CN109728256A - Composite negative electrode, preparation method thereof and flexible package battery - Google Patents
Composite negative electrode, preparation method thereof and flexible package battery Download PDFInfo
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- CN109728256A CN109728256A CN201811591616.5A CN201811591616A CN109728256A CN 109728256 A CN109728256 A CN 109728256A CN 201811591616 A CN201811591616 A CN 201811591616A CN 109728256 A CN109728256 A CN 109728256A
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- lithium
- lithium metal
- negative pole
- composite negative
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- 239000002131 composite material Substances 0.000 title claims abstract description 41
- 238000002360 preparation method Methods 0.000 title claims abstract description 25
- 229910052744 lithium Inorganic materials 0.000 claims description 100
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 41
- 229910045601 alloy Inorganic materials 0.000 claims description 21
- 239000000956 alloy Substances 0.000 claims description 21
- 238000000034 method Methods 0.000 claims description 12
- 238000003475 lamination Methods 0.000 claims description 10
- 239000007773 negative electrode material Substances 0.000 claims description 9
- 238000005507 spraying Methods 0.000 claims description 9
- 229910052782 aluminium Inorganic materials 0.000 claims description 7
- 239000011244 liquid electrolyte Substances 0.000 claims description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 6
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 6
- 239000007767 bonding agent Substances 0.000 claims description 6
- 239000006258 conductive agent Substances 0.000 claims description 6
- 239000003792 electrolyte Substances 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 6
- 238000003825 pressing Methods 0.000 claims description 6
- 150000001875 compounds Chemical class 0.000 claims description 5
- 238000001755 magnetron sputter deposition Methods 0.000 claims description 5
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 4
- 239000005864 Sulphur Substances 0.000 claims description 4
- 239000004411 aluminium Substances 0.000 claims description 4
- 229910044991 metal oxide Inorganic materials 0.000 claims description 4
- 150000004706 metal oxides Chemical class 0.000 claims description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
- 239000003575 carbonaceous material Substances 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 239000010949 copper Substances 0.000 claims description 3
- 239000011245 gel electrolyte Substances 0.000 claims description 3
- 238000007731 hot pressing Methods 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 229910052755 nonmetal Inorganic materials 0.000 claims description 3
- 239000002210 silicon-based material Substances 0.000 claims description 3
- 239000002153 silicon-carbon composite material Substances 0.000 claims description 3
- 239000007784 solid electrolyte Substances 0.000 claims description 3
- 239000010935 stainless steel Substances 0.000 claims description 3
- 229910001220 stainless steel Inorganic materials 0.000 claims description 3
- 239000002985 plastic film Substances 0.000 claims description 2
- 229920006255 plastic film Polymers 0.000 claims description 2
- 239000012530 fluid Substances 0.000 claims 1
- 239000000126 substance Substances 0.000 abstract description 2
- 238000011031 large-scale manufacturing process Methods 0.000 abstract 1
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 description 9
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 4
- 229910000733 Li alloy Inorganic materials 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 238000005275 alloying Methods 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 238000011065 in-situ storage Methods 0.000 description 2
- 239000001989 lithium alloy Substances 0.000 description 2
- 238000006479 redox reaction Methods 0.000 description 2
- 206010054949 Metaplasia Diseases 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 238000001465 metallisation Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 230000015689 metaplastic ossification Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 150000003376 silicon Chemical class 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 230000002269 spontaneous effect Effects 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 239000011135 tin Substances 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
Landscapes
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
The invention discloses a composite cathode, a preparation method thereof and a flexible package battery, belonging to the field of chemical power sources. In the invention, the application of the composite cathode enables the battery to obtain high energy density and better cycle performance. The composite cathode is simple and easy to prepare, and can realize large-scale production.
Description
Technical field
The invention belongs to field of chemical power source, in particular to a kind of composite negative pole and preparation method thereof and flexible-packed battery.
Background technique
Currently, the common negative electrode material of lithium ion battery is graphite-like, as people are more next to power-supply system energy density
Higher demand, alloy type (silicon, tin, aluminium), oxide-based (silica, tin oxide, titanium oxide) material is because having higher reason
It is more concerned by specific capacity.Silicon class cathode has the specific capacity of 4200mAh/g, is the highest cathode of current specific capacity, and its
The lithium metal deposition not easily generated in charging, is to carry out alloying with lithium to have both safety and the optimal selection of height ratio capacity.Gold
One of redox reaction and promising cathode can also be occurred by belonging to oxide and lithium.
In the battery, the specific capacity of positive electrode controls the energy of integral battery, at present the positive electrode of lithium ion battery
Nearly 300Wh/kg is had reached, and the higher sulphur of specific capacity either oxide is used cathode certainly will to be needed to provide as anode
Lithium ion.Lithium metal is directly as cathode, while providing height ratio capacity, but there is volume expansion and generates asking for dendrite
Topic, it is for the safety of battery and unfriendly, and cycle-index is less, is unable to satisfy power-supply system and powers for a long time.
Therefore, it is necessary to carry out a kind of novel cathode of lithium design, while ensureing battery performance, with good security performance.
Summary of the invention
The technical problem to be solved by the invention is to provide a kind of composite negative pole and preparation method thereof and flexible-packed battery,
In the case where positive electrode is containing lithium or is free of lithium, alloy type, oxide-based cathode and lithium metal are used in combination, it is multiple
The spontaneous carry out redox reaction of cathode energy, in-situ preparation lithium alloy are closed, while having both high-energy density and high security, is improved
Conventional metals cathode of lithium cycle life in cyclic process shorter problem.Meanwhile this method is simple and easy to do, is suitable for scale
Metaplasia produces.
In order to solve the above-mentioned technical problem, the technical solution adopted by the present invention is that: a kind of preparation method of composite negative pole is adopted
With lithium metal or lithium metal alloy, carried out with the negative electrode material without lithium metal it is compound, lithium metal or lithium metal alloy with
Without in cathode of lithium combination, the area ratio of the two is 0.05:1-1:1.1.
The lithium metal or lithium metal alloy that composite negative pole uses, with a thickness of 10 μm -200 μm, area 2cm2-300cm2。
The negative electrode material without lithium metal that composite negative pole uses is silicon materials, Si-C composite material, Carbon materials, metal
One or both of oxide.
Collector used in cathode without lithium metal is copper or nickel.
Using rubbing method, spray coating method, magnetron sputtering mode, by negative electrode material and conductive agent, bonding agent without lithium metal
It is formed by mixture preparation on a current collector.
Lithium metal or lithium metal alloy and the cathode combination without lithium are mechanical hot pressing, mechanical cold pressing, spraying；Gold
Belong to lithium perhaps lithium metal alloy with when being stacked without the cathode of lithium with the lithium metal of different area or lithium metal alloy front and back sides
The symmetrical or asymmetric mode put, fits in without lithium cathode sheet surface.
Positive electrode containing lithium or without lithium is sulphur, metal oxide, nonmetal oxide, oxidate for lithium.
Composite negative pole made from above-mentioned preparation method.
Flexible-packed battery containing above-mentioned composite negative pole, composite negative pole are combined with the anode containing lithium or without lithium, are used
The mode of lamination assembles large capacity flexible-packed battery.
Flexible-packed battery includes anode, cathode, diaphragm, electrolyte, tab, aluminum plastic film, is assembled using lamination process,
Laminated combination is carried out in the way of anode, diaphragm, cathode, is assembled into large capacity flexible-packed battery；The collector that anode uses
For aluminium, stainless steel, anode is using rubbing method, spray coating method, magnetron sputtering mode is used, by positive electrode and conductive agent, bonding agent
It is formed by mixture preparation on a current collector, electrolyte used in flexible-packed battery is liquid electrolyte, gel electrolyte
Or solid electrolyte.
The beneficial effects of the present invention are: cathode design uses lithium metal or lithium metal alloy, with high-capacity cathode material
Prepared electrode slice carries out compound, and composite negative pole can be carried out home position alloying reaction, then with containing lithium or without lithium ion
High capacity anode is assembled into battery, makes battery while with high-energy density, has preferable security performance, compares proof gold
Belong to the battery of cathode of lithium preparation, there is better cycle performance.Meanwhile program simple possible, strong operability, it is easy to accomplish batch
Amount production.
Detailed description of the invention
Fig. 1 is composite negative pole of the present invention and pure metal lithium negative battery cycle performance comparison diagram.
Specific embodiment
In order to further understand the content, features and effects of the present invention, the following examples are hereby given, and cooperate attached
Figure, in the present invention, if not refering in particular to, all parts, percentage are unit of weight, and all devices and raw material etc. can be from markets
It buys or the industry is common.
The preparation method of composite negative pole of the invention, using lithium metal or lithium metal alloy, with bearing without lithium metal
Material progress in pole is compound, and with without in cathode of lithium combination, the area ratio of the two is 0.05 for lithium metal or lithium metal alloy:
1-1:1.1。
The lithium metal or lithium metal alloy that composite negative pole uses, with a thickness of 10 μm -200 μm, area 2cm2-300cm2。
The negative electrode material without lithium metal that composite negative pole uses is silicon materials, Si-C composite material, Carbon materials, metal
One or both of oxide.
Collector used in cathode without lithium metal is copper or nickel.
Using rubbing method, spray coating method, magnetron sputtering mode, by negative electrode material and conductive agent, bonding agent without lithium metal
It is formed by mixture preparation on a current collector.
Lithium metal or lithium metal alloy and the cathode combination without lithium are mechanical hot pressing, mechanical cold pressing, spraying；Gold
Belong to lithium perhaps lithium metal alloy with when being stacked without the cathode of lithium with the lithium metal of different area or lithium metal alloy front and back sides
The symmetrical or asymmetric mode put, fits in without lithium cathode sheet surface.
Positive electrode containing lithium or without lithium is sulphur, metal oxide, nonmetal oxide, oxidate for lithium.
Composite negative pole made from above-mentioned preparation method.
Flexible-packed battery containing above-mentioned composite negative pole, composite negative pole are combined with the anode containing lithium or without lithium, are used
The mode of lamination assembles large capacity flexible-packed battery.Flexible-packed battery includes anode, cathode, diaphragm, electrolyte, tab, plastic-aluminum
Film is assembled using lamination process, and laminated combination is carried out in the way of anode, diaphragm, cathode, is assembled into large capacity Soft Roll
Packed battery；For the collector that anode uses for aluminium, stainless steel, anode, will using rubbing method, spray coating method, magnetron sputtering mode is used
Positive electrode and conductive agent, bonding agent are formed by mixture preparation on a current collector, electrolyte used in flexible-packed battery
For liquid electrolyte, gel electrolyte or solid electrolyte.
Detailed description are as follows:
Embodiment 1
Take 90 μ m-thicks, area 150cm2Lithium metal, with silicon-carbon cathode of the same area carry out it is compound, silicon-carbon cathode is
Double spread electrode slice, two-sided surface density are 25mg/cm2.Lithium metal is pasted onto the surface of the positive and negative two sides of silicon-carbon cathode piece, is made
It is suppressed with hydraulic press, pressing pressure 4Mpa is pressed into integrated composite negative pole.Positive plate is NCM electrode, pole piece surface density
For 35mg/cm2, composite negative pole, 2400 diaphragm of Celgard, anode are subjected to lamination assembling, assemble 3Ah flexible-packed battery, note
Enter liquid electrolyte, is recycled with 0.2C.
Embodiment 2
90 μ m-thicks are taken, lithium metal item totally 10 of 6mm wide, 10cm long, be 150cm with area2Silicon-carbon cathode answered
It closes, silicon-carbon cathode is double spread electrode slice, and two-sided surface density is 25mg/cm2, lithium metal item is uniformly fitted in silicon-carbon cathode two
Side, the state that the lithium item of electrode front and back sides is symmetric, is suppressed using hydraulic press, pressing pressure 4Mpa, and compacting is integral
The composite negative pole of change.Positive plate is NCM electrode, and pole piece surface density is 35mg/cm2, by composite negative pole, Celgard 2400 every
Film, anode carry out lamination assembling, assemble 3Ah flexible-packed battery, inject liquid electrolyte, are recycled with 0.2C.
Embodiment 3
90 μ m-thicks are taken, lithium metal item totally 10 of 8mm wide, 10cm long, be 150cm with area2Silicon-carbon cathode answered
It closes, silicon-carbon cathode is double spread electrode slice, and two-sided surface density is 25mg/cm2, lithium metal item is uniformly fitted in silicon-carbon cathode two
Side, the state that the lithium item of electrode front and back sides is symmetric, is suppressed using hydraulic press, pressing pressure 4Mpa, and compacting is integral
The composite negative pole of change.Positive plate is NCM electrode, and pole piece surface density is 35mg/cm2, by composite negative pole, Celgard 2400 every
Film, anode carry out lamination assembling, assemble 3Ah flexible-packed battery, inject liquid electrolyte, are recycled with 0.2C.
Comparative example 1
Take 90 μ m-thicks, area 150cm2Lithium metal.Positive plate is NCM electrode, and pole piece surface density is 35mg/cm2, will
Composite negative pole, 2400 diaphragm of Celgard, anode carry out lamination assembling, assemble 3Ah flexible-packed battery, inject liquid electrolyte,
It is recycled with 0.2C.
Battery number is 1# in embodiment 1, and battery number is 2# in embodiment 2, and battery number is 3# in embodiment 3, than
It is 4# compared with battery number in example 1.4 batteries are after circulation, by attached drawing 1 as it can be seen that 4# circulating battery recycles 26 energy holdings
Rate, which declines, is down to 52%；It declines for 2# circulating battery 39 times and to be down to 76%；It declines for 3# circulating battery 50 times and to be down to 77%, 1# circulating battery 100
Secondary decline is down to 86%.It can be seen that the additive amount of lithium metal and the cycle performance of battery are in close relations, metal in composite negative pole
The content of lithium is higher, and generated in-situ lithium alloy degree of participation in electrochemical reaction is higher, and the cycle performance of battery is better.
Above embodiment be only preferred embodiments of the present invention will be described, not to the scope of the present invention into
Row limits, under the inspiration of those skilled in the art's content according to described in Summary and embodiment, to the present invention
Technical solution carry out various changes and improvements, shall fall in protection scope determined by claims of the present invention.
Claims (10)
1. a kind of preparation method of composite negative pole, which is characterized in that use lithium metal or lithium metal alloy, be free of lithium metal
Negative electrode material carry out compound, with without in cathode of lithium combination, the area ratio of the two is for lithium metal or lithium metal alloy
0.05:1-1:1.1。
2. the preparation method of composite negative pole according to claim 1, which is characterized in that lithium metal that composite negative pole uses or
Lithium metal alloy, with a thickness of 10 μm -200 μm, area 2cm2-300cm2。
3. the preparation method of composite negative pole according to claim 1, which is characterized in that composite negative pole used is free of lithium metal
Negative electrode material be one or both of silicon materials, Si-C composite material, Carbon materials, metal oxide.
4. the preparation method of composite negative pole according to claim 3, which is characterized in that collection used in the cathode without lithium metal
Fluid is copper or nickel.
5. the preparation method of composite negative pole according to claim 4, which is characterized in that splashed using rubbing method, spray coating method, magnetic control
Mode is penetrated, the negative electrode material without lithium metal is formed by mixture preparation on a current collector with conductive agent, bonding agent.
6. the preparation method of composite negative pole according to claim 4, which is characterized in that lithium metal or lithium metal alloy with not
Cathode combination containing lithium is mechanical hot pressing, mechanical cold pressing, spraying；Lithium metal or lithium metal alloy and the cathode for being free of lithium
When stacking, in such a way that the lithium metal of different area or lithium metal alloy front and back sides are symmetrical or asymmetry is put, fit in
Without lithium cathode sheet surface.
7. the preparation method of composite negative pole according to claim 1, which is characterized in that containing lithium or without the positive electrode of lithium
For sulphur, metal oxide, nonmetal oxide, oxidate for lithium.
8. containing composite negative pole made from any one of the claim 1-7 preparation method.
9. the flexible-packed battery containing composite negative pole described in claim 8, which is characterized in that composite negative pole with containing lithium or being free of
The anode combination of lithium assembles large capacity flexible-packed battery by the way of lamination.
10. flexible-packed battery according to claim 1, which is characterized in that flexible-packed battery include anode, cathode, diaphragm,
Electrolyte, tab, aluminum plastic film, are assembled using lamination process, and laminated combination is carried out in the way of anode, diaphragm, cathode,
It is assembled into large capacity flexible-packed battery；The collector that uses of anode for aluminium, stainless steel, anode use use rubbing method, spray coating method,
Positive electrode and conductive agent, bonding agent are formed by mixture preparation on a current collector, flexible-packed battery by magnetron sputtering mode
Used in electrolyte be liquid electrolyte, gel electrolyte or solid electrolyte.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201811591616.5A CN109728256A (en) | 2018-12-25 | 2018-12-25 | Composite negative electrode, preparation method thereof and flexible package battery |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201811591616.5A CN109728256A (en) | 2018-12-25 | 2018-12-25 | Composite negative electrode, preparation method thereof and flexible package battery |
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| Publication Number | Publication Date |
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| CN109728256A true CN109728256A (en) | 2019-05-07 |
Family
ID=66297208
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108448115A (en) * | 2018-03-15 | 2018-08-24 | 清华大学 | A kind of asymmetric skeleton structure of lithium metal battery cathode |
| CN112820846A (en) * | 2019-11-15 | 2021-05-18 | 淮阴师范学院 | Manufacturing method of molybdenum lithium ion full battery |
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| CN106558692A (en) * | 2015-09-30 | 2017-04-05 | 中国科学院大连化学物理研究所 | A kind of lithium battery negative pole and its preparation and application |
| CN108183197A (en) * | 2017-12-19 | 2018-06-19 | 国联汽车动力电池研究院有限责任公司 | A kind of composite metal lithium negative pole structure and preparation method thereof |
| CN108550780A (en) * | 2018-03-22 | 2018-09-18 | 天津市捷威动力工业有限公司 | A kind of negative electrode of lithium ion battery single side prelithiation method using three-dimensional foil |
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Patent Citations (5)
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| US20150333385A1 (en) * | 2011-02-11 | 2015-11-19 | Industry-University Cooperation Foundation Hanyang University | Method for manufacturing a lithiated metal-carbon composite electrode, lithiated metal-carbon composite electrode manufactured thereby, and electrochemical device including the electrode |
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