CN109037811A - A kind of charging method of graphite cathode system lithium ion battery - Google Patents
A kind of charging method of graphite cathode system lithium ion battery Download PDFInfo
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Abstract
The present invention relates to a kind of charging methods of graphite cathode system lithium ion battery, by the incremental multistage constant-current charge initial charge process of one rate of charge of setting, charging process and a constant-voltage charge process among the multistage constant-current charge that a rate of charge successively decreases.Each stage rate of charge in initial charge process increases with SOC (state-of-charge) and is increased, and each stage rate of charge in intermediate charging process increases with SOC and reduced.Charging method of the invention has fully considered the process of intercalation and analysis lithium process of cathode graphite particle from electrochemistry level, it avoids the destruction of graphite cathode crystal structure and analyses battery capacity caused by lithium and lose, the cycle life of graphite cathode system lithium ion battery can either be improved, and the charging time charged within the scope of 20%~80%SOC can be shortened.
Description
Technical field
The invention belongs to battery boosting technology fields, and in particular to a kind of charging side of graphite cathode system lithium ion battery
Method.
Background technique
In the prior art, there are three kinds of method of charging lithium-ion battery, respectively based on charging method, the base for inhibiting temperature rise
In the charging method of SOC (battery charge state or remaining capacity) and based on the charging method for inhibiting polarizing voltage.
It wherein, will be warm based on inhibiting the charging method real-time estimation lithium ion battery of temperature rise to charge the temperature rise in each stage
Rise the most short electric current that each stage of charging is designed as target of minimum charging time.Charging method based on SOC thinks that SOC is got over
The maximum charging current that low lithium ion battery can bear is bigger, i.e. the entire charging process from SOC=0% to SOC=100%
In, the charging current of the charging method is gradually reduced with the increase of SOC.Charging method based on inhibition polarizing voltage thinks pole
Change the main reason for voltage is limiting lithium ion cell large current charge, this method is using polarizing voltage when reducing charging as mesh
, the constant-current phase in conventional constant current constant-voltage charge is divided into Multi-section constant current charging, electric current is added among each constant-current charging phase
The of short duration discharge regime for stopping the stage of filling or electric current is negative for being zero.
The most of temperature rise that only considered in formulation process in charging process of the charging method of above-mentioned lithium ion battery,
The external parameter of the batteries such as SOC, polarizing voltage seldom considers the electrochemical properties of inside lithium ion cell, especially for stone
Black negative electrode series lithium ion battery, charges the battery according to the above method, not can avoid the destruction of graphite cathode crystal structure
It is lost with battery capacity caused by analysis lithium, battery life is caused to reduce.
Summary of the invention
For based on the charging method for inhibiting temperature rise, close to the lithium-ion electric of full power state when temperature excessively high (60 DEG C or more)
Pond positive electrode oxidisability greatly enhances, and really it is possible that oxidation electrolyte releases gas and heat, leads to the rotten electricity of electrolyte
Pond bulge even thermal runaway.But at 55 DEG C hereinafter, the temperature rise of battery be instead be conducive to lithium ion from positive deintercalation, be electrolysed
It spreads and is embedded in inside negative electrode material in liquid, that is, be conducive to the progress of charging process.This is also why the internal resistance of cell is with temperature
It increases and reduces.So temperature rise should not be used as formulating the foundation of charging method, one higher temperature of setting of correct way
The upper limit only just considers influence of the temperature to charging process as secure threshold when battery temperature is more than the secure threshold.
For the charging method based on SOC, as charging progresses, when lithium ion battery SOC is more than that (20% is left for certain value
It is right) when, the position due to being easy embedding lithium in the progress cathode graphite particle with charging process gradually decreases, and lithium ion battery can
The maximum charging current of receiving is also gradually reduced really.But when electric quantity of lithium ion batteries is relatively low (SOC is about within 20%)
When, the maximum charging current that the lithium ion battery of graphite cathode system can bear is the increase with SOC and increases.This is needed
It is explained in terms of the electrochemical properties of graphite cathode lithium ion battery.Cathode graphite particle is layer structure, works as SOC=0
When, amount containing lithium is seldom in graphite particle stratiform structure, and graphite layers are away from being in minimum value.It is equal to a certain value from SOC=0 to SOC
In the charging process of (about 20%), as SOC is gradually increased, lithium-inserting amount gradually increases in graphite linings, and graphite layers are away from also gradually
Become larger；And as SOC increases, graphite layers are gradually reduced away from the speed to become larger.When SOC is more than a certain value (about 20%),
Graphite layers amount containing lithium is enough, and graphite layers are in maximum value away from no longer becoming larger substantially with SOC.Therefore at very low SOC
If directly start high current quick charge, the graphite linings on graphite particle surface quickly embedding lithium and cause interlamellar spacing to become larger rapidly；And
Graphite linings inside graphite particle have little time to be embedded in enough lithiums, and graphite layers are away from still very little.In this way, graphite particle surface layer and
Stress between inside is very big, it is possible to cause C-C chemical bond rupture, crystal structure of graphite to destroy, so as to cause available graphite
The loss of negative electrode material.The destruction of crystal structure of graphite caused by low SOC high current quick charge can be from graphite cathode material
Raman spectrum in observe and obtaining.
In addition, with the reduction of SOC, cathode graphite particle surface charge transfger impedance increases rapidly when SOC is lower than 10%
Greatly；Under identical charging current, the potential of cathode will also be reduced rapidly with the increase of Charge-transfer resistance, work as negative potential
Lower than 0 volt (relative to Li/Li+) when, negative electrode material surface will have the risk that analysis lithium occurs.So being filled with the reduction of SOC
Electric current should also be as reducing, and to offset the trend of negative potential reduction, prevent cathode from analysing lithium.Crystal structure of graphite meets in order to prevent
Generation analysis lithium under to destruction and low SOC, the maximum charging current that graphite cathode lithium ion battery can bear in the low SOC stage,
It should be the one section of curve similar to exponential relationship being gradually increased with the increase of SOC.
For filling or filling-putting-using-stopping-is filled the charging method filled is really based on the charging method for inhibiting polarizing voltage
The lithium concentration polarization being able to suppress in cathode graphite particle；By suspending embedding lithium or by the high concentration lithium deintercalation on graphite particle surface layer
Fall a part to reduce the concentration of lithium in graphite particle surface layer, lithium concentration is made to be intended to uniformly, prevent graphite particle surface layer mistake
It charges and analysis lithium occurs or generate lithium Zhi Jing.But this inhibition polarized to lithium concentration is only stopping fill or discharge period and the period
Near work, will be re-established rapidly in other constant-current charging phases, cathode graphite particle lithium concentration polarization.In this way
It is filling-stopping-to fill-in the charging cycle for stopping (or fill-put-filling-to put), if charging time/stop fills the time (or charging time/electric discharge
Time) setting it is excessive, do not have prevent analysis lithium effect；If what is be arranged is too small, charging time and electric discharge fever will all increase greatly
Greatly.It in order to shorten the charging time, fills-stopping-and fills and-stop in the charging method of (or fill-put-filling-to put) often by the electricity of charging stage
Stream is arranged bigger, and the lithium concentration polarization re-established in such graphite particle also will be bigger, be more likely to result in analysis lithium.In addition
The charging method of this positive negative pulse stuffing will make charging equipment become extremely complex.
In fact, appropriate polarize not will lead to cathode analysis reason not only when charging, be conducive to improve lithium ion battery instead
Charging rate；The polarization lithium concentration difference of graphite particle inside and outside is conducive to improve lithium to the diffusion velocity inside graphite particle.
In fact, it can guarantee that not analysing lithium does not injure battery as long as the maximum charging current that can bear with lithium ion battery persistently charges
Under the premise of in the shortest possible time complete charging；The polarization generated during this is conducive to accelerate charging rate.
Based on above-mentioned consideration, the object of the present invention is to provide a kind of charging method of graphite cathode system lithium ion battery,
Cathode analysis reason and destruction graphite cathode crystal are easy to cause for solving existing graphite cathode system method of charging lithium-ion battery
The problem of structure causes battery life to reduce.
In order to solve the above technical problems, the present invention proposes a kind of charging method of graphite cathode system lithium ion battery, packet
Include following steps:
Constant-current charge is carried out, the process of constant-current charge includes initial charging phase and intermediate charging stage, and detection battery is surplus
Remaining electricity is initial charging phase when battery dump energy is less than or equal to the first setting value, when battery dump energy is greater than
It is the intermediate charging stage when the first setting value；
Initial charging phase is divided into two first group of more than small stage constant-current charging phases, i.e. first group of constant current is filled
It include more than two sub-stages (small stage) that each sub-stage is correspondingly arranged in first group of constant-current charging phase in the electric stage
Rate of charge increases as battery dump energy increases；
The intermediate charging stage is divided into two second group of more than small stage constant-current charging phases, i.e. second group of constant current is filled
It include more than two sub-stages (small stage) that each sub-stage is correspondingly arranged in second group of constant-current charging phase in the electric stage
Rate of charge reduces as battery dump energy increases.
The considerations of the present invention is based on the electrochemical properties of graphite cathode system inside lithium ion cell, by being arranged first group
Constant-current charging phase and second group of constant-current charging phase, in first group of constant-current charging phase, the rate of charge that is correspondingly arranged with
Battery dump energy increase and increase, the rate of charge being correspondingly arranged in second group of constant-current charging phase is with remaining battery
Electricity increases and reduces, and avoids the destruction of graphite cathode crystal structure and analyses battery capacity caused by lithium and lose, can either mention
The cycle life of high graphite cathode system lithium ion battery, and the charging time in the intermediate charging stage can be shortened.
Further, during constant-current charge, the end voltage of battery is detected, when the charging that the end voltage of battery reaches setting is cut
Only when voltage, stop constant-current charge, carries out constant-voltage charge.
Further, the battery dump energy range of first setting value is 15%~25%.
As further limiting for the rate of charge being correspondingly arranged to first group of constant-current charging phase, first group of constant-current charge
The rate of charge and battery dump energy that stage is correspondingly arranged are the first incremental exponential function relation.
As further limiting for the rate of charge being correspondingly arranged to second group of constant-current charging phase, second group of constant-current charge
The rate of charge and battery dump energy that stage is correspondingly arranged are the second exponential function relation to successively decrease.
In order to guarantee that rate of charge of the battery when low SOC charges is sufficiently small, further, first exponential function relation
Curvature be greater than the second exponential function relation curvature.
The excessively high influence that battery life is generated of battery temperature in order to prevent, further, during the constant-current charge,
When battery temperature reaches the first temperature upper limit of setting, the rate of charge for reducing current setting continues to charge；Work as battery temperature
When reaching the second temperature upper limit of setting, stop charging；The second temperature upper limit of setting is greater than the first temperature upper limit.
Specifically, when battery temperature is more than or equal to the first temperature upper limit and is less than the second temperature upper limit, according to detection
Environment temperature determines the reduction amplitude of rate of charge, and the range of decrease of environment temperature more charge rate is bigger.
Analysis lithium occurs when battery low temperature charges in order to prevent, further, when battery temperature is less than the lowest temperature of setting,
The rate of charge for reducing current setting continues to charge.And when battery temperature is less than the lowest temperature of setting, according to battery temperature
The reduction amplitude of rate of charge is determined with the difference of lowest temperature, and the range of decrease of the bigger rate of charge of difference is bigger.
Detailed description of the invention
Fig. 1 is a kind of charging method schematic diagram that experiment one of the invention provides；
Fig. 2 is to test the two normal charge method schematic diagrams provided；
Fig. 3 is to carry out the obtained discharge capacitance of cycle charge-discharge using the charging method of experiment one and experiment two
Test result figure.
Specific embodiment
A specific embodiment of the invention is further described with reference to the accompanying drawing.
The present invention proposes a kind of charging method of graphite cathode system lithium ion battery, comprising the following steps:
The charging process of graphite cathode lithium ion battery is divided into three charging stages, respectively initial charging phase, in
Between charging stage and last charging stage, initial charging phase includes the small rank of constant-current charge that is gradually increased of several rate of charge
Section, intermediate charging stage include the constant-current charge small stage that several rate of charge are gradually reduced, and the last charging stage is constant pressure
Charging stage.
The transformation of initial charging phase and intermediate charging stage according to being SOC=15%~25%, the intermediate charging stage with
The transformation foundation of last charging stage is that the end voltage of battery reaches the charge cutoff voltage of setting.
In order to avoid analysis lithium and crystal structure of graphite are destroyed when low SOC charging, each constant current is filled in initial charge process
The maximum charge multiplying power in electric stage should be close to incremental exponential function relation f relative to the SOC trend incrementally increased1(x).In order to
Avoid the analysis lithium occurred when larger SOC charging because of the overcharge of graphite particle part, each constant-current charge in intermediate charging process
The maximum charge multiplying power in stage should be close to the exponential function relation f to successively decrease relative to the SOC trend gradually reduced2(x), wherein f1
(x) curvature of function curve is greater than f2(x), this is because charging the destruction of crystal structure of graphite is occurred mainly in it is lower
SOC stage, f1(x) curvature of function curve is larger can guarantee that rate of charge when low SOC charges is sufficiently small.In practical application
First determine Functional Equation f1(x)、f2(x) and the division interval of initial charge process, SOC in intermediate charging process, further according to letter
The rate of charge of each constant-current charging phase in the determining initial charge process in the division interval of number equation and SOC, intermediate charging process.
Set the first temperature upper limit Tmax1With second temperature upper limit Tmax2, battery temperature is monitored in charging process, when battery temperature
Degree reaches temperature upper limit Tmax1When reduce rate of charge continue to charge, environment temperature is higher or battery radiating condition is poorer, the range of decrease
It is bigger；When battery temperature reaches temperature upper limit Tmax2When stop charging.
Set a lowest temperature Tmin, battery temperature is monitored in charging process, when battery temperature is less than TminWhen should reduce
Rate of charge, and battery temperature and TminThe bigger range of decrease of difference it is bigger.
In order to prove the validity of charging method of the present invention, carries out experiment one and experiment two compares and analyzes, experiment one
For charging method of the invention, experiment two is the charging method of conventional constant-current constant-voltage charging, and tests one with experiment two using phase
With the ferric phosphate lithium ion battery of graphite cathode system, the anode of battery is by 95.3%LiFePO4+ 2%PVDF+2.7%SP
(conductive agent) mixes, and the cathode of battery is mixed by 98% artificial graphite+1%SBR+1%CMC, diaphragm PP/PE/
PP composite membrane, electrolyte is by organic solvent (30%EC+30%PC+40%DEC), 1mol/L LiPF6With additive (0.5%
VC, 5%FEC, 4%VEC) composition.
Specifically, the process of experiment one is as follows:
At 23 DEG C of room temperature, charge according to method of charging lithium-ion battery of the present invention to battery, charging process such as Fig. 1 institute
Show, specifically includes the following steps:
The selected foundation that the intermediate charging stage is converted to from initial charging phase is SOC=20%, selected SOC=20%~
Rate of charge when 30% is 2.5C.
In " rate of charge-SOC " coordinate system in Fig. 1, initial charge mistake is determined with point (0,0.05) and (0.2,2.5)
Exponential function curve f in journey1(x), which can be regarded as the maximum charge times that battery can be born in initial charge process
Rate curve.Since the destruction of crystal structure of graphite occurs mainly within the scope of very low SOC, the curvature of the exponential function curve is answered
It is larger, set the exponential function curve equation are as follows:
f1(x)=b1+a1e5x
It solves equation, byIt obtainsThat is f1(x)=- 1.3758+
1.4258e5x。
In " rate of charge-SOC " coordinate system in Fig. 1, intermediate charged is determined with point (0.3,2.5) and (1,0.05)
The exponential function curve f of journey2(x), which can be regarded as the maximum charge multiplying power that battery in intermediate charging process can be born
Curve.Curve f2(x) curvature should compare f1(x) bent curvature of a curve is small, sets the exponential function curve equation are as follows:
f2(x)=b2+a2e-x
It solves equation, byIt obtainsThat is f2(x)=- 2.3668+
6.5694e-x。
It is divided into 10% between the division of selected SOC, further according to f1(x) and f2(x) equation i.e. can determine initial charge process and
The rate of charge (specific value is labeled in Fig. 1) of each constant-current charging phase in intermediate charging process, each constant-current charging phase
Rate of charge value should can bear maximum charge curve of double curvature or less in battery (see Fig. 1).Due to charging to crystal structure of graphite
Destruction be concentrated mainly on the lower SOC stage, 0%~10%SOC is divided into 0%~5%SOC and 5%~10% by the present invention
Two constant-current charging phases of SOC.Since the rate of charge of 0.05C is too small, the present invention is by 0%~5%SOC and 90%~100%
The rate of charge of two constant-current charging phases of SOC is set as 0.1C.
Since experiment one uses ferric phosphate lithium cell, can select charge cutoff voltage is 3.65v, works as battery in charging process
When end voltage reaches the charge cutoff voltage 3.65v of setting, switchs to constant-voltage charge, stop filling when rate of charge drops to 0.05C
Electricity.
Using ferric phosphate lithium cell, environment temperature is 23 DEG C for experiment of the invention, can the set temperature upper limit accordingly
Tmax1=45 DEG C, Tmax2=50 DEG C.The real-time detection battery temperature in entire charging process, fills when battery temperature reaches 45 DEG C
Electric multiplying power, which is reduced to, corresponds to the 80% of rate of charge in Fig. 1.When battery temperature drop to again 45 DEG C or less and continue after ten minutes,
It is charged again according to the rate of charge in Fig. 1 to battery according to current SOC.
It chooses 30 batteries and carries out 500 charge and discharge cycles tests, specific steps are as follows:
It is charged the battery using the charging method of present invention experiment one, is charged to 100%SOC from 0%SOC, shelves
20min discharges into SOC=10% with 1C discharge-rate, and then using small multiplying power 0.2C instead and discharging into battery terminal voltage is 2.5v, then
Shelve 20min.
After so repeating 499 times, the average discharge capacity conservation rate of 30 batteries is as shown in the curve 1 in Fig. 3.
The process of experiment two is as follows:
Under 23 DEG C of environment of room temperature, conventional constant-current constant-voltage charging is carried out using lithium ion battery identical with experiment one, such as
Shown in Fig. 2, the specific steps are as follows:
Since 0%SOC, with constant multiplying power 1C charging, it is charged to blanking voltage 3.65v always.It is filled with constant voltage 3.65v
Electricity stops charging when rate of charge is reduced to 0.05C.
It chooses 30 batteries and carries out 500 charge and discharge cycles tests, specific steps are as follows:
Using experiment two charging method charge, be charged to 100%SOC from 0%SOC, then according to experiment one in remember
The charging method of the circulation electric discharge of load discharges, the average discharge capacity conservation rate such as 2 institute of curve in Fig. 3 of 30 batteries
Show.
Completely be full of from Fig. 3 graphite cathode system lithium ion battery room temperature put cyclic test result can be seen that with it is conventional
Constant-current constant-voltage charging method is compared, and can significantly improve graphite cathode system lithium ion battery using the charging method in the present invention
Cycle life.
Upper table is the charging time comparison for testing one and experiment two, as can be seen from the table, if by lithium ion battery from putting
Sky is charged to full power state, i.e., is charged to 100%SOC from 0%SOC, then the time required for being charged using the charging method of experiment one
Experiment two will be far longer than；But it if being charged to 80%SOC from 20%SOC, is filled required for the charging method using experiment one
The electric time will be than testing two fast 5.3min；In particular, if being charged to 60%SOC from 20%SOC, using the charging method of experiment one
It will be than testing two fast 10.1min.Therefore, charging method of the invention is particularly suitable for quick within the scope of 20%~80%SOC
Quick boost charge within the scope of charging and 20%~60%SOC.The present invention tests filling outside 0%~100%SOC range
Although the electric time is long, avoids the destruction of graphite cathode crystal structure and analyse battery capacity caused by lithium and lose, it is effective to protect
Battery life is hindered.
In conclusion charging method of the invention has fully considered cathode graphite from electrochemistry level in formulation process
Grain process of intercalation and analysis lithium process, improved under the premise of ensureing graphite cathode system cycle life of lithium ion battery its
Charging rate when charging within the scope of 20%~80%SOC.
The foregoing is merely optimization experiments of the invention, are not intended to restrict the invention, for those skilled in the art
For, the invention may be variously modified and varied.All within the spirits and principles of the present invention, it is made it is any modification, etc.
With replacement, improvement etc., should be included within scope of the presently claimed invention.
Claims (10)
1. a kind of charging method of graphite cathode system lithium ion battery, which comprises the following steps:
Constant-current charge is carried out, the process of constant-current charge includes initial charging phase and intermediate charging stage, detection remaining battery electricity
Amount is initial charging phase when battery dump energy is less than or equal to the first setting value, when battery dump energy is greater than first
It is the intermediate charging stage when setting value；
Initial charging phase is divided into two first group of more than small stage constant-current charging phases, first group of constant-current charging phase
The rate of charge being correspondingly arranged increases as battery dump energy increases；
The intermediate charging stage is divided into two second group of more than small stage constant-current charging phases, second group of constant-current charging phase
The rate of charge being correspondingly arranged reduces as battery dump energy increases.
2. the charging method of graphite cathode system lithium ion battery according to claim 1, which is characterized in that constant-current charge
In the process, the end voltage for detecting battery stops constant-current charge when the end voltage of battery reaches the charge cutoff voltage of setting,
Carry out constant-voltage charge.
3. the charging method of graphite cathode system lithium ion battery according to claim 1, which is characterized in that described first
The battery dump energy range of setting value is 15%~25%.
4. the charging method of graphite cathode system lithium ion battery according to claim 1, which is characterized in that first group permanent
The rate of charge and battery dump energy that the current charge stage is correspondingly arranged are the first incremental exponential function relation.
5. the charging method of graphite cathode system lithium ion battery according to claim 1, which is characterized in that second group permanent
The rate of charge and battery dump energy that the current charge stage is correspondingly arranged are the second exponential function relation to successively decrease.
6. the charging method of graphite cathode system lithium ion battery according to claim 4, which is characterized in that second group permanent
The rate of charge and battery dump energy that the current charge stage is correspondingly arranged are the second exponential function relation to successively decrease.
7. the charging method of graphite cathode system lithium ion battery according to claim 6, which is characterized in that described first
The curvature of exponential function relation is greater than the curvature of the second exponential function relation.
8. the charging method of graphite cathode system lithium ion battery according to claim 1-7, which is characterized in that
During the constant-current charge, when battery temperature reaches the first temperature upper limit of setting, the charging times of current setting is reduced
Rate continues to charge；When battery temperature reaches the second temperature upper limit of setting, stop charging；The second temperature upper limit of setting is greater than
First temperature upper limit.
9. the charging method of graphite cathode system lithium ion battery according to claim 8, which is characterized in that when battery temperature
When degree is more than or equal to the first temperature upper limit and is less than the second temperature upper limit, the drop of rate of charge is determined according to the environment temperature of detection
Low amplitude, and the range of decrease of environment temperature more charge rate is bigger.
10. the charging method of graphite cathode system lithium ion battery according to claim 1, which is characterized in that work as battery
When temperature is less than the lowest temperature of setting, the rate of charge for reducing current setting continues to charge, according to battery temperature at a temperature of
The difference of limit determines the reduction amplitude of rate of charge, and the range of decrease of the bigger rate of charge of difference is bigger.
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| CN114171811A (en) * | 2021-11-30 | 2022-03-11 | 上海瑞浦青创新能源有限公司 | Stepped charging method and charging device and application thereof |
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