CN113113591A - Method for improving rate performance of lithium-sulfur battery - Google Patents
Method for improving rate performance of lithium-sulfur battery Download PDFInfo
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- CN113113591A CN113113591A CN202110303959.2A CN202110303959A CN113113591A CN 113113591 A CN113113591 A CN 113113591A CN 202110303959 A CN202110303959 A CN 202110303959A CN 113113591 A CN113113591 A CN 113113591A
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- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 title claims abstract description 49
- 238000000034 method Methods 0.000 title claims abstract description 33
- 239000002105 nanoparticle Substances 0.000 claims abstract description 35
- QGJOPFRUJISHPQ-UHFFFAOYSA-N Carbon disulfide Chemical compound S=C=S QGJOPFRUJISHPQ-UHFFFAOYSA-N 0.000 claims abstract description 33
- 239000000463 material Substances 0.000 claims abstract description 33
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 22
- 238000003756 stirring Methods 0.000 claims abstract description 22
- 239000002033 PVDF binder Substances 0.000 claims abstract description 19
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims abstract description 19
- 238000002156 mixing Methods 0.000 claims abstract description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000006230 acetylene black Substances 0.000 claims abstract description 14
- 230000005684 electric field Effects 0.000 claims abstract description 13
- 239000007774 positive electrode material Substances 0.000 claims abstract description 11
- 239000000203 mixture Substances 0.000 claims abstract description 10
- 238000007599 discharging Methods 0.000 claims abstract description 9
- 238000005286 illumination Methods 0.000 claims abstract description 9
- OXHNLMTVIGZXSG-UHFFFAOYSA-N 1-Methylpyrrole Chemical compound CN1C=CC=C1 OXHNLMTVIGZXSG-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000003517 fume Substances 0.000 claims abstract description 8
- 238000000227 grinding Methods 0.000 claims abstract description 8
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 9
- 239000010931 gold Substances 0.000 claims description 9
- 229910052737 gold Inorganic materials 0.000 claims description 9
- 238000000926 separation method Methods 0.000 claims description 5
- 230000035484 reaction time Effects 0.000 claims description 2
- 239000002086 nanomaterial Substances 0.000 abstract description 6
- 238000012546 transfer Methods 0.000 abstract description 3
- 230000002708 enhancing effect Effects 0.000 abstract 1
- 229910052717 sulfur Inorganic materials 0.000 description 6
- 239000011593 sulfur Substances 0.000 description 6
- QGJOPFRUJISHPQ-NJFSPNSNSA-N carbon disulfide-14c Chemical compound S=[14C]=S QGJOPFRUJISHPQ-NJFSPNSNSA-N 0.000 description 5
- 238000001035 drying Methods 0.000 description 5
- 238000012360 testing method Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- 229910001416 lithium ion Inorganic materials 0.000 description 2
- GLNWILHOFOBOFD-UHFFFAOYSA-N lithium sulfide Chemical compound [Li+].[Li+].[S-2] GLNWILHOFOBOFD-UHFFFAOYSA-N 0.000 description 2
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 1
- XKTYXVDYIKIYJP-UHFFFAOYSA-N 3h-dioxole Chemical compound C1OOC=C1 XKTYXVDYIKIYJP-UHFFFAOYSA-N 0.000 description 1
- 229910001216 Li2S Inorganic materials 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
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Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
-
- 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
-
- 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
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
-
- 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 discloses a method for improving the rate capability of a lithium-sulfur battery, which comprises the following steps: mixing elemental sulfur and the nano particles in a mass ratio of 1:1 to 5: 2; s2, adding the mixed material into a carbon disulfide solution, and stirring in a fume hood until the carbon disulfide solution volatilizes; s3, placing the mixture into a high-pressure reaction kettle, reacting for 10-15 h at the temperature of 120-170 ℃, taking out and grinding the mixture; s4, mixing the acetylene black and the polyvinylidene fluoride according to the mass ratio of 5:2:2 to 8:2:1, then dropwise adding n-methyl pyrrole, stirring for 1-4 h, and taking the mixture as a positive electrode material of the lithium-sulfur battery; and S5, introducing ambient light in the charging and discharging process of the lithium-sulfur battery, and enabling the nanoparticles to generate electron-hole pairs so as to construct a local electric field on the surface of the nanoparticles. According to the invention, the nano material generates electron hole pairs through ambient illumination (mainly sunlight), so that a local electric field is constructed on the surface of the nano material, thereby reducing the transfer resistance of the electrode and enhancing the multiplying power performance.
Description
Technical Field
The invention belongs to the field of lithium-sulfur batteries, and particularly relates to a method for improving the rate capability of a lithium-sulfur battery.
Background
As the energy density of lithium ion batteries approaches the upper limit, lithium/sulfur (Li/S) batteries are increasingly attracting attention due to the abundance of elemental sulfur and low cost. From complete reduction of elemental sulphur to lithium sulphide (Li)2S), the specific capacity of sulfur delivery is expected to be 1675mAh/g, the energy density is 2600Wh/kg, which is 3-5 times higher than that of the most advanced lithium ion battery at present, so that the lithium sulfur battery becomes one of the most promising next-generation energy storage systems.
However, to realize commercialization of lithium sulfur batteries, some problems are still faced. Elemental sulfur and lithium sulfide have poor electronic and ionic conductivity, and sulfur materials have very low conductivity at room temperature (5.0X 10)-30S/cm), end product of the reaction Li2S2And Li2S is also an electronic insulator, which is not beneficial to the high rate performance of the lithium-sulfur battery, and no effective method for improving the rate performance exists at present.
Disclosure of Invention
In view of the above technical problems, the present invention provides a method for improving rate performance of a lithium-sulfur battery, comprising the following steps:
s1, mixing the elemental sulfur and the nano particles in a mass ratio of 1:1 to 5: 2;
s2, adding the mixed material into a carbon disulfide solution, and stirring in a fume hood until the carbon disulfide solution volatilizes;
s3, placing the material obtained in the step S2 in a high-pressure reaction kettle, reacting for 10-15 hours at the temperature of 120-170 ℃, taking out and grinding;
s4, mixing the material obtained in the step S3 with acetylene black and polyvinylidene fluoride according to the mass ratio of 5:2:2 to 8:2:1, then dropwise adding n-methyl pyrrole, stirring for 1-4 h, and taking the mixture as a positive electrode material of a lithium-sulfur battery;
s5, introducing ambient light in the charging and discharging process of the lithium-sulfur battery to enable the nanoparticles to generate electron hole pairs, so that a local electric field is constructed on the surface of the nanoparticles;
the nanoparticles produce electron-hole pair separation under illumination.
Preferably, in S1, gold nanoparticles are used, and the mass ratio of elemental sulfur to gold nanoparticles is 7: 3.
Preferably, in the S3, the reaction temperature is 155 ℃ and the reaction time is 12 h.
In S4, the mass ratio of the material obtained after S3, acetylene black and polyvinylidene fluoride is preferably 7:2:1, and stirring is carried out for 2.5 h.
In S4, the mass ratio of the material obtained after S3, acetylene black and polyvinylidene fluoride is preferably 9:3:2, and stirring is carried out for 4 hours.
In S4, the mass ratio of the material obtained after S3, acetylene black and polyvinylidene fluoride is preferably 8:2:1, and stirring is carried out for 3 hours.
Preferably, the ambient light is sunlight.
The invention has the following beneficial effects: the invention provides a method for improving the rate capability of a lithium-sulfur battery. A nano material capable of generating electron hole pair separation under illumination is introduced into a sulfur electrode, and the nano material generates electron hole pairs through illumination (mainly sunlight) in the working process of a lithium sulfur battery, so that a local electric field is constructed on the surface of the nano material, the transfer resistance of the electrode is reduced, the charging and discharging process of the lithium sulfur battery is effectively promoted, and the rate capability of the lithium sulfur battery is improved. Meanwhile, the illumination mode is green and environment-friendly and is easy to realize.
Drawings
FIG. 1 is a flowchart illustrating steps of a method for improving rate capability of a lithium-sulfur battery according to an embodiment of the present invention;
fig. 2 is a rate performance curve diagram of the lithium-sulfur battery obtained by the method for improving the rate performance of the lithium-sulfur battery in the embodiment of the invention under different rates of charge and discharge currents.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some, not all, embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Referring to fig. 1, the present invention provides a method for improving rate performance of a lithium-sulfur battery, including the following steps:
s1, mixing elemental sulfur with nanoparticles capable of generating electron-hole pair separation under illumination, wherein the mass ratio of the elemental sulfur to the nanoparticles is 1: 1-5: 2;
s2, adding the mixed material into carbon disulfide, and stirring in a fume hood until the carbon disulfide solution volatilizes;
s3, placing the material obtained in the step S2 in a high-pressure reaction kettle, reacting for 10-15 hours in a drying box at 120-170 ℃, taking out and grinding;
s4, mixing the material obtained in the step S3 with acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 5:2:2 to 8:2:1, then dropwise adding n-methyl pyrrole, stirring for 1-4 h, and taking the mixture as a positive electrode material of a lithium-sulfur battery;
and S5, introducing ambient light in the charging and discharging process of the lithium-sulfur battery, and promoting the introduced nano particles to generate electron-hole pairs so as to construct a local electric field on the surface of the nano particles.
In the technical scheme, firstly, a composite material of nanoparticles and elemental sulfur which can generate electron hole pair separation under illumination is used as the anode of the lithium-sulfur battery; and secondly, introducing ambient light (mainly sunlight) in the working process of the lithium-sulfur battery, wherein the illumination can promote the introduced nano particles to generate electron hole pairs, so that a local electric field is constructed on the surface of the introduced nano material, the electric field can effectively promote the charge and discharge process of the lithium-sulfur battery, and the rate capability of the lithium-sulfur battery is improved.
EXAMPLE 1
S1, mixing the elemental sulfur and the gold nanoparticles, wherein the mass ratio of the elemental sulfur to the gold nanoparticles is 7: 3; s2, adding the mixed material into carbon disulfide, and stirring in a fume hood until the carbon disulfide solution volatilizes; s3, placing the obtained material in a high-pressure reaction kettle to react for 12 hours at the temperature of 155 ℃ in a drying box, taking out and grinding the material; s4, mixing the obtained material with acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 7:2:1, then dropwise adding n-methyl pyrrole, stirring for 2.5h, and taking the mixture as a positive electrode material of a lithium-sulfur battery; s5, during the charging and discharging process of the lithium sulfur battery, the introduced nano particles are caused to generate electron hole pairs by the irradiation of the solar light, so that a local electric field is constructed on the surface of the nano particles.
Instantiation 2
S1, mixing the elemental sulfur and the gold nanoparticles in a mass ratio of 2: 1; s2, adding the mixed material into carbon disulfide, and stirring in a fume hood until the carbon disulfide solution volatilizes; s3, placing the obtained material in a high-pressure reaction kettle to react for 15 hours at 180 ℃ in a drying box, taking out and grinding the material; s4, mixing the obtained material with acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 9:3:2, then dropwise adding n-methyl pyrrole, stirring for 4h, and taking the mixture as a positive electrode material of a lithium-sulfur battery; s5, during the charging and discharging process of the lithium sulfur battery, the introduced nano particles are caused to generate electron hole pairs by the irradiation of the solar light, so that a local electric field is constructed on the surface of the nano particles.
Instantiation 3
S1, mixing the elemental sulfur and the gold nanoparticles in a mass ratio of 1: 1; s2, adding the mixed material into carbon disulfide, and stirring in a fume hood until the carbon disulfide solution volatilizes; s3, placing the obtained material in a high-pressure reaction kettle to react for 10 hours at 120 ℃ in a drying box, and then taking out and grinding the material; s4, mixing the obtained material with acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 5:2:2, then dropwise adding n-methyl pyrrole, stirring for 1h, and taking the mixture as a positive electrode material of a lithium-sulfur battery; and S5, placing the lithium-sulfur battery in a room to be irradiated by an incandescent lamp in the charging and discharging process of the lithium-sulfur battery, and prompting the introduced nano particles to generate electron-hole pairs so as to construct a local electric field on the surface of the nano particles.
Instantiation 4
S1, mixing the elemental sulfur and the gold nanoparticles in a mass ratio of 5: 2; s2, adding the mixed material into carbon disulfide, and stirring in a fume hood until the carbon disulfide solution volatilizes; s3, placing the obtained material in a high-pressure reaction kettle to react for 12 hours at the temperature of 170 ℃ in a drying box, taking out and grinding the material; s4, mixing the obtained material with acetylene black and polyvinylidene fluoride (PVDF) according to the mass ratio of 8:2:1, then dropwise adding n-methyl pyrrole, stirring for 3h, and taking the mixture as a positive electrode material of a lithium-sulfur battery; s5, during the charging and discharging process of the lithium sulfur battery, the introduced nano particles are caused to generate electron hole pairs by the irradiation of the solar light, so that a local electric field is constructed on the surface of the nano particles.
Fig. 2 is a rate performance curve of the lithium-sulfur battery obtained by the method of the present invention under different rates (0.2C,0.5C,1C,2C,1C,0.5C,0.2C, based on the theoretical capacity of sulfur 1674 mAh/g), and the specific capacity decrease ratio is smaller as the discharge rate increases. And under the same discharge rate, the specific discharge capacity of the positive electrode material is relatively stable, and when the rate is recovered to 0.2C, the recovery of the battery capacity also proves the stability of the positive electrode material.
Further, the performance test is carried out on the method. The specific test process is as follows: the anode of the selected lithium-sulfur battery to be tested is the sulfur/nanoparticle composite material, the cathode is a lithium sheet, Celgard2325 is used as a diaphragm, 1mLiTFSI is dissolved in 1, 3-Dioxolane (DOL) and ethylene glycol dimethyl ether (DME) (volume ratio of 1:1) to be used as electrolyte, and the battery is assembled by using an LIR2032 coin-shaped battery case in a glove box which is filled with argon gas for protection and has humidity and oxygen concentration lower than 1 ppm. In the charge and discharge test system, the charge and discharge test voltage is 1.7V-2.8V.
According to the analysis, the local electric field is constructed on the surface of the lithium-sulfur battery positive electrode material, so that the transfer resistance is reduced, the rate capability of the lithium-sulfur battery is stable, and when the charge and discharge rate is recovered, the specific capacity of the lithium-sulfur battery can be well recovered, which indicates that the rate capability of the lithium-sulfur battery is effectively improved by the method.
It is to be understood that the exemplary embodiments described herein are illustrative and not restrictive. Although one or more embodiments of the present invention have been described with reference to the accompanying drawings, it will be understood by those of ordinary skill in the art that various changes in form and details may be made therein without departing from the spirit and scope of the present invention as defined by the following claims.
Claims (7)
1. A method for improving the rate performance of a lithium-sulfur battery is characterized by comprising the following steps:
s1, mixing the elemental sulfur and the nano particles in a mass ratio of 1:1 to 5: 2;
s2, adding the mixed material into a carbon disulfide solution, and stirring in a fume hood until the carbon disulfide solution volatilizes;
s3, placing the material obtained in the step S2 in a high-pressure reaction kettle, reacting for 10-15 hours at the temperature of 120-170 ℃, taking out and grinding;
s4, mixing the material obtained in the step S3 with acetylene black and polyvinylidene fluoride according to the mass ratio of 5:2:2 to 8:2:1, then dropwise adding n-methyl pyrrole, stirring for 1-4 h, and taking the mixture as a positive electrode material of a lithium-sulfur battery;
s5, introducing ambient light in the charging and discharging process of the lithium-sulfur battery to enable the nanoparticles to generate electron hole pairs, so that a local electric field is constructed on the surface of the nanoparticles;
the nanoparticles produce electron-hole pair separation under illumination.
2. The method according to claim 1, wherein in S1, gold nanoparticles are used, and the mass ratio of elemental sulfur to gold nanoparticles is 7: 3.
3. The method for improving rate performance of a lithium-sulfur battery as claimed in claim 1, wherein in S3, the reaction temperature is 155 ℃ and the reaction time is 12 h.
4. The method for improving the rate capability of the lithium-sulfur battery as claimed in claim 1, wherein in S4, the mass ratio of the obtained material after S3, acetylene black and polyvinylidene fluoride is 7:2:1, and stirring is carried out for 2.5 h.
5. The method for improving the rate capability of the lithium-sulfur battery as claimed in claim 1, wherein in S4, the mass ratio of the obtained material after S3, acetylene black and polyvinylidene fluoride is 9:3:2, and stirring is carried out for 4 hours.
6. The method for improving the rate capability of the lithium-sulfur battery as claimed in claim 1, wherein in S4, the mass ratio of the obtained material after S3, acetylene black and polyvinylidene fluoride is 8:2:1, and stirring is carried out for 3 h.
7. The method of claim 1, wherein the ambient light is sunlight.
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