CN105845982A - Electrolyte and lithium ion battery comprising same - Google Patents

Electrolyte and lithium ion battery comprising same Download PDF

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CN105845982A
CN105845982A CN201610194358.1A CN201610194358A CN105845982A CN 105845982 A CN105845982 A CN 105845982A CN 201610194358 A CN201610194358 A CN 201610194358A CN 105845982 A CN105845982 A CN 105845982A
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electrolyte
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lithium
battery
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CN105845982B (en
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王耀辉
史松君
谢岚
王珂
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Jiangsu Contemporary Amperex Technology Ltd
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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
    • 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
    • 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
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • 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

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Abstract

The present application relates to an electrolyte and a lithium ion battery including the same, wherein the electrolyte includes an organic solvent, a lithium salt, and an additive including a hydrogenated thiophene-boron trifluoride complex compound and a sultone compound. The electrolyte simultaneously comprises the hydrogenated thiophene-boron trifluoride coordination compound and the sultone compound, so that the decomposition of the electrolyte on the surface of an electrode can be inhibited under the synergistic effect of the hydrogenated thiophene-boron trifluoride coordination compound and the sultone compound, the corrosion of an acidic substance generated in the electrolyte to a solid electrolyte film can be effectively reduced, and the cycle performance and the storage performance of a lithium ion battery at normal temperature and high temperature can be improved.

Description

Electrolyte and include the lithium ion battery of this electrolyte
Technical field
The application relates to field of batteries, particularly relates to a kind of electrolyte and includes the lithium ion battery of this electrolyte.
Background technology
At present, the positive electrode active materials employed in lithium ion battery mainly have LiMn2O4, cobalt acid lithium, ternary material, LiFePO 4s etc., under normal conditions, select the charge cutoff voltage of the lithium ion battery of the above-mentioned positive electrode being previously mentioned Less than 4.2V, but it is as progress and the development in market of science and technology, promotes the energy density of lithium ion battery day by day Seeming important and urgent, the effective ways of a kind of energy density promoting lithium ion battery are exploitation high-voltage lithium ion batteries.
But, under the high voltage of 4.6V, the electrolyte positive electrode surface oxidation Decomposition at battery of routine, electrolysis can be caused The oxidation Decomposition of liquid self can promote the deteriorative reaction of positive electrode active materials simultaneously, affects the performance of lithium ion battery further, Such as storage performance and cycle performance.
For defect and the deficiency of existing battery, special release the application.
Summary of the invention
The primary goal of the invention of the application is to propose a kind of electrolyte.
Second goal of the invention of the application is to propose a kind of lithium ion battery.
In order to complete the purpose of the present invention, the technical scheme of employing is:
The application relates to a kind of electrolyte, and including organic solvent, lithium salts and additive, described additive includes hydrogenating thiophene Fen-boron trifluoride coordination compound and sultone compounds.
Preferably, described hydrogenation thiophene-boron trifluoride coordination compound is in the compound of structural formula as shown in formula I At least one:
Wherein, R1, R2, R3, R4It is each independently selected from hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～20Alkane Base, substituted or unsubstituted C2～20Thiazolinyl, substituted or unsubstituted C6～26Aryl；
Substituent group is selected from halogen, cyano group.
Preferably, described hydrogenation thiophene-boron trifluoride coordination compound is in the compound of structural formula as shown in formula I A At least one；
Wherein, R3、R4It is each independently selected from hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～20Alkyl, replacement Or unsubstituted phenyl；Substituent group is selected from halogen, cyano group.
Preferably, R3、R4It is each independently selected from hydrogen atom, fluorine atom.
Preferably, described sultone compounds is in following formula II, formula III, formula IV and the compound shown in formula V At least one:
Wherein, R11、R12、R13、R14It is each independently selected from hydrogen atom, halogen atom, nitro, cyano group, carboxyl, sulfonic group, takes Generation or unsubstituted C1～20Alkyl, substituted or unsubstituted C1～20Alkoxyl, substituted or unsubstituted C2～20Thiazolinyl, replacement or not Substituted C2～20Alkynyl, substituted or unsubstituted C1～20Alkane sulfonyl, substituted or unsubstituted C2～20Alkene sulfonyl, replacement or not Substituted C2～20Alkynes sulfonyl；
Substituent group is selected from halogen, cyano group, nitro, carboxyl or sulfonic group.
Preferably, R11、R12、R13、R14It is each independently selected from hydrogen atom, substituted or unsubstituted C1～6Straight or branched Alkyl, substituted or unsubstituted C1～6Straight or branched alkoxyl；Substituted or unsubstituted C5～7Cycloalkyl, replacement or unsubstituted C2～6Thiazolinyl, substituted or unsubstituted C2～6Alkynyl；
Substituent group is selected from halogen, cyano group.
Preferably, the 0.05% of the gross weight that content is electrolyte of described hydrogenation thiophene-boron trifluoride coordination compound ～10%；The content of described sultone compounds is the 0.1%～10% of the gross weight of electrolyte.
Preferably, described organic solvent is selected from ethylene carbonate, Allyl carbonate, butylene, fluoro ethylene carbonate In ester, Ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, 1,4-fourth At least one in ester, methyl propionate, methyl butyrate, ethyl acetate, ethyl propionate, propyl propionate and ethyl n-butyrate..
Preferably, described lithium salts is selected from lithium hexafluoro phosphate, LiBF4, lithium perchlorate, hexafluoroarsenate lithium, tetrafluoro grass Acid phosphoric acid lithium, LiN (SO2RF)2、LiN(SO2F)(SO2RF), double trifluoromethanesulfonimide lithium, double (fluorine sulphonyl) imine lithium, double At least one in Lithium bis (oxalate) borate, difluorine oxalic acid boracic acid lithium, wherein, RFFor-CnF2n+1, n is the integer of 1～10, is preferably LiPF6And/or LiN (SO2RF)2；
It is furthermore preferred that the concentration that described lithium salts is in the electrolytic solution is 0.5mol L-1～2mol L-1。
The application further relates to a kind of lithium ion battery, including the positive plate containing positive electrode active materials, containing negative electrode active The electrolyte of the negative plate of material, isolating membrane and the application.
The Advantageous Effects that the application can reach includes the following:
The electrolyte of the application includes simultaneously hydrogenate thiophene-boron trifluoride coordination compound and sultone compounds Time, under the common synergism of the two, it is possible to suppression electrolyte, in the decomposition of electrode surface, effectively reduces in electrolyte and produces The acidic materials corrosion to solid electrolyte plasma membrane, improve lithium ion battery cycle performance at ambient and elevated temperatures and height Storage performance under Wen, such as lithium ion battery are respectively provided with the cyclicity of excellence under 4.6V high voltage and at 25 DEG C and 45 DEG C Can, there is at 85 DEG C excellent storage performance.
Detailed description of the invention
Being described in detail below by the application, the feature of the application and advantage will become more along with these explanations For clear, clear and definite.
The purpose of the application is to provide a kind of electrolyte, including organic solvent, lithium salts and additive, described additive bag Include hydrogenation thiophene-boron trifluoride coordination compound and sultone compounds.
In above-mentioned electrolyte, in hydrogenation thiophene-boron trifluoride coordination compound, boron trifluoride is anion, hydrogenation Thiophene is cation, and whole hydrogenation thiophene-boron trifluoride coordination compound is electric neutrality.
In above-mentioned electrolyte, sultones can be saturated sultones, it is possible to for unsaturated sulfonic acid lactone.
At least one in the compound of structural formula as shown in formula I of hydrogenation thiophene-boron trifluoride coordination compound:
Wherein, R1, R2, R3, R4It is each independently selected from hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～20Alkane Base, substituted or unsubstituted C2～20Thiazolinyl, substituted or unsubstituted C6～26Aryl,；
Substituent group is selected from halogen, cyano group.
Halogen in the application is selected from F, Cl, Br, and preferably F, Cl.
In above-mentioned formula I, substituent group is as described below.
Carbon number is the alkyl of 1～20, and alkyl can be chain-like alkyl, it is possible to for cycloalkyl, be positioned on the ring of cycloalkyl Hydrogen can be replaced by alkyl, in described alkyl, the preferred lower limit of carbon number is 2,3,4,5, preferred higher limit is 3,4,5, 6,8,10,12,14,16,18.Preferably, the alkyl selecting carbon number to be 1～10, it is further preferred that select carbon number Being the chain-like alkyl of 1～6, carbon number is the cycloalkyl of 3～8, it is further preferred that the chain selecting carbon number to be 1～4 Shape alkyl, carbon number is the cycloalkyl of 5～7.As the example of alkyl, specifically can enumerate: methyl, ethyl, n-pro-pyl, different Propyl group, normal-butyl, isobutyl group, sec-butyl, the tert-butyl group, n-pentyl, isopentyl, neopentyl, cyclopenta, cyclohexyl.
Carbon number is the thiazolinyl of 2～20, can be cyclic alkenyl radical, it is possible to for chain thiazolinyl.It addition, in thiazolinyl double bond Number is preferably 1.In described thiazolinyl, the preferred lower limit of carbon number is 3,4,5, and preferred higher limit is 3,4,5,6,8,10, 12,14,16,18.Preferably, the thiazolinyl selecting carbon number to be 2～10, it is further preferred that selecting carbon number is 2～6 Thiazolinyl, it is further preferred that selecting carbon number is the thiazolinyl of 2～5.As the example of thiazolinyl, specifically can enumerate: second Thiazolinyl, pi-allyl, isopropenyl, pentenyl, cyclohexenyl group, cycloheptenyl, cyclo-octene base.
Carbon number is the aryl of 6～26, such as phenyl, benzene alkyl, at least contain a phenyl aryl such as xenyl, Condensed-nuclei aromatics base such as naphthalene, anthracene, phenanthrene, xenyl and condensed-nuclei aromatics base also can be replaced by alkyl or thiazolinyl.Preferably, choosing Select the aryl that carbon number is 6～16, it is further preferred that the aryl selecting carbon number to be 6～14, the most preferably Ground, the aryl selecting carbon number to be 6～9.As the example of aryl, specifically can enumerate: phenyl, benzyl, xenyl, to first Phenyl, o-tolyl, a tolyl.
When the thiazolinyl that the alkyl that the carbon number being previously mentioned is 1～20, carbon number are 2～20, carbon number be 6～ The aryl of 26, replaced by halogen atom after, form haloalkyl that carbon number is 1～20 the most accordingly, carbon number be 2～ The haloalkenyl group of 20, carbon number be 6～26 halogenated aryl, wherein halogen atom is F, Cl, Br, preferably F, Cl.In institute's shape In the halo group become, halogen atom to part hydrogen atom or all hydrogen atom replace, the number of halogen atom can be 1,2 Individual, 3 or 4.
Preferably, select carbon number be 1～10 haloalkyl, carbon number be 2～10 haloalkenyl group, carbon atom Number is the halogenated aryl of 6～16；It is further preferred that the halo chain-like alkyl selecting carbon number to be 1～6, carbon number are 3 ～the halogenated aryl that haloalkenyl group that the halogenated cycloalkyl of 8, carbon number are 2～6, carbon number are 6～14；The most excellent Selection of land, select carbon number be 1～4 halo chain-like alkyl, carbon number be 5～7 halogenated cycloalkyl, carbon number be 2 ～the halogenated aryl that the haloalkenyl group of 5, carbon atom are 6～10.
As the example of halo group, specifically can enumerate: trifluoromethyl (-CF3), 2-fluoro ethyl, 3-fluorine n-pro-pyl, 2- Fluorine isopropyl, 4-fluorine normal-butyl, 3-fluorine sec-butyl, 5-fluorine n-pentyl, 4-fluorine isopentyl, 1-are fluoride-based, 3-fluorine pi-allyl, 6- Fluoro-4-hexenyl, adjacent fluorophenyl, to fluorophenyl, a fluorophenyl, 4-trifluoromethylphenyl, 2,6-difluoromethyl phenyl, the fluoro-1-of 2- Naphthyl.In above-mentioned concrete example, F can be replaced by Cl and/or Br.
As a kind of improvement of the application electrolyte, above-mentioned formula I substituent group is selected from: R1, R2, R3, R4It is each independently selected from Hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～12Alkyl, substituted or unsubstituted C1～12Thiazolinyl, replacement or unsubstituted C6～22Aryl.
As a kind of improvement of the application electrolyte, R1, R2, R3, R4It is each independently selected from hydrogen atom, halogen atom, cyanogen Base, substituted or unsubstituted C1～6Alkyl, substituted or unsubstituted phenyl.
As a kind of improvement of the application electrolyte, hydrogenation thiophene-boron trifluoride coordination compound is selected from as shown in formula I A At least one in the compound of structural formula；
Wherein, R3、R4It is each independently selected from hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～20Alkyl replaces Or unsubstituted phenyl；Substituent group is selected from halogen, cyano group.
As a kind of improvement of the application electrolyte, R3、R4It is each independently selected from hydrogen atom, halogen atom, cyano group, replacement Or unsubstituted C1～12Alkyl；Substituent group is selected from halogen, cyano group；
As a kind of improvement of the application electrolyte, R3、R4It is each independently selected from hydrogen atom, halogen atom, cyano group, replacement Or unsubstituted C1～6Alkyl；Substituent group is selected from halogen, cyano group.
As a kind of improvement of the application electrolyte, R3、R4It is each independently selected from hydrogen atom, fluorine atom.
As the example of hydrogenation thiophene-boron trifluoride coordination compound, specific as follows shown:
As a kind of improvement of the application electrolyte, hydrogenation thiophene-boron trifluoride coordination compound is also selected from:
In this application, the hydrogenation thiophene-boron trifluoride coordination compound being previously mentioned can be according to the synthesis of existing routine Method synthesizes, such as, refer to document: CN200780033378.X.
Sultone compounds in the application is in following formula II, formula III, formula IV and the compound shown in formula V At least one:
In above-mentioned formula II, formula III, formula IV and formula V, R11、R12、R13、R14Be each independently selected from hydrogen atom, halogen atom, Nitro, cyano group, carboxyl, sulfonic group, substituted or unsubstituted C1～20Alkyl, substituted or unsubstituted C1～20Alkoxyl, replacement or Unsubstituted C2～20Thiazolinyl, substituted or unsubstituted C2～20Alkynyl, substituted or unsubstituted C1～20Alkane sulfonyl, replacement or do not take The C in generation2～20Alkene sulfonyl, substituted or unsubstituted C2～20Alkynes sulfonyl；
Wherein, substituent group is selected from halogen, cyano group, nitro, carboxyl or sulfonic group；Halogen is F, Cl, Br, preferably F, Cl.
As a kind of improvement of the application electrolyte, R11、R12、R13、R14It is each independently selected from hydrogen atom, replacement or not Substituted C1～6Straight or branched alkyl, substituted or unsubstituted C1～6Straight or branched alkoxyl；Substituted or unsubstituted C5～7 Cycloalkyl, substituted or unsubstituted C2～6Thiazolinyl, substituted or unsubstituted C2～6Alkynyl；Substituent group is selected from halogen, cyano group.
As a kind of improvement of the application electrolyte, R11、R12、R13、R14It is each independently selected from hydrogen atom, replacement or not Substituted C1～3Straight or branched alkyl, substituted or unsubstituted C1～3Straight or branched alkoxyl；Substituted or unsubstituted C5～6 Cycloalkyl, substituted or unsubstituted C2～4Thiazolinyl, substituted or unsubstituted C2～4Alkynyl；Substituent group is selected from halogen, cyano group.
In above-mentioned formula II, formula III, formula IV and formula V, substituent group is as described below.
Carbon number is the alkyl of 1～20, can be chain-like alkyl, it is possible to for cycloalkyl, be positioned at the ring hydrogen of cycloalkyl Can be replaced by alkyl.In described alkyl, the preferred lower limit of carbon number is 2,3,4,5, and preferred higher limit is 3,4,5,6,8, 10,12,14,16,18.Preferably, the alkyl selecting carbon number to be 1～10, it is further preferred that selecting carbon number is 1 ～the chain-like alkyl of 6, carbon number is the cycloalkyl of 3～8, it is further preferred that the chain selecting carbon number to be 1～4 Alkyl, carbon number is the cycloalkyl of 5～7.As the example of alkyl, specifically can enumerate: methyl, ethyl, n-pro-pyl, isopropyl Base, normal-butyl, isobutyl group, sec-butyl, the tert-butyl group, n-pentyl, isopentyl, cyclopenta, cyclohexyl.
Carbon number is the unsaturated alkyl of 2～20, can be alkenyl or alkynyl.Unsaturated bond in unsaturated alkyl Number is preferably 1, say, that in thiazolinyl, the denumerable of double bond is 1, and the number of three keys in alkynyl is alternatively 1.Described In unsaturated alkyl, the preferred lower limit of carbon number is 3,4,5, and preferred higher limit is 3,4,5,6,8,10,12,14,16, 18.Preferably, the thiazolinyl, the carbon number that select carbon number to be 2～10 are the alkynyl of 2～10, it is further preferred that select carbon The alkynyl that thiazolinyl that atomic number is 2～6, carbon number are 2～6, it is further preferred that the alkene selecting carbon number to be 2～5 Base, carbon number are the alkynyl of 2～5.
As the example of unsaturated alkyl, specifically can enumerate: vinyl, pi-allyl, isopropenyl, pentenyl, hexamethylene Thiazolinyl, cycloheptenyl, cyclo-octene base, propinyl, 2-propynyl, 2-butyne base, 3-butynyl, 3-methyl isophthalic acid-propinyl, 2-first Base-3-propinyl, pentynyl, 1-hexin base, 3-methyl isophthalic acid-butynyl, 3,3-dimethyl-ethyl acetylene base, heptynyl, octyne Base.
When in the alkyl that the aforementioned carbon number being previously mentioned is 1～20 containing oxygen atom time, can be carbon number be 1～20 Alkoxyl or saturated fat ether that carbon number is 2～20.Preferably, alkoxyl, the carbon selecting carbon number to be 1～10 Atomic number is the saturated fat ether of 1～10, it is further preferred that the alkoxyl, the carbon number that select carbon number to be 1～6 It is the saturated fat ether of 1～6, it is further preferred that the alkoxyl selecting carbon number to be 1～4, carbon number are 1～4 Saturated fat ether.As the example of oxy radical, specifically can enumerate: methoxyl group, ethyoxyl, positive propoxy, isopropyl oxygen Base, n-butoxy, sec-butoxy, tert-butoxy, n-pentyloxy, isoamoxy, cyclopentyloxy, cyclohexyloxy, methoxy, Ethoxyethyl group, isopropoxy normal-butyl.
After the alkyl that the carbon number being previously mentioned is 1～20 is replaced by halogen atom, the corresponding carbon number that formed is 1 ～the haloalkyl of 20, wherein halogen atom is F, Cl, Br.In the halo group formed, halogen atom to part hydrogen atom or The whole hydrogen atom of person replaces, and such as, the number of halogen atom can be 1,2,3 or 4.
Preferably, the haloalkyl selecting carbon number to be 1～10, it is further preferred that selecting carbon number is 1～6 Halo chain-like alkyl, carbon number be the halogenated cycloalkyl of 3～8, it is further preferred that selecting carbon number is 1～4 Halo chain-like alkyl, carbon number are the halogenated cycloalkyl of 5～7.As the example of haloalkyl, specifically can enumerate: trifluoro Methyl (-CF3), 2-fluoro ethyl, 3-fluorine n-pro-pyl, 2-fluorine isopropyl, 4-fluorine normal-butyl, 3-fluorine sec-butyl, 5-fluorine n-pentyl, 4- Fluorine isopentyl, 1-fluorine cyclopenta, 1-fluoro-3-methylcyclohexyl, wherein F can be replaced by Cl and/or Br.
After the alkyl that the carbon number being previously mentioned is 1～20 is replaced by cyano group, corresponding formed carbon number be 2～ The alkane cyano group of 21, wherein cyano group can to the part hydrogen atom in abovementioned alkyl or all hydrogen atom replace, cyano group Number is preferably 1.
Preferably, the alkane cyano group selecting carbon number to be 2～10, it is further preferred that selecting carbon number is 2～6 Chain alkane cyano group, carbon number are the cycloalkanes cyano group of 4～8, it is further preferred that the chain alkane selecting carbon number to be 3～5 Cyano group, carbon number are the cycloalkanes cyano group of 4～7.As the example of the group containing cyano group, specifically can enumerate: cyanogen methyl, 2- Cyano ethyl, 3-cyano group n-pro-pyl, 2-cyanoisopropyl, 4-cyano group normal-butyl, 4-cyano group isopentyl, 6-cyano group n-hexyl, 3- Cyan cyclopentyl, 4-cyanogen methylcyclohexyl.
After the alkyl that the carbon number being previously mentioned is 1～20 is replaced by nitro, carboxyl or sulfonic group, formed accordingly 4-nitro alkyl, carboxyalkyl, sulfonic group alkyl, wherein nitro, carboxyl or sulfonic group are to part hydrogen atom or whole hydrogen atom Replacing, such as, substituted number can be 1,2,3 or 4.After alkyl is replaced by above-mentioned group, can be formed as follows Group: nitre methyl, 2-nitro-ethyl, 3-nitro n-pro-pyl, 2-nitro isopropyl, 4-nitro normal-butyl, 4-nitro isopentyl, 6- Nitro n-hexyl, 3-nitro cyclopenta, 4-nitre methylcyclohexyl etc., in the example enumerated, nitro can be by carboxyl or sulfonic group Replaced.
As a kind of improvement of the application electrolyte, shown in the example table specific as follows 1 of sultones:
Table 1
In above-mentioned electrolyte, the gross weight that content is electrolyte of hydrogenation thiophene-boron trifluoride coordination compound 0.05%～10%, preferably the 0.1%～4% of the gross weight of electrolyte；The content of sultone compounds is electrolyte The 1%～5% of the 0.1%～10% of gross weight, the preferably gross weight of electrolyte.
If the content hydrogenating thiophene-boron trifluoride coordination compound in electrolyte is excessive, then can be in positive and negative plate surface shape Become the thicker and passivating film of densification, reduce the conductive performance of lithium ion, thus deteriorate lithium ion battery at ambient and elevated temperatures Cycle performance and high-temperature storage performance；And the content of sultone compounds is excessive, also can be formed very on negative plate surface Thick and stable passivating film, again such that the impedance of negative plate is greatly increased, reduces the conductive performance of lithium ion, thus dislikes Change lithium ion battery cycle performance at ambient and elevated temperatures and high-temperature storage performance.
In above-mentioned electrolyte, described organic solvent can be non-aqueous organic solvent, described organic solvent be carbon number be 1 ～8 and containing the compound of at least one ester group.
As the example of organic solvent, can enumerate: ethylene carbonate, Allyl carbonate, butylene, fluoro ethylene Alkene ester, Ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, 1,4-fourth At least one in lactone, methyl propionate, methyl butyrate, ethyl acetate, ethyl propionate, propyl propionate, ethyl n-butyrate..
In above-mentioned electrolyte, lithium salts can be organic lithium salt, it is possible to for inorganic lithium salt, specifically, can contain in lithium salts At least one in fluorine element, boron element, P elements.Preferably, lithium salts is selected from lithium hexafluoro phosphate (LiPF6), LiBF4 (LiBF4), lithium perchlorate (LiClO4), hexafluoroarsenate lithium (LiAsF6), tetrafluoro oxalic acid lithium phosphate (LiTFOP), LiN (SO2RF)2、 LiN(SO2F)(SO2RF), double trifluoromethanesulfonimide lithium LiN (CF3SO2)2(being abbreviated as LiTFSI), double (fluorine sulphonyl) imines Lithium Li (N (SO2F)2) (being abbreviated as LiFSI), di-oxalate lithium borate LiB (C2O4)2(being abbreviated as LiBOB), difluorine oxalic acid boracic acid lithium LiBF2(C2O4) at least one in (being abbreviated as LiDFOB), wherein, substituent RF=CnF2n+1Saturated perfluoroalkyl, n is 1 ～the integer of 10, and the integer that 2n+1 is more than zero.Particularly preferably LiPF6And/or LiN (SO2RF)2。
Preferably, lithium salts concentration in the electrolytic solution is 0.5M～2M (M=mol L-1)。
In this application, the preparation method of electrolyte selects conventional method, such as can be by organic solvent, lithium salts with add Add agent mix homogeneously.
The another object of the application there are provided lithium ion battery, and lithium ion battery includes electrolyte, lives containing positive pole The property positive plate of material, the negative plate containing negative active core-shell material and isolating membrane.
In above-mentioned lithium ion battery, positive plate also includes binding agent and conductive agent, will include positive electrode active materials, glue The anode sizing agent of knot agent and conductive agent is coated on plus plate current-collecting body, treats that anode sizing agent obtains positive plate after drying.Same, will The cathode size including negative active core-shell material, binding agent and conductive agent is coated on negative current collector, treats that cathode size is dried Rear acquisition negative plate.
Preferably, positive electrode active materials is selected from cobalt acid lithium LiCoO2, cobalt nickel lithium manganate ternary material, LiFePO 4, manganese Acid lithium (LiMnO2The mixture of at least one in), such as cobalt acid lithium and lithium-nickel-manganese-cobalt ternary material can be as positive-active material Material.As the example of cobalt nickel lithium manganate ternary material, specifically can enumerate: LiNi1/3Co1/3Mn1/3O2、 LiNi0.5Co0.2Mn0.3O2、LiNi0.6Co0.2Mn0.2O2。
Preferably, negative active core-shell material is material with carbon element and/or silicon materials.
In above-mentioned lithium ion battery, the concrete kind of lithium battery diaphragm is not exposed to concrete restriction, can be existing Any diaphragm material used in lithium ion battery, such as polyethylene, polypropylene, Kynoar and their MULTILAYER COMPOSITE Film, but it is not limited only to these.
Embodiment
The application is further described below by way of instantiation.But these examples are the most exemplary, not to this The protection domain of application constitutes any restriction.
In following embodiment, comparative example and test example, reagent, material and the instrument used is as the most special Explanation, be conventional reagent, conventional material and conventional instrument, the most commercially available, wherein involved reagent also can lead to Cross conventional synthesis process synthesis to obtain.
In following embodiment, comparative example and test example, used reagent is as follows:
Additive:
Hydrogenation thiophene-boron trifluoride coordination compound: compound 1～compound 3；
Sultone compounds: the sultones 12 (1,3-propene sultone is called for short PST) mentioned in aforementioned table 1.
Lithium salts: lithium hexafluoro phosphate (LiPF6)。
Organic solvent: ethylene carbonate (EC), Ethyl methyl carbonate (EMC).
Positive electrode active materials: cobalt nickel lithium manganate ternary material: LiNi1/3Co1/3Mn1/3O2LiNi0.5Co0.2Mn0.3O2、 LiNi0.6Co0.2Mn0.2O2、LiNi0.8Co0.1Mn0.1O2Deng.
Isolating membrane: using PE porous polymer film as isolating membrane.
Embodiment 1: the preparation of lithium ion battery (following be all called for short battery) 1～29
Battery 1～29 is prepared the most by the following method:
(1) prepared by negative plate
Negative electrode active material graphite, conductive agent acetylene black, binding agent butadiene-styrene rubber, thickening agent sodium carboxymethyl cellulose are pressed It is graphite according to weight ratio: acetylene black: butadiene-styrene rubber: sodium carboxymethyl cellulose=95:2:2:1 mixes, adds deionized water After, it is thoroughly mixed, forms uniform cathode size；This slurry is coated on negative current collector Copper Foil, then dry, cold Pressure, obtains negative plate.
(2) prepared by positive plate
By positive electrode active materials lithium-nickel-manganese-cobalt ternary material, conductive agent acetylene black, binding agent polyvinylidene fluoride by weight Ratio is lithium-nickel-manganese-cobalt ternary material: acetylene black: polyvinylidene fluoride=96:2:2 mixes, and adds Solvents N-methyl pyrrolidine Ketone, after being thoroughly mixed, forms uniform anode sizing agent；This slurry is coated on plus plate current-collecting body aluminium foil, then dry, Cold pressing, obtain positive plate.
(3) prepared by electrolyte
Electrolyte 1～29 is prepared the most by the following method:
< in the argon gas atmosphere glove box of 10ppm, it is that EC:EMC=3:7 is carried out by EC, EMC according to weight ratio in water content After mixing, obtain mixed solvent, then the lithium salts LiPF that will be fully dried6It is dissolved in above-mentioned mixed solvent, adds the most wherein Enter to hydrogenate thiophene-boron trifluoride coordination compound and sultone compounds, after stirring, it is thus achieved that electrolyte, wherein LiPF6 Concentration be 1mol/L.
(4) preparation of battery
Battery 1～29 prepares the most by the following method:
Positive plate, isolating membrane, negative plate are folded in order, makes isolating membrane be between positive/negative plate to play the work of isolation With, then winding obtains naked battery core；Naked battery core is placed in outer package paper tinsel, the above-mentioned electrolyte prepared is injected into after drying Battery in, be then passed through Vacuum Package, stand, be melted into, the operation such as shaping, it is thus achieved that battery.
Above-mentioned prepare battery during, used in electrolyte selected in each battery, each electrolyte The hydrogenation kind of thiophene-boron trifluoride coordination compound and content thereof and the kind of sultone compounds and content thereof, as follows State shown in table 2.
In table 2 below, the content of hydrogenation thiophene-boron trifluoride coordination compound and the content of sultone compounds It is the calculated percetage by weight of gross weight based on electrolyte.
Table 2
Comparative example: lithium ion battery (following be all called for short battery) 1#～17#Preparation
Battery 1#～17#It is prepared the most by the following method:
Repeat the preparation of battery 1 in embodiment 1, wherein in the preparation of electrolyte, change hydrogenation thiophene-boron trifluoride and join The position kind of compound, content, and/or change the kind of sultone compounds, content, remaining condition is the most constant.
Above-mentioned prepare battery during, used in electrolyte selected in each battery, each electrolyte The hydrogenation kind of thiophene-boron trifluoride coordination compound and content thereof and the kind of sultone compounds and content thereof, as follows State shown in table 3.
In Table 3 below, the content of hydrogenation thiophene-boron trifluoride coordination compound and the content of sultone compounds It is the calculated percetage by weight of gross weight based on electrolyte.
Table 3
Note: in table 3, "-" represents and is not added with any kind of material.
Test case
(1) the high-temperature storage performance test of battery
The high-temperature storage performance of battery is characterized with the volume change before and after battery storage.
The battery prepared in embodiment and comparative example all carries out following test:
At 25 DEG C, first with the constant current of 0.5C, battery is charged to 4.6V, further with 4.6V constant-potential charge It is 0.025C to electric current, then with drainage, battery is recorded in deionized water the initial volume of battery, by battery now Initial volume as the volume before battery storage, then battery is placed at 85 DEG C storage 6h, after end to be stored, test electricity Pond volume after storage at high temperatures, then calculates the volume change of battery by following formula.It addition, test result such as following table Shown in 4.
The volume change (%) of battery=[volume before volume/battery storage after battery high-temperature storage] × 100%
(2) the normal-temperature circulating performance test of battery
The battery prepared in embodiment and comparative example all carries out following test:
At 25 DEG C, first with the constant current of 1C, battery is charged to 4.6V, further with 4.6V constant-potential charge extremely Electric current is 0.025C, then with the constant current of 1C by battery discharge to 3.0V, this is a charge and discharge cycles process, this Discharge capacity is the discharge capacity of the 1st circulation.Battery carries out repeatedly cycle charge discharge electrical testing in a manner described, and detection obtains the The discharge capacity of 100 circulations, and the circulation volume conservation rate of battery is calculated by following formula.It addition, test result is as follows Shown in table 4.
Capability retention (%) after 100 circulations of battery=[putting of the discharge capacity/1st time circulation of the 100th circulation Capacitance] × 100%
(3) the high temperature cyclic performance test of battery
The battery prepared in embodiment and comparative example all carries out following test:
At 45 DEG C, first with the constant current of 1C, lithium rechargeable battery is charged to 4.6V, constant with 4.6V further It is 0.025C that voltage charges to electric current, then with the constant current of 1C by battery discharge to 3.0V, this is a charge and discharge cycles Process, this discharge capacity is the discharge capacity of the 1st circulation.Battery carries out repeatedly cycle charge discharge electrical measurement in a manner described Examination, detection is obtained the discharge capacity of the 100th circulation, and is calculated the capability retention after the circulation of battery by following formula. It addition, test result is as shown in Table 4 below.
Capability retention (%) after 100 circulations of battery=[putting of the discharge capacity/1st time circulation of the 100th circulation Capacitance] × 100%
Table 4
Related data from above-mentioned table 4, analyzes as follows:
(1) test result analysis of high-temperature storage performance
The volume change obtained by battery 1～30 and battery 1#In the contrast of the volume change obtained it can be seen that Add hydrogenation thiophene-boron trifluoride coordination compound and sultone compounds in the electrolytic solution, it is possible to battery is had relatively Low volume change.
By battery 1#～8#The volume change that obtains is it is known that electrolyte 1#In do not add any additive so that Positive pole has the strongest oxidisability, the organic solvent in meeting oxidation electrolyte under high-voltage state, is easily caused battery producing gas, The volume change making battery is too high.
Due at battery 4#, battery 5#With battery 7#In, hydrogenation thiophene-boron trifluoride coordination compound and/or sultones Very little, the passivating film formed can not have the feature of compactness and stability concurrently to the weight percentage of compound, also cannot have Effect ground stops the side reaction between active substance and electrolyte, makes the volume change after battery storage too high.
In battery 1～8, the content of sultone compounds is 2%, and adding content is 0.05%～10% nitrogen-containing hetero Ring-boron trifluoride coordination compound, can form composite passivation film densification, stable, stop between active substance and electrolyte Side reaction, make battery have relatively low volume change after storage at high temperatures, and along with hydrogenation thiophene-boron trifluoride coordinationization The increase of compound content, after battery stores 6h at 85 DEG C, has relatively low volume change.
In battery 9～14, the content of hydrogenation thiophene-boron trifluoride coordination compound is 2%, and adding content is 0.5% ～the sultone compounds of 10%, composite passivation film densification, stable can be formed, stop between active substance and electrolyte Side reaction, make battery have relatively low volume change, and the increasing of the content with sultone compounds after storage at high temperatures Add, after battery stores 6h at 85 DEG C, there is relatively low volume change.Same, the volume of battery 15～30 gained is become Rate is analyzed, and has analysis result same as described above.
(2) test result analysis of cycle performance
Capability retention after the circulation obtained by battery 1～30 and battery 1#Capability retention after the circulation obtained can To find out, containing hydrogenation thiophene-boron trifluoride coordination compound and sultone compounds in electrolyte, battery has higher Capability retention, battery has the cycle performance of excellence under high temperature and room temperature.
By battery 1#～17#Capability retention after the circulation obtained is it is known that electrolyte 1#In do not add any adding Add agent so that organic solvent can produce more side reaction in pole piece, and the capability retention causing battery is low.
At battery 2#With battery 3#In, in respective electrolyte, add hydrogenation thiophene-boron trifluoride ligand compound respectively Thing, sultone compounds, owing to the passivating film formed can't stop the pair between active substance and electrolyte effectively Reaction so that the cycle performance of battery substantially can not get improve.
Due at battery 4#, battery 5#With battery 7#In, hydrogenation thiophene-boron trifluoride coordination compound and/or sultones Very little, the composite passivation film formed can not have the feature of compactness and stability concurrently to the weight percentage of compound, it is impossible to Effectively stop the side reaction between active substance and electrolyte, make battery cycle performance under high temperature and room temperature can not get having The improvement of effect.
At battery 6#With battery 8#In, hydrogenation thiophene-boron trifluoride coordination compound or sultone compounds content mistake Many, too much hydrogenation thiophene-boron trifluoride coordination compound and sultone compounds remain in the electrolytic solution, continue at pole piece Surface is reacted, and causes interface impedance to become big, deteriorates battery cycle performance under high temperature and room temperature.
In battery 1～8, the content of sultone compounds is 2%, and adding content is 0.05%～10% hydrogenation thiophene Fen-boron trifluoride coordination compound, can form composite passivation film densification, stable, stop between active substance and electrolyte Side reaction, make battery have higher capability retention after circulating under high temperature and room temperature.
In battery 4 and battery 9～14, the content of hydrogenation thiophene-boron trifluoride coordination compound is 2%, and addition contains Amount is the sultone compounds of 0.5%～10%, can form densification, stable composite passivation film, stop active substance with Side reaction between electrolyte, makes battery have higher capability retention after circulating under high temperature and room temperature.Same, to electricity Capability retention after the circulation of pond 15～30 is analyzed, and has analysis result same as described above.
It can be seen that work as and electrolyte hydrogenates thiophene-boron trifluoride coordination compound and sulfonic acid simultaneously in from the above During lactone compound, improving the capability retention after battery circulates under high temperature and room temperature, battery has under high temperature and room temperature Excellent cycle performance.
In sum: in the electrolytic solution, when the content of hydrogenation thiophene-boron trifluoride coordination compound is too small or excessive, When sultone compounds content is too small or excessive, all can not be formed densification, stable, interface performance is the most composite passivated Film, it is impossible to simultaneously obtain the battery of good cycle under high temperature and room temperature.When electrolyte contains the hydrogenation of 0.05%～10% Thiophene-boron trifluoride coordination compound and the sultone compounds of 0.5%～10%, especially contain 0.1%～4.0% Hydrogenation thiophene-boron trifluoride coordination compound and the sultone compounds of 1%～4%, battery following under high temperature and room temperature Ring performance and high-temperature storage performance are the most excellent.
Embodiment 2
Preparing electrolyte according to the method for embodiment 1, difference is that additive hydrogenates thiophene-boron trifluoride ligand compound Thing, the structural formula of sultone compounds and content are as shown in table 5:
Wherein, the sultones that the structural formula of sultone compounds is as shown in table 1, hydrogenation thiophene-boron trifluoride is joined Position compound, the content of sultone compounds are the calculated percetage by weight of gross weight based on electrolyte.
Table 5
The electrolyte 31～46 prepared is prepared lithium ion battery according to method in above-described embodiment, prepares The high-temperature storage performance of lithium ion battery, normal-temperature circulating performance, high temperature cyclic performance are similar to the aforementioned embodiment.
The announcement of book according to the above description, above-mentioned embodiment can also be carried out by the application those skilled in the art Suitable change and amendment.Therefore, the application is not limited to detailed description of the invention disclosed and described above, to the application's Some modifications and changes should also be as falling in the protection domain of claims hereof.

Claims (10)

1. an electrolyte, it is characterised in that include organic solvent, lithium salts and additive, described additive include hydrogenate thiophene- Boron trifluoride coordination compound and sultone compounds.
Electrolyte the most according to claim 1, it is characterised in that described hydrogenation thiophene-boron trifluoride coordination compound choosing At least one in the compound of structural formula shown in formula I freely:
Wherein, R1, R2, R3, R4It is each independently selected from hydrogen atom, halogen atom, cyano group, substituted or unsubstituted C1～20Alkyl, take Generation or unsubstituted C2～20Thiazolinyl, substituted or unsubstituted C6～26Aryl；
Substituent group is selected from halogen, cyano group.
Electrolyte the most according to claim 1, it is characterised in that described hydrogenation thiophene-boron trifluoride coordination compound choosing At least one in the compound of structural formula shown in Formulas I A freely；
Wherein, R3, R4It is each independently selected from hydrogen atom, halogen atom, the substituted or unsubstituted C of cyano group1～20Alkyl, replacement or not Substituted phenyl；Substituent group is selected from halogen, cyano group.
Electrolyte the most according to claim 1, it is characterised in that R3、R4It is each independently selected from hydrogen atom, fluorine atom.
Electrolyte the most according to claim 1, it is characterised in that described sultone compounds be selected from following formula II, At least one in formula III, formula IV and the compound shown in formula V:
Wherein, R11、R12、R13、R14Be each independently selected from hydrogen atom, halogen atom, nitro, cyano group, carboxyl, sulfonic group, replacement or Unsubstituted C1～20Alkyl, substituted or unsubstituted C1～20Alkoxyl, substituted or unsubstituted C2～20Thiazolinyl, replacement or unsubstituted C2～20Alkynyl, substituted or unsubstituted C1～20Alkane sulfonyl, substituted or unsubstituted C2～20Alkene sulfonyl, replacement or unsubstituted C2～20Alkynes sulfonyl；
Substituent group is selected from halogen, cyano group, nitro, carboxyl or sulfonic group.
Electrolyte the most according to claim 5, it is characterised in that R11、R12、R13、R14Be each independently selected from hydrogen atom, Substituted or unsubstituted C1～6Straight or branched alkyl, substituted or unsubstituted C1～6Straight or branched alkoxyl；Replace or do not take The C in generation5～7Cycloalkyl, substituted or unsubstituted C2～6Thiazolinyl, substituted or unsubstituted C2～6Alkynyl；
Substituent group is selected from halogen, cyano group.
Electrolyte the most according to claim 1, it is characterised in that described hydrogenation thiophene-boron trifluoride coordination compound Content is the 0.05%～10% of the gross weight of electrolyte；The content of described sultone compounds is the gross weight of electrolyte 0.1%～10%.
Electrolyte the most according to claim 1, it is characterised in that described organic solvent is selected from ethylene carbonate, carbonic acid third Alkene ester, butylene, fluorinated ethylene carbonate, Ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, carbon Acid first propyl ester, ethyl propyl carbonic acid ester, 1,4-butyrolactone, methyl propionate, methyl butyrate, ethyl acetate, ethyl propionate, propyl propionate with And at least one in ethyl n-butyrate..
Electrolyte the most according to claim 1, it is characterised in that
Described lithium salts be selected from lithium hexafluoro phosphate, LiBF4, lithium perchlorate, hexafluoroarsenate lithium, tetrafluoro oxalic acid lithium phosphate, LiN(SO2RF)2、LiN(SO2F)(SO2RF), double trifluoromethanesulfonimide lithium, double (fluorine sulphonyl) imine lithium, double oxalic acid boric acid At least one in lithium, difluorine oxalic acid boracic acid lithium, wherein, RF=-CnF2n+1, n is the integer of 1～10, preferably LiPF6、LiN (SO2RF)2In at least one；
It is furthermore preferred that the concentration that described lithium salts is in the electrolytic solution is 0.5mol L-1～2mol L-1。
10. a lithium ion battery, it is characterised in that include the positive plate containing positive electrode active materials, containing negative electrode active material The electrolyte according to any one of negative plate, isolating membrane and claim 1～9 expected.
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CN108400382A (en) * 2017-02-07 2018-08-14 宁德时代新能源科技股份有限公司 Electrolyte solution and secondary battery
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