CN106872905A - A kind of full battery parameter acquisition methods of monomer lithium ion - Google Patents
A kind of full battery parameter acquisition methods of monomer lithium ion Download PDFInfo
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Abstract
The present invention provides a kind of full battery parameter acquisition methods of monomer lithium ion, belongs to new energy research field.Comprise the following steps:Step one:Set up lithium ion battery electrochemical impedance spectrum Mathematical Modeling;Step 2:Survey the electrochemical impedance spectroscopy of the full battery of monomer lithium ion to be measured;Step 3:According to the Mathematical Modeling set up, the electrochemical impedance spectroscopy to surveying carries out frequency-division section parameter identification, obtains the both positive and negative polarity parameter of the full battery of monomer lithium ion to be measured.When the present invention is used for full battery for existing half-cell model, the defect of parameter identification effect difference, the characteristics of being composed with reference to lithium ion battery electrochemical impedance, by the way of a kind of frequency-division section parameter identification, can quickly, be accurately obtained the positive and negative electrode model parameter of the full battery of lithium ion.The present invention carries out Analysis on ageing mechanism, SOC and estimates and life prediction for lithium ion battery.
Description
Technical field
The present invention relates to a kind of parameter acquiring method of lithium ion battery, more particularly to a kind of full battery ginseng of monomer lithium ion
Number acquisition methods, belong to new energy research field.
Background technology
Lithium ion battery has the outstanding advantages such as high, big, the good cycle memory-less effect of energy density of voltage, obtains
It is widely applied.In the research of lithium ion battery, electrochemical impedance spectroscopy (Electrochemical has been widely applied to
Impedance Spectroscopy, abbreviation EIS) technology, also known as ac impedance spectroscopy, being characterized in can be for electrochemical impedance spectroscopy
The processes such as the interfacial reaction of electrode interior, load transfer, diffusion are effectively decoupled with the form of complex impedance in frequency domain, its measurement, analysis
Technology is widely used in the characteristic description of battery, and then can analyze battery status, improves battery and prepares.EIS technologies are also
The health state evaluation of battery provides basis for estimation, but is used for speed, the electrode of qualitative analysis inside battery process at present
The aspects such as the difficulty or ease of reaction, it is less to be applied to battery management.
Lithium ion battery electrochemical impedance spectrum Mathematical Modeling is the theory of and concentrated solution theoretical based on porous electrode, in mathematics
On describe in the condensation product that electrochemical reaction and single particle are constituted electric charge transfer, condensation product model is extended to porous electricity
Pole, accurately describes the structure of the electrode/electrolyte interface of main active substances particle, and establish electrochemical reaction and
The analytic formula of the electric charge transfer in condensation product, with precision higher.But the model is a half-cell model, it is used for half
The research of battery, three electrode lithium ion batteries (carrying reference electrode), and current commercial Li-ion battery is generally two electrodes
Full battery (referred to as full battery), if the model is used for the full battery of lithium ion, needs two model superpositions of positive and negative electrode to obtain
To full battery model, now, model parameter is excessive, intercouples, and the required identification time is long, precision is very low, therefore the model is difficult
To be applied in two electrode lithium ion batteries.
The content of the invention
Present invention offer is a kind of to be combined the electrochemical impedance spectroscopy Mathematical Modeling and parameter identification of half-cell and improves ginseng
The full battery parameter acquisition methods of monomer lithium ion of number identification precision.
A kind of full battery parameter acquisition methods of monomer lithium ion of the invention, methods described comprises the following steps:
Step one:Set up lithium ion battery electrochemical impedance spectrum Mathematical Modeling;
Step 2:Survey the electrochemical impedance spectroscopy of the full battery of monomer lithium ion to be measured;
Step 3:According to the Mathematical Modeling set up, the electrochemical impedance spectroscopy to surveying carries out frequency-division section parameter identification, obtains
The both positive and negative polarity parameter of the full battery of monomer lithium ion to be measured.
Preferably, the step 3 includes:
In the high band of actual measurement electrochemical impedance spectroscopy, electrochemical impedance spectroscopy is solved using the impedance Mathematical Modeling set up
Analysis, parameter identification is carried out using genetic algorithm, obtains the negative pole parameter of the full battery of monomer lithium ion to be measured;
In electrochemical impedance spectroscopy is surveyed, low-frequency range, electrochemical impedance spectroscopy is entered using the impedance Mathematical Modeling set up
Row parsing, parameter identification is carried out using genetic algorithm, obtains the positive pole parameter of the full battery of monomer lithium ion to be measured.
Preferably, the lithium ion battery electrochemical impedance spectrum Mathematical Modeling of foundation includes:
The single particle impedance of SEI films is not considered:
Wherein, load transfer resistance Rct=RT/ (i0F), R represents gas constant, and T represents temperature, i0Represent exchange current density,
F represents Faraday constant, and κ takes 1, j and represents imaginary number, and ω represents frequency,Represent local derviation of the potential to concentration, CdlRepresent double electricity
Layer capacitance;
Transmission function:RppRepresent particle
Radius, DsRepresent solid phase diffusion welding;
Consider the single particle impedance of SEI films:
Wherein, R0Represent ohmic internal resistance, ZseiRepresent the impedance of SEI films, CseiRepresent the electric capacity of SEI films;
The impedance of SEI moulds:
Wherein, intermediate variableDseiRepresent the diffusion coefficient in SEI films, δ 'sei=δsei-δdl, δsei
Represent the thickness of SEI films, δdlRepresent electrical double-layer thickness, σseiRepresent the electrical conductivity of SEI films, R2=Rpp+δdl, R3=R2+δ′sei;
Condensation product impedance:
Wherein, function is introducedIntermediate variable D△,e=D+,e-D-,e, D+,eRepresent positive pole liquid
Phase diffusion coefficient, D-,eRepresent negative pole Liquid Diffusion Coefficient, τspTortuosity in condensation product is represented,Represent electrolysis in condensation product
Plastid fraction, σeRepresent liquid phase electrical conductivity, RspRepresent condensation product radius, crefRepresent lithium ion reference concentration;
Porous electrode impedance:
Wherein, intermediate variableL represents thickness of electrode,Represent electrolyte volume fraction, τpeElectrode
Middle tortuosity,Disturbance component Liquid Diffusion Coefficient, DeLiquid Diffusion Coefficient,
The condensation product impedance of table 1 and the part relevant parameter of porous electrode impedance
Intermediate variable ζ=D△,e/De, intermediate variableZppTakeOrIntermediate variablet+Represent lithium ion transference number.
Preferably, the step 2 using constant potential electrochemical in-situ impedance spectrum method of testing survey monomer lithium to be measured from
The electrochemical impedance spectroscopy of sub full battery.
Preferably, in the step 2:Sinusoidal voltage amplitude during test elects 5mV~10mV, the height of test frequency as
Frequency higher limit is 1000Hz, and the low-frequency minimum of test frequency is 0.01Hz, and room temperature residing for the full battery of monomer lithium ion to be measured is 25
℃。
Above-mentioned technical characteristic can in any suitable manner be combined or substituted by equivalent technical characteristic, as long as can reach
To the purpose of the present invention.
The beneficial effects of the present invention are the present invention is used for existing lithium ion battery electrochemical impedance spectrum Mathematical Modeling
When full battery, the defect of parameter identification effect difference the characteristics of being composed with reference to lithium ion battery electrochemical impedance, is divided using one kind
The mode of section parameter identification, can quickly, be accurately obtained the positive and negative electrode model parameter of the full battery of lithium ion, realize that the model exists
Direct application in commercialized Study on Li-ion batteries, be using the model lithium ion battery is carried out Analysis on ageing mechanism,
SOC estimations, life prediction etc. lay the foundation.
Brief description of the drawings
Fig. 1 is schematic flow sheet of the invention.
Fig. 2 is the schematic flow sheet of genetic algorithm.
Fig. 3 is the electrochemical impedance spectrogram of the full battery of monomer lithium ion of actual measurement.
Fig. 4 is using the actual measurement electrochemical impedance spectroscopy and emulation electrochemical impedance spectrogram of the inventive method.
Specific embodiment
Below in conjunction with the accompanying drawing in the embodiment of the present invention, the technical scheme in the embodiment of the present invention is carried out clear, complete
Site preparation is described, it is clear that described embodiment is only a part of embodiment of the invention, rather than whole embodiments.It is based on
Embodiment in the present invention, those of ordinary skill in the art obtained on the premise of creative work is not made it is all its
His embodiment, belongs to the scope of protection of the invention.
It should be noted that in the case where not conflicting, the embodiment in the present invention and the feature in embodiment can phases
Mutually combination.
The invention will be further described with specific embodiment below in conjunction with the accompanying drawings, but not as limiting to the invention.
Present embodiment, a kind of full battery parameter acquisition methods of monomer lithium ion of present embodiment, bag are illustrated with reference to Fig. 1
Include following steps:
Step one:Set up lithium ion battery electrochemical impedance spectrum Mathematical Modeling;
Step 2:Survey the electrochemical impedance spectroscopy of the full battery of monomer lithium ion to be measured;
Step 3:According to the Mathematical Modeling set up, the electrochemical impedance spectroscopy to surveying carries out frequency-division section parameter identification, obtains
The both positive and negative polarity parameter of the full battery of monomer lithium ion to be measured.
The lithium ion battery electrochemical impedance spectrum Mathematical Modeling that present embodiment step one is set up is half-cell model, step
Two survey be full battery electrochemical impedance spectroscopy, use frequency-division section parameter identification in step 3, it is quick, to be accurately obtained lithium ion complete
The positive and negative electrode model parameter of battery, that is, obtain the parameter of the full battery of monomer lithium ion to be measured.
In preferred embodiment, step 3 includes:
In the high band of actual measurement electrochemical impedance spectroscopy, electrochemical impedance spectroscopy is solved using the impedance Mathematical Modeling set up
Analysis, parameter identification is carried out using genetic algorithm, obtains the negative pole parameter of the full battery of monomer lithium ion to be measured;
In electrochemical impedance spectroscopy is surveyed, low-frequency range, electrochemical impedance spectroscopy is entered using the impedance Mathematical Modeling set up
Row parsing, parameter identification is carried out using genetic algorithm, obtains the positive pole parameter of the full battery of monomer lithium ion to be measured.
The genetic algorithm of present embodiment is to use for reference biological natural selection and genetic evolution mechanism and one kind for developing is complete
Office's optimization adaptive probability searching algorithm, is illustrated to genetic algorithm below.
Assuming that the problem for needing optimization is:
Wherein X is parameter set to be identified, using real-valued coding, includes NdIndividual parameter to be identified;S is search space, is had:
Lower and Upper are respectively search space lower bound and the upper bound of each parameter to be identified.Algorithm flow chart such as Fig. 2 institutes
Show.
In embodiments, the object function that genetic algorithm determines is set to:
Wherein, N is the frequency number in electrochemical impedance spectroscopy test,WithRespectively actual measurement electrochemistry resistance
The real part and imaginary part of anti-spectrum,WithRespectively emulate the real part and imaginary part of electrochemical impedance spectroscopy.α is empty for adjustment
The power of portion's proportion in object function.Because the imaginary part of lithium ion battery impedance is more sensitive to low frequency, thus object function it is high,
In, the power used by low frequency be different, frequency is lower, and weight is bigger.
In the electrochemical impedance spectroscopy of lithium ion battery, the battery impedance under high band is arranged by negative pole, in low-frequency range
It is main to be contributed by positive pole.Battery impedance under high band is that high-frequency region is to pass through SEI with lithium ion by negative pole domination reason
The relevant semicircle of film, and the SEI films of negative pole play a major role;Additionally, SEI films are sufficiently stable, normally used in lithium ion battery
Will not be varied widely with during the whole charge and discharge circulation life of battery, therefore GND impedance is kept approximately constant.
The impedance of full battery is main to be contributed by positive pole, and cathode impedance is smaller, stable, and battery impedance increase in use is also
Because positive pole impedance is caused, therefore in middle low-frequency range, the impedance of full battery can be replaced with positive pole impedance.
In sum, present embodiment employs the method for frequency-division section identification and realizes half-cell model in the full electricity of commercialization
Application on pond, realizes the decoupling of battery positive and negative electrode parameter, can respectively obtain more accurate positive and negative electrode parameter.
The frequency range that the high band of present embodiment refers to frequency more than 30Hz, in, low-frequency range refer to that frequency is less than 20Hz
Frequency range.
In preferred embodiment, the lithium ion battery electrochemical impedance spectrum Mathematical Modeling of foundation includes:
In the impedance modeling of single particle, by the controlling party of the system under the excitation to the small sinusoidal signal of frequencies omega
Impedance response is set up in the solution of journey, shown in the single particle impedance such as formula (4) and (5) that obtains.
The single particle impedance of SEI films is not considered:
Wherein, load transfer resistance Rct=RT/ (i0F), R represents gas constant, and T represents temperature, i0Represent exchange current density,
F represents Faraday constant, and κ takes 1, j and represents imaginary number, and ω represents frequency,Represent local derviation of the potential to concentration, CdlRepresent double electricity
Layer capacitance;
Transmission function:
RppRepresent particle radii, DsRepresent solid phase diffusion welding;
Consider the single particle impedance of SEI films:
Wherein, R0Represent ohmic internal resistance, ZseiRepresent the impedance of SEI films, CseiRepresent the electric capacity of SEI films;
The impedance of SEI moulds:
Wherein, intermediate variableDseiRepresent the diffusion coefficient in SEI films, δ 'sei=δsei-δdl, δsei
Represent the thickness of SEI films, δdlRepresent electrical double-layer thickness, σseiRepresent the electrical conductivity of SEI films, R2=Rpp+δdl, R3=R2+δ′sei;
It is, come average microcosmic equation, such as to use volume-average approach by representative volume unit in condensation product impedance is built and touched
Average liquid phase governing equation etc., the condensation product impedance for obtaining:
Wherein, function is introducedIntermediate variable D△,e=D+,e-D-,e, D+,eRepresent positive pole liquid phase
Diffusion coefficient, D-,eRepresent negative pole Liquid Diffusion Coefficient, τspTortuosity in condensation product is represented,Represent electrolyte in condensation product
Volume fraction, σeRepresent liquid phase electrical conductivity, RspRepresent condensation product radius, crefRepresent lithium ion reference concentration;
According to porous electrode is theoretical, concentrated solution is theoretical that condensation product impedance model expanded into porous electrode impedance modeling,
Porous electrode impedance:
Wherein, intermediate variableL represents thickness of electrode,Represent electrolyte volume fraction, τpeElectrode
Middle tortuosity,Disturbance component Liquid Diffusion Coefficient, DeLiquid Diffusion Coefficient,
The condensation product impedance of table 1 and the part relevant parameter of porous electrode impedance
Intermediate variable ζ=D△,e/De, intermediate variableZppRepresent single particle impedance, intermediate variablet+Represent lithium ion transference number.Totally 26 parameters in the model, wherein 6 parameter values are, it is known that 19 need
The parameter to be recognized.Known parameter mainly includes that physical constant and a part are consulted by pertinent literature and handbook of batteries
The parameter for arriving, as shown in table 2.Needing the parameter of identification includes unknown parameter and changing during cell degradation
Parameter, as shown in table 3.
The lithium ion battery impedance model known parameters of table 2
Symbol | Physical significance | Unit | Remarks |
Reference concentration | It is relevant with battery size | ||
L | Thickness of electrode | m | It is relevant with battery size |
Lithium ion transference number | - | It is relevant with battery size | |
R | Gas constant | 8.3143 | |
F | Faraday constant | 96485 | |
T | Temperature | K | 295.15 |
The lithium ion battery impedance model of table 3 parameter to be identified
The test mode of electrochemical impedance spectroscopy generally persevering testing current and constant potential tests two kinds of test modes.Constant current
It is the compound electric flow valuve obtained by a DC current (can be 0) one sinusoidal current of superposition to the excitation of battery that test refers to, together
When measuring system alternating voltage response, the ratio according to voltage and current can obtain impedance;Constant potential test refers to swashing for battery
The sinusoidal voltage that encouraging is to be determined with an amplitude by a constant voltage is superimposed the composite voltage value for obtaining, while the alternating current of measuring system
Stream response, the ratio according to voltage and current can obtain impedance.
In the test of lithium ion battery, the mode according to constant current is measured, then battery will be in discharge and recharge
In the case of, cause testing impedance inaccurate, so the step of present embodiment two is surveyed using constant potential electrochemical in-situ impedance spectrum
Method for testing surveys the electrochemical impedance spectroscopy of the full battery of monomer lithium ion to be measured.It is permanent in the original location in electrochemical impedance spectroscopy method of testing
Determine the open-circuit voltage that current potential is set to battery, can so ensure to test keeping being carried out under stable state in inside battery, this
The mode of kind is referred to as the test of constant potential in situ EIS.
In electrochemical impedance spectroscopy test process, the sinusoidal voltage amplitude of test can not be too high, otherwise easily influences battery
System linearity feature, the sinusoidal voltage amplitude of test is too low, it is impossible to effectively encourage battery system, general sinusoidal voltage amplitude
Elect 5mV~10mV as;Measurement frequency scope considers the applying frequency scope of model and the practical significance of electrochemical impedance spectroscopy, typically
The high frequency limit value for taking frequency is 1000Hz, it is contemplated that accuracy that electrochemical workstation is measured at low frequency, time of measuring are long
It is short, can be on the premise of reaction cell dispersal behavior in satisfactionization electrochemical impedance spectroscopy, the low-frequency minimum for using is 0.01Hz;This
Outward, the electrochemical impedance spectroscopy all to battery such as constant temperature time, duration of maintenance open-circuit voltage tests important.
The measuring apparatus of present embodiment are including CS impedance spectrums tester, PC, battery tray, fixture etc..Mesuring battary is
Samsung's production model ICR18650-22F lithium ion batteries, capacity is 2200mhA, in actual measurement, sinusoidal voltage amplitude
Elect 10mV as;Measurement frequency scope is 0.01~1000Hz, and room temperature is 25 DEG C, the electrochemical impedance spectroscopy for measuring as shown in figure 3, resistance
Anti- frequency spectrum is often represented with nyquist diagram, it should be noted that Nyquist figures custom is with-Z in electrochemistry " it is the longitudinal axis, with Z '
It is transverse axis.The electrochemical impedance spectroscopy of lithium ion battery is generally by high, two capacitive semicircles of intermediate frequency and an oblique line group of low frequency
Into.Wherein, SEI films relevant semicircle is passed through during high-frequency region with lithium ion diffusive migration;Mid-frequency region is and charge transfer mistake
The semicircle of Cheng Youguan;The oblique line relevant with lithium ion solid-state diffusion during low frequency region.
The positive and negative electrode parameter of lithium ion battery is obtained using the method for step 3 as shown in table 4, table 5, table 6.Using identification
The emulation electrochemical impedance spectroscopy that the parameter for obtaining is obtained is as shown in Figure 4 with actual electrochemical impedance spectroscopy.
The lithium ion battery impedance model known parameters of table 4
Symbol | Physical significance | Unit | Value |
Reference concentration | 1000 | ||
Thickness of electrode (positive pole) | m | 2.4e-05 | |
Thickness of electrode (negative pole) | m | 1.67e-05 | |
Lithium ion transference number | - | 0.35 | |
R | Gas constant | 8.3143 | |
F | Faraday constant | 96485 | |
T | Temperature | K | 295.15 |
The positive pole lithium ion battery impedance model parameter of table 5
The negative electrode lithium ion battery impedance model parameter of table 6
Although describing the present invention herein with reference to specific implementation method, it should be understood that, these realities
Apply the example of example only principles and applications.It should therefore be understood that can be carried out to exemplary embodiment
Many modifications, and other arrangements are can be designed that, without departing from the spirit of the invention that appended claims are limited
And scope.It should be understood that can be by way of different from described by original claim come with reference to different appurtenances
Profit is required and feature specifically described herein.It will also be appreciated that the feature with reference to described by separate embodiments can be used
In other described embodiments.
Claims (5)
1. full battery parameter acquisition methods of a kind of monomer lithium ion, it is characterised in that methods described comprises the following steps:
Step one:Set up lithium ion battery electrochemical impedance spectrum Mathematical Modeling;
Step 2:Survey the electrochemical impedance spectroscopy of the full battery of monomer lithium ion to be measured;
Step 3:According to the Mathematical Modeling set up, the electrochemical impedance spectroscopy to surveying carries out frequency-division section parameter identification, obtains to be measured
The both positive and negative polarity parameter of the full battery of monomer lithium ion.
2. a kind of full battery parameter acquisition methods of monomer lithium ion according to claim 1, it is characterised in that the step
Three include:
In the high band of actual measurement electrochemical impedance spectroscopy, electrochemical impedance spectroscopy is parsed using the impedance Mathematical Modeling set up,
Parameter identification is carried out using genetic algorithm, the negative pole parameter of the full battery of monomer lithium ion to be measured is obtained;
In electrochemical impedance spectroscopy is surveyed, low-frequency range, electrochemical impedance spectroscopy is solved using the impedance Mathematical Modeling set up
Analysis, parameter identification is carried out using genetic algorithm, obtains the positive pole parameter of the full battery of monomer lithium ion to be measured.
3. a kind of full battery parameter acquisition methods of monomer lithium ion according to claim 2, it is characterised in that the lithium of foundation
Ion battery electrochemical impedance spectroscopy Mathematical Modeling includes:
The single particle impedance of SEI films is not considered:
Wherein, load transfer resistance Rct=RT/ (i0F), R represents gas constant, and T represents temperature, i0Exchange current density is represented, F is represented
Faraday constant, κ takes 1, j and represents imaginary number, and ω represents frequency,Represent local derviation of the potential to concentration, CdlRepresent electric double layer electricity
Hold;
Transmission function:RppRepresent particle half
Footpath, DsRepresent solid phase diffusion welding;
Consider the single particle impedance of SEI films:
Wherein, R0Represent ohmic internal resistance, ZseiRepresent the impedance of SEI films, CseiRepresent the electric capacity of SEI films;
The impedance of SEI moulds:
Wherein, intermediate variableDseiRepresent the diffusion coefficient in SEI films, δ 'sei=δsei-δdl, δseiRepresent
The thickness of SEI films, δdlRepresent electrical double-layer thickness, σseiRepresent the electrical conductivity of SEI films, R2=Rpp+δdl, R3=R2+δ′sei;
Condensation product impedance:
Wherein, function is introducedIntermediate variable D△,e=D+,e-D-,e, D+,eRepresent the diffusion of positive pole liquid phase
Coefficient, D-,eRepresent negative pole Liquid Diffusion Coefficient, τspTortuosity in condensation product is represented,Represent electrolyte volume in condensation product
Fraction, σeRepresent liquid phase electrical conductivity, RspRepresent condensation product radius, crefRepresent lithium ion reference concentration;
Porous electrode impedance:
Wherein, intermediate variableL represents thickness of electrode,Represent electrolyte volume fraction, τpeIt is bent in electrode
The folding factor,Disturbance component Liquid Diffusion Coefficient, DeLiquid Diffusion Coefficient,
The condensation product impedance of table 1 and the part relevant parameter of porous electrode impedance
Intermediate variable ζ=D△,e/De, intermediate variableZppTakeOrIntermediate variable
t+Represent lithium ion transference number.
4. full battery parameter acquisition methods of a kind of monomer lithium ion according to Claims 2 or 3, it is characterised in that described
Step 2 surveys the electrochemical impedance of the full battery of monomer lithium ion to be measured using constant potential electrochemical in-situ impedance spectrum method of testing
Spectrum.
5. a kind of full battery parameter acquisition methods of monomer lithium ion according to claim 4, it is characterised in that the step
In two:Sinusoidal voltage amplitude during test elects 5mV~10mV as, and the high frequency limit value of test frequency is 1000Hz, test frequency
Low-frequency minimum be 0.01Hz, room temperature residing for the full battery of monomer lithium ion to be measured be 25 DEG C.
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