CN110690437A - Sodium ion battery negative electrode sodium supplement additive, sodium ion battery negative electrode piece and sodium ion battery - Google Patents
Sodium ion battery negative electrode sodium supplement additive, sodium ion battery negative electrode piece and sodium ion battery Download PDFInfo
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- CN110690437A CN110690437A CN201910995953.9A CN201910995953A CN110690437A CN 110690437 A CN110690437 A CN 110690437A CN 201910995953 A CN201910995953 A CN 201910995953A CN 110690437 A CN110690437 A CN 110690437A
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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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
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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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
- 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
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
- 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
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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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
- 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
- H01M4/134—Electrodes based on metals, Si or alloys
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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
- 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
- H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/5805—Phosphides
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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 belongs to the technical field of sodium ion batteries, and particularly relates to a sodium supplement additive for a sodium ion battery negative electrode, a sodium ion battery negative electrode plate and a sodium ion battery. The invention provides an application of sodium phosphide with a carbon-coated structure as a sodium supplement additive for a cathode of a sodium ion battery, which is characterized in that the sodium phosphide with the carbon-coated structure is used for supplementing sodium to a cathode pole piece of the sodium ion battery, so that the cathode contains sodium and the irreversible capacity loss of the sodium ion battery in the first charging and discharging process is supplemented. In the circulation process of the sodium-ion battery, sodium phosphide not only can be used as a sodium source, but also can participate in circulation, and can be used as an active material to provide partial capacity, and the outer carbon of the sodium phosphide with the carbon-coated structure can protect the phosphorus structure to be stable, so that the loss of electric contact with a current collector due to the volume change of phosphorus in the charge-discharge process is prevented.
Description
Technical Field
The invention belongs to the technical field of sodium ion batteries, and particularly relates to a sodium supplement additive for a sodium ion battery negative electrode, a sodium ion battery negative electrode plate and a sodium ion battery.
Background
In order to meet the huge market demand, the energy storage material is gradually developed in the direction of abundant resources and environmental friendliness according to the evaluation standard of electrochemical properties such as energy density, charge-discharge rate and the like. Sodium ion batteries have many advantages over lithium ion batteries, such as: rich sodium resource, low cost, good safety performance and the like. However, sodium ion batteries have a lower theoretical energy density due to the higher relative atomic mass of elemental sodium than lithium. And during the first charging process of the sodium ion battery, sodium ions react with the negative electrode to cause irreversible capacity loss. For example, in a hard carbon negative electrode, the first irreversible capacity loss is as high as 20% or more. Therefore, to increase the energy density of the sodium ion battery, it is necessary to supplement sodium to the sodium ion battery to compensate for the irreversible capacity loss in the first cycle.
At present, two sodium ion battery sodium supplement methods are available, wherein the first method is to add a sodium-rich substance into a positive electrode, and release sodium through electrochemical reaction in the first charging process; the second method is to add sodium simple substance in the negative electrode to directly supplement sodium. However, the first method is not efficient and the remaining portion of inactive species affects the overall energy density; the second method has low safety and affects the subsequent battery assembly process because the activity of the simple substance sodium is high and the method needs to be carried out in an inert atmosphere.
Disclosure of Invention
In view of the above, the invention provides a sodium ion battery negative electrode sodium supplement additive, a sodium ion battery negative electrode plate and a sodium ion battery, which are used for solving the problems that the existing sodium ion battery sodium supplement method is low in efficiency, and the rest of inactive substances or the sodium ion battery needs to be carried out in an inert atmosphere.
The specific technical scheme of the invention is as follows:
the invention provides an application of sodium phosphide with a carbon-coated structure as a sodium supplement additive for a cathode of a sodium-ion battery.
According to the invention, the sodium phosphide with the carbon-coated structure can prevent the sodium phosphide from being decomposed in water, so that the stability of the sodium phosphide is improved, the sodium phosphide with the carbon-coated structure is used as a sodium supplement additive for the negative electrode of the sodium ion battery, and is added into the negative electrode plate of the sodium ion battery to supplement sodium for the negative electrode plate of the sodium ion battery, so that the negative electrode contains sodium, and the irreversible capacity loss of the sodium ion battery in the first charging and discharging process is supplemented. In the circulation process of the sodium-ion battery, sodium phosphide not only can be used as a sodium source, but also can participate in circulation, and can be used as an active material to provide partial capacity, and the outer carbon of the sodium phosphide with the carbon-coated structure can protect the phosphorus structure to be stable, so that the loss of electric contact with a current collector due to the volume change of phosphorus in the charge-discharge process is prevented.
Preferably, the sodium phosphide with the carbon-coated structure is in a core-shell structure, the core is sodium phosphide, and the shell layer is a carbon layer. The sodium phosphide with a carbon-coated structure is Na3P @ C. The carbon layer can prevent sodium phosphide from being decomposed in water as a protective layer, and can prevent the sodium phosphide from being structurally damaged in the circulation process of the sodium battery and losing electrical contact with the negative electrode as a skeleton of the sodium phosphide.
In the invention, the sodium phosphide with a carbon-coated structure is obtained by uniformly coating carbon with sodium phosphide in a drying environment, the humidity of the drying environment is preferably less than 10%, and carbon coating can be carried out by a ball milling method, a chemical vapor deposition method or a high-temperature pyrolysis method.
Preferably, the particle size of the sodium phosphide with the carbon coating structure is 0.1-100 μm, and more preferably 0.1-10 μm;
the thickness of the shell layer is 20nm to 800nm, and more preferably 100nm to 500 nm.
Preferably, the carbon accounts for 0.5-10% of the mass of the sodium phosphide with the carbon-coated structure, and more preferably 2-8%.
In the invention, the sodium phosphide with the carbon-coated structure can be obtained by ball milling of carbon and sodium phosphide or by mixing sodium phosphide and a carbon source and then carbonizing in a protective atmosphere.
The invention also provides a sodium ion battery negative pole piece which comprises a sodium ion battery negative pole sodium supplement additive;
the sodium supplement additive for the cathode of the sodium ion battery is sodium phosphide with a carbon-coated structure.
Preferably, the sodium supplement additive for the negative electrode of the sodium-ion battery is doped in the negative electrode active material;
the sodium supplement additive for the negative electrode of the sodium-ion battery accounts for 0.1-20% of the mass of the negative electrode active material.
In the invention, sodium phosphide with a carbon-coated structure is used as a sodium supplement additive of the negative electrode of the sodium-ion battery and added into a negative electrode active material in a dry environment to prepare the negative electrode plate of the sodium-ion battery, and the humidity of the dry environment is preferably below 30%.
Preferably, the anode active material includes one or more of hard carbon, a simple metal, an oxygen-containing compound, and a sulfide.
The invention also provides a sodium ion battery, which comprises the negative pole piece and the positive pole piece of the sodium ion battery.
Preferably, the capacity ratio of the negative electrode plate of the sodium-ion battery to the positive electrode plate of the sodium-ion battery is 1: 1-1.2: 1, and more preferably 1.05: 1-1.1: 1.
Preferably, the positive active material of the positive pole piece comprises one or more of prussian blue compounds, sodium phosphate salts, sodium sulfate salts and layered oxygen-containing sodium salts.
The sodium ion battery comprises a positive pole piece, a negative pole piece, a diaphragm, electrolyte and a shell, wherein the active material of the negative pole piece comprises one or more of hard carbon, a metal simple substance, an oxygen-containing compound and a sulfide, and the metal simple substance is preferably Sn and/or Sb; the oxygen-containing compound is preferably Na2Ti3O7、NaTi2(PO4)3CuO and SnO2One or more of; the sulfide is preferably MoS2、Sb2S3And SnS2One or more of (a).
The positive pole piece active material comprises one or more of Prussian blue compounds, sodium phosphate, sodium sulfate and layered oxygen-containing sodium salt; the Prussian blue compound is preferably AxMM’(CN)6A is Na or K, MM' is Fe, Co, Mn or Ni, and x is more than or equal to 1 and less than or equal to 2; the sodium phosphate salt is preferably Na3V2(PO4)3Or Na3M2(PO4)2F3M is Ti, Fe or V; the sodium sulfate is Na2My(SO4)2·(H2O)2M is a transition metal, y is more than or equal to 0.5 and less than or equal to 1; the layered oxygen-containing sodium salt is NaxMO2M is preferably Ni, Ti, Co, Mn or Fe, and x is 0.4. ltoreq. x.ltoreq.1.
In summary, the invention provides the application of the sodium phosphide with the carbon-coated structure as the sodium supplement additive for the cathode of the sodium ion battery, the sodium phosphide with the carbon-coated structure can avoid the sodium phosphide from being decomposed in water, so that the stability of the sodium phosphide is improved, the sodium phosphide with the carbon-coated structure is used as the sodium supplement additive for the cathode of the sodium ion battery and is added into the cathode pole piece of the sodium ion battery, the sodium supplement is carried out on the cathode pole piece of the sodium ion battery, the cathode contains sodium, and the irreversible capacity loss of the sodium ion battery in the first charge and discharge process is supplemented. In the circulation process of the sodium-ion battery, sodium phosphide not only can be used as a sodium source, but also can participate in circulation, and can be used as an active material to provide partial capacity, and the outer carbon of the sodium phosphide with the carbon-coated structure can protect the phosphorus structure to be stable, so that the loss of electric contact with a current collector due to the volume change of phosphorus in the charge-discharge process is prevented.
Detailed Description
The invention provides a sodium ion battery cathode sodium supplement additive, a sodium ion battery cathode pole piece and a sodium ion battery, which are used for solving the problems that the efficiency is not high and the rest of inactive substances or the sodium ion battery needs to be carried out in an inert atmosphere in the conventional sodium ion battery sodium supplement method.
The technical solutions in the embodiments of the present invention will be clearly and completely described below, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all 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.
Example 1
Mixing amorphous carbon and sodium phosphide according to a mass ratio of 1: 9, mixing, putting into a ball milling tank, introducing dry air for protection, and ball milling at 1000rpm for 30min to obtain sodium phosphide with a carbon-coated structure, namely Na3P @ C. The sodium phosphide with the carbon-coated structure is of a core-shell structure, the average grain diameter of the sodium phosphide with the carbon-coated structure is 10 mu m, and the thickness of a shell layer is 100 nm. The carbon accounts for 5 wt% of the mass of the sodium phosphide with the carbon-coated structure.
Mixing Na3P @ C is added into a negative active material as a sodium supplement additive of a negative electrode of the sodium-ion battery, and Na3P @ C accounts for 5 wt% of the mass of the negative active material, the negative active material is hard carbon, a negative pole piece of the sodium ion battery is prepared, then the sodium ion battery is assembled, the sodium ion battery is obtained, and the capacity ratio of the negative pole piece to the positive pole piece in the sodium ion battery is 1: 1.
example 2
Adding 1 g of Na3Mixing P with 0.2 g polyacrylonitrile, ball milling at 800rpm for 60min, placing the mixture in a tube furnace, carbonizing at 600 deg.C for 5 hr under argon atmosphere, and naturally cooling to room temperature to obtain the final productTo Na3P @ C, carbon in Na38 wt% of P @ C, Na3The particle size of P @ C is 2-15 mu m. The preparation methods of the negative pole piece and the sodium-ion battery are the same as those of the embodiment 1.
Example 3
Adding 1 g of Na3Mixing P with 0.2 g polyacrylonitrile, ball milling at 800rpm for 60min, placing the mixture in a tube furnace, carbonizing at 600 deg.C for 5 hr under argon atmosphere, and naturally cooling to room temperature to obtain Na3P @ C, carbon in Na38 wt% of P @ C, Na3The particle size of P @ C is 2-15 mu m. The preparation methods of the negative electrode plate and the sodium-ion battery are the same as those in example 1, except that the capacity ratio of the negative electrode plate to the positive electrode plate in the sodium-ion battery is 1.05: 1.
comparative example 1
The preparation of the negative electrode plate of the sodium-ion battery of the comparative example and the preparation of the sodium-ion battery are the same as those of the example 1, except that Na is not added into the negative electrode plate3P@C。
Comparative example 2
The preparation of the negative pole piece of the sodium-ion battery of the comparative example and the preparation of the sodium-ion battery are the same as those of the example 1, except that the sodium supplement additive added into the positive pole piece is 5 wt% of Na2S。
Example 4
The first coulombic efficiency test was performed on the sodium-ion batteries of examples 1-3 and comparative examples 1-2, and the results are shown in Table 1. compared with comparative example 1, the sodium-ion battery of the present invention uses Na3After P @ C is used for sodium supplement, the first-week coulombic efficiency is obviously improved, and compared with the comparative example 2, Na is adopted3P @ C for sodium supplement compared with Na2S is more beneficial to improving the first-week coulombic efficiency of the sodium-ion battery.
TABLE 1 first week coulombic efficiency test results of examples 1-3 and comparative examples 1-2 sodium ion batteries
| Example 1 | Example 2 | Example 3 | Comparative example 1 | Comparative example 2 | |
| First week coulombic efficiency | 78％ | 75％ | 80％ | 62％ | 71％ |
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (10)
1. The sodium phosphide with a carbon-coated structure is used as a sodium supplement additive for a cathode of a sodium ion battery.
2. The use according to claim 1, wherein the sodium phosphide of the carbon-coated structure is in a core-shell structure, the core is sodium phosphide and the shell layer is a carbon layer.
3. The use according to claim 2, wherein the particle size of the sodium phosphide of the carbon-coated structure is 0.1-100 μm;
the thickness of the shell layer is 20 nm-800 nm.
4. The use according to claim 1, wherein carbon comprises 0.5-10% by mass of the sodium phosphide of the carbon-coated structure.
5. A negative pole piece of a sodium ion battery is characterized by comprising a sodium supplement additive of the negative pole of the sodium ion battery;
the sodium supplement additive for the cathode of the sodium ion battery is sodium phosphide with a carbon-coated structure.
6. The negative pole piece of the sodium-ion battery of claim 5, wherein the sodium-ion battery negative sodium supplement additive is doped in the negative active material;
the sodium supplement additive for the negative electrode of the sodium-ion battery accounts for 0.1-20% of the mass of the negative electrode active material.
7. The negative electrode plate of the sodium-ion battery as claimed in claim 6, wherein the negative active material comprises one or more of hard carbon, elemental metal, oxygen-containing compound and sulfide.
8. A sodium-ion battery, characterized by comprising the negative electrode plate of the sodium-ion battery and the positive electrode plate of the sodium-ion battery according to any one of claims 5 to 7.
9. The sodium-ion battery of claim 8, wherein the capacity ratio of the negative pole piece to the positive pole piece is 1: 1-1.2: 1.
10. The sodium-ion battery of claim 9, wherein the positive active material of the positive pole piece of the sodium-ion battery comprises one or more of a prussian blue compound, a sodium phosphate salt, a sodium sulfate salt, and a layered oxygen-containing sodium salt.
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113644271A (en) * | 2021-08-12 | 2021-11-12 | 山东玉皇新能源科技有限公司 | Sodium supplement additive for negative electrode of sodium ion battery and negative electrode material |
| CN113793979A (en) * | 2021-08-18 | 2021-12-14 | 东莞塔菲尔新能源科技有限公司 | Secondary battery and power utilization device |
| CN114430061A (en) * | 2021-12-15 | 2022-05-03 | 深圳先进技术研究院 | Sodium-based dual-ion battery and preparation method thereof |
| CN114709368A (en) * | 2021-06-26 | 2022-07-05 | 宁德时代新能源科技股份有限公司 | Negative pole piece of sodium ion battery, electrochemical device and electronic equipment |
| CN115275191A (en) * | 2022-09-26 | 2022-11-01 | 江苏正力新能电池技术有限公司 | Negative electrode material, negative plate and sodium ion battery |
| CN116632220A (en) * | 2023-07-21 | 2023-08-22 | 宁德时代新能源科技股份有限公司 | Sodium supplementing material, preparation method thereof, positive electrode plate, electrode assembly, battery and electricity utilization device |
| CN116936775A (en) * | 2023-09-15 | 2023-10-24 | 宁德时代新能源科技股份有限公司 | Negative electrode material, preparation method thereof, negative electrode plate, battery and power utilization device |
| CN117199575A (en) * | 2023-11-07 | 2023-12-08 | 浙江帕瓦新能源股份有限公司 | Negative electrode plate, preparation method thereof and sodium ion battery |
| CN117199575B (en) * | 2023-11-07 | 2024-04-19 | 浙江帕瓦新能源股份有限公司 | Negative electrode plate, preparation method thereof and sodium ion battery |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114709368A (en) * | 2021-06-26 | 2022-07-05 | 宁德时代新能源科技股份有限公司 | Negative pole piece of sodium ion battery, electrochemical device and electronic equipment |
| CN113644271A (en) * | 2021-08-12 | 2021-11-12 | 山东玉皇新能源科技有限公司 | Sodium supplement additive for negative electrode of sodium ion battery and negative electrode material |
| CN113644271B (en) * | 2021-08-12 | 2023-03-14 | 山东玉皇新能源科技有限公司 | Sodium supplement additive for negative electrode of sodium ion battery and negative electrode material |
| CN113793979A (en) * | 2021-08-18 | 2021-12-14 | 东莞塔菲尔新能源科技有限公司 | Secondary battery and power utilization device |
| CN114430061A (en) * | 2021-12-15 | 2022-05-03 | 深圳先进技术研究院 | Sodium-based dual-ion battery and preparation method thereof |
| WO2023109708A1 (en) * | 2021-12-15 | 2023-06-22 | 深圳先进技术研究院 | Sodium-based dual-ion battery and preparation method therefor |
| CN115275191A (en) * | 2022-09-26 | 2022-11-01 | 江苏正力新能电池技术有限公司 | Negative electrode material, negative plate and sodium ion battery |
| CN116632220A (en) * | 2023-07-21 | 2023-08-22 | 宁德时代新能源科技股份有限公司 | Sodium supplementing material, preparation method thereof, positive electrode plate, electrode assembly, battery and electricity utilization device |
| CN116936775A (en) * | 2023-09-15 | 2023-10-24 | 宁德时代新能源科技股份有限公司 | Negative electrode material, preparation method thereof, negative electrode plate, battery and power utilization device |
| CN117199575A (en) * | 2023-11-07 | 2023-12-08 | 浙江帕瓦新能源股份有限公司 | Negative electrode plate, preparation method thereof and sodium ion battery |
| CN117199575B (en) * | 2023-11-07 | 2024-04-19 | 浙江帕瓦新能源股份有限公司 | Negative electrode plate, preparation method thereof and sodium ion battery |
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