CN108963388A - A kind of method improving lithium-air battery energy density and output power and the lithium-air battery based on this method - Google Patents
A kind of method improving lithium-air battery energy density and output power and the lithium-air battery based on this method Download PDFInfo
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- CN108963388A CN108963388A CN201810511277.9A CN201810511277A CN108963388A CN 108963388 A CN108963388 A CN 108963388A CN 201810511277 A CN201810511277 A CN 201810511277A CN 108963388 A CN108963388 A CN 108963388A
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/04—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type
- H01M12/06—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type with one metallic and one gaseous electrode
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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
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9041—Metals or alloys
Abstract
The present invention provides a kind of method for improving lithium-air battery energy density and output power and the lithium-air battery based on this method.This method is that embedding lithium type electrode material is added in air pole on the basis of traditional lithium-air battery structure, forms air/embedding lithium mixed type electrode.The intercalation materials of li ions used has the effect of ORR catalyst, is provided simultaneously with the embedding lithium characteristic of high magnification, is provided simultaneously with the characteristic that operating voltage is lower than ORR response voltage.During discharge, the energy density that lithium sky battery is improved by the ORR catalytic action of embedding lithium type electrode material improves the output power of battery by the embedding lithium characteristic of the high magnification of embedding lithium type electrode material.In addition, intercalation materials of li ions can be returned to original state by spontaneous oxidation reaction, in the case where not needing charging after high power discharge, it is ensured that the renewable use of the power of battery.The present invention especially possesses huge application value in electric car field to demand high specific energy-high power type accumulation power supply field.
Description
Technical field
The invention belongs to lithium-air battery fields, and in particular to improve lithium-air battery energy density and output power.
Background technique
In recent years, with mobile electronic device, smart grid is grid-connected and the fast development of the industries such as new-energy automobile, change
Accumulation power supply, especially lithium ion battery is learned to have been widely used.Currently, high specific energy-high power type accumulation power supply
Exploitation, becomes the focus of scientific circles and industrial circle, the especially application in electric car field.However, even at present most
Good lithium ion battery, energy density also can only achieve 250-300Wh kg-1, still can not meet the needs of future market.
The novel battery that research and development surmount lithium ion battery seems most important.A kind of alternative is exploitation lithia (sky) gas.
The theoretical energy density in lithia (sky) pneumoelectric pond is up to~3500Wh kg-1, the almost current highest lithium-ion electric of energy density
More than 10 times of pond, have shown huge application value, receive global extensive research.A large amount of researchers not
Under slack effort, it is already possible to prepare energy density in 500-800Wh kg-1Monomer lithium-air battery.For example, section in China
Changchun Institute of Applied Chemistry of institute, it has been disclosed that report a kind of energy density and be up to 523Wh kg-1Lithium-air battery.
However, that there are energy efficiencies is low, ORR and OER charge transport capability difference and actual energy density are low for lithium-air battery
The problems such as.In order to solve these problems, a kind of method being widely adopted is to prepare efficient ORR and OER catalyst, passes through drop
Low reaction energy barrier changes reaction microprocess, to reduce the polarization of charge and discharge process.This method can effectively improve electricity
The energy density in pond.But ORR reacting quintessence is a slow process, and lithium sky battery is difficult to discharge under high current, because without
High-power output can be provided.It is corresponding to be, it is equally used as lithium system battery, lithium ion battery can but pass through high-rate type
Electrode material realize high-power output.Such as the LiFePO being widely used4And LiMn2O4.However, their work electricity
(>3.5V) is pressed to be higher than (<the 2.9V) of ORR reaction, it is always preferential to participate in reaction when being applied in lithium-air battery, it can not
Accomplish when needed, to play the role of high-power output.Therefore such material is not suitable for being applied in lithium-air battery.
Summary of the invention
In view of the above-mentioned deficiencies in the prior art, it is an object of the present invention to provide a kind of raising lithium-air battery energy density and defeated
The method of power and the lithium-air battery based on this method are changed simultaneously out with further increasing the energy density of lithium-air battery
The high-power output ability of kind lithium-air battery.
Design of the invention is as follows: on the basis of traditional lithium-air battery structure, (having ORR reaction in air pole
Active material) in embedding lithium type electrode material is added, form air/embedding lithium mixed type electrode.The intercalation materials of li ions used has ORR
The effect of catalyst is provided simultaneously with the embedding lithium characteristic of high magnification, is provided simultaneously with the characteristic that operating voltage is lower than ORR response voltage.?
In discharge process, the energy density of lithium sky battery is improved by the ORR catalytic action of embedding lithium type electrode material, passes through embedding lithium type
The embedding lithium characteristic of the high magnification of electrode material improves the output power of battery.In addition, intercalation materials of li ions can after high power discharge
It is returned to original state by spontaneous oxidation reaction, in the case where not needing charging, it is ensured that the power of battery is renewable
It uses.The present invention especially possesses huge application in electric car field to demand high specific energy-high power type accumulation power supply field
Value.
Based on the above design, the method provided by the invention for improving lithium-air battery energy density and output power are as follows:
Embedding lithium type electrode material is additionally added in air electrode of lithium air battery, forms air/embedding lithium mixed type anode, the embedding lithium type electricity
Pole material has the embedding lithium characteristic of ORR catalytic activity, high magnification and operating voltage is lower than 3 kinds of characteristics of ORR response voltage.
Above scheme, further, the embedding lithium type electrode material are TiO2、TiS2、LiTi2(PO4)3、Li2Ti3O7、
Li4Ti5O12、TiP2O7One of.
Further the method for embedding lithium type electrode material is added in above scheme in air electrode of lithium air battery are as follows: will
The active material of ORR reaction and embedding lithium type electrode material mechanical mixture, and be coated on nickel foam or carbon paper collector, it is formed empty
Gas/embedding lithium mixed type electrode；Or the active material of ORR reaction and embedding lithium type electrode material are respectively coated in nickel foam or carbon paper
Collector two sides form air/embedding lithium mixed type electrode, and make in battery envelope group ORR reactivity material close to air side,
Embedding lithium type electrode material is close to diaphragm side.
Above scheme, further, the active material of the ORR reaction select graphene, SP carbon, KB carbon, carbon nanotube
And one of carbon fiber.
Air/embedding lithium mixed type electrode with above method production is the lithium-air battery of anode, is mixed by air/embedding lithium
Type anode, cathode, diaphragm, electrolyte assembling are constituted；Cell internal environment is purity oxygen environment, or includes the inertia of oxygen
Gaseous environment, or anode are in the environment containing oxygen.When the air/embedding lithium mixed type anode is reacted using ORR
Active material and embedding lithium type electrode material are respectively coated when the method production of nickel foam or carbon paper collector two sides, in assembling
In battery, the material side of reactivity containing ORR contains embedding lithium type electrode material side towards diaphragm towards air.
Above-mentioned lithium-air battery, the cathode are the alloying material of lithium metal or embedding lithium type electrode material such as graphite or lithium
Material such as silicon.
Above-mentioned lithium-air battery, the electrolyte are 1mol L-1LiTFSI-DME、1mol L-1LiTFSI-TEGDME、
1mol L-1One of LiTFSI-DMSO.
Above-mentioned lithium-air battery, diaphragm are the polymer separators that fibreglass diaphragm or lithium ion battery use.
Above-mentioned lithium-air battery, operating voltage range 1.0-4.5V.
Conceive according to the present invention, when lithium-air battery need to only utilize the high power characteristic of intercalation materials of li ions, and in order to avoid embedding
When lithium material is passivated by ORR reaction product, embedding lithium type electrode material is coated on aluminium foil or foamed nickel current collector surface, is used as single
Only high power anode.When assembled battery, the air cathode of high power anode and lithium sky battery is respectively placed in battery cathode two
Side forms the lithium-air battery structure of a cathode, two anodes.It is the embedding lithium electrode material, air pole ORR active material, negative
Pole material, electrolyte and diaphragm are listed substance above.In cell operations, air cathode provides high-energy output, embedding
Lithium material anode provides high-power output.
The working mechanism of lithium-air battery of the present invention based on blended anode: in low discharging current, since ORR is anti-
The operating voltage answered is higher than the operating voltage of embedding lithium type electrode material, therefore ORR preferentially plays the role of energy output, to protect
The characteristic of lithium air electricity high specific energy is demonstrate,proved.Simultaneously as intercalation materials of li ions has the function of ORR catalyst, therefore it can be improved ORR's
Discharge voltage and discharge capacity further increase the energy density of battery.When discharging under high current, since ORR is slow
Slow dynamics is unable to satisfy high-power output, and voltage rapidly drops to the operating voltage range of embedding lithium type electrode material at this time.
Intercalation materials of li ions provides high-power output for by its outstanding high power performance at this time.After the completion of high-power output, in addition to
It is outer that ORR reaction continues to provide energy output, due to embedding lithium type electrode material react with ORR between there are voltage differences, thus can lead to
It crosses and O2Spontaneous oxidation reaction makes it be restored to initial state, it is ensured that the recycling of the material.In every case above-mentioned work is used
The lithium-air battery that mechanism is prepared belongs to the protection category of this patent.
Compared with prior art, the invention has the following advantages:
1. the present invention is on the basis of lithium-air battery high specific energy characteristic, for the deficiency of its power-performance, by lithium ion
The electrode material (embedding lithium type electrode material) for having high-rate characteristics in battery has been integrated into lithium sky battery system, is prepared
The lithium-air battery for having both high specific energy and high power performance can be used for demand high specific energy-high power type accumulation power supply field, especially
In electric car field.
2. based on thought of the invention, using lithium as negative electrode material, 1mol L-1LiTFSI-TEGDME is electrolyte, and SP carbon is
The active material of ORR reaction, bronze type TiO2(TiO2(B)) it is high-rate type intercalation materials of li ions, constructs with O2/TiO2(B) it mixes
Close the lithium-air battery of anode.It is as shown in Figure 1 to test obtained energy-power figure.There it can be seen that having O2/TiO2(B)
Not only energy density is higher than based on traditional O the lithium-air battery of blended anode2(SP) positive lithium-air battery, power density
Also it has obtained greatly being promoted.
Detailed description of the invention
Fig. 1 is with O2(SP)/TiO2(B) lithium-air battery of blended anode, with traditional O2(SP) positive lithium is empty
Pneumoelectric pond and with TiO2It (B) is the lithium ion battery of anode, the energy-power comparison diagram of 3 kinds of batteries.
Fig. 2 (a) is with traditional O2(SP) positive lithium-air battery (b) is O2(SP)/TiO2(B) blended anode
Lithium-air battery, the constant-current discharge curve under different current densities.
Fig. 3 is the schematic diagram of lithium-air battery described in embodiment 1.
Specific embodiment
It is described further below by specific embodiment to of the present invention.Following embodiment is to be thought based on the present invention
Think, the experimental result of the selectivity of given 3 kinds different battery structures, but scope of the presently claimed invention is not limited to
This.According to essential characteristic and theoretical foundation of the invention as defined in the claims, as long as those skilled in the art institute into
Capable any improved form, belongs to scope of the presently claimed invention.
Embodiment 1
Cathode is lithium metal, and ORR reactivity material is SP carbon, and the embedding lithium type electrode material of high magnification is TiO2(B), it is electrolysed
Liquid is 1mol L-1LiTFSI-TEGDME.SP carbon and TiO2(B) it is respectively coated in plus plate current-collecting body two sides.SP carbon is close to air
Side, TiO2(B) close to diaphragm side.
The preparation of SP electrode: active material SP carbon and bonding agent PVDF are matched according to mass ratio for 90:10, in Ma
It is ground uniformly in Nao mortar, then instills suitable NMP and be slurried, place into and disperse 1h in ultrasonic disperser.Obtained mixing
Slurry is coated on foam nickel surface, then in a vacuum drying oven, and SP anode can be obtained in dry 10h at 120 DEG C.
TiO2(B) preparation of electrode: by active material TiO2(B), conductive agent SP carbon, bonding agent PVDF are according to mass ratio
80:10:10 is matched, and grinding uniformly, then instills suitable NMP and is slurried in the agate mortar, places into ultrasonic wave dispersion
Disperse 1h in device.Obtained mixed slurry is coated on foam nickel surface, then in a vacuum drying oven, dry 10h at 120 DEG C, i.e.,
Required TiO can be obtained2(B) positive.
O2(SP)/TiO2(B) preparation of mixed electrode: firstly, requiring to obtain the mixed of the pole SP according to the preparation of above-mentioned SP electrode
Slurry, the side coated on nickel foam are closed, then in a vacuum drying oven, dry 10h, is obtaining side carbon containing SP just at 120 DEG C
Pole；Then, according to above-mentioned TiO2(B) preparation of electrode requires to obtain TiO2(B) mixed slurry of pole is coated on the positive other side,
Namely the side not containing SP carbon, then in a vacuum drying oven, dry 10h, can be obtained mixed electrode at 120 DEG C.
With in the preparation of top electrode, either individual SP anode and individual TiO2(B) positive or blended anode
Two sides, the loading capacity of every kind of active material are 1mg cm-2。
By the anode of preparation, cathode lithium, diaphragm glass fibre, electrolyte 1molL-1LiTFSI-TEGDME, in oxygen content and
Water content all < glove box of 0.1ppm in complete the assembling of battery.
Assemble obtained battery standing for 24 hours more than, be then passed through the oxygen that purity is 99.99% in the battery, pressure is
0.02MPa.It is 0.05-6.00mA cm in current densitycathode -2, under conditions of discharge cut-off voltage is 1.0V, test battery
Discharge performance.
It is as shown in Figure 2 to test obtained discharge curve.From the figure, it can be seen that discharge under same current density, O2
(SP)/TiO2(B) capacity of blended anode is apparently higher than pure SP anode.Such as in 0.05mAcmcathode -2Lower electric discharge, mixing
The capacity of electrode is 3.38mAh cmcathode -2, higher than the 2.00mAh cm of traditional SP anodecathode -2.In addition, from figure also
It can be seen that the high rate performance of blended anode is obviously improved.When current density is higher than 2.00mA cmcathode -2When, it passes
The SP anode of system can hardly discharge.But mixed electrode maximum current density can reach 6.00mA cmcathode -2。
It is as shown in Figure 1 to test obtained energy-power data.It can be seen from the figure that O2(SP)/TiO2(B) blended anode
Peak power be 11mW cmcathode -2, it is 2.75 times of ((4mW cm of traditional SP anodecathode -2).Blended anode is most
High-energy density is 8mWh cmcathode -2, higher than the 5mWh cm of traditional SP anodecathode -2.Data fully confirm this hair
Bright feasibility.
Embodiment 2
Cathode is lithium metal, and ORR reactivity material is SP carbon, and high-rate type intercalation materials of li ions is TiO2(B), electrolyte is
1mol L-1LiTFSI-TEGDME.SP carbon and TiO2(B) mechanical mixture is coated on foam nickel surface and prepares blended anode.
The preparation of anode: by active material SP carbon, active material TiO2(B), bonding agent PVDF is 50 according to mass ratio:
40:10 is matched, and grinding uniformly, then instills suitable NMP and is slurried, place into ultrasonic disperser in the agate mortar
Disperse 1h.Obtained mixed slurry is coated on foam nickel surface, then in a vacuum drying oven, and dry 10h, can obtain at 120 DEG C
To required blended anode.
The assembling of battery, the test method and condition of battery are as described for example 1.
It is 10mW cm by the battery maximum power density that the lithium-air battery that the blended anode assembles obtainscathode -2, most
High-energy density is 9mWh cmcathode -2。
Embodiment 3
Cathode is lithium metal, and ORR reactivity material is SP carbon, and high power type intercalation materials of li ions is TiO2(B), electrolyte is
1mol L-1LiTFSI-TEGDME.The electrode being made of SP carbon is as air cathode, by TiO2(B) electrode constituted is as Gao Gong
Rate anode, is respectively placed in lithium piece two sides.
The preparation of SP electrode and TiO2(B) electrode prepare it is as described in Example 1.
By the SP electrode and TiO of preparation2(B) electrode, cathode lithium, diaphragm glass fibre, electrolyte 1mol L-1LiTFSI-
TEGDME, oxygen content and water content all < glove box of 0.1ppm in complete the assembling of battery.The battery is by SP electrode and TiO2
(B) two anode composition of electrode, is respectively placed in the two sides of common cathode lithium.Wherein SP anode-diaphragm-lithium constitutes class lithium air electricity
The structure in pond, TiO2(B) anode-diaphragm-lithium constitutes the structure of Li-like ions battery.
Assemble obtained battery standing for 24 hours more than.Before test, in air pole side, it is passed through the oxygen that purity is 99.99%
Gas, pressure 0.02MPa.When test, two anodes are linked together as a common anode.It tests in current density and is
0.05-6.00mA cmcathode -2, discharge cut-off voltage be 1.0V under conditions of carry out.
Obtained lithium-air battery maximum power density is 12mW cmcathode-2, highest energy density is 7mWh
cmcathode -2。
Claims (9)
1. a kind of method for improving lithium-air battery energy density and output power, it is characterised in that in air electrode of lithium air battery
It is middle that embedding lithium type electrode material is added, air/embedding lithium mixed type anode is formed, the embedding lithium type electrode material has ORR catalysis and lives
Property, the embedding lithium characteristic of high magnification and operating voltage be lower than 3 kinds of characteristics of ORR operating voltage.
2. according to raising lithium-air battery energy density described in claim 1 and the method for output power, it is characterised in that described embedding
Lithium type electrode material is TiO2、TiS2、LiTi2(PO4)3、Li2Ti3O7、Li4Ti5O12、TiP2O7One of.
3. the method according to claim 1 or claim 2 for improving lithium-air battery energy density and output power, which is characterized in that
The method of embedding lithium type electrode material is added in air electrode of lithium air battery are as follows: by the active material of ORR reaction and embedding lithium type electricity
The mixing of pole material mechanical, and be coated on nickel foam or carbon paper collector, form air/embedding lithium mixed type electrode；Or it is ORR is anti-
The active material and embedding lithium type electrode material answered are respectively coated in nickel foam or carbon paper collector two sides, and it is mixed to form air/embedding lithium
Mould assembly electrode, and make ORR reactivity material close to air side in battery assembly, embedding lithium type electrode material is close to diaphragm
Side.
4. improving the method for lithium-air battery energy density and output power according to claim 3, it is characterised in that described
The active material of ORR reaction is one of graphene, SP carbon, KB carbon, carbon nanotube and carbon fiber.
5. a kind of method for improving lithium-air battery energy density and output power, is characterized in that, applied with embedding lithium type electrode material
It is overlying on aluminium foil or foamed nickel current collector surface, is used alone as high power anode；It is when assembled battery, high power anode and lithium is empty
The air cathode of battery is respectively placed in battery cathode two sides, forms the lithium-air battery structure of a cathode, two anodes.
6. air/embedding lithium mixed type electrode with the production of claim 1 the method is the lithium-air battery of anode, feature exists
In battery is made of air/embedding lithium mixed type anode, cathode, diaphragm, electrolyte assembling, and cell internal environment is pure oxygen compression ring
Border, or include the inert gas environment of oxygen, or anode is in the environment containing oxygen；When the air/embedding
Lithium mixed type anode is respectively coated using ORR reactivity material and embedding lithium type electrode material in nickel foam or carbon paper collector two
When the method production of side, in the battery of assembling, the material side of reactivity containing ORR contains embedding lithium type electrode material side towards air
Towards diaphragm.
7. lithium-air battery according to claim 6, it is characterised in that the cathode is lithium metal or embedding lithium type electrode material
The alloying material of material or lithium.
8. lithium-air battery according to claim 6, it is characterised in that the electrolyte is 1mol L-1LiTFSI-DME、
1mol L-1LiTFSI-TEGDME、1mol L-1One of LiTFSI-DMSO.
9. lithium-air battery according to claim 6, it is characterised in that the diaphragm is fibreglass diaphragm or lithium-ion electric
The polymer separators that pond uses.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109742489A (en) * | 2019-02-02 | 2019-05-10 | 北京师范大学 | A kind of lithium-oxygen/air battery and preparation method thereof |
| CN109860958A (en) * | 2019-02-02 | 2019-06-07 | 北京师范大学 | A kind of lithium-carbon dioxide battery and preparation method thereof |
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| US7147967B1 (en) * | 2003-07-29 | 2006-12-12 | The United States Of America As Represented By The Secretary Of The Army | Cathode for metal-oxygen battery |
| CN101960664A (en) * | 2008-12-25 | 2011-01-26 | 丰田自动车株式会社 | Lithium air battery |
| US20120180945A1 (en) * | 2009-09-10 | 2012-07-19 | Battelle Memorial Institute | Air electrodes for high-energy metal air batteries and methods of making the same |
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| US7147967B1 (en) * | 2003-07-29 | 2006-12-12 | The United States Of America As Represented By The Secretary Of The Army | Cathode for metal-oxygen battery |
| CN101960664A (en) * | 2008-12-25 | 2011-01-26 | 丰田自动车株式会社 | Lithium air battery |
| US20120180945A1 (en) * | 2009-09-10 | 2012-07-19 | Battelle Memorial Institute | Air electrodes for high-energy metal air batteries and methods of making the same |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109742489A (en) * | 2019-02-02 | 2019-05-10 | 北京师范大学 | A kind of lithium-oxygen/air battery and preparation method thereof |
| CN109860958A (en) * | 2019-02-02 | 2019-06-07 | 北京师范大学 | A kind of lithium-carbon dioxide battery and preparation method thereof |
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Application publication date: 20181207 |