CN104393344A - Indoor temperature sodium and sulfur secondary battery electrolyte solution - Google Patents
Indoor temperature sodium and sulfur secondary battery electrolyte solution Download PDFInfo
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- CN104393344A CN104393344A CN201410560253.4A CN201410560253A CN104393344A CN 104393344 A CN104393344 A CN 104393344A CN 201410560253 A CN201410560253 A CN 201410560253A CN 104393344 A CN104393344 A CN 104393344A
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- electrolyte
- sodium
- secondary battery
- sulfur secondary
- battery
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- 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
- H01M10/0568—Liquid materials characterised by the solutes
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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
Abstract
The invention discloses indoor temperature sodium and sulfur secondary battery electrolyte solution. The electrolyte contained in the electrolyte solution comprises imidazole electrolyte, and further comprises catenarian and ring-shaped ether electrolyte and/or catenarian and ring-shaped ester electrolyte. According to the invention, addition of the imidazole electrolyte reduces internal resistance of a battery, improves solvability to sulfur and polysulphide, and electric discharge capacity and efficiency of the battery, and greatly promotes whole performance of the battery; the electrolyte solution is used for the sodium and sulfur secondary battery, reduces the internal resistance of the battery, improves capacity and energy density of the battery, and cycle performance and efficiency, and enables the low-temperature sodium and sulfur secondary battery to have relatively high competitiveness in a future secondary battery market.
Description
Technical field
The present invention relates to sodium-sulphur battery technical field, be specifically related to the electrolyte that a kind of room temperature sodium-sulfur secondary battery is used.
Background technology
Secondary cell is one of new forms of energy epoch necessary energy-storage facility, and along with the exploitation of resource, normally used lithium rechargeable battery cost can be more and more higher, and lithium resource is limited, therefore needs to find novel cheapness and rich in natural resources product as an alternative.Low temperature sodium sulfur rechargeable battery is a kind of novel secondary cell, and active material used is sulphur and sodium, and the content of these two kinds of elements in the earth's crust is all high, has and is similar to endless reserves, low price, is therefore a kind of secondary cell having actual application value.
Current business-like sodium-sulfur secondary battery is generally high temperature sodium-sulphur battery, cell operating temperature at 300 ~ 350 DEG C, by means of solid electrolyte β-Al
2o
3selectivity by the principle of sodium ion, make electronics by external circuit, and ion is by solid electrolyte, thus reaches discharge process, and charging is its inverse process.Because operating temperature is higher, at this temperature, sodium and sulphur are liquid, active high, great danger of combustion will be produced after battery generation rupture and leakage, and owing to there is oxidant and reducing agent in battery simultaneously, even if the isolated air of the high temperature sodium-sulphur battery after therefore out of control also can spontaneous combustion, Risk health behavior difficulty is large.
And room temperature sodium-sulfur secondary battery operating temperature is lower, relative danger reduces, in room temperature sodium-sulfur secondary battery, electrolyte is the key factor that low temperature sodium sulfur rechargeable battery plays capacity and energy, existing low temperature sodium sulfur rechargeable battery is often due to the problem such as the internal resistance of cell is excessive and stability test is poor, cause the utilization ratio of secondary cell low, battery life is short and affect its application.Therefore research and develop low temperature sodium sulfur rechargeable battery electrolyte and can make full use of sodium-sulfur secondary battery performance.
Summary of the invention
Technical problem to be solved by this invention is: the deficiency existed for prior art, there is provided one can stable existence between battery plus-negative plate, battery charge and discharge process stablized, there is high conductivity, sulphur and sodium polysulfide are had to higher solubility, both positive and negative polarity active material can be made full use of and the cycle performance of sodium-sulfur secondary battery and the room temperature sodium-sulfur secondary battery electrolyte of cycle efficieny can be significantly improved.
For solving the problems of the technologies described above, technical scheme of the present invention is:
A kind of room temperature sodium-sulfur secondary battery electrolyte, the electrolyte contained in described electrolyte comprises imidazoles electrolyte, and described electrolyte also comprises the ester electrolyte of chain, the ether electrolyte of ring-type and/or chain, ring-type.
Preferably, described imidazoles electrolyte comprises at least one in imidazoles, 1-methylimidazole, 1,2-methylimidazole, 1-butyl-3 methylimidazole villaumite, 1-butyl tri-methylimidazolium perchlorate, chlorination 1-methylimidazole.
Preferably, the ether electrolyte of described chain, ring-type comprises at least one in dimethoxy-ethane (DME), diethoxyethane (DEE), oxolane (THF), 2-methyltetrahydrofuran (MeTHF), diglycol ethylene dimethyl ether (DGM), contracting TRIGLYME (TGM), contracting tetraethyleneglycol dimethyl ether (TEGM), DOX (DOL), benzo-15-crown-5.
Preferably, described chain, the ester electrolyte of ring-type comprises ethylene carbonate (EC), propene carbonate (PC), butylene (BC), 1, 2-dimethylvinylsiloxy carbonic ester (1, 2-BC), ethylene carbonate (BEC), carbonic acid first butyl ester (BMC), dibutyl carbonate (DBC), diethyl carbonate (DEC), dimethyl carbonate (DMC), chloro-ethylene carbonate (CIEC), trifluoromethyl ethylene carbonate (CF3-EC), carbonic acid di-n-propyl ester (DPC), diisopropyl carbonate (DIPC), methyl ethyl carbonate (EMC), ethyl propyl carbonic acid ester (EPC), ethylene isopropyl ester (EIPC), methyl propyl carbonate (MPC), at least one in carbonic acid first isopropyl ester (MIPC).
As further preferred, the ester electrolyte of described chain, ring-type comprises at least one in ethylene carbonate (EC), propene carbonate (PC), diethyl carbonate (DEC), dimethyl carbonate (DMC).
Preferably, the content in the electrolyte that contains in described electrolyte of the ester electrolyte of described chain, ring-type is minimum.
Preferably, volume percent content≤20% of ester electrolyte in described electrolyte of described chain, ring-type.
Preferably, the electrolytical volume percent content of the imidazoles contained in described electrolyte is 5 ~ 60%, and the chain contained in described electrolyte, the electrolytical volume percent content of the ether of ring-type are 30 ~ 95%.
Also containing the electrolyte sodium salt being used for realizing ionic conduction effect in described electrolyte.
Preferably, described electrolyte sodium salt comprises at least one in sodium chloride, sodium phosphate, vulcanized sodium, sodium polysulfide, sodium perchlorate, sodium hexafluoro phosphate, trifluoromethyl sulfonate, two (trimethyl fluoride sulfonyl) imines sodium.
The molar concentration of described electrolyte sodium salt is 0.5 ~ 2.5mol/L.
Described electrolyte is keep liquid in-20 DEG C ~ 120 DEG C in temperature range.Be liquid condition in sodium-sulfur secondary battery temperature range of operation, the effect of inside battery sodium ion-conductive can be realized, the active material in battery can be made full use of.
For realizing making full use of active material, described electrolyte fully can infiltrate the both positive and negative polarity active material in sodium-sulfur secondary battery.
The discharge process of sodium-sulfur secondary battery drives electronics to pass through external circuit under the electrical potential difference of sodium and sulphur, electronics reaches sulphur through external circuit, sulphur obtains electronics and forms sulphion, sodium loses an electronics simultaneously, form sodium ion, by the sodium salt conduction in electrolyte, sulphion and sodium ion form sodium polysulfide.In this process, battery is different and have different electromotive force according to the electromotive force of sulphur atom and many sulphions, cell emf according to different active materials and depth of discharge different and there is different scopes, be generally 0.8-1.5V.Charging process is its inverse process, under the effect of extra electric field, electronics reverse flow, reach the sodium ion of anode later in solution to be combined, lose electronics at negative pole end sulphion simultaneously, general charging voltage has different scopes according to the composition of the active material of concrete battery and structure difference, and general final voltage is arranged between 2.4-2.8V.
Owing to have employed technique scheme, beneficial effect of the present invention is:
Room temperature sodium-sulfur secondary battery electrolyte of the present invention, the electrolyte contained in described electrolyte comprises imidazoles electrolyte, and described electrolyte also comprises the ester electrolyte of chain, the ether electrolyte of ring-type and/or chain, ring-type.Imidazoles is electrolytical adds the internal resistance reducing battery, improves the solubility to sulphur and polysulfide, adds discharge capacity of the cell and efficiency, has great promotion to the whole performance of battery.
The preferred electrolyte solution of the present invention can make full use of the active material of battery plus-negative plate, realizes higher capacity density and energy density.Electrolyte solution can have higher cycle efficieny to battery plus-negative plate, has good process based prediction model, can have good solubility through preferred electrolyte solution to sulphur and polysulfide, can realize the abundant release of battery capacity.
The present invention has wider electrochemical window through preferred electrolyte, aligns negative electrode active material and stablizes, within the scope of charging/discharging voltage, the reactions such as decomposition do not occur, to battery other parts, as barrier film, collector, electrode material etc. have good compatibility.
The present invention, through preferred sodium salt compound, serves sodium ion and transmits intermediation, ensure that the timely conduction of sodium ion in battery charge and discharge process, improve battery conductance rate simultaneously, reduce the internal resistance of cell, battery operating voltage is had certain lifting.Sodium salt compound to have within the scope of battery applications Heat stability is good, not easily decompose, have wider electrochemical window, with the advantage such as other material of battery does not react.
The present invention is used for sodium-sulfur secondary battery, reduces the internal resistance of battery, improves capacity density and the energy density of battery, add cycle performance and cycle efficieny, make low temperature sodium sulfur rechargeable battery have larger competitiveness in the secondary cell market in future.The electric discharge utilance of the sodium-sulphur battery utilizing the present invention to prepare is dump energy more than 60% after more than 70%, 1C discharge cycles 100 times.
Embodiment
The present invention is set forth further below in conjunction with specific embodiment.Should be understood that following examples only for illustration of the present invention, and can not limit the scope of the invention.
Embodiment 1
A kind of room temperature sodium-sulfur secondary battery electrolyte is that 1:1:1 is mixed with mixed solution with imidazoles and dimethoxy-ethane (DME) and ethylene carbonate (EC) three kinds of solution proportion.The trifluoromethyl sulfonate electrolyte of 1.0mol/L is become with above-mentioned electrolyte quota.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 59% after 58%, 1C discharge cycles 100 times.
Embodiment 2
A kind of room temperature sodium-sulfur secondary battery electrolyte is that 1:1:1 is mixed with mixed solution with 1-methylimidazole, dimethyl carbonate and diethoxyethane (DEE) three kinds of solution proportion.The trifluoromethyl sulfonate electrolyte of 1.0mol/L is become with above-mentioned electrolyte quota.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 56% after 52%, 1C discharge cycles 100 times.
Embodiment 3
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: 1-butyl-3 methylimidazole villaumite of 30%, the oxolane (THF) of 60% and the propene carbonate (PC) of 10%, be mixed with the sodium perchlorate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 69% after 76%, 1C discharge cycles 100 times.
Embodiment 4
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the 1-butyl tri-methylimidazolium perchlorate of 40%, with the diglycol ethylene dimethyl ether (DGM) of 45% and the carbonic acid first butyl ester (BMC) of 15%, be mixed with the sodium phosphate electrolyte of 0.5mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 53% after 72%, 1C discharge cycles 100 times.
Embodiment 5
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the chlorination 1-methylimidazole of 25%, with 65% 1,3-dioxolanes (DOL) and 10% butylene (BC), be mixed with the sodium perchlorate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 58% after 79%, 1C discharge cycles 100 times.
Embodiment 6
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: 1-butyl-3 methylimidazole villaumite of 60%, with the dimethyl carbonate (DMC) of 10% and 30% 1,3-dioxolanes (DOL), is mixed with the sodium perchlorate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 60% after 85%, 1C discharge cycles 100 times.
Embodiment 7
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the imidazoles electrolyte 1 of 20%, 2-methylimidazole, with the contracting TRIGLYME (TGM) of 68% and the chloro-ethylene carbonate (CIEC) of 12%, be mixed with the sodium perchlorate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 61% after 80%, 1C discharge cycles 100 times.
Embodiment 8
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the chlorination 1-methylimidazole of 15%, with the benzo-15-crown-5 of 80% and the carbonic acid di-n-propyl ester (DPC) of 5%, be mixed with the trifluoromethyl sulfonate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 72% after 70%, 1C discharge cycles 100 times.
Embodiment 9
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the 1-methylimidazole of 30%, with the 2-methyltetrahydrofuran (MeTHF) of 35% and the dimethoxy-ethane (DME) of 35%, be mixed with two (trimethyl fluoride sulfonyl) imines sodium electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 84% after 85%, 1C discharge cycles 100 times.
Embodiment 10
A kind of room temperature sodium-sulfur secondary battery electrolyte, preparation mixed solution, the percent by volume of mixed solution consists of: the 1-methylimidazole of 20%, with the diethoxyethane (DEE) of 40% and the contracting TRIGLYME (TGM) of 40%, be mixed with the sodium hexafluoro phosphate electrolyte of 1.0mol/L with above-mentioned mixed solution.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 88% after 82%, 1C discharge cycles 100 times.
Comparative example 1
Not containing electrolyte 1-methylimidazole in the electrolyte of comparative example 1, all the other are identical with embodiment 10.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 48% after 65%, 1C discharge cycles 100 times.
Comparative example 2
Not containing electrolyte 1-methylimidazole in the electrolyte of comparative example 2, all the other are identical with embodiment 9.Adopt this electrolyte, use the sodium-sulfur secondary battery of positive plate and negative plate and battery diaphragm assembling, test battery at 25 DEG C, initial open circuit voltage 2.3V, electric discharge utilance is electricity residue 25% after 69%, 1C discharge cycles 100 times.
Claims (10)
1. a room temperature sodium-sulfur secondary battery electrolyte, is characterized in that: the electrolyte contained in described electrolyte comprises imidazoles electrolyte, and described electrolyte also comprises the ester electrolyte of chain, the ether electrolyte of ring-type and/or chain, ring-type.
2. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 1, it is characterized in that: described imidazoles electrolyte comprises at least one in imidazoles, 1-methylimidazole, 1,2-methylimidazole, 1-butyl-3 methylimidazole villaumite, 1-butyl tri-methylimidazolium perchlorate, chlorination 1-methylimidazole.
3. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 1, it is characterized in that: the ether electrolyte of described chain, ring-type comprises at least one in dimethoxy-ethane, diethoxyethane, oxolane, 2-methyltetrahydrofuran, diglycol ethylene dimethyl ether, contracting TRIGLYME, contracting tetraethyleneglycol dimethyl ether, DOX, benzo-15-crown-5.
4. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 1, it is characterized in that: the ester electrolyte of described chain, ring-type comprises at least one in ethylene carbonate, propene carbonate, butylene, 1,2-dimethylvinylsiloxy carbonic ester, ethylene carbonate, carbonic acid first butyl ester, dibutyl carbonate, diethyl carbonate, dimethyl carbonate, chloro-ethylene carbonate, trifluoromethyl ethylene carbonate, carbonic acid di-n-propyl ester, diisopropyl carbonate, methyl ethyl carbonate, ethyl propyl carbonic acid ester, ethylene isopropyl ester, methyl propyl carbonate, carbonic acid first isopropyl ester.
5. the room temperature sodium-sulfur secondary battery electrolyte as described in any one of Claims 1-4, is characterized in that: the content in the electrolyte that the ester electrolyte of described chain, ring-type contains in described electrolyte is minimum.
6. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 5, is characterized in that: volume percent content≤20% of ester electrolyte in described electrolyte of described chain, ring-type.
7. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 5, it is characterized in that: the electrolytical volume percent content of the imidazoles contained in described electrolyte is 5-60%, the electrolytical volume percent content of ether of described chain, ring-type is 30 ~ 95%.
8. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 5, is characterized in that: also containing electrolyte sodium salt in described electrolyte.
9. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 8, is characterized in that: described electrolyte sodium salt comprises at least one in sodium phosphate, vulcanized sodium, sodium polysulfide, sodium perchlorate, sodium hexafluoro phosphate, trifluoromethyl sulfonate, trifluoromethane sulfonic acid imines sodium, two (trimethyl fluoride sulfonyl) imines sodium.
10. room temperature sodium-sulfur secondary battery electrolyte as claimed in claim 5, is characterized in that: described electrolyte is keep liquid in-20 DEG C ~ 120 DEG C in temperature range.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410560253.4A CN104393344B (en) | 2014-10-18 | A kind of room temperature sodium-sulfur secondary battery electrolyte |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410560253.4A CN104393344B (en) | 2014-10-18 | A kind of room temperature sodium-sulfur secondary battery electrolyte |
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| Publication Number | Publication Date |
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| CN104393344A true CN104393344A (en) | 2015-03-04 |
| CN104393344B CN104393344B (en) | 2017-01-04 |
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| CN102956866A (en) * | 2011-08-26 | 2013-03-06 | 中国科学院物理研究所 | Chargeable alkali metal-sulfur liquid flow battery |
| CN103227348A (en) * | 2013-04-03 | 2013-07-31 | 山东默锐科技有限公司 | Sodium-sulfur electrical storage battery |
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Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| JP2004207451A (en) * | 2002-12-25 | 2004-07-22 | Sanyo Chem Ind Ltd | Electrolyte |
| CN102804470A (en) * | 2009-06-09 | 2012-11-28 | 夏普株式会社 | Redox flow battery |
| EP2485317A1 (en) * | 2009-09-28 | 2012-08-08 | Sumitomo Electric Industries, Ltd. | Battery and energy system |
| CN102956866A (en) * | 2011-08-26 | 2013-03-06 | 中国科学院物理研究所 | Chargeable alkali metal-sulfur liquid flow battery |
| CN102938475A (en) * | 2012-11-08 | 2013-02-20 | 中国科学院化学研究所 | Sodium-sulfur battery and manufacture method thereof |
| CN103227348A (en) * | 2013-04-03 | 2013-07-31 | 山东默锐科技有限公司 | Sodium-sulfur electrical storage battery |
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