CN105355976A - An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte - Google Patents
An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte Download PDFInfo
- Publication number
- CN105355976A CN105355976A CN201510780494.4A CN201510780494A CN105355976A CN 105355976 A CN105355976 A CN 105355976A CN 201510780494 A CN201510780494 A CN 201510780494A CN 105355976 A CN105355976 A CN 105355976A
- Authority
- CN
- China
- Prior art keywords
- electrolyte
- lithium
- carbonate
- propyl ester
- boronic acid
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Classifications
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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
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to the technical filed of lithium ion batteries and discloses an electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte. The electrolyte contains a conductive lithium salt, an organic solvent and the tripropylborate additive. The tripropylborate additive optimizes the cathode/electrolyte interface, reduces surface activity of the cathode, inhibits oxygenolysis of the electrolyte, and improves cycle performance and rate performance of a lithium ion battery having high voltage (4.8 V) and adopting a rich lithium material as the cathode.
Description
Technical field
The invention belongs to technical field of lithium ion, be specifically related to electrolyte of a kind of boronic acid containing three propyl ester additive and preparation method thereof and application.
Background technology
In existing commercialization secondary cell, the specific energy of lithium ion battery is the highest, cycle performance is best, and the diversity selected because of its electrode material, has vast potential for future development as energy-storage battery.At present, the positive electrode of business lithium ion battery mainly contains LiMn2O4, cobalt acid lithium, ternary material, LiFePO 4 are several, and its charge cutoff voltage is generally no more than 4.2V.Along with the progress of science and technology and the development in market, promote the energy density of lithium battery and day by day seem important and urgent.Therefore promote the use voltage of lithium ion battery thus improve the emphasis that the energy density of battery is research at present.
The 5V positive electrode of current discovery comprises: (1) has the manganese series oxides of spinel structure, as LiMn
2-xli
xo
4and LiMn
2-xm
xo
4deng; (2) there is the composite phosphate of olivine structural: LiMPO4 (M=Ni, Co) etc.; (3) there is the ternary metal hydrochlorate oxide LiMVO of inverse spinel structure
4(M=Cu, Ni, Mn) etc.(4) there is the ternary metal hydrochlorate oxide xLi of layer structure
2mnO
3(1-x) LiMO
2(0 < x < 1, M=Mn, Co, Ni) etc.Due to the ternary metal hydrochlorate oxide xLi of layer structure
2mnO
3(1-x) LiMO
2the theoretical capacity of (0 < x < 1, M=Mn, Co, Ni) can more than 250mAhg
-1, by one of important candidate's positive electrode becoming lithium ion battery of future generation.
But while raising positive electrode voltage, the electrical properties such as the charge and discharge cycles of battery are but in decline, and reason is that the rich lithium material structure of stratiform is stable not on the one hand, is then the matching problem of electrolyte on the other hand.Conventional commercial electrolyte liquid easily decomposes at anode surface oxidation under 5V high potential, and the oxidative decomposition of electrolyte self also can impel the pernicious reactions such as the change of positive electrode pattern, structure collapses simultaneously.Therefore must develop the high-tension electrolyte of a kind of ability 5V, and then realize the excellent performance of lithium battery performance, improve lithium battery cycle life.Improve the most economical method of the most convenient of performance of lithium ion battery by adding a small amount of electrolysis additive in the lithium-ion battery electrolytes of routine.
Summary of the invention
In order to solve the shortcoming and defect part of above prior art, primary and foremost purpose of the present invention is the electrolyte providing a kind of boronic acid containing three propyl ester additive.This electrolyte is by adding triproylborate, when being applied to lithium ion battery, optimizing positive pole/electrolyte interface, reducing the surface activity of positive pole, suppress the oxidation Decomposition of electrolyte, circulation and high rate performance that high voltage (4.8V) rich lithium is the lithium battery of positive electrode can be improved.
Another object of the present invention is to the preparation method of the electrolyte that a kind of above-mentioned boronic acid containing three propyl ester additive is provided.
Another object of the present invention is the application of electrolyte in lithium ion battery providing a kind of above-mentioned boronic acid containing three propyl ester additive.
The object of the invention is achieved through the following technical solutions:
An electrolyte for boronic acid containing three propyl ester additive, described electrolyte comprises electric conducting lithium salt, organic solvent and triproylborate additive, and described triproylborate additive has the structural formula shown in formula (1):
Preferably, described electric conducting lithium salt is selected from hexafluoro lithium borate (LiPF
6), LiBF4 (LiBF
4), dioxalic acid lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium (LiDFOB), trifluoromethyl sulfonic acid lithium (LiSO
3cF
3), lithium perchlorate (LiClO
4), hexafluoroarsenate lithium (LiAsF
6) and bis trifluoromethyl sulfimide lithium (Li (CF
3sO
2)
2n) one or more in.
Preferably, described organic solvent is by cyclic carbonate solvents and linear carbonate solvent composition; The mass ratio of cyclic carbonate solvents and linear carbonate solvent is 1:(1 ~ 3).
Described cyclic carbonate solvents is preferably ethylene carbonate (EC); The described preferred dimethyl carbonate of linear carbonate solvent (DMC), methyl ethyl carbonate (EMC), one or more in diethyl carbonate (DEC) and methyl propyl carbonate (MPC).
Preferably, described electric conducting lithium salt concentration is in the electrolytic solution 1.0mol/L.
Preferably, the content of described triproylborate additive is 1% ~ 3% of electrolyte total weight.
The preparation method of the electrolyte of above-mentioned boronic acid containing three propyl ester additive, comprises the steps:
(1) by organic solvent purifying removal of impurities, dewater;
(2) at ambient temperature, electric conducting lithium salt is added in the solvent that step (1) obtains, obtain general electrolytic liquid;
(3) add triproylborate additive in the general electrolytic liquid obtained in step (2), obtain described electrolyte.
Clarification described in step (1), dewater preferably by any one in molecular sieve, active carbon, calcium hydride, lithium hydride, anhydrous calcium oxide, calcium chloride, phosphorus pentoxide, alkali metal or alkaline-earth metal or two or morely to process.
Described molecular sieve can adopt
type,
type or
type, preferably
type or
type.
The application of electrolyte in lithium ion battery of above-mentioned boronic acid containing three propyl ester additive.
Electrolyte tool of the present invention has the following advantages and beneficial effect:
The present invention uses triproylborate as the high pressure film for additive of lithium-ion electrolyte, because such additive has lower oxidation and reduction potential, one deck densification, stable SEI film can be formed at positive pole and negative terminal surface in first charge-discharge process, optimize both positive and negative polarity skin covering of the surface, suppress the surface activity of electrode, thus suppress electrolyte to contact with the further of electrode active material, reduce the oxidation Decomposition of electrolyte bulk solvent at electrode surface.The cycle performance of lithium ion battery containing this electrolysis additive under 2 ~ 4.8V improves.
Accompanying drawing explanation
Fig. 1 is that the high-voltage electrolyte of the lithium ion battery that embodiment 1 prepares and general electrolytic liquid carry out discharge cycles the performance test results figure;
Fig. 2 is the high-voltage electrolyte of the lithium ion battery that embodiment 1 prepares and the multiplying power discharging property result figure of general electrolytic liquid.
Embodiment
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention are not limited thereto.
Embodiment 1
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, and adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt LiPF
6be dissolved in the solvent that step (1) obtains, final concentration is 1.0mol/L, stirs, and obtains general electrolytic liquid;
(3) add the triproylborate of 1% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high-voltage electrolyte for lithium ion battery.
The high-voltage electrolyte of the lithium ion battery that the present embodiment prepares and step (2) gained general electrolytic liquid carry out discharge cycles Performance comparision, and result as shown in Figure 1.As seen from Figure 1: the capability retention of 88.2% can also be kept after high-voltage electrolyte prepared by the present embodiment carries out 200 circles, and general electrolytic liquid can only keep the capability retention of 29.8% after carrying out 200 circles.As can be seen from the results, add the used for electrolyte of triproylborate in electrolyte and can improve its cycle performance under high voltages in lithium ion battery, have reasonable application prospect in high-voltage battery system.
The multiplying power discharging property result figure of the high-voltage electrolyte of the lithium ion battery that the present embodiment prepares and step (2) gained general electrolytic liquid as shown in Figure 2.As seen from Figure 2: high-voltage electrolyte prepared by the present embodiment, under multiplying power is 4C electric discharge, still 142.3mAhg is had
-1, general electrolytic liquid then only has 91.8mAhg
-1.As can be seen from the results, add the used for electrolyte of triproylborate in electrolyte and can improve its high rate performance under high voltages in lithium ion battery, have reasonable application prospect in high-voltage battery system.
Embodiment 2
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, and adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt LiPF
6be dissolved in the solvent that step (1) obtains, final concentration is 1.0mol/L, stirs, and is made into general electrolytic liquid;
(3) add the triproylborate of 2% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high voltage functionality electrolyte for lithium ion battery.
Embodiment 3
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt LiPF
6be dissolved in the solvent that step (1) obtains, final concentration is 1.0mol/L, stirs, and is made into general electrolytic liquid;
(3) add the triproylborate of 3% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high voltage functionality electrolyte for lithium ion battery.
Embodiment 4
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt LiAsF
6be dissolved in the solvent that step (1) obtains, final concentration is 1.0mol/L, stirs, and is made into general electrolytic liquid;
(3) add the triproylborate of 1% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high-voltage electrolyte for lithium ion battery.
Embodiment 5
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt Li (CF
3sO
2)
2n is dissolved in the solvent that step (1) obtains, and final concentration is 1.0mol/L, stirs, and is made into general electrolytic liquid;
(3) add the triproylborate of 1% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high-voltage electrolyte for lithium ion battery.
Embodiment 6
(1) by cyclic carbonate solvents ethylene carbonate (EC) and linear carbonate solvent methyl ethyl carbonate (EMC) and dimethyl carbonate (DMC) EC: EMC: DMC=3: 5: 2 mixing in mass ratio, adopt molecular sieve, calcium hydride, lithium hydride clarification, dewater;
(2) at ambient temperature, by electric conducting lithium salt LiSO
3cF
3be dissolved in the solvent that step (1) obtains, final concentration is 1.0mol/L, stirs, and is made into general electrolytic liquid;
(3) add the triproylborate of 1% of electrolyte quality in the general electrolytic liquid prepared in step (2), obtain the high-voltage electrolyte for lithium ion battery.
Above-described embodiment is the present invention's preferably execution mode; but embodiments of the present invention are not restricted to the described embodiments; change, the modification done under other any does not deviate from Spirit Essence of the present invention and principle, substitute, combine, simplify; all should be the substitute mode of equivalence, be included within protection scope of the present invention.
Claims (9)
1. an electrolyte for boronic acid containing three propyl ester additive, is characterized in that: described electrolyte comprises electric conducting lithium salt, organic solvent and triproylborate additive, and described triproylborate additive has the structural formula shown in formula (1):
2. the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 1, is characterized in that: described electric conducting lithium salt is one or more in hexafluoro lithium borate, LiBF4, dioxalic acid lithium borate, difluorine oxalic acid boracic acid lithium, trifluoromethyl sulfonic acid lithium, lithium perchlorate, hexafluoroarsenate lithium and bis trifluoromethyl sulfimide lithium.
3. the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 1, is characterized in that: described organic solvent is by cyclic carbonate solvents and linear carbonate solvent composition; The mass ratio of cyclic carbonate solvents and linear carbonate solvent is 1:(1 ~ 3).
4. the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 3, is characterized in that: described cyclic carbonate solvents refers to ethylene carbonate; Described linear carbonate solvent refers to dimethyl carbonate, methyl ethyl carbonate, one or more in diethyl carbonate and methyl propyl carbonate.
5. the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 1, is characterized in that: described electric conducting lithium salt concentration is in the electrolytic solution 1.0mol/L.
6. the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 1, is characterized in that: the content of described triproylborate additive is 1% ~ 3% of electrolyte total weight.
7. the preparation method of the electrolyte of the boronic acid containing three propyl ester additive described in any one of claim 1 ~ 6, is characterized in that comprising the steps:
(1) by organic solvent purifying removal of impurities, dewater;
(2) at ambient temperature, electric conducting lithium salt is added in the solvent that step (1) obtains, obtain general electrolytic liquid;
(3) add triproylborate additive in the general electrolytic liquid obtained in step (2), obtain described electrolyte.
8. the preparation method of the electrolyte of a kind of boronic acid containing three propyl ester additive according to claim 7, is characterized in that: the clarification described in step (1), dewatering refers to by any one in molecular sieve, active carbon, calcium hydride, lithium hydride, anhydrous calcium oxide, calcium chloride, phosphorus pentoxide, alkali metal or alkaline-earth metal or two or morely to process.
9. the application of electrolyte in lithium ion battery of the boronic acid containing three propyl ester additive described in any one of claim 1 ~ 6.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510780494.4A CN105355976A (en) | 2015-11-13 | 2015-11-13 | An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510780494.4A CN105355976A (en) | 2015-11-13 | 2015-11-13 | An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106099186A (en) * | 2016-07-12 | 2016-11-09 | 华南师范大学 | A kind of high pressure corrosion resistant erosion electrolyte and preparation method and application |
| CN109065952A (en) * | 2018-08-07 | 2018-12-21 | 常州大学 | A kind of high voltage functionality electrolyte and preparation method thereof |
| CN109565080A (en) * | 2016-07-25 | 2019-04-02 | 三星Sdi株式会社 | The additive of electrolyte for lithium battery, the electrolyte of lithium battery including the additive and the lithium battery using the electrolyte |
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| US20100143806A1 (en) * | 2007-07-04 | 2010-06-10 | Rainer Dietz | Method for producing low-acid lithium borate salts and mixtures of low-acid lithium borate salts and lithium hydride |
| CN102760906A (en) * | 2012-07-18 | 2012-10-31 | 珠海市赛纬电子材料有限公司 | Electrolyte additive, electrolyte comprising additive and lithium ion battery |
| CN103311571A (en) * | 2013-05-21 | 2013-09-18 | 东莞新能源科技有限公司 | Lithium ion secondary battery and electrolyte thereof |
| CN104885290A (en) * | 2013-01-28 | 2015-09-02 | 株式会社杰士汤浅国际 | Nonaqueous electrolyte rechargeable battery |
-
2015
- 2015-11-13 CN CN201510780494.4A patent/CN105355976A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20100143806A1 (en) * | 2007-07-04 | 2010-06-10 | Rainer Dietz | Method for producing low-acid lithium borate salts and mixtures of low-acid lithium borate salts and lithium hydride |
| CN102760906A (en) * | 2012-07-18 | 2012-10-31 | 珠海市赛纬电子材料有限公司 | Electrolyte additive, electrolyte comprising additive and lithium ion battery |
| CN104885290A (en) * | 2013-01-28 | 2015-09-02 | 株式会社杰士汤浅国际 | Nonaqueous electrolyte rechargeable battery |
| CN103311571A (en) * | 2013-05-21 | 2013-09-18 | 东莞新能源科技有限公司 | Lithium ion secondary battery and electrolyte thereof |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106099186A (en) * | 2016-07-12 | 2016-11-09 | 华南师范大学 | A kind of high pressure corrosion resistant erosion electrolyte and preparation method and application |
| CN109565080A (en) * | 2016-07-25 | 2019-04-02 | 三星Sdi株式会社 | The additive of electrolyte for lithium battery, the electrolyte of lithium battery including the additive and the lithium battery using the electrolyte |
| CN109065952A (en) * | 2018-08-07 | 2018-12-21 | 常州大学 | A kind of high voltage functionality electrolyte and preparation method thereof |
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Application publication date: 20160224 |
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