CN113764651A - High-capacity lithium ion battery negative electrode active material, negative electrode plate and lithium ion battery - Google Patents
High-capacity lithium ion battery negative electrode active material, negative electrode plate and lithium ion battery Download PDFInfo
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- CN113764651A CN113764651A CN202110973237.8A CN202110973237A CN113764651A CN 113764651 A CN113764651 A CN 113764651A CN 202110973237 A CN202110973237 A CN 202110973237A CN 113764651 A CN113764651 A CN 113764651A
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- active material
- negative electrode
- ion battery
- lithium ion
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 21
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 21
- 239000007773 negative electrode material Substances 0.000 title claims abstract description 19
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 claims abstract description 14
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000010703 silicon Substances 0.000 claims abstract description 11
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 9
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 7
- 239000011777 magnesium Substances 0.000 claims abstract description 7
- 150000003377 silicon compounds Chemical class 0.000 claims abstract description 7
- 239000006182 cathode active material Substances 0.000 claims abstract description 5
- 239000000126 substance Substances 0.000 claims abstract description 3
- 229910052744 lithium Inorganic materials 0.000 claims description 10
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 6
- 239000007774 positive electrode material Substances 0.000 claims description 3
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 claims description 2
- 229910000676 Si alloy Inorganic materials 0.000 claims description 2
- 229910001128 Sn alloy Inorganic materials 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims description 2
- 239000011149 active material Substances 0.000 claims description 2
- 229910021383 artificial graphite Inorganic materials 0.000 claims description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 2
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 claims description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 2
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 claims description 2
- YTHCQFKNFVSQBC-UHFFFAOYSA-N magnesium silicide Chemical compound [Mg]=[Si]=[Mg] YTHCQFKNFVSQBC-UHFFFAOYSA-N 0.000 claims description 2
- 229910021338 magnesium silicide Inorganic materials 0.000 claims description 2
- ZAUUZASCMSWKGX-UHFFFAOYSA-N manganese nickel Chemical compound [Mn].[Ni] ZAUUZASCMSWKGX-UHFFFAOYSA-N 0.000 claims description 2
- 239000002931 mesocarbon microbead Substances 0.000 claims description 2
- 229910021382 natural graphite Inorganic materials 0.000 claims description 2
- 239000001301 oxygen Substances 0.000 claims description 2
- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 239000002245 particle Substances 0.000 claims description 2
- 229910021483 silicon-carbon alloy Inorganic materials 0.000 claims description 2
- 229910052596 spinel Inorganic materials 0.000 claims description 2
- 239000011029 spinel Substances 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 abstract description 10
- 239000000463 material Substances 0.000 abstract description 8
- 229910052814 silicon oxide Inorganic materials 0.000 abstract description 8
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 8
- MKPXGEVFQSIKGE-UHFFFAOYSA-N [Mg].[Si] Chemical compound [Mg].[Si] MKPXGEVFQSIKGE-UHFFFAOYSA-N 0.000 description 4
- 229910052786 argon Inorganic materials 0.000 description 4
- 239000011887 silicon containing negative electrode material Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 239000006258 conductive agent Substances 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 238000012216 screening Methods 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 238000000889 atomisation Methods 0.000 description 2
- 239000006229 carbon black Substances 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 239000011889 copper foil Substances 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000005086 pumping Methods 0.000 description 2
- 229910019752 Mg2Si Inorganic materials 0.000 description 1
- 229910017639 MgSi Inorganic materials 0.000 description 1
- 238000003723 Smelting Methods 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 239000006183 anode active material Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 230000006698 induction Effects 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/386—Silicon or alloys based on silicon
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to a high-capacity lithium ion battery cathode active material, a cathode sheet and a lithium ion battery, wherein the cathode active material contains one or more of a silicon simple substance or a silicon compound, and silicon oxide contains magnesium, wherein the magnesium content accounts for 5-40% of the total weight of the material. By adopting the negative electrode material with high specific capacity, the first charge-discharge efficiency of the silicon monoxide can be obviously improved, and the cycle performance of the battery can be improved.
Description
Technical Field
The invention belongs to the technical field of battery materials, and relates to a high-capacity lithium ion battery negative electrode material, a negative electrode plate and a lithium ion battery.
Background
Since lithium (Li) has the lowest reduction potential and the smallest ionic radius, in metal-ion batteries, lithiumThe primary rechargeable battery is considered to be the most promising battery system to achieve high mass/volume energy density and power density. Through research in the last two decades, lithium ion rechargeable batteries have been widely used in daily life, including electric tools, notebook computers, digital products, mobile phones, electric vehicles, unmanned aerial vehicles, and the like. In recent years, the dramatic growth in the market has required the development of commercial lithium ion batteries in the direction of lighter, thinner, and cheaper batteries. However, the LIBs commercially available today have reached their theoretical limits (250 wh/kg and 680 wh/L). Because the graphite-based negative electrode has lower theoretical specific capacity (372 mAh/g) and volume capacity (735 mAh/cm)3) Further increases in energy density of commercial LIBs are limited. Innovations in battery materials, including positive and negative electrodes, are then mainly aimed at increasing the energy density of the next generation lithium-based batteries and assembling lighter and thinner batteries to meet the needs of various applications.
In the high-capacity negative electrode, the silicon negative electrode is considered as the material with the largest development potential, the specific capacity of the silicon negative electrode is 4400mAh/g, and the specific capacity of the silicon negative electrode is almost 10 times of that of the graphite negative electrode commonly used in the current industry. However, the silicon negative electrode has a great problem in practical application that the capacity is too fast due to too much expansion. Therefore, researchers adopt the scheme of the silicon oxide, and the specific capacity is about 1500 mAh/g. The adoption of the silicon oxide can effectively reduce the expansion problem of the negative electrode and improve the cycle performance, however, the silicon oxide brings about another problem that the first charge-discharge efficiency is too low, only about 75 percent or even lower, which leads to that nearly 25 percent of lithium ions in the positive electrode active material are consumed, and the capacity loss of the battery is caused.
Therefore, it is necessary to provide a lithium ion battery cathode material and a lithium ion battery to solve the above problems in the prior art.
Disclosure of Invention
The invention aims to provide a high-capacity lithium ion battery negative electrode active material, a negative electrode sheet and a lithium ion battery.
The purpose of the invention can be realized by the following technical scheme:
one of the technical schemes of the invention provides a high-capacity lithium ion battery cathode active material, which contains one or more of simple substance silicon or compound silicon, and the compound silicon contains magnesium, wherein the content of the magnesium accounts for 5% -40% of the total weight of the cathode active material.
Further, the particle size of the negative active material is between 1 μm and 50 μm.
Further, the weight ratio of oxygen in the silicon compound is less than 40%.
Further, the silicon compound includes silicon monoxide and magnesium silicide.
Further, the negative active material can be doped with a second active material which is selected from one or more of natural graphite, artificial graphite, mesocarbon microbeads, lithium titanate, silicon or silicon-carbon alloy, tin alloy and active lithium metal.
The second technical scheme of the invention provides a negative electrode sheet, which comprises the negative electrode active material. In addition, the negative electrode sheet may further include necessary materials such as a solid electrolyte, a conductive agent, a negative electrode carrier, etc. for making the negative electrode sheet.
Further, the mass percentage of the negative electrode active material is 5% -100% (excluding the negative electrode carrier), and can be selected as 93%.
The third technical scheme of the invention provides a lithium ion battery, which comprises the negative plate.
Further, the positive active material in the positive plate of the lithium ion battery is any one or a combination of a plurality of lithium cobaltate, lithium manganate, lithium iron phosphate, lithium iron manganese phosphate, lithium nickel cobalt manganese oxide and nickel manganese spinel.
Compared with the prior art, the cathode material with high specific capacity can obviously improve the first charge-discharge efficiency of the silicon monoxide and improve the cycle performance of the battery.
Drawings
Fig. 1 is an SEM image and an EDS image of an anode active material according to the present invention;
fig. 2 is an XRD pattern of the negative active material of the present invention.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. The present embodiment is implemented on the premise of the technical solution of the present invention, and a detailed implementation manner and a specific operation process are given, but the scope of the present invention is not limited to the following embodiments.
In the following examples, unless otherwise specified, all the conventional commercially available raw materials or conventional processing techniques in the art are indicated.
Example 1:
MgSi is Mg2Si and pure SiO are mixed (the mol ratio of the Si to the pure SiO is 1: 1), and the purity of the SiO is 99.99 percent.
After the materials are loaded into a melting crucible, starting vacuum pumping by using vacuum equipment, synchronously starting a power supply of an induction melting system and a heat preservation system to preheat, filling argon into a vacuum chamber of the equipment after the vacuum degree is pumped to be lower than 1Pa, then carrying out secondary vacuum pumping, stopping the vacuum system after the vacuum degree is also pumped to be lower than 1Pa, filling the argon to the atmospheric pressure, and then increasing the power to carry out melting.
The smelting temperature is 1300 ℃ and 1400 ℃, argon is used for atomization, and the atomization pressure is about 2.8 MPa. The temperature is kept for more than 30 minutes.
After the powder is atomized by argon gas and cooled in a wall-cooling vacuum cavity for more than two hours, a powder accumulation barrel is opened, the atomized powder is transferred to an atmosphere protection state for screening treatment, ultrasonic vacuum screening is used, strict atmosphere protection is carried out in the screening process, safety accidents are prevented, and finally the magnesium-silicon-containing negative electrode active material is obtained. Fig. 1 and 2 are SEM, EDS, XRD, and the like of the prepared magnesium-silicon-containing negative active material.
And (3) manufacturing a button cell, wherein the manufactured magnesium-silicon-containing negative electrode active material is subjected to button cell manufacturing:
the mixture ratio is as follows: the magnesium-silicon-containing negative active material accounts for 93 percent of the total material weight, 2 percent of PAALi and 5 percent of carbon black conductive agent SP.
The negative carrier is a porous copper foil.
The electrolytic liquid system is EC: EMC 3: 7, 1M LiPF6，2％VC，2％FEC；
The counter electrode is a lithium metal sheet.
Comparative example 1
Silica is used as a negative active material.
The mixture ratio is as follows: the negative active material accounts for 93 percent of the total weight of the material, 2 percent of PAALi and 5 percent of carbon black conductive agent SP;
the negative carrier is a porous copper foil.
The electrolytic liquid system is EC: EMC 3: 7, 1M LiPF6，2％VC，2％FEC。
The counter electrode is a lithium metal sheet.
The button cells prepared in example 1 and comparative example 1 were subjected to electrical property tests, as shown in table 1 below.
TABLE 1 comparison of the Electrical Properties of the examples and comparative examples
As can be seen from the table 1, the alloyed silicon oxide cathode after magnesium addition shows good electrical property, the specific capacity of the alloyed silicon oxide cathode is slightly reduced compared with that of pure silicon oxide, but the specific capacity of the alloyed silicon oxide cathode is far higher than that of a graphite cathode, the primary efficiency is greatly improved and reaches 82%; the cycle performance is also well improved, and the residual rate after 100 cycles is 75 percent.
The embodiments described above are described to facilitate an understanding and use of the invention by those skilled in the art. It will be readily apparent to those skilled in the art that various modifications to these embodiments may be made, and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above embodiments, and those skilled in the art should make improvements and modifications within the scope of the present invention based on the disclosure of the present invention.
Claims (10)
1. The high-capacity lithium ion battery cathode active material is characterized by comprising one or more of a silicon simple substance or a silicon compound, wherein the silicon compound contains magnesium, and the total content of the magnesium accounts for 5-40% of the total weight.
2. The negative active material of claim 1, having a particle size of between 1 μm and 50 μm.
3. The negative active material of claim 1, wherein the weight ratio of oxygen in the silicon compound is less than 40%.
4. The negative active material of claim 1, wherein the silicon compound is a combination of silicon monoxide and magnesium silicide.
5. The negative active material of claim 1, further comprising a second active material selected from one or more of natural graphite, artificial graphite, mesocarbon microbeads, lithium titanate, silicon or silicon-carbon alloy, tin alloy, and active lithium metal.
6. A negative electrode sheet comprising the negative electrode active material according to any one of claims 1 to 5.
7. A negative electrode sheet according to claim 6, wherein the negative electrode active material is present in an amount of 5 to 100% by mass.
8. A negative electrode sheet according to claim 7, wherein the negative electrode active material is 93% by mass.
9. A lithium ion battery comprising the negative electrode sheet according to claim 6.
10. The lithium ion battery of claim 9, wherein the positive active material in the positive plate is any one or a combination of more of lithium cobaltate, lithium manganate, lithium iron phosphate, lithium iron manganese phosphate, lithium nickel cobalt manganese oxide, and nickel manganese spinel.
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| CN202110973237.8A CN113764651A (en) | 2021-08-24 | 2021-08-24 | High-capacity lithium ion battery negative electrode active material, negative electrode plate and lithium ion battery |
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| CN202110973237.8A CN113764651A (en) | 2021-08-24 | 2021-08-24 | High-capacity lithium ion battery negative electrode active material, negative electrode plate and lithium ion battery |
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Citations (6)
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|---|---|---|---|---|
| CN104241620A (en) * | 2013-06-21 | 2014-12-24 | 国立大学法人蔚山科学技术大学校产学协力团 | Porous silicon based negative electrode active material, method for manufacturing the same, and rechargeable lithium battery including the same |
| CN104659333A (en) * | 2015-01-04 | 2015-05-27 | 合肥国轩高科动力能源股份公司 | Preparation method of Mg2Si/SiOx/C composite cathode material membrane electrode of lithium ion secondary battery |
| US20160164084A1 (en) * | 2013-07-25 | 2016-06-09 | The Regents Of The University Of California | High energy density silicide-air batteries |
| CN110311120A (en) * | 2019-07-10 | 2019-10-08 | 洛阳联创锂能科技有限公司 | A kind of lithium ion battery negative electrode material of SiClx containing magnesia and preparation method thereof |
| CN111816855A (en) * | 2020-07-20 | 2020-10-23 | 长沙晟天新材料有限公司 | Preparation method of magnesium-containing silicon monoxide/silicon @ resin carbon/CVD carbon material |
| CN112349900A (en) * | 2019-08-07 | 2021-02-09 | 珠海冠宇电池股份有限公司 | Negative pole piece and lithium ion battery containing same |
-
2021
- 2021-08-24 CN CN202110973237.8A patent/CN113764651A/en active Pending
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN104241620A (en) * | 2013-06-21 | 2014-12-24 | 国立大学法人蔚山科学技术大学校产学协力团 | Porous silicon based negative electrode active material, method for manufacturing the same, and rechargeable lithium battery including the same |
| US20160164084A1 (en) * | 2013-07-25 | 2016-06-09 | The Regents Of The University Of California | High energy density silicide-air batteries |
| CN104659333A (en) * | 2015-01-04 | 2015-05-27 | 合肥国轩高科动力能源股份公司 | Preparation method of Mg2Si/SiOx/C composite cathode material membrane electrode of lithium ion secondary battery |
| CN110311120A (en) * | 2019-07-10 | 2019-10-08 | 洛阳联创锂能科技有限公司 | A kind of lithium ion battery negative electrode material of SiClx containing magnesia and preparation method thereof |
| CN112349900A (en) * | 2019-08-07 | 2021-02-09 | 珠海冠宇电池股份有限公司 | Negative pole piece and lithium ion battery containing same |
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Application publication date: 20211207 |