CN109065952A - A kind of high voltage functionality electrolyte and preparation method thereof - Google Patents

A kind of high voltage functionality electrolyte and preparation method thereof Download PDF

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Publication number
CN109065952A
CN109065952A CN201810889004.8A CN201810889004A CN109065952A CN 109065952 A CN109065952 A CN 109065952A CN 201810889004 A CN201810889004 A CN 201810889004A CN 109065952 A CN109065952 A CN 109065952A
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high voltage
solvent
mixture
electrolyte
voltage functionality
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任玉荣
汤长坤
丁建宁
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Changzhou University
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Changzhou University
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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
    • H01M10/058—Construction or manufacture
    • 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
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • H01M2300/0037—Mixture of solvents
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Secondary Cells (AREA)

Abstract

The present invention relates to this kind of high voltage functionality electrolyte and preparation method thereof, it includes the additive for being electrolysed mixture and being dissolved in the electrolysis mixture；The electrolysis mixture includes cyclic carbonate solvents, linear carbonates solvent and electric conducting lithium salt；The additive is triamylborate, and quality is the 0.5% ~ 5% of the electrolysis mixture quality.To inhibit further contacting for electrolyte and electrode active material, electrolyte bulk solvent is reduced in the oxygenolysis of electrode surface, so as to improve the cycle performance with lithium ion battery that cobalt acid lithium is anode at 3 ~ 4.5 V.

Description

A kind of high voltage functionality electrolyte and preparation method thereof
Technical field
The invention belongs to electrolyte fields, are related to a kind of high-voltage electrolyte, and in particular to a kind of high voltage functionality electrolyte and Preparation method.
Background technique
More stringent requirements are proposed for the specific capacity of Large-scale Mobile equipment or energy-accumulating power station to lithium ion battery, therefore high-energy Density lithium ion battery becomes research hotspot in recent years.Current commercial anode material for lithium-ion batteries has LiMn2O4, cobalt acid Lithium, LiFePO4 and ternary material etc. are several, but their charge cutoff voltage is generally no more than 4.2V, and with science and technology Progress and market continuous development, to the performance of lithium battery, more stringent requirements are proposed.
Cobalt acid lithium as a kind of successfully commercialization lithium electricity positive electrode because its structural instability and electrolyte restriction because Element can only show good cyclical stability under 4.2V charging voltage, but its reason can only be utilized under 4.2V charging voltage By the 50% of capacity.There is document report by improving the charging voltage of lithium battery to 4.5V, theoretical specific capacity will increase by 30%, but Cyclical stability is deteriorated, this is because cobalt acid lithium is unstable in 4.5V voltage flowering structure, and conventional electrolyte is in 4.5V Oxygenolysis can occur, and one layer of high impedance substance can be covered on the surface of the material as the cycle progresses, deteriorate following for battery Ring performance.Therefore, electrolyte has become one of the key factor for restricting lithium ion battery development.
Summary of the invention
A kind of high voltage functionality electrolyte is provided the invention aims to overcome the deficiencies in the prior art.
In order to achieve the above objectives, the technical solution adopted by the present invention is that: a kind of high voltage functionality electrolyte, it includes that electrolysis is mixed It closes object and is dissolved in the additive of the electrolysis mixture；The electrolysis mixture includes cyclic carbonate solvents, linear carbonic acid Ester solvent and electric conducting lithium salt；The additive be triamylborate, quality be it is described electrolysis mixture quality 0.5%~ 5%.
Optimally, the volume ratio of the cyclic carbonate solvents and the linear carbonates solvent is 1:1~2, described to lead Concentration of the electric lithium salts in the cyclic carbonate solvents and the linear carbonates solvent is 0.8~1.5mol/L.
Optimally, the electric conducting lithium salt is selected from LiPF6、LiBF4、LiBOB、LiDFOB、LiSO3CF3And LiC (CF3SO2)3One of or a variety of compositions mixture.
Optimally, the cyclic carbonate solvents are ethylene carbonate or/and propene carbonate, and the linear carbonates are molten Agent is the mixture selected from one of dimethyl carbonate, methyl ethyl carbonate and diethyl carbonate or a variety of compositions.
Another object of the present invention is to provide a kind of preparation method of above-mentioned high voltage functionality electrolyte, it includes following step It is rapid:
(a) clarification is carried out after mixing the cyclic carbonate solvents and the linear carbonates solvent, is removed water Mixed solvent；
(b) electric conducting lithium salt is dissolved in the in the mixed solvent, forms electrolysis mixture；
(c) additive is dissolved in the electrolysis mixture.
Optimally, in step (a), the clarification, water removal refer to through molecular sieve, active carbon, calcium hydride, hydrogenation One of lithium, anhydrous calcium oxide, calcium chloride phosphorus pentoxide, alkali and alkaline earth metal ions a variety of are handled.
Optimally, in step (b), the electric conducting lithium salt is dissolved in the in the mixed solvent at room temperature.
Due to the above technical solutions, the present invention has the following advantages over the prior art: high voltage functionality of the present invention Electrolyte has the triamylborate compared with low oxidation potential as functional additive, in head by adding into electrolysis mixture The electrode material surface that is formed to that SEI film is participated in secondary charge and discharge process forms one layer of fine and close protective film, and can press down The oxygenolysis of electrolyte processed, it is suppressed that the surface-active of electrode, to inhibit the further of electrolyte and electrode active material Contact reduces electrolyte bulk solvent in the oxygenolysis of electrode surface, so as to improve the lithium-ion electric for taking cobalt acid lithium as anode Cycle performance of the pond at 3~4.5V.
Detailed description of the invention
Fig. 1 is to be compared with the charge and discharge of 200 circle of lithium ion battery circulation of electrolyte production in embodiment 1 and comparative example 1 Figure；
Fig. 2 is resistance comparison diagram after 200 circle of lithium ion battery circulation with electrolyte production in embodiment 1 and comparative example 1.
Specific embodiment
High voltage functionality electrolyte of the present invention, it includes the additive for being electrolysed mixture and being dissolved in the electrolysis mixture； The electrolysis mixture includes cyclic carbonate solvents, linear carbonates solvent and electric conducting lithium salt；The additive is boric acid three Pentyl ester, quality are the 0.5%~5% of the electrolysis mixture quality.Have by being added into electrolysis mixture compared with hypoxemia Change the triamylborate of current potential as functional additive, SEI film is participated in during first charge-discharge is formed to electrode material Expect that surface forms one layer of fine and close protective film, and the oxygenolysis of electrolyte can be inhibited, it is suppressed that the surface-active of electrode, To inhibit further contacting for electrolyte and electrode active material, electrolyte bulk solvent is reduced in the oxidation point of electrode surface Solution, so as to improve being cycle performance of the positive lithium ion battery at 3~4.5V with cobalt acid lithium.
The volume ratio of the cyclic carbonate solvents and the linear carbonates solvent is preferably 1:1~2, and electric conducting lithium salt Concentration in the cyclic carbonate solvents and the linear carbonates solvent is preferably 0.8~1.5mol/L.The conduction Lithium salts is selected from LiPF6、LiBF4、LiBOB、LiDFOB、LiSO3CF3With LiC (CF3SO2)3One of or a variety of compositions it is mixed Object is closed, wherein LiPF6It is best with the matching of triamylborate.Above-mentioned cyclic carbonate solvents and linear carbonates solvent use Existing conventional, if cyclic carbonate solvents are ethylene carbonate or/and propene carbonate, and linear carbonates solvent is Mixture selected from one of dimethyl carbonate, methyl ethyl carbonate and diethyl carbonate or a variety of compositions.Above-mentioned high voltage functionality The preparation method of electrolyte, it is the following steps are included: (a) mixes the cyclic carbonate solvents and the linear carbonates solvent Clarification is carried out after conjunction, removes water to obtain mixed solvent；(b) electric conducting lithium salt is dissolved in the in the mixed solvent, forms electrolysis Mixture；(c) additive is dissolved in the electrolysis mixture.In step (a), the clarification, water removal are excellent Gate over-molecular sieve, active carbon, calcium hydride, lithium hydride, anhydrous calcium oxide, calcium chloride phosphorus pentoxide, alkali metal and alkaline earth gold One of belong to or a variety of is handled.In step (b), the electric conducting lithium salt is dissolved in the mixed solvent at room temperature In.
The preferred embodiment of the invention is described in detail below in conjunction with attached drawing:
Embodiment 1
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it the following steps are included:
(a) by cyclic carbonate vinyl acetate (EC) and diethyl carbonate (DEC), 1:1 mixes to obtain mixed solvent by volume, according to It is secondary that clarification, water removal are carried out using molecular sieve, calcium hydride and lithium hydride；
(b) at room temperature, electric conducting lithium salt (LiPF6) is dissolved in the in the mixed solvent (ultimate density 1.0mol/ L), electrolysis mixture is stirred evenly to obtain；
(c) triamylborate that its quality 0.5% is added into electrolysis mixture, obtains the high pressure for lithium ion battery Electrolyte.
Embodiment 2
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (c), the triamylborate of its quality 1% is added into electrolysis mixture.
Embodiment 3
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (c), the triamylborate of its quality 2% is added into electrolysis mixture.
Embodiment 4
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (c), the triamylborate of its quality 4% is added into electrolysis mixture.
Embodiment 5
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (c), the triamylborate of its quality 5% is added into electrolysis mixture.
Embodiment 6
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (b), the electric conducting lithium salt used is LiBF4。
Embodiment 7
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (b), the electric conducting lithium salt used is LiBOB.
Embodiment 8
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (b), the electric conducting lithium salt used is LiDFOB.
Embodiment 9
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (b), the electric conducting lithium salt used is LiSO3CF3。
Embodiment 10
The present embodiment provides a kind of preparation method of high voltage functionality electrolyte, it and it is almost the same in embodiment 1, it is different : in step (b), the electric conducting lithium salt used is LiC (CF3SO2)3。
Comparative example 1
This example provides a kind of preparation method of electrolyte, it with it is almost the same in embodiment 1, unlike: do not carry out Step (c).
Comparative example 2
This example provides a kind of preparation method of electrolyte, it with it is almost the same in embodiment 1, unlike: step (c) In, it is fluorine material using conventional fluorinated ethylene carbonate functional additive, it is unfriendly to environment.
It is negative with positive plate made of electrolyte obtained in embodiment 1-10, comparative example 1-2 and cobalt acid lithium, lithium metal respectively Pole and diaphragm are assembled into lithium ion battery (existing conventional assembling process).Then to each lithium ion battery obtained above into Row electro-chemical test, the result is shown in tables 1.As shown in Figure 1, after triamylborate being added in electrolyte, anode is made with cobalt acid lithium The cyclical stability of lithium ion battery under high pressure is improved；As shown in Figure 2, after triamylborate being added in electrolyte, Become smaller (the chemical property parameter of specific lithium ion battery is shown in Table 1) with the resistance that cobalt acid lithium makees the lithium ion battery of anode.
Also by electrolyte and LiNi obtained in embodiment 1, comparative example 11Co1Mn1O2Manufactured positive plate, lithium metal are negative Pole and diaphragm are assembled into lithium ion battery, and performance is embodiment 1LiNi after 200 circulations1Co1Mn1O2/ Li half-cell capacity Conservation rate is 72%, and 1 capacity retention ratio of comparative example is only 24%, it is seen that the suitability of the electrolyte and cobalt acid lithium is more excellent.
The performance of lithium ion battery table that electrolyte is assembled into 1 embodiment 1-10 of table, comparative example 1-2
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 cans understand the content of the present invention and implement it accordingly, and it is not intended to limit the scope of the present invention, it is all according to the present invention Equivalent change or modification made by Spirit Essence, should be covered by the protection scope of the present invention.

Claims (7)

1. a kind of high voltage functionality electrolyte, it is characterised in that: it includes electrolysis mixture and is dissolved in the electrolysis mixture Additive；The electrolysis mixture includes cyclic carbonate solvents, linear carbonates solvent and electric conducting lithium salt；The additive is Triamylborate, quality are the 0.5% ~ 5% of the electrolysis mixture quality.
2. high voltage functionality electrolyte according to claim 1, it is characterised in that: the cyclic carbonate solvents and the line Property carbonate solvent volume ratio be 1:1 ~ 2, the electric conducting lithium salt is in the cyclic carbonate solvents and the linear carbonates Concentration in solvent is 0.8 ~ 1.5mol/L.
3. high voltage functionality electrolyte according to claim 1, it is characterised in that: the electric conducting lithium salt is selected from LiPF6、 LiBF4、LiBOB、LiDFOB、LiSO3CF3With LiC (CF3SO2)3One of or a variety of compositions mixture.
4. high voltage functionality electrolyte according to claim 1, it is characterised in that: the cyclic carbonate solvents are carbonic acid second Enester or/and propene carbonate, the linear carbonates solvent are selected from dimethyl carbonate, methyl ethyl carbonate and diethyl carbonate One of or a variety of compositions mixture.
5. the preparation method of any high voltage functionality electrolyte in Claims 1-4, which is characterized in that it includes following step It is rapid:
(a) clarification is carried out after mixing the cyclic carbonate solvents and the linear carbonates solvent, removes water to obtain mixing Solvent；
(b) electric conducting lithium salt is dissolved in the in the mixed solvent, forms electrolysis mixture；
(c) additive is dissolved in the electrolysis mixture.
6. the preparation method of high voltage functionality electrolyte according to claim 5, it is characterised in that: in step (a), the purifying Removal of impurities, water removal refer to through molecular sieve, active carbon, calcium hydride, lithium hydride, anhydrous calcium oxide, calcium chloride phosphorus pentoxide, alkali gold Belong to and one of alkaline-earth metal or a variety of is handled.
7. the preparation method of high voltage functionality electrolyte according to claim 5, it is characterised in that: in step (b), in room temperature item The electric conducting lithium salt is dissolved in the in the mixed solvent under part.
CN201810889004.8A 2018-08-07 2018-08-07 A kind of high voltage functionality electrolyte and preparation method thereof Pending CN109065952A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112751079A (en) * 2019-10-31 2021-05-04 苏州微木智能系统有限公司 Lithium ion battery

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CN105355976A (en) * 2015-11-13 2016-02-24 华南师范大学 An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte
CN105390747A (en) * 2015-11-13 2016-03-09 华南师范大学 Trimethyl borate additive-containing electrolyte solution, preparation method therefor and application thereof
CN105633464A (en) * 2016-03-09 2016-06-01 华南师范大学 Trimethyl borate additive contained high-voltage functional electrolyte and preparation method and application therefor
CN105849967A (en) * 2013-12-26 2016-08-10 国立大学法人京都大学 Secondary battery
CN107431245A (en) * 2015-02-04 2017-12-01 斯泰拉化工公司 Non-aqueous electrolyte for secondary battery and the secondary cell for possessing it
CN107615555A (en) * 2015-06-09 2018-01-19 斯泰拉化工公司 Non-aqueous electrolyte for secondary battery and the secondary cell for possessing it

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CN105849967A (en) * 2013-12-26 2016-08-10 国立大学法人京都大学 Secondary battery
CN107431245A (en) * 2015-02-04 2017-12-01 斯泰拉化工公司 Non-aqueous electrolyte for secondary battery and the secondary cell for possessing it
CN107615555A (en) * 2015-06-09 2018-01-19 斯泰拉化工公司 Non-aqueous electrolyte for secondary battery and the secondary cell for possessing it
CN105244540A (en) * 2015-11-13 2016-01-13 华南师范大学 Electrolyte containing triethyl borate additive as well as preparation method and application thereof
CN105355976A (en) * 2015-11-13 2016-02-24 华南师范大学 An electrolyte containing a tripropylborate additive, a preparing method thereof and applications of the electrolyte
CN105390747A (en) * 2015-11-13 2016-03-09 华南师范大学 Trimethyl borate additive-containing electrolyte solution, preparation method therefor and application thereof
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112751079A (en) * 2019-10-31 2021-05-04 苏州微木智能系统有限公司 Lithium ion battery
CN112751079B (en) * 2019-10-31 2024-07-19 苏州微木智能系统有限公司 Lithium ion battery

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Application publication date: 20181221