CN108933310A - A kind of high capacity high power type lithium ion/air hybrid battery system - Google Patents
A kind of high capacity high power type lithium ion/air hybrid battery system Download PDFInfo
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- CN108933310A CN108933310A CN201810511225.1A CN201810511225A CN108933310A CN 108933310 A CN108933310 A CN 108933310A CN 201810511225 A CN201810511225 A CN 201810511225A CN 108933310 A CN108933310 A CN 108933310A
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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
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
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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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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
- H01M2250/00—Fuel cells for particular applications; Specific features of fuel cell system
- H01M2250/20—Fuel cells in motive systems, e.g. vehicle, ship, plane
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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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- 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
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
The present invention provides a kind of high capacity high power type lithium ion/air hybrid battery system and achievees the effect that maximize favourable factors and minimize unfavourable ones to the performance of the two by lithium ion battery and lithium-air battery construction and integration hybrid battery system.By the high capacity feature of lithium-air battery ORR, to make up the low deficiency of lithium ion battery energy density.Feature high using air pole active material specific surface area simultaneously, further improves the output power of lithium ion battery.Using anode active material of lithium ion battery have be higher than ORR reaction operating voltage (>3.0V) and outstanding cycle performance, increase lithium ion battery access times, effectively compensate for the problem of lithium-air battery cycle performance deficiency, while being that the use of lithium-air battery provides a method.The battery system has both the advantages of lithium ion battery and lithium-air battery, realizes in performance and maximizes favourable factors and minimizes unfavourable ones to lithium ion battery and lithium-air battery, obtains a kind of battery system with high capacity high power.
Description
Technical field
The invention belongs to lithium ion battery and lithium-air battery field, in particular to a kind of lithium ion/air hybrid battery
System.
Background technique
With the development of society, chemical energy source constantly consumes, while bringing many convenient, problem of environmental pollution becomes
It obtains increasingly severe.In addition to developing clear energy sources come other than solving the problems, such as this, a kind of effective mode is using electrochmical power source.Since
After lithium ion battery enters consumption market within 1991, in mobile electronic device, smart grid is grid-connected and new-energy automobile etc.
Field is widely used.Especially in recent years, under policies of various countries A clear guidance, electric car has obtained swift and violent hair
Exhibition, has shown urgent demand to high specific energy-high power type lithium ion battery, thus becomes scientific circles and industrial circle
Research focus.However limited by anode material for lithium-ion batteries self-capacity is low, the energy density of lithium ion battery is difficult to reach
To very high numerical value.For example, even lithium ion battery best at present, energy density also can only achieve 250-300Wh
kg-1, still can not meet the needs of future market.Therefore, the novel battery that research and development surmount lithium ion battery seems most important.
A kind of mode is exploitation lithium-air battery, theoretical energy density up to~3500Wh kg-1, almost the 10 of lithium ion battery
More times, huge application value has been shown, thus has received in the whole world and widely pays close attention to.Each battery enterprise also one after another will
Its final goal as the development of lithium system battery.Under the unremitting effort of researcher, can it prepare in the world at present
Energy density is in 500-800Whkg-1Lithium sky full battery.China also achieves good achievement in the field.For example, the Chinese Academy of Sciences
The Zhang Xinbo team of Changchun Institute of Applied Chemistry has disclosed and reports a kind of energy density and be up to 523Wh kg-1Lithium-air battery.
However, lithium-air battery still remains, charge-discharge energy low efficiency, ORR and OER charge transport capability are poor, actually put
The problems such as capacitance is low, electrolyte easily decomposes and carbon is just extremely unstable.In addition, in order to improve the charge transfer energy of charge and discharge process
Power, it usually needs use noble metal catalyst, such as Ag, Ru, Au, Pt and Pd etc..High cost also limits lithium air electricity
The extensive use in pond.In author, it is based on existing science and technology, following within considerable time, pure lithium air
Battery is to be difficult to obtain practical application.Therefore, how the characteristic of its high specific energy is applied, while the influence for reducing its unfavorable factor is aobvious
It obtains most important.
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 high capacity high power type lithium ion/air
The advantages of hybrid battery system, which has both lithium ion battery and lithium-air battery, is realized in performance to lithium ion battery
It maximizes favourable factors and minimizes unfavourable ones with lithium-air battery, obtains a kind of battery system with high capacity high power.
Design of the invention is as follows：By lithium ion battery and lithium-air battery construction and integration hybrid battery system, reach pair
The effect that the performance of the two is maximized favourable factors and minimized unfavourable ones.It is close to make up lithium ion battery energy by the high capacity feature of lithium-air battery ORR
Spend low deficiency.Feature high using air pole active material specific surface area simultaneously, further improves the output of lithium ion battery
Power.Using anode active material of lithium ion battery have be higher than ORR reaction operating voltage (>3.0V) and outstanding cyclicity
Can, increase lithium ion battery access times, effectively compensates for the problem of lithium-air battery cycle performance deficiency, while empty for lithium
The use in pneumoelectric pond provides a method.The present invention is mainly characterized by：By lithium-air battery part, improve indirectly
Lithium ion battery energy density and output power；By lithium ion battery part, lithium-air battery poor circulation, energy are reduced
Influence of the unfavorable factors such as amount efficiency is low and electrode and electrolyte liquor is unstable to entire battery system, has reached the effect maximized favourable factors and minimized unfavourable ones
Fruit.A kind of practical way is provided simultaneously for the use of lithium-air battery.
High capacity high power type lithium ion of the present invention/air hybrid battery system, is in traditional lithium ion battery
On the basis of structure, an air cathode is added；Or be connected in parallel lithium ion battery and lithium-air battery, to constitute lithium
Ion/air hybrid battery system.Anode active material of lithium ion battery need to have higher than ORR reaction operating voltage (>
3.0V), outstanding cycle performance.Air pole active material need to have high ORR reaction discharge capacity, have high specific surface
Product has the ability for capableing of oxygenolysis ORR discharging product during the charging process.Specific structure is as follows：
Negative grade is shared including a lithium ion anode, an air cathode and one, it is empty by lithium ion battery part and lithium
Gas battery portion composition, lithium ion battery part by lithium ion cell positive-lithium-ion battery electrolytes-lithium ion battery every
Film-is shared cathode and is constituted, and lithium-air battery part is shared by air cathode-lithium-air battery electrolyte-diaphragm for lithium-air battery-
Cathode is constituted, and wherein lithium ion anode links together with air cathode short circuit, shares a cathode；
Or be made of individual lithium ion battery and lithium-air battery parallel connection, connection type is that cathode links together
As the cathode of hybrid battery system, anode is connected together as the anode of hybrid battery system.
In above-mentioned technical proposal of the invention, commercialized positive electrode is can be used in anode material for lithium-ion batteries, such as
LiCoO2、LiFePO4、LiMn2O4And LiNi1-x-yCoxMnyO2、LiNi0.8Co0.15Al0.05O2One of ternary material.
In above-mentioned technical proposal of the invention, air cathode active material need to have high ORR discharge capacity, have height
Specific surface area, the ability with oxygenolysis ORR discharging product namely material have sufficiently accommodate ORR discharging product energy
Power and ORR and OER catalytic activity.Such as the composite material, graphene and transition metal oxide of graphene, graphene and noble metal
Composite material etc..It is further preferred that the composite material of such as graphene and Ru, Pt, Au, Pd substance, graphene and MnO2、
Co3O4, the substances such as NiO composite material.
In above-mentioned technical proposal of the invention, the electrolyte of lithium ion battery part is the electricity of traditional lithium ion battery
Liquid is solved, such as 1mol L-1LiPF6-EC/DEC.The electrolyte that lithium-air battery part uses is the electrolysis of common lithium-air battery
Liquid, such as 1mol L-1LiTFSI-DME、1mol L-1LiTFSI-TEGDME and 1mol L-1LiTFSI-DMSO etc..
In the inventive solutions, the diaphragm that lithium ion battery part uses is the height that conventional lithium ion battery uses
Molecule diaphragm, such as the serial diaphragm of Celgard.The diaphragm that lithium-air battery part uses be common lithium-air battery every
Film, such as fibreglass diaphragm.
In above-mentioned technical proposal of the invention, lithium ion battery part is a closed system, avoids O2、H2O and CO2
The entrance of equal ambient atmos.Lithium-air battery part or air pole need to be under purity oxygens or inert gas environment containing oxygen
It uses.The operating voltage range of the hybrid battery is 2.3-4.4V.
Lithium ion of the present invention/air hybrid battery system, in low discharging current, due to lithium ion cell positive
Operating voltage is higher than the operating voltage of air cathode ORR, therefore lithium ion anode preferentially provides energy output.When it is unable to satisfy
When outside energy demand, system voltage will drop to the voltage of ORR, and air pole starts to provide energy release at this time.Due to ORR
Capacity be much higher than li-ion electrode materials, thus efficiently solve the problems, such as that lithium ion battery energy density is low.Another party
Face, air pole can be mentioned due to the feature with high-specific surface area by the charge electric double layer capacity and ORR fake capacitance on its surface
For high-power output, capacitance pole use can be used as.When discharging under high current, if li-ion electrode is unable to satisfy external power
When demand, air pole can provide high-power output by its surface capacitance.When turning again to low discharging current, in addition to lithium ion
Electrode is again supplied to outside outside energy output, since there are potentials between the air pole after li-ion electrode and high power discharge
Difference, therefore li-ion electrode will charge to air pole, be restored to it to a new state, to ensure that its renewable makes
With.In practical applications, by preferentially participating in the characteristic of electric discharge using li-ion electrode, increase lithium ion battery part uses secondary
Number, can effectively make up the deficiency of air pole poor circulation.Air pole is only applied to increase journey and instantaneous high power output.
In short, the characteristics of present invention is using lithium ion battery high operating voltage, can give full play to its cycle performance advantage；
The characteristics of using lithium sky battery high specific energy and air pole active material high-specific surface area, plays the work for increasing journey and high-power output
With.Meanwhile in hybrid battery system, by reducing lithium-air battery part access times, repeats itself can be efficiently reduced
Adverse effect of the performance deficiency to entire hybrid battery system.
Compared with prior art the invention has the advantages that：
1, the present invention passes through the characteristic of the characteristics of lithium-air battery part high specific energy and the output of air pole instantaneous high power,
Ground connection improves lithium ion battery energy density and output power；The characteristics of reaction is preferentially participated in using li-ion electrode, is increased
Lithium ion battery part access times significantly reduce lithium-air battery part unfavorable factor to the shadow of hybrid battery system
It rings, obtains a kind of high capacity high power type, and have the battery system of certain circulation ability.
2, present invention utilizes the characteristics of lithium-air battery high specific energy, while reducing its own defect to the shadow of practical application
It rings, provides a kind of usage mode of practicable lithium-air battery.
3, the present invention provides the methods for improving lithium ion battery energy density and output high-power, while being lithium air electricity
The practical application in pond provides a kind of mode.It can be used for demand high specific energy-high power type accumulation power supply field, especially electronic
Automotive field.
Detailed description of the invention
Fig. 1 is 1 lithium ion of embodiment/air hybrid battery system constant-current discharge curve.
Fig. 2 is 1 lithium ion of embodiment/air hybrid battery system compared with the power that the 60s of lithium ion battery discharges.
Fig. 3 is 1 lithium ion of embodiment/air hybrid battery system 8000mA gNCM -1The pulsed discharge of -30s-standing is bent
Line.
Fig. 4 is 1 hybrid battery system schematic of embodiment, and a is low discharging current process, and b is high-power output process, c
For regenerative power process.
Specific embodiment
Below by specific embodiment to high capacity high power type lithium ion/air hybrid battery of the present invention do into
One step explanation.Following embodiment is the experimental result of the selectivity of the 2 kinds of different battery structures provided based on thought of the invention,
But scope of the presently claimed invention is not limited to this.According to essential characteristic and theory of the invention as defined in the claims
Foundation, as long as any improved form that those skilled in the art is carried out, belongs to scope of the presently claimed invention.
Embodiment 1
Cathode is lithium metal, and lithium ion anode activity material is LiNi1/3Co1/3Mn1/3O2(NCM), air cathode active material
For Ru@graphen (Ru@G), lithium ion battery partial electrolyte liquid is 1mol L-1LiPF6- EC/DEC, lithium-air battery part electricity
Solution liquid is 1mol L-1LiTFSI-TEGDME, lithium ion battery portion septum be Celgard 2500, lithium-air battery part every
Film is fibreglass diaphragm.Individual lithium ion battery and individual lithium-air battery are connected in parallel, lithium ion/air is constituted
Hybrid battery system.
The preparation of lithium ion cell positive：By active material NCM, conductive agent acetylene black, bonding agent PVDF (polyvinylidene fluoride
Alkene) according to mass ratio be 80:10:10 are matched, and grinding uniformly, then instills suitable NMP and is slurried in the agate mortar, then
It is put into ultrasonic disperser and disperses 1h.Obtained mixed slurry is coated on aluminium foil surface, then in a vacuum drying oven at 120 DEG C
Dry 12h, can be obtained required lithium ion cell positive.
The preparation of lithium air battery positive electrode：It according to mass ratio is 90 by active material Ru@G and bonding agent PVDF:10 carry out
Proportion, grinding uniformly, then instills suitable NMP and is slurried, place into and disperse 1h in ultrasonic disperser in the agate mortar.?
The mixed slurry arrived is coated on foam nickel surface, then dry 10h at 120 DEG C in a vacuum drying oven, and required sky can be obtained
Gas anode.
The loading capacity for controlling active material is all 2mg cm in lithium ion anode and air cathode-2。
By the lithium ion cell positive of preparation, cathode lithium, diaphragm Celgard 2500, electrolyte 1molL-1LiPF6-EC/
DEC, oxygen content and water content all<The assembling of lithium ion battery is completed in the glove box of 0.1ppm.
By the lithium air battery positive electrode of preparation, cathode lithium, diaphragm glass fibre, electrolyte 1mol L-1LiTFSI-
TEGDME, oxygen content and water content all<The assembling of lithium-air battery is completed in the glove box of 0.1ppm.
Assemble obtained battery standing for 24 hours more than, the oxygen that purity is 99.99% is then passed through in lithium-air battery,
Pressure is 0.02MPa.Then the cathode of the cathode of lithium ion battery and lithium-air battery is connected, forms the negative of hybrid system
Pole；The anode of lithium ion battery is connect with the anode of lithium-air battery, is the anode of hybrid system.
Using Land tester, using constant current test method, system is 50mA g in current densityNCM -1, difference cut-off
It discharges under voltage (2.7V, 2.6V, 2.5V).It is as shown in Figure 1 to test obtained discharge curve.From the figure, it can be seen that discharging
Platform there are two in journey significantly,>3.0V is the workspace of lithium ion battery, and discharge capacity is about 71mAh
gNCM+Ru@G -1If according to the Mass Calculation of NCM, for 142mAh gNCM -1.<The workbench of 3.0V, corresponding air pole ORR are anti-
The workspace answered.Therefrom it can be seen that, lithium ion/air hybrid battery system capacity is apparently higher than lithium ion battery NCM's.
For example, the discharge capacity of mixed system is 3820mAh g when discharge cut-off voltage is 2.5VNCM+Ru@G -1, it is lithium ion battery
(about 142mAh g more than 27 timesNCM -1(NCM Mass Calculation is pressed, by capacity 71mAh gNCM+Ru@G -1Conversion obtains)).
The discharge power curve tested under obtained 60s continuous several times difference electric current is as shown in Figure 2.It can from figure
It arrives, lithium ion/air hybrid battery system power is substantially better than lithium ion battery.In continuous operation, mixed system is obtained
Obtained a high output power 4521W kgNCM+Ru@G -1, higher than the peak power 2916W kg of lithium ion batteryNCM -1.Work as replacement
One new battery system, in 5000mA gNCM -1Electric current under when discharging, the power of hybrid battery can reach
8982WkgNCM+Ru@G -1, it is lithium ion battery peak power more than 3 times.
Test obtained 8000mA gNCM -1The pulsed discharge of -30s-standing curve is as shown in Figure 3.From the figure, it can be seen that
Pulsed discharge curve has shown the feature of typical capacitance curve, and when showing heavy-current discharge, air pole is by feat of its surface
Capacitor provides power output.It can be seen that from standing in curve when completing high-power output, discharge voltage is gradually recovered
The operating voltage 3.76V of NCM is arrived, it is meant that air pole is after high power discharge, by the spontaneous charging of NCM electrode.Therefore,
It ensure that the renewable use of air pole.
Embodiment 2
Cathode is lithium metal, and lithium ion anode activity material is LiNi1/3Co1/3Mn1/3O2(NCM), air cathode active material
For Ru@graphen (Ru@G), lithium ion battery partial electrolyte liquid is 1mol L-1LiPF6- EC/DEC, lithium-air battery part electricity
Solution liquid is 1mol L-1LiTFSI-TEGDME, lithium ion battery portion septum be Celgard 2500, lithium-air battery part every
Film is fibreglass diaphragm.Lithium ion anode connect to form common anode with air cathode short circuit, shares a cathode lithium, constitutes
Lithium ion/air hybrid battery (system).
The preparation for preparing lithium ion cell positive as described in Example 1 of li-ion electrode, the preparation of air cathode is such as
The preparation of lithium air battery positive electrode described in embodiment 1.
By the lithium ion anode and air cathode of preparation, cathode lithium, diaphragm Celgard 2500 and glass fibre, electrolyte
1molL-1LiTFSI-TEGDME, oxygen content and water content all<The assembling of battery is completed in the glove box of 0.1ppm.Lithium ion
Anode and air cathode are respectively placed in the two sides of common cathode lithium.Wherein, 2500 diaphragm of lithium ion anode-Celgard-is negative
The structure of pole lithium composition Li-like ions battery；Air cathode-fibreglass diaphragm-cathode lithium constitutes the knot of class lithium-air battery
Structure.
Assemble obtained battery standing for 24 hours more than, then carry out test same as Example 1.Before test, in air pole
Side is passed through the oxygen that purity is 99.99%, pressure 0.02MPa.When test, lithium ion anode and lithium air cathode are connected
It is connected together and constitutes the same anode.Test condition is as described for example 1.
System is 50mA g in current densityNCM -1Under conditions of constant current discharge, blanking voltage be 2.5V when, obtain
Discharge capacity is 3905mAh gNCM+Ru@G -1；In 5000mA gNCM -1It discharges under conditions of -60s, obtained power is 9124W
kgNCM+Ru@G -1.It is apparently higher than the capacity 142mAh g of lithium ion batteryNCM -1And peak power 2916W kgNCM -1。
Claims (10)
1. a kind of high capacity high power type lithium ion/air hybrid battery system, which is characterized in that just including a lithium ion
Pole, an air cathode and one share negative grade, are made of lithium ion battery part and lithium-air battery part, lithium ion battery
Part is shared cathode by lithium ion cell positive-lithium-ion battery electrolytes-lithium ion battery separator-and is constituted, lithium-air battery
Part is shared cathode by air cathode-lithium-air battery electrolyte-diaphragm for lithium-air battery-and is constituted, and wherein lithium ion battery is being just
Pole is connect with air cathode short circuit, shares a cathode；
Or be made of individual lithium ion battery and lithium-air battery parallel connection, connection type is that cathode is connected together as
The cathode of hybrid battery system, anode are connected together as the anode of hybrid battery system.
2. high capacity high power type lithium ion/air hybrid battery system according to claim 1, it is characterised in that lithium ion
Cell positive material is LiCoO2、LiFePO4、LiMn2O4、LiNi1-x-yCoxMnyO2、LiNi0.8Co0.15Al0.05O2Ternary material
One of.
3. high capacity high power type lithium ion/air hybrid battery system according to claim 1, it is characterised in that air pole
Active material is the composite material of graphene, the composite material of graphene and noble metal or graphene and transiting metal oxidation.
4. high capacity high power type lithium ion/air hybrid battery system according to claim 2, it is characterised in that the stone
The composite material of black alkene and noble metal is selected from the composite material of at least one of graphene and Ru, Pt, Au, Pd, the graphene
Graphene and MnO are selected from the composite material of transition metal oxide2、Co3O4, at least one of NiO composite material.
5. the high power type lithium ion of high capacity described in any claim/air hybrid battery system according to claim 1~4
System, it is characterised in that the electrolyte of lithium ion battery part is 1mol L-1LiPF6-EC/DEC。
6. the high power type lithium ion of high capacity described in any claim/air hybrid battery system according to claim 1~4
System, it is characterised in that the electrolyte of lithium-air battery part is 1mol L-1LiTFSI-DME、1mol L-1LiTFSI-TEGDME、
1mol L-1One of LiTFSI-DMSO.
7. the high power type lithium ion of the high capacity according to any claim in claim 5/air hybrid battery system,
The electrolyte for being characterized in that lithium-air battery part is 1mol L-1LiTFSI-DME、1mol L-1LiTFSI-TEGDME、1mol
L-1One of LiTFSI-DMSO.
8. the high power type lithium ion of high capacity described in any claim/air hybrid battery system according to claim 1~4
System, it is characterised in that the diaphragm of lithium ion battery part is the serial diaphragm of Celgard.
9. the high power type lithium ion of high capacity described in any claim/air hybrid battery system according to claim 1~4
System, it is characterised in that the diaphragm of lithium-air battery part is fibreglass diaphragm.
10. the high power type lithium ion of the high capacity according to any claim in claim 5/air hybrid battery system,
It is characterized in that the diaphragm of lithium-air battery part is fibreglass diaphragm.
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