiCoO 2 The cycle performance test was carried out in a/Li cell (type CR 2032). The test temperature was 25 ℃, the voltage range was 3-4.6V, the first three weeks were activated with 0.1C (1C ═ 274mA/g), followed by long cycles with 0.5C.
Example 2
The positive and negative electrodes used in this example 2 were the same as those used in example 1, except that LiPF was used 6 The concentration was 0.9M and the concentration of LiDFOB was 0.1M. The electrolyte is noted as 0.9M-0.1M.
Example 3
The positive and negative electrodes used in this example 3 were the same as those used in example 1, except that LiPF was used 6 The concentration was 0.5M and the concentration of LiDFOB was 0.5M. The electrolyte is noted as 0.5M-0.5M。
Comparative example 1
The positive and negative electrodes used in comparative example 1 were the same as in example 1, except that the electrolyte solvents used were EC and DMC at a volume ratio of 1:1, and the lithium salt was 1M LiPF 6 . This electrolyte was designated as EC-DMC.
Comparative example 2
The positive and negative electrodes used in comparative example 2 were the same as in example 1, except that the electrolyte solvents used were PC, EC and DMC at a volume ratio of 45:10:45, and the lithium salt was 1M LiPF 6 . The electrolyte was designated as PC-EC-DMC.
Comparative example 3
The positive and negative electrodes used in this comparative example 3 are the same as in example 1, except that the solvents used were PC, EC, DMC and 1,1,2, 2-tetrafluoroethyl-2 ', 2', 3 ', 3' -tetrafluoropropyl ether (TTE) in the volume ratios: 40.5:9:40.5:10, lithium salt is 1M LiPF 6 . The electrolyte is designated as Bl + 10% TTE.
Comparative example 4
The positive and negative electrodes used in this comparative example 4 were the same as in example 1, except that FEC, EC, PC, EMC, and DEC were used as solvents, and the respective volume ratios were FEC: EC: PC: EMC: DEC of 3.8:11.3:25:41.2:18.7, and 1M LiPF as the lithium salt 6 . This electrolyte was designated PC-25.
Application experiments of examples and comparative examples:
and (3) cycle experiment: the specific discharge capacity at 1 week, 50 week and 100 week was recorded by performing a charge-discharge cycle test at room temperature (25 ℃) at a rate of 0.5C (the first three weeks were the 0.1C rate activated batteries), and the specific discharge capacity at 100 weeks was divided by the specific discharge capacity at 4 weeks to obtain the capacity retention rate of the battery, and the results are shown in table 1. The cycle results of the test are shown in fig. 1.
Table 1 shows the test results of examples and comparative examples
The data clearly show that the nonaqueous lithium ion battery electrolyte effectively improves the high-voltage cycle performance of the battery, and the cycle stability of the nonaqueous lithium ion battery electrolyte is far better than that of a commercial double-solvent electrolyte (1M LiPF) 6 EC-DMC) and the commonly used three-solvent electrolytes (PC-EC-DMC), four-solvent electrolytes (Bl + 10% TTE). Moreover, the performance of the double-salt electrolyte is better than that of the electrolyte adopting only 1M LiPF 6 The electrolyte (PC-25) of lithium salt is prepared, which shows that the double-salt electrolyte of the invention is beneficial to the cycle stability of the battery under high voltage.
Experimental test analysis:
the electrolyte prepared in this example was subjected to a linear voltammetric scan test in the range of open circuit voltage to 6V (vs + Li), the sweep rate is 1mV/s, the battery adopts a lithium sheet as a counter electrode, and SuperP-PVDF is used as a working electrode. The mass ratio of the SuperP to the PVDF in the SuperP-PVDF electrode is 75:25, and the current is calculated according to the actual active mass of the SuperP. Results referring to fig. 2, commercial EC-DMC electrolyte started to oxidize at 4.7V, PC-25 started to oxidize at 5.2V, 0.6M-0.4M started to oxidize at 5.0V, and had an oxidation peak at 5.17V, which was known to correspond to oxidative decomposition of LiDFOB from a review of the literature. The above data illustrate that the multi-solvent electrolyte of the present invention helps to improve the electrochemical window of the electrolyte, and that the oxidation of the liddob helps to build a stable anode-electrolyte interface, avoiding the continuous decomposition of the electrolyte. Therefore, the battery using the electrolyte of the present invention has very good cycle stability.
The above embodiments are not intended to limit the present invention, and the present invention is not limited to the above examples, and those skilled in the art may make variations, modifications, additions or substitutions within the technical scope of the present invention.
Claims (7)
1. A non-aqueous lithium ion battery electrolyte comprising a lithium salt and an organic solvent, characterized in that: the lithium salt is LiPF 6 And LiDFOB, the organic solvent is a mixture of ethylene carbonate EC, fluoroethylene carbonate FEC, propylene carbonate PC, ethyl methyl carbonate EMC, diethyl carbonate DEC.
2. The nonaqueous lithium ion battery electrolyte of claim 1, wherein: the LiPF 6 The concentration of (B) is 0.5 to 0.9mol/L, and the concentration of LiDFOB is 0.1 to 0.5 mol/L.
3. The nonaqueous lithium ion battery electrolyte of claim 2, wherein: the LiPF 6 The concentration of (B) is 0.5 to 0.8mol/L, and the concentration of LiDFOB is 0.2 to 0.5 mol/L.
4. The non-aqueous lithium ion battery electrolyte of claim 1, wherein: the content of the organic solvent is respectively EC: 5-15%, FEC: 3-5%, PC: 20-30%, EMC: 35-45%, DEC: 15 to 25 percent.
5. The non-aqueous lithium ion battery electrolyte of claim 4, wherein: the content of the organic solvent is respectively EC: 10-15%, FEC: 3-4%, PC: 20-25%, EMC: 40-45%, DEC: 15 to 20 percent.
6. A lithium ion battery, characterized by: the lithium ion battery comprises a positive electrode, a negative electrode, a separator and the nonaqueous lithium ion battery electrolyte according to any one of claims 1 to 5.
7. The lithium ion battery of claim 6, wherein: the positive electrode material is selected from lithium transition metal oxide LiCoO 2 、LiNiO 2 、LiNi x Co y Mn 1-x-y O 2 In the method, the negative electrode material is metal lithium.
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| CN202210560342.3A CN114865092A (en) | 2022-05-23 | 2022-05-23 | Nonaqueous lithium ion battery electrolyte and lithium ion battery |
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| CN202210560342.3A CN114865092A (en) | 2022-05-23 | 2022-05-23 | Nonaqueous lithium ion battery electrolyte and lithium ion battery |
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Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1363124A (en) * | 2000-02-24 | 2002-08-07 | 日本电池株式会社 | Nonaqueous electrolyte secondary cell |
| CN105470563A (en) * | 2015-01-28 | 2016-04-06 | 万向A一二三系统有限公司 | Lithium ion battery electrolyte suitably used for silicon-carbon negative electrode |
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- 2022-05-23 CN CN202210560342.3A patent/CN114865092A/en active Pending
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1363124A (en) * | 2000-02-24 | 2002-08-07 | 日本电池株式会社 | Nonaqueous electrolyte secondary cell |
| CN105470563A (en) * | 2015-01-28 | 2016-04-06 | 万向A一二三系统有限公司 | Lithium ion battery electrolyte suitably used for silicon-carbon negative electrode |
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