CN117476923A - Positive electrode material composition with high battery energy density, positive electrode sheet and sodium ion battery - Google Patents
Positive electrode material composition with high battery energy density, positive electrode sheet and sodium ion battery Download PDFInfo
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- FKNQFGJONOIPTF-UHFFFAOYSA-N Sodium cation Chemical compound [Na+] FKNQFGJONOIPTF-UHFFFAOYSA-N 0.000 title claims abstract description 171
- 229910001415 sodium ion Inorganic materials 0.000 title claims abstract description 171
- 239000007774 positive electrode material Substances 0.000 title claims abstract description 38
- 239000000203 mixture Substances 0.000 title claims abstract description 36
- 239000011734 sodium Substances 0.000 claims abstract description 37
- 239000002245 particle Substances 0.000 claims abstract description 31
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 26
- 239000011572 manganese Substances 0.000 claims description 26
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 16
- 229910052748 manganese Inorganic materials 0.000 claims description 15
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 14
- -1 sodium nickel copper iron manganese oxide Chemical compound 0.000 claims description 10
- 239000010949 copper Substances 0.000 claims description 9
- 229910052742 iron Inorganic materials 0.000 claims description 9
- 239000011575 calcium Substances 0.000 claims description 8
- 239000011651 chromium Substances 0.000 claims description 8
- 239000011133 lead Substances 0.000 claims description 8
- 239000010936 titanium Substances 0.000 claims description 8
- 239000011230 binding agent Substances 0.000 claims description 7
- 239000006258 conductive agent Substances 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 7
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 6
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 6
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 6
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 6
- 229910052791 calcium Inorganic materials 0.000 claims description 6
- 229910052804 chromium Inorganic materials 0.000 claims description 6
- 229910017052 cobalt Inorganic materials 0.000 claims description 6
- 239000010941 cobalt Substances 0.000 claims description 6
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 6
- 229910052759 nickel Inorganic materials 0.000 claims description 6
- 229910052712 strontium Inorganic materials 0.000 claims description 6
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 6
- 229910052719 titanium Inorganic materials 0.000 claims description 6
- WFSRWJJESXWWSH-UHFFFAOYSA-N [O-2].[Fe+2].[Mn+2].[Ni+2].[Na+] Chemical compound [O-2].[Fe+2].[Mn+2].[Ni+2].[Na+] WFSRWJJESXWWSH-UHFFFAOYSA-N 0.000 claims description 5
- 229910052802 copper Inorganic materials 0.000 claims description 5
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 4
- CROQDZTZYUXPHE-UHFFFAOYSA-N [O-2].[Mn+2].[Fe+2].[Na+] Chemical compound [O-2].[Mn+2].[Fe+2].[Na+] CROQDZTZYUXPHE-UHFFFAOYSA-N 0.000 claims description 4
- XLCPLIJTRIGVDU-UHFFFAOYSA-N [O-2].[Mn+2].[Ni+2].[Na+] Chemical compound [O-2].[Mn+2].[Ni+2].[Na+] XLCPLIJTRIGVDU-UHFFFAOYSA-N 0.000 claims description 4
- 238000005056 compaction Methods 0.000 claims description 4
- 239000011701 zinc Substances 0.000 claims description 4
- 229910052725 zinc Inorganic materials 0.000 claims description 4
- YGSBPUVMACUETM-UHFFFAOYSA-N [O-2].[Mn+2].[Cu+2].[Fe+2].[Na+] Chemical compound [O-2].[Mn+2].[Cu+2].[Fe+2].[Na+] YGSBPUVMACUETM-UHFFFAOYSA-N 0.000 claims description 2
- 229910052708 sodium Inorganic materials 0.000 abstract description 30
- 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 abstract description 28
- 229910052723 transition metal Inorganic materials 0.000 abstract description 18
- 150000003624 transition metals Chemical class 0.000 abstract description 18
- 238000002156 mixing Methods 0.000 abstract description 8
- 229910001428 transition metal ion Inorganic materials 0.000 abstract description 6
- 230000007547 defect Effects 0.000 abstract description 5
- 230000003647 oxidation Effects 0.000 abstract description 5
- 238000007254 oxidation reaction Methods 0.000 abstract description 5
- 230000007704 transition Effects 0.000 abstract 1
- 239000002243 precursor Substances 0.000 description 8
- 238000005245 sintering Methods 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 239000010410 layer Substances 0.000 description 7
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 7
- 239000000463 material Substances 0.000 description 6
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 6
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 4
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 239000002033 PVDF binder Substances 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 4
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 4
- 238000001035 drying Methods 0.000 description 4
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 4
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 4
- 229920000573 polyethylene Polymers 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- 239000011267 electrode slurry Substances 0.000 description 3
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- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- 229910014507 Na0.67Ni0.33Mn0.67O2 Inorganic materials 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- VMHLLURERBWHNL-UHFFFAOYSA-M Sodium acetate Chemical compound [Na+].CC([O-])=O VMHLLURERBWHNL-UHFFFAOYSA-M 0.000 description 2
- UIIMBOGNXHQVGW-DEQYMQKBSA-M Sodium bicarbonate-14C Chemical compound [Na+].O[14C]([O-])=O UIIMBOGNXHQVGW-DEQYMQKBSA-M 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 238000000498 ball milling Methods 0.000 description 2
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- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 2
- 235000014413 iron hydroxide Nutrition 0.000 description 2
- NCNCGGDMXMBVIA-UHFFFAOYSA-L iron(ii) hydroxide Chemical compound [OH-].[OH-].[Fe+2] NCNCGGDMXMBVIA-UHFFFAOYSA-L 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- PPNAOCWZXJOHFK-UHFFFAOYSA-N manganese(2+);oxygen(2-) Chemical compound [O-2].[Mn+2] PPNAOCWZXJOHFK-UHFFFAOYSA-N 0.000 description 2
- VASIZKWUTCETSD-UHFFFAOYSA-N manganese(II) oxide Inorganic materials [Mn]=O VASIZKWUTCETSD-UHFFFAOYSA-N 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- 239000004570 mortar (masonry) Substances 0.000 description 2
- 125000004430 oxygen atom Chemical group O* 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- 239000001632 sodium acetate Substances 0.000 description 2
- 235000017281 sodium acetate Nutrition 0.000 description 2
- 229910000029 sodium carbonate Inorganic materials 0.000 description 2
- 235000017550 sodium carbonate Nutrition 0.000 description 2
- 239000001509 sodium citrate Substances 0.000 description 2
- NLJMYIDDQXHKNR-UHFFFAOYSA-K sodium citrate Chemical compound O.O.[Na+].[Na+].[Na+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O NLJMYIDDQXHKNR-UHFFFAOYSA-K 0.000 description 2
- 235000011083 sodium citrates Nutrition 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 229920003048 styrene butadiene rubber Polymers 0.000 description 2
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 2
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
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- 239000006230 acetylene black Substances 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
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- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000006256 anode slurry Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
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- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
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- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- VEPSWGHMGZQCIN-UHFFFAOYSA-H ferric oxalate Chemical compound [Fe+3].[Fe+3].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O VEPSWGHMGZQCIN-UHFFFAOYSA-H 0.000 description 1
- ZYMKZMDQUPCXRP-UHFFFAOYSA-N fluoro prop-2-enoate Chemical compound FOC(=O)C=C ZYMKZMDQUPCXRP-UHFFFAOYSA-N 0.000 description 1
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- 229910021389 graphene Inorganic materials 0.000 description 1
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- MVFCKEFYUDZOCX-UHFFFAOYSA-N iron(2+);dinitrate Chemical compound [Fe+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MVFCKEFYUDZOCX-UHFFFAOYSA-N 0.000 description 1
- DCYOBGZUOMKFPA-UHFFFAOYSA-N iron(2+);iron(3+);octadecacyanide Chemical compound [Fe+2].[Fe+2].[Fe+2].[Fe+3].[Fe+3].[Fe+3].[Fe+3].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-].N#[C-] DCYOBGZUOMKFPA-UHFFFAOYSA-N 0.000 description 1
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Abstract
The application relates to the technical field of sodium ion batteries and provides a positive electrode material composition with high battery energy density, a positive electrode plate and a sodium ion battery. Wherein the positive electrode material composition comprises (1-9) O3 type sodium ion layered oxide and P2 type sodium ion layered oxide in a mass ratio of (2-8), and the particle size of the O3 type sodium ion layered oxide is larger than that of the P2 type sodium ion layered oxide. The positive electrode material composition provided by the application contains O3 type and P2 type sodium ion layered oxides, and enables the particle size of the O3 type sodium ion layered oxides to be larger than that of the P2 type sodium ion layered oxides, so that uniform mixing of the O3 type sodium ion layered oxides and the P2 type sodium ion layered oxides is facilitated, the defect of the P2 type sodium ion layered oxides with low sodium content can be overcome, the average valence state of transition metal ions in the O3 type can be raised by the P2 type sodium ion layered oxides, transition of the transition metal with the lowest oxidation valence state in the structure to the high valence state is promoted, and higher voltage and larger capacity are successfully realized.
Description
Technical Field
The application belongs to the technical field of batteries, and particularly relates to a positive electrode material composition with high battery energy density, a positive electrode plate and a sodium ion battery.
Background
The sodium ion battery has the advantages of abundant raw material resources, low price and similar working principle as the lithium ion battery, and is therefore widely concerned. Because the total amount of the global lithium resources is limited and unevenly distributed, and along with the mass application of the lithium ion battery in the field of electric vehicles, the shortage of the lithium resources becomes an important factor for restricting the development of the lithium ion battery, the price of the lithium carbonate serving as a main raw material is greatly increased, so that the production cost of industrial chain enterprises is greatly increased, and the advantages of the sodium ion battery are gradually developed under the environment.
At present, research on positive electrode materials of sodium ion batteries mainly focuses on three positive electrode technical routes of layered oxides, polyanions and Prussian blue. The layered oxide is the most widely used material in sodium ion battery research, and is mainly divided into O3 type and P2 type materials, wherein the O3 type layered structure is octahedron, and has abundant sodium storage amount, high capacity and low voltage; the P2 type layered structure is a triangular prism, and the voltage is high due to the structural characteristics of the material, but the sodium content and the capacity are low. Therefore, the existing sodium ion layered oxide positive electrode material is difficult to simultaneously combine high voltage and high capacity, so that the overall energy density of the sodium ion battery is low.
Disclosure of Invention
The invention aims to provide a positive electrode material composition with high battery energy density, a positive electrode plate and a sodium ion battery, and aims to solve the problem that the energy density of the sodium ion battery is low due to low voltage or low capacity of the existing sodium ion layered oxide positive electrode material.
In order to achieve the purposes of the application, the technical scheme adopted by the application is as follows:
in a first aspect, the present application provides a positive electrode material composition with high battery energy density, the positive electrode material composition comprising (1-9): (2-8) O3 type sodium ion layered oxide and P2 type sodium ion layered oxide in a mass ratio, and the particle size of the O3 type sodium ion layered oxide is larger than the particle size of the P2 type sodium ion layered oxide.
In a second aspect, the present application provides a positive electrode sheet comprising the positive electrode material composition of high battery energy density provided herein.
In a third aspect, the present application provides a sodium ion battery, including a positive plate and a negative plate, the positive plate being the positive plate provided herein.
Compared with the prior art, the application has the following beneficial effects:
according to the positive electrode material composition with high battery energy density, as the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide are contained, and the particle size of the O3 type sodium ion layered oxide is larger than that of the P2 type sodium ion layered oxide, the two types of sodium ion layered oxides are uniformly mixed, the O3 type sodium ion layered oxide with high sodium content can compensate the defect of the P2 type sodium ion layered oxide with low sodium content to improve the capacity, the P2 type sodium ion layered oxide can improve the average valence state of transition metal ions in the O3 type sodium ion layered oxide, and the transition metal with the lowest oxidation valence state in the structure is converted to the high valence state to improve the voltage, so that the sodium ion battery can simultaneously give consideration to the higher charge-discharge voltage and the larger capacity by using the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide in a compounding mode, and the energy density of the battery is further improved.
The positive plate provided in the second aspect of the application contains the positive material composition with high battery energy density, so that the positive plate can simultaneously give consideration to higher charge-discharge voltage and larger capacity, and the energy density of the battery can be further improved.
The third aspect of the application provides a sodium ion battery, and because the sodium ion battery contains the positive plate provided by the application, the sodium ion battery can simultaneously give consideration to higher charge-discharge voltage, larger capacity and larger energy density.
Detailed Description
In order to make the technical problems, technical schemes and beneficial effects to be solved by the present application more clear, the present application is further described in detail below with reference to the embodiments. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the present application.
In this application, the term "and/or" describes an association relationship of an association object, which means that there may be three relationships, for example, a and/or B may mean: a alone, a and B together, and B alone. Wherein A, B may be singular or plural. The character "/" generally indicates that the context-dependent object is an "or" relationship.
In the present application, "at least one" means one or more, and "a plurality" means two or more. "at least one of" or the like means any combination of these items, including any combination of single item(s) or plural items(s). For example, "at least one (individual) of a, b, or c," or "at least one (individual) of a, b, and c," may each represent: a, b, c, a-b (i.e., a and b), a-c, b-c, or a-b-c, wherein a, b, c may be single or multiple, respectively.
The terminology used in the embodiments of the application is for the purpose of describing particular embodiments only and is not intended to be limiting of the application. As used in this application and the appended claims, the singular forms "a," "an," and "the" are intended to include the plural forms as well, unless the context clearly indicates otherwise.
The weights of the relevant components mentioned in the embodiments of the present application may refer not only to specific contents of the components, but also to the proportional relationship between the weights of the components, and thus, any ratio of the contents of the relevant components according to the embodiments of the present application may be enlarged or reduced within the scope disclosed in the embodiments of the present application. Specifically, the mass described in the specification of the examples of the present application may be a mass unit known in the chemical industry such as μ g, mg, g, kg.
The terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying a relative importance or implicitly indicating the number of technical features indicated for distinguishing between objects such as substances from each other. For example, a first XX may also be referred to as a second XX, and similarly, a second XX may also be referred to as a first XX, without departing from the scope of embodiments of the present application. Thus, a feature defining "a first" or "a second" may explicitly or implicitly include one or more such feature.
The first aspect of the embodiment of the application provides a positive electrode material composition with high battery energy density, which comprises an O3 type sodium ion layered oxide and a P2 type sodium ion layered oxide in a mass ratio of (1-9): (2-8), wherein the particle size of the O3 type sodium ion layered oxide is larger than that of the P2 type sodium ion layered oxide.
The O3 type sodium ion layered oxide refers to a sodium ion-rich layered oxide, which is formed by stacking a plurality of oxide layers, wherein each oxide layer consists of metal ions and oxygen atoms, and a planar structure is formed, and the layered structure enables the O3 type sodium ion layered oxide to have a larger specific surface area and rich adjustable interlayer gaps, so that the rich sodium storage amount and high capacity are provided. The P2 type sodium ion layered oxide refers to a sodium ion-poor layered oxide, which is formed by stacking a plurality of oxide sheets, wherein each oxide sheet consists of metal ions and oxygen atoms, and a planar structure is formed.
According to the positive electrode material composition with high battery energy density, as the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide are contained, and the particle size of the O3 type sodium ion layered oxide is larger than that of the P2 type sodium ion layered oxide, the two types of sodium ion layered oxides are uniformly mixed, the O3 type sodium ion layered oxide with high sodium content can make up the defect of the P2 type sodium ion layered oxide with low sodium content to improve the capacity, the P2 type sodium ion layered oxide can improve the average valence state of transition metal ions in the O3 type sodium ion layered oxide, and the transition metal with the lowest oxidation valence state in the structure is promoted to be converted to be in a high valence state to improve the voltage, so that the sodium ion battery can be simultaneously in consideration of higher charging and discharging voltage and larger capacity by using the O3 type sodium ion layered oxide in a compound manner, and the energy density of the battery is further improved.
In some embodiments, the O3 type sodium ion layered oxide comprises elemental manganese and iron.
In some embodiments, the O3 sodium ion layered oxide has the chemical formula Na a1 Mn x1 Fe y1 T 1-x1-y1 O 2 Wherein a1 is more than or equal to 0.5 and less than or equal to 1, x1 is more than 0 and less than 1, y1 is more than 0 and less than 1, and T comprises at least one of copper (Cu), chromium (Cr), zinc (Zn), lead (Pb), calcium (Ca), cobalt (Co), nickel (Ni), strontium (Sr) and titanium (Ti). In an exemplary embodiment, the O3 type sodium ion layered oxide may include at least one of sodium nickel iron manganese oxide, sodium copper iron manganese oxide, sodium nickel copper iron manganese oxide, and sodium iron manganese oxide. The O3 type sodium ion layered oxide has high sodium content, and can be used by being compounded with the high-voltage P2 type sodium ion layered oxide, so that the low sodium content of the P2 type sodium ion layered oxide can be compensated, and meanwhile, the P2 type sodium ion layered oxide can compensate the low voltage of the O3 type sodium ion layered oxide, so that the advantages of the two are complemented, and the capacity and the charge-discharge voltage of the battery can be improved.
In some embodiments, the step of preparing the O3 sodium ion layered oxide comprises:
s11: according to Na a1 Mn x1 Fe y1 T 1-x1-y1 O 2 The stoichiometric ratio of the elements shown in Na, mn, fe, T in (a) provides a sodium source, a manganese source, an iron source and a transition metal source containing T;
s12: mixing a sodium source, a manganese source, an iron source and a transition metal source containing T, and drying to obtain a precursor;
s13: and sintering the precursor to obtain the O3 type sodium ion layered oxide.
In step S11, the sodium source may be selected from at least one of sodium carbonate, sodium bicarbonate, sodium citrate, sodium acetate; the manganese source can be at least one selected from manganous oxide, manganese dioxide and manganese oxide; the iron source may include at least one of iron oxide, iron nitrate, iron chloride, iron hydroxide, iron acetate, iron hydroxide, iron oxalate; the T-containing transition metal source may be a copper source, a chromium source, a zinc source, a lead source, a calcium source, a cobalt source, a nickel source, a strontium source, a titanium source, or the like.
In step S12, the step of mixing the sodium source, the manganese source, the iron source, and the T-containing transition metal source includes: the sodium source, the manganese source, the iron source and the transition metal source containing T are placed in an agate mortar or a ball milling pot to be ground and mixed uniformly, and the dispersing agent such as ethanol, acetone or glycol is added in the grinding process to increase the mixing uniformity.
In step S13, the step of sintering the precursor includes: transferring the precursor to an aluminum oxide crucible, placing the aluminum oxide crucible in a muffle furnace, and sintering the aluminum oxide crucible in an air atmosphere at 800-1000 ℃ for 14-18 h. In the sintering process, because the sodium source, the manganese source, the iron source and the T-containing transition metal source are in different particle contact, the material mesophase is gradually expanded, and when the ions reach equilibrium, the O3 type sodium ion layered oxide is formed.
In some embodiments, the P2 type sodium ion layered oxide comprises elemental manganese.
In some embodiments, the P2 type sodium ion layered oxide has the chemical formula Na a2 Mn x2 M 1-x2 O 2 Wherein a2 is more than or equal to 0 and less than 0.8, x2 is more than or equal to 0 and less than 1, M comprises at least one of (Cu), chromium (Cr), zinc (Zn), lead (Pb), calcium (Ca), cobalt (Co), iron (Fe), nickel (Ni), strontium (Sr) and titanium (Ti). In an exemplary embodiment, the P2 type sodium ion layered oxide includes at least one of sodium nickel manganese oxide, sodium manganese cobalt oxide, sodium iron manganese oxide, and sodium copper manganese oxide.
In some embodiments, the step of preparing a P2 type sodium ion layered oxide comprises:
s21: according to Na a2 Mn x2 M 1-x2 O 2 The stoichiometric ratio of Na, mn and T elements provides a sodium source, a manganese source and a transition metal source containing T;
s22: mixing a sodium source, a manganese source and a transition metal source containing T, and drying to obtain a precursor;
s23: and sintering the precursor to obtain the P2 type sodium ion layered oxide.
In step S21, the sodium source may be selected from at least one of sodium carbonate, sodium bicarbonate, sodium citrate, sodium acetate; the manganese source can be at least one selected from manganous oxide, manganese dioxide and manganese oxide; the T-containing transition metal source may be a copper source, a chromium source, a zinc source, a lead source, a calcium source, a cobalt source, a nickel source, a strontium source, a titanium source, or the like.
In step S22, the step of subjecting the sodium source, the manganese source and the T-containing transition metal source to the mixing process includes: the sodium source, the manganese source and the transition metal source containing T are put into an agate mortar or a ball milling pot to be ground and mixed uniformly, and the dispersing agent such as ethanol, acetone or glycol is added in the grinding process to increase the mixing uniformity.
In step S23, the step of subjecting the precursor to the sintering process includes: transferring the precursor to an aluminum oxide crucible, placing the aluminum oxide crucible in a muffle furnace, and sintering the aluminum oxide crucible in an air atmosphere at 800-1000 ℃ for 14-18 h. In the sintering process, because the contact of the sodium source, the manganese source and the particles of the transition metal source containing T is different, the material mesophase is gradually enlarged, and when the ions reach balance, the P2 type sodium ion layered oxide is formed.
In some embodiments, the mass ratio of the O3 type sodium ion layered oxide to the P2 type sodium ion layered oxide is (1-9): 2-8), further may be (6-9): 2-4), and in the exemplary case may be a typical but non-limiting mass ratio of 9:2, 8:2, 7.5:2.5, 7:3, 6.4:3.6, 5:4, 4:3, 3:5, 2:6, 1:8, etc. In the mass ratio range, the O3 type sodium ion layered oxide with high sodium content can make up the defect of the P2 type sodium ion layered oxide with low sodium content to improve the capacity, the P2 type sodium ion layered oxide can improve the average valence state of transition metal ions in the O3 type sodium ion layered oxide, and the transition metal with the lowest oxidation valence state in the structure is promoted to be converted to a high valence state to improve the voltage, so that the sodium ion battery can simultaneously give consideration to higher voltage and larger capacity, and the energy density of the battery can be further improved.
In some embodiments, the O3 type sodium ion layered oxide has a particle size that is more than 60% greater than the P2 type sodium ion layered oxide. Further, the particle size may be controlled to be 65% to 95% higher, specifically 60%, 65%, 70%, 75%, 80%, 85%, 90%, 95% higher, etc., which is typical but not limiting. The difference ratio of the particle sizes of the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide is controlled, for example, the difference ratio is controlled in the range, so that the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide are uniformly mixed, the O3 type sodium ion layered oxide with high sodium content can make up for the low capacity of the P2 type ion layered oxide, the P2 type sodium ion layered oxide can raise the average valence state of transition metal ions in the O3 type sodium ion layered oxide, and the transition metal is promoted to be converted to a high valence state to raise the voltage, so that the advantages of the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide can be simultaneously considered, and the sodium ion battery can have higher charge and discharge voltage, larger capacity and larger energy density.
In some embodiments, the sodium ion layered oxide of O3 type has a particle size Dv50 of 5 μm to 12 μm, a particle size Dv10.gtoreq.3 μm (i.e., 10% of the particles in the volume distribution have a particle size greater than 3 μm), a particle size Dv90.ltoreq.25 μm, and the three satisfy 0.5.ltoreq.Dv50/(Dv90—Dv1). Ltoreq.5. The particle diameter Dv50 of the P2 type sodium ion layered oxide is 2-9 mu m, the particle diameter Dv10 is more than or equal to 2 mu m, dv90 is less than or equal to 20 mu m, and the three satisfy 0.1 less than or equal to Dv50/(Dv90-Dv10) is less than or equal to 5.
In some embodiments, the O3 type sodium ion layered oxide has a compacted density of 3.0g/cm 3 ～3.3g/cm 3 In an exemplary embodiment, the concentration may be 3.0g/cm 3 、3.1g/cm 3 、3.2g/cm 3 、3.3g/cm 3 Etc. typical but non-limiting compaction densities. The compacted density of the P2 type sodium ion layered oxide is 3.2g/cm 3 ～3.7g/cm 3 . In an example, it may be 3.2g/cm 3 、3.3g/cm 3 、3.4g/cm 3 、3.5g/cm 3 、3.6g/cm 3 、3.7g/cm 3 Etc. typical but non-limiting compaction densities. Due to the interlayer spacing and compaction density of the P2 type sodium ion layered oxide compared with the O3 type sodium ion layered oxideThe interlayer spacing and the compacted density of the oxide are large, and by controlling the compacted densities of both the P2 type sodium ion layered oxide and the O3 type sodium ion layered oxide to be within the range of the present embodiment, the compacted density of the positive electrode active layer can be increased, thereby increasing the battery energy density.
In some embodiments, the positive electrode material composition further includes a conductive agent and a binder, and the mass ratio of the O3 type sodium ion layered oxide, the P2 type sodium ion layered oxide, the conductive agent and the binder is (1-9): 2-8): 0.25-1.0): 0.125-0.5.
In some embodiments, the binder may be selected from at least one of ethylene terpolymers, tetrafluoroethylene-hexafluoropropylene copolymers, and fluoroacrylate resins. The adhesive can bond O3 type sodium ion layered oxide, P2 type sodium ion layered oxide and conductive agent on the current collector well, so that the stability of the positive electrode active layer structure can be improved, and the integrity of the electrode during charge and discharge can be maintained.
In some embodiments, the conductive agent may be selected from at least one of acetylene black, superconducting carbon, carbon black, ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers. The conductive agents can be uniformly dispersed, and can play a role in synergy with components such as O3 type sodium ion layered oxide, P2 type sodium ion layered oxide, binder and the like on the basis of endowing the positive electrode active layer with high electron conductivity, so that the stability of the positive electrode active layer is improved.
A second aspect of embodiments of the present application provides a positive electrode sheet comprising the positive electrode material composition of high battery energy density provided herein.
The positive plate provided by the embodiment of the application can simultaneously give consideration to higher charge-discharge voltage and larger capacity due to the positive electrode material composition provided by the application, so that the energy density of the battery is further improved.
The third aspect of the embodiment of the application provides a sodium ion battery, which comprises a positive plate and a negative plate, wherein the positive plate is provided by the application.
The sodium ion battery provided by the embodiment of the application can simultaneously give consideration to higher charge and discharge voltage, larger capacity and larger energy density due to the fact that the sodium ion battery comprises the positive plate.
In some embodiments, the sodium ion battery has an N/P ratio (ratio of negative reversible surface capacity to positive reversible surface capacity) of 1.0 to 1.3.
The following description is made with reference to specific embodiments.
1. Positive electrode material composition examples and comparative examples
Example 1
The present embodiment provides a positive electrode material composition with high battery energy density, the positive electrode material composition includes O3 type sodium ion layered oxide, P2 type sodium ion layered oxide, conductive carbon black and polyvinylidene fluoride in a mass ratio of 7:3:0.5:0.5, and the particle diameter Dv50 of the O3 type sodium ion layered oxide is 7.32 μm, dv10 is 4.5 μm, dv90 is 13.9 μm, the particle diameter Dv50 of the P2 type sodium ion layered oxide is 3.1 μm, dv10 is 2.2 μm, dv90 is 12.5 μm, wherein the O3 type sodium ion layered oxide is sodium nickel iron manganese oxide (NaNi) 0.33 Fe 0.33 Mn 0.33 O 2 ) The P2 type sodium ion layered oxide is sodium nickel manganese oxide (Na 0.67 Ni 0.33 Mn 0.67 O 2 )。
Example 2
The present embodiment provides a positive electrode material composition with high battery energy density, the positive electrode material composition comprising O3 type sodium ion layered oxide, P2 type sodium ion layered oxide, conductive carbon black and polyvinylidene fluoride in a mass ratio of 6.4:3.6:0.5:0.5, wherein the particle diameter Dv50 of the O3 type sodium ion layered oxide is 7.32 μm, dv10 is 4.5 μm, dv90 is 13.9 μm, the particle diameter Dv50 of the P2 type sodium ion layered oxide is 6.0 μm, dv10 is 3.8 μm, dv90 is 9.35 μm, wherein the O3 type sodium ion layered oxide is nickel copper sodium iron manganese oxide (NaNi 0.23 Cu 0.11 Fe 0.33 Mn 0.33 O 2 ) The P2 type sodium ion layered oxide is sodium copper manganate (Na 0.7 Mn 0.7 Cu 0.3 O 2 )。
Example 3
The present embodiment providesA positive electrode material composition with high battery energy density comprises O3 type sodium ion layered oxide, P2 type sodium ion layered oxide, conductive carbon black and polyvinylidene fluoride in a mass ratio of 7.5:2.5:0.5:0.5, wherein the particle size Dv50 of the O3 type sodium ion layered oxide is 11.8 mu m, dv10 is 7.3 mu m, dv90 is 19.4 mu m, the particle size Dv50 of the P2 type sodium ion layered oxide is 6.0 mu m, dv10 is 3.8 mu m and Dv90 is 9.35 mu m, and the O3 type sodium ion layered oxide is sodium nickel iron manganese oxide (NaNi 0.33 Fe 0.33 Mn 0.33 O 2 ) The P2 type sodium ion layered oxide is sodium nickel manganese oxide (Na 0.67 Ni 0.33 Mn 0.67 O 2 )。
Comparative example 1
The present comparative example provides a positive electrode material composition comprising an O3 type sodium ion layered oxide, conductive carbon black and polyvinylidene fluoride in a mass ratio of 10:0.5:0.5, and having a particle diameter Dv50 of 11.8 μm, dv10 of 7.3 μm, dv90 of 19.4 μm, wherein the O3 type sodium ion layered oxide is sodium nickel iron manganese oxide (NaNi 0.33 Fe 0.33 Mn 0.33 O 2 )。
2. Sodium ion battery examples and comparative examples:
the positive electrode material compositions provided in examples 1 to 3 and comparative examples 1 to 2 described above were assembled into sodium ion batteries, respectively, as follows:
positive pole piece: adding the positive electrode material composition into N-methyl pyrrolidone solvent, and uniformly stirring to prepare positive electrode slurry with the solid content of 50%; and coating the anode slurry on an anode current collector aluminum foil, and drying and cold pressing to obtain an anode plate.
Negative pole piece: adding hard carbon, conductive carbon black, a binder (styrene butadiene rubber, SBR) and a thickener (carboxymethyl cellulose, CMC) in a mass ratio of 9.0:0.4:0.3:0.3 into deionized water, and uniformly mixing to prepare negative electrode slurry; and coating the negative electrode slurry on a negative electrode current collector copper foil, and drying and cold pressing to obtain a negative electrode plate.
Electrolyte solution: ethylene Carbonate (EC) and ethylmethyl carbonate (DEC) in a volume ratio of 3:7Mixing and adding NaPF 6 An electrolyte solution having a concentration of 1mol/L was formed.
A diaphragm: polyethylene (PE) microporous separator membranes.
And (3) assembling a lithium ion battery: sequentially stacking the positive electrode plate, polyethylene (PE) microporous membrane and the negative electrode plate, winding to form an electrode assembly, packaging the electrode assembly in a packaging shell, and adding NaPF 6 And (3) packaging, forming, standing and the like the electrolyte to obtain the sodium ion battery.
3. Sodium ion battery related performance measurement:
the positive electrode active layers of the positive electrode sheets of examples 1 to 3 and comparative examples 1 to 2 were examined for their compacted densities, and the charge-discharge voltages and energy densities of the respective sodium-ion batteries, respectively, and the test results are shown in table 1 below.
TABLE 1
As can be seen from table 1, the charge-discharge median voltage and the energy density of the sodium ion batteries of examples 1 to 3 of the present application are significantly higher than those of the sodium ion battery of comparative example 1, which indicates that the O3 type sodium ion layered oxide and the P2 type sodium ion layered oxide are used in a compounding manner, the O3 type sodium ion layered oxide with high sodium content can compensate the defect of the P2 type sodium ion layered oxide with low sodium content to raise the capacitance, and the P2 type sodium ion layered oxide can raise the average valence state of the transition metal ion in the O3 type sodium ion layered oxide, so that the transition metal with the lowest oxidation valence state in the structure is converted to the high valence state to raise the voltage, and the advantage complementation of the two is realized, thereby making the sodium ion battery of the present application capable of simultaneously giving consideration to the higher charge-discharge voltage and the larger energy density.
The foregoing description of the preferred embodiments of the present application is not intended to be limiting, but is intended to cover any and all modifications, equivalents, and alternatives falling within the spirit and principles of the present application.
Claims (10)
1. The positive electrode material composition with high battery energy density is characterized by comprising O3 type sodium ion layered oxide and P2 type sodium ion layered oxide in a mass ratio of (1-9): (2-8), wherein the particle size of the O3 type sodium ion layered oxide is larger than that of the P2 type sodium ion layered oxide.
2. The high battery energy density positive electrode material composition of claim 1, the O3 type sodium ion layered oxide comprising manganese and elemental iron; and/or
The P2 type sodium ion layered oxide contains manganese element.
3. The high battery energy density positive electrode material composition according to claim 2, wherein the O3 type sodium ion layered oxide has a chemical formula of Na a1 Mn x1 Fe y1 T 1-x1-y1 O 2 Wherein a1 is more than or equal to 0.5 and less than or equal to 1, x1 is more than 0 and less than 1, y1 is more than 0 and less than 1, and T comprises at least one of copper, chromium, zinc, lead, calcium, cobalt, nickel, strontium and titanium elements; and/or
The chemical general formula of the P2 type sodium ion layered oxide is Na a2 Mn x2 M 1-x2 O 2 Wherein a2 is more than or equal to 0 and less than 0.8, x2 is more than or equal to 0 and less than 1, and M comprises at least one of copper, chromium, zinc, lead, calcium, cobalt, iron, nickel, strontium and titanium.
4. The high battery energy density positive electrode material composition of claim 3 wherein said O3 type sodium ion layered oxide comprises at least one of sodium nickel iron manganese oxide, sodium copper iron manganese oxide, sodium nickel copper iron manganese oxide, sodium iron manganese oxide; and/or
The P2 type sodium ion layered oxide comprises at least one of sodium nickel manganese oxide, sodium manganese cobalt oxide, sodium iron manganese oxide and sodium copper manganese oxide.
5. The positive electrode material composition having a high battery energy density according to any one of claims 1 to 4, wherein the particle size of the O3 type sodium ion layered oxide is 60% or more higher than the particle size of the P2 type sodium ion layered oxide.
6. The positive electrode material composition having a high battery energy density according to claim 5, wherein the O3 type sodium ion layered oxide has a particle diameter Dv50 of 5 μm to 12 μm; and/or
The particle diameter Dv50 of the P2 type sodium ion layered oxide is 2-9 mu m.
7. The high battery energy density positive electrode material composition according to claim 5, wherein the O3 type sodium ion layered oxide has a compacted density of 3.0g/cm 3 ～3.3g/cm 3 The method comprises the steps of carrying out a first treatment on the surface of the And/or
The compaction density of the P2 type sodium ion layered oxide is 3.2g/cm 3 ～3.7g/cm 3 。
8. The positive electrode material composition with high battery energy density according to claim 5, wherein the positive electrode material composition further comprises a conductive agent and a binder, and the mass ratio of the O3 type sodium ion layered oxide, the P2 type sodium ion layered oxide, the conductive agent and the binder is (1 to 9): (2 to 8): (0.25 to 1.0): (0.125 to 0.5).
9. A positive electrode sheet comprising the positive electrode material composition of any one of claims 1 to 8.
10. A sodium ion battery comprising a positive electrode sheet and a negative electrode sheet, wherein the positive electrode sheet is the positive electrode sheet of claim 9.
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