CN117199389A - Negative electrode composite current collector, composite pole piece, lithium battery and manufacturing method of lithium battery - Google Patents
Negative electrode composite current collector, composite pole piece, lithium battery and manufacturing method of lithium battery Download PDFInfo
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- CN117199389A CN117199389A CN202311227768.8A CN202311227768A CN117199389A CN 117199389 A CN117199389 A CN 117199389A CN 202311227768 A CN202311227768 A CN 202311227768A CN 117199389 A CN117199389 A CN 117199389A
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- 239000002131 composite material Substances 0.000 title claims abstract description 144
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 40
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 39
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 27
- 239000010410 layer Substances 0.000 claims abstract description 680
- 229920000307 polymer substrate Polymers 0.000 claims abstract description 125
- 239000012790 adhesive layer Substances 0.000 claims abstract description 28
- 230000004888 barrier function Effects 0.000 claims description 92
- 239000000463 material Substances 0.000 claims description 53
- 239000000758 substrate Substances 0.000 claims description 51
- 239000010949 copper Substances 0.000 claims description 50
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 42
- 229910052782 aluminium Inorganic materials 0.000 claims description 41
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 40
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 37
- 229910052751 metal Inorganic materials 0.000 claims description 37
- 239000002184 metal Substances 0.000 claims description 37
- 229910045601 alloy Inorganic materials 0.000 claims description 35
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- 229910052802 copper Inorganic materials 0.000 claims description 33
- 238000000034 method Methods 0.000 claims description 31
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 30
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- 239000011651 chromium Substances 0.000 claims description 19
- 229910052750 molybdenum Inorganic materials 0.000 claims description 19
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- 238000009792 diffusion process Methods 0.000 claims description 15
- 239000010936 titanium Substances 0.000 claims description 15
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 14
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 14
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 14
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 14
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- 229910017052 cobalt Inorganic materials 0.000 claims description 14
- 239000010941 cobalt Substances 0.000 claims description 14
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 14
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- XECAHXYUAAWDEL-UHFFFAOYSA-N acrylonitrile butadiene styrene Chemical compound C=CC=C.C=CC#N.C=CC1=CC=CC=C1 XECAHXYUAAWDEL-UHFFFAOYSA-N 0.000 claims description 3
- 229920000122 acrylonitrile butadiene styrene Polymers 0.000 claims description 3
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- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 3
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- 229910052710 silicon Inorganic materials 0.000 claims description 3
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- MHSKRLJMQQNJNC-UHFFFAOYSA-N terephthalamide Chemical compound NC(=O)C1=CC=C(C(N)=O)C=C1 MHSKRLJMQQNJNC-UHFFFAOYSA-N 0.000 claims description 3
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- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims 1
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 7
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- 229910001416 lithium ion Inorganic materials 0.000 description 7
- 239000011889 copper foil Substances 0.000 description 6
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- 229910018182 Al—Cu Inorganic materials 0.000 description 3
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- 229910000943 NiAl Inorganic materials 0.000 description 2
- NPXOKRUENSOPAO-UHFFFAOYSA-N Raney nickel Chemical compound [Al].[Ni] NPXOKRUENSOPAO-UHFFFAOYSA-N 0.000 description 2
- 229910000676 Si alloy Inorganic materials 0.000 description 2
- NRTOMJZYCJJWKI-UHFFFAOYSA-N Titanium nitride Chemical compound [Ti]#N NRTOMJZYCJJWKI-UHFFFAOYSA-N 0.000 description 2
- 238000005411 Van der Waals force Methods 0.000 description 2
- 229910001297 Zn alloy Inorganic materials 0.000 description 2
- WPPDFTBPZNZZRP-UHFFFAOYSA-N aluminum copper Chemical compound [Al].[Cu] WPPDFTBPZNZZRP-UHFFFAOYSA-N 0.000 description 2
- VNNRSPGTAMTISX-UHFFFAOYSA-N chromium nickel Chemical compound [Cr].[Ni] VNNRSPGTAMTISX-UHFFFAOYSA-N 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
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- 229910001120 nichrome Inorganic materials 0.000 description 2
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N phenol group Chemical group C1(=CC=CC=C1)O ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 2
- 239000007774 positive electrode material Substances 0.000 description 2
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- 229910000838 Al alloy Inorganic materials 0.000 description 1
- 229910000881 Cu alloy Inorganic materials 0.000 description 1
- 229910000570 Cupronickel Inorganic materials 0.000 description 1
- 229910010199 LiAl Inorganic materials 0.000 description 1
- 229910000914 Mn alloy Inorganic materials 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- JRBRVDCKNXZZGH-UHFFFAOYSA-N alumane;copper Chemical compound [AlH3].[Cu] JRBRVDCKNXZZGH-UHFFFAOYSA-N 0.000 description 1
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 description 1
- FJMNNXLGOUYVHO-UHFFFAOYSA-N aluminum zinc Chemical compound [Al].[Zn] FJMNNXLGOUYVHO-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
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- 239000011247 coating layer Substances 0.000 description 1
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- YOCUPQPZWBBYIX-UHFFFAOYSA-N copper nickel Chemical compound [Ni].[Cu] YOCUPQPZWBBYIX-UHFFFAOYSA-N 0.000 description 1
- KUNSUQLRTQLHQQ-UHFFFAOYSA-N copper tin Chemical class [Cu].[Sn] KUNSUQLRTQLHQQ-UHFFFAOYSA-N 0.000 description 1
- TVZPLCNGKSPOJA-UHFFFAOYSA-N copper zinc Chemical compound [Cu].[Zn] TVZPLCNGKSPOJA-UHFFFAOYSA-N 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
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- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
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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
- Cell Electrode Carriers And Collectors (AREA)
Abstract
The present disclosure provides a negative electrode composite current collector, a composite pole piece, a lithium battery and a manufacturing method thereof, wherein the negative electrode composite current collector comprises: a polymer substrate layer; the first conductive layer is arranged on one side of the polymer substrate layer and comprises a plurality of discrete first linear conductive structures; a first adhesive layer disposed between the first conductive layer and the polymer substrate layer; the first composite layer is arranged on one side of the first conductive layer far away from the polymer substrate layer and among the plurality of discrete first linear conductive structures; the second conductive layer is arranged on one side of the polymer substrate layer, which is far away from the first conductive layer, and comprises a plurality of discrete second linear conductive structures; a second adhesive layer disposed between the second conductive layer and the polymer substrate layer; the second composite layer is arranged on one side of the second conductive layer far away from the polymer substrate layer and among the plurality of discrete second linear conductive structures.
Description
Cross Reference to Related Applications
The present disclosure claims chinese patent application No. submitted in china at 2023, 6 and 30.
202310804530.0, the entire contents of which are incorporated herein by reference.
Technical Field
The disclosure relates to the technical field of lithium batteries, in particular to a negative electrode composite current collector, a composite pole piece, a lithium battery and a manufacturing method thereof.
Background
Lithium ion batteries, abbreviated as lithium batteries, are widely used in human daily life as a kind of efficient energy storage device. The traditional lithium ion battery cell internally comprises a pair of positive plate and negative plate, and the positive plate and the negative plate are stacked in multiple layers or wound to realize battery cells with different capacities. In the traditional lithium ion battery, aluminum foil is used as a positive current collector metal material, copper foil is used as a negative current collector metal material, and in the process of preparing the lithium ion battery, cutting ends of the current collector are exposed easily, so that oxidation or corrosion of copper or aluminum ends is caused.
Disclosure of Invention
The invention aims to provide a composite current collector with a composite negative electrode, a composite pole piece, a lithium battery and a manufacturing method thereof, which at least can solve the technical problem of end oxidation or corrosion after cutting of the current lithium battery.
The embodiment of the disclosure provides a negative electrode composite current collector for a lithium battery, the negative electrode composite current collector comprising:
A polymer substrate layer;
a first conductive layer disposed on one side of the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures;
a first adhesive layer disposed between the first conductive layer and the polymer substrate layer, configured to adhere the first conductive layer and the polymer substrate layer;
a first composite layer disposed on a side of the first conductive layer remote from the polymeric substrate layer and disposed between a plurality of discrete first-line-type conductive structures;
a second conductive layer disposed on a side of the polymeric substrate layer remote from the first conductive layer, the second conductive layer comprising a plurality of discrete second linear conductive structures;
a second adhesive layer disposed between the second conductive layer and the polymer substrate layer, configured to adhere the second conductive layer and the polymer substrate layer;
a second composite layer disposed on a side of the second conductive layer remote from the polymeric substrate layer and disposed between a plurality of discrete second linear conductive structures;
wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
In some embodiments of the present invention, in some embodiments,
the orthographic projection of the first bonding layer on the polymer substrate layer is overlapped with the orthographic projection of the first conductive layer on the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second bonding layer on the polymer substrate layer is overlapped with the orthographic projection of the second conductive layer on the polymer substrate layer.
In some embodiments of the present invention, in some embodiments,
the orthographic projection of the first bonding layer on the polymer substrate layer is overlapped with the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second bonding layer on the polymer substrate layer is overlapped with the polymer substrate layer.
In some embodiments of the present invention, in some embodiments,
the orthographic projection of the first composite layer on the polymer substrate layer covers the orthographic projection of the first conductive layer on the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second composite layer on the polymer substrate layer covers the orthographic projection of the second conductive layer on the polymer substrate layer.
In some embodiments of the present invention, in some embodiments,
the first composite layer includes:
a first barrier layer arranged on one side of the first conductive layer away from the polymer substrate layer,
a first intermediate layer disposed on a side of the first barrier layer adjacent to the first conductive layer, configured to prevent diffusion between the first barrier layer and the first conductive layer; the method comprises the steps of,
The second composite layer includes:
a second barrier layer arranged on one side of the second conductive layer away from the polymer substrate layer,
and a second intermediate layer, disposed on a side of the second barrier layer near the second conductive layer, configured to prevent diffusion between the second barrier layer and the second conductive layer.
In some embodiments of the present invention, in some embodiments,
the orthographic projection of the first bonding layer, the first barrier layer and the first intermediate layer on the polymer substrate layer is overlapped; the method comprises the steps of,
and the orthographic projection of the second bonding layer, the second barrier layer and the second intermediate layer on the polymer substrate layer is overlapped.
In some embodiments, the polymeric substrate layer is selected from at least one of acrylonitrile-butadiene-styrene copolymer, polybutylene terephthalate, poly-paraphenylene terephthalamide, polyimide, polyamide, polyethylene, polystyrene, polyvinylidene fluoride, polyvinyl chloride, polytetrafluoroethylene, polypropylene, polycarbonate, polyoxymethylene, epoxy, and phenolic.
In some embodiments of the present invention, in some embodiments,
the tensile strength of the material of the polymer substrate layer is more than or equal to 150MPa; or,
The heat shrinkage rate of the material of the polymer substrate layer after being treated for 30min at 150 ℃ is less than or equal to 3%; or,
the thickness of the polymer substrate layer is 1-15 mu m.
In some embodiments of the present invention, in some embodiments,
the material of the first conductive layer and/or the second conductive layer is selected from at least one of the following:
a single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; or alternatively;
selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, tungsten, manganese, magnesium and zinc, and/or the non-metal in the alloy is selected from silicon and/or carbon.
In some embodiments of the present invention, in some embodiments,
the thickness of the first conductive layer and/or the second conductive layer is 0.1-2 mu m respectively; or,
the binding force between the first conductive layer and/or the second conductive layer and the polymer substrate layer is more than or equal to 0.5N/15mm;
the resistivity of the first conductive layer and/or the second conductive layer is less than or equal to 8 mu omega cm.
In some embodiments of the present invention, in some embodiments,
the material of the first conductive layer and/or the second conductive layer comprises Al, and the material of the first barrier layer and/or the second barrier layer comprises Cu.
In some embodiments of the present invention, in some embodiments,
the material of the first barrier layer and/or the second barrier layer is selected from at least one of the following:
a single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; or alternatively;
selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, and tungsten.
In some embodiments of the present invention, in some embodiments,
the thicknesses of the first barrier layer and the second barrier layer are respectively 1-1500nm; or,
the binding force between the first barrier layer and the first conductive layer and/or the binding force between the second barrier layer and the second conductive layer is more than or equal to 0.5N/15mm.
In some embodiments of the present invention, in some embodiments,
the material of the first intermediate layer and/or the second intermediate layer is selected from at least one of the following: from a single metal, alloy, oxide semiconductor or conductive compound.
In some embodiments of the present invention, in some embodiments,
the material of the first intermediate layer and/or the second intermediate layer is selected from at least one of the following:
the single metal is selected from one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
The metal in the alloy is selected from at least one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
the oxide semiconductor is selected from Cu 2 O、ZnO、SnO 2 、Fe 2 O 3 、TiO 2 、ZrO 2 、Co 2 O 3 、WO 3 、In 2 O 3 、Al 2 O 3 And Fe (Fe) 3 O 4 At least one of (a) and (b);
the conductive compound is selected from TiB 2 、TiC、TiN、ZrB 2 、ZrC、ZrN、VB 2 、VC、VN、NbB 2 、NbC、NbN、TaB 2 、TaC、CrB 2 、Cr 3 C 2 、CrN、Mo 2 C、Mo 2 B 5 、W 2 B 5 WC and LaB 6 At least one of them.
In some embodiments, the first intermediate layer and/or the second intermediate layer has a thickness of 1-1000nm.
In some embodiments, the first barrier layer and the second barrier layer are the same material, and the first conductive layer and the second conductive layer are the same material; the first intermediate layer and the second intermediate layer are the same material; the first barrier layer, the first conductive layer, and the first intermediate layer are different from each other in material.
In some embodiments, the material of the first and/or second adhesive layer is selected from at least one of: a single metal or alloy or metal compound;
wherein the single metal is selected from at least one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
the alloy is at least one of nickel-based alloy and aluminum-based alloy;
The metal compound is AlOx, tiB 2 、TiC、TiN、ZrB 2 、ZrC、ZrN、VB 2 、VC、VN、NbB 2 、NbC、NbN、TaB 2 、TaC、CrB 2 、Cr 3 C 2 、CrN、Mo 2 C、Mo 2 B 5 、W 2 B 5 WC and LaB 6 At least one of them.
In some embodiments, the first adhesive layer and/or the second adhesive layer is prepared in a manner selected from at least one of the following: magnetron sputtering, ion plating, vacuum evaporation plating or in-situ reaction.
The present disclosure also provides a composite pole piece comprising a negative electrode composite current collector as described in any one of the above.
The present disclosure also provides a lithium battery comprising a composite pole piece as described above.
The present disclosure also provides a method of manufacturing a negative electrode composite current collector, the method comprising:
providing a polymeric substrate layer;
providing a first tie layer on one side of the polymeric substrate layer;
providing a first conductive layer on a side of the first tie layer remote from the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures;
disposing a first composite layer on a side of the first conductive layer remote from the polymeric substrate layer, and disposing a first composite layer between a plurality of discrete first-line-type conductive structures;
providing a second tie layer on a side of the polymeric substrate layer remote from the first tie layer;
providing a second conductive layer on a side of the second tie layer remote from the polymeric substrate layer, the second conductive layer comprising a plurality of discrete second linear conductive structures;
Disposing a second composite layer on a side of the second conductive layer remote from the polymeric substrate layer, and disposing a second composite layer between a plurality of discrete second linear conductive structures;
wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
In some embodiments of the present invention, in some embodiments,
disposing a first composite layer on a side of the first conductive layer remote from the polymeric substrate layer, and disposing a first composite layer between a plurality of discrete first-line-type conductive structures comprises:
a first intermediate layer is arranged on one side of the first barrier layer, which is close to the first conductive layer;
providing a first barrier layer on a side of the first intermediate layer remote from the polymer substrate layer, wherein the first intermediate layer is configured to prevent diffusion between the first barrier layer and the first conductive layer, and,
disposing a second composite layer on a side of the second conductive layer remote from the polymeric substrate layer, and disposing a second composite layer between a plurality of discrete second linear conductive structures comprises:
a second intermediate layer is arranged on one side of the second barrier layer, which is close to the second conductive layer;
A second barrier layer is disposed on a side of the second intermediate layer remote from the polymeric substrate layer, wherein the second intermediate layer is configured to prevent diffusion between the second barrier layer and the second conductive layer.
In some embodiments, the method of disposing a first conductive layer on a side of the first adhesive layer remote from the polymer substrate layer and/or disposing a second conductive layer on a side of the second adhesive layer remote from the polymer substrate layer comprises: one or more of evaporation, deposition and sputtering.
The disclosure also provides a method for manufacturing a composite pole piece, comprising the method for manufacturing the negative electrode composite current collector.
The present disclosure also provides a method of manufacturing a lithium battery, including a method of manufacturing a composite pole piece as described above.
Compared with the related art, the method has the following technical effects:
1. the negative electrode composite current collector provided by the disclosure can replace the traditional copper as the negative electrode current collector, so that copper resources and cost are saved;
2. the barrier layer in the present disclosure is a continuous and compact thin film structure, which can prevent alloying of the negative electrode Li-Al material and can improve the conductivity of the composite current collector;
3. A bonding layer structure is designed between the polymer layer and the conductive layer by a PVD method, so that the bonding force between the polymer layer and the conductive layer is enhanced;
4. the coating layer is arranged outside the discrete linear conductive structure in the negative electrode composite current collector, so that corrosion of the end part of Li-Al can be prevented in the cutting application process;
5. the negative electrode composite current collector disclosed by the disclosure can be very thin in thickness, and the effective energy volume ratio of the lithium battery can be improved.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, illustrate embodiments consistent with the disclosure and together with the description, serve to explain the principles of the disclosure. It will be apparent to those of ordinary skill in the art that the drawings in the following description are merely examples of the disclosure and that other drawings may be derived from them without undue effort. In the drawings:
fig. 1 is a schematic cross-sectional structure view of a negative electrode composite current collector cut along an N line according to some embodiments of the present disclosure;
fig. 2 is a schematic diagram of another side cross-sectional structure of a negative electrode composite current collector according to some embodiments of the present disclosure;
fig. 3 is a schematic cross-sectional structure of a negative electrode composite current collector according to other embodiments of the present disclosure;
FIG. 4 is a flow chart of a method of manufacturing a composite current collector provided in some embodiments of the present disclosure;
FIG. 5 is a flow chart of a method of manufacturing a composite current collector according to further embodiments of the present disclosure; and
fig. 6 is a flow chart of a method of manufacturing a composite current collector according to further embodiments of the present disclosure.
Detailed Description
For the purpose of promoting an understanding of the principles and advantages of the disclosure, reference will now be made in detail to the drawings, in which it is apparent that the embodiments described are only some, but not all embodiments of the disclosure. Based on the embodiments in this disclosure, all other embodiments that a person of ordinary skill in the art would obtain without making any inventive effort are within the scope of protection of this disclosure.
The terminology used in the embodiments of the disclosure is for the purpose of describing particular embodiments only and is not intended to be limiting of the disclosure. As used in this disclosure of embodiments and the appended claims, the singular forms "a," "an," and "the" are intended to include the plural forms as well, unless the context clearly indicates otherwise, the "plurality" generally includes at least two.
It should be understood that the term "and/or" as used herein is merely one relationship describing the association of the associated objects, meaning that there may be three relationships, e.g., a and/or B, may represent: a exists alone, A and B exist together, and B exists alone. In addition, the character "/" herein generally indicates that the front and rear associated objects are an "or" relationship.
It should be understood that although the terms first, second, third, etc. may be used in embodiments of the present disclosure, these should not be limited to these terms. These terms are only used to distinguish one from another. For example, a first may also be referred to as a second, and similarly, a second may also be referred to as a first, without departing from the scope of embodiments of the present disclosure.
It should also be noted that the terms "comprises," "comprising," or any other variation thereof, are intended to cover a non-exclusive inclusion, such that a product or apparatus that comprises a list of elements does not include only those elements but may include other elements not expressly listed or inherent to such product or apparatus. Without further limitation, an element defined by the phrase "comprising" does not exclude the presence of other like elements in a commodity or device comprising such element.
In the related art, a lithium battery generally comprises a positive electrode plate and a negative electrode plate, and the positive electrode plate and the negative electrode plate realize battery cells with different capacities through multilayer superposition or positive electrode winding. The positive electrode sheet generally includes a positive electrode current collector and positive electrode active materials coated on both sides of the positive electrode current collector. The positive current collector typically employs aluminum foil, which is typically 10 to 15 microns thick. The negative electrode sheet generally includes a negative electrode current collector and coating both sides of the negative electrode current collectorNegative electrode active material. The negative current collector typically employs copper foil, which is typically 4.5 to 9 microns thick. The lithium ion battery generally adopts aluminum as a positive electrode current collector metal material and copper as a negative electrode current collector metal material. This is because the oxidation potential of the metal aluminum is high, and the size of the lattice octahedral voids of the metal aluminum is similar to that of lithium, so that the metal aluminum is extremely easy to react with lithium to form LiAl and Li 3 Al 2 、Li 4 Al 3 Such alloys consume not only a large amount of li+ but also destroy the structure and morphology of the metallic aluminum itself, so that aluminum can serve as a current collector for the positive electrode of a lithium ion battery, but cannot serve as a current collector for the negative electrode of a lithium ion battery. Cu has little lithium intercalation capacity in the charge and discharge process of the battery, and keeps stable structure and electrochemical performance, so the Cu can be used as a current collector of the negative electrode of the ion battery.
The positive electrode active material is coated on two sides of an aluminum foil, and then the positive electrode plate is manufactured after baking, rolling, slitting and die cutting, and the negative electrode active material is coated on two sides of a copper foil, and then the negative electrode plate is manufactured after baking, rolling, slitting and die cutting. And then sequentially superposing or winding the negative plate/the diaphragm/the positive plate to form the battery core of the lithium battery. Because the aluminum foil and the copper foil are thicker, the positive electrode current collector and the negative electrode current collector occupy a considerable volume, so that the effective energy volume ratio of the lithium battery is low, and the miniaturization of the lithium battery is not facilitated.
The embodiment of the disclosure provides a negative electrode composite current collector for a lithium battery, the negative electrode composite current collector comprising: a polymer substrate layer; a first conductive layer disposed on one side of the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures; a first adhesive layer disposed between the first conductive layer and the polymer substrate layer, configured to adhere the first conductive layer and the polymer substrate layer; a first composite layer disposed between a side of the first conductive layer remote from the polymeric substrate layer and a plurality of discrete first-line-type conductive structures; a second conductive layer disposed on a side of the polymeric substrate layer remote from the first conductive layer, the second conductive layer comprising a plurality of discrete second linear conductive structures; a second adhesive layer disposed between the second conductive layer and the polymer substrate layer, configured to adhere the second conductive layer and the polymer substrate layer; a second composite layer disposed between a side of the second conductive layer remote from the polymeric substrate layer and a plurality of discrete second linear conductive structures; wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
Alternative embodiments of the present disclosure are described in detail below with reference to the drawings.
Fig. 1 is a schematic cross-sectional structure view of a negative electrode composite current collector cut along an N line according to some embodiments of the present disclosure; fig. 2 is a schematic diagram of another side cross-sectional structure of a negative electrode composite current collector according to some embodiments of the present disclosure; specifically, the embodiment of the present disclosure provides a negative electrode composite current collector 100 for a lithium battery, the negative electrode composite current collector 100 including: a polymer substrate layer 1; a first conductive layer 2, wherein the first conductive layer 2 is disposed on one side of the polymer substrate layer 1, and the first conductive layer 2 includes a plurality of discrete first-line conductive structures; a first adhesive layer 8, the first adhesive layer 8 being disposed between the first conductive layer 2 and the polymer base material layer 1, configured to adhere the first conductive layer 2 and the polymer base material layer 1; a first composite layer 10, the first composite layer 10 being disposed between a side of the first conductive layer 2 remote from the polymer substrate layer 1 and a plurality of discrete first linear conductive structures; a second conductive layer 3, the second conductive layer 3 being disposed on a side of the polymeric substrate layer 1 remote from the first conductive layer 2, the second conductive layer 3 comprising a plurality of discrete second linear conductive structures; a second adhesive layer 9, the second adhesive layer 9 being disposed between the second conductive layer 3 and the polymer base material layer 1, configured to adhere the second conductive layer 3 and the polymer base material layer 1; a second composite layer 10, the second composite layer 10 being disposed between a side of the second conductive layer 3 remote from the polymer substrate layer 1 and a plurality of discrete second linear conductive structures; wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
As shown in fig. 2, the first conductive layer 2 includes a plurality of discrete first linear conductive structures, the second conductive layer 3 includes a plurality of discrete second linear conductive structures, the first linear conductive structures and the second linear conductive structures are respectively wrapped by the first composite layer 10 and the second composite layer 20, and when the small-area negative electrode composite current collector 100 is cut from the large-area negative electrode composite current collector 100, for example, the small-area negative electrode composite current collector 100 can be cut along the line M in fig. 2 for assembling a lithium battery, so that the exposed ends of the first conductive layer 2 and the second conductive layer 3 are not caused, and oxidation or corrosion of the first conductive layer 2 and the second conductive layer 3 due to exposure to air is avoided. The first linear conductive structure and the second linear conductive structure may be linear or curved structures, and the problem of exposed end portions caused by cutting can be solved as long as the first linear conductive structure and the second linear conductive structure are formed in a discrete and approximately parallel arrangement along the surface of the polymer substrate layer 1. The plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically arranged relative to the polymer substrate layer, so that the grooves (without conductive layers) on one side can be cut to the grooves (without conductive layers) on the other corresponding side when the grooves are cut, and the grooves are prevented from being cut to the conductive layers to expose the conductive layers.
In some embodiments, as shown in fig. 2, the orthographic projection of the first composite layer 10 on the polymer substrate layer 1 covers the orthographic projection of the first conductive layer 2 on the polymer substrate layer 1; and, the orthographic projection of the second composite layer 20 on the polymer substrate layer 1 covers the orthographic projection of the second conductive layer 3 on the polymer substrate layer 1. The projections of the first and second linear conductive structures on the polymer substrate layer 1 substantially overlap, which ensures that the ends of the first and second conductive layers 2 and 3 are not exposed as long as they are cut from between the linear conductive structures.
In some embodiments, as shown in fig. 2, the orthographic projection of the first adhesive layer 8 on the polymer substrate layer 1 overlaps with the orthographic projection of the first conductive layer 2 on the polymer substrate layer 1; and, the orthographic projection of the second adhesive layer 9 on the polymer substrate layer 1 overlaps the orthographic projection of the second conductive layer 3 on the polymer substrate layer 1, so as to ensure the complete adhesion of the first conductive layer 2 and the polymer substrate layer 1, and ensure the complete adhesion of the second conductive layer 3 and the polymer substrate layer 1. In the forming process, for example, a mask is arranged, a bonding material is deposited in a mask gap by means of magnetron sputtering, ion plating, vacuum evaporation or in-situ reaction, and then a conductive layer is deposited, so that a structure of a conductive layer and a bonding layer are laminated, and the conductive layer can be stably combined with a polymer substrate layer through the bonding layer.
In other embodiments, as shown in fig. 3, the orthographic projection of the first adhesive layer 8 on the polymer substrate layer 1 overlaps the polymer substrate layer 1; and, the orthographic projection of the second adhesive layer 9 on the polymer substrate layer 1 overlaps with the polymer substrate layer 1, and then the first conductive layer 2 is formed on the first adhesive layer 8, and the second conductive layer 3 is formed on the second adhesive layer 9, so as to ensure the complete adhesion of the first conductive layer 2 and the polymer substrate layer 1, and ensure the complete adhesion of the second conductive layer 3 and the polymer substrate layer 1. In the forming process, for example, the bonding material can be deposited on two sides of the polymer substrate layer 1 by means of magnetron sputtering, ion plating, vacuum evaporation or in-situ reaction, and then the conductive layer can be deposited in a mask gap by means of magnetron sputtering, ion plating, vacuum evaporation or in-situ reaction by means of setting a mask, so that a stacked structure of the conductive layer and the bonding layer is formed, and the conductive layer can be stably combined with the polymer substrate layer through the bonding layer.
In some embodiments, the polymeric substrate layer 1 is selected from at least one of acrylonitrile-butadiene-styrene copolymer, polybutylene terephthalate, poly-paraphenylene terephthalamide, polyimide, polyamide, polyethylene, polystyrene, polyvinylidene fluoride, polyvinyl chloride, polytetrafluoroethylene, polypropylene, polycarbonate, polyoxymethylene, epoxy, and phenolic. Compared with the traditional copper foil layer, the polymer substrate layer is lighter in weight and thinner in thickness, thereby being beneficial to reducing the volume of the lithium battery and improving the performance of the lithium battery.
In some embodiments, the tensile strength of the material of the polymer substrate layer 1 is equal to or greater than 150MPa, preferably 150-400MPa; the polymer substrate layer 1 is used for supporting the whole negative electrode composite current collector, and the negative electrode composite current collector is supported by the polymer substrate layer with high tensile strength in the deposition process, so that the broken coil deformation cannot occur in the manufacturing process of the coated and rolled pole piece, and therefore, when the tensile strength is less than 150Mpa, the supporting effect in the coating and rolling process cannot be met, and the broken coil deformation is easy to occur. The heat shrinkage rate of the material of the polymer substrate layer 1 after being treated for 30min at 150 ℃ is less than or equal to 3%, and the heat shrinkage rate of the polymer substrate layer 1 is too large, so that the negative electrode composite current collector is broken and deformed, and therefore, according to the experimental verification of the embodiment, the heat shrinkage rate of the material of the polymer substrate layer 1 after being treated for 30min at 150 ℃ is less than or equal to 3%, so that the preparation process of the negative electrode composite current collector can be met; the thickness of the polymer substrate layer 1 is 1-15 μm, preferably 1-10 μm, and the excessive thickness of the polymer substrate layer 1 increases the volume of the negative electrode composite current collector and increases the internal resistance of the lithium battery, so the polymer substrate layer 1 with the thickness in the above range is selected in the present disclosure. The polymer substrate layer 1 has the characteristics of light weight, good ductility, high tensile strength, small thermal shrinkage rate and the like, the volume and the weight of the lithium battery can be effectively reduced, and due to the existence of the polymer substrate layer 1, the short circuit of the battery can not be formed even if the conductive layer is broken down, so that the safety of the battery is improved.
In some embodiments, the material of the first conductive layer 2 and/or the second conductive layer 3 is selected from at least one of the following: a single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; preferably, one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum and tungsten with a purity of 99-100 wt%; or alternatively; selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, tungsten, manganese, magnesium and zinc, and/or the non-metal in the alloy is selected from silicon and/or carbon. Preferably, the alloy is at least one selected from aluminum copper alloy, aluminum manganese alloy, aluminum silicon alloy, aluminum magnesium silicon alloy and aluminum zinc alloy. The higher the purity of the conductive layer material, the better the conductivity, which is more advantageous for enhancing the conductivity efficiency.
In some embodiments, the most preferred first conductive layer 2 and/or the second conductive layer 3 is aluminum, which has the characteristics of good conductivity, light weight, low price, good flexibility, etc., so that aluminum is preferred as the conductive material when preparing the first conductive layer 2 and/or the second conductive layer 3. Aluminum is selected as a material of the first conductive layer 2 and/or the second conductive layer 3, an aluminum layer is deposited on the polymer substrate layer 1 in a PVD mode, conductivity is enhanced, the aluminum layer is wrapped between the polymer substrate layer and the composite layer, the defect that aluminum cannot be used as a negative plate in a traditional lithium battery is overcome, the thickness of the negative plate is further reduced, and the conductivity of the negative plate is not weakened.
In some embodiments, the thickness of the first conductive layer 2 and/or the second conductive layer 3 is 0.1-2 μm, respectively; preferably 0.2-1.5 μm; the vacuum equipment can realize micron-level vacuum deposition, the thicker the metal conductive layer is, the lower the resistance is, but the thickness of the metal layer is increased, the difficulty in the process realization is increased, in the experiment disclosed by the disclosure, the film can be formed at one time at 800-2000 nm, and the metal film resistivity at the thickness section of 800-1500 nm is stable through the optimization of the process parameters. The conductive layer can be formed into a stable conductive effect by the directional movement of free electrons as long as it is a continuous film (thickness: 30nm or more). However, if the conductive layer is too thin, the resistivity will be high due to the too large size effect of the metal film, which affects the internal resistance of the cell, so, through experiments, the present disclosure selects a conductive layer with a thickness above 200 nm.
In some embodiments, the bonding force between the first conductive layer 2 and/or the second conductive layer 3 and the polymer substrate layer 1 is greater than or equal to 0.5N/15mm, so that the first conductive layer 2 and/or the second conductive layer 3 are prevented from being peeled off from the polymer substrate layer 1 during curling or application, and the conductivity is prevented from being affected.
In some embodiments, the resistivity of the first conductive layer 2 and/or the second conductive layer 3 is less than or equal to 8μΩ·cm.
The interface bonding phenomenon can occur between the polymer substrate layer and the metal conductive layer due to different inherent properties of materials, and because only van der Waals force exists between the polymer substrate layer and the metal conductive layer and no chemical bond exists between the polymer substrate layer and the metal conductive layer, the composite current collector structure is expected to be a composite structure with high conductivity and high bonding strength, the bonding force is larger and better, the bonding force is more than or equal to 0.5N/15mm, the upper limit is not less, and the resistivity of the bulk metal material is less than or equal to the resistivity of the composite current collector and less than or equal to 8uΩ & cm.
In some embodiments, the first composite layer 10 comprises: a first barrier layer 4, the first barrier layer 4 being disposed on a side of the first conductive layer 2 remote from the polymer substrate layer 1, a first intermediate layer 6 being disposed on a side of the first barrier layer 4 proximate to the first conductive layer 2, the first intermediate layer 6 being configured to prevent diffusion between the first barrier layer 4 and the first conductive layer 2; and, the second composite layer 20 includes: a second barrier layer 5 disposed on a side of the second conductive layer 3 away from the polymer substrate layer 1, a second intermediate layer 7 disposed on a side of the second barrier layer 5 adjacent to the second conductive layer 3, the second intermediate layer 7 being configured to prevent diffusion between the second barrier layer 5 and the second conductive layer 3. The first composite layer 10 and the second composite layer 20 completely encapsulate the first conductive layer 2 and the second conductive layer 3, so that aluminum is a viable solution as a negative electrode, and due to the discrete structural design and the encapsulated composite layer, the problem of exposing the end of the aluminum layer due to cutting during manufacturing of the lithium battery is overcome.
In some embodiments, the material of the first barrier layer 4 and/or the second barrier layer 5 is selected from at least one of the following: a single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; preferably, one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum and tungsten with a purity of 99-100 wt%; or alternatively; selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, and tungsten; further preferably, the alloy is selected from at least one of copper-aluminum alloy, copper-nickel alloy, copper-zinc alloy and copper-tin alloy.
In some embodiments, the thickness of the first barrier layer 4 and the second barrier layer 5 is 1-1500nm, preferably 30-1000nm, respectively; compared with the traditional copper foil cathode, the first barrier layer 4 and the second barrier layer 5 can deposit thinner copper layers in a PVD mode, so that copper materials are saved, and the overall thickness of the cathode plate is reduced.
In some embodiments, the bonding force between the first barrier layer 4 and the first conductive layer 2 and/or the bonding force between the second barrier layer 5 and the second conductive layer 3 is greater than or equal to 0.5N/15mm, and the stronger bonding force avoids peeling between the first barrier layer 4 and the first conductive layer 2 or between the second barrier layer 5 and the second conductive layer 3 in the curling or application process, thereby affecting conductivity.
The barrier layer is used for preventing the conductive layer Al from being exposed, and the operation can be realized as long as the barrier layer is a continuous compact film (for example, the thickness is more than or equal to 30 nm); another function of the barrier layer is to conduct electricity, but if the barrier layer is too thin (several tens of nanometers), interdiffusion with the conductive layer occurs in a short time (several days or several weeks), so that Al is exposed, the original function of the barrier layer is lost, and if the barrier layer is too thick, the process cost, the material use efficiency and the like are increased, so that the barrier layer may be set between 1 and 1500nm, preferably 30 to 1000nm.
The interface bonding phenomenon of the conductive layer and the barrier layer is unstable, because only van der Waals force exists between the conductive layer and the barrier layer, a layer of aluminum oxide film is naturally formed on the aluminum surface of the conductive layer, so that the bonding strength between Cu and Al is not high, and if CuAl is layered due to the not high bonding strength in the use process of the battery, the conductive effect is lost, so that the bonding force of the conductive layer and the barrier layer is hoped to be more than or equal to 0.5N/15mm.
Because aluminum is used as the conductive layer, the aluminum composite current collector is used as the negative electrode, alloying reaction can be carried out with metal lithium, and the conductive performance is invalid, therefore, a barrier layer (Cu) is arranged on the aluminum layer, an aluminum-copper composite layer is formed, the alloying reaction between Li and Al can be blocked while the conductivity is not reduced, and the stability of the lithium battery is improved.
In some embodiments, the AI serving as the conductive layer and the Cu serving as the barrier layer are both positioned at the negative electrode, under the action of the electrolyte, mutual diffusion and galvanic corrosion of Al-Cu can possibly occur, and the interlayer is designed between the Al-Cu layers, so that the mutual diffusion and corrosion of the Al-Cu layers can be prevented or slowed down, the conductive effect can be achieved, and the binding force between the aluminum and the copper can be enhanced. Specifically, the material of the first intermediate layer 6 and/or the second intermediate layer 7 is selected from at least one of the following: from a single metal, alloy, oxide semiconductor or conductive compound.
In some embodiments, the material of the first intermediate layer 6 and/or the second intermediate layer 7 is selected from at least one of the following: the single metal is selected from one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc; the metal in the alloy is selected from at least one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc; the oxide semiconductor is selected from Cu 2 O、ZnO、SnO 2 、Fe 2 O 3 、TiO 2 、ZrO 2 、Co 2 O 3 、WO 3 、In 2 O 3 、Al 2 O 3 And Fe (Fe) 3 O 4 At least one of (a) and (b); the conductive compound is selected from TiB 2 、TiC、TiN、ZrB 2 、ZrC、ZrN、VB 2 、VC、VN、NbB 2 、NbC、NbN、TaB 2 、TaC、CrB 2 、Cr 3 C 2 、CrN、Mo 2 C、Mo 2 B 5 、W 2 B 5 WC and LaB 6 At least one of them. Preferably, the first intermediate layer 6 and/or the second intermediate layer 7 are respectively selected from at least one of nickel, nickel-based alloys, copper-based alloys and titanium nitride, preferably titanium nitride.
In some embodiments, the thickness of the first intermediate layer 6 and/or the second intermediate layer 7 is 1-1000nm, preferably 5-500nm. The intermediate layer has the functions of conducting electricity and enhancing the bonding strength between CuAl, prevents mutual diffusion of the CuAl and the CuAl, is generally thinner, and can be made as thin as possible as long as the intermediate layer has the functions, so that raw materials and cost are saved, and the film can be formed generally by 1-1000nm, preferably 5-100 nm or 5-500nm.
In some embodiments, the first barrier layer 4 and the second barrier layer 5 are the same material, and the first conductive layer 2 and the second conductive layer 3 are the same material; the first intermediate layer 6 and the second intermediate layer 7 are the same material; the materials of the first barrier layer 4, the first conductive layer 2 and the first intermediate layer 6 are different from each other. In some embodiments, the material of the first conductive layer 2 and/or the second conductive layer 3 comprises Al and the material of the first barrier layer 4 and/or the second barrier layer 5 comprises Cu.
Examples:
in the first embodiment, al layers with a thickness of 1um are deposited on the upper and lower surfaces of a PET substrate with a thickness of 6um in vacuum, and Cu layers with a thickness of 300nm are deposited on the upper and lower surfaces of the Al layers in vacuum. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the second embodiment, alOx with the thickness of 10nm is reacted in situ on the upper and lower surfaces of a PET substrate with the thickness of 6um, an Al layer with the thickness of 1um is continuously formed, and Cu layers with the thickness of 300nm are vacuum-evaporated on the upper and lower surfaces of the Al layer. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the third embodiment, alOx with the thickness of 10nm is generated on the upper and lower surfaces of the PET substrate with the thickness of 6um through in-situ reaction, an Al layer with the thickness of 1um is continuously formed, ni layers with the thickness of 10nm are subjected to magnetron sputtering on the upper and lower surfaces of the Al layer, and Cu layers with the thickness of 300nm are subjected to vacuum evaporation on the upper and lower surfaces of the Ni layer. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the fourth embodiment, 10nm of NiCr layers are magnetron-sputtered on the upper and lower surfaces of a PET substrate with a thickness of 6um, 1um of Al layers are vacuum-deposited on the upper and lower surfaces of the NiCr layers, 10nm of Ni layers are magnetron-sputtered on the upper and lower surfaces of the Al layers, and 300nm of Cu is vacuum-deposited on the upper and lower surfaces of the Ni layers. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the fifth embodiment, ti layers with the thickness of 10nm are magnetron sputtered on the upper and lower surfaces of a PET substrate with the thickness of 6um, al layers with the thickness of 1um are vacuum-deposited on the upper and lower surfaces of the Ti layers, ni layers with the thickness of 10nm are magnetron sputtered on the upper and lower surfaces of the Al layers, and Cu layers with the thickness of 300nm are vacuum-deposited on the upper and lower surfaces of the Ni layers. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the sixth embodiment, 10nm of NiAl layer is magnetron sputtered on the upper and lower surfaces of the PET substrate with the thickness of 6um, 1um of Al layer is vacuum deposited on the upper and lower surfaces of the NiAl layer, 10nm of Ni layer is magnetron sputtered on the upper and lower surfaces of the Al layer, and 300nm of Cu layer is vacuum deposited on the upper and lower surfaces of the Ni layer. The battery is prepared, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
In the comparative example, 1um metal Al is directly evaporated on the upper surface and the lower surface of a PET substrate with the thickness of 6um, a composite current collector after film formation is used as a negative current collector to prepare a battery, the first effect and the cycle performance of the battery are represented, and the corrosiveness of the battery after the battery pole piece is disassembled is compared.
Table 1 comparative performance of composite current collector cell
| Numbering device | Sheet resistance mΩ/sq | Binding force N/15mm | First effect% | 1C cycle-turns | Whether or not the battery core is pulverized |
| Example 1 | 26.92 | 4.36 | 91.5 | 1163 | Whether or not |
| Example 2 | 26.88 | 8.45 | 91.24 | 1165 | Whether or not |
| Example 3 | 26.29 | 8.26 | 91.45 | 1189 | Whether or not |
| Example 4 | 26.82 | 7.38 | 91.71 | 1152 | Whether or not |
| Example 5 | 26.55 | 7.29 | 91.27 | 1141 | Whether or not |
| Example 6 | 26.32 | 7.74 | 91.36 | 1153 | Whether or not |
| Comparative example | 32.13 | 4.36 | 91.23 | / | Is that |
As can be seen from the comparison results of the performances of the composite current collectors in Table 1, the square resistance values of the embodiment 1 to the embodiment 6 are lower and lower than 27mΩ/sq, and the square resistance value of the comparative example is higher than 32mΩ/sq, which indicates that the composite current collectors formed by the embodiments of the application have better conductivity.
According to the application, the bonding layer is added between the Al layer and the substrate in the embodiment 2 to the embodiment 6, the bonding force is improved from 4.36N/15mm to 7-8N/15mm, and the bonding force of the composite current collector is greatly increased.
The first coulomb efficiency of the application in the examples 1 to 6 is close to that of the comparative example, which shows that the composite current collector cell formed by the examples of the application has better discharge performance.
As can be seen from comparison of the present application with the comparative examples of examples 1 to 6, the first effects of examples 1 to 6 and comparative examples are substantially the same, while the internal resistance is significantly reduced, and in addition, the cycle numbers of examples 1 to 6 are higher, indicating that the composite current collector is better applied as a negative electrode current collector.
As can be seen from the cell results in table 1, the examples 1 to 6 according to the present application can be used as negative electrode current collectors (wherein the binding force of examples 2 to 6 is better), and the cell performance is good, the barrier layer Cu is not pulverized after the battery is disassembled, and the comparative example battery is disassembled and is directly pulverized, which means that Al cannot be directly applied to the negative electrode. The present disclosure also provides a composite pole piece comprising the negative composite current collector 100 as described in the above embodiments.
The present disclosure also provides a lithium battery comprising the composite pole piece as described in the above embodiments.
The present disclosure also provides a method for manufacturing the negative electrode composite current collector 100, as shown in fig. 4, including the steps of:
step S102: providing a polymeric substrate layer;
step S104: providing a first tie layer on one side of the polymeric substrate layer;
step S106: providing a first conductive layer on a side of the first tie layer remote from the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures;
step S108: disposing a first composite layer between a side of the first conductive layer remote from the polymeric substrate layer and a plurality of discrete first-line-type conductive structures;
step S110: providing a second tie layer on a side of the polymeric substrate layer remote from the first tie layer;
step S112: providing a second conductive layer on a side of the second tie layer remote from the polymeric substrate layer, the second conductive layer comprising a plurality of discrete second linear conductive structures;
step S114: disposing a second composite layer between a side of the second conductive layer remote from the polymeric substrate layer and a plurality of discrete second linear conductive structures;
Wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
In some embodiments, as shown in fig. 5, step S108 includes the following sub-steps:
step S108-1: a first intermediate layer is arranged on one side of the first barrier layer, which is close to the first conductive layer;
step S108-2: a first barrier layer is disposed on a side of the first intermediate layer remote from the polymer substrate layer, wherein the first intermediate layer is configured to prevent diffusion between the first barrier layer and the first conductive layer.
In some embodiments, as shown in fig. 6, step S114 includes the following sub-steps:
step S114-1: a second intermediate layer is arranged on one side of the second barrier layer, which is close to the second conductive layer;
step S114-2: a second barrier layer is disposed on a side of the second intermediate layer remote from the polymeric substrate layer, wherein the second intermediate layer is configured to prevent diffusion between the second barrier layer and the second conductive layer.
In some embodiments, the method of disposing a first conductive layer on a side of the first adhesive layer remote from the polymer substrate layer and/or disposing a second conductive layer on a side of the second adhesive layer remote from the polymer substrate layer comprises: one or more of evaporation, deposition and sputtering.
The present disclosure also provides a method of manufacturing a composite pole piece, including a method of manufacturing a negative electrode composite current collector 100 as described in any one of the above.
The present disclosure also provides a method of manufacturing a lithium battery, including a method of manufacturing a composite pole piece as described above.
The thickness of the negative electrode composite pole piece formed by the negative electrode composite current collector disclosed by the disclosure is very thin compared with that of a negative electrode piece of a conventional lithium battery, and the negative electrode composite pole piece can be used for improving the effective energy volume ratio of the lithium battery; in addition, the negative electrode current collector provided by the invention can replace the traditional copper as the negative electrode current collector, thereby saving copper resources and cost and improving safety; the barrier layer in the present disclosure is a continuous and compact thin film structure, which can prevent alloying of the negative electrode Li-Al material and can improve the conductivity of the composite current collector; a bonding layer structure is designed between the polymer layer and the conductive layer by a PVD method, so that the bonding force between the polymer layer and the conductive layer is enhanced; the negative electrode composite current collector of the present disclosure can prevent Li-Al end corrosion during cutting applications.
Finally, it should be noted that: in the present specification, each embodiment is described in a progressive manner, and each embodiment is mainly described in a different point from other embodiments, and identical and similar parts between the embodiments are all enough to refer to each other.
The above embodiments are merely for illustrating the technical solution of the present disclosure, and are not limiting thereof; although the present disclosure has been described in detail with reference to the foregoing embodiments, it should be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present disclosure.
Claims (26)
1. A negative electrode composite current collector for a lithium battery, the negative electrode composite current collector comprising:
a polymer substrate layer;
a first conductive layer disposed on one side of the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures;
a first adhesive layer disposed between the first conductive layer and the polymer substrate layer, configured to adhere the first conductive layer and the polymer substrate layer;
a first composite layer disposed on a side of the first conductive layer remote from the polymeric substrate layer and disposed between a plurality of discrete first-line-type conductive structures;
a second conductive layer disposed on a side of the polymeric substrate layer remote from the first conductive layer, the second conductive layer comprising a plurality of discrete second linear conductive structures;
A second adhesive layer disposed between the second conductive layer and the polymer substrate layer, configured to adhere the second conductive layer and the polymer substrate layer;
a second composite layer disposed on a side of the second conductive layer remote from the polymeric substrate layer and disposed between a plurality of discrete second linear conductive structures;
wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
2. The negative electrode composite current collector according to claim 1, wherein,
the orthographic projection of the first bonding layer on the polymer substrate layer is overlapped with the orthographic projection of the first conductive layer on the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second bonding layer on the polymer substrate layer is overlapped with the orthographic projection of the second conductive layer on the polymer substrate layer.
3. The negative electrode composite current collector according to claim 1, wherein,
the orthographic projection of the first bonding layer on the polymer substrate layer is overlapped with the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second bonding layer on the polymer substrate layer is overlapped with the polymer substrate layer.
4. The negative electrode composite current collector according to claim 1, wherein,
the orthographic projection of the first composite layer on the polymer substrate layer covers the orthographic projection of the first conductive layer on the polymer substrate layer; the method comprises the steps of,
the orthographic projection of the second composite layer on the polymer substrate layer covers the orthographic projection of the second conductive layer on the polymer substrate layer.
5. The negative electrode composite current collector according to claim 1, wherein,
the first composite layer includes:
a first barrier layer arranged on one side of the first conductive layer away from the polymer substrate layer,
a first intermediate layer disposed on a side of the first barrier layer adjacent to the first conductive layer, configured to prevent diffusion between the first barrier layer and the first conductive layer; the method comprises the steps of,
the second composite layer includes:
a second barrier layer arranged on one side of the second conductive layer away from the polymer substrate layer,
and a second intermediate layer, disposed on a side of the second barrier layer near the second conductive layer, configured to prevent diffusion between the second barrier layer and the second conductive layer.
6. The negative electrode composite current collector according to claim 5, wherein,
The orthographic projection of the first bonding layer, the first barrier layer and the first intermediate layer on the polymer substrate layer is overlapped; the method comprises the steps of,
and the orthographic projection of the second bonding layer, the second barrier layer and the second intermediate layer on the polymer substrate layer is overlapped.
7. The negative electrode composite current collector according to claim 1, wherein the polymer base material layer is at least one selected from the group consisting of acrylonitrile-butadiene-styrene copolymer, polyethylene terephthalate, polybutylene terephthalate, poly-paraphenylene terephthalamide, polyimide, polyamide, polyethylene, polystyrene, polyvinylidene fluoride, polyvinyl chloride, polytetrafluoroethylene, polypropylene, polycarbonate, polyoxymethylene, epoxy, and phenolic resin.
8. The negative electrode composite current collector according to claim 1, wherein,
the tensile strength of the material of the polymer substrate layer is more than or equal to 150MPa; or,
the heat shrinkage rate of the material of the polymer substrate layer after being treated for 30min at 150 ℃ is less than or equal to 3%; or,
the thickness of the polymer substrate layer is 1-15 mu m.
9. The negative electrode composite current collector according to claim 1, wherein the material of the first conductive layer and/or the second conductive layer is selected from at least one of:
A single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; or alternatively;
selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, tungsten, manganese, magnesium and zinc, and/or the non-metal in the alloy is selected from silicon and/or carbon.
10. The negative electrode composite current collector according to claim 1, wherein the thickness of the first conductive layer and/or the second conductive layer is 0.1-2 μm, respectively; or,
the binding force between the first conductive layer and/or the second conductive layer and the polymer substrate layer is more than or equal to 0.5N/15mm;
the resistivity of the first conductive layer and/or the second conductive layer is less than or equal to 8 mu omega cm.
11. The anode composite current collector according to claim 5, wherein the material of the first conductive layer and/or the second conductive layer comprises Al and the material of the first barrier layer and/or the second barrier layer comprises Cu.
12. The anode composite current collector according to claim 5, wherein the material of the first barrier layer and/or the second barrier layer is selected from at least one of:
A single metal with purity of more than or equal to 98 wt%: aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, or tungsten; or alternatively;
selected from an alloy, wherein the metal in the alloy is selected from at least one of aluminum, copper, nickel, iron, titanium, silver, gold, cobalt, chromium, molybdenum, and tungsten.
13. The negative electrode composite current collector according to claim 5, wherein,
the thicknesses of the first barrier layer and the second barrier layer are respectively 1-1500nm; or,
the binding force between the first barrier layer and the first conductive layer and/or the binding force between the second barrier layer and the second conductive layer is more than or equal to 0.5N/15mm.
14. The anode composite current collector according to claim 5, wherein the material of the first intermediate layer and/or the second intermediate layer is selected from at least one of: from a single metal, alloy, oxide semiconductor or conductive compound.
15. The anode composite current collector according to claim 14, wherein the material of the first intermediate layer and/or the second intermediate layer is selected from at least one of:
the single metal is selected from one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
The metal in the alloy is selected from at least one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
the oxide semiconductor is selected from Cu 2 O、ZnO、SnO 2 、Fe 2 O 3 、TiO 2 、ZrO 2 、Co 2 O 3 、WO 3 、In 2 O 3 、Al 2 O 3 And Fe (Fe) 3 O 4 At least one of (a) and (b);
the conductive compound is selected from TiB 2 、TiC、TiN、ZrB 2 、ZrC、ZrN、VB 2 、VC、VN、NbB 2 、NbC、NbN、TaB 2 、TaC、CrB 2 、Cr 3 C 2 、CrN、Mo 2 C、Mo 2 B 5 、W 2 B 5 WC and LaB 6 At least one of them.
16. The anode composite current collector according to claim 5, wherein the thickness of the first intermediate layer and/or the second intermediate layer is 1-1000nm.
17. The anode composite current collector of claim 5, wherein said first and second barrier layers are the same material, and said first and second conductive layers are the same material; the first intermediate layer and the second intermediate layer are the same material; the first barrier layer, the first conductive layer, and the first intermediate layer are different from each other in material.
18. The negative electrode composite current collector according to claim 1, wherein the material of the first and/or second adhesive layers is selected from at least one of: a single metal or alloy or metal compound;
wherein the single metal is selected from at least one of Cu, cr, ta, zn, cd, in, tl, mn, co, mo, fe, sn, ge, bi, sb, re, ti, V, ni, nb and Tc;
The alloy is at least one of nickel-based alloy and aluminum-based alloy;
the metal compound is AlOx, tiB 2 、TiC、TiN、ZrB 2 、ZrC、ZrN、VB 2 、VC、VN、NbB 2 、NbC、NbN、TaB 2 、TaC、CrB 2 、Cr 3 C 2 、CrN、Mo 2 C、Mo 2 B 5 、W 2 B 5 WC and LaB 6 At least one of them.
19. The negative electrode composite current collector according to claim 1, wherein the first bonding layer and/or the second bonding layer is prepared in a manner selected from at least one of: magnetron sputtering, ion plating, vacuum evaporation plating or in-situ reaction.
20. A composite pole piece, characterized in that it comprises a negative electrode composite current collector according to any one of claims 1 to 19.
21. A lithium battery comprising the composite pole piece of claim 20.
22. A method of manufacturing a negative electrode composite current collector, the method comprising:
providing a polymeric substrate layer;
providing a first tie layer on one side of the polymeric substrate layer;
providing a first conductive layer on a side of the first tie layer remote from the polymeric substrate layer, the first conductive layer comprising a plurality of discrete first-line-type conductive structures;
disposing a first composite layer on a side of the first conductive layer remote from the polymeric substrate layer, and disposing a first composite layer between a plurality of discrete first-line-type conductive structures;
Providing a second tie layer on a side of the polymeric substrate layer remote from the first tie layer;
providing a second conductive layer on a side of the second tie layer remote from the polymeric substrate layer, the second conductive layer comprising a plurality of discrete second linear conductive structures;
disposing a second composite layer on a side of the second conductive layer remote from the polymeric substrate layer, and disposing a second composite layer between a plurality of discrete second linear conductive structures;
wherein the plurality of discrete first linear conductive structures and the plurality of discrete second linear conductive structures are symmetrically disposed with respect to the polymer substrate layer.
23. The method of manufacturing according to claim 22, wherein,
disposing a first composite layer on a side of the first conductive layer remote from the polymeric substrate layer, and disposing a first composite layer between a plurality of discrete first-line-type conductive structures comprises:
a first intermediate layer is arranged on one side of the first barrier layer, which is close to the first conductive layer;
providing a first barrier layer on a side of the first intermediate layer remote from the polymer substrate layer, wherein the first intermediate layer is configured to prevent diffusion between the first barrier layer and the first conductive layer, and,
Disposing a second composite layer on a side of the second conductive layer remote from the polymeric substrate layer, and disposing a second composite layer between a plurality of discrete second linear conductive structures comprises:
a second intermediate layer is arranged on one side of the second barrier layer, which is close to the second conductive layer;
a second barrier layer is disposed on a side of the second intermediate layer remote from the polymeric substrate layer, wherein the second intermediate layer is configured to prevent diffusion between the second barrier layer and the second conductive layer.
24. The method of manufacturing according to claim 22, wherein the method of providing a first conductive layer on a side of the first adhesive layer remote from the polymer substrate layer and/or providing a second conductive layer on a side of the second adhesive layer remote from the polymer substrate layer comprises: one or more of evaporation, deposition and sputtering.
25. A method of manufacturing a composite pole piece, characterized by comprising the method of manufacturing a negative electrode composite current collector according to any one of claims 22 to 24.
26. A method of manufacturing a lithium battery comprising the method of manufacturing a composite pole piece of claim 25.
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