CN108933310B - A high-capacity and high-power lithium-ion/air hybrid battery system - Google Patents
A high-capacity and high-power lithium-ion/air hybrid battery system Download PDFInfo
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- H01M12/00—Hybrid cells; Manufacture thereof
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- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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Abstract
本发明提供一种高容量高功率型锂离子/空气混合电池系统，将锂离子电池和锂空气电池整合构建混合电池系统，达到对二者的性能扬长避短的效果。通过锂空气电池ORR的高容量特点，来弥补锂离子电池能量密度低的不足。同时利用空气极活性材料比表面积高的特点，进一步改善锂离子电池的输出功率。利用锂离子电池正极活性材料具有高于ORR反应的工作电压(>3.0V)及优秀的循环性能，增加锂离子电池使用次数，有效地弥补了锂空气电池循环性能不足的问题，同时为锂空气电池的使用提供了一种方法。该电池系统兼具锂离子电池和锂空气电池的优点，在性能上实现对锂离子电池和锂空气电池扬长避短，获得一种具有高容量高功率特点的电池系统。
The invention provides a high-capacity and high-power lithium-ion/air hybrid battery system, which integrates the lithium-ion battery and the lithium-air battery to construct a hybrid battery system, so as to achieve the effect of improving the performance of the two and avoiding the disadvantages. The low energy density of lithium-ion batteries is compensated for by the high-capacity characteristics of the lithium-air battery ORR. At the same time, the high specific surface area of the air electrode active material is used to further improve the output power of the lithium-ion battery. The use of lithium-ion battery cathode active materials has a working voltage (>3.0V) higher than the ORR reaction and excellent cycle performance, increasing the number of lithium-ion batteries used, effectively making up for the insufficient cycle performance of lithium-air batteries. The use of batteries provides one way. The battery system has the advantages of both the lithium-ion battery and the lithium-air battery, realizes the advantages and avoids the disadvantages of the lithium-ion battery and the lithium-air battery in terms of performance, and obtains a battery system with the characteristics of high capacity and high power.
Description
Technical Field
The invention belongs to the field of lithium ion batteries and lithium air batteries, and particularly relates to a lithium ion/air hybrid battery system.
Background
With the development of society, chemical energy is continuously consumed, and the problem of environmental pollution becomes more and more serious while bringing convenience. In addition to developing clean energy to solve this problem, one effective approach is to use a chemical source of electrical energy. Since 1991, lithium ion batteries have entered the consumer market, they have been widely used in the fields of portable electronic devices, smart grid-connected and new energy vehicles. Particularly, in recent years, under the active guidance of policies of various countries, electric vehicles have been rapidly developed, and urgent needs are presented for high specific energy-high power lithium ion batteries, so that they have become the research focus in the scientific community and the industrial community. However, the energy density of the lithium ion battery is difficult to reach a high value due to the limitation of low capacity of the lithium ion battery cathode material. For example, even the best lithium ion battery at present can only reach the energy density of 250-300Wh kg-1The demand of the future market cannot be met. Therefore, it is very important to develop new batteries beyond lithium ion batteries. One way is to develop a lithium air battery with a theoretical energy density as high as 3500Wh kg-1Almost 10 times as much as lithium ion batteries exhibit great application value, and thus have received wide attention all over the world. All the battery enterprisesThey are regarded as the ultimate goal of the development of lithium batteries. Under the continuous effort of scientific researchers, the energy density of 500-800Wh kg can be prepared internationally-1The lithium air battery of (1). China also achieves good results in the field. For example, Zhang Xinbo team, the Changchun institute of China's institute of technology, has publicly reported an energy density as high as 523Wh kg-1The lithium air battery of (1).
However, the lithium air battery still has the problems of low charge-discharge energy efficiency, poor charge transfer capability of ORR and OER, low actual discharge capacity, easy decomposition of electrolyte, unstable carbon anode, and the like. In addition, in order to improve charge transfer ability during charge and discharge, it is generally necessary to use a noble metal catalyst such as Ag, Ru, Au, Pt, Pd, and the like. The high cost also limits the widespread use of lithium air batteries. In the opinion of the authors, purely lithium-air batteries are difficult to put into practical use for a considerable time in the future, based on the existing scientific technology. Therefore, it is important how to apply its high specific energy characteristics while reducing the influence of its adverse factors.
Disclosure of Invention
The invention aims to provide a high-capacity high-power lithium ion/air hybrid battery system aiming at the defects of the prior art, the battery has the advantages of a lithium ion battery and a lithium air battery, the advantages of the lithium ion battery and the lithium air battery are improved and the disadvantages of the lithium ion battery and the lithium air battery are avoided in performance, and the battery system with the characteristics of high capacity and high power is obtained.
The concept of the invention is as follows: the lithium ion battery and the lithium air battery are integrated to construct a hybrid battery system, so that the effects of making good use of the performance of the lithium ion battery and the lithium air battery and avoiding the disadvantages of the lithium ion battery and the lithium air battery are achieved. The defect of low energy density of the lithium ion battery is made up by the high-capacity characteristic of the ORR of the lithium air battery. Meanwhile, the output power of the lithium ion battery is further improved by utilizing the characteristic of high specific surface area of the air electrode active material. The positive active material of the lithium ion battery has the working voltage (>3.0V) higher than the ORR reaction and excellent cycle performance, so that the use frequency of the lithium ion battery is increased, the problem of insufficient cycle performance of the lithium air battery is effectively solved, and a method is provided for the use of the lithium air battery. The invention is mainly characterized in that: the energy density and the output power of the lithium ion battery are indirectly improved through the lithium air battery part; through the lithium ion battery part, the influence of adverse factors such as poor cycle performance, low energy efficiency, unstable electrode electrolyte and the like of the lithium air battery on the whole battery system is reduced, and the effects of improving the advantages and avoiding the disadvantages are achieved. While providing a practical way for the use of lithium air batteries.
The high-capacity high-power lithium ion/air hybrid battery system is characterized in that an air anode is added on the basis of the traditional lithium ion battery structure; or the lithium ion battery and the lithium air battery are connected in parallel to form a lithium ion/air hybrid battery system. The lithium ion battery positive active material needs to have a working voltage (>3.0V) higher than the ORR reaction and excellent cycle performance. The air cathode active material needs to have a high ORR reaction discharge capacity, a high specific surface area, and the ability to oxidatively decompose ORR discharge products during charging. The concrete structure is as follows:
the lithium ion battery comprises a lithium ion anode, an air anode and a shared cathode, and consists of a lithium ion battery part and a lithium air battery part, wherein the lithium ion battery part consists of the lithium ion battery anode, a lithium ion battery electrolyte, a lithium ion battery diaphragm and the shared cathode, and the lithium air battery part consists of the air anode, the lithium ion battery electrolyte, the lithium ion battery diaphragm and the shared cathode, wherein the lithium ion anode and the air anode are connected together in a short circuit and share one cathode;
or the lithium ion battery and the lithium air battery are connected in parallel, the negative electrodes are connected together to be used as the negative electrode of the hybrid battery system, and the positive electrodes are connected together to be used as the positive electrode of the hybrid battery system.
In the above technical solution of the present invention, the lithium ion battery cathode active material may use a commercial cathode material, such as LiCoO2、LiFePO4、LiMn2O4And LiNi1-x-yCoxMnyO2、LiNi0.8Co0.15Al0.05O2One of ternary materials.
In the above technical solution of the present invention, the air cathode active material has to have a high ORR discharge capacity, a high specific surface area, and an ability to oxidatively decompose an ORR discharge product, that is, the material has an ability to sufficiently contain an ORR discharge product and ORR and OER catalytic activities. Such as graphene, a composite of graphene and a noble metal, a composite of graphene and a transition metal oxide, and the like. Further preferred are, for example, a composite material of graphene and Ru, Pt, Au, Pd or the like, and graphene and MnO2、Co3O4And NiO, etc.
In the above technical solution of the present invention, the electrolyte of the lithium ion battery part is the electrolyte of a traditional lithium ion battery, such as 1mol L of electrolyte-1LiPF6-EC/DEC. The electrolyte used in the lithium air battery part is a common electrolyte of the lithium air battery, such as 1mol L-1LiTFSI-DME、1mol L-1LiTFSI-TEGDME and 1mol L-1LiTFSI-DMSO, and the like.
In the technical scheme of the invention, the diaphragm used by the lithium ion battery part is a polymer diaphragm used by the traditional lithium ion battery, such as Celgard series diaphragms. The separator used in the lithium air battery part is a separator of a commonly used lithium air battery, such as a glass fiber separator.
In the technical scheme of the invention, the lithium ion battery part is a closed system, so that O is avoided2、H2O and CO2And the entry of outside gases. The lithium air battery part or the air electrode needs to be used in pure oxygen or inert gas environment containing oxygen. The working voltage range of the hybrid battery is 2.3-4.4V.
In the lithium ion/air hybrid battery system, when the lithium ion/air hybrid battery system is discharged at a low current, the working voltage of the lithium ion battery anode is higher than that of the air anode ORR, so that the lithium ion anode preferentially provides energy output. When it fails to meet the external energy demand, the system voltage drops to the ORR voltage, at which time the air electrode begins to provide energy release. The ORR capacity is far higher than that of the lithium ion electrode material, so that the problem of low energy density of the lithium ion battery is effectively solved. On the other hand, the air electrode has a characteristic of high specific surface area, and can provide high power output by the electric charge double layer capacity and the ORR pseudo capacitance on the surface thereof, and can be used as a capacitor electrode. When discharging under large current, if the lithium ion electrode can not meet the external power requirement, the air electrode can provide high power output through the surface capacitor. When the lithium ion battery returns to the low current for discharging again, except that the lithium ion electrode provides external energy for outputting again, the lithium ion electrode charges the air electrode due to the potential difference between the lithium ion electrode and the air electrode after high-power discharging, so that the air electrode is restored to a new state, and the lithium ion battery is guaranteed to be reused. In practical application, the defect of poor cycle performance of the air electrode can be effectively overcome by utilizing the characteristic that the lithium ion electrode preferentially participates in discharging and increasing the use times of the lithium ion battery. The air pole is only applied to range extension and instantaneous high power output.
In a word, the invention utilizes the characteristic of high working voltage of the lithium ion battery to give full play to the cycle performance advantage; the characteristics of high specific energy of the lithium air battery and high specific surface area of the active material of the air electrode are utilized, and the functions of range extension and high power output are achieved. Meanwhile, in the hybrid battery system, by reducing the number of times of using the lithium-air battery part, the adverse effect of insufficient self-circulation performance on the whole hybrid battery system can be effectively reduced.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention indirectly improves the energy density and the output power of the lithium ion battery through the characteristics of high specific energy of the lithium air battery and the instantaneous high power output of the air electrode; the characteristic that the lithium ion electrode preferentially participates in the reaction is utilized, the number of times of using the lithium ion battery is increased, the influence of partial adverse factors of the lithium air battery on a hybrid battery system is effectively reduced, and the battery system with high capacity and high power and certain cycle capacity is obtained.
2. The invention utilizes the characteristic of high specific energy of the lithium-air battery, reduces the influence of the defects on the practical application, and provides a practical and feasible use mode of the lithium-air battery.
3. The invention provides a method for improving the energy density and the output high power of a lithium ion battery, and provides a mode for the practical application of the lithium air battery. The method can be used in the field of high specific energy-high power type energy storage power supply, especially in the field of electric automobiles.
Drawings
Fig. 1 is a constant current discharge curve of a lithium ion/air hybrid battery system of example 1.
Fig. 2 is a comparison of the power of 60s discharge of the lithium ion/air hybrid battery system of example 1 and the lithium ion battery.
FIG. 3 shows 8000mA g of a lithium ion/air hybrid battery system according to example 1NCM -1-a pulsed discharge-rest curve of 30 s.
Fig. 4 is a schematic diagram of a hybrid battery system of example 1, where a is a low current discharge process, b is a high power output process, and c is a power regeneration process.
Detailed Description
The high capacity and high power type lithium ion/air hybrid battery according to the present invention will be further described with reference to the following embodiments. The following examples are experimental results of the selectivity of 2 different battery structures given based on the idea of the present invention, but the scope of the claims of the present invention is not limited thereto. The essential features and the theoretical basis for the present invention as defined in the claims, but any modification made by those skilled in the art will fall within the scope of the claims.
Example 1
The negative electrode is metallic lithium, and the lithium ion positive electrode active material is LiNi1/3Co1/3Mn1/3O2(NCM), wherein the active material of the air positive electrode is Ru @ graphene (Ru @ G), and the partial electrolyte of the lithium ion battery is 1mol L-1LiPF6EC/DEC, 1mol L of partial electrolyte for lithium-air batteries-1And the lithium ion battery part separation membrane is Celgard 2500, and the lithium air battery part separation membrane is a glass fiber diaphragm. And connecting the single lithium ion battery and the single lithium air battery in parallel to form a lithium ion/air hybrid battery system.
Preparing the anode of the lithium ion battery: mixing an active material NCM, a conductive agent acetylene black and a binding agent PVDF (polyvinylidene fluoride) according to a mass ratio of 80:10:10, uniformly grinding in an agate mortar, then dropping a proper amount of NMP into the mixture to form slurry, and then putting the slurry into an ultrasonic disperser to disperse for 1 hour. And coating the obtained mixed slurry on the surface of an aluminum foil, and drying in a vacuum drying oven at 120 ℃ for 12 hours to obtain the required lithium ion battery anode.
Preparing the lithium-air battery anode: the active material Ru @ G and the adhesive PVDF are proportioned according to the mass ratio of 90:10, are uniformly ground in an agate mortar, then are dripped with a proper amount of NMP to form slurry, and are placed in an ultrasonic disperser to be dispersed for 1 hour. And coating the obtained mixed slurry on the surface of the foamed nickel, and drying in a vacuum drying oven at 120 ℃ for 10 hours to obtain the required air anode.
The loading of active material was controlled to be 2mg cm in both the lithium ion positive electrode and the air positive electrode-2。
Preparing the anode, cathode lithium, diaphragm Celgard 2500 and electrolyte 1mol L-1LiPF6EC/DEC, in both oxygen and water content<And assembling the lithium ion battery in a 0.1ppm glove box.
Preparing the anode, cathode lithium, diaphragm glass fiber and electrolyte of 1mol L of the lithium-air battery-1LiTFSI-TEGDME for oxygen and water content<The assembly of the lithium air cell was completed in a 0.1ppm glove box.
The assembled battery is stood for more than 24 hours, and then oxygen with the purity of 99.99 percent is introduced into the lithium air battery, and the pressure is 0.02 MPa. Then connecting the negative electrode of the lithium ion battery with the negative electrode of the lithium air battery to form the negative electrode of the hybrid system; and connecting the positive electrode of the lithium ion battery with the positive electrode of the lithium air battery to form the positive electrode of the hybrid system.
The system adopts a Land tester and a constant current test method, and the current density of the system is 50mA gNCM -1And discharge at different cut-off voltages (2.7V, 2.6V and 2.5V). The discharge curve obtained from the test is shown in fig. 1. As can be seen from the figure, there are two distinct plateaus during the dischargeThe table is provided with a plurality of tables,>3.0V is the working area of the lithium ion battery, and the discharge capacity is about 71mAh gNCM+Ru@G -1142mAh g, calculated as the mass of NCMNCM -1。<And the working platform of 3.0V corresponds to a working area of the ORR reaction of the air electrode. It can be seen that the capacity of the lithium ion/air hybrid battery system is significantly higher than that of the lithium ion battery NCM. For example, when the discharge cut-off voltage is 2.5V, the discharge capacity of the mixed system is 3820mAh gNCM+Ru@G -1More than 27 times (about 142mAh g) of lithium ion batteryNCM -1(calculated as NCM mass, from a capacity of 71mAh gNCM+Ru@G -1Converted).
The discharge power curve obtained by the test under different currents for 60s is shown in figure 2. As can be seen from the figure, the power of the lithium ion/air hybrid battery system is significantly better than that of the lithium ion battery. In continuous operation, the mixed system obtains a high output power of 4521W kgNCM+Ru@G -1The peak power is 2916W kg higher than that of the lithium ion batteryNCM -1. When a new battery system is replaced, at 5000mA gNCM -1When discharging under the current of (3), the power of the hybrid battery can reach 8982W kgNCM+Ru@G -1More than 3 times of the peak power of the lithium ion battery.
8000mA g obtained by testNCM -1The pulsed discharge-rest curve for-30 s is shown in FIG. 3. As can be seen, the pulsed discharge curve exhibits the characteristic capacitance curve, indicating that the air electrode provides power output by virtue of its surface capacitance when discharged at high current. As can be seen from the stationary curve, when the high power output is completed, the discharge voltage is gradually restored to the working voltage of NCM of 3.76V, meaning that the air electrode is spontaneously charged by the NCM electrode after the high power discharge. Thus, the reproducible use of the air electrode is ensured.
Example 2
The negative electrode is metallic lithium, and the lithium ion positive electrode active material is LiNi1/3Co1/3Mn1/3O2(NCM), the active material of the air positive electrode is Ru @ graphene (Ru @ G), and the lithium ion battery is partially powered by electricityThe amount of the hydrolyzed solution is 1mol L-1LiPF6EC/DEC, 1mol L of partial electrolyte for lithium-air batteries-1And the lithium ion battery part separation membrane is Celgard 2500, and the lithium air battery part separation membrane is a glass fiber diaphragm. The lithium ion positive electrode and the air positive electrode are connected in a short circuit mode to form a common positive electrode, and share one negative electrode lithium, so that the lithium ion/air hybrid battery (system) is formed.
Preparation of lithium ion electrode the preparation of the lithium ion battery positive electrode described in example 1 and the preparation of the air positive electrode the lithium air battery positive electrode described in example 1 was prepared.
Mixing the prepared lithium ion anode, air anode, cathode lithium, diaphragm Celgard 2500, glass fiber and electrolyte solution 1mol L-1LiTFSI-TEGDME for oxygen and water content<The cell assembly was completed in a 0.1ppm glove box. The lithium ion anode and the air anode are respectively arranged on two sides of the common cathode lithium. Wherein, the lithium ion anode-Celgard 2500 diaphragm-cathode lithium form the structure of the lithium ion battery; the air anode, the glass fiber diaphragm and the cathode lithium form a structure of the lithium-like air battery.
The assembled battery was left to stand for 24 hours or more, and then the same test as in example 1 was performed. Before testing, oxygen with the purity of 99.99 percent is introduced into one side of the air electrode, and the pressure is 0.02 MPa. During testing, the lithium ion anode and the lithium air anode are connected together to form the same anode. The test conditions were as described in example 1.
The system is at a current density of 50mA gNCM -1Under the condition of (1), discharging at constant current, and when the cut-off voltage is 2.5V, the obtained discharge capacity is 3905mAh gNCM+Ru@G -1(ii) a At 5000mA gNCM -1Discharging under-60 s condition to obtain a power of 9124W kgNCM+Ru@G -1. The capacity of the lithium ion battery is obviously higher than 142mAh gNCM -1And peak power 2916W kgNCM -1。
Claims (6)
1. A high-capacity high-power lithium ion/air hybrid battery system is characterized by comprising a lithium ion anode, an air anode and a shared cathode, wherein the lithium ion anode, the air anode and the shared cathode are composed of a lithium ion battery part and a lithium air battery part, the lithium ion battery part is composed of the lithium ion battery anode, a lithium ion battery electrolyte, a lithium ion battery diaphragm and the shared cathode, the lithium air battery part is composed of the air anode, the lithium ion battery electrolyte, the lithium air battery diaphragm and the shared cathode, the lithium ion battery anode and the air anode are in short circuit connection, and share one cathode;
the working voltage of the lithium ion battery anode active material is higher than that of an air anode ORR reaction; the positive active material of the lithium ion battery is LiCoO2、LiFePO4、LiMn2O4、 LiNi0.8Co0.15Al0.05O2One of ternary materials; the air positive active material is graphene, a composite material of graphene and a noble metal or a composite material of graphene and a transition metal oxide, the composite material of graphene and a noble metal is selected from the composite materials of graphene and at least one of Ru, Pt, Au and Pd, and the composite material of graphene and a transition metal oxide is selected from the composite materials of graphene and MnO2、Co3O4And NiO.
2. The high-capacity high-power type lithium ion/air hybrid battery system according to claim 1, wherein the electrolyte of the lithium ion battery portion is 1mol L-1 LiPF6-EC/DEC。
3. The high-capacity high-power type lithium ion/air hybrid battery system according to claim 1, wherein the electrolyte of the lithium air battery portion is 1mol L-1 LiTFSI-DME、1 mol L-1 LiTFSI-TEGDME、1 mol L-1One of LiTFSI-DMSO.
4. The high-capacity high-power type lithium ion/air hybrid battery system according to claim 2, wherein the electrolyte of the lithium air battery portion is 1mol L-1 LiTFSI-DME、1 mol L-1 LiTFSI-TEGDME、1 mol L-1One in LiTFSI-DMSOAnd (4) seed preparation.
5. The high-capacity high-power type lithium ion/air hybrid battery system according to claim 1, wherein the separator of the lithium ion battery part is a Celgard series separator.
6. The high-capacity high-power type lithium ion/air hybrid battery system according to claim 1, wherein the separator of the lithium air battery portion is a glass fiber separator.
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| CN103460502A (en) * | 2011-04-19 | 2013-12-18 | 本田技研工业株式会社 | Lithium ion oxygen battery |
| JP2013254647A (en) * | 2012-06-07 | 2013-12-19 | Nec Corp | Lithium ion-lithium air composite secondary battery, charging/discharging method using the same, and cathode material for lithium ion-lithium air composite secondary battery |
| CN107611527A (en) * | 2017-09-14 | 2018-01-19 | 上海轩玳科技有限公司 | A kind of fuel cell and lithium ion battery composite power supply unit |
| CN107871915A (en) * | 2017-09-22 | 2018-04-03 | 北京机械设备研究所 | A kind of AC-battery power source and thermal management algorithm of fuel cell and battery |
| CN107871908A (en) * | 2017-09-22 | 2018-04-03 | 北京机械设备研究所 | The power supply and control method that metal air fuel cell mixes with lithium ion battery |
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| CN108933310A (en) | 2018-12-04 |
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