CN105161757B - A kind of lithium-ion battery electrolytes containing the anti-overcharge additive of oxidation-reduction type - Google Patents
A kind of lithium-ion battery electrolytes containing the anti-overcharge additive of oxidation-reduction type Download PDFInfo
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- CN105161757B CN105161757B CN201510443504.5A CN201510443504A CN105161757B CN 105161757 B CN105161757 B CN 105161757B CN 201510443504 A CN201510443504 A CN 201510443504A CN 105161757 B CN105161757 B CN 105161757B
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- additive
- lithium
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- ion battery
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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
- 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
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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
- 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
- H01M10/0567—Liquid materials characterised by the additives
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- 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
A kind of lithium-ion battery electrolytes containing the anti-overcharge additive of oxidation-reduction type, including organic solvent, lithium salts and additive, additive include additive A, and the quality of additive A accounts for the 0.5%~20% of electrolyte gross mass, and the structural formula of additive A is:Wherein:R1、R2Independently selected from any of hydrogen, alkyl, haloalkyl, cycloalkyl, alkylene, aryl;R3、R4、R5、R6Independently selected from any of hydrogen, alkyl, halogen, nitro, itrile group, alkylene, aryl, hydroxyl, carboxyl, halogen is F, Cl or Br, and halo is part substitution or full substitution.The present invention can preferably play by adding additive A in electrolyte solution and overcharge protection, protection mechanism is reversible, and not influence the interval cycle performance of battery normal voltage, greatly improve the overcharge resistance performance energy and explosion-proof performance of electrolyte solution.
Description
Technical field
The invention belongs to electrochemical technology field, and in particular to a kind of lithium containing the anti-overcharge additive of oxidation-reduction type from
Sub- battery electrolyte.
Background technology
Significant advantage of the lithium rechargeable battery due to having high-energy-density and high-specific-power concurrently, it is considered to be most develop latent
The electrokinetic cell system of power.But we often can be appreciated that some reports about safety issue, there is lithium ion secondary electricity again and again
Pond thing on fire from explosion occurs, and this is also that consumer buys one used than larger misgivings always in fact.Wherein, overcharge
Electricity is one of common factor for causing cell safety sex chromosome mosaicism.
When lithium ion battery is overcharged, because cell voltage increases with polarization and rises rapidly, positive-active certainly will be triggered
The irreversible change of the structure of matter and the oxidation Decomposition of electrolyte, and then produce substantial amounts of gas and release substantial amounts of heat, cause
Inner pressure of battery and temperature are steeply risen, there is the hidden dangers such as blast, burning, meanwhile, the Carbon anode in overcharging state
Surface can also reduce its security because of the deposition of lithium metal.At present, many methods industrially go to avoid over-charging of battery, it is most simple
Single method is to monitor lithium ion battery with charger, once finding that voltage has the phenomenon of spilling, charging process is cut off at once,
This is a kind of very effective method, but this method may apply to a battery or a battery pack, but if being
Large-scale discharge and recharge, this method cost is that comparison is high.The additives for overcharge protection of battery is realized by additive, with use
The characteristics of amount is small, effect is obvious, and battery manufacturing process can be simplified, reduce battery production cost.In lithium battery overcharge-prevention
In electrolyte patent, over-charging of battery peace is mainly improved using two types (electropolymerization and oxidation-reduction type) anti-overcharge additive
Full performance, electropolymerization additive such as alkylbenzene and fluorobenzene can effectively suppress over-charging of battery, but its addition can damage battery
Cycle performance.The oxidation-reduction type additive studied at present such as 2,5- di-t-butyls -1,4- dimethoxy benzenes and phenothiazines
Though it is reversible but due to its relatively low oxidation potential to overcharge protection mechanism, fail to reach lithium ion battery normal working voltage 4.2V just
Generation redox reaction, often limits its large-scale use in the lithium ion battery of different battery material systems.
The content of the invention
The technical problems to be solved by the invention be to provide it is a kind of let off fill work well contain the anti-mistake of oxidation-reduction type
Fill the lithium-ion battery electrolytes of additive.
To reach above-mentioned purpose, the technical solution adopted by the present invention is:
A kind of lithium-ion battery electrolytes containing the anti-overcharge additive of oxidation-reduction type, including organic solvent, lithium salts and
Additive, described additive includes additive A, and the quality of described additive A accounts for the 0.5% of described electrolyte gross mass
~20%, the structural formula of described additive A is:
Wherein:R1、R2Independently selected from any of hydrogen, alkyl, haloalkyl, cycloalkyl, alkylene, aryl;R3、
R4、R5、R6Independently selected from any of hydrogen, alkyl, halogen, nitro, itrile group, alkylene, aryl, hydroxyl, carboxyl, halogen
For F, Cl or Br, halo is part substitution or full substitution.
Preferably, the quality of described additive A accounts for the 1%~5% of described electrolyte gross mass.
Preferably, described R1、R2It independently is alkyl or haloalkyl;Described R3、R4、R5、R6Independently selected from hydrogen,
Any of nitro, halogen.
It is further preferred that described additive A is(the chloro- 2,5- dimethoxys nitros of 4-
Benzene) or(1,4- dimethoxys phenyl tetrafluoride).
Preferably, described organic solvent is the mixture of cyclic ester and/or chain ester, and described cyclic ester is selected from carbon
One or more groups in vinyl acetate (EC), propene carbonate (PC), gamma-butyrolacton (GBL), butylene carbonate (BC)
Close;Described chain ester is selected from dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), methyl
One or more combinations in ethyl ester (EMC).
It is further preferred that described organic solvent is mixing for ethylene carbonate (EC) and methyl ethyl ester (EMC)
Compound, wherein, the mass ratio of described ethylene carbonate (EC) and described methyl ethyl ester (EMC) is 1:0.8~
1.2。
Preferably, described lithium salts is LiPF6(lithium hexafluoro phosphate), LiBF4(LiBF4), LiAsF6(hexafluoroarsenate
Lithium), LiClO4(lithium perchlorate), LiN (SO2CF3)2(two (trimethyl fluoride sulfonyl) imine lithiums), LiN (SO2C2F5)2(two (five fluorine
Ethyl sulphonyl) imine lithium), LiFSI (two (fluosulfonic acid acyl) imine lithiums), LiSO3CF3One kind in (trifluoromethyl sulfonic acid lithium) or
A variety of, the concentration of described lithium salts is 0.1~2mol/L.
It is further preferred that the concentration of described lithium salts is 0.9~1.2mol/L.
Preferably, described additive also includes other additives, the concentration of described other additives for 0.1~
0.5mol/L。
It is further preferred that other described additives are selected from biphenyl (BP), fluorinated ethylene carbonate (FEC), carbonic acid
Vinylene (VC), vinylethylene carbonate (VEC), 1,3-N-morpholinopropanesulfonic acid lactone (PS), 1,4- butyl sultones (BS), 1,3-
One or more in (1- propylene) sultone (PST), ethylene sulfite (ESI), sulfuric acid vinyl ester (ESA).
Above-mentioned electrolyte can be widely applied in the lithium ion batteries such as lithium primary battery, lithium secondary battery.
Because above-mentioned technical proposal is used, the present invention has following advantages compared with prior art:
The additive A added in the electrolytic solution of the present invention, overcharges that protection mechanism is reversible, and once overcharging rear battery does not almost have
Damage, greatly improves the overcharge resistance performance energy and explosion-proof performance of electrolyte;Additive A is added with most of similar (oxidation-reduction type)
Agent is compared, and additive oxidizing potential is higher (> 4.5V), it is adaptable to the lithium ion battery of the multiple material such as LCO, NCM, using model
Enclose wider;The lithium ion battery that lithium-ion electrolyte containing this additive A is prepared, has been likewise supplied with these advantages,
Simultaneously to the normal performance impact very little of lithium ion battery, the need for can meeting application completely.And the operability of the present invention
By force, cost is low.
Brief description of the drawings
Accompanying drawing 1 is the CV test curves of the Pt systems of the addition chloro- 2,5- dimethoxys nitrobenzene of 4- in embodiment 1;
Accompanying drawing 2 is the CV test curves of the Pt systems of addition 1,4- dimethoxy phenyl tetrafluorides in embodiment 1;
Accompanying drawing 3 is the addition chloro- 2,5- dimethoxys nitrobenzene of 4- following under normal charging/discharging voltage scope in embodiment 2
Ring capacity curve;
Accompanying drawing 4 is circulation appearance of the addition 1,4- dimethoxys phenyl tetrafluoride under normal charging/discharging voltage scope in embodiment 2
Measure curve;
Accompanying drawing 5 is the over-charging of battery test curve of the addition chloro- 2,5- dimethoxys nitrobenzene of 4- in embodiment 3;
Accompanying drawing 6 is the over-charging of battery test curve of addition 1,4- dimethoxy phenyl tetrafluorides in embodiment 3.
Embodiment
The present invention is elaborated below in conjunction with specific embodiment:
Embodiment 1:
In the argon gas glove box that moisture content is less than 10ppm, lithium-ion battery electrolytes are prepared:By lithium salts LiPF6It is dissolved in EC/
EMC (mass ratio is 1: 1) in the mixed solvent, wherein LiPF6Ultimate density be 1mol/L;Then above-mentioned electrolyte is divided into
Two parts, it is separately added into chloro- 2, the 5- dimethoxys nitrobenzene of 4- or 5% Isosorbide-5-Nitrae-dimethoxy four for accounting for electrolyte gross mass 1%
Fluorobenzene, prepares the CV tests that obtained electrolyte carries out Pt, working electrode and be Pt to electrode, and reference electrode is lithium piece, CV
Curve is as shown in accompanying drawing 1,2.
As a result find, chloro- 2, the 5- dimethoxys nitrobenzene of additive 4- and Isosorbide-5-Nitrae-dimethoxy phenyl tetrafluoride about exist respectively
Oxidation takes place at 4.45V, 4.5V, the redox reversible of molecule is good.
Embodiment 2:
In the argon gas glove box that moisture content is less than 10ppm, lithium-ion battery electrolytes are prepared, by lithium salts LiPF6It is dissolved in EC/
DMC/EMC (three's volume ratio is 1: 1: 1) in the mixed solvent, wherein LiPF6Ultimate density be 1mol/L, other additives
Addition species and amount be VC, 0.1mol/L.Above-mentioned electrolyte is divided into three parts, wherein two parts are added account for electrolyte respectively
Chloro- 2, the 5- dimethoxys nitrobenzene of 4- or 5% Isosorbide-5-Nitrae-dimethoxy phenyl tetrafluoride of gross mass 1%, another is not added with, and uses respectively
These three electrolyte prepare 1.3Ah LCO lithium ion batteries.Battery is charged to 4.2V under normal temperature 1C, then discharged into
2.75V, circulation, test discharge capacity of the cell and capability retention.Capacity circulating curve is as shown in accompanying drawing 3,4.
Comparative result finds un-added battery and contains the chloro- 2,5- dimethoxys nitrobenzene of 1% 4- or 5% 1,4-
The discharge capacity of the cell of dimethoxy phenyl tetrafluoride is almost consistent with capability retention, it is believed that the addition of additive A will not be right
The normal discharge and recharge of battery has obvious negative influence.
Embodiment 3:
(the H in the glove box of applying argon gas2O < 10ppm) lithium-ion battery electrolytes are prepared, by lithium salts LiPF6It is dissolved in EC/
(mass ratio is 1 to EMC:1) in the mixed solvent, wherein LiPF6Ultimate density be 1M, the addition species and amount of other additives
For VC, 0.1mol/L.Then the electrolyte is divided into two parts, addition respectively accounts for chloro- 2, the 5- diformazans of 4- of electrolyte gross mass 1%
Epoxide nitrobenzene or 5% Isosorbide-5-Nitrae-dimethoxy phenyl tetrafluoride, prepare 1.3Ah LCO lithium ion batteries with the electrolyte, carried out
Test is filled, rate of charge is 0.1C, and constant-current charge to 2.5Ah (equivalent to 1.2Ah electricity is overcharged) is discharged to 2.75V, circulated.
Cyclic curve is overcharged as shown in accompanying drawing 5,6.
As a result find, containing chloro- 2, the 5- dimethoxys nitrobenzene of 1% 4- or 5% Isosorbide-5-Nitrae-dimethoxy phenyl tetrafluoride
Battery is crossed be charged to 4.51V respectively, and during 4.57V, additive works, and is no longer raised after cell voltage is locked, and overcharges process not
Blast is not on fire, and battery still can back and forth carry out discharge and recharge after electric discharge.
The above embodiments merely illustrate the technical concept and features of the present invention, and its object is to allow person skilled in the art
Scholar can understand present disclosure and implement according to this, and it is not intended to limit the scope of the present invention, all according to the present invention
The equivalent change or modification that Spirit Essence is made, should all be included within the scope of the present invention.
Claims (8)
1. a kind of lithium-ion battery electrolytes containing the anti-overcharge additive of oxidation-reduction type, including organic solvent, lithium salts and add
Plus agent, it is characterised in that:Described additive includes additive A, and the quality of described additive A accounts for the described total matter of electrolyte
The 0.5% ~ 20% of amount, the structural formula of described additive A is:
。
2. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 1, it is characterised in that:
The quality of described additive A accounts for the 1% ~ 5% of described electrolyte gross mass.
3. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 1, it is characterised in that:
Described organic solvent is the mixture of cyclic ester and/or chain ester, and described cyclic ester is selected from ethylene carbonate, carbonic acid third
One or more combinations in alkene ester, gamma-butyrolacton, butylene carbonate;Described chain ester is selected from dimethyl carbonate, carbon
One or more combinations in diethyl phthalate, dipropyl carbonate, methyl ethyl ester.
4. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 3, it is characterised in that:
Described organic solvent is the mixture of ethylene carbonate and methyl ethyl ester, wherein, described ethylene carbonate and institute
The mass ratio for the methyl ethyl ester stated is 1:0.8~1.2.
5. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 1, its feature exists
In:Described lithium salts is LiPF6、LiBF4、LiAsF6、LiClO4、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiFSI、
LiSO3CF3In one or more, the concentration of described lithium salts is 0.1 ~ 2 mol/L.
6. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 5, its feature exists
In:The concentration of described lithium salts is 0.9 ~ 1.2 mol/L.
7. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 1, its feature exists
In:Described additive also includes other additives, and the concentration of other described additives is 0.1 ~ 0.5 mol/L.
8. the lithium-ion battery electrolytes of the anti-overcharge additive of oxidation-reduction type according to claim 7, its feature exists
In:Other described additives are selected from biphenyl, fluorinated ethylene carbonate, vinylene carbonate, vinylethylene carbonate, 1,3-
One in propane sultone, 1,4- butyl sultones, 1,3- (1- propylene) sultone, ethylene sulfite, sulfuric acid vinyl ester
Plant or a variety of.
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CN106898816A (en) * | 2015-12-17 | 2017-06-27 | 张家港市国泰华荣化工新材料有限公司 | A kind of lithium battery electrolytes and lithium battery |
CN106920993A (en) * | 2015-12-28 | 2017-07-04 | 张家港市国泰华荣化工新材料有限公司 | A kind of high temperature resistant and high-tension lithium-ion battery electrolytes and lithium ion battery |
CN106920994A (en) * | 2015-12-28 | 2017-07-04 | 张家港市国泰华荣化工新材料有限公司 | A kind of Overcharge prevention electrolyte and lithium battery |
KR102328258B1 (en) | 2017-10-17 | 2021-11-18 | 주식회사 엘지에너지솔루션 | Electrolyte for lithium metal battery and lithium metal battery comprising thereof |
CN108736067B (en) * | 2018-05-28 | 2020-08-14 | 合肥国轩高科动力能源有限公司 | Lithium ion battery electrolyte for improving flatulence and cycle performance under high voltage |
CN112670571A (en) * | 2020-12-01 | 2021-04-16 | 湖南博信新能源科技有限公司 | Multifunctional electrolyte additive, electrolyte and preparation method and application thereof |
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JP3493873B2 (en) * | 1995-04-28 | 2004-02-03 | ソニー株式会社 | Non-aqueous electrolyte secondary battery |
JP2928779B1 (en) * | 1998-07-31 | 1999-08-03 | 三洋電機株式会社 | Electrolyte for non-aqueous battery and secondary battery using this electrolyte |
JP2939468B1 (en) * | 1998-07-31 | 1999-08-25 | 三洋電機株式会社 | Electrolyte for non-aqueous battery and secondary battery using this electrolyte |
KR100812056B1 (en) * | 2005-10-24 | 2008-03-07 | 주식회사 엘지화학 | Inhibitor of reduction of life cycle of redox shuttle additive and non-aqueous electrolyte and secondary battery comprising the same |
US8367253B2 (en) * | 2006-02-02 | 2013-02-05 | U Chicago Argonne Llc | Lithium-ion batteries with intrinsic pulse overcharge protection |
KR101115028B1 (en) * | 2007-05-15 | 2012-03-09 | 주식회사 엘지화학 | Additive for non-aqueous electrolyte and secondary battery using the same |
CN101494305B (en) * | 2008-01-25 | 2011-05-18 | 比亚迪股份有限公司 | Lithium ion battery electrolyte and battery and battery set containing the same |
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CN101577348B (en) * | 2009-05-15 | 2011-03-23 | 中南大学 | Multiplex overcharging protection functional electrolyte for lithium ion battery |
US20110311879A1 (en) * | 2010-06-17 | 2011-12-22 | Sony Corporation | Nonaqueous electrolyte and nonaqueous electrolyte battery |
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US9005822B2 (en) * | 2013-03-06 | 2015-04-14 | Uchicago Argonne, Llc | Functional electrolyte for lithium-ion batteries |
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