CN113972361A - Application of metal oxide/carbon intercalated layer two-dimensional composite material in lithium ion battery cathode material - Google Patents
Application of metal oxide/carbon intercalated layer two-dimensional composite material in lithium ion battery cathode material Download PDFInfo
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- CN113972361A CN113972361A CN202010725068.1A CN202010725068A CN113972361A CN 113972361 A CN113972361 A CN 113972361A CN 202010725068 A CN202010725068 A CN 202010725068A CN 113972361 A CN113972361 A CN 113972361A
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- carbon
- metal oxide
- composite material
- dimensional composite
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 156
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 143
- 229910044991 metal oxide Inorganic materials 0.000 title claims abstract description 136
- 150000004706 metal oxides Chemical class 0.000 title claims abstract description 136
- 239000002131 composite material Substances 0.000 title claims abstract description 109
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 23
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 23
- 239000010406 cathode material Substances 0.000 title claims abstract description 7
- 239000000463 material Substances 0.000 claims abstract description 57
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 31
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 23
- 238000009830 intercalation Methods 0.000 claims abstract description 23
- 230000002687 intercalation Effects 0.000 claims abstract description 22
- 239000002135 nanosheet Substances 0.000 claims abstract description 11
- 239000010410 layer Substances 0.000 claims description 81
- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 claims description 28
- 238000000034 method Methods 0.000 claims description 28
- 229910052901 montmorillonite Inorganic materials 0.000 claims description 28
- 238000006116 polymerization reaction Methods 0.000 claims description 25
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 22
- 239000003575 carbonaceous material Substances 0.000 claims description 19
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- 239000012298 atmosphere Substances 0.000 claims description 18
- 238000006243 chemical reaction Methods 0.000 claims description 17
- 230000008569 process Effects 0.000 claims description 17
- 239000000243 solution Substances 0.000 claims description 17
- 239000000203 mixture Substances 0.000 claims description 16
- 238000010438 heat treatment Methods 0.000 claims description 15
- 239000002253 acid Substances 0.000 claims description 13
- 238000002156 mixing Methods 0.000 claims description 13
- 239000002052 molecular layer Substances 0.000 claims description 12
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 11
- 238000005245 sintering Methods 0.000 claims description 10
- 239000007787 solid Substances 0.000 claims description 10
- 239000011230 binding agent Substances 0.000 claims description 9
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 claims description 9
- 238000003763 carbonization Methods 0.000 claims description 8
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- 238000006011 modification reaction Methods 0.000 claims description 8
- 239000007773 negative electrode material Substances 0.000 claims description 8
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- 239000000126 substance Substances 0.000 claims description 7
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- 238000005470 impregnation Methods 0.000 claims description 6
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- 238000010000 carbonizing Methods 0.000 claims description 4
- 238000000576 coating method Methods 0.000 claims description 4
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 claims description 4
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 4
- 229910052752 metalloid Inorganic materials 0.000 claims description 4
- 150000002738 metalloids Chemical class 0.000 claims description 4
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- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 claims description 3
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- 229910052688 Gadolinium Inorganic materials 0.000 claims description 2
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 2
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- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
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- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 2
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 2
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 2
- 229910052788 barium Inorganic materials 0.000 claims description 2
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 2
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 claims description 2
- 229910052791 calcium Inorganic materials 0.000 claims description 2
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- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- KBQHZAAAGSGFKK-UHFFFAOYSA-N dysprosium atom Chemical compound [Dy] KBQHZAAAGSGFKK-UHFFFAOYSA-N 0.000 claims description 2
- UYAHIZSMUZPPFV-UHFFFAOYSA-N erbium Chemical compound [Er] UYAHIZSMUZPPFV-UHFFFAOYSA-N 0.000 claims description 2
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 claims description 2
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- LSYIMYXKHWXNBV-UHFFFAOYSA-N lanthanum(3+) oxygen(2-) titanium(4+) Chemical compound [O-2].[La+3].[Ti+4] LSYIMYXKHWXNBV-UHFFFAOYSA-N 0.000 claims description 2
- OHSVLFRHMCKCQY-UHFFFAOYSA-N lutetium atom Chemical compound [Lu] OHSVLFRHMCKCQY-UHFFFAOYSA-N 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
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- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 claims description 2
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Abstract
The invention discloses an application of a metal oxide/carbon intercalated layer two-dimensional composite material in a lithium ion battery cathode material. The metal oxide/carbon intercalated layer two-dimensional composite material comprises metal oxide layers and carbon layers positioned between the metal oxide layers, wherein the carbon layers and the metal oxide layers are mutually interpenetrated. The original embedded lithium storage is changed into the capacitive lithium storage of a metal oxide/carbon interface by intercalation of the carbon nano sheets of the layered metal oxide, and simultaneously, the electrical conductivity, the thermal conductivity and the physical stability of the material are greatly improved by embedding of the carbon nano sheets.
Description
Technical Field
The invention belongs to the field of lithium ion batteries, and particularly relates to an application of a metal oxide/carbon intercalated layer two-dimensional composite material in a lithium ion battery cathode material.
Background
In the prior art, a lithium ion battery cathode material mainly adopts a diffusion type energy storage mode, the poor cycle stability caused by limited charging and discharging speed, large expansion coefficient in an embedding process and the like possibly exist in the charging and discharging process, and the low multiplying power performance of the battery is caused by the low conductivity of part of the material.
Disclosure of Invention
The invention provides an application of a metal oxide/carbon intercalated layer two-dimensional composite material in a lithium ion battery cathode material.
According to an embodiment of the present invention, the metal oxide/carbon intercalated two-dimensional composite comprises metal oxide layers and carbon layers between the metal oxide layers, the carbon layers being intercalated with the metal oxide layers.
Preferably, the metal oxide may be selected from alkaline earth-transition metal oxides and metalloid oxides, for example, one, two or more of oxides of elements such as calcium, aluminum, silicon, lithium, nickel, cobalt, barium, titanium, niobium, ruthenium, vanadium, tungsten, tantalum, hafnium, zirconium, chromium, molybdenum, manganese, lanthanum, cerium, praseodymium, neodymium, scandium, yttrium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, etc.; preferably, the metal oxide may be selected from alkaline earth-transition metal oxides and metalloid oxides containing one, two or more of the above elements; illustratively, the metal oxide is one, two or more of titanium dioxide, niobium oxide, lanthanum oxide, tungsten oxide, vanadium oxide, perovskite-type lanthanum titanium oxide, and natural montmorillonite.
Preferably, the carbon material in the carbon layer is a two-dimensional carbon-based material in which organic molecules (including macromolecules) are formed in a layered metal oxide by intercalation into the layered metal oxide, and then by polymerization, carbonization, or the like in the metal oxide layered material; further, the composition of the carbon layer may be doped with at least one element such as oxygen, nitrogen, sulfur, etc., to a different degree depending on the organic molecule, in addition to carbon. I.e. the carbon-based material may be all carbon or contain other doped carbon-based materials. Illustratively, the two-dimensional carbon-based material may be one, two, or more of graphite-like, two-dimensional carbon-based nanosheets material (single-layer graphene, multi-layer graphene, nitrogen-doped graphene, nitrogen and sulfur-doped graphene, amorphous layered carbon, and other nitrogen or sulfur-doped amorphous sheet carbon materials.
According to an embodiment of the invention, the metal oxide/carbon intercalated two-dimensional composite has a repeat unit thickness of 0.5 to 5nm, such as 0.4 to 3nm, and as an example a repeat unit thickness of 1.1 nm. Wherein the repeating unit is composed of a metal oxide layer and a carbon layer.
Wherein, the "one metal oxide layer" refers to a structural layer formed by metal oxide, and can be a single layer of metal oxide or multiple layers of metal oxide. The "carbon layer" refers to a structural layer formed of the above carbon-based material, and may be a single layer of carbon or a plurality of layers of carbon.
According to embodiments of the present invention, the metal oxide/carbon intercalated two-dimensional composite material may be arranged in a substantially overlapping manner from layer to layer, or in a staggered manner from layer to layer.
According to embodiments of the present invention, the metal oxide/carbon intercalated two-dimensional composite may have a thickness of 20 nm to 50 microns, for example a thickness of 100 nm to 30 microns, 500 nm to 15 microns.
According to an embodiment of the present invention, the specific surface area of the metal oxide/carbon intercalated layer two-dimensional composite material is 10 to 480m2G, e.g. 100-470m2/g、300-450m2/g。
According to an embodiment of the present invention, the metal oxide/carbon intercalated layer two-dimensional composite may be a metal oxide/graphite-like intercalated layer two-dimensional composite, a kaolin/carbon two-dimensional composite, or a montmorillonite/carbon two-dimensional composite; may illustratively be a layered TiO2Graphite-like two-dimensional composite material and TiO2Nano sheet/graphite-like two-dimensional composite materialA material or a montmorillonite/carbon two-dimensional composite material.
According to an embodiment of the present invention, the process for preparing the metal oxide/carbon intercalated layer two-dimensional composite material comprises the following steps:
(1) carrying out intercalation reaction or surface modification reaction on the metal oxide two-dimensional material and an organic matter containing amino, and introducing an organic molecular layer between layers of the metal oxide two-dimensional material or the surface of the metal oxide two-dimensional material to obtain an organic molecular layer/metal oxide two-dimensional composite material;
(2) carbonizing the organic molecular layer/metal oxide two-dimensional composite material obtained in the step (1) to obtain the metal oxide/carbon intercalated layer two-dimensional composite material; alternatively, the first and second electrodes may be,
(3) carrying out polymerization reaction on the organic molecular layer/metal oxide two-dimensional composite material obtained in the step (1) to obtain a high molecular layer/metal oxide two-dimensional composite material; and carbonizing the polymer layer/metal oxide two-dimensional composite material to obtain the metal oxide/carbon intercalated layer two-dimensional composite material.
According to an embodiment of the present invention, in step (1), the metal oxide two-dimensional material may be selected from at least one of an aprotic, metal ion-exchange, protonated metal oxide layered material, and porous and/or non-porous metal oxide nanoplates; wherein the metal oxide has the meaning as described above. Preferably, the metal oxide two-dimensional material may be selected from protonated layered TiO2Material, montmorillonite layered material, kaolin layered material, nickel ion-exchanged layered TiO2Material, layered TiO partially substituted with lithium2Material, non-porous TiO2Nanosheet, porous TiO2Nanosheets.
According to an embodiment of the invention, the metal oxide layered material has a lamella size of 50 nm to 50 μm and a thickness of 20 nm to 50 μm. Wherein the size of the sheet layer of the metal oxide nano sheet is 50 nanometers to 50 micrometers, and the thickness of the metal oxide nano sheet is 0.5 nanometers to 20 nanometers.
According to an embodiment of the present invention, the metal oxide two-dimensional material can be prepared by a method known in the art, such as a solid-thermal sintering method, a hydrothermal method, a solvothermal method, a liquid phase exfoliation method, a mechanical exfoliation method, an ion exchange method, and the like; or the metal oxide two-dimensional material can be a natural two-dimensional layered material, such as kaolin, montmorillonite, hydrotalcite, and the like, and the natural layered material can be obtained by alkali washing, acid washing, ion exchange, and the like.
According to an embodiment of the present invention, in the step (1), the organic substance containing an amino group may be selected from an organic small molecule containing at least one amino group, or one, two or more of hydrochloride, hydrobromide, nitrate thereof; for example, the organic small molecule may be selected from at least one of saturated alkylamine, aromatic amine, alcohol amine, amino acid and its corresponding hydrochloride, hydrobromide, nitrate, and the like; wherein the saturated alkylamine may be selected from C3-C16The aromatic amine may be selected from one, two or more of melamine, pyrrole, aniline, diphenylamine (e.g., o-diphenylamine, m-diphenylamine, p-diphenylamine), benzidine, 3' -diaminobenzidine, benzylamine, and derivatives of the above aromatic amines (e.g., vinylaniline, vinylbenzylamine, methylbenzylamine, phenylbenzylamine, etc.); the alcohol amine may be selected from one, two or more of ethanolamine, diethanolamine, isopropanolamine, etc.; the amino acid may be selected from one, two or more of p-aminobenzoic acid, p-aminomethyl benzoic acid, glycine, alanine, leucine, phenylalanine, tryptophan, serine, tyrosine, etc.; illustratively, the amino group-containing organic substance is selected from octylamine, benzylamine, benzidine, or p-aminobenzoic acid.
According to an embodiment of the present invention, in step (1), the number of the intercalation reaction or modification reaction is not limited, and may be one, two or more; namely, products after intercalation or modification reaction can be re-intercalated or re-modified by using other organic matters containing amino. Wherein the amino group-containing organic substance has the meaning as described above. Illustratively, first by octylamine with protonated layered TiO2Intercalation is realized, the obtained solid is subjected to a displacement reaction with an aniline solution to obtain a new intercalation product, and the intercalated small molecular layer in the product can be any mol ratio of octylamine to aniline, such as 1/1 or 1/4.
According to an embodiment of the present invention, in step (1), the intercalation reaction and the surface modification reaction may be performed in a solvent, which may be one, two or more selected from water, alcohols, aromatic hydrocarbons, esters, and saturated alkanes. Wherein, the alcohol can be selected from one, two or more of methanol, ethanol, isopropanol, butanol and the like, the aromatic hydrocarbon can be selected from one, two or more of toluene, xylene, benzene and the like, the ester can be selected from one, two or more of ethyl acetate, ethyl formate and the like, and the saturated alkane can be selected from one, two or more of cyclohexane, normal hexane and the like. Preferably, the organic solvent may be selected from one, two or more of methanol, ethanol, isopropanol; illustratively, the solvent is selected from a mixed solution of ethanol and water. The volume ratio of ethanol to water in the mixed solution of ethanol and water is not particularly limited, and for example, the volume ratio of ethanol to water may be (1-20):1, preferably (1-10):1, and illustratively, the volume ratio of ethanol to water may be 1:1, 7:1, or 11: 1. When the organic substance containing an amino group is in a liquid state or in a liquid state in a reaction temperature range, any other solvent may not be used, and the organic substance may be used as a reactant or a solvent.
According to an embodiment of the present invention, in step (1), the intercalation reaction comprises the following processes: and (2) mixing the metal oxide two-dimensional material and the organic matter containing amino, or mixing the metal oxide two-dimensional material, the organic matter containing amino and the solvent, and then reacting in a normal pressure heating mode, a hydrothermal mode, a solvothermal mode, a stirring mode, an ultrasonic mode or a microwave heating mode and the like. Preferably, the intercalation comprises the following processes: mixing the metal oxide two-dimensional material and the organic matter containing amino, or mixing the metal oxide two-dimensional material, the organic matter containing amino and the solvent, performing ultrasonic dispersion, and placing the mixture in a hydrothermal reaction kettle for heating reaction; wherein the heating temperature may be 50 to 180 deg.C, such as 80 to 140 deg.C, and as an example, the temperature may be 90 deg.C, 100 deg.C, 110 deg.C. Further, when the metal oxide two-dimensional material is selected from metal oxide layered materials, an organic molecular layer is introduced between layers of the metal oxide layered materials by using intercalation reaction.
According to an embodiment of the present invention, in the step (1), the surface modification reaction includes the following processes: mixing the metal oxide two-dimensional material and the organic matter containing amino, or mixing the metal oxide two-dimensional material, the organic matter containing amino and the solvent, and then reacting in the modes of normal pressure heating, hydrothermal reaction, stirring, ultrasonic heating or microwave heating and the like; preferably, stirring or sonication or the like is used. For example, the stirring time may be 1-48h, such as 2-24h, as an example, time may be 4h, 12h, 16 h; the reaction temperature may be room temperature to 180 deg.C, such as 50 to 140 deg.C, and as an example, the temperature may be room temperature, 60 deg.C, 100 deg.C, 120 deg.C.
According to an embodiment of the present invention, in the step (1), the mass-to-volume ratio (g/mL) of the metal oxide two-dimensional material, the amino group-containing organic substance, and the solvent may be 1 (0.05-200): (0-200); for example, the mass-to-volume ratio is 1 (0.15-5): 15-100) or 1 (0.2-2): 20-80, and for example, the mass-to-volume ratio may be 1:5:0 (in the case of no solvent), 1:0.4:75 or 1:1: 24.
According to the embodiment of the present invention, in the step (2) and the step (3), the temperature of the carbonization treatment may be 300-. The time of the carbonization treatment can be 0.5-24h, such as 1.5-5h, and as an example, the time can be 2h, 4h, 8 h. Further, the carbonization treatment is performed in vacuum, inert atmosphere and/or reducing atmosphere, for example, the inert atmosphere may be at least one of nitrogen, helium, argon and the like, and the reducing atmosphere may be any mixture of hydrogen and ammonia with the inert atmosphere; illustratively, the carbonization treatment may be performed in an atmosphere of hydrogen, nitrogen, or a mixture of nitrogen and hydrogen.
According to an embodiment of the present invention, in the step (3), the polymerization reaction may be selected from photo polymerization, thermal polymerization, or oxidative polymerization. Wherein the light polymerization can be light polymerization of visible light, ultraviolet light, X-ray and the like; the thermal polymerization or oxidative polymerization can be solid-gas thermal polymerization, solid-liquid thermal polymerization, solid-gas oxidative polymerization or solid-liquid oxidative polymerization. For example, the solid-gas oxidative polymerization is carried out in an oxygen-containing atmosphere (e.g., an oxygen atmosphere, an oxygen-containing oxygen-nitrogen mixed gas, an oxygen-argon mixed gas, etc.); for example, the oxidizing agent for the solid-liquid oxidative polymerization may be one, two or more selected from oxygen, hydrogen peroxide, ferric chloride, nitric acid, sulfuric acid, ammonium persulfate, potassium persulfate, sodium persulfate, potassium permanganate, sodium permanganate, and the like. Wherein the solid-gas thermal polymerization may incorporate an initiator into the metal oxide two-dimensional material by impregnation methods known in the art. Wherein, the solid-liquid thermal polymerization can directly introduce an initiator into a reaction solution; the initiator can be at least one of BPO, AIBN and the like; or other small molecules capable of reacting with amino groups, wherein the small molecules and the amino groups on the intercalated organic molecule layer are subjected to polymerization through amidation reaction or aldehyde-amine condensation reaction. Wherein the small molecule may be selected from at least one of terephthalic acid, isophthalic acid, phthalic acid, biphenyldicarboxylic acid, citric acid, oxalic acid, malonic acid, succinic acid, glutaric acid, adipic acid, terephthalaldehyde, isophthalaldehyde, phthalaldehyde, terephthalaldehyde, glyoxal, malondialdehyde, succindialdehyde, glutaraldehyde, and adipaldehyde, etc. Further, the temperature of the photo polymerization, thermal polymerization or oxidative polymerization may be room temperature to 400 ℃, such as 50 to 300 ℃, 100-; the time of the solid gas oxidative polymerization can be 0.5 to 12 hours, such as 1.5 to 5 hours, and as an example, the time can be 2 hours, 3 hours and 4 hours. Further, the temperature of the solid-liquid oxidation polymerization can be-40 to 200 ℃, for example-30 to 150 ℃; the time for the solid-liquid oxidative polymerization may be from 0.6 to 12 hours, for example from 1.5 to 5 hours. Wherein the amount of the oxidizing agent is an amount known in the art. Wherein the solvent in the polymerization reaction system has the meaning as described above.
According to an embodiment of the present invention, in the step (3), the solid-liquid thermal polymerization, the solid-liquid oxidative polymerization are carried out in a solvent, which may be at least one selected from water and organic solvents; for example, the organic solvent may be selected from one, two or more of alcohols, aromatic hydrocarbons, esters, and saturated alkanes; wherein, the alcohol can be selected from one, two or more of methanol, ethanol, isopropanol and the like, the aromatic hydrocarbon can be selected from one, two or more of toluene, benzene and the like, the ester can be selected from one, two or more of ethyl acetate, ethyl formate and the like, and the saturated alkane can be selected from one, two or more of cyclohexane, normal hexane and the like. Preferably, the organic solvent may be selected from one, two or more of methanol, ethanol, isopropanol; illustratively, the solvent is selected from a mixed solution of ethanol and water. The volume ratio of ethanol to water in the mixed solution of ethanol and water is not particularly limited, and for example, the volume ratio of ethanol to water may be (1-20):1, preferably (1-10):1, and illustratively, the volume ratio of ethanol to water may be 1:1, 7:1, or 11: 1.
And (3) carrying out polymerization reaction, wherein the purpose is to prevent evaporation loss of organic matters in the high-temperature carbonization process, and the organic molecules with modified surfaces or intercalated organic molecules are polymerized to prepare a polymer macromolecule layer.
According to an embodiment of the present invention, optionally, after the intercalation reaction or surface modification reaction of step (1) and the polymerization reaction of step (3) are completed, a solid powder may be obtained by separation and post-treatment using centrifugation, filtration, drying, and the like. The drying may be any one of air drying, vacuum drying, oven drying, spray drying, and freeze drying.
According to an embodiment of the present invention, the preparation method further comprises step (4): and (4) carrying out acid cleaning on the metal oxide/carbon intercalated layer two-dimensional composite material obtained in the step (2) and the step (3). The metal oxide/carbon intercalated layer two-dimensional composite material obtained by the treatment of the steps (2) and (3) has carbon thermal reaction in reducing atmosphere or inert atmosphereIt should be noted that there may be precipitation of metal particles in the partially doped metal oxide material. For example, nickel doped TiO2The layered structure will have nickel particles precipitated after heat treatment and the precipitated metal particles can be removed by pickling. The acid washing may be one, two or more of nitric acid, sulfuric acid, citric acid, hydrochloric acid, acetic acid and other common acids, such as hydrochloric acid or nitric acid. The acid used for the acid wash may be present in a concentration of 0.01mol/L to 10mol/L, preferably in a concentration of 0.1 to 5mol/L, such as 0.5mol/L, 1mol/L or 2 mol/L. The acid wash temperature may be room temperature to 95 deg.C, preferably room temperature to 60 deg.C, illustratively room temperature or 50 deg.C. The pickling process can be carried out by standing, normal-pressure heating, hydrothermal reaction, stirring, ultrasonic or microwave heating and the like; preferably, stirring or sonication or the like is used. For example, the stirring time may be 1-48h, such as 2-24h, as an example, time may be 4h, 12h, 16 h; the solid matter after acid washing can be obtained by filtering, centrifuging, standing, removing the upper layer acid liquor after the solid matter is precipitated, and the like; the acid washing process may be repeated, for example, after acid washing, filtering and then acid washing again, and the process is repeated 1 to 5 times, preferably 2 to 4 times, and exemplarily 3 times. The acid-washed sample may be dried, vacuum dried, spray dried, etc. as known in the art to obtain a solid sample, illustratively, vacuum dried at 60 ℃ for 2 hours.
Wherein room temperature means 15-40 deg.C, such as 20-35 deg.C.
According to the embodiment of the invention, the metal oxide/carbon intercalated layer two-dimensional composite material can be used in a negative electrode material of a lithium ion battery after being reprocessed.
According to an embodiment of the present invention, the re-treatment may include at least one of a carbon wrapping process, a heat treatment process, a pre-lithiation process, an ion exchange process, and the like, to change the shape, crystallinity, composition, and the like of the two-dimensional metal oxide (i.e., metal oxide layer) and/or the two-dimensional carbon material (i.e., carbon layer).
According to an embodiment of the present invention, the carbon coating process is selected from hydrothermal treatment of the metal oxide/carbon intercalated layer two-dimensional composite material in a sugar solution, or treatment of the metal oxide/carbon intercalated layer two-dimensional composite material by a sugar solution impregnation method. Preferably, the sugar in the sugar solution is selected from at least one of sucrose, glucose and fructose.
Preferably, the mass ratio of the sugar to the metal oxide/carbon two-dimensional composite material is (1-50):100, such as 10: 100.
Preferably, the solvent in the sugar solution is water or a mixture of water and alcohol. Wherein the alcohol is one, two or more of common industrial alcohols, such as methanol, ethanol, n-propanol, isopropanol and n-butanol. The ratio of water to alcohol is not particularly limited, and may be any ratio, for example, water to ethanol is 1:1 (volume ratio).
Preferably, the mass to volume ratio of sugar to solvent is 1mg (1-1000) ml, such as 1mg:100 ml.
Preferably, the hydrothermal method may use a general hydrothermal tank or microwave hydrothermal method. Further, the temperature of the hydrothermal treatment is 120-330 ℃, for example, 180 ℃; the reaction time of the hydrothermal treatment is 1 to 24 hours, such as 12 hours.
Preferably, after the hydrothermal treatment, the reaction system is filtered, washed, dried, vacuum-dried, and/or carbonized (carbonization temperature is 500-900 ℃), and the like, so as to obtain the carbon-coated metal oxide/carbon two-dimensional composite material.
According to an embodiment of the present invention, the sugar solution impregnation method includes mixing a sugar solution with a metal oxide/carbon two-dimensional composite material, drying, and sintering in an inert atmosphere or a reducing atmosphere. Preferably, the inert atmosphere is selected from one or a mixture of any of nitrogen, argon and helium. Preferably, the reducing atmosphere is selected from one or two of hydrogen and ammonia, or a mixed gas of hydrogen and/or ammonia and one or more inert atmospheres in any proportion. Preferably, the sintering temperature is 500-1200 ℃, for example 600-1000 ℃. Preferably, the sintering time is from 0.1 to 12 hours, such as from 2 to 8 hours. Illustratively, sintering is carried out at 800 degrees Celsius for 2 hours under a nitrogen atmosphere.
According to an embodiment of the invention, the heat treatment comprises direct sintering of the metal oxide/carbon two-dimensional composite. Preferably, the atmosphere, temperature and time of the sintering are the same as those of the sugar solution impregnation method.
According to an embodiment of the present invention, the prelithiation refers to a process in which particles containing lithium metal, lithium flakes, or other lithium metal-containing materials (e.g., carbon-coated lithium particles, mixture materials of lithium and other materials, etc.) are added during the assembly of the negative electrode to construct the negative electrode.
According to an embodiment of the invention, the ion exchange comprises mixing and reacting the metal oxide/carbon composite material with an aqueous solution of metal ions, introducing the metal ions at the metal oxide/carbon interface. Wherein the metal ion aqueous solution contains at least one of alkali metal ions, alkaline earth metal ions, chlorides, nitric acid compounds, sulfuric acid compounds, hydroxides and the like of transition metal ions, for example, the metal ion aqueous solution contains LiCl, KOH and Ni (NO)3)2And the like. Preferably, the mixing reaction includes stirring, sonication, hydrothermal methods, and the like. Preferably, the temperature of the reaction is between 0-200 degrees Celsius, such as 30-100 degrees Celsius. Preferably, the concentration of the metal ion is between 0.001M and 10M, for example between 0.1 and 5M. For example, a 0.1M aqueous LiCl solution is stirred with the metal oxide/carbon composite at room temperature for 2 hours, filtered and washed with water and dried in vacuo.
The invention also provides a lithium ion battery cathode which contains the metal oxide/carbon intercalation layer two-dimensional composite material and/or the reprocessed metal oxide/carbon intercalation layer two-dimensional composite material.
According to the embodiment of the invention, the metal oxide/carbon intercalated layer two-dimensional composite material can be independently used as a negative electrode material of a lithium ion battery; or the metal oxide/carbon intercalated layer two-dimensional composite material is blended with other materials to be used as a negative electrode material of the lithium ion battery.
Preferably, the mass ratio of the metal oxide/carbon intercalated layer two-dimensional composite material to other materials is (1-99): (99-1), such as (5-95): (95-5), (10-90): (90-10).
Preferably, the other materials may be selected from commonly used additive materials for batteries: the mass ratio of the conductive carbon material, binder, etc., such as carbon material/binder in the whole of the other material, may be (90-10)/(10-90).
Preferably, the other materials may be selected from common negative electrode materials other than the additive materials, such as one or two of graphite and silicon carbon materials, and the mass ratio of the other materials to the additive materials may be 90-0%.
Illustratively, the negative electrode contains a binder, a conductive agent and a current collector in addition to the metal oxide/carbon intercalation two-dimensional composite material. Wherein the binder, the conductive agent and the current collector may be selected from those known in the art. For example, the binder may be selected from at least one of polyvinyl alcohol (PVA), Polytetrafluoroethylene (PTFE), carboxymethylcellulose sodium (CMC), polyolefins (PE, PP, polyvinylidene fluoride (PVDF), modified Styrene Butadiene Rubber (SBR), and the like.
The invention also provides a lithium ion battery which contains the metal oxide/carbon intercalated layer two-dimensional composite material, the reprocessed metal oxide/carbon intercalated layer two-dimensional composite material and/or the negative electrode.
According to an embodiment of the present invention, the lithium ion battery may be various types of lithium ion batteries known in the art, such as a pouch lithium battery, a cylindrical lithium battery, a button lithium battery, an all solid state lithium battery, and the like.
The invention has the beneficial effects that:
when the metal oxide/carbon intercalated layer two-dimensional composite material and/or the reprocessed metal oxide/carbon intercalated layer two-dimensional composite material is used as the lithium ion negative electrode material, the two-dimensional intercalated layer composite material provides higher electron mobility in the composite material; meanwhile, the mechanical and thermal conductivity of the carbon nanosheets can obviously improve the long-term stability of the electrode material; the metal oxide/carbon two-dimensional interface provides the characteristic of capacitive energy storage, so that the power density, the energy density, the long-term stability and the faster charge and discharge performance of the material can be obviously improved by the metal oxide material subjected to the intercalation post-treatment.
Drawings
FIG. 1 is a representation of a montmorillonite/carbon two-dimensional composite:
a) TEM and elemental profile of the montmorillonite/carbon two-dimensional composite;
b) high power TEM of montmorillonite/carbon two-dimensional composite material;
and c) the grey value corresponding to the line in the graph b, with a thickness of 10.1nm for the 6 repeating units, i.e. 1.7nm per unit thickness.
Figure 2 is the rate performance of example 3 and a comparative half cell.
Fig. 3 shows the performance of the full cell of example 4: (a) a charge-discharge curve; (b) cycling stability during charging and discharging and coulombic efficiency.
FIG. 4 shows TiO prepared in example 62And (3) a shape picture of the/carbon two-dimensional composite material by a scanning electron microscope.
FIG. 5 shows TiO in example 72Comparison of first effect of the/C two-dimensional composite with or without pre-lithium by lithium metal.
Detailed Description
The technical solution of the present invention will be further described in detail with reference to specific embodiments. It is to be understood that the following examples are only illustrative and explanatory of the present invention and should not be construed as limiting the scope of the present invention. All the technologies realized based on the above-mentioned contents of the present invention are covered in the protection scope of the present invention.
Unless otherwise indicated, the raw materials and reagents used in the following examples are all commercially available products or can be prepared by known methods.
Example 1
The preparation process of the montmorillonite/carbon two-dimensional composite material comprises the following steps: 10g of montmorillonite was immersed in a 1mol/L nitric acid solution, left to stand overnight at room temperature, then the upper layer liquid was poured out, left to stand overnight after adding new nitric acid, the above operation was repeated three times, then filtered, and washed with a large amount of water to neutrality. The montmorillonite is added into 100mL of water-ethanol (volume ratio is 1:1) mixed solution, 8g of mixed solid with 1:2 (molar ratio) of aniline/benzidine is added, the mixture is stirred for 12 hours in a reflux state, after filtration, the mixture is heated for 3 hours by using a 200 ℃ pure oxygen atmosphere tube furnace, then the tube furnace is switched to a nitrogen atmosphere, the mixture reacts for 2 hours in a 700 ℃ nitrogen atmosphere, and the mixture is cooled to room temperature, so that the montmorillonite/carbon two-dimensional composite material is obtained, as shown in figure 1.
Example 2
Carbon coating of the montmorillonite/carbon two-dimensional composite material: 5g of the montmorillonite/carbon two-dimensional composite material in the example 1 and 0.5g/5mL of sucrose aqueous solution are fully and uniformly mixed, the mixture is heated to 80 ℃ by a glass rod under the heating condition while stirring until no water vapor comes out, then the obtained mixture is sintered for 2 hours at 700 ℃ in a nitrogen atmosphere of a tubular furnace, and the carbon-coated montmorillonite/carbon two-dimensional composite material is obtained after cooling.
Example 3
The carbon-coated montmorillonite/carbon two-dimensional composite material prepared in example 2 was used as an electrode material, lithium metal was used as a counter electrode material, 1mol/L lithium hexafluorophosphate/vinyl carbonate and dimethyl carbonate mixed solution (the volume ratio of the two solvents is 1:1) was used as an electrolyte, the electrode material was mixed with a binder (PVDF) and activated carbon (Super-P) in a mass ratio of 8:1:1, and then a slurry mixed with azomethylpyrrolidone as a solvent was applied to a current collector of a copper sheet to obtain a button cell with a half cell type test system.
For comparison, a half-cell study was conducted in which a montmorillonite raw material that had not been subjected to carbon intercalation treatment was used in place of a carbon-coated montmorillonite/carbon two-dimensional composite material to construct a half-cell with lithium as a counter electrode.
The rate capability of the two half-cells is shown in fig. 2, and the half-cell containing the carbon-coated montmorillonite/carbon two-dimensional composite material of example 2 shows that the specific capacity and rate capability of the half-cell are about an order of magnitude higher than those of the half-cell containing montmorillonite.
Example 4
A full cell was prepared by using the carbon-coated montmorillonite/carbon two-dimensional composite material prepared in example 2 as a negative electrode, the lithium iron phosphate/conductive carbon Super-J/PVDF 8/1/1 coating material as a positive electrode, 1mol/L lithium hexafluorophosphate/vinyl carbonate and dimethyl carbonate mixed solution (solvent volume ratio of the two is 1; 1) as an electrolyte, and Celgard 2400 as a separator, and using a button cell grinder. The specific capacity and the cycling stability of the full cell after being activated by 20mA/g for one time after being charged and discharged for 50 times at 100mA/g are shown in figure 3. The test results in fig. 3 show that the carbon-coated montmorillonite/carbon material prepared in example 2 shows better performances such as cycling stability and capacity as a negative electrode.
Example 5
Hydrothermal prelithiation of montmorillonite/carbon composite: 1.0g of the montmorillonite/carbon two-dimensional composite material of example 1 was hydrothermally treated in 0.1mol/L aqueous solution of lithium hydroxide LiOH at 100 ℃ for 12 hours, and then the resulting mixture was cooled to room temperature, filtered, washed with water to neutrality, and dried in an air-blast drying oven to obtain 1.0g of a prelithiated montmorillonite/carbon two-dimensional composite material.
Example 6
TiO2The preparation process of the/carbon two-dimensional composite material comprises the following steps: protonated layered TiO2By reacting anhydrous potassium carbonate with anatase TiO2Grinding and mixing according to the molar ratio of 1.3/4.1, then carrying out solid phase sintering at 950 ℃, and then protonating in 1mol/L nitric acid to prepare the catalyst. 3.0g of protonated layered TiO2The material, 1.5mL of benzylamine, 1g of p-phenylenediamine, and 120mL of a mixed solution of ethanol/water (1/1 vol/vol) were heated to 80 ℃ in a 200mL flask with a reflux condenser for reflux reaction for 14 hours, cooled to room temperature, filtered, washed with a large amount of water, dried, polymerized at 200 ℃ for 2 hours in an oxygen atmosphere, and then carbonized at 700 ℃ for 6 hours in a nitrogen atmosphere to give 3.8g of TiO2A carbon two-dimensional composite material. TiO 22The morphology of the/carbon two-dimensional composite material is shown in figure 4. As can be seen from FIG. 4, the prepared TiO2The carbon/carbon composite material has a regular intercalated layered structure.
Example 7
TiO2The lithium metal pre-lithium preparation process of the/carbon two-dimensional composite material comprises the following steps: TiO prepared in example 6 in a glove box under argon atmosphere2The carbon/carbon two-dimensional composite material, the binder (PVDF), the activated carbon (Super-P) and the lithium metal particles are mixed according to the mass ratio of 7.5:1:1:0.5, then slurry mixed by taking the azomethyl pyrrolidone as a solvent is coated on a current collector of a copper sheet to be used as an electrode sheet, and TiO without pre-lithium treatment is used as a contrast2The/carbon fiber composite material, a binder (PVDF) and active carbon (Super-P) are mixed according to a mass ratio of 8:1:1, and then slurry mixed by taking nitrogen methyl pyrrolidone as a solvent is coated on a current collector of a copper sheet. Both of them use lithium sheet as counter electrode, 1mol/L lithium hexafluorophosphate/ethylene carbonate and dimethyl carbonate mixed solution (the volume ratio of the two solvents is 1:1) as electrolyte, and Celgard 2400 as diaphragm, and the obtained test system is half-cell type button cell.
The first effect of two button cells was tested by blue cell, as shown in fig. 5, by mixing TiO samples with lithium metal2The first effect of the carbon/carbon composite material was 96.1%, while the first effect of the sample not produced by the lithium metal particles was only 44.4%.
The embodiments of the present invention have been described above. However, the present invention is not limited to the above embodiment. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. An application of a metal oxide/carbon intercalated layer two-dimensional composite material in a lithium ion battery cathode material.
2. The use according to claim 1, wherein the metal oxide/carbon intercalated two-dimensional composite comprises a metal oxide layer and a carbon layer between the metal oxide layer, the carbon layer being intercalated with the metal oxide layer.
Preferably, the metal oxide is selected from alkaline earth-transition metal oxides and metalloid oxides, such as one, two or more of oxides of elements such as calcium, aluminum, silicon, lithium, nickel, cobalt, barium, titanium, niobium, ruthenium, vanadium, tungsten, tantalum, hafnium, zirconium, chromium, molybdenum, manganese, lanthanum, cerium, praseodymium, neodymium, scandium, yttrium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, and the like; preferably, the metal oxide may be selected from alkaline earth-transition metal oxides and metalloid oxides containing one, two or more of the above elements; illustratively, the metal oxide is selected from one, two or more of titanium dioxide, niobium oxide, lanthanum oxide, tungsten oxide, vanadium oxide, perovskite-type lanthanum titanium oxide, and natural montmorillonite.
Preferably, the carbon material in the carbon layer is a two-dimensional carbon-based material in which organic molecules (including macromolecules) are formed in a layered metal oxide by intercalation into the layered metal oxide, and then by polymerization, carbonization, or the like in the metal oxide layered material; preferably, the carbon layer is all carbon or contains other doped carbon-based materials. Illustratively, the carbon layer is one, two or more of two-dimensional graphite-like, two-dimensional carbon-based nanosheets material (single-layer graphene, multi-layer graphene, nitrogen-doped graphene, nitrogen and sulfur-doped graphene, amorphous layered carbon, and other nitrogen or sulfur-doped amorphous sheet carbon materials.
Preferably, the repeating unit thickness of the metal oxide/carbon intercalated layer two-dimensional composite material is 0.5-5 nm. Preferably, the repeating unit is composed of one metal oxide layer and one carbon layer.
Preferably, the metal oxide/carbon intercalated layer two-dimensional composite material is basically arranged in an overlapping mode between layers or staggered mode between layers.
3. Use according to claim 1 or 2, wherein the thickness of the metal oxide/carbon intercalated two-dimensional composite is between 20 nm and 50 μm.
Preferably, the specific surface area of the metal oxide/carbon intercalated layer two-dimensional composite material is 10-480m2/g。
Preferably, the metal oxide/carbon intercalated layer two-dimensional composite material is metal oxideA/type graphite intercalation two-dimensional composite material, a kaolin/carbon two-dimensional composite material, or a montmorillonite/carbon two-dimensional composite material; illustratively layered TiO2Graphite-like two-dimensional composite material and TiO2A nano sheet/graphite-like two-dimensional composite material or a montmorillonite/carbon two-dimensional composite material.
4. Use according to any one of claims 1 to 3, wherein the preparation of the metal oxide/carbon intercalated two-dimensional composite comprises the following steps:
(1) carrying out intercalation reaction or surface modification reaction on the metal oxide two-dimensional material and an organic matter containing amino, and introducing an organic molecular layer between layers of the metal oxide two-dimensional material or the surface of the metal oxide two-dimensional material to obtain an organic molecular layer/metal oxide two-dimensional composite material;
(2) carbonizing the organic molecular layer/metal oxide two-dimensional composite material obtained in the step (1) to obtain the metal oxide/carbon intercalated layer two-dimensional composite material; alternatively, the first and second electrodes may be,
(3) carrying out polymerization reaction on the organic molecular layer/metal oxide two-dimensional composite material obtained in the step (1) to obtain a high molecular layer/metal oxide two-dimensional composite material; and carbonizing the polymer layer/metal oxide two-dimensional composite material to obtain the metal oxide/carbon intercalated layer two-dimensional composite material.
5. The use according to claim 4, wherein optionally, after the intercalation reaction or surface modification reaction of step (1) and the polymerization reaction of step (3) are completed, the solid powder is obtained by separation by centrifugation, filtration, drying and the like, and post-treatment.
Preferably, the preparation method further comprises step (4): and (4) carrying out acid cleaning on the metal oxide/carbon intercalated layer two-dimensional composite material obtained in the step (2) and the step (3).
6. The use according to any one of claims 1 to 5, wherein the metal oxide/carbon intercalated two-dimensional composite material is used in a negative electrode material of a lithium ion battery after being reprocessed.
Preferably, the reprocessing includes at least one of a carbon wrapping process, a heat treatment process, a prelithiation process, an ion exchange process, and the like, to change the shape, crystallinity, and/or composition of the two-dimensional metal oxide (i.e., metal oxide layer) and/or the two-dimensional carbon material (i.e., carbon layer).
7. The use according to claim 6, wherein the carbon coating process is selected from hydrothermal treatment of the metal oxide/carbon intercalated two-dimensional composite in a sugar solution or treatment of the metal oxide/carbon intercalated two-dimensional composite by sugar solution impregnation. Preferably, the sugar in the sugar solution is selected from at least one of sucrose, glucose and fructose.
Preferably, the sugar solution impregnation method comprises mixing the sugar solution with the metal oxide/carbon two-dimensional composite material, drying, and sintering in an inert atmosphere or a reducing atmosphere.
Preferably, the heat treatment comprises direct sintering of the metal oxide/carbon two-dimensional composite.
Preferably, the prelithiation refers to a process of adding particles containing lithium metal, lithium flakes, or other substances containing lithium metal to construct a negative electrode in the negative electrode assembly process.
Preferably, the ion exchange comprises mixing and reacting the metal oxide/carbon composite material with an aqueous solution of metal ions to introduce the metal ions at the metal oxide/carbon interface.
8. A negative electrode for a lithium ion battery, comprising the metal oxide/carbon intercalation two-dimensional composite material according to any one of claims 1 to 5 and/or the reprocessed metal oxide/carbon intercalation two-dimensional composite material according to claim 6 or 7.
Preferably, the metal oxide/carbon intercalated layer two-dimensional composite material is independently used as a negative electrode material of a lithium ion battery; or the metal oxide/carbon intercalated layer two-dimensional composite material is blended with other materials to be used as a negative electrode material of the lithium ion battery.
Preferably, the mass ratio of the metal oxide/carbon intercalated layer two-dimensional composite material to other materials is (1-99): (99-1), such as (5-95): (95-5), (10-90): (90-10).
Preferably, the other material is selected from at least one of conductive carbon materials, binders, graphite, silicon carbon materials.
9. A lithium ion battery comprising the metal oxide/carbon intercalated two-dimensional composite material according to any one of claims 1 to 5, the reprocessed metal oxide/carbon intercalated two-dimensional composite material according to claim 6 or 7, and/or the negative electrode according to claim 8.
10. The lithium ion battery of claim 9, wherein the lithium ion battery is a lithium pouch battery, a lithium cylindrical battery, a lithium button battery, or an all solid state lithium battery.
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