CN112952125A - Electrolyte structure of thermal activation battery and application thereof - Google Patents
Electrolyte structure of thermal activation battery and application thereof Download PDFInfo
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- CN112952125A CN112952125A CN202110231455.4A CN202110231455A CN112952125A CN 112952125 A CN112952125 A CN 112952125A CN 202110231455 A CN202110231455 A CN 202110231455A CN 112952125 A CN112952125 A CN 112952125A
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- thermally activated
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 66
- 238000007725 thermal activation Methods 0.000 title abstract description 4
- 239000007791 liquid phase Substances 0.000 claims description 6
- 229920006254 polymer film Polymers 0.000 claims description 6
- 239000007790 solid phase Substances 0.000 claims description 6
- 239000012071 phase Substances 0.000 claims description 5
- 239000007787 solid Substances 0.000 claims description 5
- 230000007704 transition Effects 0.000 claims description 5
- 230000009471 action Effects 0.000 claims description 4
- 238000002347 injection Methods 0.000 claims description 4
- 239000007924 injection Substances 0.000 claims description 4
- 239000007788 liquid Substances 0.000 claims description 4
- 230000008859 change Effects 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 239000011148 porous material Substances 0.000 claims description 2
- 239000000126 substance Substances 0.000 claims description 2
- 150000002500 ions Chemical class 0.000 abstract description 15
- 230000004913 activation Effects 0.000 abstract description 12
- 238000001994 activation Methods 0.000 abstract description 12
- 102000004310 Ion Channels Human genes 0.000 abstract description 3
- 230000005518 electrochemistry Effects 0.000 abstract description 2
- 238000000034 method Methods 0.000 abstract 1
- 239000007773 negative electrode material Substances 0.000 description 11
- 239000004698 Polyethylene Substances 0.000 description 10
- 239000007774 positive electrode material Substances 0.000 description 9
- 230000008018 melting Effects 0.000 description 6
- 238000002844 melting Methods 0.000 description 6
- -1 polyethylene Polymers 0.000 description 6
- 238000007789 sealing Methods 0.000 description 6
- 229920000642 polymer Polymers 0.000 description 5
- 239000004743 Polypropylene Substances 0.000 description 4
- 239000011888 foil Substances 0.000 description 4
- 229920000139 polyethylene terephthalate Polymers 0.000 description 4
- 239000005020 polyethylene terephthalate Substances 0.000 description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 239000002033 PVDF binder Substances 0.000 description 3
- 239000004952 Polyamide Substances 0.000 description 3
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 3
- 229920002647 polyamide Polymers 0.000 description 3
- 239000004926 polymethyl methacrylate Substances 0.000 description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 3
- 229910052683 pyrite Inorganic materials 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- 238000002076 thermal analysis method Methods 0.000 description 3
- 239000004642 Polyimide Substances 0.000 description 2
- 239000000956 alloy Substances 0.000 description 2
- 229910045601 alloy Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000000499 gel Substances 0.000 description 2
- 239000010416 ion conductor Substances 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 229910052960 marcasite Inorganic materials 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000012188 paraffin wax Substances 0.000 description 2
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 2
- 229920001721 polyimide Polymers 0.000 description 2
- 238000002604 ultrasonography Methods 0.000 description 2
- LLLVZDVNHNWSDS-UHFFFAOYSA-N 4-methylidene-3,5-dioxabicyclo[5.2.2]undeca-1(9),7,10-triene-2,6-dione Chemical compound C1(C2=CC=C(C(=O)OC(=C)O1)C=C2)=O LLLVZDVNHNWSDS-UHFFFAOYSA-N 0.000 description 1
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 1
- 235000015842 Hesperis Nutrition 0.000 description 1
- 235000012633 Iberis amara Nutrition 0.000 description 1
- 229910013618 LiCl—KCl Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000002202 Polyethylene glycol Substances 0.000 description 1
- 229920002367 Polyisobutene Polymers 0.000 description 1
- 229920000388 Polyphosphate Polymers 0.000 description 1
- 229920001328 Polyvinylidene chloride Polymers 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000005496 eutectics Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 229920002239 polyacrylonitrile Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 229920000306 polymethylpentene Polymers 0.000 description 1
- 239000011116 polymethylpentene Substances 0.000 description 1
- 239000001205 polyphosphate Substances 0.000 description 1
- 235000011176 polyphosphates Nutrition 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004814 polyurethane Substances 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 239000005033 polyvinylidene chloride Substances 0.000 description 1
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 description 1
- 239000011028 pyrite Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/30—Deferred-action cells
- H01M6/36—Deferred-action cells containing electrolyte and made operational by physical means, e.g. thermal cells
-
- 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
- H01M2300/0088—Composites
- H01M2300/0094—Composites in the form of layered products, e.g. coatings
Abstract
The invention belongs to the field of electrochemistry, and particularly relates to an electrolyte structure of a thermally activated battery and application thereof. The invention discloses an electrolyte structure, which solves the problem of overhigh thermal activation temperature of a thermal battery. The electrolyte with the ion conducting structure in the battery is wrapped by the inert layer without conducting ions, so that the battery has no ion channel in the storage process, the battery can be stored for a long time without self-discharge, and the battery can be stored for a long time without losing electric quantity. The inert layer which wraps the electrolyte and is not conductive to ions can be flexibly selected according to the service environment of the battery, and then the flexible adjustment of the activation temperature and the activation form is realized.
Description
Technical Field
The invention belongs to the field of electrochemistry, and particularly relates to an electrolyte structure of a thermally activated battery and application thereof.
Background
Thermally activated batteries are an important reserve battery. The electrolyte is non-conductive solid when stored, and the electrolyte is activated by igniting the heating agent in the electrolyte when in use, so that the electrolyte is melted into an ion conductor. The thermal battery has higher specific energy and specific power, long storage time and normal work in various severe environments, so the thermal battery can be used as a power supply in the fields of missiles, rockets and the like, and has wider application in non-military equipment such as aircraft emergency power supplies and underground high-temperature mine exploration power supplies.
However common halogenationThe melting point of eutectic salt formed by salt is higher, so that the activation temperature of the battery is mostly above 400 ℃, and the high activation temperature brings many adverse effects: 1. more pyrotechnic material is needed inside the battery to reach the required activation temperature, which is not beneficial to the miniaturization of the battery and the improvement of the energy density; 2. the requirements on the heat-insulating layer and the shell of the battery are higher, and the cost of the battery is increased; 3. the application scenes of lower temperature (below 300 ℃) such as oil gas exploitation are not applicable, so that the universality of the thermal battery is not strong; 4. common positive electrode material pyrite (FeS) of thermal battery2) And decompose at higher temperatures, resulting in a loss of battery capacity.
It would be advantageous to solve the above-mentioned problems if the activation temperature of a thermally activated battery could be reduced and flexible control of the thermal activation temperature of the battery could be achieved.
Disclosure of Invention
The invention aims to overcome the defects in the prior art, provides an electrolyte wrapping structure and application thereof, and solves the problem of overhigh activation temperature of a thermally activated battery in the prior art.
One of the technical solutions of the present invention is to provide an electrolyte structure of a thermally activated battery: the electrolyte structure comprises an electrolyte with an ion conduction function and an inert layer which is wrapped outside the electrolyte and does not have the ion conduction function; and below 300 ℃, the inert layer can be converted into a liquid phase from a solid phase under the condition of energy injection.
In a preferred embodiment, the electrolyte is completely encapsulated by the inert layer.
In a preferred embodiment, the electrolyte is in one of three states, liquid, solid and gel.
In preferred embodiments, the injection energy comprises heat or mechanical vibration or ultrasound action.
In a preferred embodiment, the inert layer undergoes a phase transition from a solid phase to a liquid phase upon application of heat or mechanical vibration or ultrasound.
In a preferred embodiment, the inert layer in which the phase transition from the solid phase to the liquid phase occurs is one of a polymer film and an organic substance.
In a preferred embodiment, the polymer film composition is preferably at least one of PE (polyethylene), PP (polypropylene), polyvinyl chloride, polyimide poly, Polyamide (PA), polyvinylidene chloride, polymethylpentene, polyvinylidene fluoride (PVDF), polyethylene terephthalate, polyethylene oxide, polyethylene glycol, polymethyl methacrylate (PMMA), polyethylene terephthalate (PET), polyvinyl butyral (PVB), Polyurethane (PU), polytetrafluoroethylene, polysiloxane, polyacrylonitrile, polypropylene oxide, polyisobutylene, and polyphosphate, and the thickness of the above polymer film is 1nm to 10 μm.
In a preferred embodiment, the organic material is preferably at least one of Ethylene Carbonate (EC), paraffin, and phenol.
In a preferred embodiment, the inert layer without ion conducting effect is dense and does not have a pore structure.
In a preferred embodiment, the inert layer without ion-conducting action has a thickness of 1nm to 500. mu.m.
The second technical scheme of the invention is to provide the application of the electrolyte structure in the battery.
The technical scheme has the following beneficial effects:
1. the electrolyte with the ion conduction function in the battery is completely wrapped by the inert layer without the ion conduction function, so that no ion channel exists in the battery when the battery is stored (not activated), the battery can be stored for a long time without self-discharge, and the electric quantity is not lost;
2. the state of the electrolyte with the ion conducting function wrapped in the inert layer can be a solid state or a liquid state or a gel state, and the universality is strong;
3. the inert layer wrapping the electrolyte and having no ion conduction function can be flexibly selected according to the service environment of the battery, so that the flexible adjustment of the activation temperature and the activation form is realized;
4. the inert layer without ion conduction function can be a polymer film, and the melting point of the polymer can be flexibly adjusted through molecular weight, so that the continuous adjustment of the activation temperature and the activation at a lower temperature of below 200 ℃ are finally realized.
Drawings
The invention is further illustrated by the following figures and examples.
FIG. 1 is a schematic diagram of the electrolyte structure of a thermally activated battery of the present invention.
Fig. 2 is a schematic diagram of a battery comprising an electrolyte structure according to the present invention.
FIG. 3 is a graph of cell voltage as a function of temperature for example 7 (multimeter measured cell voltage, thermometer being the temperature of the environment in which the cell is located).
Fig. 4 discharge curve of the cell in example 11.
Fig. 5 discharge curve of the cell in example 14.
FIG. 6 thermal analysis curve of PE sealing film in example 14.
Detailed Description
The present invention will be described in more detail by way of examples, but the scope of the present invention is not limited to these examples.
Example 1
An electrolyte structure for a thermally activated battery: completely wrapping 1mol/L LiDFOB (lithium bis (fluorooxalato) borate) -PC electrolyte in a PE film.
Example 2
An electrolyte structure for a thermally activated battery: adding EO: li+Peo (litfsi) electrolyte, 15, was completely wrapped in PE film.
Example 3
An electrolyte structure for a thermally activated battery: 1mol/L LiPF6The EC/DMC electrolyte is completely encapsulated in paraffin.
Example 4
An electrolyte structure for a thermally activated battery: EO: li+Peo (litfsi) electrolyte, 15, was completely encapsulated in PP sealing film.
Example 5
An electrolyte structure for a thermally activated battery: a LiCl-KCl (molar ratio LiCl: KCl ═ 58.8:41.2) electrolyte sheet was completely wrapped in the polyimide sealing film.
Example 6
An electrolyte structure for a thermally activated battery: completely wrapping 1mol/L LiDFOB-PVDF-EC/DMC electrolyte in an ethylene terephthalate sealing film.
Example 7
A thermally activated battery: the positive electrode material is mainly V2O5The negative electrode material was mainly Li foil, and the electrolyte structure in example 1 was between the positive electrode material and the negative electrode material. The cell was placed in an oven at 5 ℃/min to 140 ℃ and the open circuit voltage of the cell during the temperature ramp was recorded with a multimeter and the results are shown in fig. 3.
From the multimeter readings, it is known that when the temperature is lower than 132 ℃ (i.e. the inert membrane of the electrolyte outer layer is not melted), the internal ions of the cell are not conducted, the cell is in an inactivated state and does not display a voltage; when the temperature is higher than 132 ℃, the non-ionic conductor film wrapping the electrolyte is melted to form an ion path, and the battery displays normal voltage.
Example 8
A thermally activated battery has a positive electrode made of V2O5The negative electrode material was mainly Li foil, and the electrolyte structure in example 2 was between the positive electrode material and the negative electrode material. The cell was placed in an oven at 5 ℃/min to 140 ℃ and held at temperature, and the open circuit voltage of the cell during the temperature ramp was recorded with a multimeter and reported, with the results shown in table 1. The cell was discharged at 140 ℃ at a rate of 0.2C, and the discharge curve is shown in fig. 4. As can be seen from fig. 4, after the thermally activated battery is activated at a high temperature, the primary battery having the above electrolyte structure is normally discharged at a temperature of 140 ℃, and the specific discharge capacity above the effective voltage (1.5V) is 256 mAh/g.
Example 9
The positive electrode material of soft package battery is mainly V2O5The negative electrode material was mainly Li foil, and the electrolyte structure in example 3 was between the positive electrode material and the negative electrode material. The cell was placed in an oven at 5 ℃/min to 60 ℃ and the open circuit voltage of the cell during the temperature ramp was recorded and the results are shown in table 2.
TABLE 1 variation of cell terminal voltage with temperature in example 8
Table 2 change of terminal voltage of battery with temperature in example 9
| Temperature (. degree.C.) | 25 | 30 | 41.2 | 43 | 60 |
| Voltage (V) | 0.020 | 0.020 | 3.372 | 3.372 | 3.372 |
From both the data of table 1 and table 2, it can be confirmed that the battery including the electrolyte of the structure of the present invention shows a normal operating voltage after being activated.
Example 10
A thermally activated battery with positive electrode made of FeS2The negative electrode material is mainly Li (B) alloy, and electricity in example 4 is provided between the positive electrode material and the negative electrode materialAnd (4) decomposing the material. The cell was placed in an oven at 5 ℃/min to 180 ℃ and held at temperature, the open circuit voltage of the cell during the temperature rise was recorded with a multimeter and discharged at 180 ℃.
Example 11
A thermally activated battery with positive electrode made of FeS2The negative electrode material was mainly li (b) alloy, and the electrolyte structure in example 5 was between the positive electrode material and the negative electrode material. The cell was placed in a muffle furnace at 5 ℃/min to 400 ℃ and held at temperature, the open circuit voltage of the cell during the temperature rise was recorded with a multimeter and the cell was discharged at 400 ℃ with the discharge curve shown in fig. 5. As can be seen from fig. 5, the primary battery having the above electrolyte structure, after being activated at a high temperature, is normally discharged at a temperature of 400 c, and the molten salt electrolyte of the conventional thermal battery is also suitable.
Example 12
A thermally activated battery has a positive electrode made of V2O5The negative electrode material was mainly Li foil, and the electrolyte structure in example 6 was between the positive electrode material and the negative electrode material. The cell was placed in an oven at 5 ℃/min to 200 ℃ and the open circuit voltage of the cell during the temperature ramp was recorded with a multimeter.
Example 13
A conductivity testing apparatus, having the electrolyte structure of example 2 sandwiched between two steel sheets, was placed in an oven and the temperature was raised to 180 ℃ at a rate of 5 ℃/min, and the conductivity of the new electrolyte system at different temperatures was tested and recorded as shown in table 3. The data in table 3 also demonstrate that the electrolyte forms ion channels at high temperatures, enabling ion access inside the cell.
Table 3 conductivity of the structured electrolyte at different temperatures in example 13
| Temperature (. degree.C.) | 0 | 100 | 150 | 180 |
| Conductivity (S/cm) | 0 | 0 | 1.65×10-4 | 1.82×10-4 |
Example 14
The results of thermal analysis of the electrolyte-encapsulating films PE of examples 1, 2 and 13 are shown in fig. 6. It can be seen from the thermal analysis curve of the PE sealing film in fig. 6 that the PE sealing film starts to melt at 120.9 c, i.e., a transition from a solid state to a liquid state occurs, and the PE melts to expose the electrolyte, thereby forming an ion path inside the battery.
Table 4 shows the melting points of different polymers used as inert layers in the electrolyte structure. Because different polymers have different melting points and thus the inert layers have different phase transition temperatures, flexible adjustment of the activation temperature of a thermally activated cell can be achieved by selecting different inert layers.
TABLE 4 melting Point ranges for different polymers
| Class of polymers | PE | PP | PVDF | PMMA | PA | PET |
| Melting Point (. degree.C.) | 120-136 | 148-176 | 156-170 | 130-140 | 215-260 | 225-260 |
The foregoing is for illustrative purposes only, and therefore the scope of the invention should not be limited by this description, and all modifications made within the scope of the invention and the contents of the description should be considered within the scope of the invention.
Claims (9)
1. An electrolyte structure for a thermally activated battery, comprising: the electrolyte structure comprises an electrolyte with an ion conduction function and an inert layer which is wrapped outside the electrolyte and does not have the ion conduction function; and below 300 ℃, the inert layer can be converted into a liquid phase from a solid phase under the condition of energy injection.
2. An electrolyte structure for a thermally activated battery as claimed in claim 1, wherein: the electrolyte is in one of three states, namely a liquid state, a solid state and a gel state.
3. An electrolyte structure for a thermally activated battery as claimed in claim 1, wherein: the injection energy comprises heating or mechanical vibration or ultrasonic action.
4. An electrolyte structure for a thermally activated battery as claimed in claim 1, wherein: the inert layer has a phase change from a solid phase to a liquid phase under the action of heat or mechanical vibration or ultrasonic waves.
5. An electrolyte structure of a thermally activated battery as claimed in claim 4, wherein: the inert layer in which the phase transition from the solid phase to the liquid phase occurs is one of a polymer film and an organic substance.
6. An electrolyte structure for a thermally activated battery as claimed in claim 1, wherein: the inert layer is dense and has no pore structure.
7. An electrolyte structure for a thermally activated battery as claimed in claim 1, wherein: the thickness of the inert layer is 1nm-500 mu m.
8. An electrolyte structure of a thermally activated battery as claimed in claim 7, wherein: the thickness of the polymer film is 1nm-10 mu m.
9. Use of an electrolyte structure according to any of claims 1 to 7 in a battery.
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| Application Number | Priority Date | Filing Date | Title |
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| CN202110231455.4A CN112952125A (en) | 2021-03-02 | 2021-03-02 | Electrolyte structure of thermal activation battery and application thereof |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202110231455.4A CN112952125A (en) | 2021-03-02 | 2021-03-02 | Electrolyte structure of thermal activation battery and application thereof |
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105048004A (en) * | 2015-06-18 | 2015-11-11 | 中国科学院青岛生物能源与过程研究所 | Thermally activated secondary battery using low-temperature molten salt electrolyte |
| CN106602099A (en) * | 2016-11-28 | 2017-04-26 | 中国工程物理研究院电子工程研究所 | Novel reserve cell adopting thermal activation mode |
| WO2020076099A1 (en) * | 2018-10-11 | 2020-04-16 | 주식회사 엘지화학 | Composite electrolyte membrane and all-solid-state battery including said composite electrolyte membrane |
-
2021
- 2021-03-02 CN CN202110231455.4A patent/CN112952125A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105048004A (en) * | 2015-06-18 | 2015-11-11 | 中国科学院青岛生物能源与过程研究所 | Thermally activated secondary battery using low-temperature molten salt electrolyte |
| CN106602099A (en) * | 2016-11-28 | 2017-04-26 | 中国工程物理研究院电子工程研究所 | Novel reserve cell adopting thermal activation mode |
| WO2020076099A1 (en) * | 2018-10-11 | 2020-04-16 | 주식회사 엘지화학 | Composite electrolyte membrane and all-solid-state battery including said composite electrolyte membrane |
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