CN104716328A - Composite current collector material and preparation method thereof - Google Patents
Composite current collector material and preparation method thereof Download PDFInfo
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- CN104716328A CN104716328A CN201410658494.2A CN201410658494A CN104716328A CN 104716328 A CN104716328 A CN 104716328A CN 201410658494 A CN201410658494 A CN 201410658494A CN 104716328 A CN104716328 A CN 104716328A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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Abstract
The invention discloses a composite current collector material for aqueous solution batteries. The composite current collector material is composed of a conductive film, a metal or alloy foil or net and another conductive film fused into one in a sandwich manner. The invention further provides a preparation method for the composite current collector material. The preparation method is characterized in that the three layers of the conductive film, the metal or alloy foil or net and the another conductive film are stacked up in the sandwich manner and pressed together by using two heating pressure plates or pressure blocks so as to form the composite current collector material, wherein the heating temperature of the heating pressure plates or pressure blocks is in a range of 70 to 390 DEG C, pressure intensity is in a range of 1 to 1000 N/cm2, and hot pressing time is in a range of 0.1 to 15 s. The composite current collector material provided by the invention has substantially superior corrosion resistance and almost unchanged conductive capability compared with traditional metal (or alloy) current collectors, can be widely applied to a plurality of aqueous solution batteries and improves long-term cycle performance of the batteries.
Description
Technical field
The present invention relates to physics, field of chemical power source, particularly relate to current collector material field.
Background technology
Both positive and negative polarity collector in lithium ion battery is aluminium foil and Copper Foil respectively; Both positive and negative polarity collector in Ni-H cell is nickel foam and brass screen respectively; Both positive and negative polarity current collector material in lead-acid battery is lead alloy (or electrolytic lead) and lead alloy respectively.People, in long-term practice process, for the physical chemistry power supply of different electrochemical systems have selected distinct current collector material, mainly consider following several respects:
1. current collector material will be stablized under this electrochemical system, self does not occur or redox corrosion or other chemical corrosion occur less in charge and discharge process;
2. the electron conduction of current collector material wants high;
3 collectors finally need to be connected reliably with the busbar of power source internal or pole, and this connection is all welding (welding) usually, therefore generally all contain the composition of metal or metalloid or alloy in current collector material;
4. the active material electrode in current collector material and system will have good compatibility, and contact resistance is to each other little;
5. the density of current collector material is the smaller the better.
But, the current collector material of prior art above-mentioned performance one or several in still need improvement.
Summary of the invention
The present invention proposes a kind of composite current collector material can stablized, work in aqueous efficiently.The present invention is in order to solve the corrosion of metals problem of current collector material in aqueous solution battery.
The invention provides a kind of composite current collector material, it is characterized in that, this composite current collector material is fused into one in " sandwich " mode by conductive film, metal or alloy foil or net material, conductive film three layers.
Described composite current collector material is except the few part in lug top of described metal or alloy foil or net material, surface, the edge of described metal or alloy foil or net material are all covered by described conductive film, capped metal or alloy part by conductive film and outside completely isolated.
Conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent, and the thickness of conductive film and collector are grown or wide ratio is not more than 2%, are preferably 0.1%-0.5%; For the current collector material of 120mm*120mm size, the preferred thickness of conductive film is 0.2mm-0.3mm.Conductive agent in described conductive film is carbon atoms s
pthe material of 2 hydridization covalent bonds, is preferably one or more in graphite powder, super conductive black, CNT (carbon nano-tube), carbon nano-fiber; Be more preferably super conductive black or graphite powder.High molecular polymer in described conductive film is one or more in polyethylene, polypropylene, polyethylene terephthalate, nylon, polytetrafluoroethylene, fluorocarbon resin; Be preferably polyethylene or polypropylene material.The ratio of described conductive agent in described conductive film is 30%-95% by mass.
The described metal or alloy foil of composite current collector material of the present invention or net material are the one in iron foil, aluminium foil, Copper Foil, filtter gold, titanium foil, nickel foil, stainless steel foil or iron net, aluminium net, copper mesh, brass screen, titanium net, nickel screen, stainless (steel) wire; Be preferably stainless (steel) wire, the thickness of metal or alloy foil or net material and the length of collector or wide ratio are not more than 1%, are preferably 0.01%-0.05%; For the current collector material of 120mm*120mm size, the preferred thickness range of metal material is 0.025mm-0.045mm.
The thickness of described conductive film and the thickness ratio of described metal or alloy foil or net material are 50.1%-2000%, are preferably 80%-400%.
The conductive film of composite current collector material of the present invention, metal or alloy foil or net material, conductive film are fused into one by the mode of heating pressurization.
The preparation method of composite current collector material of the present invention, it is characterized in that, conductive film, metal or alloy foil or net material, conductive film three layers are stacked in " sandwich " mode, the pressing plate heated with two or briquetting pressing form, the heating temperature range of its center platen or briquetting is 70 DEG C-390 DEG C, pressure range is 1N/cm2-1000N/cm2, and hot pressing time scope is 0.1s-15s.
In the method for the invention, described composite current collector material is except the few part in lug top of described metal or alloy foil or net material, surface, the edge of described metal or alloy foil or net material are all covered by described conductive film, capped metal or alloy part by conductive film and outside completely isolated.
In the method for the invention, conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent, and the thickness of conductive film and collector are grown or wide ratio is not more than 2%, are preferably 0.1%-0.5%; For the current collector material of 120mm*120mm size, the preferred thickness of conductive film is 0.2mm-0.3mm.Conductive agent in described conductive film is the material of carbon atoms sp2 hydridization covalent bond, is preferably one or more in graphite powder, super conductive black, CNT (carbon nano-tube), carbon nano-fiber; Be more preferably super conductive black or graphite powder.High molecular polymer in described conductive film is one or more in polyethylene, polypropylene, polyethylene terephthalate, nylon, polytetrafluoroethylene, fluorocarbon resin; Be preferably polyethylene or polypropylene material.The ratio of described conductive agent in described conductive film is 30%-95% by mass.
In the method for the invention, the described metal or alloy foil of composite current collector material of the present invention or net material are the one in iron foil, aluminium foil, Copper Foil, filtter gold, titanium foil, nickel foil, stainless steel foil or iron net, aluminium net, copper mesh, brass screen, titanium net, nickel screen, stainless (steel) wire; Be preferably stainless (steel) wire, the thickness of metal or alloy foil or net material and the length of collector or wide ratio are not more than 1%, are preferably 0.01%-0.05%; For the current collector material of 120mm*120mm size, the preferred thickness range of metal material is 0.025mm-0.045mm.
In the method for the invention, the thickness of described conductive film and the thickness ratio of described metal or alloy foil or net material are 50.1%-2000%, are preferably 80%-400%.
By high molecular polymer conductive film, by the method uniform fold that merges after heating pressurization on the surface of metal or alloy foil or net material, thus formed a kind of with the composite current collector material of conductive carbon film and metal (or alloy) series-parallel connection conduction.The conductive film used in the present invention, role stops electrolyte molecule, electrolyte ion and dissolves long-term, the lasting corrosion of various gas molecules in the electrolytic solution to metal (or alloy) current collector material; And take into account the effect that electronics is transmitted in short distance (thickness direction of conductive film).Metal (or alloy) paper tinsel (net) material mainly plays the effect electronics of being come by film transfer (or to film transfer electronics) being delivered to battery pole ear along the direction (long distance) on foil surface.Current collector material resistance to corrosion of the present invention is better than traditional metal (or alloy) collector greatly, the conductive capability of collector but has almost no change simultaneously, multiple aqueous solution battery can be widely used in, improve the long-term cycle performance of battery.
Accompanying drawing explanation
Fig. 1 a shows the front view of composite current collector material; Fig. 1 b shows the amplification view of composite current collector edge of materials part.
Fig. 2 shows 304 stainless steel substrate CV scanning curves (relative to (VS.) saturated calomel electrode).
Fig. 3 shows 304 and covers conductive film base material CV scanning curve (relative to saturated calomel electrode).
Fig. 4 shows and covers the CV scintigram of stainless (steel) wire collector of conductive film and the contrast figure of the CV scintigram of stainless (steel) wire collector.
Embodiment
Illustrate technical scheme of the present invention below in conjunction with accompanying drawing, but protection scope of the present invention is not limited to following embodiment.
Below illustrate the making that length and width are respectively the collector of the band lug of L mm, W mm (assuming that L > W).
The first step, selects thickness to be no more than one in the iron foil of W*1%mm, aluminium foil, Copper Foil, filtter gold, titanium foil, nickel foil, stainless steel foil or iron net, aluminium net, copper mesh, brass screen, titanium net, nickel screen, stainless (steel) wire, and cuts into required shape.
Second step, select one or more being no more than in the polyethylene of W*2%mm, polypropylene, polyethylene terephthalate, nylon, polytetrafluoroethylene, fluorocarbon resin of thickness to be the conductive film two panels of base material, conductive additive is wherein the carbon atoms sp such as graphite powder, super conductive black, CNT (carbon nano-tube), carbon nano-fiber
2one or more mixtures of hydridization covalent bond.The mass fraction of the conductive agent in selected conductive film is 30%-95%.Conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent.Conductive film is cut into the shape needed for collector, conductive film should large 3-6mm more each than the length and width of metal (or alloy) paper tinsel (net) material, to guarantee in the final composite current collector material made except the few part in metal (or alloy) paper tinsel (net) material lug top, metal (or alloy) paper tinsel (net) material surface, edge all covers by conductive film, capped metal (or alloy) part with air without directly contacting.
3rd step, conductive film, metal (or alloy) paper tinsel (net) material, conductive film three layers are stacked in " sandwich " mode, and to guarantee in composite current collector material except the few part in metal (or alloy) paper tinsel (net) material lug top at this, metal (or alloy) paper tinsel (net) material surface, edge all covers by conductive film, capped metal (or alloy) part with air without directly contacting.
4th step, utilize self-control hot press, by the temperature increase of briquetting or pressing plate to a certain suitable temperature in 70 DEG C-390 DEG C, maintain more than the 30 minutes time (such as 30 minutes to 1 hour), after temperature stabilization (fluctuation is no more than 2 DEG C), the semi-finished product collector that 3rd step is folded is placed on the centre of two briquettings or pressing plate, the pressure of regulator solution cylinder pressure is to 1N/cm
2-1000N/cm
2, depress rapidly, keep pressure 0.1s-15s, pressure relief, collector is taken out and cools to room temperature, namely obtain the finished product required for us: a kind of collector of composite material of conductive film coated metal (alloy).
As shown in Figure 1a, composite current collector material of the present invention is fused into one in " sandwich " mode by conductive film 1, metal or alloy foil or net material 2, conductive film 1 three layers.Described composite current collector material is except the few part 3 on the lug of described metal or alloy foil or net material, surface, the edge of described metal or alloy foil or net material are all covered by described conductive film, capped metal or alloy part by conductive film and outside completely isolated.Fig. 1 b shows the amplification view of composite current collector edge of materials part.Size due to conductive film is slightly larger than the size of metal (alloy) foil/net material to guarantee that metal (alloy) foil/net material wraps by conductive film completely, so be territory, conductive film mutual tabetisol at the fringe region of composite material.Metal (alloy) foil/net material is not had in the middle of this region.Except the small part on the lug top of fringe region and described metal (or alloy) foil/net material, composite current collector material (main body) is made up of upper and lower two-layer conductive film and middle metal (alloy) foil/net material.
Embodiment 1
Below illustrate the making of the collector of the band lug of 120mm*120mm size.
The first step, selects the stainless (steel) wire of thickness 0.03mm, and cuts into required shape.
Second step, select the polyethylene of thickness 0.2mm to be the conductive film two panels of base material, conductive additive is wherein graphite powder.The mass fraction of the conductive agent in selected conductive film is 30%.Conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent.Conductive film is cut into the shape needed for collector, conductive film should large 3mm more each than the length and width of metal (or alloy) paper tinsel (net) material, to guarantee in the final composite current collector material made except the few part in metal (or alloy) paper tinsel (net) material lug top, metal (or alloy) paper tinsel (net) material surface, edge all covers by conductive film, capped metal (or alloy) part with air without directly contacting.
3rd step, conductive film, metal (or alloy) paper tinsel (net) material, conductive film three layers are stacked in " sandwich " mode, and to guarantee in composite current collector material except the few part in metal (or alloy) paper tinsel (net) material lug top at this, metal (or alloy) paper tinsel (net) material surface, edge all covers by conductive film, capped metal (or alloy) part with air without directly contacting.
4th step, utilizes self-control hot press, by the temperature increase of stainless steel flat plate to 70 DEG C of temperature, maintain 35 minutes, after temperature stabilization (fluctuation is no more than 2 DEG C), the semi-finished product collector that the 3rd step is folded is placed on the centre of two corrosion resistant plates, the pressure of regulator solution cylinder pressure is to 1N/cm
2-1000N/cm
2, depress rapidly, keep pressure 0.1s-15s, pressure relief, collector is taken out and cools to room temperature, namely obtain the finished product required for us: a kind of collector of composite material of conductive film coated metal (or alloy).
Embodiment 2
Below illustrate the making of the collector of the band lug of 120mm*120mm size.
The first step, selects the nickel foil of thickness 0.04mm, and cuts into required shape.
Second step, select the polypropylene of thickness 0.3mm to be the conductive film two panels of base material, conductive additive is wherein super conductive black.The mass fraction of the conductive agent in selected conductive film is 95%.Conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent.Conductive film is cut into the shape needed for collector, conductive film should large 6mm more each than the length and width of metal foil (i.e. nickel foil), to guarantee in the final composite current collector material made except the few part in metal foil lug top, metal foil surface, edge all covers by conductive film, capped metallic member with air without directly contacting.
3rd step, conductive film, metal foil (i.e. nickel foil), conductive film three layers are stacked in " sandwich " mode, and to guarantee in composite current collector material except the few part in metal foil lug top at this, metal foil surface, edge all covers by conductive film, capped metallic member with air without directly contacting.
4th step, utilizes self-control hot press, by the temperature increase of stainless steel flat plate to 390 DEG C of temperature, maintain 45 minutes, after temperature stabilization (fluctuation is no more than 2 DEG C), the semi-finished product collector that the 3rd step is folded is placed on the centre of two corrosion resistant plates, the pressure of regulator solution cylinder pressure is to 1N/cm
2-1000N/cm
2, depress rapidly, keep pressure 0.1s-15s, pressure relief, collector is taken out and cools to room temperature, namely obtain the finished product required for us: a kind of collector of composite material of conductive film coated metal.
Advantage of the present invention:
After metal or alloy being wrapped up with high molecular film material (i.e. conductive film), make aqueous solution battery collector, compare the collector of metal or alloy, there are significant following three advantages:
1. electrochemically resistant corrosion or other corrosive power strong.Below the common metallic element for battery afflux liquid standard electrode potential data in an acidic solution.
Table 1
For Aqueous solution secondary battery, charging latter end, positive electrode (comprising collector) often reaches more than 0.8V (standard electrode potential).Under so high current potential, the common metal such as obvious Fe, Cr, Ni, Cu are difficult to tolerance and oxidation does not occur self.C material is a kind of extraordinary inert electrode material, and the standard electrode potential data of the C electrode in acid solution are difficult to obtain, but rule of thumb, electrode reaction is: C+2H
2o-2e=CO
2↑+2H
2↑ should much larger than 1.29v (H
2the decomposition voltage of O), between possible 3-4V.
Comparison diagram 2 and Fig. 3, can find out, when forward scan is to 0.8V (normal potential is about 1.04V), obviously there is oxidation peak in naked stainless (steel) wire, the nearly 3mA of peak current, and the collector covering the stainless steel substrate of conductive diaphragm occurs without obvious oxidation peak herein.Fig. 4 better illustrates and covers the CV scintigram of stainless (steel) wire collector of conductive film and the contrast figure of the CV scintigram of stainless (steel) wire collector.The abscissa of Fig. 4 is the current potential (unit is V) relative to saturated calomel electrode (SCE).
2. conductive polymer plastic film covering metal or alloy material, make collector, electron conduction does not almost affect.Below the resistivity data of common metal or alloy and conductive film material:
Table 2
| Material | Resistivity (Ω cm) |
| Al | 0.00000265 |
| Ni | 0.00000684 |
| Cu | 0.00000168 |
| Stainless steel | 0.000075 |
| Conducting film | 0.6 |
According to resistance calculations formula: R=ρ * L/S (ρ is the resistivity of material, and L is the path on current delivery direction, and S is the sectional area of the conductor vertical with current delivery direction).Let us be easy to the stainless steel collector of the generous 12cm*12cm*0.03cm of being respectively of calculating one segment length and length and width are thick is respectively: the approximation of the resistance of the collector after the composite conductive thin film of 0.02cm*12cm*12cm.
Table 3
Collector resistance test adopts the test of HIOKI-3554 battery Inner Resistance Tester in Virtual Instrument.Gap between calculated value and measured value mainly cannot comparatively accurately be estimated from the resistance of some contact interfaces.
As can be seen from the above table, at the metal collector surface recombination conductive polymer film of routine, 5% is less than on the impact of the conductivity of collector.
3. conductive film is compounded on metal foil or net material, in Aqueous solution secondary battery, greatly can improve the life-span of battery.This is mainly because of the charging latter end at battery, positive electrode is in higher potential region, now often self there is oxidation reaction in plus plate current-collecting body, collector and the internal resistance of electrode active material contact site is caused constantly to increase, the depth of discharge of active material constantly shoals, and the capacity of battery decays to life termination rapidly.Adopt composite current collector of the present invention, metal base wraps up by conductive polymer film completely, and metal no longer directly contacts with electrolyte, and the electrochemical corrosion of metal base slows down greatly, and battery life is greatly improved.
Although describe the present invention in the mode of specific embodiment, but be apparent that to those skilled in the art, when not departing from the spirit and scope of the present invention that appended claims limits, can carry out variations and modifications to the present invention, these changes and amendment comprise within the scope of the invention equally.
Claims (10)
1. a composite current collector material, is characterized in that, this composite current collector material is fused into one in " sandwich " mode by conductive film, metal or alloy foil or net material, conductive film three layers.
2. composite current collector material according to claim 1, it is characterized in that, described composite current collector material is except the small part on the lug top of described metal or alloy foil or net material, surface and the edge of described metal or alloy foil or net material are all covered by described conductive film, capped metal or alloy part by conductive film and outside completely isolated.
3. composite current collector material according to claim 1, it is characterized in that, conductive film is dispersed in blowing or drawing and forming after in high molecular polymer by conductive agent, and the thickness of conductive film and collector are grown or wide ratio is not more than 2%, are preferably 0.1%-0.5%; For the current collector material of 120mm*120mm size, the preferred thickness of conductive film is 0.2mm-0.3mm.
4. composite current collector material according to claim 3, it is characterized in that, conductive agent in described conductive film is the material of carbon atoms sp2 hydridization covalent bond, is preferably one or more in graphite powder, super conductive black, CNT (carbon nano-tube), carbon nano-fiber; Be more preferably super conductive black or graphite powder.
5. composite current collector material according to claim 3, it is characterized in that, the high molecular polymer in described conductive film is one or more in polyethylene, polypropylene, polyethylene terephthalate, nylon, polytetrafluoroethylene, fluorocarbon resin; Be preferably polyethylene or polypropylene material.
6. composite current collector material according to claim 3, is characterized in that, the ratio of described conductive agent in described conductive film is 30%-95% by mass.
7. composite current collector material according to claim 1, it is characterized in that, described metal or alloy foil or net material are the one in iron foil, aluminium foil, Copper Foil, filtter gold, titanium foil, nickel foil, stainless steel foil or iron net, aluminium net, copper mesh, brass screen, titanium net, nickel screen, stainless (steel) wire; Be preferably stainless (steel) wire, the thickness of metal or alloy foil or net material and the length of collector or wide ratio are not more than 1%, are preferably 0.01%-0.05%; For the current collector material of 120mm*120mm size, the preferred thickness range of metal material is 0.025mm-0.045mm.
8. composite current collector material according to claim 1, it is characterized in that, the thickness of described conductive film and the thickness ratio of described metal or alloy foil or net material are 50.1%-2000%, are preferably 80%-400%.
9. composite current collector material according to claim 1, is characterized in that, conductive film, metal or alloy foil or net material, conductive film are fused into one by the mode of heating pressurization.
10. the preparation method of composite current collector material according to any one of claim 1-9, it is characterized in that, conductive film, metal or alloy foil or net material, conductive film three layers are stacked in " sandwich " mode, the pressing plate heated with two or briquetting pressing form, the heating temperature range of its center platen or briquetting is 70 DEG C-390 DEG C, and pressure range is 1N/cm
2-1000N/cm
2, hot pressing time scope is 0.1s-15s.
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| CN114551786A (en) * | 2022-02-07 | 2022-05-27 | 大连中比动力电池有限公司 | Large-size cylindrical lithium ion secondary battery pole piece and preparation method thereof |
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