CN114613946A - Manufacturing method of electrode pole piece of sodium-ion battery and semisolid sodium-ion battery - Google Patents
Manufacturing method of electrode pole piece of sodium-ion battery and semisolid sodium-ion battery Download PDFInfo
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- CN114613946A CN114613946A CN202210359527.8A CN202210359527A CN114613946A CN 114613946 A CN114613946 A CN 114613946A CN 202210359527 A CN202210359527 A CN 202210359527A CN 114613946 A CN114613946 A CN 114613946A
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- ion battery
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- 229910001415 sodium ion Inorganic materials 0.000 title claims abstract description 37
- FKNQFGJONOIPTF-UHFFFAOYSA-N Sodium cation Chemical compound [Na+] FKNQFGJONOIPTF-UHFFFAOYSA-N 0.000 title claims abstract description 29
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 25
- 238000006243 chemical reaction Methods 0.000 claims abstract description 27
- 238000000034 method Methods 0.000 claims abstract description 21
- 239000007772 electrode material Substances 0.000 claims abstract description 18
- 239000000463 material Substances 0.000 claims abstract description 15
- 229920001940 conductive polymer Polymers 0.000 claims abstract description 14
- 239000011258 core-shell material Substances 0.000 claims abstract description 14
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 14
- 239000007787 solid Substances 0.000 claims abstract description 12
- 238000001035 drying Methods 0.000 claims abstract description 9
- 238000005098 hot rolling Methods 0.000 claims abstract description 9
- 239000000843 powder Substances 0.000 claims abstract description 9
- 239000002562 thickening agent Substances 0.000 claims abstract description 9
- POAOYUHQDCAZBD-UHFFFAOYSA-N 2-butoxyethanol Chemical compound CCCCOCCO POAOYUHQDCAZBD-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000007810 chemical reaction solvent Substances 0.000 claims abstract description 7
- 238000010438 heat treatment Methods 0.000 claims abstract description 7
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 claims abstract description 5
- 239000012736 aqueous medium Substances 0.000 claims abstract description 5
- 239000011230 binding agent Substances 0.000 claims abstract description 5
- 239000011267 electrode slurry Substances 0.000 claims abstract description 5
- 239000003999 initiator Substances 0.000 claims abstract description 5
- 238000002156 mixing Methods 0.000 claims abstract description 5
- 239000000203 mixture Substances 0.000 claims abstract description 5
- 239000000178 monomer Substances 0.000 claims abstract description 5
- 150000003254 radicals Chemical class 0.000 claims abstract description 5
- 238000012216 screening Methods 0.000 claims abstract description 5
- 239000011257 shell material Substances 0.000 claims abstract description 5
- 159000000000 sodium salts Chemical class 0.000 claims abstract description 5
- 239000011734 sodium Substances 0.000 claims description 5
- 229910021385 hard carbon Inorganic materials 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- -1 sodium ion compound Chemical class 0.000 claims description 3
- 229910021384 soft carbon Inorganic materials 0.000 claims description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 2
- 238000002844 melting Methods 0.000 claims description 2
- 230000008018 melting Effects 0.000 claims description 2
- 239000007784 solid electrolyte Substances 0.000 claims description 2
- 230000002441 reversible effect Effects 0.000 abstract description 6
- 239000007773 negative electrode material Substances 0.000 description 9
- 229910020288 Na2Ti6O13 Inorganic materials 0.000 description 4
- 239000003792 electrolyte Substances 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 229910052744 lithium Inorganic materials 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 229910001416 lithium ion Inorganic materials 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 238000012512 characterization method Methods 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 239000002322 conducting polymer Substances 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 239000002001 electrolyte material Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- 238000003780 insertion Methods 0.000 description 1
- 230000037431 insertion Effects 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000013589 supplement Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
-
- 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
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/137—Electrodes based on electro-active polymers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1399—Processes of manufacture of electrodes based on electro-active polymers
Abstract
The invention discloses a manufacturing method of a sodium ion battery electrode plate and a semisolid sodium ion battery, wherein the method comprises the steps of adding ethylene glycol monobutyl ether into a reaction kettle, adding a free radical initiator into an acrylate monomer mixture, dissolving uniformly and then dripping into the reaction kettle; the polymer electrolyte is prepared by taking a high molecular material as a framework material and embedding sodium salt; dissolving polymer electrolyte in a reaction kettle, sequentially heating, drying, vacuumizing, and removing a reaction solvent to obtain an ionic conductive polymer; preparing a shell by using an ionic conductive polymer, and wrapping an electrode material to form a core-shell material; preparing an aqueous electrode slurry by mixing a screen-passing part, which is obtained by screening a thickener powder containing a core-shell material, with an electrode active material, an aqueous binder, a screen-passing part, and an aqueous medium; and carrying out hot rolling treatment on the coated pole piece to obtain an electrode pole piece, so that the first reversible capacity of the semi-solid battery is higher.
Description
Technical Field
The invention relates to the technical field of sodium ion batteries, in particular to a manufacturing method of a sodium ion battery electrode plate and a semisolid sodium ion battery.
Background
In the current art, a sodium ion battery is a battery in which sodium ions migrate between a positive electrode and a negative electrode. Since Na is present in a larger amount than Li, sodium ion batteries have an advantage that cost reduction is easier to achieve than lithium ion batteries.
In general, a sodium ion battery has a positive electrode active material layer containing a positive electrode active material, a negative electrode active material layer containing a negative electrode active material, and an electrolyte layer formed between the positive electrode active material layer and the negative electrode active material layer.
Prior art document, patent document 1: japanese patent laid-open publication No. 2009-117259 and patent document 2: japanese patent application laid-open publication No. 2011-: japanese patent laid-open publication No. 2007-048682;
non-patent document 1: trinh et al, "Synthesis, Characterization and Electrochemical students of Active Materials for Sodium Ion Batteries", ECS Transactions,35(32) (2011)
Non-patent document 2: J.C. Perez-Flores et al, "On the Mechanism of Lithium Insertion inter A2Ti6O13(A = Na, Li)", ECS Transactions,41 (41)195-
Na2Ti6O13 is known as a negative electrode active material used in a sodium ion battery. For example, non-patent document 1 discloses a sodium ion battery using Na2Ti6O13 as a negative electrode active material. Although not a sodium ion battery, non-patent document 2 discloses a lithium ion battery using Na2Ti6O13 as a negative electrode active material. The same description is also given in the prior art of patent document 1. Patent document 2 discloses a sodium ion battery using lithium titanate (Li 4Ti5O 12) as a negative electrode active material. Patent document 3 discloses that an active material and a carbon material are combined by a ball mill.
Non-patent document 1 discloses a sodium ion battery using Na2Ti6O13 as a negative electrode active material. However, as documented in Figure8, the initial charge-discharge efficiency of the cell was as low as about 27% and the reversible capacity was as low as about 20 mAh/g.
The current solid-state batteries are mainly divided into the following types according to the material types: a polymer solid-state battery; (ii) an oxide solid state battery; and thirdly, sulfide solid-state batteries. Wherein, the stability of the oxide is better, but the conductivity of the electrolyte is low, and the same level as that of the traditional electrolyte can not be achieved; although the conductivity of the sulfide electrolyte is high, hydrogen sulfide gas can be generated due to instability in water and air, and the harm to a human body is very large; the polymer electrolyte has higher conductivity, lower material density, lower requirement on air moisture and simple process production, and is called as an electrolyte material with wider application.
The solid-state battery can be divided into a semi-solid battery and an all-solid battery in terms of the manufacturing method. The positive and negative diaphragms of the all-solid-state battery are in solid-solid contact, so that Na + conduction resistance is high, and the performance of the all-solid-state battery is difficult to reach the level of the traditional liquid battery; the semi-solid battery is used as a transition state between the traditional liquid battery and the all-solid battery, the operability of the preparation, the rate performance and the cycle performance of the battery are very close to those of the traditional liquid battery, and the safety performance of the semi-solid battery is better than that of the traditional liquid battery.
The silicon negative electrode has high theoretical specific capacity (up to 4200mAh/g), but has a serious problem of volume expansion and low first reversible capacity, which is because silicon is alloyed with sodium ions in the charging and discharging processes, most of the sodium ions are difficult to be separated out after entering, and the first reversible capacity is reduced, so that the supplement of the sodium ions to the negative electrode material is the key for improving the first reversible capacity.
The information disclosed in this background section is only for enhancement of understanding of the general background of the invention and should not be taken as an acknowledgement or any form of suggestion that this information forms the prior art already known to a person skilled in the art.
Disclosure of Invention
In order to meet the above requirements, a first object of the present invention is to provide a method for manufacturing an electrode plate of a sodium-ion battery, comprising:
adding ethylene glycol monobutyl ether into a reaction kettle, adding a free radical initiator into an acrylate monomer mixture, uniformly dissolving, and then dripping into the reaction kettle;
preparing a polymer electrolyte by taking a high molecular material as a framework material and embedding sodium salt;
dissolving the polymer electrolyte in the reaction kettle, sequentially heating, drying and vacuumizing, and removing a reaction solvent to obtain an ionic conductive polymer;
preparing a shell by using the ionic conductive polymer, and wrapping an electrode material to form a core-shell material;
preparing an aqueous electrode slurry by mixing a screen-passing part in which a thickener powder containing the core-shell material is obtained by screening the thickener powder, and an electrode active material, an aqueous binder, the screen-passing part, and an aqueous medium;
and carrying out hot rolling treatment on the coated pole piece to obtain the electrode pole piece.
According to an embodiment of the present invention, the step of adding ethylene glycol monobutyl ether to the reaction kettle comprises raising the temperature inside the reaction kettle to 70-100 ℃.
According to an embodiment of the present invention, the step of dissolving the polymer electrolyte in the reaction kettle comprises a reaction temperature of 50 ℃ to 55 ℃.
According to an embodiment of the invention, said step of removing the reaction solvent is preceded by a drying at 70 ℃ to 75 ℃ for 20 hours.
According to the embodiment of the invention, when the method is used for manufacturing the positive pole piece, the electrode material comprises any one or more of Prussian white and a layered oxide sodium ion compound.
According to the embodiment of the invention, when the method is used for manufacturing the negative pole piece, the electrode material comprises any one or more of hard carbon and soft carbon.
According to an embodiment of the invention, the step of hot rolling the coated pole piece comprises melting the ion-conducting polymer to form a sodium ion conducting network.
According to an embodiment of the present invention, the step of performing hot rolling treatment on the coated pole piece includes uniformly distributing the core-shell material in the electrode pole piece.
In another aspect, a second objective of the present invention is to provide a semi-solid sodium-ion battery, including a positive electrode plate and a negative electrode plate manufactured by the manufacturing method described in any one of the above.
According to the embodiment of the invention, the battery is in a layered structure of a positive pole piece, a semi-solid electrolyte material and a negative pole piece.
Compared with the prior art, the invention has the beneficial effects that: according to the manufacturing method of the sodium battery electrode piece, the polymer electrolyte in the electrode piece is uniformly dispersed and has higher compaction density, and the normal migration of sodium ions in the electrode piece is ensured, so that the first reversible capacity of the semi-solid battery is higher.
Additional aspects and advantages of the invention will be set forth in part in the description which follows and, in part, will be obvious from the description, or may be learned by practice of the invention.
The invention is further described below with reference to the accompanying drawings and specific embodiments.
Drawings
FIG. 1 is a schematic flow chart of a method for manufacturing an electrode plate of a sodium-ion battery according to the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the description herein, references to the description of the term "one embodiment," "some embodiments," "an example," "a specific example," or "some examples," etc., mean that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the invention. In this specification, the schematic representations of the terms used above should not be understood to necessarily refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples described in this specification can be combined and combined by those skilled in the art.
Example one
As shown in fig. 1, the present embodiment provides a method for manufacturing an electrode plate of a sodium-ion battery, which specifically includes:
adding ethylene glycol monobutyl ether into a reaction kettle, heating the interior of the reaction kettle to 75 ℃, adding a free radical initiator into an acrylate monomer mixture, uniformly dissolving, and then dripping into the reaction kettle, wherein the reaction temperature is 53 ℃; preparing a polymer electrolyte by taking a high molecular material as a framework material and embedding sodium salt; dissolving the polymer electrolyte in the reaction kettle, sequentially heating, drying, vacuumizing, drying at 72 ℃ for 20 hours, and removing the reaction solvent to obtain the ionic conductive polymer; preparing a shell by using the ionic conductive polymer, and wrapping an electrode material to form a core-shell material; preparing an aqueous electrode slurry by mixing a screen-passing part in which a thickener powder containing the core-shell material is obtained by screening the thickener powder, and an electrode active material, an aqueous binder, the screen-passing part, and an aqueous medium; and carrying out hot rolling treatment on the coated pole piece, so that the core-shell material is uniformly distributed in the electrode pole piece, and further the ion conductive polymer is melted to form a sodium ion conductive network, so as to obtain the electrode pole piece.
When the method is used for manufacturing the positive pole piece, the electrode material comprises Prussian white. When the method is used for manufacturing a negative pole piece, the electrode material comprises hard carbon.
Example two
A manufacturing method of an electrode plate of a sodium-ion battery comprises the following steps:
adding ethylene glycol monobutyl ether into a reaction kettle, heating the interior of the reaction kettle to 80 ℃, adding a free radical initiator into the acrylate monomer mixture, uniformly dissolving, and then dripping into the reaction kettle, wherein the reaction temperature is 54 ℃; preparing a polymer electrolyte by taking a high molecular material as a framework material and embedding sodium salt; dissolving the polymer electrolyte in the reaction kettle, sequentially heating, drying, vacuumizing, drying at 73 ℃ for 18 hours, and removing the reaction solvent to obtain the ionic conductive polymer; preparing a shell by using the ionic conductive polymer, and wrapping an electrode material to form a core-shell material; preparing an aqueous electrode slurry by mixing a screen-passing part in which a thickener powder containing the core-shell material is obtained by screening the thickener powder, and an electrode active material, an aqueous binder, the screen-passing part, and an aqueous medium; and carrying out hot rolling treatment on the coated pole piece, so that the core-shell material is uniformly distributed in the electrode pole piece, and further the ion conductive polymer is melted to form a sodium ion conductive network, so as to obtain the electrode pole piece.
When the method is used for manufacturing the positive pole piece, the electrode material comprises a layered oxide sodium ion compound. When the method is used for manufacturing the negative pole piece, the electrode material comprises soft carbon.
It should be noted that, as can be clearly understood by those skilled in the art, the specific implementation process of the electronic module may refer to the corresponding description in the foregoing method embodiment, and for convenience and brevity of description, no further description is provided herein.
The steps in the method of the embodiment of the invention can be sequentially adjusted, combined and deleted according to actual needs.
Various other modifications and changes may be made by those skilled in the art based on the above-described technical solutions and concepts, and all such modifications and changes should fall within the scope of the claims of the present invention.
Claims (10)
1. A manufacturing method of an electrode plate of a sodium-ion battery is characterized by comprising the following steps:
adding ethylene glycol monobutyl ether into a reaction kettle, adding a free radical initiator into the acrylate monomer mixture, uniformly dissolving, and then dripping into the reaction kettle;
preparing a polymer electrolyte by taking a high molecular material as a framework material and embedding sodium salt;
dissolving the polymer electrolyte in the reaction kettle, sequentially heating, drying and vacuumizing, and removing a reaction solvent to obtain an ionic conductive polymer;
preparing a shell by using the ionic conductive polymer, and wrapping an electrode material to form a core-shell material;
preparing an aqueous electrode slurry by mixing a screen-passing part in which a thickener powder containing the core-shell material is obtained by screening the thickener powder, and an electrode active material, an aqueous binder, the screen-passing part, and an aqueous medium;
and carrying out hot rolling treatment on the coated pole piece to obtain the electrode pole piece.
2. The method according to claim 1, wherein the step of adding ethylene glycol monobutyl ether to the reaction vessel includes raising the temperature inside the reaction vessel to 70 ℃ to 100 ℃.
3. The method of claim 1, wherein the step of dissolving the polymer electrolyte in the reaction vessel comprises a reaction temperature of 50 ℃ to 55 ℃.
4. The method of claim 1, wherein the step of removing the reaction solvent is preceded by a drying at 70 ℃ to 75 ℃ for 20 hours.
5. The manufacturing method according to claim 1, wherein when the method is used for manufacturing a positive electrode plate, the electrode material comprises any one or more of Prussian white and a layered oxide sodium ion compound.
6. The manufacturing method of claim 1, wherein when the method is used for manufacturing a negative pole piece, the electrode material comprises any one or more of hard carbon and soft carbon.
7. A method of making as set forth in claim 1, wherein the step of hot rolling the coated pole piece includes melting the ionically conductive polymer to form a sodium ionically conductive network.
8. The method of claim 1, wherein the step of hot rolling the coated pole piece comprises uniformly distributing the core-shell material in the electrode pole piece.
9. A semi-solid sodium ion battery, characterized by comprising a positive electrode plate and a negative electrode plate manufactured by the manufacturing method of any one of claims 1 to 8.
10. The semi-solid sodium-ion battery of claim 9, wherein the battery is a layered structure of positive electrode sheet-semi-solid electrolyte material-negative electrode sheet.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210359527.8A CN114613946A (en) | 2022-04-07 | 2022-04-07 | Manufacturing method of electrode pole piece of sodium-ion battery and semisolid sodium-ion battery |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202210359527.8A CN114613946A (en) | 2022-04-07 | 2022-04-07 | Manufacturing method of electrode pole piece of sodium-ion battery and semisolid sodium-ion battery |
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-
2022
- 2022-04-07 CN CN202210359527.8A patent/CN114613946A/en active Pending
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