CN108417843A - A kind of porous aluminum collector inhibiting sodium dendrite - Google Patents
A kind of porous aluminum collector inhibiting sodium dendrite Download PDFInfo
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- CN108417843A CN108417843A CN201810155115.6A CN201810155115A CN108417843A CN 108417843 A CN108417843 A CN 108417843A CN 201810155115 A CN201810155115 A CN 201810155115A CN 108417843 A CN108417843 A CN 108417843A
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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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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0438—Processes of manufacture in general by electrochemical processing
- H01M4/044—Activating, forming or electrochemical attack of the supporting material
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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
- H01M4/70—Carriers or collectors characterised by shape or form
- H01M4/80—Porous plates, e.g. sintered carriers
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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
Abstract
The present invention relates to a kind of porous aluminum collectors inhibiting sodium dendrite.Porous aluminum is the three-dimensional porous structure closely arranged；Thickness is 1nm~3000 μm；Pore size should be 1nm~1000 μm；Porous structure collector hole density is 10~106Mesh.Porous structure collector is prepared by chemical etching method, electrochemistry removal alloying method, electrochemical deposition method or metal sintering method.Compared to the conventional collector such as copper, iron, titanium, nickel, the quality of aluminium is lighter, is conducive to the lightweight of battery.Especially the special construction of porous aluminum can deposit for metallic sodium and provide more active sites, so that metal ion profile is more uniform, while the densely arranged pore passage structure of porous aluminum can alleviate volume change of the metallic sodium in depositing course of dissolution by confinement effect.This porous aluminum collector is applied to sodium sky battery, sodium vanadium phosphate sode cell and " no sodium " sodium titanium disulfide battery, and performance, which has, significantly to be improved.
Description
Technical field
The present invention relates to battery technology fields, more particularly to a kind of porous aluminum collector inhibiting sodium dendrite.
Background technology
Lithium ion battery have high specific energy, high voltage, high efficiency, without self discharge, memory-less effect many advantages, such as, thus
It is widely studied and applied in recent years, but abundance is only 17~20mg g to lithium metal on earth-1, metallic sodium conduct
It is only second to the second light metallic element of lithium, abundance is up to 2.3%~2.8%, 4~5 orders of magnitude higher than lithium.From this angle
For, sodium is applied to technical field of energy storage, there is the great potential and advantage of commercialization and sustainable use.
Sodium-ion battery can be used in due to its cost advantage on large-scale energy storage device, thus be received in recent years
The extensive concern of researcher.However, since its energy density is not high enough, it is difficult to meet requirement of the society to high energy storage device.Cause
This, many researchers focus on sight on sodium metal battery.However, as lithium metal battery, sodium metal battery is equally deposited
In dendrite problems.Since metallic sodium is in depositing course of dissolution, the uneven distribution of charge over time and space results in gold
The inhomogeneous growth for belonging to sodium, with the increase of cycle-index, diaphragm may can be pierced through or be formed " dead by growing too fast sodium dendrite
Sodium " in turn results in the lasting reduction of battery short circuit or coulombic efficiency.In addition, the body due to metallic sodium in depositing course of dissolution
Product variation, it is totally unfavorable for stablizing solid liquid interface (SEI), the lasting consumption of electrolyte can be caused, and then reduce following for battery
The ring service life.
Invention content
In order to solve the deficiencies in the prior art, the present invention creatively uses collector of the porous aluminum as metallic sodium, makes
Metallic sodium is more uniform in the distribution of cyclic process intermediate ion, and then can prevent the generation of sodium dendrite.Pass through porous aluminum simultaneously
Pore passage structure can alleviate volume change of the metallic sodium in depositing course of dissolution, play the role of stable solid liquid interface.
Technical scheme is as follows：
A kind of porous aluminum collector inhibiting sodium dendrite.
Porous aluminum is the three-dimensional porous structure closely arranged；Thickness is 1nm~3000 μm；Pore size should be 1nm~
1000μm；Porous structure collector hole density is 10~106Mesh.
Porous structure collector passes through chemical etching method, electrochemistry removal alloying method, electrochemical deposition method or metal sintering
Method is prepared.
Porous aluminum collector is applied to sodium sky battery, sodium-vanadium phosphate sode cell or " no sodium " sodium-titanium disulfide battery.
Wherein in chemical etching method, etching liquid is hydrochloric acid, sulfuric acid, sodium hydroxide, nitric acid, phosphoric acid, hydrogen peroxide, ammonium chloride
At least one of solution, metabisulfite solution, hypo solution, vulcanized sodium, salpeter solution, concentration range 0.1mol/L
~6mol/L.
In chemical etching method, current density is 0.005 μ A cm-2~100mA cm-2, the duration is 1s~for 24 hours, work
Electrode is aluminium foil, is platinized platinum to electrode, by applying voltage electroetching.
It is described as follows：
The present invention relates to a kind of porous aluminum collectors that can inhibit sodium dendrite, it is characterised in that the three-dimensional closely arranged is more
Pore structure.Disperse Sodium distribution by three-dimensional open-framework, realizes the homoepitaxial of metallic sodium.Simultaneously by densely arranged
Pore passage structure alleviates volume change of the metallic sodium in depositing course of dissolution.
As a kind of improvement for the porous aluminum collector that can inhibit sodium dendrite of the present invention, the porous structure collector can
To improve the deposition of metallic sodium by adjusting its thickness, thus, thickness is 1nm~3000 μm.
As a kind of improvement for the porous aluminum collector that can inhibit sodium dendrite of the present invention, the porous structure collector can
To improve the depositing behavior of metallic sodium by adjusting pore size, enough space metals are difficult to as aperture is too small
Sodium, aperture is too big to reduce electronic contact again, weaken the confinement effect in metal sodian deposition course of dissolution, therefore its pore size
It should be 1nm~1000 μm.
As a kind of improvement for the porous metals aluminium collector that can inhibit sodium dendrite of the present invention, the porous structure afflux
Body can be prepared by chemical etching method, electrochemistry removal alloying method, electrochemical deposition method or metal sintering method.
As a kind of improvement for the porous aluminum collector that can inhibit sodium dendrite of the present invention, the porous structure collector its
The range of hole density is 10~1010Mesh.The difference of hole density determines the distributed effect of sodium ion, while the size of hole density
Determine the power that collector acts on metallic sodium confinement.
Compared to traditional technology, the invention has the characteristics that, compared to the conventional collector such as copper, iron, titanium, nickel, the quality of aluminium
It is lighter, be conducive to the lightweight of battery.Especially the special construction of porous aluminum can deposit for metallic sodium and provide more active sites
Point so that metal ion profile is more uniform, while the densely arranged pore passage structure of porous aluminum can be alleviated by confinement effect
Volume change of the metallic sodium in depositing course of dissolution.Based on the above advantage, electricity can be substantially improved using porous aluminum collector
The energy density and cyclical stability in pond.In addition, can the microscopic appearance of the porous current collector effectively inhibit sodium dendrite extremely to it
Close it is important, as its aperture, aperture density will all influence the depositing behavior of metallic sodium.Meanwhile the thickness of porous aluminum is also to metallic sodium
Deposition constitute influence.
This porous aluminum collector is applied to sodium sky battery, sodium-vanadium phosphate sode cell and " no sodium " sodium-curing by us
Titanium battery, performance, which has, significantly to be improved.
Description of the drawings
Fig. 1 is porous aluminum schematic diagram.
Fig. 2 is the porous aluminum obtained with 6% salt acid etch.
Fig. 3 is that porous aluminum honeycomb and the SEM of normal aluminium foil cathode difference sodian deposition amount scheme, wherein (a) is negative for porous aluminum
Pole (b) is normal aluminium foil cathode.
Specific implementation mode
The present invention relates to a kind of porous aluminum collectors inhibiting sodium dendrite, it is characterised in that the three-dimensional porous knot closely arranged
Structure.Disperse Sodium distribution by three-dimensional open-framework, realizes the homoepitaxial of metallic sodium.Pass through densely arranged duct simultaneously
Structure alleviates volume change of the metallic sodium in depositing course of dissolution.
It is further illustrated the present invention with reference to embodiment, but the scope of protection of present invention is not limited to implement
The range of example statement.
Embodiment 1
In the glove box full of argon gas, using porous aluminum and the normal aluminium foil of comparison as cathode, the structure of porous aluminum is
The pore structure of perforation, aperture 200nm, porous aluminum thickness are 100 μm, and the hole density of porous aluminum is 1000 mesh, and metallic sodium is made
For reference electrode and to electrode, diaphragm uses Celgard 2325, is assembled into button cell, deposit with blue electricity/dissolve reality
It tests.Electrolyte used is made of certain density sodium salt and organic solvent in the present invention.Sodium salt is sodium hexafluoro phosphate, solvent two
Glyme.Deposition current is 0.1~50mA cm-2, deposition capacity is 0.5~20mAh cm-2, when current density is
0.5mA cm-2, capacity is 0.5mAh cm-2When, after cycle 1000 hours, still there is the stagnant ring of small voltage, and it is common
The circulating battery that aluminium foil is assembled into causes voltage is stagnant to increase sharply less than 60 circles due to depositing uneven.When current density is
0.5mA cm-2, capacity is 0.25mAh cm-2When, the average coulombic efficiency of 1000 circle of cycle still can be maintained at 99.9%, work as electricity
Current density is 1.0mA cm-2, capacity is 0.5mAh cm-2When, the average coulombic efficiency of 1000 circle of cycle still can be maintained at
99.8%, and normal aluminium foil, under above two test condition, in the case where cycle is less than 200 circle, coulombic efficiency is down to
60% less than.
Embodiment 2
For this example unlike example 1 so sodium salt is sodium perchlorate, solvent is ethylene carbonate and diethyl carbonate
Volume ratio 1：1,.When current density is 0.25mA cm-2When, deposition dissolution time control is 15 minutes, after 1200 circle of cycle,
Still there is smaller voltage hysteresis.
Embodiment 3
By the battery after having deposited sodium or repeatedly having recycled unlike example 1, is dismantled in glove box, cathode is carried out
Processing is dried in flushing, observes metallic sodium deposition morphology with cold field emission scanning electron microscope (SEM), as shown in Figure 2.Compared to general
Logical aluminium foil, porous aluminum sodian deposition are obviously improved, and deposition is more uniform.
Embodiment 4
By depositing dosed quantities sodium metal unlike example 1, porous aluminum honeycomb and common aluminum honeycomb are in glove box
It dismantles, with Super P air electrodes, is assembled into button cell and carries out full battery test, positive and negative anodes capacity matches by a certain percentage,
Wherein air cell test carries out in pure oxygen environment.Sodium salt used in sodium-air battery is NaTFSI, NaPF6, NaClO4In one
Kind, solvent is diethylene glycol dimethyl ether, tetraethylene glycol dimethyl ether, ethylene carbonate, a kind of in diethyl carbonate.Due to the knot of porous aluminum
Structure advantage, these battery cathode stability are obviously improved, thus are greatly changed compared to normal aluminium foil battery life
It is kind.The air cell that porous aluminum is assembled into is existed in the still apparent decaying of 200 circle of cycle by the battery that normal aluminium foil is assembled into
After cycle is less than 30 circles, capacity drastically declines.
Embodiment 5
By depositing dosed quantities sodium metal unlike example 1, porous aluminum honeycomb and common aluminum honeycomb are in glove box
It dismantles, with Na3V2(PO4)3Anode is assembled into button cell and carries out full battery test, and positive and negative anodes capacity matches by a certain percentage.
Sodium salt used is NaTFSI, NaPF6, NaClO4Middle one kind, solvent are diethylene glycol dimethyl ether, tetraethylene glycol dimethyl ether, ethylene carbonate
Ester, it is a kind of in diethyl carbonate.Due to the structural advantage of porous aluminum, these battery cathode stability are obviously improved, because
And it is greatly improved compared to normal aluminium foil battery life.The battery being assembled by porous aluminum still has after 350 circle cycles
60mAh g-1Capacity, and use the collector of normal aluminium foil after 150 circle of cycle, capacity i.e. drastically near 30mAh g-1。
Embodiment 6
Use the titanium disulfide of pre- sodium as anode unlike example 1, porous aluminum or normal aluminium foil are as cathode, group
" no sodium " negative battery is dressed up, sodium salt used is NaTFSI, NaPF6, NaClO4Middle one kind, solvent are diethylene glycol dimethyl ether,
Tetraethylene glycol dimethyl ether, ethylene carbonate are a kind of in diethyl carbonate.Compared to normal aluminium foil, porous aluminum is used to be assembled into as cathode
Battery life it is longer, stability is more preferable." no sodium " negative battery being made of porous aluminum, current density are 0.1mA cm-2,
After 200 circle of cycle, still there is preferable capacity to keep, and use " no sodium " negative battery of normal aluminium foil, is followed less than 50 circles
After ring, capacity drastically declines.
Embodiment 7
The porous aluminum collector, can be obtained by chemical etching method, and the aluminium foil cleaned is put into 6% dilute salt of concentration
In acid, platinum plate electrode is used as to electrode, and current density is 100mA cm-2, the duration is 50 seconds, and obtained porous aluminum uses
The method of example 1 is used as sodium metal battery collector, when current density is 0.5mA cm-2, capacity is 0.5mAh cm-2
When, after cycle 500 hours, still maintain preferable cyclical stability.
Embodiment 8
The porous aluminum collector, can be obtained by chemical etching method, and the aluminium foil cleaned is put into 6% dilute salt of concentration
In acid, platinum plate electrode is used as to electrode, and current density is 0.05 μ A cm-2, the duration is obtained porous aluminum after 10 hours,
Sodium metal battery collector is used as using the method for example 1, when current density is 10mA cm-2, capacity is 1mAh cm-2
When, after cycle 100 hours, still maintain preferable cyclical stability.
Embodiment 9
The porous aluminum collector, can be obtained by chemical etching method, and the aluminium foil cleaned is put into 6% dilute salt of concentration
In acid, platinum plate electrode is used as to electrode, and current density is 200 μ A cm-2, the duration is two hours, and obtained porous aluminum is adopted
It is used as sodium metal battery collector with the method for example 1, when current density is 3mA cm-2, capacity is 6mAh cm-2When,
After cycle 200 hours, preferable cyclical stability is still maintained.
Embodiment 10
Unlike example 1-4, the aperture of porous aluminum is 10nm, and the thickness of porous aluminum is to 3000 μm, the hole of porous aluminum
Density is 106Mesh, using metallic sodium piece as to electrode, electrolyte NaPF6The deposition of in Diglyme, metallic sodium can increase
It is added to 20mAh cm-2, repeatedly without apparent dendrite after cycle.
Embodiment 11
Unlike example 1-4, the aperture of porous aluminum is 300nm, and the thickness of porous aluminum is to 3000 μm, the hole of porous aluminum
Density is 5000 mesh, using metallic sodium piece as to electrode, electrolyte NaPF6In Diglyme, the deposition of metallic sodium can be with
Increase to 20mAh cm-2, repeatedly without apparent dendrite after cycle.
Embodiment 12
Unlike example 1-4, the aperture of porous aluminum is 1000nm, the thickness of porous aluminum to 1200 μm, porous aluminum
Hole density is 100 mesh, using metallic sodium piece as to electrode, electrolyte NaPF6In Diglyme, the deposition of metallic sodium can be with
Increase to 120mAh cm-2, repeatedly without apparent dendrite after cycle.
Embodiment 13
Unlike example 10-12, the aperture of porous aluminum is 500nm, the thickness of porous aluminum to 300 μm, porous aluminum
Hole density is 2000 mesh, using metallic sodium piece as to electrode, electrolyte NaPF6In EC/DEC, the deposition of metallic sodium can be with
Increase to 10mAh cm-2, repeatedly without apparent dendrite after cycle.
Embodiment 14
Unlike example 10-12, the aperture of porous aluminum is 500nm, the thickness of porous aluminum to 100 μm, porous aluminum
Hole density is 6000 mesh, using metallic sodium piece as to electrode, electrolyte NaClO4The deposition of in EC/DEC, metallic sodium can
To increase to 30mAh cm-2, repeatedly without apparent dendrite after cycle.
The above is merely a preferred embodiment of the present invention, and is not intended to limit embodiment of the present invention, and this field is general
Logical technical staff's central scope according to the present invention and spirit can very easily carry out corresponding flexible or modification, therefore
Protection scope of the present invention should be subject to the protection domain required by claims.
In conclusion the collector by using porous aluminum as metallic sodium cathode, can significantly improve metallic sodium
Deposition problems prevent the generation of sodium dendrite, improve the cyclical stability of metallic sodium cathode.This method simple possible, it is at low cost, it fits
In large-scale application.
Claims (6)
1. a kind of porous aluminum collector inhibiting sodium dendrite.
2. collector as described in claim 1；It is characterized in that porous aluminum is the three-dimensional porous structure closely arranged；Thickness is
1nm~3000 μm；Pore size should be 1nm~1000 μm；Porous structure collector hole density is 10~1010Mesh.
3. collector as described in claim 1；It is characterized in that porous structure collector goes to close by chemical etching method, electrochemistry
Aurification method, electrochemical deposition method or metal sintering method are prepared.
4. collector as described in claim 1；It is characterized in that porous aluminum collector is applied to sodium sky battery, sodium-vanadium phosphate sodium
Battery or " no sodium " sodium-titanium disulfide battery.
5. collector as claimed in claim 3；It is characterized in that in chemical etching method, etching liquid is hydrochloric acid, sulfuric acid, hydroxide
In sodium, nitric acid, phosphoric acid, hydrogen peroxide, ammonium chloride solution, metabisulfite solution, hypo solution, vulcanized sodium, salpeter solution
At least one, concentration range be 0.1mol/L~6mol/L.
6. collector as claimed in claim 3；It is characterized in that in chemical etching method, current density is 0.005 μ A cm-2~
100mA cm-2, the duration is 1s~for 24 hours, and working electrode is aluminium foil, is platinized platinum to electrode, passes through and apply voltage electroetching.
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| CN201810155115.6A CN108417843A (en) | 2018-02-23 | 2018-02-23 | A kind of porous aluminum collector inhibiting sodium dendrite |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112290081A (en) * | 2020-09-22 | 2021-01-29 | 江苏大学 | Manufacturing method of high-energy-density quasi-solid sodium ion battery |
| CN112599784A (en) * | 2020-12-16 | 2021-04-02 | 南京邮电大学 | Porous aluminum alloy current collector and preparation method thereof, and porous aluminum alloy composite sodium negative electrode and preparation method thereof |
| CN112886021A (en) * | 2021-04-30 | 2021-06-01 | 中南大学 | Three-dimensional porous current collector with gradient pore structure and preparation method and application thereof |
| EP3883022A1 (en) * | 2020-03-18 | 2021-09-22 | Kabushiki Kaisha Toshiba | Electrode current collector, electrode, secondary battery, battery pack, vehicle, and stationary power supply |
| CN113451586A (en) * | 2021-05-27 | 2021-09-28 | 天津国安盟固利新材料科技股份有限公司 | Electrode plate of secondary battery, secondary battery and preparation method of secondary battery |
| CN114284505A (en) * | 2021-12-23 | 2022-04-05 | 山东大学 | Porous copper current collector, preparation method thereof and application thereof in zinc/sodium ion battery |
| CN114583174A (en) * | 2022-03-21 | 2022-06-03 | 蜂巢能源科技股份有限公司 | Sodium ion battery and preparation method thereof |
| CN115050968A (en) * | 2022-08-16 | 2022-09-13 | 溧阳紫宸新材料科技有限公司 | High-capacity porous current collector pre-sodium ion battery composite negative electrode and preparation method thereof |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP3883022A1 (en) * | 2020-03-18 | 2021-09-22 | Kabushiki Kaisha Toshiba | Electrode current collector, electrode, secondary battery, battery pack, vehicle, and stationary power supply |
| CN112290081A (en) * | 2020-09-22 | 2021-01-29 | 江苏大学 | Manufacturing method of high-energy-density quasi-solid sodium ion battery |
| CN112599784A (en) * | 2020-12-16 | 2021-04-02 | 南京邮电大学 | Porous aluminum alloy current collector and preparation method thereof, and porous aluminum alloy composite sodium negative electrode and preparation method thereof |
| CN112599784B (en) * | 2020-12-16 | 2022-02-11 | 南京邮电大学 | Porous aluminum alloy current collector and preparation method thereof, and porous aluminum alloy composite sodium negative electrode and preparation method thereof |
| CN112886021A (en) * | 2021-04-30 | 2021-06-01 | 中南大学 | Three-dimensional porous current collector with gradient pore structure and preparation method and application thereof |
| CN113451586A (en) * | 2021-05-27 | 2021-09-28 | 天津国安盟固利新材料科技股份有限公司 | Electrode plate of secondary battery, secondary battery and preparation method of secondary battery |
| CN114284505A (en) * | 2021-12-23 | 2022-04-05 | 山东大学 | Porous copper current collector, preparation method thereof and application thereof in zinc/sodium ion battery |
| CN114583174A (en) * | 2022-03-21 | 2022-06-03 | 蜂巢能源科技股份有限公司 | Sodium ion battery and preparation method thereof |
| CN114583174B (en) * | 2022-03-21 | 2024-03-26 | 蜂巢能源科技股份有限公司 | Sodium ion battery and preparation method thereof |
| CN115050968A (en) * | 2022-08-16 | 2022-09-13 | 溧阳紫宸新材料科技有限公司 | High-capacity porous current collector pre-sodium ion battery composite negative electrode and preparation method thereof |
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