CN109585842A - A kind of hybrid electrochemical energy storage system based on absorption counterfeit potential and embedded reactive - Google Patents
A kind of hybrid electrochemical energy storage system based on absorption counterfeit potential and embedded reactive Download PDFInfo
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Abstract
The invention discloses a kind of based on the hybrid electrochemical energy storage system for adsorbing counterfeit potential and embedded reactive, including anode, cathode and electrolyte, and the active material of anode is nano material MXy, wherein M is selected from one of Ti, V, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ta, Ru and W element or a variety of, and X is selected from one of O, S, Se, F, N and P element or a variety of, 0≤y≤5；The charge/discharge capacity contribution sources of the energy storage system are in the counterfeit potential of absorption and embedded reactive.During the charging process, electrolysis solution anion is attracted in the surface of active material of anode, is oxidized simultaneously；During discharge, electrolysis solution anion is desorbed from the surface of active material of anode, is reduced simultaneously, to generate the counterfeit potential of considerable absorption.Adsorbing counterfeit potential makes the hybrid electrochemical energy storage system of invention capacity on the basis of embedded reactive be improved significantly, and has the characteristics that high-energy density.
Description
Technical field
The invention belongs to secondary cell and electrochemical field, it is related to a kind of based on adsorbing the new of counterfeit potential and embedded reactive
Type hybrid electrochemical energy storage system.
Background technique
For many years from battery invention 200, it plays effect more and more prominent in energy storage and converting system,
Substantially increase people's lives quality.From one-shot battery to secondary cell, it can be divided according to the electrochemical reaction process of battery
For many systems, such as Zn-MnO2One-shot battery, lead-acid battery, nickel-metal hydride battery and current widely used lithium ion battery.With
The development of advanced material and the introducing of novel reaction mechanism, the chemical property of battery is greatly improved, such as lithium
The embedded reactive mechanism of ion battery can inhibit the formation of Li dendrite, increase the operating voltage of battery, improve battery
Energy density, the development of portable electronic product is greatly facilitated in this.Due to the rapid development of electric automobile market, lithium-ion electric
The positive electrode in pond needs to have higher energy density, to meet the needs of course continuation mileage.In lithium-rich anode material system,
Due to the additional contribution of anion redox, specific energy density is significantly promoted than traditional positive electrode, causes the world
Extensive concern.However in order to further enhance energy density, it is necessary to have the positive electrodes of higher capacity.In other words, this
Need to increase the content of lithium in positive electrode, but from the angle of thermodynamic stability for this is difficult to realize.Therefore, lithium ion
The upper limit of the energy density of battery receives the restriction of battery material.On the other hand, in recent years, since lithium ion battery short circuit is led
Cause fire and explosion caused people for electric car use lithium ion battery with high energy density worry, main cause be by
It will lead to the phase transformation and avalanche of material structure in the mechanism of lithium insertion abjection, and anion redox reaction will cause oxygen
It is precipitated.Thus, it is necessary to explore new electrochemical energy storage mechanism, high-energy density can either be kept, also there is better peace
Full property and long cycle life.
Summary of the invention
It is an object of the present invention to propose it is a kind of novel based on the electrochemical energy storage mechanism for adsorbing counterfeit potential, pass through by
The mechanism is combined with existing embedded reactive mechanism, constructs the hybrid battery system with high-energy density.
To achieve the goals above, the invention adopts the following technical scheme:
A kind of hybrid electrochemical energy storage system, including anode, cathode and electrolyte, which is characterized in that the work of the anode
Property material be nano material, chemical general formula MXy, wherein M be selected from Ti, V, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ta,
One of Ru and W element is a variety of, and X is selected from one of O, S, Se, F, N and P element or a variety of, 0≤y≤5；The energy storage
The charge/discharge capacity contribution sources of system are in the counterfeit potential of absorption and embedded reactive, the electrochemical reaction mistake of the counterfeit potential of absorption
Journey is as follows: during the charging process, electrolysis solution anion is attracted in the surface of active material of anode, while being electrolysed solution anion
It is oxidized；During discharge, electrolysis solution anion is desorbed from the surface of active material of anode, while being electrolysed solution anion and being gone back
It is former.
The active material of the anode is nano material, and form can be nano particle, nanometer sheet, nano wire etc.,
Nano material can be amorphous.The size of the nano material preferably at least in one dimension is less than 100 nanometers.
The active material MX of the anodeyIn, it is preferred that in M Mn, Fe, Co, Ni, Nb, Mo, Ta, Ru and W element
It is one or more, one of X O, S and F element or a variety of.It is furthermore preferred that the active material of the anode is Mn3O4、
MnO2、Mn5O8、RuO2、Fe2O3、Fe3O4、NiO、MoS2、FeF3Deng.
Hybrid electrochemical energy storage system of the invention is based on the electrochemical energy storage mechanism and existing insertion for adsorbing counterfeit potential
The combination of formula reaction mechanism, has the characteristics that high-energy density.
In hybrid electrochemical energy storage system of the invention, the cathode can use arbitrary battery cathode, existing
Lithium, sodium, potassium, calcium, magnesium cell negative electrode material can be applied to hybrid electrochemical energy storage system of the invention.
In hybrid electrochemical energy storage system of the invention, the electrolyte can be arbitrary battery electrolyte, existing
Lithium, the electrolyte that uses of sodium, potassium, calcium, magnesium cell can be applied to hybrid electrochemical energy storage system of the invention.Such as it is existing
There is commercialized 5V high-voltage lithium-ion battery electrolyte, wherein common anion is PF6 -、ClO4 -、BF4 -One of or
It is a variety of.It is PF with anion6 -Electrolyte for, the electrochemical reaction process of the counterfeit potential of the absorption is electrolysis solution anion
(PF6 -) be adsorbed on surface of positive electrode active material during the charging process, it is desorbed during discharge from surface of positive electrode active material,
Fluorine element in anion participates in the oxidation-reduction process during this.
The electrochemical reaction process of the counterfeit potential of absorption and the main distinction of traditional cell oxidation reduction reaction are:
It is usually generation on electrode material that traditional battery electrode, which reacts its oxidation-reduction process, and in adsorbing counterfeit potential,
Oxidation-reduction process occurs on electrolysis solution anion；The electrode reaction of conventional batteries system will lead to electrode material component
It changes and (has lithium ion when such as anode active material of lithium ion battery charges to deviate from from material), and adsorb counterfeit potential
Reaction process pertains only to absorption and desorption of the surface of positive electrode active material to anion, and positive electrode active materials itself become without component
Change (but have variation) on electronic structure.Since the process is mainly surface reaction process, for positive electrode active materials
Size has certain requirement, and material specific surface area is bigger, and the capacity for reacting contribution is more.
Compared with prior art, beneficial effects of the present invention:
Under normal conditions, transition metal oxide, sulfide, fluoride etc. are generally used for lithium ion battery negative material,
Of the invention based in the energy storage system for adsorbing counterfeit potential and embedded reactive, it is counterfeit that these materials show considerable absorption
Potential, so that these materials may be used as positive electrode active materials.These materials can be made to be embedded in lithium in addition, adsorbing counterfeit potential
Capacity is improved significantly on the basis of formula reaction, and voltage range is usually between 1.5-5.0V, with Mn3O4For, Mn3O4
It is typically used as lithium ion battery negative material, in the system, Mn3O4In the voltage range of 1.5V to 4.8V, 60mA/g's
Electric discharge can contribute the specific capacity of 300mAh/g for the first time under current density, wherein adsorb counterfeit potential and contribute to about 150mAh/g, lithium
Ion insertion abjection mechanism contributes to 150mAh/g.
Detailed description of the invention
Fig. 1 is the Mn for the 20nm that the embodiment of the present invention 1 synthesizes3O4The transmission electron microscope picture of material.
It in voltage range is 1.5-4.8V that Fig. 2, which is battery in the embodiment of the present invention 1, and current density is filling under 60mA/g
Discharge curve.
It in voltage range is 1.5-4.8V that Fig. 3, which is battery in the embodiment of the present invention 1, and current density is under 600mA/g
Charging and discharging curve figure.
It in voltage range is 1.5-4.8V that Fig. 4, which is battery in the embodiment of the present invention 1, and current density is under 600mA/g
Cycle performance figure.
It in voltage range is 1.5-4.8V that Fig. 5, which is battery in the embodiment of the present invention 2, and current density is under 600mA/g
Charging and discharging curve figure.
It in voltage range is 1.5-4.8V that Fig. 6, which is battery in the embodiment of the present invention 2, and current density is under 600mA/g
Cycle performance figure.
It in voltage range is 1.5-4.8V that Fig. 7, which is battery in the embodiment of the present invention 3, and current density is under 300mA/g
Charging and discharging curve figure.
Specific embodiment
With reference to the accompanying drawing, technical solution of the present invention is further elaborated on by embodiment, but not in any way
It limits the scope of the invention, protection scope of the present invention is defined by the appended claims.
1 Mn of embodiment3O4Hybrid energy-storing system as positive electrode active materials
By the MnCl of 1.2945g2·4H2The O dissolution of the ethyl alcohol of 10mL and ultrasound 10min, then by the Li of 0.3g2O2?
Ultrasonic disperse forms suspension in the ethyl alcohol of 30mL, then by MnCl2Li is added dropwise in solution2O2Suspension, and continue to stir.
It after being added dropwise to complete, filters and washs, in 80 DEG C of drying overnight, the Mn of 20nm can be obtained3O4Nano particle, transmission electron microscope picture
As shown in Figure 1.
With the Mn of 20nm3O4As positive electrode active materials, super P is as conductive agent, and PVDF is as binder, by quality
Anode is prepared into than 7:2:1；Using lithium piece as cathode, electrolyte is that (solvent is ethylene carbonate to commercialized 5V lithium-ion electrolyte
Ester (EC) and dimethyl carbonate (DMC) are mixed by 1:1 volume ratio, and solute is the LiPF of 1mol/L6), in the gloves of argon atmosphere
It is assembled into button cell in case, then carries out electrochemical property test.First charge for the first time, after discharge.In 60mA/g
Current density under, voltage range is 1.5V to 4.8V, and reversible capacity can achieve 250mAh/g (see Fig. 2)；600mA/g's
Under current density, voltage range is 1.5V to 4.8V, and capacity is 170mAh/g (see Fig. 3), and 50 circle capacity retention ratio of circulation is
83% (see Fig. 4).
2 MnO of embodiment2Hybrid energy-storing system as positive electrode active materials
By the MnCl of 1.2945g2·4H2O dissolution and ultrasound 10min in the deionized water of 10mL, then by 0.5500g's
NaOH ultrasonic dissolution in the deionized water of 30mL, then by MnCl2Solution is added dropwise in NaOH solution, and continues to stir.
It after being added dropwise to complete, filters and washs, in 80 DEG C of drying overnight, the MnO of 20nm or so can be obtained2Nano particle.
With the MnO of 20nm2As positive electrode active materials, super P is as conductive agent, and PVDF is as binder, by quality
Anode is prepared into than 7:2:1；Using lithium piece as cathode, electrolyte is that (solvent is ethylene carbonate to commercialized 5V lithium-ion electrolyte
Ester (EC) and dimethyl carbonate (DMC) are mixed by 1:1 volume ratio, and solute is the LiPF of 1mol/L6), in the gloves of argon atmosphere
It is assembled into button cell in case, then carries out electrochemical property test.First charge for the first time, after discharge.In 60mA/g
Current density under, voltage range is 1.5V to 4.8V, and reversible capacity can achieve 275mAh/g or more；In the electricity of 600mA/g
Under current density, voltage range is 1.5V to 4.8V, and capacity is 175mAh/g (see Fig. 5), and 100 circle capacity retention ratio of circulation is 80%
(see Fig. 6).
The unbodied RuO of embodiment 32Hybrid energy-storing system of the nano particle as positive electrode active materials
By the RuCl of 1.0372g3With dissolution and ultrasound 10min in the deionized water of 50mL, then the NaOH of 0.6g existed
Ultrasonic dissolution in the deionized water of 50mL, then by RuCl3Solution is added dropwise in NaOH solution, and continues to stir.It drips
Cheng Hou is filtered and is washed, and in 80 DEG C of drying overnight, powder is calcined 2h at 150 DEG C after drying, can be obtained unbodied
RuO2Nano particle.
With unbodied RuO2As positive electrode active materials, super P is as conductive agent, and PVDF is as binder, by matter
Amount is prepared into anode than 7:2:1；Using lithium piece as cathode, electrolyte is that (solvent is carbonic acid second to commercialized 5V lithium-ion electrolyte
Enester (EC) and dimethyl carbonate (DMC) are mixed by 1:1 volume ratio, and solute is the LiPF of 1mol/L6), in the hand of argon atmosphere
It is assembled into button cell in casing, then carries out electrochemical property test.First charge for the first time, after discharge.?
Under the current density of 300mA/g, voltage range is 1.5V to 4.8V, and reversible capacity can achieve 400mAh/g or more；?
Under the current density of 600mA/g, voltage range is 1.5V to 4.8V, and reversible capacity is 350mAh/g (see Fig. 7).
The MoS of 4 20nm of embodiment2Hybrid energy-storing system of the nanometer sheet as positive electrode active materials
By the MoO of 0.2718g3With the Na of 1.699g2S·9H2O is dissolved in together in the deionized water of 30mL, then will
The hydrochloric acid of the 4mol/L concentration of 2.2mL is slowly added dropwise to the solution, then transfers the solution into the reaction kettle of 50mL, is drying
200 DEG C of reaction 8h in case.To after reaction, filter and wash, is dried overnight in 80 DEG C of vacuum, can be obtained 20nm's or so
MoS2Nanometer sheet.
With the MoS of 20nm or so2Nanometer sheet is as positive electrode active materials, and super P is as conductive agent, and PVDF is as bonding
Agent, in mass ratio 7:2:1 are prepared into anode；Using lithium piece as cathode, electrolyte is that (solvent is commercialized 5V lithium-ion electrolyte
Ethylene carbonate (EC) and dimethyl carbonate (DMC) are mixed by 1:1 volume ratio, and solute is the LiPF of 1mol/L6), in argon gas gas
It is assembled into button cell in the glove box of atmosphere, then carries out electrochemical property test.First charge for the first time, after discharge.
Under the current density of 60mA/g, voltage range is 1.5V to 4.8V, and reversible capacity can achieve 250mAh/g or more；?
Under the current density of 600mA/g, voltage range is 1.5V to 4.8V, reversible capacity 200mAh/g, recycles 50 capacity and keeps
Rate is 82%.
The FeF of 5 70nm of embodiment3Hybrid energy-storing system of the nanosphere as positive electrode active materials
By the FeCl of 100mL 1mol/L3Aqueous solution be added to excessive 10% NaOH aqueous solution (concentration 1mol/L)
In, Fe (OH) is obtained after stirring 20min3Precipitating, and be aged 12h, then filter and wash.Excessive HF solution is added to again
It in the precipitating, is encapsulated in the bottle of PTFE, persistently stirs 12h at 70 DEG C.Then it filters and washs, in 80 DEG C of vacuum drying oven
In dry overnight, FeF can be obtained3Nanosphere.
With the FeF of 70nm or so3Nanosphere is as positive electrode active materials, and super P is as conductive agent, and PVDF is as bonding
Agent, in mass ratio 7:2:1 are prepared into anode；Using lithium piece as cathode, electrolyte is that (solvent is commercialized 5V lithium-ion electrolyte
Ethylene carbonate (EC) and dimethyl carbonate (DMC) are mixed by 1:1 volume ratio, and solute is the LiPF of 1mol/L6), in argon gas gas
It is assembled into button cell in the glove box of atmosphere, then carries out electrochemical property test.First charge for the first time, after discharge.
Under the current density of 60mA/g, voltage range is 1.5V to 4.8V, and reversible capacity can achieve 300mAh/g or more；?
Under the current density of 600mA/g, voltage range is 1.5V to 4.8V, reversible capacity 250mAh/g, recycles 50 capacity and keeps
Rate is 85%.
Claims (7)
1. a kind of hybrid electrochemical energy storage system, including anode, cathode and electrolyte, which is characterized in that the activity of the anode
Material is nano material, chemical general formula MXy, wherein M is selected from Ti, V, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ta, Ru
With one of W element or a variety of, X is selected from one of O, S, Se, F, N and P element or a variety of, 0≤y≤5；The storage bodies
The charge/discharge capacity contribution sources of system are in the counterfeit potential of absorption and embedded reactive, the electrochemical reaction process of the counterfeit potential of absorption
As follows: during the charging process, electrolysis solution anion is attracted in the surface of active material of anode, while being electrolysed solution anion quilt
Oxidation；During discharge, electrolysis solution anion is desorbed from the surface of active material of anode, while being electrolysed solution anion and being gone back
It is former.
2. hybrid electrochemical energy storage system as described in claim 1, which is characterized in that the active material of the anode is at least
Nano material of the size in one dimension less than 100 nanometers.
3. hybrid electrochemical energy storage system as described in claim 1, which is characterized in that the active material of the anode is nanometer
Particle, nanometer sheet, nano wire or unbodied nano material.
4. hybrid electrochemical energy storage system as described in claim 1, which is characterized in that the active material MX of the anodeyIn, M
For one of Mn, Fe, Co, Ni, Nb, Mo, Ta, Ru and W element or a variety of, one of X O, S and F element or a variety of, 0
≤y≤5。
5. hybrid electrochemical energy storage system as described in claim 1, which is characterized in that the active material of the anode is selected from down
One of column material is a variety of: Mn3O4、MnO2、Mn5O8、RuO2、Fe2O3、Fe3O4、NiO、MoS2And FeF3。
6. the hybrid electrochemical energy storage system as described in Claims 1 to 5 is any, which is characterized in that the hybrid electrochemical storage
Energy system is lithium ion battery；The cathode is negative electrode of lithium ion battery；The electrolyte is 5V high-voltage lithium ion batteries electricity
Solve liquid.
7. hybrid electrochemical energy storage system as claimed in claim 6, which is characterized in that the anion of the electrolyte is PF6 -、
ClO4 -、BF4 -One of or it is a variety of.
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| CN110148526A (en) * | 2019-04-24 | 2019-08-20 | 金华莱顿新能源科技有限公司 | A kind of ZnSN nano-material and preparation method thereof for supercapacitor |
| CN110148526B (en) * | 2019-04-24 | 2021-05-04 | 金华莱顿新能源科技有限公司 | ZnSN nanowire material for super capacitor and preparation method thereof |
| CN111313019A (en) * | 2020-01-19 | 2020-06-19 | 贵州梅岭电源有限公司 | Ultrahigh-power-output high-voltage positive electrode material for thermal battery |
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