CN105374982A - Electrode structure of lithium sulfur battery and processing technology therefor - Google Patents
Electrode structure of lithium sulfur battery and processing technology therefor Download PDFInfo
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- CN105374982A CN105374982A CN201510923554.3A CN201510923554A CN105374982A CN 105374982 A CN105374982 A CN 105374982A CN 201510923554 A CN201510923554 A CN 201510923554A CN 105374982 A CN105374982 A CN 105374982A
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- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 title claims abstract description 30
- 238000012545 processing Methods 0.000 title abstract description 5
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 78
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 76
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000003792 electrolyte Substances 0.000 claims abstract description 11
- 229910052717 sulfur Inorganic materials 0.000 claims abstract description 9
- 239000011593 sulfur Substances 0.000 claims abstract description 9
- 239000011248 coating agent Substances 0.000 claims description 53
- 238000000576 coating method Methods 0.000 claims description 53
- 239000011149 active material Substances 0.000 claims description 27
- 239000000463 material Substances 0.000 claims description 13
- 239000005864 Sulphur Substances 0.000 claims description 10
- 238000002156 mixing Methods 0.000 claims description 10
- 239000002002 slurry Substances 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 10
- 229910052744 lithium Inorganic materials 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 7
- 230000008569 process Effects 0.000 claims description 7
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 6
- 230000004888 barrier function Effects 0.000 claims description 4
- 239000000835 fiber Substances 0.000 claims description 4
- 239000003292 glue Substances 0.000 claims description 4
- 239000003273 ketjen black Substances 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 239000010410 layer Substances 0.000 abstract description 28
- 239000005077 polysulfide Substances 0.000 abstract description 10
- 229920001021 polysulfide Polymers 0.000 abstract description 10
- 150000008117 polysulfides Polymers 0.000 abstract description 10
- 230000000694 effects Effects 0.000 abstract description 7
- 239000013543 active substance Substances 0.000 abstract 7
- 239000011247 coating layer Substances 0.000 abstract 7
- 239000003575 carbonaceous material Substances 0.000 abstract 4
- 238000004090 dissolution Methods 0.000 abstract 1
- 238000003411 electrode reaction Methods 0.000 abstract 1
- 239000011229 interlayer Substances 0.000 description 5
- 238000012360 testing method Methods 0.000 description 3
- 239000002131 composite material Substances 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- GJEAMHAFPYZYDE-UHFFFAOYSA-N [C].[S] Chemical compound [C].[S] GJEAMHAFPYZYDE-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 239000005030 aluminium foil Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 239000008187 granular material Substances 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
-
- 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
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
-
- 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)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention discloses an electrode structure of a lithium sulfur battery and a processing technology therefor. The electrode structure comprises a sulfur-containing active substance layer and a current collector; the upper surface of the active substance layer is coated with a first carbon coating layer; the lower surface of the active substance layer is coated with a second carbon coating layer; and the second carbon coating layer is positioned between the active substance layer and the current collector. The electrode structure has the main characteristics that the two sides of the sulfur-containing active substance layer are coated with the carbon coating layers; namely, the surface of the active substance layer, and the space between the active substance layer and the current collector are coated with the carbon coating layers, wherein a carbon material is taken as the main component, and the carbon material with a large specific surface area or low bulk density is preferable; the carbon material with the relatively large specific surface area can absorb polysulfide and restrain a shuttle effect; meanwhile, the carbon material with the low bulk density can form the relatively loosen carbon coating layer so as to store a large amount of electrolyte in the carbon coating layer, and the dissolution of sulfur and the polysulfide is facilitated, a positive electrode reaction is promoted, and the increase of electrolyte viscosity caused by resolution is restrained.
Description
Technical field
The invention belongs to lithium-sulfur cell technical field, particularly relate to a kind of electrode structure of lithium-sulfur cell.
Background technology
In lithium-sulfur cell system, take lithium metal as negative pole, elemental sulfur is positive pole, and theoretical specific energy can reach 2600Wh/kg, much larger than the lithium ion battery of modern commercial.In addition elemental sulfur also has cheap, eco-friendly characteristic.Therefore, lithium-sulfur cell has high business application potential.But lithium-sulfur cell also also exists many problems.Wherein most importantly in the middle of the process of discharge and recharge, the utilance of sulphur is low, and in cyclic process, capacity attenuation is fast.
At present, think that the reason causing this problem comprises many aspects, one of them is elemental sulfur is insulator, and in sulfur electrode, active material activation difficulty is large.And elemental sulfur, in discharge process, produces a large amount of intermediate products, i.e. polysulfide.Polysulfide can be dissolved in the middle of electrolyte, and leaves original position, along with the precipitation of the final reduzate of elemental sulfur, forms a large amount of bulky grains, reduces the invertibity of reduzate oxidation.In addition, polysulfide can be diffused into the surface of negative metal lithium, with lithium metal generation reduction reaction, and returns positive pole, then oxidation reaction occurs, be i.e. " effect of shuttling back and forth ".This effect not only reduces the coulombic efficiency of lithium-sulfur cell, corroding metal cathode of lithium, and can generate a large amount of reduzates at metallic lithium surface, and this product is insulation, and the internal resistance of battery can be caused to increase.
For above problem, researcher proposes more lithium-sulfur cell improvement opportunity.Carbon sulphur composite material is adopted comprising positive pole; Polymer overmold is carried out to the sulfur granules of positive pole or carbon sulphur composite material granular; Single ion permeable film is used to replace existing barrier film; Develop dissimilar electrolyte and electrolysis additive; Use polymer dielectric; Prepare independently self-supporting carbon film.
In these improvement projects, preparing independently self-supporting carbon film and the present invention has certain similitude.At present, the lithium-sulfur cell research of all employing carbon interlayers, all adopts the carbon film with self-supporting ability.By material with carbon element and PTFE binding agent being mixed and roll-in film forming, or use the materials such as carbon cloth.These independently self-supporting carbon film all there is preparation difficulty, and thickness is large, and weight is high, the problem of inconvenience application in battery assembling process.These problems significantly can reduce the energy density of lithium-sulfur cell, improve production cost, therefore, do not have application potential.
Summary of the invention
The technical problem to be solved in the present invention is: low in order to solve lithium-sulphur cell positive electrode utilization efficiency, the problem that cycle life is short, patent proposition of the present invention is a kind of prepares the triple electrode technology of preparing simple, thickness is thin, lightweight, raw material are cheap and easy to get, make it can possess the good hoisting power of similar independent self-supporting carbon interlayer to lithium-sulfur cell performance, simple again, be easy to practical.
The technical scheme that the present invention takes for the technical problem existed in solution known technology is:
An electrode structure for lithium-sulfur cell, comprises active material layer (2) and the collector (4) of sulfur-bearing; The first carbon coating (1) is coated with at the upper surface of described active material layer (2), be coated with the second carbon coating (3) at the lower surface of described active material layer (2), described second carbon coating (3) is positioned between active material layer (2) and collector (4).
Further: the specific area of described first carbon coating (1) is greater than 20m
2/ g.
Further: the bulk density of described first carbon coating (1) is less than 1g/m
3.
Further: the specific area of described second carbon coating (3) is greater than 20m
2/ g.
Further: the bulk density of described second carbon coating (3) is less than 1g/m
3.
Further: the thickness of described first carbon coating (1) and the second carbon coating (3) is greater than 5 microns.
A processing technology for the electrode structure of lithium-sulfur cell, comprises the steps:
Prepared by carbon coating material: by SP, LA132 9:1 mixing in mass ratio, use water as decentralized medium; The slurry mixed to be coated on ready active material layer and to dry, obtaining the first carbon coating (1);
By the 7:1:1:1 mixing in mass ratio of sulphur, Ketjen black, gas-phase growth of carbon fibre, LA132 glue, use water as decentralized medium; The slurry mixed is coated in the first carbon coating (1) go up and dry, obtains active material layer (2);
Prepared by carbon coating material: by SP, LA132 9:1 mixing in mass ratio, use water as decentralized medium; The slurry mixed is coated in ready active material layer (2) go up and dry, obtains the second carbon coating (3); And then obtain positive pole;
Positive pole, barrier film, lithium anode are assembled into CR2430 type button cell; The DOL-DME solution that the electrolyte used is 1mol/LLiTFSI, the volume ratio of DOL and DME is 1:1, and adds 0.4MLiNO3.
The advantage that the present invention has and good effect are:
1, the main feature of patent of the present invention is the active material layer coating on both sides carbon coating at sulfur-bearing, namely on active material layer surface, and between active material layer and collector, and carbon coating coating respectively, or only at active material layer surface-coated carbon coating.Wherein, material with carbon element is main component, should select the material with carbon element that specific area is large or bulk density is low.Higher specific area can adsorb polysulfide, suppresses to shuttle back and forth effect.Meanwhile, the material with carbon element that bulk density is low can form comparatively loose carbon coating, thus in carbon coating, store a large amount of electrolyte, is conducive to the dissolving of sulphur and polysulfide, is beneficial to the generation of positive pole reaction, and alleviates the electrolyte viscosity rising of dissolving and bringing.
2, relative to existing electrode technology, the carbon coating that the present invention adds has very high specific area, effectively can adsorb sulphur and the polysulfide of dissolving, suppresses " effect of shuttling back and forth " in lithium-sulfur cell, thus improve the cycle life of battery, and improve coulombic efficiency.
3, relative to existing electrode technology, the carbon coating that the present invention adds has certain thickness, and is the open structure of porous.Relative to ordinary electrode, a certain amount of electrolyte can be stored, be conducive to the dissolving of sulphur and polysulfide, thus ensure that the generation that anode electrode reacts, improve the discharge capacity of battery.This technology also effectively alleviates the electrolyte viscosity that the dissolving due to sulphur and polysulfide causes and raises.
4, existingly in lithium-sulfur cell, use independently carbon interlayer technology, carbon interlayer is self-supported membrane, and thickness is large, weight is large and preparation difficulty.Relative to independently carbon interlayer technology, the carbon coating in the present invention has that thickness is little, weight is little, it is simple and easy to get to prepare, and spendable material with carbon element wide material sources, also have feature simple to operate in battery assembling process.
Accompanying drawing illustrates:
Fig. 1 is the electrode structure schematic diagram of lithium-sulfur cell in the preferred embodiment of the present invention;
Fig. 2 does not adopt above preferred embodiment structure to contrast with adopting the discharge performance of above preferred embodiment.
In figure: 1, the first carbon coating; 2, active material layer; 3, the second carbon coating; 4, collector.
Embodiment
For summary of the invention of the present invention, Characteristic can be understood further, hereby exemplify following examples, and coordinate accompanying drawing to be described in detail as follows:
Refer to Fig. 1 and Fig. 2, a kind of electrode structure of lithium-sulfur cell, comprise active material layer 2 and the collector 4 of sulfur-bearing; Be coated with the first carbon coating 1 at the upper surface of described active material layer 2, be coated with the second carbon coating 3 at the lower surface of described active material layer 2, described second carbon coating 3 is between active material layer 2 and collector 4.
Further: the specific area of described first carbon coating 1 is greater than 20m
2/ g.
Further: the bulk density of described first carbon coating 1 is less than 1g/m
3.
Further: the specific area of described second carbon coating 3 is greater than 20m
2/ g.
Further: the bulk density of described second carbon coating 3 is less than 1g/m
3.
Further: the thickness of described first carbon coating 1 and the second carbon coating 3 is greater than 5 microns.
A processing technology for the electrode structure of lithium-sulfur cell, comprises the steps:
Prepared by carbon coating material: by the 9:1 mixing in mass ratio of SuperP-Li (SP), LA132 water-base cement, use water as decentralized medium.The slurry mixed to be coated on ready active material layer and to dry, obtaining ground floor---carbon coating.
By the 7:1:1:1 mixing in mass ratio of sulphur, Ketjen black, gas-phase growth of carbon fibre, LA132 glue, use water as decentralized medium.The slurry mixed applied on the first layer and dry, obtaining the second layer---active material layer.
Prepared by carbon coating material: by SP, LA132 9:1 mixing in mass ratio, use water as decentralized medium.The slurry mixed to be coated on ready active material layer and to dry, obtaining third layer---carbon coating.Three layers be painted with after obtain positive pole, anode structure is as shown in Figure 2.
Positive plate, barrier film, lithium anode are assembled into CR2430 type button cell.The DOL-DME solution that the electrolyte used is 1mol/LLiTFSI, the volume ratio of DOL and DME is 1:1, and adds 0.4MLiNO3.
In order to contrast effect, by the 6:2:1:1 mixing in mass ratio of sulphur, Ketjen black, gas-phase growth of carbon fibre, LA132 glue, use water as decentralized medium.The slurry mixed to be coated on aluminium foil and to dry, obtaining comparison electrode.
Carried out charge-discharge test to the positive pole that example 1 obtains, test result is shown in Fig. 2.
The charge-discharge test of example 1 be the results are shown in Figure shown in 2 figure to the discharge performance contrast of the flexible-packed battery being same design capacity, the flexible-packed battery maximum discharge capacity adopting triple electrode to prepare reaches 3.5Ah, circulation volume keeps better, and adopt the discharge capacity of the cell of single-layer electrodes only to reach 2.1Ah, and in circulation, capacity continues to reduce.
In sum, specific discharge capacity and the cycle performance of lithium-sulfur cell can be improved in the present invention significantly for the triple electrode technology of lithium-sulfur cell.And thickness thin, lightweight, prepare simple to operation, also easily apply in battery assembling process.
Above embodiments of the invention have been described in detail, but described content being only preferred embodiment of the present invention, can not being considered to for limiting practical range of the present invention.All equalizations done according to the present patent application scope change and improve, and all should still belong within patent covering scope of the present invention.
Claims (7)
1. an electrode structure for lithium-sulfur cell, comprises active material layer (2) and the collector (4) of sulfur-bearing; It is characterized in that: be coated with the first carbon coating (1) at the upper surface of described active material layer (2), be coated with the second carbon coating (3) at the lower surface of described active material layer (2), described second carbon coating (3) is positioned between active material layer (2) and collector (4).
2. the electrode structure of lithium-sulfur cell according to claim 1, is characterized in that: the specific area of described first carbon coating (1) is greater than 20m
2/ g.
3. the electrode structure of lithium-sulfur cell according to claim 2, is characterized in that: the bulk density of described first carbon coating (1) is less than 1g/m
3.
4. the electrode structure of lithium-sulfur cell according to claim 1, is characterized in that: the specific area of described second carbon coating (3) is greater than 20m
2/ g.
5. the electrode structure of lithium-sulfur cell according to claim 4, is characterized in that: the bulk density of described second carbon coating (3) is less than 1g/m
3.
6. the electrode structure of lithium-sulfur cell according to claim 3 or 5, is characterized in that: the thickness of described first carbon coating (1) and the second carbon coating (3) is greater than 5 microns.
7. a process for the electrode structure of lithium-sulfur cell described in manufacturing claims 6, is characterized in that, comprise the steps:
Prepared by carbon coating material: by SP, LA132 9:1 mixing in mass ratio, use water as decentralized medium; The slurry mixed to be coated on ready active material layer and to dry, obtaining the first carbon coating (1);
By the 7:1:1:1 mixing in mass ratio of sulphur, Ketjen black, gas-phase growth of carbon fibre, LA132 glue, use water as decentralized medium; The slurry mixed is coated in the first carbon coating (1) go up and dry, obtains active material layer (2);
Prepared by carbon coating material: by SP, LA132 9:1 mixing in mass ratio, use water as decentralized medium; The slurry mixed is coated in ready active material layer (2) go up and dry, obtains the second carbon coating (3); And then obtain positive pole;
Positive pole, barrier film, lithium anode are assembled into CR2430 type button cell; The DOL-DME solution that the electrolyte used is 1mol/LLiTFSI, the volume ratio of DOL and DME is 1:1, and adds 0.4MLiNO3.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510923554.3A CN105374982A (en) | 2015-12-11 | 2015-12-11 | Electrode structure of lithium sulfur battery and processing technology therefor |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201510923554.3A CN105374982A (en) | 2015-12-11 | 2015-12-11 | Electrode structure of lithium sulfur battery and processing technology therefor |
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| CN105374982A true CN105374982A (en) | 2016-03-02 |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106058150A (en) * | 2016-08-15 | 2016-10-26 | 柔电（武汉）科技有限公司 | Electrode of lithium sulfur battery and preparation method thereof |
| CN107579200A (en) * | 2016-07-04 | 2018-01-12 | 杭州聚力氢能科技有限公司 | A kind of full encapsulation sulfur electrode |
| CN108630890A (en) * | 2018-04-28 | 2018-10-09 | 四川华昆能源有限责任公司 | A kind of multi-layer electrode structure and preparation method thereof for lithium-sulfur cell |
| CN113383445A (en) * | 2019-08-12 | 2021-09-10 | 株式会社Lg化学 | Positive electrode for lithium secondary battery and lithium secondary battery comprising same |
| CN114079038A (en) * | 2020-08-12 | 2022-02-22 | 清华大学 | A high-sulfur-loaded lithium-sulfur battery positive electrode and preparation method thereof |
| CN115315831A (en) * | 2020-03-13 | 2022-11-08 | 株式会社Lg新能源 | Negative electrode active material, method for producing the same, and lithium secondary battery including the same |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107579200A (en) * | 2016-07-04 | 2018-01-12 | 杭州聚力氢能科技有限公司 | A kind of full encapsulation sulfur electrode |
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| CN108630890A (en) * | 2018-04-28 | 2018-10-09 | 四川华昆能源有限责任公司 | A kind of multi-layer electrode structure and preparation method thereof for lithium-sulfur cell |
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| CN115315831A (en) * | 2020-03-13 | 2022-11-08 | 株式会社Lg新能源 | Negative electrode active material, method for producing the same, and lithium secondary battery including the same |
| CN114079038A (en) * | 2020-08-12 | 2022-02-22 | 清华大学 | A high-sulfur-loaded lithium-sulfur battery positive electrode and preparation method thereof |
| CN114079038B (en) * | 2020-08-12 | 2023-09-26 | 清华大学 | High-sulfur-load lithium-sulfur battery positive electrode and preparation method thereof |
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