CN105006579A - Electrolyte functional additive, non-aqueous electrolyte used for lithium primary battery and lithium primary battery - Google Patents
Electrolyte functional additive, non-aqueous electrolyte used for lithium primary battery and lithium primary battery Download PDFInfo
- Publication number
- CN105006579A CN105006579A CN201510449318.2A CN201510449318A CN105006579A CN 105006579 A CN105006579 A CN 105006579A CN 201510449318 A CN201510449318 A CN 201510449318A CN 105006579 A CN105006579 A CN 105006579A
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- Prior art keywords
- electrolyte
- lithium
- primary battery
- lithium primary
- battery
- Prior art date
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Classifications
-
- 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
- H01M6/168—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by additives
-
- 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
Abstract
The invention discloses an organic electrolyte capable of improving cryogenic property of a lithium primary battery, the lithium primary battery and a functional additive added into the electrolyte. According to the organic electrolyte capable of improving cryogenic property of the lithium primary battery, the lithium primary battery and the functional additive added into the electrolyte, a new electrolyte functional additive is added into the electrolyte, and the general chemical formula of the electrolyte is AXB or AB. The internal resistance of the lithium battery is lowered effectively through the addition of the additive. The electrolyte can lower the internal resistance of the lithium battery obviously, the problem that the pressure drop is too high when the lithium battery is stored is solved, the normal-temperature discharge performance, the low-temperature discharge performance, the high-power discharge performance and the high-temperature storage performance of the lithium battery are improved greatly, and the application range of the lithium primary battery is enlarged effectively.
Description
Technical field
The present invention relates to a kind of lithium battery electrolytes, belong to electrochemical field, specifically refer to a kind of lithium primary battery having the lithium primary battery electrolyte of good normal temperature and cryogenic property, the functional additive of this electrolyte and contain this battery electrolyte.
Background technology
Along with the fast development of electronic information technology and consumption electronic product, to the performance requirement of battery each side also in fast lifting, the particularly low temperature performance of battery, high-temperature storage performance and high power discharge performance, this has become the guardian technique difficult point that lithium primary battery runs in expansive approach field.The solvent of current commercial lithium manganese cell electrolyte mostly is cyclic organic carbonate ester, organic ether system, when ambient temperature is lower than-20 DEG C, the viscosity of electrolyte increases exponentially, lithium salts partially crystallizable is separated out, conductivity significantly reduces, battery voltage platform in loaded situation obviously declines, cause the discharge time of battery, capacity also obviously reduces thereupon, this greatly limits the use of lithium primary battery under low temperature and high-power condition.Simultaneously under high temperature storage conditions, the capability retention of primary cell is not high, and pressure drop is obvious, which also limits it and uses under the high temperature conditions.
Summary of the invention
For problems of the prior art, the object of this invention is to provide a kind of novel non-water organic electrolyte for lithium primary battery, add the functional additive in this electrolyte to and contain the lithium primary battery of this electrolyte.Described electrolyte obviously can reduce the internal resistance of lithium battery, improve pressure drop problems of too when lithium battery is deposited, significantly improve normal temperature and the low temperature performance of lithium battery, high power discharge performance and high-temperature storage performance, effectively expand the scope of application of lithium primary battery.
The technical scheme that electrolyte functional additive of the present invention adopts is: the chemical general formula of described functional additive is AXB or AB, wherein,
A is one or more the mixture in Cs, Rb, Sr, Ba;
X is C
5h
5n, (C
2h
5)
3n, CH
3cN, (CH
2cN)
2, (C
2h
4cN)
2, one or more mixture in glycol dimethyl ether (DME) or oxolane (THF);
B is one or more the mixture in following structural formula: PF
6 -, CH
3cOO
-, CO
3 2-, BF
4 -, AsF
6 -, N (SO
2c
2f
5)
2 -, N (SO
2cF
3)
2 -, N (SO
2f)
2 -, CF
3sO
3 -, ClO
4 -, BC
4o
8 -(BOB
-), BC
2o
4f
2 -(DFOB
-), PF
3(CF
2cF
3)
3 -(FAP
-), F
-, Br
-, I
-, Cl
-, NO
3 -, SO
4 2-.
The technical scheme that lithium primary battery nonaqueous electrolytic solution of the present invention adopts is: this electrolyte comprises non-aqueous organic solvent and electrolytic salt, and it also comprises functional additive as above.
Further, the molar concentration of described functional additive in described nonaqueous electrolytic solution is 0.001 ~ 0.1 mol/L, preferably 0.03 ~ 0.06 mol/L.
Further, conventional lithium primary battery electrolysis additive can also be comprised in described nonaqueous electrolytic solution, as vinylene carbonate, ethylene carbonate vinylene, 1,3-propane sultone, 1, one or more mixture in 4-butane sultones, fluorinated ethylene carbonate, difluoroethylene carbonate, PST; Its content in lithium primary battery electrolyte is 0 ~ 5.0wt%.For a person skilled in the art, also can add the lithium primary battery electrolysis additive except above-mentioned other listed routine, this is unrestricted in the present invention.
Further, described non-aqueous organic solvent is ethylene carbonate (EC), propene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), gamma-butyrolacton (GBL), dimethyl-tetrahydrofuran, oxolane, glycol dimethyl ether, ethylene glycol diethyl ether, ethylene glycol methyl ether, 1, 3-dioxolane, 1, 3-dioxane, 1, 4-dioxane, vinyl sulfone(RemzaolHuo Xingranliaohuoxingjituan), methyl-sulfoxide, sulfolane, N, N-dimethyl formamide, linear carboxylate, methyl acetate (MA), ethyl acetate (EA), propyl acetate (EP), butyl acetate, ethyl propionate, one or more mixture in propyl propionate or butyl propionate.Generally speaking, described organic solvent is the mixed solvent of cyclic ester class, ol ester class, ethers, sulfone class.Except above-mentioned enumerating, can also be well known to a person skilled in the art any conventional non-aqueous organic solvent, this limit in the present invention.
Further, described electrolytic salt is LiPF
6, LiBF
4, LiClO
4, LiBOB, LiDFOB, LiFAP, LiAsF
6, LiSbF
6, LiCF
3s0
3, LiN (SO
2cF
3)
2, LiN (SO
2c
2f
5)
2, LiN (SO
2cF
3)
2, LiN (SO
2c
4f
9)
2, LiC (SO
2cF
3)
3, LiPF
3(C
3f
7)
3, LiB (CF
3)
4, LiBF
3(C
2f
5), one or more mixture in LiI, LiCl or LiBr, described electrolytic salt concentration is in the electrolytic solution 0.5 ~ 2.5mol/L.In the present invention, the main salt of electrolytic salt is wherein lithium perchlorate, and auxiliary salt is selected from lithium hexafluoro phosphate, LiBF4, trifluoromethyl sulfonic acid lithium, di-oxalate lithium borate, two (trimethyl fluoride sulfonyl) imine lithium, two (fluorine sulphonyl) imine lithium, difluorine oxalic acid boracic acid lithium or anhydrous lithium iodide.
The technical scheme that lithium primary battery of the present invention adopts is: this lithium primary battery comprises positive pole, negative pole, barrier film and electrolyte, and this lithium primary battery adopts nonaqueous electrolytic solution as above.
Further, described negative pole is selected from one or more the mixture in lithium metal or lithium alloy.
Further, described positive pole comprises and is selected from Mn0
2, fluorographite or fluorocarbons (CF
x)
n, V
2o
5, CuO, CuS, FeS
2, TiS
2, Ag
2crO
4, MoO
3, Bi
2o
3, Bi
2pb
2o
5, Cu
4o (PO
4)
2in one or more mixture, wherein, (CF
x)
nin X value be 0 < X < 1.
The structure of non-water lithium primary battery of the present invention has no particular limits.Such as, this non-water primary cell can be Coin-shaped battery, comprise a positive pole, a negative pole and single or multiple barrier film, or cylinder type or diamond-shaped (comprising Soft Roll, aluminum hull, box hat, plastic casing) battery, comprise a positive pole, a negative pole and membrane coil.Described barrier film can be known microporous polyolefin film, fabric or non-woven.
The invention has the beneficial effects as follows: using new function additive as lithium primary battery electrolyte main additive in the present invention.Electrolyte obviously can reduce the internal resistance of lithium battery, improves pressure drop problems of too when lithium battery is deposited, and significantly improves normal temperature and the low temperature performance of lithium battery, high power discharge performance and high-temperature storage performance, effectively expands the scope of application of lithium primary battery.
Embodiment
Below in conjunction with specific embodiment, the present invention is further described.
embodiment 1:
1, electrolyte preparation: prepare electrolyte in BRAUN glove box, be full of the nitrogen that purity is 99.999% in glove box, in glove box, moisture controls at≤5ppm, and temperature is in room temperature.Add propene carbonate and glycol dimethyl ether with the ratio of 1:1, then add LiClO
4form the nonaqueous electrolytic solution that lithium salts molar concentration is the lithium primary battery of 1.0 mol/L, in above nonaqueous electrolytic solution, add CsC
5h
5nPF
6make the CsC that it obtains containing 0.01M
5h
5nPF
6nonaqueous electrolytic solution, after Homogeneous phase mixing, obtain lithium primary battery nonaqueous electrolytic solution.
2, the preparation of lithium ferrous sulfide AA type battery: adopt FeS
2for positive electrode, positive plate is made with current techique, metal Li is negative material, negative pole lithium band is made with current techique, insert lithium battery dedicated diaphragm between positive/negative plate, take winding method that positive/negative plate is made into battery core, battery core puts into No. 5 AA battery cases, after injecting the electrolyte of 2.0g the various embodiments described above and comparative example gained respectively, namely steel ball sealing, cleaning obtain each corresponding lithium Fe battery.Test: the lithium Fe battery that embodiment 1 is obtained is carried out respectively 1000mA and connect and put electric discharge to 0.8V, respectively at room temperature, test under low temperature and hot conditions, high power discharge carries out company at 2000mA puts test for often kind of battery.
3, lithium-manganese dioxide 2032 detains electricity preparation: adopt MnO
2for positive electrode, positive plate is made with current techique, before assembling battery, positive plate uses the organic electrolyte of the various embodiments described above and comparative example gained to soak 6 hours respectively, lithium metal is negative material, negative pole lithium sheet is made with current techique, lithium battery dedicated diaphragm is inserted between positive/negative plate, take lamination process that positive/negative plate is made into battery core, battery core puts into the special button cell shell of CR2032, inject the organic electrolyte of the various embodiments described above and comparative example gained respectively, electric pressing machine edge curling seal, namely each corresponding CR2032 button type lithium-manganese battery is obtained after cleaning.The each CR2032 button type lithium-manganese battery made carries out 15000 ohm of constant-resistance discharges to 2.0V respectively under normal temperature 20 ° of C, low temperature-20 ° of C environment, and large multiplying power discharging carries out constant-resistance discharge to 2.0V according to 1000 ohm.
In the present invention, also carry out the test of embodiment 2 ~ 6, and the contrast test of comparative example 1 ~ 3, the compound method of embodiment and comparative example is carried out with reference to the compound method of embodiment 1.
As shown in table 1 to table 2, the indices of the embodiment that the present invention carries out and comparative example and performance test are as shown in Table.
Table 1: the battery positive and negative electrode that comparative example 1 ~ 3, embodiment 1 ~ 6 use and solvent material and content balance table.
Table 2: the electrolytic salt in comparative example 1 ~ 3, embodiment 1 ~ 6 and salinity, additive and additive amount and when carrying out battery testing, the contrast table of discharge performance.
As shown in table 1 to table 2, invention has been 6 groups of embodiments, also carried out 3 groups of comparative examples simultaneously and come to contrast with embodiment.As can be seen from embodiment, new additive agent add the normal temperature and low temperature performance that significantly improve lithium battery, high power discharge performance, during effective minimizing high temperature storage, internal resistance increase and high temperature storage capability retention, expand the scope of application of lithium primary battery effectively.
Above-described embodiment is the explanation of inventor to several embodiments that the present invention carries out, and also can be other functional additive, as CsBF in certain embodiment
4, CsAsF
6, CsN (SO
2c
2f
5)
2, CsN (SO
2cF
3)
2, CsCF
3sO
3, CsClO
4, CsF, CsCl, Cs
2sO
4, RbBF
4, RbAsF
6, RbN (SO
2c
2f
5)
2, RbN (SO
2cF
3)
2, RbCF
3sO
3, RbClO
4, RbF, RbCl, Rb
2sO
4, Sr (BF
4)
2, Sr (AsF
6)
2, Sr (N (SO
2c
2f
5)
2)
2, Sr (N (SO
2cF
3)
2)
2, Sr (CF
3sO
3)
2, Sr (ClO
4)
2, SrF
2, SrCl
2, SrSO
4, Ba (BF
4)
2, Ba (AsF
6)
2, Ba (N (SO
2c
2f
5)
2)
2, Ba (N (SO
2cF
3)
2)
2, Ba (CF
3sO
3)
2, Ba (ClO
4)
2, BaF
2, BaCl
2, BaSO
4, Cs (CH
2cN)
2bF
4, Rb (CH
2cN)
2clO
4, Sr (CH
2cN)
2cO
3, Ba (CH
2cN)
2(CF
3sO
3)
2, Cs (C
2h
4cN)
2cH
3cOO, Rb (C
2h
4cN)
2f, Sr (C
2h
4cN)
2i
2, Ba (C
2h
4cN)
2(CF
3sO
3)
2, etc., all can reach effect of the present invention.Because length limit, just do not enumerate at this.Above-described embodiment is described in detail the present invention, but and does not mean that the present invention is only confined to these examples.When not departing from the technology of the present invention principle, making improvements and being out of shape within the claims in the present invention and technology, also should belong to protection scope of the present invention.
Claims (8)
1. for a functional additive for primary cell electrolyte, it is characterized in that: the chemical general formula of described functional additive is AXB or AB, wherein,
A is one or more the mixture in Cs, Rb, Sr, Ba;
X is C
5h
5n, (C
2h
5)
3n, CH
3cN, (CH
2cN)
2, (C
2h
4cN)
2, one or more mixture in glycol dimethyl ether (DME) or oxolane (THF);
B is one or more the mixture in following structural formula: PF
6 -, CH
3cOO
-, CO
3 2-, BF
4 -, AsF
6 -, N (SO
2c
2f
5)
2 -, N (SO
2cF
3)
2 -, N (SO
2f)
2 -, CF
3sO
3 -, ClO
4 -, BC
4o
8 -(BOB
-), BC
2o
4f
2 -(DFOB
-), PF
3(CF
2cF
3)
3 -(FAP
-), F
-, Br
-, I
-, Cl
-, NO
3 -, SO
4 2-.
2. for a nonaqueous electrolytic solution for lithium primary battery, this electrolyte comprises non-aqueous organic solvent and electrolytic salt, it is characterized in that: it also comprises functional additive as claimed in claim 1.
3. electrolyte according to claim 2, is characterized in that: the molar concentration of described functional additive in described nonaqueous electrolytic solution is 0.001 ~ 0.1 mol/L, preferably 0.03 ~ 0.06 mol/L.
4. electrolyte according to claim 2, it is characterized in that: described non-aqueous organic solvent is ethylene carbonate (EC), propene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), gamma-butyrolacton (GBL), dimethyl-tetrahydrofuran, oxolane, glycol dimethyl ether, ethylene glycol diethyl ether, ethylene glycol methyl ether, 1, 3-dioxolane, 1, 3-dioxane, 1, 4-dioxane, vinyl sulfone(RemzaolHuo Xingranliaohuoxingjituan), methyl-sulfoxide, sulfolane, N, N-dimethyl formamide, linear carboxylate, methyl acetate (MA), ethyl acetate (EA), propyl acetate (EP), butyl acetate, ethyl propionate, one or more mixture in propyl propionate or butyl propionate.
5. electrolyte according to claim 2, is characterized in that: described electrolytic salt is LiPF
6, LiBF
4, LiClO
4, LiBOB, LiDFOB, LiFAP, LiAsF
6, LiSbF
6, LiCF
3s0
3, LiN (SO
2cF
3)
2, LiN (SO
2c
2f
5)
2, LiN (SO
2cF
3)
2, LiN (SO
2c
4f
9)
2, LiC (SO
2cF
3)
3, LiPF
3(C
3f
7)
3, LiB (CF
3)
4or LiBF
3(C
2f
5), one or more mixture in LiI, LiCl and LiBr, described electrolytic salt concentration is in the electrolytic solution 0.5 ~ 2.5mol/L.
6. a lithium primary battery, comprises positive pole, negative pole, barrier film and electrolyte, it is characterized in that: this lithium primary battery adopts nonaqueous electrolytic solution as claimed in claim 2.
7. lithium primary battery according to claim 6, is characterized in that: described negative pole is selected from one or more the mixture in lithium metal or lithium alloy.
8. lithium primary battery according to claim 6, is characterized in that: described positive pole comprises and is selected from Mn0
2, fluorographite or fluorocarbons (CF
x)
n, V
2o
5, CuO, CuS, FeS
2, TiS
2, Ag
2crO
4, MoO
3, Bi
2o
3, Bi
2pb
2o
5, Cu
4o (PO
4)
2in one or more mixture, wherein, (CF
x)
nin X value be 0 < X < 1.
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Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN105977536A (en) * | 2016-07-08 | 2016-09-28 | 珠海市赛纬电子材料股份有限公司 | Electrolyte functional additive, non-aqueous lithium ion battery electrolyte and lithium ion battery |
CN106450365A (en) * | 2016-07-22 | 2017-02-22 | 惠州市惠德瑞锂电科技股份有限公司 | Anticorrosive electrolyte of lithium battery and obtained lithium primary battery |
CN112271306A (en) * | 2020-10-30 | 2021-01-26 | 上海空间电源研究所 | Low-temperature electrolyte for lithium-cobalt disulfide primary battery and lithium-cobalt disulfide primary battery |
CN114122440A (en) * | 2021-08-18 | 2022-03-01 | 厦门大学 | Lithium/carbon fluoride or lithium/metal fluoride battery electrolyte |
WO2023140429A1 (en) * | 2022-01-18 | 2023-07-27 | 삼성에스디아이 주식회사 | Electrolyte for rechargeable lithium battery and rechargeable lithium battery including same |
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CN102934264A (en) * | 2010-06-07 | 2013-02-13 | 奈克松有限公司 | Additive for lithium ion rechargeable battery cells |
CN104094452A (en) * | 2012-02-07 | 2014-10-08 | ***纪念研究院 | Methods and energy storage devices utilizing electrolytes having surface-smoothing additives |
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2015
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Patent Citations (2)
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CN102934264A (en) * | 2010-06-07 | 2013-02-13 | 奈克松有限公司 | Additive for lithium ion rechargeable battery cells |
CN104094452A (en) * | 2012-02-07 | 2014-10-08 | ***纪念研究院 | Methods and energy storage devices utilizing electrolytes having surface-smoothing additives |
Cited By (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN105977536A (en) * | 2016-07-08 | 2016-09-28 | 珠海市赛纬电子材料股份有限公司 | Electrolyte functional additive, non-aqueous lithium ion battery electrolyte and lithium ion battery |
CN106450365A (en) * | 2016-07-22 | 2017-02-22 | 惠州市惠德瑞锂电科技股份有限公司 | Anticorrosive electrolyte of lithium battery and obtained lithium primary battery |
CN112271306A (en) * | 2020-10-30 | 2021-01-26 | 上海空间电源研究所 | Low-temperature electrolyte for lithium-cobalt disulfide primary battery and lithium-cobalt disulfide primary battery |
CN112271306B (en) * | 2020-10-30 | 2022-03-25 | 上海空间电源研究所 | Low-temperature electrolyte for lithium-cobalt disulfide primary battery and lithium-cobalt disulfide primary battery |
CN114122440A (en) * | 2021-08-18 | 2022-03-01 | 厦门大学 | Lithium/carbon fluoride or lithium/metal fluoride battery electrolyte |
CN114122440B (en) * | 2021-08-18 | 2023-10-13 | 厦门大学 | Lithium/carbon fluoride or lithium/metal fluoride battery electrolyte |
WO2023140429A1 (en) * | 2022-01-18 | 2023-07-27 | 삼성에스디아이 주식회사 | Electrolyte for rechargeable lithium battery and rechargeable lithium battery including same |
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