CN111416155A - Oxide solid electrolyte material and preparation method and application thereof - Google Patents
Oxide solid electrolyte material and preparation method and application thereof Download PDFInfo
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- 239000007784 solid electrolyte Substances 0.000 title claims abstract description 57
- 239000000463 material Substances 0.000 title claims abstract description 30
- 238000002360 preparation method Methods 0.000 title claims abstract description 17
- 238000000034 method Methods 0.000 claims abstract description 28
- 238000000498 ball milling Methods 0.000 claims abstract description 24
- 239000000843 powder Substances 0.000 claims abstract description 23
- 238000001035 drying Methods 0.000 claims abstract description 22
- 239000002001 electrolyte material Substances 0.000 claims abstract description 22
- 238000010304 firing Methods 0.000 claims abstract description 17
- 238000000227 grinding Methods 0.000 claims abstract description 14
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims abstract description 14
- AJNVQOSZGJRYEI-UHFFFAOYSA-N digallium;oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Ga+3].[Ga+3] AJNVQOSZGJRYEI-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910001195 gallium oxide Inorganic materials 0.000 claims abstract description 7
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 claims abstract description 7
- 229910052808 lithium carbonate Inorganic materials 0.000 claims abstract description 7
- 239000003960 organic solvent Substances 0.000 claims abstract description 5
- 229920000642 polymer Polymers 0.000 claims description 29
- 239000007787 solid Substances 0.000 claims description 22
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 18
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical group CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 15
- 238000005266 casting Methods 0.000 claims description 6
- 239000003792 electrolyte Substances 0.000 claims description 5
- 238000004519 manufacturing process Methods 0.000 claims description 4
- 239000000945 filler Substances 0.000 claims description 3
- 238000005119 centrifugation Methods 0.000 claims 1
- 229910052760 oxygen Inorganic materials 0.000 abstract description 5
- 229910052733 gallium Inorganic materials 0.000 abstract description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 3
- 239000001301 oxygen Substances 0.000 abstract description 3
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 abstract description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 2
- 230000015572 biosynthetic process Effects 0.000 abstract description 2
- 229910052746 lanthanum Inorganic materials 0.000 abstract description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 abstract description 2
- 229910052744 lithium Inorganic materials 0.000 abstract description 2
- 230000000877 morphologic effect Effects 0.000 abstract description 2
- 238000010532 solid phase synthesis reaction Methods 0.000 abstract description 2
- 238000003786 synthesis reaction Methods 0.000 abstract description 2
- 239000000470 constituent Substances 0.000 abstract 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 29
- 238000010586 diagram Methods 0.000 description 9
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 7
- 229910001416 lithium ion Inorganic materials 0.000 description 7
- 238000005245 sintering Methods 0.000 description 5
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 4
- 239000000126 substance Substances 0.000 description 3
- 238000003917 TEM image Methods 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 229910021525 ceramic electrolyte Inorganic materials 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 238000000703 high-speed centrifugation Methods 0.000 description 1
- 229910003480 inorganic solid Inorganic materials 0.000 description 1
- 230000037427 ion transport Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000005486 organic electrolyte Substances 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 229920005597 polymer membrane Polymers 0.000 description 1
- -1 polytetrafluoroethylene Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 229910001251 solid state electrolyte alloy Inorganic materials 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
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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
- H01M10/058—Construction or manufacture
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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
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
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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
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
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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
- H01M2300/0088—Composites
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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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- 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
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Abstract
The invention relates to an oxide solid electrolyte material and a preparation method and application thereof, wherein the preparation method of the oxide solid electrolyte material comprises the steps of 1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in an organic solvent, carrying out ball milling, centrifuging and drying, 2) carrying out primary air-firing at 870-1050 ℃, collecting powder, grinding and tabletting, and 3) carrying out secondary air-firing at 950-1050 ℃ to obtain L i19La36Ga7O74Compared with the prior art, the oxide solid electrolyte material is prepared by taking lithium, lanthanum, gallium and oxygen as constituent elements through the solid-phase synthesis reaction at low temperature, has uniform and regular morphological characteristics, is effectively dispersed in the electrolyte material by L a, Ga and O elements, has higher ionic conductivity, and is applied to polymerizationThe solid electrolyte is assembled into the battery, so that the electrochemical performance of the battery can be effectively improved, the preparation process temperature is low, and the synthesis process is simple.
Description
Technical Field
The invention belongs to the technical field of solid electrolyte materials, and relates to an oxide solid electrolyte material, and a preparation method and application thereof.
Background
At present, commercial lithium ion batteries mainly adopt organic electrolyte, and potential safety hazards such as liquid leakage, combustion, explosion and the like exist in unconventional environments. The solid-state battery based on the inorganic solid ceramic electrolyte has important significance for solving the safety problem of the traditional liquid-state battery. In general, solid-state electrolytes should possess high lithium ion conductivity, wide chemical windows, and good chemical stability to the electrode material.
Most studied garnet-structured lithium ion solid electrolyte (L i)7La3Zr2O12LL ZO) has high conductivity (approximately 10%-4S cm-1) The sintering temperature is higher, and is usually more than 1100 ℃, and the current solid-state battery based on LL ZO ceramic has less research work, and the battery performance is not good, so that a great deal of research and improvement are still needed.
Disclosure of Invention
The oxide solid electrolyte material has high ionic conductivity and low sintering temperature, is used as an active filler and added into a polymer solid electrolyte to be finally assembled into a battery, and can effectively improve the electrochemical performance of the battery.
The purpose of the invention can be realized by the following technical scheme:
a method for producing an oxide solid state electrolyte material, the method comprising the steps of:
1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in an organic solvent, and centrifuging and drying after ball milling;
2) carrying out primary air firing at 870 and 930 ℃, and then collecting powder and grinding and tabletting;
3) secondary air-firing at 950-1050 ℃ to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
Further, in the step 1), the organic solvent is isopropanol.
Further, in the step 1), the ball milling is wet ball milling, in the ball milling process, the ball milling rotation speed is 500-.
Further, in the step 1), the centrifugal rotation speed is 7000-9000r/min during the centrifugal process.
Further, in the step 1), the drying temperature is 50-70 ℃ and the drying time is 8-16h in the drying process.
Further, in the step 2), the time of the primary empty burning is 4-6 h; in the step 3), the time of the secondary air-firing is 4-6 h.
An oxide solid electrolyte material is prepared by the method.
The application of an oxide solid electrolyte material as an active filler in the preparation of a polymer solid electrolyte.
A preparation method of a PEO-based polymer solid electrolyte comprises the steps of grinding an oxide solid electrolyte material into powder, adding the powder into acetonitrile together with PEO (polyethylene oxide) and L iTFSI (lithium bis (trifluoromethylsulfonyl) imide), and drawing a film by a solution casting method to obtain the PEO-based polymer solid electrolyte, wherein the weight ratio of the PEO, L iTFSI to the oxide solid electrolyte material is 8:1: 1-5.
A PEO-based polymer solid electrolyte is prepared by the method.
In the invention, the one-time empty sintering is sintering at a slightly low temperature and a slightly high temperature to form the cubic phase solid electrolyte with high lithium ion conductivity, and then sintering at a higher temperature after tabletting is carried out, so that the electrolyte sheet has higher density, thereby better transmitting lithium ions.
Compared with the prior art, the solid electrolyte formed by the four elements has more oxygen vacancies and lithium ion transmission channels, compared with the current LL ZO electrolyte, the oxide solid electrolyte material can be prepared by the solid-phase synthesis reaction at lower temperature in the preparation process, so that the scale is easier, the morphological characteristics are uniform and regular, the L a, Ga and O elements are effectively dispersed in the electrolyte material, and the ionic conductivity is higher (10)-4S/cm) is applied to the polymer solid electrolyte and assembled into a battery, so that the electrochemical performance of the battery can be effectively improved, the preparation process temperature is low, and the synthesis process is simple.
Drawings
Fig. 1 is a TEM image of an oxide solid state electrolyte material produced in example 1;
fig. 2 is an EDS diagram of the oxide solid state electrolyte material produced in example 1;
fig. 3 is an XRD pattern of the oxide solid state electrolyte material prepared in example 1;
FIG. 4 is a cross-sectional and sectional SEM photograph of a PEO-based polymer solid electrolyte prepared in example 1;
FIG. 5 is a resistance diagram of an oxide solid state electrolyte material produced in example 1;
FIG. 6 is an impedance diagram of a PEO-based polymer solid electrolyte prepared in example 1 at 60 ℃;
FIG. 7 is L i/PEO-L iTFSI-L i 19/L iFePO assembled from the PEO-based polymer solid electrolyte prepared in example 14The polymer solid state battery has a power cycle diagram at 70 ℃.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. The present embodiment is implemented on the premise of the technical solution of the present invention, and a detailed implementation manner and a specific operation process are given, but the scope of the present invention is not limited to the following embodiments.
Example 1:
oxide solidThe preparation method of the state electrolyte material comprises the steps of dissolving lithium carbonate, lanthanum oxide and gallium oxide in isopropanol, ball-milling for 24-48 hours by using an isopropanol wet method at the ball-milling rotating speed of 500-800r/min, drying for 12 hours at 60 ℃ after high-speed centrifugation at 8000r/min, then carrying out air firing for 5 hours at 900 ℃, collecting powder, grinding and tabletting, and then carrying out air firing for 5 hours at 950-1050 ℃ to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
Doped L i19La36Ga7O74The PEO-based polymer solid electrolyte is prepared by mixing PEO, L iTFSI and L i19La36Ga7O74Dissolving the oxide solid electrolyte material powder in acetonitrile at a weight ratio of 8:1:1-5, and then drawing a film by adopting a solution casting method to obtain the PEO-based polymer solid electrolyte.
And slicing the obtained film-shaped PEO-based polymer solid electrolyte, and assembling the slice-shaped PEO-based polymer solid electrolyte, a lithium iron phosphate material and a lithium sheet into a full cell. The preparation method of the lithium iron phosphate material comprises the following steps: grinding lithium iron phosphate, acetylene black and a binder (polyvinylidene fluoride, polytetrafluoroethylene or the like) into slurry according to the mass ratio of 8:1:1, then drawing and grinding the slurry on an aluminum foil, and carrying out vacuum drying at 80 ℃ for one night. Cutting the dried lithium iron phosphate material into pieces, and selecting a 2032 battery case to assemble the whole battery in a glove box. The assembled cells were allowed to air for one night and then subjected to electrochemical performance testing using blue dots.
Fig. 1 is a TEM image of the obtained oxide solid electrolyte material, and it can be seen from fig. 1 that the solid electrolyte powder has a particle size of 800 × 400nm, which is small and more favorable for ion transport in the solid phase after tabletting.
Fig. 2 is an EDS diagram of the oxide solid electrolyte material obtained, and it can be seen that lanthanum, gallium and oxygen are distributed more uniformly.
FIG. 3 is an XRD pattern of the obtained oxide solid electrolyte material, and it can be seen from FIG. 3 that XRD peaks of the measured material substantially coincide with main peaks of standard contrast card, indicating that L i was successfully synthesized19La36Ga7O74A substance.
FIG. 4 is the PEO radical producedSEM image of cross section and section of polymer solid electrolyte, as can be seen from FIG. 4, the cross section is flat, L i19La36Ga7O74The powder is uniformly distributed in the polymer electrolyte membrane, and the thickness of the polymer membrane is about 120 mu m according to the section.
FIG. 5 is a resistance diagram of the oxide solid electrolyte material obtained from FIG. 5, as can be seen from L i19La36Ga7O74The resistance value of the electrolyte sheet measured by the blocking electrode method after the sheet was pressed was 830 Ω, and the resistance value of the electrolyte sheet was calculated to be 8 × 10-4S/cm, which is larger than LL ZO type solid electrolyte widely used at present.
FIG. 6 is an impedance diagram of the prepared PEO-based polymer solid electrolyte at 60 deg.C, and it can be seen from FIG. 6 that the impedance value at the left side of the diagram is L i19La36Ga7O74The powder measured was less than the resistance of the right side without powder indicating the addition of L i19La36Ga7O74After the powder is prepared, the impedance value of the system is reduced, and the conduction of lithium ions is facilitated.
FIG. 7 is L i/PEO-L iTFSI-L i 9/L iFePO assembled by prepared PEO-based polymer solid electrolyte4The polymer solid state battery has a power cycle diagram at 70 ℃. As can be seen from fig. 7, the assembled polymer solid-state battery has good cycling stability, can maintain a high specific capacity at 0.5C, has low capacity loss per cycle, and has good rate capability.
Example 2:
an oxide solid state electrolyte material, the preparation method of which comprises the following steps:
1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in isopropanol, performing wet ball milling, centrifuging and drying. In the ball milling process, the ball milling speed is 500r/min, and the ball milling time is 48 h; in the centrifugal process, the centrifugal rotating speed is 7000 r/min; in the drying process, the drying temperature is 70 ℃, and the drying time is 8 h.
2) Carrying out primary air firing at 930 ℃ for 4h, and then collecting powder, grinding and tabletting;
3) at 1050 DEG CCarrying out secondary air-firing for 4h to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
The PEO-based polymer solid electrolyte is prepared by grinding an oxide solid electrolyte material into powder, adding the powder into acetonitrile together with PEO and L iTFSI, wherein the weight ratio of the PEO to L iTFSI to the oxide solid electrolyte material is 8:1:5, and then drawing a film by adopting a solution casting method to obtain the PEO-based polymer solid electrolyte.
Example 3:
an oxide solid state electrolyte material, the preparation method of which comprises the following steps:
1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in isopropanol, performing wet ball milling, centrifuging and drying. In the ball milling process, the ball milling rotating speed is 800r/min, and the ball milling time is 24 h; in the centrifugal process, the centrifugal rotating speed is 9000 r/min; in the drying process, the drying temperature is 50 ℃ and the drying time is 16 h.
2) Carrying out primary air firing at 870 ℃ for 6h, then collecting powder, grinding and tabletting;
3) twice air-firing at 950 ℃ for 6h to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
The PEO-based polymer solid electrolyte is prepared by grinding an oxide solid electrolyte material into powder, adding the powder into acetonitrile together with PEO and L iTFSI, wherein the weight ratio of the PEO to L iTFSI to the oxide solid electrolyte material is 8:1:1, and then drawing a film by adopting a solution casting method to obtain the PEO-based polymer solid electrolyte.
Example 4:
an oxide solid state electrolyte material, the preparation method of which comprises the following steps:
1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in isopropanol, performing wet ball milling, centrifuging and drying. In the ball milling process, the ball milling rotating speed is 600r/min, and the ball milling time is 36 h; in the centrifugal process, the centrifugal rotating speed is 8000 r/min; in the drying process, the drying temperature is 60 ℃, and the drying time is 12 h.
2) Carrying out primary air firing at 900 ℃ for 5h, then collecting powder, grinding and tabletting;
3) twice air-firing at 1000 ℃ for 5h to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
The PEO-based polymer solid electrolyte is prepared by grinding an oxide solid electrolyte material into powder, adding the powder into acetonitrile together with PEO and L iTFSI, wherein the weight ratio of the PEO to L iTFSI to the oxide solid electrolyte material is 8:1:3, and then drawing a film by adopting a solution casting method to obtain the PEO-based polymer solid electrolyte.
The embodiments described above are described to facilitate an understanding and use of the invention by those skilled in the art. It will be readily apparent to those skilled in the art that various modifications to these embodiments may be made, and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above embodiments, and those skilled in the art should make improvements and modifications within the scope of the present invention based on the disclosure of the present invention.
Claims (10)
1. A method for producing an oxide solid electrolyte material, characterized by comprising the steps of:
1) dissolving lithium carbonate, lanthanum oxide and gallium oxide in an organic solvent, and centrifuging and drying after ball milling;
2) carrying out primary air firing at 870 and 930 ℃, and then collecting powder and grinding and tabletting;
3) secondary air-firing at 950-1050 ℃ to obtain L i19La36Ga7O74An oxide solid state electrolyte material.
2. The method for producing an oxide solid state electrolyte material according to claim 1, wherein in step 1), the organic solvent is isopropyl alcohol.
3. The method as claimed in claim 1, wherein the ball milling in step 1) is wet ball milling, the rotation speed of the ball milling is 500-.
4. The method as claimed in claim 1, wherein the centrifugation speed in step 1) is 7000-9000 r/min.
5. The method for producing an oxide solid state electrolyte material according to claim 1, wherein in the step 1), the drying temperature is 50 to 70 ℃ and the drying time is 8 to 16 hours in the drying process.
6. The method for preparing an oxide solid state electrolyte material according to claim 1, wherein in the step 2), the time of the primary air-firing is 4 to 6 hours; in the step 3), the time of the secondary air-firing is 4-6 h.
7. An oxide solid state electrolyte material, characterized in that it is produced by the method according to any one of claims 1 to 6.
8. Use of the oxide solid state electrolyte material of claim 7 as an active filler in the preparation of a polymer solid state electrolyte.
9. A preparation method of a PEO-based polymer solid electrolyte is characterized in that the method comprises the steps of grinding the oxide solid electrolyte material in claim 7 into powder, adding the powder into acetonitrile together with PEO and L iTFSI, and then drawing a film by a solution casting method to obtain the PEO-based polymer solid electrolyte.
10. A PEO-based polymer solid electrolyte prepared by the method of claim 9.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112563575A (en) * | 2020-12-08 | 2021-03-26 | 上海电力大学 | Composite solid electrolyte with transition molybdenum trioxide as filler, preparation method and application |
| CN112573563A (en) * | 2020-12-08 | 2021-03-30 | 上海电力大学 | Lithium ion negative electrode material, battery negative electrode sheet, preparation method and battery |
| CN113161607A (en) * | 2021-02-04 | 2021-07-23 | 广西科技大学 | Preparation method of high-conductivity solid-state battery electrolyte for battery of energy storage charging system |
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| CN111416155B (en) | 2021-10-08 |
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