CN106450365A - Anticorrosive electrolyte of lithium battery and obtained lithium primary battery - Google Patents
Anticorrosive electrolyte of lithium battery and obtained lithium primary battery Download PDFInfo
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- CN106450365A CN106450365A CN201610583631.XA CN201610583631A CN106450365A CN 106450365 A CN106450365 A CN 106450365A CN 201610583631 A CN201610583631 A CN 201610583631A CN 106450365 A CN106450365 A CN 106450365A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
- H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
- H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
- H01M6/166—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by the solute
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/50—Methods or arrangements for servicing or maintenance, e.g. for maintaining operating temperature
- H01M6/5072—Preserving or storing cells
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/50—Methods or arrangements for servicing or maintenance, e.g. for maintaining operating temperature
- H01M2006/5094—Aspects relating to capacity ratio of electrolyte/electrodes or anode/cathode
Abstract
The invention belongs to the technical field of chemical batteries, and particularly relates to an anticorrosive electrolyte of a lithium battery and an obtained lithium primary battery. The anticorrosive electrolyte of the lithium battery comprises an organic solvent and an electrolyte, wherein the electrolyte is a mixed lithium salt; and the mixed lithium salt comprises lithium bis(trifluoromethanesulfonyl ) imide LiTFSI, lithium bis(oxalatoe ) borate LiBOB and lithium perchlorate. The lithium salt with a good anticorrosive effect and good heat stability is added to the electrolyte, so that the problems that aluminum foil is corroded and the battery is short in service life and poor in safety due to use of a high-conductivity fluorine-containing lithium salt are solved on the basis of not reducing the capacity of the battery and the protection effect on the aluminum foil. In addition, the electrolyte provided by the invention is suitable for the electrolytes, such as lithium/manganese dioxide (Li/MnO2), lithium/iron disulfide (Li/FeS2), lithium/copper oxide (Li/CuO), lithium/fluorinated carbon [Li/(CF)x], used for the lithium primary battery, and has the advantages of high applicability, a wide range and the like.
Description
Technical field
The present invention relates to a kind of chemical cell field, particularly relate to the lithium of a kind of lithium battery anticorrosion electrolyte and gained once
Battery.
Background technology
Lithium primary battery is high because of its specific energy, and energy density is big,(Open/put)Road voltage is high, discharging voltage balance, work temperature
The advantages such as degree scope is wide, cryogenic property length good storage life, occupy leading position in the market comsupton of one-shot battery.At height
In the selection of the electrolyte lithium salt of quality lithium primary battery, we tend to select electrical conductivity high, Heat stability is good, safety system
The lithium salts that inside battery structure is not destroyed by number height simultaneously.However, it is necessary to the lithium salts possessing many merits is quite few, big many places
In laboratory development, also has suitable distance apart from its industrialization.And produce the upper most existing defects of lithium salts used, for example
Lithium perchlorate, it is cheap, it is easy to preparation, and electrical conductivity is big simultaneously, and heat endurance is strong, but it holds under some extreme conditions
Easily react cause battery catches fire to explode with organic bath.For another example fluorine-containing high conductivity lithium salts:Double fluoroform sulphonyl are sub-
Amine lithium, it has very high degree of dissociation and electrical conductivity, but it in use has strong corrosiveness to aluminium foil, leads
Send a telegraph pond cannot normally work, cause battery life greatly to reduce.Therefore, during manufacturing one-shot battery, how
By the maximum advantage of the lithium salts of commercialization, shortcoming minimizes or by due for lithium salts effect by way of pluses and minuses are complementary
All embodying in battery is the problem that battery development & production enterprise is paid high attention to.And by adjusting lithium salts and organic bath
Ratio thus reach the optimization to battery allomeric function, this fully application to lithium salts and development tool to lithium primary battery
Significant.
Content of the invention
For above-mentioned technical problem, the technical issues that need to address of the present invention are to provide a kind of capacity height, have aluminium foil
Excellent passivation, reduce the corrosion, safety excellent performance of positive pole aluminium foil collector lithium primary battery anticorrosion electrolyte and
The lithium primary battery of gained.
In order to solve above-mentioned technical problem, the present invention adopts the technical scheme that:A kind of lithium battery anticorrosion electrolyte, including
Organic solvent and electrolyte, described electrolyte is mixing lithium salts, and described mixing lithium salts is bis-trifluoromethylsulfoandimide lithium
LiTFSI, di-oxalate lithium borate LiBOB and lithium perchlorate, the headformulae of corresponding lithium salts is as follows, and lithium perchlorate is mixing
Closing the quality proportion in lithium salts is 0.01%~5 as inorganic auxiliary salt.
Further:In above-mentioned rotten lithium battery electrolytes, described bis-trifluoromethylsulfoandimide lithium LiTFSI is in mixing lithium salts
Quality proportion be 10~90.The volume basis of described organic solvent consist of carbonates 10 ~ 50%, sulfurous esters 10 ~
50% and carboxylic acid esters 10 ~ 50%, and the volume composition sum of this three kinds of materials is 100%.
Described carbonates includes butylene BC, vinylene carbonate VC, dimethyl carbonate DMC, carbonic acid diethyl
In ester DEC, methyl propyl carbonate MPC, methyl ethyl carbonate EMC at least one or more of;Carbonates volume hundred in the electrolytic solution
Content is divided to be 1 ~ 50%.
Or:Described carbonates also includes in ethylene carbonate EC or propene carbonate PC at least one or two;
Volumn concentration in the electrolytic solution is 1 ~ 50%.
Described sulfurous esters is ethylene sulfite ES, propylene sulfite PS, dimethyl sulfite DMS, sulfurous
At least one in diethyl phthalate DES, sulfurous esters volumn concentration in the electrolytic solution is 10 ~ 50%.
Described carboxylic acid esters is methyl formate MF, Ethyl formate EF, ethyl acetate EA, methyl acetate MA, ethyl butyrate
At least one in EB, ethyl propionate EP, carboxylic acid esters volumn concentration in the electrolytic solution is 10 ~ 50%.
The concentration of described mixing lithium salts is 0.6 ~ 1.2M, if lithium salt too low (being less than 0.6M), the then electricity of electrolyte
Conductance can reduce, and the electrical property of battery reduces;If lithium salt is too high.More than 1.2M, then the viscosity of electrolyte increases, lithium from
Sub-migration resistance increases, and the cryogenic property of battery reduces.
Present invention also offers by the lithium primary battery of above-mentioned anticorrosion electrolyte gained, it also comprises metal collector and painting
Apply positive pole, negative pole and the shell of active material coating on its surface;Wherein, positive electrode active materials is ferrous disulfide, titanium dioxide
In manganese, cupric oxide and carbon monofluoride any one;Described metal collector is aluminium foil;Negative pole is lithium metal or lithium-aluminium alloy;Shell
For any one in box hat, aluminum hull or aluminum plastic film.
Compared with prior art, lithium primary battery electrolyte of the present invention, including organic solvent and electrolyte, described electrolysis
Matter is mixing lithium salts, and described mixing lithium salts is bis-trifluoromethylsulfoandimide lithium LiTFSI, di-oxalate lithium borate LiBOB and perchloric acid
Lithium.LiBOB is used in mixed way with PC or EC, on the one hand electrolyte can be made to be formed and stablize effective SEI film, prevents in electric discharge
During graphite linings peeling phenomenon occurs, on the other hand, the electrolyte adding LiBOB in electrolyte is conducive to aluminium foil surface to be formed
Passivating film effectively, prevents from being corroded by the fluoric-containing acid matter in electrolyte.Meanwhile, BOB-Anion can also build SEI effectively
Film.In other words, LiTFSI and LiBOB be applied in combination the corrosiveness not only eliminating LiTFSI to aluminium foil, and LiBOB
There is in organic dielectric stronger electrical conductivity, can significantly improve mixing lithium salts by the interpolation of auxiliary salt perchlorate
Electrical conductivity, the comprehensive chemical property improving battery, the problem simultaneously solving existing lithium primary battery poor stability.Except electrolysis
Beyond liquid, other materials of battery are restricted little, and optional scope is big.It is strong that the lithium battery electrolytes that the present invention provides has applicability,
The wide advantage of application.
Detailed description of the invention
The purport of the present invention is to provide a kind of lithium battery electrolytes, i.e. bis-trifluoromethylsulfoandimide lithium LiTFSI, double oxalic acid
Lithium borate LiBOB and lithium perchlorate, be used in mixed way, the comprehensive chemical property improving battery, solves existing lithium primary battery
The service life causing because of corrosion is short, the problem of poor stability.Below in conjunction with embodiment, present disclosure is made further
Describe in detail, content mentioned in embodiment not limitation of the invention, the selection of battery material can suit measures to local conditions and to result
There is no substantial effect.
Embodiment 1
Positive active material selects ferrous disulfide, conductive agent acetylene black and graphite, binding agent, adds pure water to be stirred until homogeneous, will
Scattered anode active material slurry is coated on positive pole aluminium foil collector, is cut into the positive plate of battery after rolling.Positive pole
After piece is by being dried and removing moisture therein completely, in the environment of putting into relative humidity less than 1.0%, at negative pole(Metallic aluminium
Or lithium-aluminium alloy)Play the porous isolating membrane separating both positive and negative polarity effect with insertion in the middle of positive plate, be wound into columned electricity
Core, the battery core of winding puts into battery case(Shell is box hat, aluminum hull or aluminum plastic film), fluid injection is assembled into battery.
At anolyte portion, use bis-trifluoromethylsulfoandimide lithium LiTFSI and di-oxalate lithium borate LiBOB and perchloric acid
Lithium makees lithium salts, and wherein quality proportion in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI is 50, double oxalic acid boric acid
Quality proportion in mixing lithium salts for the lithium LiBOB is 49, and quality proportion in mixing lithium salts for the lithium perchlorate is 1, mixing
The concentration of lithium salts is 1.2M.Select ethylene carbonate EC, butylene BC, ethylene sulfite ES and methyl formate MF conduct
Electrolyte, wherein ethylene carbonate EC volumn concentration is 40%, and volume butene esters BC volumn concentration is 10%, sulfurous acid
Vinyl acetate ES volumn concentration is 10%, and methyl formate MF volumn concentration is 40%.The positive pole of the present invention, negative pole, electrolysis
The method that liquid and barrier film are commonly used according to those skilled in the art, as described in content of the invention, prepares Li/FeS2Lithium primary battery.
Embodiment 2
By embodiment 1 the same manner, positive electrode material selects carbon monofluoride, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 60, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 39, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1.1M.Select ethylene carbonate EC, vinylene carbonate VC, sulfurous acid two
Methyl esters DMS and Ethyl formate EF is as electrolyte, and wherein ethylene carbonate EC volumn concentration is 30%, vinylene carbonate
VC volumn concentration is 20%, and dimethyl sulfite DMS volumn concentration is 20%, and Ethyl formate EF volumn concentration is
30%.The method that the positive pole of the present invention, negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, such as content of the invention institute
State, preparation Li/ (CF)xLithium primary battery.
Embodiment 3
By embodiment 1 the same manner, positive electrode material selects manganese dioxide, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 70, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 29, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1.2M.Select ethylene carbonate EC, dimethyl carbonate DMC, sulfurous acid two
Ethyl ester DES and ethyl acetate EA is as electrolyte, and wherein ethylene carbonate EC volumn concentration is 45%, dimethyl carbonate DMC
Volumn concentration is 5%, and sulfurous acid diethyl ester DES volumn concentration is 30%, and ethyl acetate EA volumn concentration is
20%.The method that the positive pole of the present invention, negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, such as content of the invention institute
State, prepare Li/MnO2Lithium primary battery.
Embodiment 4
By embodiment 1 the same manner, positive electrode material selects cupric oxide, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double oxalic acid
Lithium borate LiBOB and lithium perchlorate make lithium salts, wherein mass ratio in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Being heavily 80, quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 19, and lithium perchlorate is in mixing lithium salts
Quality proportion is 1, and the concentration of mixing lithium salts is 1M.Select ethylene carbonate EC, diethyl carbonate DEC, dimethyl sulfite
DMS and methyl acetate MA is as electrolyte, and wherein ethylene carbonate EC volumn concentration is 20%, diethyl carbonate DEC volume
Percentage composition is 30%, and dimethyl sulfite DMS volumn concentration is 30%, and methyl acetate MA volumn concentration is 20%.This
The method that the positive pole of invention, negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, as described in content of the invention, preparation
Li/CuO lithium primary battery.
Embodiment 5
By embodiment 1 the same manner, positive electrode material selects manganese dioxide, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 85, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 14, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1.2M.Select ethylene carbonate EC, methyl propyl carbonate MPC, methyl ethyl carbonate
Ester EMC, ethylene sulfite ES and ethyl butyrate EB are as electrolyte, and wherein ethylene carbonate EC volumn concentration is 20%,
Methyl propyl carbonate(MPC volumn concentration is 15%, and methyl ethyl carbonate EMC volumn concentration is 15%, ethylene sulfite ES
Volumn concentration is 30%, and ethyl butyrate EB volumn concentration is 20%.The positive pole of the present invention, negative pole, electrolyte and barrier film
The method commonly used according to those skilled in the art, as described in content of the invention, prepares Li/MnO2Lithium primary battery.
Embodiment 6
By embodiment 1 the same manner, positive electrode material selects carbon monofluoride, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 59, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 40, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1M.Select ethylene carbonate EC, propene carbonate PC, ethylene sulfite
ES and ethyl propionate EP is as electrolyte, and wherein ethylene carbonate EC volumn concentration is 25%, propene carbonate PC volume hundred
Dividing content to be 25%, ethylene sulfite ES volumn concentration is 30%, and ethyl propionate EP volumn concentration is 20%.This
The method that bright positive pole, negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, as described in content of the invention, prepares Li/
(CF)xLithium primary battery.
Embodiment 7
By embodiment 1 the same manner, positive electrode material selects ferrous disulfide, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 55, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 44, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1.1M.Select propene carbonate PC, butylene BC sulfurous acid ethene
Ester ES and ethyl propionate EP is as electrolyte, and wherein butylene BC volumn concentration is 20%, propene carbonate PC volume
Percentage composition is 30%, and ethylene sulfite ES volumn concentration is 25%, ethyl propionate EP)Volumn concentration is 25%.This
The method that the positive pole of invention, negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, as described in content of the invention, preparation
Li/FeS2Lithium primary battery.
Embodiment 8
By embodiment 1 the same manner, positive electrode material selects manganese dioxide, uses bis-trifluoromethylsulfoandimide lithium LiTFSI and double grass
Acid lithium borate LiBOB and lithium perchlorate make lithium salts, wherein quality in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Proportion is 49, and quality proportion in mixing lithium salts for the di-oxalate lithium borate LiBOB is 50, and lithium perchlorate is in mixing lithium salts
Quality proportion be 1, mixing lithium salts concentration be 1.2M.Select propene carbonate PC ethylene sulfite ES and ethyl propionate
EP is as electrolyte, and wherein propene carbonate PC volumn concentration is 50%, and ethylene sulfite ES volumn concentration is
25%, ethyl propionate EP volumn concentration is 25%.The positive pole of the present invention, negative pole, electrolyte and barrier film are according to art technology
The method that personnel commonly use, as described in content of the invention, prepares Li/MnO2Lithium primary battery.
Comparative example 1
By embodiment 1 the same manner, but as a control group, positive electrode material selects ferrous disulfide, and this group is with double fluoroform sulphonyl
The main salt of imine lithium LiTFSI and lithium perchlorate make auxiliary salt.Wherein matter in mixing lithium salts for the bis-trifluoromethylsulfoandimide lithium LiTFSI
Amount proportion is 99, and quality proportion in mixing lithium salts for the lithium perchlorate is 1, and the concentration of mixing lithium salts is 1M.Select carbonic acid
Propylene PC ethylene sulfite ES and ethyl propionate EP is as electrolyte, and wherein propene carbonate PC volumn concentration is
50%, ethylene sulfite ES volumn concentration is 25%, and ethyl propionate EP volumn concentration is 25%.The positive pole of the present invention,
The method that negative pole, electrolyte and barrier film are commonly used according to those skilled in the art, as described in content of the invention, prepares Li/FeS2Lithium one
Primary cell.
After measured, embodiment 1 to example 8 is owing to the addition of di-oxalate lithium borate LiBOB, and battery aluminium foil is not subject in test
To corrosion, showing that passivation is good, battery discharge is normal.Comparative example is not owing to adding LiBOB, and battery aluminium foil surface is by corruption
Erosion, in test period, aluminium foil surface occurs in that the phenomenon that is corroded, and finally results in battery discharge abnormal.
Last institute is it should be noted that, the present invention is only protected by above example in order to technical scheme to be described
Protecting the restriction of scope, although being explained in detail the present invention with reference to preferred embodiment, those of ordinary skill in the art should
Understand, technical scheme can be modified or equivalent, without deviating from the essence of technical solution of the present invention
And scope.
Claims (9)
1. a lithium battery anticorrosion electrolyte, including organic solvent and electrolyte, it is characterised in that:Described electrolyte is mixing
Lithium salts, described mixing lithium salts is bis-trifluoromethylsulfoandimide lithium LiTFSI, di-oxalate lithium borate LiBOB and lithium perchlorate, corresponding
The headformulae of lithium salts is as follows:
2. anticorrosion lithium battery electrolytes according to claim 1, it is characterised in that:Described bis-trifluoromethylsulfoandimide lithium
Quality proportion in mixing lithium salts for the LiTFSI is 10~90.
3. anticorrosion lithium battery electrolytes according to claim 2, it is characterised in that:The volume basis group of described organic solvent
Become carbonates 10~50%, sulfurous esters 10~50% and carboxylic acid esters 10~50%, and the volume of this three kinds of materials
Composition sum is 100%.
4. anticorrosion lithium battery electrolytes according to claim 3, it is characterised in that:Described carbonates includes carbonic acid fourth
Alkene ester BC, vinylene carbonate VC, dimethyl carbonate DMC, diethyl carbonate DEC, methyl propyl carbonate MPC, methyl ethyl carbonate EMC
In at least one or more of;Carbonates volumn concentration in the electrolytic solution is 1~50%.
5. anticorrosion lithium battery electrolytes according to claim 3, it is characterised in that:Described carbonates includes ethylene
At least one in alkene ester EC, propene carbonate PC;Carbonates volumn concentration in the electrolytic solution is 1~50%.
6. anticorrosion lithium battery electrolytes according to claim 3, it is characterised in that:Described sulfurous esters is sulfurous acid
At least one in vinyl acetate ES, propylene sulfite PS, dimethyl sulfite DMS, sulfurous acid diethyl ester DES;Sulfurous esters
Volumn concentration in the electrolytic solution is 10~50%.
7. anticorrosion lithium battery electrolytes according to claim 3, it is characterised in that:Described carboxylic acid esters is methyl formate
At least one in MF, Ethyl formate EF, ethyl acetate EA, methyl acetate MA, ethyl butyrate EB, ethyl propionate EP;Carboxylic acid esters
Volumn concentration in the electrolytic solution is 10~50%.
8. anticorrosion lithium battery electrolytes according to claim 3, it is characterised in that:The concentration of described mixing lithium salts is 0.6
~1.2M.
9. one kind by the lithium primary battery of anticorrosion electrolyte gained according to any one of claim 1 to 8, it is characterised in that:It
The positive pole of the active material coating also comprising metal collector and being coated in its surface, negative pole and shell;Wherein, positive-active material
Material is any one in ferrous disulfide, manganese dioxide, cupric oxide and carbon monofluoride;Described metal collector is aluminium foil;Negative pole is gold
Belong to lithium or lithium-aluminium alloy;Shell is any one in box hat, aluminum hull or aluminum plastic film.
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CN112331874A (en) * | 2020-10-23 | 2021-02-05 | 复旦大学 | Wide-temperature-range electrolyte for lithium-carbon fluoride battery |
CN112510264A (en) * | 2020-12-02 | 2021-03-16 | 电子科技大学 | Lithium-carbon fluoride battery with ultralow-concentration electrolyte and preparation method thereof |
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