CN108539272A - A kind of electrolyte of lithium metal battery - Google Patents
A kind of electrolyte of lithium metal battery Download PDFInfo
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- CN108539272A CN108539272A CN201810442544.1A CN201810442544A CN108539272A CN 108539272 A CN108539272 A CN 108539272A CN 201810442544 A CN201810442544 A CN 201810442544A CN 108539272 A CN108539272 A CN 108539272A
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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
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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Abstract
A kind of electrolyte of lithium metal battery, the electrolyte are using esters, ethers or ether-ether blended liquid as organic solvent, wherein containing the lithium salts that molar concentration is 1.0~5.0mol/L, and the additive that is made of lithium nitrate and metal halide.Electrolyte system containing the additive is used for lithium metal battery, stable mixed ion conductor boundary layer can be formed on cathode of lithium surface, being in direct contact for electrolyte and lithium metal is avoided to greatest extent, reduce the irreversible loss of lithium dendrite growth and lithium source, realize lithium ion boundary layer fast transferring and uniform deposition on the electrode, electrolyte containing the additive can significantly improve the coulombic efficiency of lithium metal and the service life of full battery, have a good application prospect.
Description
Technical field
The present invention relates to a kind of electrolyte of lithium metal battery, belong to lithium metal battery technical field.
Background technology
Under the new era of high specific energy batteries demand, lithium metal is because of its lower electrode potential (- 3.04V vs standard hydrogen electricity
Pole) and superelevation theoretical specific capacity (3860mAh g-1) become a kind of negative material of great potential.Lithium metal is in functionization
It is faced with the technical issues of need solving in the process；First, the thermodynamic phase of lithium metal and electrolyte is easy to cause gold
Belong to lithium surface and forms unstable solid liquid interface layer；Secondly, with the progress of charge and discharge, unstable solid liquid interface can induce lithium
The nonuniform deposition of ion leads to the generation of Li dendrite and dead lithium；The presence of Li dendrite may pierce through battery diaphragm so that positive and negative
Pole is in contact and short circuit, has hidden peril of explosion；The presence of dead lithium layer causes the polarization of battery to increase the decline with coulombic efficiency.
Therefore, for how solving metal Li dendrite and how to improve the coulombic efficiency of metal lithium electrode, researcher carries
A variety of resolution policies are gone out：Increase the specific surface area of electrode to reduce the local current densities (patent No.：CN105845891A)；It is logical
Hardness and the skeleton of lithium boron alloy are crossed to control the epitaxial growth (Small, 2014,10,4257) of lithium metal；Introduce silica
Chemical composition regulates and controls the uniform deposition (Adv.Mater.2016,28,2888) of lithium ion；By the screening of electrolyte prescription come
The stable solid liquid interface layer (patent No. is formed on the surface of lithium metal：CN105870502A)；In the recent period, have it was discovered by researchers that
Orientation reaction (the Nature of lithium ion can be induced with the metal or non-metal simple-substance of lithium metal generation alloy behavior
Energy, 2016,1,16010), to control the growth of lithium metal.
Invention content
The object of the present invention is to provide a kind of electrolyte of lithium metal battery, by preparing the electrolyte containing additive,
Stable mixed ion conductor boundary layer can be formed on cathode of lithium surface, avoid electrolyte and lithium metal to the maximum extent
It is in direct contact, reduces the irreversible loss of lithium dendrite growth and lithium source, realize lithium ion in the fast transferring of boundary layer and in electricity
Uniform deposition on extremely, to further increase the coulombic efficiency of lithium metal and the service life of full battery.
Technical scheme is as follows：
A kind of electrolyte of lithium metal battery, which is characterized in that the electrolyte is blended with esters, ethers or ether-ether
Liquid is as organic solvent, wherein contain lithium salts, and the additive being made of lithium nitrate and metal halide.
Preferably, the molar concentration of lithium salts is 1.0~5.0mol/L in the electrolyte；Lithium nitrate accounts in the additive
0.001wt%~10.0wt% of total electrolyte quality score, metal halide account for total electrolyte quality score
0.001wt.%~10.0wt.%.
In above-mentioned technical proposal, it is preferable that the metal halide is silver fluoride, copper fluoride, cupric iodide, silver iodide, fluorine
Change the mixing of one or more of iron, zinc chloride, iron chloride and nickel fluoride.
In above-mentioned technical proposal, it is preferable that the based organic solvent is ethylene carbonate or diethyl carbonate；Ethers
Organic solvent is the one or two of tetraethyleneglycol dimethyl ether and glycol dimethyl ether；The lithium salts is lithium hexafluoro phosphate, double
One or more of lithium trifluoromethanesulp,onylimide and double fluorine sulfimide lithiums.
The present invention compared with prior art, has the following advantages that and high-lighting effect：1. being different from traditional artificial solid-liquid circle
Face layer can form ion-electron mixed interface layer, the formation of the boundary layer under the system of the additive on the surface of lithium metal
Accelerate lithium ion interface migration rate；2. the presence of mixed interface layer can uniformly regulate and control the forming core of lithium metal,
So that cathode of lithium surface is generated without dendrite；3. the presence of hybrid ionic boundary layer can utilize the lithium storage function of nano-interface layer
The buffer layer of lithium metal is built, the nonuniform deposition brought by diffusion control is reduced；4. additive is cheap, in electrolyte
Middle dosage is low, does not have particular/special requirement for use environment.
Specific implementation mode
A kind of electrolyte of lithium metal battery provided by the invention, preparation method are by metal halide and lithium nitrate group
At additive be added in the esters dissolved with lithium salts, the organic solvent that ethers or ether-ether are blended.Lithium salts in the electrolyte
Molar concentration is 1.0~5.0mol/L；In the additive lithium nitrate account for the 0.001wt% of total electrolyte quality score~
10.0wt%, metal halide account for 0.001wt.%~10.0wt.% of total electrolyte quality score.
Metal halide in the additive preferably uses silver fluoride, copper fluoride, ferric flouride, nickel fluoride, zinc chloride, chlorine
Change the mixing of one or more of iron, cupric iodide and silver iodide；Organic solvent in electrolyte solution is ethylene carbonate, carbonic acid
The one or more of diethylester, tetraethyleneglycol dimethyl ether, glycol dimethyl ether.The soluble lithium salt of electrolyte is hexafluorophosphoric acid
The one or more of lithium, bis trifluoromethyl sulfimide lithium and double fluorine sulfimide lithiums, the electrolyte system containing the additive
Suitable for the full battery type using lithium metal as cathode.
It is further appreciated that the present invention from following embodiment, but the present invention is not limited solely to following embodiment.
Embodiment 1：Preparation accounts for total electrolyte quality score and is 1.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene glycol dimethyl ether solution of 0.001wt.% silver fluorides, lithium salts are double trifluorosulfonimide lithiums, a concentration of 1.0mol/L.It should
Electrolyte system is used for using metal lithium sheet as cathode, and sulphur is tested as the full battery of anode, is found by test, the library of battery
Human relations efficiency can reach 99.0%, and cycle life can reach 500 circles.
Embodiment 2：Preparation accounts for total electrolyte quality score and is 0.01wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene carbonate ester solution of 1wt.% copper fluorides, lithium salts are lithium hexafluoro phosphate, a concentration of 1.0mol/L.The electrolyte system is used
In using metal lithium sheet as cathode, LiFePO4 is the full battery test of anode, finds that the coulombic efficiency of battery can by test
To reach 99.9%, cycle life can reach 2000 circles.
Embodiment 3：Preparation accounts for total electrolyte quality score and is 5.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene carbonate ester solution of 3.0wt.% cupric iodides, lithium salts are lithium hexafluoro phosphate, a concentration of 2.0mol/L.By the electrolyte system
For using metal lithium sheet as cathode, nickel-cobalt-manganese ternary material to be the full battery test of anode, is found by test, the library of battery
Human relations efficiency can reach 99.8%, and cycle life can reach 1000 circles.
Embodiment 4：Preparation accounts for total electrolyte quality score and is 2.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The tetraethyleneglycol dimethyl ether solution of 5.0wt.% silver iodide, lithium salts are double fluorine sulfimide lithiums, a concentration of 5.0mol/L.By the electricity
It solves liquid system to be used for using metal lithium sheet as cathode, LiFePO4 is the full battery test of anode, is found by test, battery
Coulombic efficiency can reach 99.9%, and cycle life can reach 800 circles.
Embodiment 5：Preparation accounts for total electrolyte quality score and is 5.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene glycol dimethyl ether solution of 0.01wt.% ferric flourides, lithium salts are double trifluorosulfonimide lithiums, a concentration of 2.0mol/L.It should
Electrolyte system is used for using metal lithium sheet as cathode, and sulphur is tested as the full battery of anode, is found by test, the library of battery
Human relations efficiency can reach 98.0%, and cycle life can reach 600 circles.
Embodiment 6：Preparation accounts for total electrolyte quality score and is 0.5wt.% lithium nitrates and accounts for total electrolyte quality score and be
The diethyl carbonate solution of 0.05wt.% zinc chloride, lithium salts are lithium hexafluoro phosphate, a concentration of 2.0mol/L.By the electrolyte
System is for using metal lithium sheet as cathode, nickel-cobalt-manganese ternary material to be the full battery test of anode, is found by test, battery
Coulombic efficiency can reach 99.9%, and cycle life can reach 1200 circles.
Embodiment 7：Preparation accounts for total electrolyte quality score and is 10.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene carbonate ester solution of 5.0wt.% nickel fluorides, lithium salts are lithium hexafluoro phosphate, a concentration of 1.0mol/L.By the electrolyte system
For using metal lithium sheet as cathode, LiFePO4 to be the full battery test of anode, is found by test, the coulombic efficiency of battery
99.2% can be reached, cycle life can reach 400 circles.
Embodiment 8：Preparation accounts for total electrolyte quality score and is 2.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The divinyl carbonate and ethylene carbonate ester solution (volume ratio 1 of 1.0wt.% iron chloride：1), lithium salts is lithium hexafluoro phosphate, concentration
For 1.0mol/L.The electrolyte system is used for using metal lithium sheet as cathode, LiMn2O4 is the full battery test of anode, is passed through
Test finds that the coulombic efficiency of battery can reach 99.2%, and cycle life can reach 400 circles.
Embodiment 9：Preparation accounts for total electrolyte quality score and is 5.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The tetraethyleneglycol dimethyl ether and ethylene carbonate ester solution (volume ratio 1 of 0.5wt.% silver fluorides：1), lithium salts is lithium hexafluoro phosphate,
A concentration of 3.0mol/L.The electrolyte system is used for using metal lithium sheet as cathode, cobalt acid lithium is the full battery test of anode,
It is found by test, the coulombic efficiency of battery can reach 99.9%, and cycle life can reach 1400 circles.
Embodiment 10：Preparation accounts for total electrolyte quality score and is 5.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene glycol dimethyl ether solution of 3.0wt.% copper fluorides, lithium salts are double trifluorosulfonimide lithiums, a concentration of 5.0mol/L.By the electricity
It solves liquid system to be used for using metal lithium sheet as cathode, sulphur is tested as the full battery of anode, is found by test, the coulomb of battery
Efficiency can reach 99.7%, and cycle life can reach 1000 circles.
Embodiment 11：Preparation accounts for total electrolyte quality score and is 5.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene glycol dimethyl ether solution of 7.0wt.% ferric flourides, lithium salts are double fluorine sulfimide lithiums, a concentration of 4.0mol/L.By the electrolysis
Liquid system is used for using metal lithium sheet as cathode, and LiFePO4 is the full battery test of anode, is found by test, the library of battery
Human relations efficiency can reach 99.9%, and cycle life can reach 1500 circles.
Embodiment 12：Preparation accounts for total electrolyte quality score and is 2.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene carbonate ester solution of 5.0wt.% nickel fluorides, lithium salts are lithium hexafluoro phosphate, a concentration of 2.0mol/L.By the electrolyte system
For using metal lithium sheet as cathode, nickel-cobalt-manganese ternary material to be the full battery test of anode, is found by test, the library of battery
Human relations efficiency can reach 99.9%, and cycle life can reach 1000 circles.
Embodiment 13：Preparation accounts for total electrolyte quality score and is 1.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The diethyl carbonate solution of 2.0wt.% zinc chloride, lithium salts are lithium hexafluoro phosphate, a concentration of 1.0mol/L.By the electrolyte system
For using metal lithium sheet as cathode, LiMn2O4 to be the full battery test of anode, finds that the coulombic efficiency of battery can by test
To reach 99.3%, cycle life can reach 500 circles.
Embodiment 14：Preparation accounts for total electrolyte quality score and is 2.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The ethylene carbonate ester solution of 5.0wt.% iron chloride, lithium salts are lithium hexafluoro phosphate, a concentration of 3.0mol/L.By the electrolyte system
For using metal lithium sheet as cathode, cobalt acid lithium to be the full battery test of anode, finds that the coulombic efficiency of battery can by test
To reach 99.9%, cycle life can reach 1500 circles.
Embodiment 15：Preparation accounts for total electrolyte quality score and is 1.0wt.% lithium nitrates and accounts for total electrolyte quality score and be
The tetraethyleneglycol dimethyl ether solution of 3.0wt.% cupric iodides, lithium salts are double fluorine sulfimide lithiums, a concentration of 4.0mol/L.By the electricity
It solves liquid system to be used for using metal lithium sheet as cathode, sulphur is tested as the full battery of anode, is found by test, the coulomb of battery
Efficiency can reach 99.7%, and cycle life can reach 1500 circles.
Claims (5)
1. a kind of electrolyte of lithium metal battery, which is characterized in that the electrolyte is with esters, ethers or ether-ether blended liquid
As organic solvent, wherein contain lithium salts, and the additive being made of lithium nitrate and metal halide.
2. a kind of electrolyte of lithium metal battery described in accordance with the claim 1, which is characterized in that lithium salts in the electrolyte
Molar concentration is 1.0~5.0mol/L；In the additive lithium nitrate account for the 0.001wt% of total electrolyte quality score~
10.0wt%, metal halide account for 0.001wt.%~10.0wt.% of total electrolyte quality score.
3. according to a kind of electrolyte of lithium metal battery as claimed in claim 1 or 2, which is characterized in that the metal halide
For the mixed of one or more of silver fluoride, copper fluoride, cupric iodide, silver iodide, ferric flouride, zinc chloride, iron chloride and nickel fluoride
It closes.
4. a kind of electrolyte of lithium metal battery according to claim 1 or 2, it is characterised in that：The esters are organic
Solvent is ethylene carbonate or diethyl carbonate；Ether organic solvent is one kind of tetraethyleneglycol dimethyl ether and glycol dimethyl ether
Or two kinds.
5. a kind of electrolyte of lithium metal battery according to claim 1 or 2, it is characterised in that：The lithium salts is six
One or more of lithium fluophosphate, bis trifluoromethyl sulfimide lithium and double fluorine sulfimide lithiums.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201810442544.1A CN108539272A (en) | 2018-05-10 | 2018-05-10 | A kind of electrolyte of lithium metal battery |
| PCT/CN2018/094687 WO2019214035A1 (en) | 2018-05-10 | 2018-07-05 | Lithium metal battery electrolyte |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201810442544.1A CN108539272A (en) | 2018-05-10 | 2018-05-10 | A kind of electrolyte of lithium metal battery |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109585947A (en) * | 2018-12-04 | 2019-04-05 | 安徽盟维新能源科技有限公司 | A kind of lithium an- ode double protection method and application |
| CN110828896A (en) * | 2019-11-21 | 2020-02-21 | 国网上海市电力公司 | Application of metal dendrite inhibiting additive, electrolyte containing additive and battery |
| CN111477957A (en) * | 2020-04-22 | 2020-07-31 | 浙江大学 | Lithium metal battery electrolyte containing composite additive and preparation method thereof |
| CN112687960A (en) * | 2020-12-28 | 2021-04-20 | 浙江省科创新材料研究院 | Method for stabilizing solid electrolyte/metal negative electrode interface by using zinc salt |
| CN113206293A (en) * | 2021-04-14 | 2021-08-03 | 华中科技大学 | Lithium metal battery electrolyte and preparation method and application thereof |
| CN113659203A (en) * | 2021-07-18 | 2021-11-16 | 哈尔滨工业大学 | Electrolyte containing composite additive and application thereof |
| CN114094180A (en) * | 2021-11-22 | 2022-02-25 | 浙江工业大学 | Ether electrolyte containing silver nitrate additive for lithium metal battery |
| CN114447426A (en) * | 2021-12-22 | 2022-05-06 | 清华大学 | Lithium-sulfur battery electrolyte, preparation method thereof and lithium-sulfur battery |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107093705A (en) * | 2017-03-22 | 2017-08-25 | 清华大学 | A kind of cathode of lithium surface treatment method of lithium metal battery |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20140023936A1 (en) * | 2012-07-17 | 2014-01-23 | Ilias Belharouak | Lithium-sulfur electrolytes and batteries |
| CN105870502B (en) * | 2016-04-21 | 2019-07-02 | 清华大学 | A kind of electrolysis additive and its application |
-
2018
- 2018-05-10 CN CN201810442544.1A patent/CN108539272A/en active Pending
- 2018-07-05 WO PCT/CN2018/094687 patent/WO2019214035A1/en active Application Filing
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107093705A (en) * | 2017-03-22 | 2017-08-25 | 清华大学 | A kind of cathode of lithium surface treatment method of lithium metal battery |
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109585947A (en) * | 2018-12-04 | 2019-04-05 | 安徽盟维新能源科技有限公司 | A kind of lithium an- ode double protection method and application |
| CN110828896A (en) * | 2019-11-21 | 2020-02-21 | 国网上海市电力公司 | Application of metal dendrite inhibiting additive, electrolyte containing additive and battery |
| CN111477957A (en) * | 2020-04-22 | 2020-07-31 | 浙江大学 | Lithium metal battery electrolyte containing composite additive and preparation method thereof |
| WO2021213132A1 (en) * | 2020-04-22 | 2021-10-28 | 浙江大学 | Lithium metal battery electrolyte containing composite additive, and preparation method therefor |
| CN112687960A (en) * | 2020-12-28 | 2021-04-20 | 浙江省科创新材料研究院 | Method for stabilizing solid electrolyte/metal negative electrode interface by using zinc salt |
| CN113206293A (en) * | 2021-04-14 | 2021-08-03 | 华中科技大学 | Lithium metal battery electrolyte and preparation method and application thereof |
| CN113659203A (en) * | 2021-07-18 | 2021-11-16 | 哈尔滨工业大学 | Electrolyte containing composite additive and application thereof |
| CN114094180A (en) * | 2021-11-22 | 2022-02-25 | 浙江工业大学 | Ether electrolyte containing silver nitrate additive for lithium metal battery |
| CN114447426A (en) * | 2021-12-22 | 2022-05-06 | 清华大学 | Lithium-sulfur battery electrolyte, preparation method thereof and lithium-sulfur battery |
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| WO2019214035A1 (en) | 2019-11-14 |
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Application publication date: 20180914 |