CN112240986B - Evaluation method for lithium separation and uniformity of large-size soft-package lithium ion battery - Google Patents
Evaluation method for lithium separation and uniformity of large-size soft-package lithium ion battery Download PDFInfo
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- G—PHYSICS
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- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/385—Arrangements for measuring battery or accumulator variables
- G01R31/387—Determining ampere-hour charge capacity or SoC
- G01R31/388—Determining ampere-hour charge capacity or SoC involving voltage measurements
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01R—MEASURING ELECTRIC VARIABLES; MEASURING MAGNETIC VARIABLES
- G01R31/00—Arrangements for testing electric properties; Arrangements for locating electric faults; Arrangements for electrical testing characterised by what is being tested not provided for elsewhere
- G01R31/36—Arrangements for testing, measuring or monitoring the electrical condition of accumulators or electric batteries, e.g. capacity or state of charge [SoC]
- G01R31/396—Acquisition or processing of data for testing or for monitoring individual cells or groups of cells within a battery
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Abstract
The invention provides a method for evaluating lithium precipitation and uniformity of a large-size soft-package lithium ion battery, which comprises the steps of carrying out charge test and discharge test on the lithium ion battery, recording the capacity, absolute voltage of the battery, difference value between an auxiliary tab pair and a main tab and voltage change condition, and comparing time for reaching stable state of voltage at different positions with a dV/dT curve and a dV/dQ curve obtained by processing; and judging the rate distribution and the lithium precipitation amount of the lithium ion intercalation graphite according to the dV/dT curve and the dV/dQ curve. The operation method is simple, has no damage to the battery, has accurate and reliable data, realizes the real-time analysis of the lithium precipitation uniformity of the negative electrode in the lithium ion battery, and can provide key technical support for soft package single batteries, module design and prediction of the actual service life of the battery pack.
Description
Technical Field
The embodiment of the invention relates to the technical field of lithium ion batteries, in particular to a method for evaluating lithium precipitation and uniformity of a large-size soft-package lithium ion battery.
Background
In recent years, lithium ion batteries are receiving more and more attention as novel green energy sources, and as the application range of lithium ion batteries is expanding, the requirements on the application conditions of lithium ion batteries are becoming more and more severe, and accordingly, how to solve the problem of improving the cycle performance and the high-rate charging performance of lithium batteries at low temperature in the lithium battery industry is also being carried out. The commercial lithium ion battery cathode material comprises carbon, silicon-based materials and the like, and has the advantages that the reaction potential is similar to the deposition potential of metal lithium, and when the lithium ion battery is charged at a high multiplying power, low temperature or overcharged, the lithium intercalation space of the cathode is insufficient or the lithium intercalation resistance is overlarge, so that lithium precipitation and lithium dendrite formation on the surface of the cathode can be caused, and the safety problems of battery capacity reduction, service life attenuation, short circuit and the like are caused. Therefore, detection and analysis of lithium ion battery lithium precipitation have become a technical hotspot in the industry.
The patent with application number 201810769863.3 proposes a method for judging lithium ion battery lithium-ion battery critical conditions, charging the lithium ion battery at the same temperature by adopting different multiplying powers, and recording the relationship between the potential of the negative electrode and the charging current or the charging multiplying power to obtain the critical lithium-ion battery or the critical lithium-ion battery multiplying power. Patent application number 201810576440.X proposes a lithium ion battery lithium analysis detection method and system, wherein the lithium ion battery charging voltage and capacity data are subjected to differential processing to obtain a dV/dQ curve, and the lithium analysis state inside the lithium ion battery is judged. Patent application No. 2016610367810. X proposes a method for comparing coulombic efficiency data of a lithium ion battery in charge-discharge cycles before and after standing, and directly judging whether lithium precipitation occurs in the lithium ion battery.
The technical scheme is only related analysis performed after lithium is separated from the negative electrode of the lithium ion battery, accurate tests cannot be performed on the non-uniform distribution of the lithium separated from the interior of the lithium ion battery, the design size of the lithium ion battery is required to be continuously increased in the market of the power lithium ion battery, related technical support cannot be provided in the prior art, and the latest market demand is met.
Disclosure of Invention
The invention provides a method for evaluating lithium precipitation and uniformity of a large-size soft-package lithium ion battery, which aims to solve the problem that accurate test cannot be performed on the lithium precipitation non-uniform distribution in the lithium ion battery, and provides a multi-lug lithium ion battery.
In order to achieve the above object, the present invention provides the following technical solutions:
the evaluation method of lithium separation and uniformity of the large-size soft-package lithium ion battery comprises the following steps:
step S1: carrying out charge test and discharge test on the lithium ion battery, and recording capacity, absolute voltage of the battery, difference value between the auxiliary tab pair and the main tab and voltage change condition;
step S2: comparing the time of the voltage at different positions reaching a stable state, and drawing a dV/dT curve by taking the time T as an X axis and dV/dT as a Y axis;
step S3: performing differential treatment on the dV/dT curve, and then plotting with the discharge capacity Q as an X axis and the dV/dQ as a Y axis to obtain a dV/dQ curve;
step S4: and judging the rate distribution and the lithium precipitation amount of the lithium ion intercalated graphite by taking the discharge capacity Q as an X axis and the dV/dQ as a Y axis according to the dV/dT curve and the dV/dQ curve.
After the lithium ion battery is charged and discharged with high current, the duration time of voltage stabilization depends on the rate capability of lithium ion intercalation graphite, and parameters such as intercalation exchange current density, solid state diffusivity of graphite, temperature and the like, and even under the condition of the same lithium metal content, the voltage curve can be obviously influenced. Therefore, it is reasonable to compare the lithium plating amounts at different positions of the battery at a certain constant temperature using the same pack of batteries using a voltage plateau.
The step of carrying out charging test on the soft package lithium ion battery comprises the following steps:
step 101: treating the soft package lithium ion battery at low temperature;
step 102: charging to a specified amount of electricity with a constant current, and keeping open for a period of time;
step 103: and observing and recording the capacity, the absolute voltage of the battery, the difference value between the auxiliary tab pair and the main tab and the voltage change condition.
The step of discharging the soft package lithium ion battery comprises the following steps:
step 111: the soft package lithium ion battery is positioned at a low temperature;
step 112: charging to a specified electric quantity with a constant current and then immediately discharging;
step 113: and observing and recording the capacity, the absolute voltage of the battery, the difference value between the auxiliary tab pair and the main tab and the voltage change condition.
The step of judging the rate distribution and the lithium precipitation amount of the lithium ion intercalated graphite comprises the following steps:
step 401: the dV/dT curve is characterized in that the X axis is time, the Y axis is dV/dT, and any X coordinate is perpendicular to intersect with a corresponding point of the dV/dT curve to obtain an intersection point; the intersection point is used as a tangent line of the dV/dT curve, the slope of the tangent line is obtained, namely the rate of the lithium ion intercalation graphite is obtained, and the rate corresponding to the X coordinate required by repeated measurement is obtained, so that the rate distribution of the lithium ion intercalation graphite is obtained;
step 402: according to the dV/dQ curve, any X sign is marked as a vertical line to intersect with a corresponding point of the curve to obtain an intersection point; crossing the crossing point to obtain a point crossing the Y axis, taking the capacity corresponding to the point crossing the Y axis, and calculating the mass of precipitated lithium according to the formula that mlithium (g) =Q.3600.94/96500.
Preferably, during discharge, the discharge current is in the range of 0.3-1.0C and the cut-off voltage is 2.7V.
Preferably, the low-temperature environment temperature ranges from-10 ℃ to 5 ℃, and the temperature values and the current values selected in the charge test step and the discharge test step are kept consistent.
Preferably, the tab difference between the auxiliary tab and the main tab is measured using a high-precision analog data recorder.
The invention designs a multipolar ear soft-pack battery by utilizing an autonomous design, and adopts a high-precision analog data recorder to study the relaxation behaviors of the battery under low temperature with different multiplying powers. By comparing the voltage stabilization time at different positions with dV/dT and dV/dQ curves, the speed distribution and the lithium precipitation amount of lithium ion intercalated graphite can be intuitively obtained, and the influence of the battery size on the local uniformity of the battery is obtained. The operation method is simple, has no damage to the battery, has accurate and reliable data, realizes the real-time analysis of the lithium precipitation uniformity of the negative electrode in the lithium ion battery, and can provide key technical support for soft package single batteries, module design and prediction of the actual service life of the battery pack.
Drawings
FIG. 1 is a schematic diagram of a multi-lug large-size soft-pack lithium ion battery;
wherein: 1. cell main lug 2, auxiliary lug pair 3 and temperature probe
Fig. 2 is a flow chart of a method for detecting lithium precipitation of a soft-pack lithium ion battery.
FIG. 3 is a chart showing the quality of lithium analysis during charging at different locations
FIG. 4 is a time chart of the voltage balance at different locations during the discharge process
FIG. 5 is a time chart of the voltage balance at different locations during the charging process
FIG. 6 is a graph of the discharge process dV-dT
FIG. 7 is a diagram of the charging process dV-dT
Fig. 8 is a plot of the different bit placement processes dV/dQ (with the embedded portion being a partial enlarged view) of a multi-lug battery.
Detailed Description
Examples: the method is suitable for a multi-lug large-size soft-package lithium ion battery, please refer to fig. 1, which is a schematic diagram of the multi-lug large-size soft-package lithium ion battery, and the multi-lug large-size soft-package lithium ion battery comprises a battery main body, a main lug of an electric core and an auxiliary lug pair, wherein the main lug of the electric core is positioned on the same side; the auxiliary electrode lug pairs are symmetrically distributed on two sides of the length of the battery, the adjacent auxiliary electrode lugs are equally spaced, the battery main body comprises a positive electrode plate and a negative electrode plate, the positive electrode material is layered transition metal oxide, the negative electrode material is silicon-based material, 6 temperature probes are arranged in the middle of the auxiliary electrode lug pairs, and the temperature probes are positioned in the middle of the auxiliary electrode lug pairs.
The auxiliary electrode lugs are symmetrically distributed at equal intervals and are respectively numbered 1#, 2#, 3#, 4#, 5# and 6#, positions to be measured can be arranged in an array mode, a certain rule is provided, analysis of measurement data is facilitated, and accordingly analysis results are more accurate.
The position of the auxiliary tab pair is a measured position, the temperature probe is positioned at the middle position of the auxiliary tab pair, and the temperature measured by the temperature probe can reflect the temperature of the measured position of the auxiliary tab pair and can be synchronously processed with other parameters such as voltage, capacity and the like.
Referring to fig. 2, a flow chart of a method for detecting lithium precipitation of a soft-package lithium ion battery is shown, which is a method for evaluating lithium precipitation and uniformity of a large-size soft-package lithium ion battery, wherein a lithium ion battery is subjected to a charge test and a discharge test, the difference value and voltage change conditions between a capacity, an absolute voltage of the battery, an auxiliary tab pair and a main tab are recorded, and a dV/dT curve is drawn by comparing time when voltages at different positions reach a steady state with time T as an X axis and dV/dT as a Y axis; performing differential treatment on the dV/dT curve, and plotting the dV/dQ curve by taking the discharge capacity Q as an X axis and the dV/dQ as a Y axis; and judging the rate distribution and the lithium precipitation amount of the lithium ion intercalation graphite according to the dV/dT curve and the dV/dQ curve. After the lithium ion battery is charged and discharged with high current, the duration time of voltage stabilization depends on the rate capability of lithium ion intercalation graphite, and parameters such as intercalation exchange current density, solid state diffusivity of graphite, temperature and the like, and even under the condition of the same lithium metal content, the voltage curve can be obviously influenced. Therefore, it is reasonable to compare the lithium plating amounts at different positions of the battery at a certain constant temperature using the same pack of batteries using a voltage plateau.
The soft package lithium ion battery is subjected to charging test, which comprises the following steps:
step 101: placing the soft package lithium ion battery in a low-temperature environment of-10 ℃ for 4 hours;
step 102: charged to 75% soc at constant current 3C, left open for 3 hours;
step 103: the capacity and the absolute voltage of the battery are observed and recorded, and the auxiliary pole difference value and the voltage change are measured by using a high-precision analog data recorder.
The soft package lithium ion battery is subjected to discharge test, which comprises the following steps:
step 111: placing the soft package lithium ion battery in a low-temperature environment of-10 ℃ for 4 hours, wherein the low-temperature environment and the treatment time are consistent with each other when the battery is subjected to a charging test, the battery is comparable under the same condition, and the two groups of data can be combined and compared;
step 112: charging to 75% SOC under constant current 3C, discharging immediately, wherein the discharging current is 0.3C, and the cut-off voltage is 2.7V;
step 113: the capacity and the absolute voltage of the battery are observed and recorded, and the auxiliary pole difference value and the voltage change are measured by using a high-precision analog data recorder.
The step of judging the rate distribution and the lithium precipitation amount of the lithium ion intercalated graphite comprises the following steps:
comparing the time of reaching the stable state of the voltage at different positions with the dV/dT curve obtained by processing, processing the data recorded in the discharging process to obtain the dV/dQ curve, wherein dV/dQ is obtained by differentiating the discharging curve, and then plotting with the discharging capacity Q as the X axis and dV/dQ as the Y axis, as shown in figure 8. And intuitively obtaining the rate distribution of the lithium ion intercalation graphite according to the dV/dT curve, and estimating Li precipitation amounts at different positions according to the dV/dQ curve.
In combination with fig. 4-7, it can be seen that the voltage at different positions reaches a different stabilization time in the charge relaxation phase, which is related to the lithium precipitation rate at different positions, and the faster the lithium precipitation rate, the faster the voltage is stabilized. But the dV/dT maps at different locations are very close as all locations have reached stability in a short time.
The voltage plateau of the discharge curve of a lithium ion battery represents the phase change process in the electrode, and the oxidation reaction, namely the delithiation process, occurs on the negative electrode during the discharge process, wherein the oxidation reaction comprises the removal of the intercalated lithium inside the negative electrode and the oxidation of surface lithium precipitation, wherein the surface lithium precipitation is generated during the previous step of the charging process and can react preferentially during the delithiation process, so the high voltage plateau of the discharge curve represents the oxidation reaction of the surface lithium precipitation of the negative electrode, and is caused by the phase balance of the surface lithium precipitation and the first delithiation stage of graphite. In the invention, a low-temperature test environment is adopted, so that the film-forming side reaction of the surface precipitated lithium is negligible, and therefore, the capacity Q (mAh) corresponding to the peak position of the discharge curve dV/dQ is caused by the complete oxidation reaction of the surface precipitated lithium, and then the method comprises the following steps of:
m lithium (g) =q.3600.94/96500
The quality of the precipitated lithium can be calculated. The specific calculation results are shown in a lithium-precipitation quality table in the charging process at different positions in fig. 3, and it can be seen that in the same test step, the lithium-precipitation quality of the same battery at different positions is obviously different, which is related to the dynamic process of the lithium-precipitation reaction at different positions. Comparing the time of reaching a stable state by the voltages at different positions with a dV/dT curve obtained by processing, wherein the dV/dT curve is time on an X axis, dV/dT is on a Y axis, and any X coordinate is perpendicular to intersect with a corresponding point of the dV/dT curve to obtain an intersection point; the intersection point is used as a tangent line of the dV/dT curve, the slope of the tangent line is obtained, namely the rate of the lithium ion intercalation graphite is obtained, and the rate corresponding to the X coordinate required by repeated measurement is obtained, so that the rate distribution of the lithium ion intercalation graphite is obtained; the effect of cell size on the local uniformity of the cell was analyzed. The data recorded in the discharging process are processed to obtain a dV/dQ curve, and the discharge capacity of the peak of the dV/dQ curve can be approximately equal to the amount of lithium deposited in the charging period, so that the lithium precipitation amount at different positions can be estimated.
The embodiment of the invention provides a multi-lug large-size lithium ion soft package battery which is used for testing the relaxation behaviors of the battery under low temperature and different multiplying powers. By comparing the voltage stabilization time at different positions with dV/dT and dV/dQ curves, the speed distribution and the lithium precipitation amount of lithium ion intercalated graphite can be intuitively obtained, and the influence of the battery size on the local uniformity of the battery can be obtained on the premise of not damaging the battery.
The invention utilizes the autonomous design multipolar ear soft-package battery, the provided embodiment adopts a high-precision analog data recorder, the relaxation behavior of the low-temperature battery is researched, the operation method is simple, the battery is not damaged, the data is accurate and reliable, the real-time analysis of the lithium-ion battery internal negative electrode lithium-precipitation uniformity is realized, and the key technical support can be provided for soft-package single batteries, module design and the estimation of the actual service life of the battery pack.
Claims (7)
1. The method for evaluating the lithium precipitation and uniformity of the large-size soft-package lithium ion battery is characterized by comprising the following steps of:
step S1: carrying out charge test and discharge test on the lithium ion battery, and recording capacity, absolute voltage of the battery, difference value between the auxiliary tab pair and the main tab and voltage change condition;
step S2: comparing the time of the voltage at different positions reaching a stable state, and drawing a dV/dT curve by taking the time T as an X axis and dV/dT as a Y axis;
step S3: performing differential treatment on the dV/dT curve, and plotting the dV/dQ curve by taking the discharge capacity Q as an X axis and the dV/dQ as a Y axis;
step S4: judging the rate distribution and the lithium precipitation amount of the lithium ion intercalation graphite according to the dV/dT curve and the dV/dQ curve; the step of judging the rate distribution and the lithium precipitation amount of the lithium ion intercalated graphite comprises the following steps:
step 401: the dV/dT curve, the X axis is time T, the Y axis is dV/dT, and any X coordinate is perpendicular to intersect with the corresponding point of the dV/dT curve to obtain an intersection point; the intersection point is used as a tangent line of the dV/dT curve, the slope of the tangent line is obtained, namely the rate of the lithium ion intercalation graphite is obtained, and the rate corresponding to the X coordinate required by repeated measurement is obtained, so that the rate distribution of the lithium ion intercalation graphite is obtained;
step 402: according to the dV/dQ curve, making a vertical line at any X coordinate to intersect with a corresponding point of the curve to obtain an intersection point; crossing the crossing point to obtain a point crossing the Y axis, taking the capacity corresponding to the point crossing the Y axis, and calculating the mass of precipitated lithium according to the formula that mlithium (g) =Q.3600.94/96500.
2. The method for evaluating lithium separation and uniformity of a large-sized soft-pack lithium ion battery according to claim 1, wherein the step of performing a charge test on the soft-pack lithium ion battery comprises:
step 101: treating the soft package lithium ion battery at low temperature;
step 102: charging to a specified amount of electricity with a constant current, and keeping an open circuit;
step 103: and observing and recording the capacity, the absolute voltage of the battery, the difference value between the auxiliary tab pair and the main tab and the voltage change condition.
3. The method for evaluating lithium separation and uniformity of a large-sized soft-pack lithium ion battery according to claim 2, wherein the step of performing a discharge test on the soft-pack lithium ion battery comprises:
step 111: treating the soft package lithium ion battery at low temperature;
step 112: charging to a specified electric quantity with a constant current and then immediately discharging;
step 113: and observing and recording the capacity, the absolute voltage of the battery, the difference value between the auxiliary tab pair and the main tab and the voltage change condition.
4. The method for evaluating lithium separation and uniformity of a large-size soft-pack lithium ion battery according to claim 1 or 3, wherein the discharge current is in the range of 0.3-1.0C and the cut-off voltage is 2.7V during discharge.
5. The method for evaluating lithium ion battery lithium deposition and uniformity of large-sized soft package according to claim 3, wherein,
the temperature value and the current value selected in the charge test step and the discharge test step are kept consistent.
6. The method for evaluating lithium separation and uniformity of a large-sized soft-pack lithium ion battery according to claim 3, wherein the low-temperature ambient temperature range is-10 ℃ to 5 ℃.
7. The method for evaluating lithium ion battery separation and uniformity of a large-size soft package lithium ion battery according to claim 1, 2 or 3, wherein the tab difference between the auxiliary tab and the main tab is measured by using a high-precision analog data recorder.
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| CN112782582B (en) * | 2021-01-29 | 2023-09-15 | 远景动力技术(江苏)有限公司 | Method for detecting lithium ion battery negative electrode lithium precipitation |
| CN113193249B (en) * | 2021-04-27 | 2023-02-10 | 广州小鹏汽车科技有限公司 | Method and device for determining lithium analysis threshold value and electric automobile |
| CN113189498A (en) * | 2021-05-16 | 2021-07-30 | 广州菲利斯太阳能科技有限公司 | Nondestructive lithium analysis detection method |
| KR20220159818A (en) * | 2021-05-26 | 2022-12-05 | 주식회사 엘지에너지솔루션 | Apparatus and method for monitoring battery |
| CN113466708A (en) * | 2021-07-27 | 2021-10-01 | 上海纳米技术及应用国家工程研究中心有限公司 | Method for evaluating low-temperature performance of lithium battery |
| CN114094215B (en) * | 2021-10-21 | 2023-04-14 | 合肥国轩高科动力能源有限公司 | Charging strategy making method for improving battery cycle |
| CN115060320B (en) * | 2022-06-20 | 2023-09-29 | 武汉涛初科技有限公司 | Online monitoring and analyzing system for production quality of power lithium battery based on machine vision |
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