CN108963196B - Lithium-sulfur battery positive electrode material containing metal boride - Google Patents
Lithium-sulfur battery positive electrode material containing metal boride Download PDFInfo
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- CN108963196B CN108963196B CN201710357015.7A CN201710357015A CN108963196B CN 108963196 B CN108963196 B CN 108963196B CN 201710357015 A CN201710357015 A CN 201710357015A CN 108963196 B CN108963196 B CN 108963196B
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- sulfur battery
- metal boride
- positive electrode
- electrode material
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- 229910052751 metal Inorganic materials 0.000 title claims abstract description 48
- 239000002184 metal Substances 0.000 title claims abstract description 48
- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 239000007774 positive electrode material Substances 0.000 title claims abstract description 22
- 239000002245 particle Substances 0.000 claims abstract description 14
- 239000010405 anode material Substances 0.000 claims abstract description 9
- 229910052720 vanadium Inorganic materials 0.000 claims description 5
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 5
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 4
- 229910007948 ZrB2 Inorganic materials 0.000 claims description 3
- UHPOHYZTPBGPKO-UHFFFAOYSA-N bis(boranylidyne)chromium Chemical compound B#[Cr]#B UHPOHYZTPBGPKO-UHFFFAOYSA-N 0.000 claims description 3
- XSPFOMKWOOBHNA-UHFFFAOYSA-N bis(boranylidyne)tungsten Chemical compound B#[W]#B XSPFOMKWOOBHNA-UHFFFAOYSA-N 0.000 claims description 3
- ZDVYABSQRRRIOJ-UHFFFAOYSA-N boron;iron Chemical compound [Fe]#B ZDVYABSQRRRIOJ-UHFFFAOYSA-N 0.000 claims description 3
- TWSYZNZIESDJPJ-UHFFFAOYSA-N boron;molybdenum Chemical compound B#[Mo]#B TWSYZNZIESDJPJ-UHFFFAOYSA-N 0.000 claims description 3
- JEUVAEBWTRCMTB-UHFFFAOYSA-N boron;tantalum Chemical compound B#[Ta]#B JEUVAEBWTRCMTB-UHFFFAOYSA-N 0.000 claims description 3
- VWZIXVXBCBBRGP-UHFFFAOYSA-N boron;zirconium Chemical compound B#[Zr]#B VWZIXVXBCBBRGP-UHFFFAOYSA-N 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- 239000010955 niobium Substances 0.000 claims description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 3
- 229910052702 rhenium Inorganic materials 0.000 claims description 3
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 claims description 3
- 230000000694 effects Effects 0.000 abstract description 10
- 238000000034 method Methods 0.000 abstract description 10
- 239000005077 polysulfide Substances 0.000 abstract description 9
- 229920001021 polysulfide Polymers 0.000 abstract description 9
- 150000008117 polysulfides Polymers 0.000 abstract description 9
- 230000003197 catalytic effect Effects 0.000 abstract description 6
- 238000006243 chemical reaction Methods 0.000 abstract description 6
- 238000007599 discharging Methods 0.000 abstract description 4
- 238000011031 large-scale manufacturing process Methods 0.000 abstract description 3
- 230000008569 process Effects 0.000 abstract description 3
- 150000001875 compounds Chemical class 0.000 abstract description 2
- 238000012983 electrochemical energy storage Methods 0.000 abstract description 2
- 230000009286 beneficial effect Effects 0.000 abstract 1
- 230000001737 promoting effect Effects 0.000 abstract 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 16
- 229910052744 lithium Inorganic materials 0.000 description 9
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 7
- 239000003575 carbonaceous material Substances 0.000 description 6
- 238000001179 sorption measurement Methods 0.000 description 6
- 239000000463 material Substances 0.000 description 4
- 238000002844 melting Methods 0.000 description 4
- 230000008018 melting Effects 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 229910052717 sulfur Inorganic materials 0.000 description 4
- 239000011593 sulfur Substances 0.000 description 4
- 239000003792 electrolyte Substances 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000013329 compounding Methods 0.000 description 2
- 230000001351 cycling effect Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000007806 chemical reaction intermediate Substances 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
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
- H01M4/362—Composites
-
- 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
-
- 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
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
-
- 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
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Composite Materials (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention relates to a lithium-sulfur battery positive electrode material containing metal boride. The invention belongs to the technical field of electrochemical energy storage. A lithium-sulfur battery anode material containing metal boride is characterized in that: a positive electrode material for a lithium-sulfur battery containing a metal boride contains metal boride particles. The method utilizes the metal boride to have strong polarity characteristics and catalytic conversion function, effectively adsorbs and catalytically converts polysulfide generated in the charging and discharging process of the lithium-sulfur battery, inhibits the shuttle effect of the lithium-sulfur battery, improves the cycle performance and the coulombic efficiency of the lithium-sulfur battery, and is beneficial to promoting the practicability of the lithium-sulfur battery. The invention has the advantages of simple compound mode, convenient operation, easy large-scale production, strong practicability, capability of effectively prolonging the cycle life of the lithium-sulfur battery and the like.
Description
Technical Field
The invention belongs to the technical field of electrochemical energy storage, and particularly relates to a metal boride-containing lithium-sulfur battery positive electrode material.
Background
In a lithium-sulfur battery system, metal lithium is used as a negative electrode, elemental sulfur is used as a positive electrode, the theoretical specific energy can reach 2600Wh/kg, and the theoretical specific energy is far greater than that of a modern commercial lithium ion battery. In addition, the elemental sulfur also has the characteristics of low price and environmental friendliness. Therefore, lithium sulfur batteries have a very high commercial potential. However, lithium sulfur batteries also have a number of problems, the most significant of which is the low utilization of the active material due to the non-conductivity of elemental sulfur and the poor cyclability due to the "shuttle effect". The main reason for generating the "shuttle effect" is that elemental sulfur generates a large amount of intermediate products, namely lithium polysulfide, in the discharging process, the lithium polysulfide can be dissolved in the electrolyte, polysulfide negative ions generated after the dissolution can be diffused to the surface of the metal lithium of the negative electrode, and then are subjected to reduction reaction with the metal lithium, and are returned to the positive electrode, and then oxidation reaction occurs, namely the "shuttle effect". The effect not only reduces the coulombic efficiency of the lithium-sulfur battery and corrodes the lithium metal cathode, but also generates a large amount of insulating reduction products on the surface of the lithium metal, thereby increasing the internal resistance of the battery.
In order to solve the above problems, researchers have improved the cycle stability of lithium-sulfur batteries by loading elemental sulfur into mesoporous carbon Materials with high specific surface area through the physical adsorption of the mesoporous carbon Materials (Ji XL, et al. nature Materials,2009,8, 500-; researchers have also used the chemisorption of polar substances to polysulfides to inhibit their migration to the negative electrode, for example: nitrogen is doped in mesoporous carbon to improve the surface polarity of the carbon material, thereby improving the cycle performance of the lithium-sulfur battery (Song JX et al, adv. Funct. Mater.,2014,24, 1243-1250). However, the method for producing the mesoporous carbon material and the method for doping the same are complicated, have poor adsorption to polysulfide, and have a problem of a long difference from practical performance.
Disclosure of Invention
The invention provides a positive electrode material of a lithium-sulfur battery containing metal boride for solving the technical problems in the prior art.
The invention aims to provide the positive electrode material containing the metal boride for the lithium-sulfur battery, which has the characteristics of simple compounding mode, convenience in operation, easiness in large-scale production, strong practicability, capability of effectively prolonging the cycle life of the lithium-sulfur battery and the like.
The patent proposes that a non-carbon material, namely metal boride, is used as a carrier of elemental sulfur, and the cycling stability of the lithium-sulfur battery anode material is improved by utilizing the strong chemical adsorption capacity and the catalytic conversion capacity of the metal boride.
The invention solves the problems of weak adsorption capacity and low catalytic conversion capacity of a positive electrode material to a reaction intermediate product in a lithium-sulfur battery, and promotes the chemical adsorption and electrochemical catalytic conversion of polysulfide by introducing transition metal boride particles into the positive electrode material and utilizing the strong polarity characteristic and the catalytic conversion function of the metal boride. On the basis, the method improves the capacity and the cycling stability of the lithium-sulfur battery cathode material, and promotes the practicability of the lithium-sulfur battery.
The technical scheme adopted by the lithium-sulfur battery anode material containing the metal boride is as follows:
a lithium-sulfur battery anode material containing metal boride is characterized in that: a positive electrode material for a lithium-sulfur battery containing a metal boride contains metal boride particles.
The lithium-sulfur battery anode material containing the metal boride can also adopt the following technical scheme:
the lithium-sulfur battery positive electrode material containing the metal boride is characterized in that: the metal boride is one or more of vanadium diboride, molybdenum diboride, zirconium diboride, chromium diboride, aluminum diboride, tungsten diboride, rhenium diboride, niobium diboride, tantalum diboride and iron boride.
The lithium-sulfur battery positive electrode material containing the metal boride is characterized in that: the metal boride particles have a size of from 1 nanometer to 500 micrometers.
The lithium-sulfur battery positive electrode material containing the metal boride is characterized in that: the mass percentage of the metal boride in the anode material is 1-50%.
The invention has the advantages and positive effects that:
compared with the prior art, the anode material of the lithium-sulfur battery containing the metal boride has the following obvious characteristics due to the adoption of the brand-new technical scheme of the invention:
1. according to the lithium-sulfur battery, the metal boride particles are added into the positive electrode material, and can generate a strong chemical adsorption effect and a strong catalytic conversion effect with polysulfide negative ions in a lithium-sulfur battery system, so that the polysulfide negative ions can be effectively prevented from migrating to a lithium negative electrode along with electrolyte, a shuttle effect is inhibited, the coulombic efficiency of the lithium-sulfur battery is effectively improved, and the cycle life of the battery is prolonged;
2. the metal boride particles adopted by the invention have good conductive property, can be directly used as a carrier of elemental sulfur, and a conductive carbon material is not added or is added in a small amount, so that the sulfur carrying capacity of the lithium-sulfur battery is effectively improved;
3. the method has the advantages of simple compounding mode of the metal boride and the elemental sulfur, capability of adopting a mechanical mixing or heating melting method, simple operation, easiness for large-scale production and strong practicability.
Detailed Description
In order to further understand the contents, features and effects of the present invention, the following examples are illustrated and described in detail as follows:
example 1
A positive electrode material for a lithium-sulfur battery containing a metal boride comprises metal boride particles. The metal boride particle for the lithium-sulfur secondary battery anode material adopts one or a mixture of more of vanadium diboride, molybdenum diboride, zirconium diboride, chromium diboride, aluminum diboride, tungsten diboride, rhenium diboride, niobium diboride, tantalum diboride and iron boride. The metal boride is compounded with elemental sulfur or other sulfur-containing materials by mechanical mixing or heating and melting methods. The mass fraction of the metal boride particles in the cathode material (comprising elemental sulfur, a conductive agent, a binder and an additive) is between 1 and 50 percent, and the size of the metal boride particles is between 1 nanometer and 500 micrometers.
The specific implementation process of the embodiment:
firstly, vanadium diboride particles with the particle size of 200-500 nanometers and elemental sulfur are uniformly mixed according to the mass ratio of 2:3, sulfur melting is carried out for 6 hours at 155 ℃, then, the sulfur melting composite material, SP and LA132 are ball-milled and uniformly mixed according to the mass ratio of 8:1:1, slurry with the solid content of 30 percent is formed to be used as a positive electrode material, the positive electrode material is coated on an aluminum foil positive current collector, and the positive electrode material is pressed into a positive electrode piece after being dried for 6 hours in a vacuum drying box; the method comprises the steps of preparing a CR2430 type lithium-sulfur button cell by using a Celgard2400 diaphragm as a cell diaphragm, a metal lithium sheet as a cathode and a DOL/DME (1:1) solution of 1M LiTFSI as an electrolyte, testing after the cell is prepared, calculating the charging and discharging specific capacity based on an elemental sulfur active material, performing charge-discharge cycle test by using a current density of 0.1C, wherein the first discharging specific capacity is 1280mAh/g, and the specific capacity is 987mAh/g after 100 cycles.
Comparative example 1
The vanadium diboride in the example 1 is replaced by SP, the other materials, the material proportion and the battery manufacturing process are the same as those in the example 1, the charge-discharge cycle test is carried out by using the current density of 0.1C, the first discharge specific capacity is 1012mAh/g, and the specific capacity is 601mAh/g after 30 cycles.
It can be seen from example 1 and comparative example 1 that the lithium-sulfur battery using the metal boride has significant advantages over the cycle performance and specific capacity of the conventional lithium-sulfur battery, indicating that the metal boride can effectively inhibit the shuttle effect of the lithium-sulfur battery, improve the battery performance, and prolong the cycle life of the battery.
The embodiment has the advantages of simple compound mode, convenient operation, easy mass production, strong practicability, effective improvement of the cycle life of the lithium-sulfur battery, and the like.
Claims (3)
1. A positive electrode material for a lithium-sulfur battery containing a metal boride, characterized by: the positive electrode material of the lithium-sulfur battery containing the metal boride contains metal boride particles; the metal boride is one or more of vanadium diboride, molybdenum diboride, zirconium diboride, chromium diboride, aluminum diboride, tungsten diboride, rhenium diboride, niobium diboride, tantalum diboride and iron boride.
2. The metal boride-containing lithium sulfur battery positive electrode material as claimed in claim 1, wherein: the metal boride particles have a size of from 1 nanometer to 500 micrometers.
3. The metal boride-containing lithium sulfur battery positive electrode material as claimed in claim 1, wherein: the mass percentage of the metal boride in the anode material is 1-50%.
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| CN114695884B (en) * | 2020-12-29 | 2023-06-27 | 天目湖先进储能技术研究院有限公司 | Method and material for inhibiting polysulfide shuttle effect in lithium-sulfur battery and application of material |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102683659A (en) * | 2012-05-31 | 2012-09-19 | 中国科学院物理研究所 | Lithium-sulphur battery anode material and preparation method thereof |
| CN103201885A (en) * | 2010-06-17 | 2013-07-10 | L·F·纳扎尔 | Multicomponent electrodes for rechargeable batteries |
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| KR20120051549A (en) * | 2010-11-12 | 2012-05-22 | 현대자동차주식회사 | Cathode active material for metal-sulfur battery and process for preparing the same |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103201885A (en) * | 2010-06-17 | 2013-07-10 | L·F·纳扎尔 | Multicomponent electrodes for rechargeable batteries |
| CN102683659A (en) * | 2012-05-31 | 2012-09-19 | 中国科学院物理研究所 | Lithium-sulphur battery anode material and preparation method thereof |
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