CN106654289A - Porous aluminum-foil cathode, preparation method of porous aluminum-foil cathode and lithium secondary battery - Google Patents
Porous aluminum-foil cathode, preparation method of porous aluminum-foil cathode and lithium secondary battery Download PDFInfo
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- CN106654289A CN106654289A CN201611250050.0A CN201611250050A CN106654289A CN 106654289 A CN106654289 A CN 106654289A CN 201611250050 A CN201611250050 A CN 201611250050A CN 106654289 A CN106654289 A CN 106654289A
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- aluminium foil
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- hole
- porous aluminium
- negative pole
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 24
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 23
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000011888 foil Substances 0.000 title abstract 11
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 12
- 239000003792 electrolyte Substances 0.000 claims abstract description 12
- 239000005030 aluminium foil Substances 0.000 claims description 149
- 239000000463 material Substances 0.000 claims description 27
- 239000003575 carbonaceous material Substances 0.000 claims description 23
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 17
- 229910002804 graphite Inorganic materials 0.000 claims description 14
- 239000010439 graphite Substances 0.000 claims description 14
- 239000005416 organic matter Substances 0.000 claims description 12
- 239000011148 porous material Substances 0.000 claims description 11
- 230000004888 barrier function Effects 0.000 claims description 10
- 239000011258 core-shell material Substances 0.000 claims description 10
- 239000007789 gas Substances 0.000 claims description 8
- 238000010000 carbonizing Methods 0.000 claims description 7
- 238000005245 sintering Methods 0.000 claims description 7
- 239000003610 charcoal Substances 0.000 claims description 6
- 239000011261 inert gas Substances 0.000 claims description 6
- 238000000465 moulding Methods 0.000 claims description 6
- 230000008859 change Effects 0.000 claims description 5
- 239000002243 precursor Substances 0.000 claims description 5
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 238000005530 etching Methods 0.000 claims description 4
- 229910021389 graphene Inorganic materials 0.000 claims description 4
- 230000009467 reduction Effects 0.000 claims description 4
- 238000001020 plasma etching Methods 0.000 claims description 3
- 238000003486 chemical etching Methods 0.000 claims description 2
- 238000003698 laser cutting Methods 0.000 claims description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 abstract description 13
- 229910001416 lithium ion Inorganic materials 0.000 abstract description 13
- 238000000034 method Methods 0.000 abstract description 10
- 230000008569 process Effects 0.000 abstract description 10
- 239000007784 solid electrolyte Substances 0.000 abstract description 4
- 239000012528 membrane Substances 0.000 abstract description 3
- 239000006182 cathode active material Substances 0.000 abstract 1
- 230000001351 cycling effect Effects 0.000 abstract 1
- 230000000694 effects Effects 0.000 abstract 1
- 238000005516 engineering process Methods 0.000 description 11
- 238000012545 processing Methods 0.000 description 11
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 10
- 238000013461 design Methods 0.000 description 10
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 9
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 8
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 8
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 8
- 239000011149 active material Substances 0.000 description 7
- 239000000243 solution Substances 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- 239000004743 Polypropylene Substances 0.000 description 6
- 210000004027 cell Anatomy 0.000 description 6
- -1 polypropylene Polymers 0.000 description 6
- 229920001155 polypropylene Polymers 0.000 description 6
- WHNWPMSKXPGLAX-UHFFFAOYSA-N N-Vinyl-2-pyrrolidone Chemical compound C=CN1CCCC1=O WHNWPMSKXPGLAX-UHFFFAOYSA-N 0.000 description 5
- 229910052786 argon Inorganic materials 0.000 description 5
- 229940069328 povidone Drugs 0.000 description 5
- 229910001290 LiPF6 Inorganic materials 0.000 description 4
- 239000002033 PVDF binder Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 239000011259 mixed solution Substances 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- 238000004886 process control Methods 0.000 description 4
- 238000010926 purge Methods 0.000 description 4
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 3
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Chemical compound OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 description 3
- 239000004372 Polyvinyl alcohol Substances 0.000 description 3
- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 description 3
- 229930006000 Sucrose Natural products 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 3
- 239000001989 lithium alloy Substances 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 229920001568 phenolic resin Polymers 0.000 description 3
- 239000005011 phenolic resin Substances 0.000 description 3
- 229920002451 polyvinyl alcohol Polymers 0.000 description 3
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 3
- 230000001737 promoting effect Effects 0.000 description 3
- 239000005720 sucrose Substances 0.000 description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 2
- 229910001148 Al-Li alloy Inorganic materials 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 240000007594 Oryza sativa Species 0.000 description 2
- 235000007164 Oryza sativa Nutrition 0.000 description 2
- FCVHBUFELUXTLR-UHFFFAOYSA-N [Li].[AlH3] Chemical compound [Li].[AlH3] FCVHBUFELUXTLR-UHFFFAOYSA-N 0.000 description 2
- 150000001398 aluminium Chemical class 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- 238000003763 carbonization Methods 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 125000004122 cyclic group Chemical group 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- VIKNJXKGJWUCNN-XGXHKTLJSA-N norethisterone Chemical compound O=C1CC[C@@H]2[C@H]3CC[C@](C)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 VIKNJXKGJWUCNN-XGXHKTLJSA-N 0.000 description 2
- 239000007774 positive electrode material Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 235000009566 rice Nutrition 0.000 description 2
- 238000013112 stability test Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 229910000838 Al alloy Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910000733 Li alloy Inorganic materials 0.000 description 1
- 229910010199 LiAl Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- JFBZPFYRPYOZCQ-UHFFFAOYSA-N [Li].[Al] Chemical compound [Li].[Al] JFBZPFYRPYOZCQ-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 238000005255 carburizing Methods 0.000 description 1
- 230000010261 cell growth Effects 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000003754 machining Methods 0.000 description 1
- 238000001465 metallisation Methods 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 241000894007 species Species 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
- H01M4/64—Carriers or collectors
- H01M4/70—Carriers or collectors characterised by shape or form
- H01M4/80—Porous plates, e.g. sintered carriers
- H01M4/801—Sintered carriers
-
- 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- 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
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
-
- 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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
-
- 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
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Cell Electrode Carriers And Collectors (AREA)
Abstract
The invention provides a porous aluminum-foil cathode. The porous aluminum-foil cathode comprises a porous aluminum foil; porous holes which are uniformly arranged are formed in the porous aluminum foil; triangular areas formed by connecting the centers of every three adjacent holes are taken as minimum units; the area ratio of the holes in each minimum unit is 10-79%; and the distance between the porous aluminum foil and the outermost porous hole is 0.1-10mm. The porous aluminum-foil cathode can be applied in a novel lithium-ion battery system which takes the aluminum foil as a current collector and a cathode active material at the same time, and has the effects of effectively solving the battery expansion problem, effectively reducing the problem that the solid electrolyte membranes are damaged to decompose in the battery charge-discharge cycle process of electrolyte, and effectively reducing the short-circuit problem caused by puncturing the membranes by burs of the aluminum foil, so as to improve the charge-discharge efficiency, cycling stability and safety of the batteries. The invention furthermore provides a preparation method of the porous aluminum-foil cathode and a lithium secondary battery.
Description
Technical field
The present invention relates to lithium secondary battery technical field, more particularly to a kind of porous aluminium foil negative pole and preparation method thereof and
Lithium secondary battery.
Background technology
2016, Shenzhen Institutes of Advanced Technology, Chinese Academy of Science's making a breakthrough property in terms of new and effective battery research was entered
Exhibition, develops a kind of brand-new aluminium-graphite Dual-ion cell technology, and the achievement in research is issued《Advanced Energy
Materials》Upper (DOI:10.1002/aenm.201502588), the new and effective battery system is by the use of aluminium foil as negative pole
Piece, aluminium foil functions simultaneously as collector and negative active core-shell material, and due to reducing traditional negative active core-shell material, specific energy density is more
High, cost is lower, and with great application prospect, but the battery system has in the course of the work aluminium foil volumetric expansion and electrolysis
The problem of liquid compatibility, so as to affect efficiency for charge-discharge, cycle performance and security performance.
The content of the invention
In consideration of it, first aspect present invention provide a kind of porous aluminium foil negative pole, the porous aluminium foil negative pole can be applicable to
In aluminium foil novel battery system simultaneously as collector and negative active core-shell material, its can with effectively solving cell expansion problem,
And the problem that can effectively reduce electrolyte solid electrolyte film in battery charging and discharging cyclic process destroyed and decompose, and
Solve because aluminium foil burr punctures short circuit problem caused by barrier film, so improve the efficiency for charge-discharge of battery, cycle performance and
Security performance.
Specifically, in a first aspect, the invention provides a kind of porous aluminium foil negative pole, including porous aluminium foil, the porous aluminum
Paper tinsel is provided with the porous hole of uniform arrangement, single as minimum with the delta-shaped region that the line of centres of adjacent three holes is constituted
Unit, the area accounting of each minimum unit Hole is 10%-79%, edge and the outermost of the porous aluminium foil
The distance between porous hole is 0.1mm-10mm.In heretofore described porous aluminium foil negative pole, the porous aluminium foil fills simultaneously
When collector and negative active core-shell material.
It is well known that at present positive electrode plate and negative electrode plate of lithium ion battery active material stores up lithium ability according to certain ratio according to material
Example, is uniformly coated on both positive and negative polarity collector by coating method.When the coating of both positive and negative polarity active material is inhomogenous, negative pole
Easily there is lithium metal deposition in surface, is very that Li dendrite is produced, and deteriorates the capacity and cycle performance of battery, and battery can be present
Security hidden trouble.It can be seen that battery pole piece active material coating uniformity and uniformity are the passes of battery electrical property and security performance
Key factor, therefore in lithium battery manufacture process, need the uniformity of strict control positive/negative plate active material coating.Equally exist
Using porous aluminium foil while as in the new type lithium ion battery system of collector and negative active core-shell material, it is also desirable to which strict control is more
The homogeneity of hole aluminium foil, so the size in the aperture of porous aluminium foil and the uniformity of pore size distribution are to determine that can it live as negative pole
The rigid index of property material and collector.In the present invention, it is with the delta-shaped region that the line of centres of adjacent three holes is constituted
Minimum unit, in each described minimum unit, the area accounting of hole is 10%-79%；Still optionally further, the face of hole
Product accounting is 25%-60%.In the present invention, it is preferable that the hole area accounting of each minimum unit is equal.
The hole area accounting of minimum unit determines the embedding lithium volumetric expansion size that porous aluminium foil negative pole can bear, therefore
The area accounting of collector and active material can be each acted as according to porous aluminium foil negative pole in pre-designed battery and be set.Specifically
Ground, when forming aluminium lithium alloy due to Lithium-ion embeding aluminium foil, its volumetric expansion is up to 97%, therefore the present invention is when pressing aluminium lithium alloy
Monoploid product rate of change carries out headspace design.In even pre-designed battery, porous aluminium foil negative pole serves as in minimum unit
The area accounting of active material is 20%, and the area accounting for serving as collector is 20%-60%, then the hole face in minimum unit
Product accounting is preferably set to 20%, or more than 20%, such as 20%-60% is closed so as to form aluminium for Lithium-ion embeding aluminium foil
The Volume Changes that gold ribbon comes provide headspace.
The big size porous aluminium foil for obtaining is machined at present, and when pole piece is cut into, aluminium foil edge can be because hole be broken
Badly, there is substantial amounts of burr in workprint.When battery is assembled into, aluminium foil burr can puncture barrier film and form short circuit, affect cell performance
Energy.The present invention can be prevented effectively from workprint and hair by the way that the reserved certain distance in the edge of porous aluminium foil negative pole is not provided with into hole
The generation of thorn, improves stability test and security.In the present invention, still optionally further, the edge of the porous aluminium foil with most
The distance between peripheral porous hole is 2mm-5mm.
In the present invention, on the porous aluminium foil, with the line of centres of adjacent two horizontally-arranged adjacent three holes constituted etc.
Lumbar triangle shape region is minimum unit, and the hole area accounting of each minimum unit is equal.Still optionally further, laterally arbitrarily
The spacing of adjacent two circular cavities is equal, and the spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
Alternatively, the spacing phase of the spacing of the two circular cavities of horizontal arbitrary neighborhood and the two circular cavities of longitudinal arbitrary neighborhood
Deng.Alternatively, the spacing of the two circular cavities of the horizontal arbitrary neighborhood spacing horizontally-arranged with adjacent two is equal.
Alternatively, the porous aperture of the porous aluminium foil is 20nm-2mm.Further, porous aperture be 50 μm-
1.5mm.It is further preferred that the pore size of porous hole is equal.
In the present invention, the shape of the porous hole of the porous aluminium foil can be circle, ellipse, square, rectangle,
Prismatic, triangle, polygon, five-pointed star, quincunx etc., shape is not restricted.The length of side of hole is bigger, is more conducive to lithium ion
It is embedded.
In the present invention, the surface of the porous aluminium foil is further provided with carbon material layer, wherein, the material of the carbon material layer
Matter includes one or more material in conductive black, Graphene, graphite flake, CNT and organic matter carbonizing thing, described to have
Machine thing carbide includes carbide of the carbonization temperature for 200-700 DEG C of organic matter.Specifically, the organic matter carbonizing thing is Portugal
Grape sugar charcoal compound, char sucrose thing, citric acid carbide, polyvinylpyrrolidone carbide, polyvinyl alcohol carbide, polypropylene
One or more material such as alcohol carbide, phenolic resin carbide.
Alternatively, the thickness of the carbon material layer is 2nm-5 μm.Further, the thickness of the carbon material layer is
200nm-3μm。
The porous aluminium foil negative pole that first aspect present invention is provided, its porous hole can form aluminium for Lithium-ion embeding aluminium foil
The Volume Changes that lithium alloy brings provide enough headspaces, so that negative pole pole will not expand problem, solve electricity
Pond expansion issues；The reserved certain distance in the edge of porous aluminium foil negative pole is not provided with into hole, workprint and burr can be prevented effectively from
Generation, improve stability test and security；And by arranging carbon material layer in porous aluminium foil surface, battery can be caused to fill
Electrolyte forms stable solid electrolyte film in porous aluminium foil negative terminal surface during electric discharge, effectively reduces electrolyte in battery charge and discharge
The problem that solid electrolyte film is destroyed and decomposes in electric cyclic process, and then improve efficiency for charge-discharge, the cycle performance of battery
And security performance.
Second aspect, the invention provides a kind of preparation method of porous aluminium foil negative pole, comprises the following steps：
Using one or more side in mechanical molding, chemical etching, laser cutting, plasma etching and electrochemical etching
Formula processing obtains porous aluminium foil, that is, obtain porous aluminum paper tinsel negative pole；The porous aluminium foil is provided with porous hole, with adjacent three holes
The delta-shaped region that the line of centres in hole is constituted is minimum unit, and the area accounting of each minimum unit Hole is
The distance between 10%-79%, edge and outermost porous hole of the porous aluminium foil are 0.1mm-10mm.
Specifically, the preparation of porous aluminium foil can first according to the model or battery capacity design requirement of battery, with reference to positive pole material
The factor design positive plate surface densities such as material species, specific capacity, compacted density, subsequently form lithium-aluminium alloy according to lithium ion and aluminium foil
LiAl materials, specific capacity is 993mAh/g, designs porosity, the size (length, width, thickness) of battery cathode sheet；Further according to
The porosity of negative plate, the pore size of size design porous aluminium foil, hole shape and pore size distribution；Finally using machinery molding, change
The mode of any one or more the common processing such as etching, plasma etching, electrochemical etching is learned, with reference to above-mentioned design
Porous aluminium foil is fabricated out, and purging is carried out using compressed air and remove flash removed.
In the present invention, on the porous aluminium foil, with the line of centres of adjacent two horizontally-arranged adjacent three holes constituted etc.
Lumbar triangle shape region is minimum unit, and the hole area accounting of each minimum unit is equal.Still optionally further, laterally arbitrarily
The spacing of adjacent two circular cavities is equal, and the spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
Alternatively, the spacing phase of the spacing of the two circular cavities of horizontal arbitrary neighborhood and the two circular cavities of longitudinal arbitrary neighborhood
Deng.Alternatively, the spacing of the two circular cavities of the horizontal arbitrary neighborhood spacing horizontally-arranged with adjacent two is equal.
Alternatively, the porous aperture of the porous aluminium foil is 20nm-2mm.Further, porous aperture be 50 μm-
1.5mm.It is further preferred that the pore size of porous hole is equal.
In the present invention, the shape of the porous hole of the porous aluminium foil can be circle, ellipse, square, rectangle,
Prismatic, triangle, polygon, five-pointed star, quincunx etc., shape is not limited.
Still optionally further, in each described minimum unit, the area accounting of hole is 25%-60%.
Still optionally further, the distance between the edge of the porous aluminium foil and outermost porous hole are 2mm-5mm.This
Sample when the big size porous aluminium foil that obtains of machining is cut into into pole piece, aluminium foil edge would not because hole is destroyed hair
Piece, so as to avoid the occurrence of substantial amounts of burr.
Alternatively, the thickness of porous aluminium foil is 10-100 microns.
Wherein, alternatively, carbon material layer is further prepared on the porous aluminium foil, is concretely comprised the following steps：
Solution containing material with carbon element is coated to into the surface of the porous aluminium foil, is dried, obtain porous aluminium foil negative pole；
Or the solution containing carbon materials material precursor is coated to into the surface of the porous aluminium foil, be subsequently placed in inert gas or
0.5-6 hours are heat-treated in the sintering furnace of reducibility gas, make the carbon materials material precursor be carbonized, that is, obtained porous aluminum paper tinsel and bear
Pole, the porous aluminium foil negative pole includes porous aluminium foil and is arranged at the carbon material layer of the porous aluminium foil surface.
The material with carbon element includes leading the one kind or many in carbon black, Graphene, graphite flake, CNT and organic matter carbonizing thing
Material is planted, the carbon materials material precursor includes the organic matter that carburizing temperature is 200-700 DEG C.Specifically, the organic matter is Portugal
One or more material such as grape sugar, sucrose, citric acid, polyvinylpyrrolidone, polyvinyl alcohol, POLYPROPYLENE GLYCOL, phenolic resin.Institute
The temperature for stating heat treatment is 200-700 DEG C.The time of the heat treatment is 2-4 hours.
Alternatively, the thickness of the carbon material layer is 2nm-5 μm.Further, the thickness of the carbon material layer is
200nm-3μm。
The inert gas is argon gas, nitrogen etc..The reducibility gas can be hydrogen.The operation of the drying is：In
80 DEG C of -100 DEG C of drying 2-6 hours.
The preparation method of the porous aluminium foil negative pole that second aspect present invention is provided, process is simple, low cost, it is easy to industrialize
Production.
The third aspect, the invention provides a kind of lithium secondary battery, including positive plate, electrolyte, barrier film, negative plate, institute
Negative plate is stated for the porous aluminium foil negative pole described in first aspect present invention.The porous aluminium foil negative pole includes porous aluminium foil, described
Porous aluminium foil is provided with the porous hole of uniform arrangement, and the delta-shaped region constituted with the line of centres of adjacent three holes is as most
Junior unit, the area accounting of each minimum unit Hole is 10%-79%, the edge and outermost of the porous aluminium foil
The distance between porous hole for enclosing is 0.1mm-10mm, and in the porous aluminium foil negative pole, the porous aluminium foil functions simultaneously as collection
Fluid and negative active core-shell material.
Lithium secondary battery of the present invention, in each described minimum unit, face of the porous aluminium foil as collector
Product accounting is 20-60%, is 1-40% as the area accounting of negative active core-shell material.
Still optionally further, in each described minimum unit, the area accounting of hole is 25-60%.It is further optional
The distance between ground, edge and outermost porous hole of the porous aluminium foil are 2mm-5mm.
In the present invention, on the porous aluminium foil, with the line of centres of adjacent two horizontally-arranged adjacent three holes constituted etc.
Lumbar triangle shape region is minimum unit, and the hole area accounting of each minimum unit is equal.Still optionally further, laterally arbitrarily
The spacing of adjacent two circular cavities is equal, and the spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
Alternatively, the spacing phase of the spacing of the two circular cavities of horizontal arbitrary neighborhood and the two circular cavities of longitudinal arbitrary neighborhood
Deng.Alternatively, the spacing of the two circular cavities of the horizontal arbitrary neighborhood spacing horizontally-arranged with adjacent two is equal.
Alternatively, the porous aperture of the porous aluminium foil is 20nm-2mm.Further, porous aperture be 50 μm-
1.5mm.It is further preferred that the pore size of porous hole is equal.
In the present invention, the shape of the porous hole of the porous aluminium foil can be circle, ellipse, square, rectangle,
Prismatic, triangle, polygon, five-pointed star, quincunx etc., shape is not limited.
Alternatively, the thickness of porous aluminium foil is 10-100 microns.
In the present invention, the surface of the porous aluminium foil is further provided with carbon material layer, wherein, the material of the carbon material layer
Matter includes one or more material in conductive black, Graphene, graphite flake, CNT and organic matter carbonizing thing, described to have
Machine thing carbide includes carbide of the carbonization temperature for 200-700 DEG C of organic matter.Specifically, the organic matter carbonizing thing is Portugal
Grape sugar charcoal compound, char sucrose thing, citric acid carbide, polyvinylpyrrolidone carbide, polyvinyl alcohol carbide, polypropylene
One or more material such as alcohol carbide, phenolic resin carbide.
Alternatively, the thickness of the carbon material layer is 2nm-5 μm.Further, the thickness of the carbon material layer is
200nm-3μm。
In the present invention, the positive plate includes positive electrode active materials, the positive electrode active materials be graphite or lithium ion just
Pole material, such as LiFePO4, cobalt acid lithium, lithium titanate etc..I.e. lithium secondary battery can be conventional lithium ion battery, it is also possible to
It is aluminium-graphite Dual-ion cell.When for aluminium-graphite Dual-ion cell when, the positive plate include graphite, i.e., using graphite as just
Pole active material.
Wherein, electrolyte and barrier film are existing conventional lithium-ion battery electrolytes and barrier film.
The lithium secondary battery that third aspect present invention is provided, using the porous aluminium foil that designs with particular bore simultaneously as afflux
Body and negative active core-shell material, cycle performance is good, security performance is high.
Advantages of the present invention will be illustrated partly in the following description, and a part is apparent according to specification
, or can be known by the enforcement of the embodiment of the present invention.
Description of the drawings
Fig. 1 is the structural representation of the porous aluminium foil of the embodiment of the present invention 1；
Fig. 2 is the structural representation of the porous aluminium foil of the embodiment of the present invention 2；
Fig. 3 is the structural representation of the porous aluminium foil of the embodiment of the present invention 64.
Specific embodiment
Described below is the preferred embodiment of the embodiment of the present invention, it is noted that for the common skill of the art
For art personnel, on the premise of without departing from embodiment of the present invention principle, some improvements and modifications can also be made, these improvement
With the protection domain that retouching is also considered as the embodiment of the present invention.
Multiple embodiments are divided to be further detailed the embodiment of the present invention below.Wherein, the embodiment of the present invention is not limited
Due to following specific embodiment.In the range of constant principal right, can be appropriate carry out change enforcement.
Embodiment 1
A kind of preparation method of porous aluminium foil negative pole, comprises the following steps：
(1) it is the milli of 25%, aperture 1 according to the area accounting of each minimum unit Hole by the aluminium foil of 50 micron thickness
Rice, hole shape is circular hole, outermost bore edges and the design parameter that aluminium foil Edge Distance is 2 millimeters, is processed using machinery molding
Mode, fabricates out porous aluminium foil, and carries out purging using compressed air and remove flash removed；
(2) subsequently porous aluminium foil is immersed in containing 10 minutes in 20% aqueous povidone solution, then will be above-mentioned
Porous aluminium foil place and be connected with the sintering furnace of nitrogen with the ramp of 3 DEG C/min to 400 DEG C, and perseverance is carried out at 400 DEG C
Warm 4 hours charing process, you can obtain porous aluminium foil negative pole.
Fig. 1 is the structural representation of the porous aluminium foil of the embodiment of the present invention 1；In figure, d is outermost bore edges and aluminium foil side
The distance (2 millimeters) of edge；R is circular hole hole radius, and the isosceles triangle region that the line of centres in adjacent three holes is constituted is most
Junior unit, in each described minimum unit, area (the π r of hole2)/2 account for the ratio of the gross area (h*L)/2 of delta-shaped region
For 25%.In the present embodiment, porous hole rectangular array arrangement, the spacing of the two circular cavities of horizontal arbitrary neighborhood is equal, indulges
Spacing to the two circular cavities of arbitrary neighborhood is equal, and the laterally spacing of the two circular cavities of arbitrary neighborhood and longitudinal arbitrary neighborhood
The spacing of two circular cavities is equal.Laterally the hole number of each row is equal, and the hole number of each row in longitudinal direction is equal, each hole aligning
Arrangement, pore size is equal.
The preparation of traditional lithium-ion battery
Lithium iron phosphate positive material of the specific capacity for 140mAh/g is pressed into 95 with PVDF, conductive black:3:2 are coated in aluminium foil
On as positive plate.The processing technology of positive plate and process control, finally will processing using the technology of current industrialization
Porous aluminium foil negative pole afterwards and above-mentioned positive pole, electrolyte is the ethylene carbonate (EC) and dimethyl carbonic acid of 1mol/L LiPF6
(volume ratio is=1 to the mixed solution of ester (DMC)：1), barrier film is celgard2400 polypropylene porous films in the hand full of argon gas
Assembling in casing helps battery and obtains battery sample C1.
Comparative example 1 (traditional lithium-ion battery)
The aluminium foil of 50 micron thickness is immersed in containing 10 minutes in 20% aqueous povidone solution, then will be above-mentioned
Porous aluminium foil place and be connected with the sintering furnace of nitrogen with the ramp of 3 DEG C/min to 400 DEG C, and perseverance is carried out at 400 DEG C
Warm 4 hours charing process, you can obtain aluminium foil negative plate.By specific capacity for 140mAh/g lithium iron phosphate positive material with
PVDF, conductive black press 95:3:2 are coated on aluminium foil as positive plate.The processing technology of positive plate and process control are adopted
The technology of industrialization at present, finally by the positive plate after processing and aluminium foil negative plate, electrolyte is 1mol/L LiPF6's
(volume ratio is=1 to the mixed solution of ethylene carbonate (EC) and dimethyl carbonate (DMC)：1), barrier film is celgard2400
Polypropylene porous film assembling in the glove box full of argon gas helps battery and obtains battery sample C0.
Embodiment 2-38
With reference to the concrete steps of embodiment 1, relevant parameter is adjusted different embodiments 2-38 are obtained.Specifically
Embodiment parameter and test result are as shown in table 1：
Table 1
Embodiment 39
A kind of preparation method of porous aluminium foil negative pole, comprises the following steps：
(1) it is the milli of 25%, aperture 1 according to the area accounting of each minimum unit Hole by the aluminium foil of 20 micron thickness
Rice, hole shape is circular hole, outermost bore edges and the design parameter that aluminium foil Edge Distance is 2 millimeters, is processed using machinery molding
Mode, fabricates out porous aluminium foil, and carries out purging using compressed air and remove flash removed；
(2) subsequently porous aluminium foil is immersed in containing 10 minutes in 20% aqueous povidone solution, then will be above-mentioned
Porous aluminium foil place be connected with inert gas or reduction promoting the circulation of qi body sintering furnace in the ramp of 3 DEG C/min to 400 DEG C, and
4 hours charing process of constant temperature are carried out at a temperature of 400 DEG C, you can obtain porous aluminium foil negative pole.
The preparation of aluminium-graphite Dual-ion cell
Graphite positive electrode of the specific capacity for 100mAh/g is pressed into 95 with PVDF, conductive black:3:2 are coated in work on aluminium foil
For positive plate.The processing technology of positive plate and process control adopt the technology of current industrialization, finally by after processing
Porous aluminium foil negative pole and above-mentioned positive pole, electrolyte is the ethylene carbonate (EC) and methyl ethyl carbonate of 4mol/L LiPF6
(EMC) (volume ratio is=1 to mixed solution：1)+2% sub- vinyl carbonate (VC), barrier film is that celgard2400 polypropylene is more
Pore membrane assembling in the glove box full of argon gas helps battery and obtains battery sample C10.
Comparative example 2 (aluminium-graphite Dual-ion cell)
The aluminium foil of 20 micron thickness is immersed in containing 10 minutes in 20% aqueous povidone solution, then will be above-mentioned
Porous aluminium foil place be connected with inert gas or reduction promoting the circulation of qi body sintering furnace in 3 DEG C per minute of ramp to 400 DEG C,
And carry out 4 hours charing process of constant temperature at a temperature of 400 DEG C, you can obtain the modified aluminium foil cathode pole piece of charcoal.It is by specific capacity
The graphite positive electrode of 100mAh/g presses 95 with PVDF, conductive black:3:2 are coated on aluminium foil as positive plate, positive plate
Processing technology and process control adopt the technology of current industrialization, finally by the positive plate after processing and the modified aluminium foil of charcoal
Used as cathode pole piece, electrolyte is the ethylene carbonate (EC) of 4mol/L LiPF6 and the mixed solution of methyl ethyl carbonate (EMC)
(volume ratio is=1：1)+2% sub- vinyl carbonate (VC), barrier film is celgard2400 polypropylene porous films full of argon gas
Assembling in glove box helps battery and obtains battery sample C00.
Embodiment 40-63 is adjusted to relevant parameter and different realities is obtained with reference to the concrete steps of embodiment 39
Apply a 40-63.Specific embodiment parameter and test result are as shown in table 2：
Table 2
Embodiment 64
A kind of preparation method of porous aluminium foil negative pole, comprises the following steps：
(1) by the aluminium foil of 20 micron thickness, 1 millimeter of 25%, aperture is according to the area accounting of minimum unit Hole,
Hole shape is circular hole, outermost bore edges and the design parameter that aluminium foil Edge Distance is 2 millimeters, using machinery molding processing side
Formula, fabricates out porous aluminium foil, and carries out purging using compressed air and remove flash removed；
(2) subsequently porous aluminium foil is immersed in containing 10 minutes in 20% aqueous povidone solution, then will be above-mentioned
Porous aluminium foil place be connected with inert gas or reduction promoting the circulation of qi body sintering furnace in the ramp of 3 DEG C/min to 400 DEG C, and
4 hours charing process of constant temperature are carried out at a temperature of 400 DEG C, you can obtain porous aluminium foil negative pole.
Fig. 3 show the structural representation of the porous aluminium foil of the embodiment of the present invention 64.In figure, d be outermost bore edges with
The distance (2 millimeters) at aluminium foil edge, circular hole hole radius is r, is constituted with the line of centres in adjacent two horizontally-arranged adjacent three holes
Isosceles triangle region is minimum unit, in each described minimum unit, area (the π r of hole2)/2 account for the total of delta-shaped region
The ratio of area is 25%.In the present embodiment, the spacing in two holes of horizontal arbitrary neighborhood is equal, two of longitudinal arbitrary neighborhood
The spacing in hole is equal, and the spacing spacing horizontally-arranged with adjacent two of horizontal two circular cavities of arbitrary neighborhood is equal.In other enforcements
In example, the spacing of the two circular cavities of the horizontal arbitrary neighborhood spacing horizontally-arranged with adjacent two also can be unequal.Odd number laterally respectively row or
The hole number of each row in longitudinal direction is equal, and laterally respectively the hole number of row or each row in longitudinal direction is equal for even number.The horizontal each round hole of odd number
Alignment, the horizontal each round hole alignment of even number, and pore size is equal.
It should be noted that according to the above description the announcement of book and and illustrate, those skilled in the art in the invention are also
Above-mentioned embodiment can be changed and changed.Therefore, the invention is not limited in concrete reality disclosed and described above
Mode is applied, some equivalent modifications and change to the present invention should also be as within the scope of the claims of the present invention.This
Outward, although some specific terms used in this specification, these terms merely for convenience of description, not to the present invention
Constitute any restriction.
Claims (22)
1. a kind of porous aluminium foil negative pole, it is characterised in that including porous aluminium foil, the porous aluminium foil is provided with many of uniform arrangement
Hole hole, the delta-shaped region constituted with the line of centres of adjacent three holes as minimum unit, in each described minimum unit
The area accounting of hole is 10%-79%, and the distance between the edge of the porous aluminium foil and porous hole of outermost are
0.1mm-10mm。
2. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that with adjacent two horizontally-arranged adjacent three holes
The isosceles triangle region that heart line is constituted is minimum unit, and the hole area accounting of each minimum unit is equal.
3. porous aluminium foil negative pole as claimed in claim 2, it is characterised in that the horizontal spacing phase of the two circular cavities of arbitrary neighborhood
Deng the spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
4. porous aluminium foil negative pole as claimed in claim 3, it is characterised in that laterally the spacing of the two circular cavities of arbitrary neighborhood with
The spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
5. porous aluminium foil negative pole as claimed in claim 3, it is characterised in that laterally the spacing of the two circular cavities of arbitrary neighborhood with
Adjacent two horizontally-arranged spacing are equal.
6. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that the pore size of the porous hole is equal.
7. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that in each described minimum unit, the area of hole
Accounting is 25%-60%.
8. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that the edge of the porous aluminium foil and outermost porous
The distance between hole is 2mm-5mm.
9. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that the aperture of the porous hole is 20nm-2mm,
The shape of described hole includes circle, ellipse, square, rectangle, prismatic, triangle, polygon, five-pointed star, quincunx
In one or more.
10. porous aluminium foil negative pole as claimed in claim 1, it is characterised in that the surface of the porous aluminium foil is further arranged
There is carbon material layer, the thickness of the carbon material layer is 2nm-5 μm.
11. porous aluminium foil negative poles as claimed in claim 10, it is characterised in that the material of the carbon material layer includes conductive charcoal
One or more in black, Graphene, graphite flake, CNT and organic matter carbonizing thing, the organic matter carbonizing thing includes charcoal
Change the carbide of the organic matter that temperature is 200 DEG C -700 DEG C.
12. a kind of preparation methods of porous aluminium foil negative pole, it is characterised in that comprise the following steps：
Added using one or more mode in mechanical molding, chemical etching, laser cutting, plasma etching and electrochemical etching
Work obtains porous aluminium foil, that is, obtain porous aluminum paper tinsel negative pole；The porous aluminium foil is provided with the porous hole of uniform arrangement, with adjacent
The delta-shaped region that the line of centres of three holes is constituted is minimum unit, the area accounting of each minimum unit Hole
It is 0.1mm-10mm to be the distance between 10%-79%, edge and outermost porous hole of the porous aluminium foil.
13. preparation methods as claimed in claim 12, it is characterised in that further prepare material with carbon element on the porous aluminium foil
Layer, concretely comprises the following steps：
Solution containing material with carbon element is coated to into the surface of the porous aluminium foil, is dried, obtain porous aluminium foil negative pole；
Or the solution containing carbon materials material precursor is coated to into the surface of the porous aluminium foil, it is subsequently placed in inert gas or reduction
Property gas sintering furnace in be heat-treated 0.5-6 hours, make the carbon materials material precursor be carbonized, obtain porous aluminium foil negative pole.
14. a kind of lithium secondary batteries, it is characterised in that including positive plate, electrolyte, barrier film, negative plate, the negative plate is many
Hole aluminium foil negative pole, the porous aluminium foil negative pole includes porous aluminium foil, and the porous aluminium foil is provided with the porous hole of uniform arrangement,
The delta-shaped region constituted with the line of centres of adjacent three holes as minimum unit, the face of each minimum unit Hole
It is 0.1mm- that product accounting is the distance between 10%-79%, the edge of the porous aluminium foil and porous hole of outermost
10mm, in the porous aluminium foil negative pole, the porous aluminium foil functions simultaneously as collector and negative active core-shell material.
15. lithium secondary batteries as claimed in claim 14, it is characterised in that with adjacent two horizontally-arranged adjacent three holes
The isosceles triangle region that heart line is constituted is minimum unit, and the hole area accounting of each minimum unit is equal.
16. lithium secondary batteries as claimed in claim 15, it is characterised in that the spacing phase of the two circular cavities of horizontal arbitrary neighborhood
Deng the spacing of the two circular cavities of longitudinal arbitrary neighborhood is equal.
17. lithium secondary batteries as claimed in claim 16, it is characterised in that laterally the spacing of the two circular cavities of arbitrary neighborhood with
The spacing in two holes of longitudinal arbitrary neighborhood is equal.
18. lithium secondary batteries as claimed in claim 16, it is characterised in that laterally the spacing of the two circular cavities of arbitrary neighborhood with
Adjacent two horizontally-arranged spacing are equal.
19. lithium secondary batteries as claimed in claim 14, it is characterised in that the pore size of the porous hole is equal.
20. lithium secondary batteries as claimed in claim 14, it is characterised in that the aperture of the porous hole is 20nm-2mm,
The shape of described hole includes circle, ellipse, square, rectangle, prismatic, triangle, polygon, five-pointed star, quincunx
In one or more.
21. lithium secondary batteries as claimed in claim 14, it is characterised in that the surface of the porous aluminium foil is further provided with
Carbon material layer, the thickness of the carbon material layer is 2nm-5 μm.
22. lithium secondary batteries as claimed in claim 14, it is characterised in that in each described minimum unit, the porous aluminum
Paper tinsel is 20-60% as the area accounting of collector, is 1-40% as the area accounting of negative active core-shell material.
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