Automated testing method, apparatus, medium, and product for solid-state electrolyte conductivity

Abstract

The application provides a kind of solid electrolyte conductivity automated test method, device, medium and product, it is related to performance test technical field.The method comprises: first determining the baseline data comprising absolute zero point thickness and system stiffness compensation curve, then preparing the solid electrolyte sample to be measured and loading into sealed mold.Afterwards, pressurizing module is pressurized according to the test pressure parameter input by user, and pressure sensor and displacement sensor monitor pressure value and sample thickness value in real time, dynamic pressurization compensation is carried out according to pressure value to maintain pressure stability.Subsequently, electrochemical workstation carries out alternating current impedance test on sample to obtain impedance data, and finally combines baseline data, real-time thickness value and impedance data to complete the calculation of ion conductivity of the solid electrolyte sample to be measured.The whole process is through module cooperation and data linkage, to realize the automatic and accurate test of conductivity.

Description

Technical Field

[0001] This application relates to the field of performance testing technology, and in particular to an automated testing method, apparatus, medium, and product for the conductivity of solid electrolytes. Background Technology

[0002] As a next-generation energy storage device with high energy density and high safety, the core of all-solid-state batteries lies in the development of solid-state electrolytes. During operation, solid-phase material transport occurs between the positive and negative electrodes via the electrolyte, which typically requires applying extremely high external pressures (e.g., greater than 100 MPa) to facilitate interfacial contact and material transport. Literature reports indicate that many solid-state electrolytes (such as coordination hydrides) only exhibit excellent electrochemical performance under high pressure.

[0003] The existing automated testing method for the conductivity of solid electrolytes involves the following steps: first, pressing solid electrolyte powder into a sheet under high pressure; then, sputtering gold onto the surface of the resulting solid electrolyte sheet; finally, placing the gold-sputtered electrolyte sheet in a blocking electrode and performing an AC impedance test; and then calculating the ionic conductivity of the electrolyte based on the impedance value.

[0004] However, in the existing technology, this automated testing method for the conductivity of solid electrolytes is not only costly, but also suffers from rebound error when sampling and measuring thickness, resulting in inaccurate ionic conductivity data. Summary of the Invention

[0005] This application provides an automated testing method, apparatus, medium, and product for the conductivity of solid electrolytes, which enables automated in-situ pressurization of solid electrolytes under variable pressure conditions, real-time monitoring of the true thickness based on stiffness compensation, and accurate calculation of ionic conductivity.

[0006] In a first aspect, this application provides an automated method for testing the conductivity of solid electrolytes, applied to a variable-pressure automated solid electrolyte testing device. The device includes a pressurization module, a screw-locking module, and a testing module. The testing module includes a pressure sensor, a displacement sensor, and an electrochemical workstation. The method includes: determining baseline data, which includes the absolute zero-point thickness and a system stiffness compensation curve; acquiring a solid electrolyte sample to be tested; after determining that the solid electrolyte sample to be tested is loaded into a sealed mold, controlling the pressurization module to pressurize the sealed mold according to user-inputted test pressure parameters; during the pressurization test, using the pressure sensor and the displacement sensor to monitor the pressure value of the sealed mold and the thickness value of the solid electrolyte sample to be tested in real time; based on the pressure value, controlling the pressurization module to perform dynamic pressurization compensation to maintain the pressure value stable at the test pressure parameters; controlling the electrochemical workstation to perform AC impedance testing on the solid electrolyte sample to be tested and acquiring impedance data; and calculating the ionic conductivity of the solid electrolyte sample to be tested by combining the baseline data, the thickness value, and the impedance data.

[0007] By adopting the above technical solution and pre-calibrating the absolute zero point and stiffness curve, the elastic deformation error of the equipment itself can be effectively eliminated. During the test, the use of a pressurization module in conjunction with dual closed-loop monitoring of pressure and displacement sensors not only applies high pressure to replace the expensive gold sputtering process to improve the contact interface, but also obtains the real thickness value of the sample under pressure in real time. Combined with dynamic pressure compensation to eliminate pressure decay caused by powder creep, this ensures that the electrochemical workstation collects impedance data under an extremely stable set pressure field. This series of steps works synergistically to eliminate the "springback error" caused by removing the sample to measure the thickness in traditional offline testing. While significantly reducing testing costs and complexity, it significantly improves the authenticity and accuracy of the conductivity data of all-solid-state battery materials.

[0008] In conjunction with some embodiments of the first aspect, in some embodiments, the step of obtaining the solid electrolyte sample to be tested specifically includes: after determining that the solid electrolyte powder is loaded into the sealed mold, controlling the pressurizing module to pressurize to a first specified pressure input by the user, and maintaining it for a first preset time, and then controlling the pressurizing module to reset; after determining that the first electrode is loaded into the set first position of the sealed mold, controlling the pressurizing module to pressurize to a second specified pressure input by the user and maintaining it for a second preset time, and then controlling the pressurizing module to reset; after determining that the second electrode is loaded into the set second position of the sealed mold, controlling the pressurizing module to pressurize to the second specified pressure and maintaining it for the second preset time, and then controlling the pressurizing module to reset, thereby obtaining the solid electrolyte sample to be tested.

[0009] By adopting the above technical solution and utilizing an automated control strategy of stepwise pressurization and holding, the interfacial contact quality inside the all-solid-state testing mold was significantly optimized. First, the solid electrolyte powder was pressed and held at a specified pressure, promoting particle rearrangement and densification to form a stable substrate. Then, the first and second electrodes were added sequentially and subjected to high-pressure pressing respectively. This progressive lamination process ensured a tight solid-solid atomic-level contact between the positive and negative electrode materials and the electrolyte layer. Compared to traditional one-time mixing and pressing, this scheme effectively reduced interfacial porosity and contact resistance, allowing the subsequently measured conductivity to better reflect the intrinsic properties of the material rather than defects in the preparation process. Simultaneously, the automated program ensured the consistency and repeatability of sample preparation, avoiding the force deviations caused by manual assembly, and laying a solid structural foundation for high-precision electrochemical testing.

[0010] In conjunction with some embodiments of the first aspect, in some embodiments, the step of determining baseline data specifically includes: controlling the pressurization module to compress the unloaded sealing mold at a first speed; recording the displacement value of the displacement sensor when the pressure reaches a preset calibration pressure; determining the absolute zero-point thickness based on the displacement value, the absolute zero-point thickness being the displacement sensor reading when the upper and lower pressurization heads inside the sealing mold are in direct contact; recording the displacement change of the absolute zero-point thickness at different pressure points according to a preset pressure gradient to generate a system stiffness compensation curve, the system stiffness compensation curve being used to characterize the system deformation of the device itself under different pressures; and controlling the pressurization module to reset.

[0011] By adopting the above technical solution, in actual high-pressure testing environments, the metal mold and the testing frame themselves will undergo significant elastic deformation. Without correction, this deformation will be mistakenly included in the sample thickness, leading to an underestimation of the conductivity calculation. This solution calibrates the "absolute zero point" through no-load compression and generates stiffness compensation curves by collecting frame deformation data under different pressures, essentially establishing a "mechanical fingerprint" for the system. During subsequent testing of actual samples, the system can accurately deduct the corresponding system deformation from the total displacement based on the instantaneous pressure value. This process improves the accuracy of thickness measurement to the micrometer level, ensuring that the "net thickness" used for formula calculations is the sample's "net thickness," thus solving the industry-wide problem of geometric dimension measurement distortion of solid electrolytes under high-pressure conditions.

[0012] In conjunction with some embodiments of the first aspect, in some embodiments, the step of controlling the pressurization module to perform dynamic pressurization compensation based on the pressure value specifically includes: setting an allowable pressure deviation range and a thickness fluctuation threshold; reading the values ​​of the pressure sensor and displacement sensor at a preset sampling frequency; if it is detected that the pressure value drops due to powder creep and exceeds the pressure deviation range, controlling the servo mechanism of the pressurization module to feed downwards to perform active pressure compensation; and recording the thickness change trajectory during the compensation process in real time as a basis for determining the sample molding density.

[0013] By adopting the above technical solution, this application solves the problem of "pressure drift" caused by stress relaxation during long-term pressure application of solid powder materials. Solid electrolytes and electrode powders exhibit creep characteristics; under constant pressure, the pressure naturally decays over time, leading to changes in contact impedance and affecting the comparability of test results. This solution sets a sensitive pressure deviation threshold. Once a pressure drop due to powder creep is detected, the servo mechanism immediately performs micron-level downward feed compensation, forcing the system to maintain a constant pressure field. Simultaneously, the real-time recorded thickness change trajectory reflects the powder densification rate. This not only ensures that AC impedance testing is always conducted under strictly defined pressure conditions but also provides an additional dimension for analyzing material mechanical properties, enriching the value of the test data.

[0014] In conjunction with some embodiments of the first aspect, in some embodiments, after correcting the thickness value based on the baseline data to obtain the true thickness of the solid electrolyte sample to be tested, the step of calculating the ionic conductivity of the solid electrolyte sample to be tested by combining the true thickness and the impedance data specifically includes: acquiring the AC impedance spectrum generated by the electrochemical workstation, and determining the bulk resistance value of the solid electrolyte sample to be tested by fitting a circuit model. Based on the system stiffness compensation curve, the system deformation under the current pressure is determined; the real-time readings of the displacement sensor at the test moment are obtained, and the absolute zero-point thickness, the thicknesses of the first and second electrodes, and the system deformation corresponding to the baseline data are subtracted to obtain the true thickness of the sample. Obtain the inner diameter cross-sectional area of ​​the sealing mold. Calculate the ionic conductivity of the solid electrolyte sample to be tested. The specific formula is as follows: .

[0015] By adopting the above technical solution, the volume resistance value R obtained by fitting the circuit model not only represents the material resistance, but also eliminates the interference of contact resistance due to high-voltage contact. More importantly, the thickness L in the formula is not the value measured after depressurization, but the "true thickness in situ under high pressure" obtained by subtracting the absolute zero point and the real-time deformation of the system from the displacement sensor reading. This calculation method perfectly avoids the volume rebound phenomenon caused by the elastic modulus after depressurization of the solid electrolyte, and prevents the problem of inflated conductivity σ due to an artificially large thickness L.

[0016] In conjunction with some embodiments of the first aspect, some embodiments further include: setting a set of test pressure sequences that increase in a gradient; controlling the pressurization module to sequentially apply each pressure value in the test pressure sequence to the sealed mold; performing the dynamic pressurization compensation step at each pressure value; and after the pressure stabilizes within a preset deviation range, triggering the electrochemical workstation to perform testing and record the ionic conductivity at the current pressure; and after traversing all pressure values, generating a correlation curve of the ionic conductivity of the solid electrolyte sample under test as a function of pressure.

[0017] By adopting the above technical solution, a gradient sequence from low pressure to high pressure can be automatically executed, and voltage stabilization, testing, and recording can be automatically completed at each pressure step without manual intervention. This not only saves a significant amount of manpower and time costs, but also continuously and dynamically reveals the evolution of the electrochemical behavior of solid electrolytes under different pressures.

[0018] In conjunction with some embodiments of the first aspect, in some embodiments, after the step of calculating the ionic conductivity of the solid electrolyte sample to be tested, the method further includes: controlling the pressurization module to pressurize to a third specified pressure input by the user; and controlling the screw-locking module to tighten the fastening screws of the sealing mold to a set torque.

[0019] By adopting the above technical solution, the third specified pressure provides a stable internal pressure environment for screw locking, avoiding sample structure deformation caused by pressure changes during the locking process. The constant torque locking of the screw locking module can keep the mold in a stable sealing and pressurized state, so that the sample after the test can still maintain the structure and pressure conditions at the time of the test, which is convenient for subsequent secondary testing or structural analysis of the sample, and ensures the stability of the sample after the test.

[0020] In a second aspect, this application provides a variable-pressure automated solid-state electrolyte testing device, which includes: one or more processors and a memory; the memory is coupled to the one or more processors, and the memory is used to store computer program code, which includes computer instructions, and the one or more processors call the computer instructions to cause the variable-pressure automated solid-state electrolyte testing device to perform the method described in the first aspect and any possible implementation thereof.

[0021] Thirdly, this application provides a computer-readable storage medium including instructions that, when executed on a variable-pressure automated solid-state electrolyte testing device, cause the variable-pressure automated solid-state electrolyte testing device to perform the method described in the first aspect and any possible implementation thereof.

[0022] Fourthly, this application provides a computer program product, including a computer program that, when run on a variable-pressure automated solid-state electrolyte testing device, causes the variable-pressure automated solid-state electrolyte testing device to perform the method described in the first aspect and any possible implementation thereof.

[0023] One or more technical solutions provided in the embodiments of this application have at least the following technical effects or advantages:

[0024] 1. By employing baseline data calibration combined with dual closed-loop monitoring and dynamic compensation of pressure and displacement, i.e., eliminating system deformation errors before testing, maintaining constant high pressure during testing, and obtaining the true thickness and impedance data of the sample in situ, the technical problems of existing solid electrolyte testing requiring expensive gold sputtering processes and large rebound errors and inaccurate data due to pressure relief and thickness measurement are effectively solved. This enables high-precision, low-cost automated in-situ testing of the ionic conductivity of all-solid-state battery materials, significantly improving the authenticity and accuracy of test data.

[0025] 2. By employing the technical means of calibrating the absolute zero point under no-load compression and generating system stiffness compensation curves under different pressures, a mechanical deformation error correction mechanism is established for the test system. In subsequent tests, the elastic deformation of the device itself is deducted in real time. Therefore, the technical problem of inflated sample thickness measurement and low conductivity calculation results caused by mold and frame deformation under high pressure test environment is effectively solved. This enables micron-level accurate correction of the true thickness of solid electrolyte under high pressure in situ, ensuring the accuracy of key parameters in the ionic conductivity calculation formula.

[0026] 3. By adopting a technique of setting a gradient increasing pressure sequence and coordinating with automatic voltage stabilization trigger testing, that is, controlling the pressurization module to automatically traverse multiple pressure points and automatically recording the conductivity after dynamic compensation and stabilization at each pressure point, the technical problem of traditional single-point manual testing being unable to continuously reveal the law of pressure's impact on performance and low R&D efficiency is effectively solved. This enables the fully automatic generation of correlation graphs of solid electrolyte ionic conductivity with pressure, providing comprehensive and quantitative data support for determining the optimal operating pressure of all-solid-state batteries and engineering packaging design. Attached Figure Description

[0027] Figure 1 This is a schematic diagram of the overall structure of the variable pressure automated solid electrolyte testing device in the embodiments of this application; Figure 2 This is a partial structural schematic diagram of the variable pressure automated solid electrolyte testing device in the embodiments of this application;

[0028] Figure 3 This is a flowchart illustrating an automated testing method for the conductivity of solid electrolytes in an embodiment of this application.

[0029] Figure 4 This is a schematic diagram of the physical structure of a variable pressure automated solid electrolyte testing device in the embodiments of this application. Detailed Implementation

[0030] The terminology used in the following embodiments of this application is for the purpose of describing particular embodiments only and is not intended to be limiting of this application. The singular expressions “a,” “an,” “the,” “the,” “the,” and “this” are intended to include the plural expressions as well, unless the context clearly indicates otherwise. It should also be understood that the term “and / or” as used in this application refers to and includes any or all possible combinations of one or more of the listed items.

[0031] Hereinafter, the terms "first" and "second" are used for descriptive purposes only and should not be construed as implying or suggesting relative importance or implicitly indicating the number of indicated technical features. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature, and in the description of the embodiments of this application, unless otherwise stated, "multiple" means two or more.

[0032] For ease of understanding, the structure of the variable-pressure automated solid-state electrolyte testing device provided in this embodiment is described below. Please refer to [link / reference]. Figure 1 This is a schematic diagram of the overall structure of the variable pressure automated solid electrolyte testing device in the embodiments of this application.

[0033] exist Figure 1The variable pressure automated solid electrolyte testing device includes a pressurization module, a screw-locking module, and a testing module. The testing module includes a pressure sensor, a displacement sensor, and an electrochemical workstation. The pressurization module, located in the lower cabinet area of ​​the device, provides controllable testing pressure and dynamic pressure compensation for the sealed mold, ensuring the sample is in a stable pressure environment.

[0034] The screw-locking module is located on the left side of the upper chamber of the device (corresponding to the sealing mold) and is used to tighten the fastening screws of the sealing mold to the set torque to maintain the structure and pressure state of the sample after testing.

[0035] The testing module is located in the internal area of ​​the upper chamber of the device: the pressure sensor is integrated into the output end of the pressurization module (connected to the sealing mold) to monitor the pressure value inside the sealing mold in real time; the displacement sensor is integrated next to the testing station inside the chamber to collect the thickness and displacement data of the sealing mold and the sample in real time; the electrochemical workstation is integrated into an independent cabinet on the right side of the device to apply AC signals to the sample and collect impedance data to provide electrical parameters for calculating ionic conductivity.

[0036] For a more detailed understanding, please refer to the following: Figure 2 This is a partial structural diagram of the variable pressure automated solid electrolyte testing device in an embodiment of this application.

[0037] exist Figure 2 In the test chamber, the control system of the variable pressure automated solid electrolyte test device is located in the upper part of the chamber (integrating a display screen and control buttons), which is used to receive user operation commands, process test data, and coordinate the operation of various modules; the mold part is located in the middle station of the chamber (corresponding to the actuator below the control system), which is used to accommodate the solid electrolyte sample to be tested and provide a sealed test environment; the test module is located in the right side of the chamber, which is used to integrate the core test components of the pressure sensor, displacement sensor, and electrochemical workstation.

[0038] Combination Figure 1 and Figure 2 The overall work process is as follows:

[0039] First pass Figure 1 The pressurization module completes the baseline data calibration, and then the solid electrolyte powder is loaded into... Figure 2 The mold part is made of Figure 1 The pressurization module prepares the test sample by pressurizing it in stages; the test sample is then... Figure 2 After being placed in the mold section, Figure 1 The pressurization module applies pressure to the mold section according to the test pressure parameters set by the user, while... Figure 2 The pressure and displacement sensors in the testing module monitor pressure and thickness data in real time; if pressure fluctuations occur, Figure 1 The pressurization module performs dynamic compensation to maintain pressure stability. Once the pressure stabilizes, Figure 2 The test module triggers the electrochemical workstation to complete the impedance test; the ionic conductivity is calculated by combining baseline data, real-time thickness and impedance data. If it is necessary to retain the sample state, Figure 1 The pressurization module then pressurizes the pressure to the third specified pressure, which is then... Figure 1 The screw-locking module tightens the screws, thus completing the testing process.

[0040] The following describes the process of the method provided in this implementation. Please refer to [link / reference]. Figure 3 This is a flowchart illustrating an automated testing method for the conductivity of solid electrolytes in this application.

[0041] S101. Determine the baseline data, which includes the absolute zero-point thickness and the system stiffness compensation curve;

[0042] Baseline data refers to the set of reference data pre-calibrated by the test device under no-load conditions, which is used to correct measurement errors caused by the device itself in subsequent tests.

[0043] This step is performed before the preparation of the sample to be tested and the formal testing. It is a core pre-calibration step to ensure the accuracy of the test data and is applicable to all solid electrolyte conductivity testing scenarios based on this device.

[0044] Specifically, the variable-pressure automated solid-state electrolyte testing device first receives a calibration command from the control system, then controls the pressurization module to start at a preset first speed, applying pressure to the unloaded sealed mold. At this time, there are no test-related components inside the mold; it only simulates the closed state during testing. During the pressurization process, the pressure sensor collects the pressure data inside the mold in real time and feeds it back to the system. When the pressure reaches the preset calibration pressure, the system immediately triggers the displacement sensor to record the current displacement value. Since the upper and lower pressure heads inside the mold are in complete contact without gaps under the calibration pressure at this time, this displacement value is determined as the absolute zero thickness. The pressure is set as the reference starting point for subsequent sample thickness measurements. Then, the system controls the pressurization module to continue applying pressure according to the preset pressure gradient (e.g., from 10MPa to 200MPa, with each gradient being 15MPa). The pressure is maintained for 5 seconds at each pressure gradient to ensure the frame deformation is stable. The frame deformation corresponding to that pressure point is then recorded. After all pressure gradient tests are completed, the pressure value is correlated with the corresponding frame deformation using a data fitting algorithm to generate a system stiffness compensation curve. After all calibration operations are completed, the system controls the pressurization module to move in the reverse direction and reset to the initial position, waiting for the subsequent test process to start.

[0045] This step, through precise no-load calibration, clarifies the absolute zero-point thickness and the deformation law of the device, solving the problem of sample thickness measurement distortion caused by the failure to consider the elastic deformation of the device itself in the existing technology. It provides a precise basis for deducting the influence of device deformation when calculating the true thickness of the sample, and ensures the accuracy of the basic data for calculating ionic conductivity from the source.

[0046] S102. Obtain the solid electrolyte sample to be tested;

[0047] Among them, the solid electrolyte sample to be tested refers to an integrated structural component that has been powder-formed and electrode-assembled to meet the conditions for ionic conductivity testing.

[0048] This step is performed after the baseline data is determined and before the sample is loaded into the sealed mold for pressure testing. It is applicable to all testing scenarios where the sample to be tested is prepared based on powder raw materials and is the core step in constructing a qualified test sample.

[0049] Specifically, the device first detects through sensors that the solid electrolyte powder has been manually or automatically loaded into the central area of ​​the cavity of the sealed mold. Then, it immediately starts the pressurization module, controls it to pressurize at a preset speed to the first specified pressure input by the user, and maintains it for a first preset time. Under the pressure, the electrolyte powder particles rearrange and densify to form a structurally stable electrolyte sheet. Then, the pressurization module is controlled to depressurize and reset. After the solid electrolyte powder is pressed into a sheet by the first specified pressure, an electrode needs to be assembled on one side of the sheet to make the electrode and the electrolyte sheet in close contact. On the one hand, this provides a carrier for the current input / output of the subsequent AC impedance test, and on the other hand, it simulates the actual interface structure of "electrode-electrolyte" in an all-solid-state battery. Next, after detecting that the worker or automated mechanism has installed the first electrode in the first position of the sealed mold, the pressurization module is controlled to pressurize again to the second specified pressure input by the user and maintain it for a second preset time, so that the first electrode and the surface of the electrolyte sheet form a tight physical contact, reducing the interface gap. After that, the pressurization module is reset. The first electrode installed is usually made of a material with excellent conductivity (such as lithium metal sheet, nickel sheet, etc.), and its size matches the sealed mold cavity and electrolyte sheet. When installing, it is necessary to ensure that the electrode surface is clean and undamaged, and completely covers the corresponding surface of the electrolyte sheet to avoid affecting the test results due to insufficient contact area or interface contamination.

[0050] Finally, after the second electrode is installed in the second position of the sealed mold, the pressure holding operation of the second specified pressure and the second preset time is repeated to make the second electrode also fit tightly with the other side of the electrolyte sheet, and finally form a solid electrolyte sample to be tested with a regular structure of "first electrode-electrolyte sheet-second electrode" and good interface contact.

[0051] This step, through an automated control strategy of step-by-step pressurization and pressure holding, solves the problems of uneven sample molding and poor electrode-electrolyte contact caused by traditional one-time mixing and pressing. It ensures the consistency of sample interface contact quality, avoids test errors caused by excessive interface porosity, and provides a sample basis with excellent morphology and structure for subsequent high-precision conductivity testing.

[0052] S103. After confirming that the solid electrolyte sample to be tested has been loaded into the sealed mold, the pressurization module is controlled to pressurize the sealed mold according to the test pressure parameters input by the user.

[0053] Among them, the test pressure parameter refers to the target pressure value set by the user according to the test requirements (such as simulating the actual working pressure of all-solid-state batteries, performance comparison under different pressures), which must meet the requirements of solid electrolyte solid phase material transmission. The pressurization module refers to the core execution component in the device used to provide controllable pressure, which usually includes servo motors, lead screws, pressure output terminals, etc., and can achieve precise pressure adjustment. The sealing mold refers to the rigid structural component used to contain the sample to be tested, ensure the sealing of the test environment, and withstand high pressure (such as ≥200MPa). The pressurization test refers to the process of applying the target pressure to the sealing mold and maintaining it in order to simulate the working environment of all-solid-state batteries.

[0054] This step is performed after the sample to be tested has been prepared and confirmed to be installed in the sealed mold, and before the pressure and thickness values ​​are monitored in real time. It is applicable to the conductivity testing scenarios of all samples to be tested and is the core step in constructing the high-pressure environment required for testing.

[0055] Specifically, the device confirms that the solid electrolyte sample to be tested has been correctly placed in the center of the sealed mold cavity and that the mold has been closed in place by feedback signals from the position sensor or pressure sensor on the mold. Then, it receives the test pressure parameters input by the user through the operation interface (these parameters can be set arbitrarily within the range of 10MPa to 200MPa to adapt to the test requirements of different types of solid electrolytes). Subsequently, the system calculates the output force of the pressurization module based on the test pressure parameters (combined with the cross-sectional area of ​​the mold inner diameter) and controls the pressurization module to apply pressure to the sealed mold at a preset second speed (e.g., 0.5mm / min, lower than the calibrated speed to ensure pressure stability). During the pressurization process, the system receives feedback data from the pressure sensor in real time and adjusts the feed rate of the pressurization module through closed-loop control. When the pressure reaches within ±0.5% of the test pressure parameters, the rapid feed of the pressurization module is paused and switched to fine-tuning mode until the pressure stabilizes at the test pressure parameters, completing the start process of the pressurization test.

[0056] This step, through automated and precise pressurization, solves the problems of uneven pressure and inability to meet high-pressure requirements in existing technologies by manually pressurizing. It provides a stable high-pressure testing environment for solid electrolytes, promotes the solid-phase material transport between the electrolyte and the electrode, and replaces the traditional gold sputtering process to improve interface contact and reduce testing costs.

[0057] S104. During the pressure test, the pressure sensor and the displacement sensor are used to monitor the pressure value of the sealed mold and the thickness value of the solid electrolyte sample to be tested in real time.

[0058] Among them, the pressure sensor refers to the force-sensitive element installed at the output end of the pressurization module or inside the mold, which is used to detect the actual pressure inside the sealed mold in real time; the displacement sensor refers to the grating ruler measuring component installed on the pressurization module or the mold, which is used to detect the displacement after the mold is closed in real time, and then deduce the sample thickness.

[0059] This step is performed after the pressurization module reaches the test pressure parameters, during dynamic pressurization compensation and AC impedance testing, and is a core monitoring link to ensure the controllability of the testing process, running through the entire pressurization testing phase.

[0060] Specifically, during the pressure test, the device controls the pressure sensor and displacement sensor to continuously collect data according to a preset sampling frequency. The pressure sensor directly detects the pressure signal inside the sealed mold, converts it into an electrical signal, and transmits it to the control system. The system displays and stores the pressure value in real time to determine whether the pressure is stable within the test pressure parameter range. The displacement sensor detects the feed displacement of the pressure module or the closing displacement of the mold in real time. Combined with the absolute zero point thickness determined in S101, the current thickness value of the solid electrolyte sample to be tested is initially calculated. This thickness value is updated in real time with pressure changes and sample deformation. At the same time, the system verifies the collected pressure and thickness values ​​in real time. If any abnormal data is found (such as sudden pressure changes or no reading from the displacement sensor), an alarm signal is immediately issued and the test is suspended to ensure the safety of the test process and the validity of the data.

[0061] This step, through real-time monitoring by dual sensors, solves the problem of not being able to monitor pressure and sample thickness changes during testing in real time in existing technologies. It provides a precise triggering basis for subsequent dynamic pressure compensation, while making parameter changes during testing visible, facilitating timely detection of test anomalies and ensuring the continuity and reliability of test data.

[0062] S105. Based on the pressure value, control the pressurization module to perform dynamic pressurization compensation to keep the pressure value stable at the test pressure parameter;

[0063] This step is performed during the pressure test and is synchronized with the real-time monitoring of S104. It is applicable to all solid electrolyte test scenarios where there is a risk of powder creep.

[0064] Specifically, the device first presets a reasonable pressure deviation range (e.g., 99-101 MPa when the test pressure is 100 MPa) and a thickness fluctuation threshold based on the test pressure parameters and sample characteristics. Then, it continuously reads the real-time values ​​from the pressure sensor and displacement sensor at a preset sampling frequency and analyzes the data in real time. During the pressurization test, due to the creep characteristics of the solid electrolyte and electrode powder, slow plastic deformation occurs, causing the pressure inside the sealed mold to gradually decrease. When the system detects a pressure drop exceeding the preset pressure deviation range, and the thickness change does not exceed the thickness fluctuation threshold (excluding abnormal situations such as severe sample damage), it immediately sends a compensation command to the servo mechanism of the pressurization module. After receiving the command, the servo mechanism slowly feeds downwards with micron-level precision, gradually increasing the pressure on the sealed mold until the pressure sensor detects that the actual pressure value has returned to the test pressure parameter range. During the compensation process, the system records the sample thickness change trajectory in real time and judges the sample's molding density by the thickness change rate. If the thickness change rate gradually decreases and tends to stabilize, it indicates that the sample has been sufficiently densified.

[0065] This step, through closed-loop dynamic pressure compensation, solves the problems of pressure decay and unstable testing environment caused by powder creep in existing technologies. It ensures that the electrochemical workstation always performs impedance testing under the set stable pressure field, avoiding the interference of pressure fluctuations on the test results. At the same time, it provides a basis for judging the sample density through the thickness change trajectory, enriching the value of the test data.

[0066] S106. Control the electrochemical workstation to perform AC impedance testing on the solid electrolyte sample to be tested and obtain impedance data;

[0067] Among them, the electrochemical workstation refers to the core instrument used to carry out electrochemical tests, which can generate AC signals and collect the impedance response of samples.

[0068] This step is performed after the pressure test has stabilized and before the ionic conductivity is calculated. It is the core testing step for obtaining the electrical properties data of the sample and must be carried out in an environment with stable pressure and no external electromagnetic interference.

[0069] Specifically, after the device confirms through dynamic pressure compensation via S105 that the pressure value inside the sealed mold is stable within the deviation range of the test pressure parameters and that the sample thickness does not fluctuate significantly, it automatically sends a test start command to the electrochemical workstation. Upon receiving the command, the electrochemical workstation applies an AC voltage signal to the first and second electrodes inside the sealed mold according to the preset test parameters (e.g., AC voltage amplitude of 10mV, test frequency range of 1Hz-1MHz, and 50 frequency points). The solid electrolyte sample under test generates an impedance response under the action of the AC signal. The electrochemical workstation collects the real and imaginary impedance data of the sample at different frequencies in real time and generates an AC impedance spectrum. After the test is completed, the electrochemical workstation transmits the collected impedance data to the device's control system. The control system stores and preprocesses the data to prepare for subsequent ionic conductivity calculations.

[0070] This step, by automating the AC impedance test, solves the problem of asynchronous pressure stabilization and test initiation caused by manual test in existing technologies. It ensures that the test is conducted under optimal pressure stability. At the same time, the high-frequency range of test parameter settings can accurately capture the bulk resistance information of the sample, providing reliable impedance data support for the accurate calculation of ionic conductivity.

[0071] S107. Based on the baseline data, the thickness value is corrected to obtain the true thickness of the solid electrolyte sample to be tested. Then, the ionic conductivity of the solid electrolyte sample to be tested is calculated by combining the true thickness and the impedance data.

[0072] This step is performed after the AC impedance test is completed. It is the final data processing step in the entire testing process and is applicable to the calculation of ionic conductivity of all samples to be tested.

[0073] Specifically, the device first extracts the AC impedance spectrum from the impedance data transmitted by the electrochemical workstation. It then performs fitting analysis on the spectrum using a preset equivalent circuit model to separate interfering factors such as interface resistance and contact resistance, accurately determining the bulk resistance value R of the solid electrolyte sample to be tested. Subsequently, the thickness value is corrected based on this baseline data. Specifically, the real-time reading of the displacement sensor recorded in S104 at the test moment is retrieved. This real-time reading serves as the current thickness value of the solid electrolyte sample. Combined with the baseline data determined in S101, the real-time reading of the displacement sensor (i.e., the thickness value) is subtracted from the corresponding absolute zero-point thickness, the thickness of the first electrode, and the thickness of the second electrode. Then, the system deformation corresponding to the system stiffness compensation curve under the current pressure is subtracted to obtain the true thickness L of the sample under the test pressure, ensuring that the thickness data excludes interference from the device's own deformation. Next, the inner diameter cross-sectional area S of the sealing mold is retrieved (this parameter is a preset fixed data of the device, determined by the mold design parameters, and can be queried and corrected through the operation interface). Finally, the true thickness L, the bulk resistance value R, and the inner diameter cross-sectional area S are substituted into the ionic conductivity calculation formula. The calculation is completed by the computing module of the control system to obtain the ionic conductivity value of the solid electrolyte sample to be tested.

[0074] This step, through the comprehensive application and precise correction of multi-dimensional data, solves the problems in existing technologies where the conductivity calculation is inaccurate due to springback error in thickness measurement and failure to separate interface resistance. It achieves accurate calculation of ionic conductivity, making the calculation results more reflective of the intrinsic conductivity of the sample, and providing reliable core data for the performance evaluation of solid electrolytes.

[0075] In some embodiments, after calculating the ionic conductivity of the solid electrolyte sample to be tested, if secondary characterization of the sample is required (such as microstructure analysis, interface performance testing, etc.), or if the sample needs to be stored for a long time to maintain the pressure state and structural integrity during testing, depressurization may cause the sample to elastically rebound and the electrode-electrolyte interface to separate, thus destroying the original test state of the sample. In this case, the following steps can be performed:

[0076] This step is performed after the ionic conductivity calculation is completed and is suitable for scenarios where the original test state of the sample needs to be preserved. The device first receives the user-input third specified pressure and set torque, controlling the pressurization module to slowly increase the pressure to the third specified pressure and stabilize it for a set time, maintaining the sample's current dense state and interface contact. Then, the screw-locking module moves to the fastening screw position of the sealing mold, starts the servo motor to drive the screwdriver head to rotate, and tightens the screw according to the set torque. During the process, the torque sensor provides real-time feedback data to ensure accurate tightening force. After tightening, the pressurization module depressurizes and resets, and the sealing mold remains closed under the tightening action of the screws, stabilizing and locking the sample's structure and pressure environment. This step solves the problems of sample rebound and interface separation after testing, providing a stable sample state for secondary characterization or long-term preservation, and enhancing the extended value of the test data.

[0077] In the above embodiment, the adoption of a collaborative technical solution encompassing "baseline data calibration - stepwise sample preparation - high-pressure precision pressurization - real-time monitoring by dual sensors - dynamic pressure compensation - impedance testing - multi-data fusion calculation" effectively solves the problems of high cost in solid-state electrolyte conductivity testing, springback error in sample thickness measurement, inaccurate test results due to unstable pressure, and difficulty in automated continuous testing. This solution enables automated, high-precision, and low-cost in-situ testing of solid-state electrolyte ionic conductivity, ensuring the authenticity and consistency of test data. Furthermore, it is adaptable to testing scenarios with different pressure requirements, providing a reliable and efficient technical solution for evaluating the performance of all-solid-state battery electrolytes.

[0078] In some embodiments, during the ionic conductivity testing of solid electrolyte samples, if it is necessary to investigate the effect of pressure changes on sample conductivity, or to determine the critical pressure at which the sample exhibits optimal electrochemical performance, traditional single-point pressure testing may not be able to obtain continuous data, and manual pressure switching is inefficient and prone to large errors, making it impossible to fully grasp the relationship between pressure and conductivity. In such cases, the following steps can be performed:

[0079] The variable-pressure automated solid-state electrolyte testing device first receives pressure sequence parameters input by the user through the operating interface, including the starting pressure, ending pressure, and pressure interval (selectable as equal or unequal intervals). The system automatically generates and stores a gradient-increasing test pressure sequence. Then, the system retrieves the first pressure value in sequence and controls the pressurization module to apply pressure to the sealed mold at a preset speed. When the pressure approaches the target value, it switches to fine-tuning mode until the pressure reaches that value. Afterward, a dynamic pressure compensation step is executed. The pressure sensor monitors the pressure value in real time at a preset sampling frequency. If the pressure exceeds the preset deviation range due to sample creep or other factors, the servo mechanism of the pressurization module immediately performs active compensation until the pressure stabilizes within the deviation range. The system continuously sets the duration; once the pressure stabilizes, the electrochemical workstation automatically triggers the start of AC impedance testing. After acquiring the impedance data, it combines the baseline data and the actual sample thickness at the current pressure to quickly calculate the ionic conductivity corresponding to that pressure value, and stores the pressure value and conductivity data in a one-to-one association. After completing the test for the first pressure value, the system controls the pressurization module to depressurize, and then retrieves the next pressure value in sequence, repeating the above process of pressurization, compensation, testing, calculation, and storage until all pressure values ​​have been traversed. Finally, the system uses the data processing module to perform fitting analysis on all associated data, generating a correlation curve of ionic conductivity versus pressure. The curve can be displayed in real time on the operation interface or exported as a data file for subsequent analysis.

[0080] This step solves the problems of traditional single-point pressure testing, which makes it difficult to continuously obtain pressure-conductivity relationships and the low efficiency and large errors of manual pressure switching. It realizes automated continuous testing under multiple pressure conditions, which not only greatly improves testing efficiency and data integrity, but also provides comprehensive and quantitative data support for pressure optimization design and electrolyte performance evaluation of all-solid-state batteries.

[0081] The variable-pressure automated solid-state electrolyte testing device in the embodiments of this invention is described below from the perspective of hardware processing. Please refer to [link to relevant documentation]. Figure 4 This is a schematic diagram of the physical structure of a variable pressure automated solid electrolyte testing device in the embodiments of this application.

[0082] It should be noted that, Figure 4 The structure of the variable pressure automated solid electrolyte testing device shown is merely an example and should not impose any limitations on the functionality and scope of use of the embodiments of the present invention.

[0083] like Figure 4As shown, the variable-pressure automated solid-state electrolyte testing device includes a Central Processing Unit (CPU) 401, which can perform various appropriate actions and processes according to a program stored in Read-Only Memory (ROM) 402 or a program loaded from storage section 408 into Random Access Memory (RAM) 403, such as performing the methods described in the above embodiments. The RAM 403 also stores various programs and data required for system operation. The CPU 401, ROM 402, and RAM 403 are interconnected via a bus 404. An Input / Output (I / O) interface 405 is also connected to the bus 404.

[0084] The following components are connected to I / O interface 405: input section 406 including audio input devices, push-button switches, etc.; output section 407 including a liquid crystal display (LCD) and audio output devices, indicator lights, etc.; storage section 408 including a hard disk, etc.; and communication section 409 including a network interface card such as a LAN (Local Area Network) card, modem, etc. Communication section 409 performs communication processing via a network such as the Internet. Drive 410 is also connected to I / O interface 405 as needed. Removable media 411, such as a disk, optical disk, magneto-optical disk, semiconductor memory, etc., are installed on drive 410 as needed so that computer programs read from them can be installed into storage section 408 as needed.

[0085] In particular, according to embodiments of the present invention, the processes described above with reference to the flowcharts can be implemented as computer software programs. For example, embodiments of the present invention include a computer program product comprising a computer program carried on a computer-readable medium, the computer program containing computer programs for performing the methods shown in the flowcharts. In such embodiments, the computer program can be downloaded and installed from a network via communication section 409, and / or installed from removable medium 411. When the computer program is executed by central processing unit (CPU) 401, it performs the various functions defined in the present invention.

[0086] It should be noted that specific examples of computer-readable storage media may include, but are not limited to: electrical connections having one or more wires, portable computer disks, hard disks, random access memory (RAM), read-only memory (ROM), erasable programmable read-only memory (EPROM), flash memory, optical fiber, portable compact disc read-only memory (CD-ROM), optical storage devices, magnetic storage devices, or any suitable combination thereof. In this invention, a computer-readable storage medium can be any tangible medium containing or storing a program that can be used by or in conjunction with an instruction execution system, apparatus, or device.

[0087] The flowcharts and block diagrams in the accompanying drawings illustrate the architecture, functionality, and operation of possible implementations of systems, methods, and computer program products according to various embodiments of the present invention. Each block in a flowchart or block diagram may represent a module, program segment, or portion of code, which contains one or more executable instructions for implementing a specified logical function. It should also be noted that in some alternative implementations, the functions indicated in the blocks may occur in a different order than those shown in the drawings.

[0088] Specifically, the variable pressure automated solid electrolyte testing device of this embodiment includes a processor and a memory. The memory stores a computer program. When the computer program is executed by the processor, it implements the automated solid electrolyte conductivity testing method provided in the above embodiment.

[0089] In another aspect, the present invention also provides a computer-readable storage medium, which may be included in the variable-pressure automated solid-state electrolyte testing device described in the above embodiments; or it may exist independently and not assembled into the variable-pressure automated solid-state electrolyte testing device. The storage medium carries one or more computer programs, which, when executed by a processor of the variable-pressure automated solid-state electrolyte testing device, cause the variable-pressure automated solid-state electrolyte testing device to implement the automated solid-state electrolyte conductivity testing method provided in the above embodiments.

[0090] The above-described embodiments are only used to illustrate the technical solutions of this application, and are not intended to limit it. Although this application has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some of the technical features. Such modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of this application.

[0091] As used in the above embodiments, depending on the context, the term "when..." can be interpreted as meaning "if...", "after...", "in response to determining...", or "in response to detecting...". Similarly, depending on the context, the phrase "when determining..." or "if (the stated condition or event) is interpreted as meaning "if determining...", "in response to determining...", "when (the stated condition or event) is detected", or "in response to detecting (the stated condition or event)".

[0092] Those skilled in the art will understand that all or part of the processes in the methods of the above embodiments can be implemented by a computer program instructing related hardware. This program can be stored in a computer-readable storage medium, and when executed, it can include the processes described in the above method embodiments. The aforementioned storage medium includes various media capable of storing program code, such as ROM or random access memory (RAM), magnetic disks, or optical disks.

Claims

1. An automated method for testing the conductivity of solid electrolytes, characterized in that, An automated solid-state electrolyte testing device with variable pressure is provided. The device includes a pressurization module, a screw-locking module, and a testing module. The testing module includes a pressure sensor, a displacement sensor, and an electrochemical workstation. The method includes: Determine baseline data, which includes absolute zero-point thickness and system stiffness compensation curve. The absolute zero-point thickness is the displacement sensor reading when the upper and lower pressure heads inside the sealing mold are in direct contact. The system stiffness compensation curve is used to characterize the system deformation of the device itself under different pressures. Obtain the solid electrolyte sample to be tested; After confirming that the solid electrolyte sample to be tested has been loaded into the sealed mold, the pressurization module is controlled to pressurize the sealed mold according to the test pressure parameters input by the user. During the pressure test, the pressure value of the sealed mold and the thickness value of the solid electrolyte sample to be tested are monitored in real time using the pressure sensor and the displacement sensor. Based on the pressure value, the pressurization module is controlled to perform dynamic pressurization compensation to keep the pressure value stable at the test pressure parameter; The electrochemical workstation is controlled to perform AC impedance testing on the solid electrolyte sample to be tested, and impedance data is obtained. Based on the baseline data, the thickness value is corrected to obtain the true thickness of the solid electrolyte sample to be tested. Then, the ionic conductivity of the solid electrolyte sample to be tested is calculated by combining the true thickness and the impedance data. The steps for obtaining the solid electrolyte sample to be tested specifically include: After confirming that the solid electrolyte powder has been loaded into the sealed mold, the pressurization module is controlled to pressurize to the first specified pressure input by the user, and after maintaining the pressure for a first preset time, the pressurization module is controlled to reset. After the first electrode is inserted into the first position of the sealing mold, the pressurization module is controlled to pressurize to the second specified pressure input by the user and maintain it for a second preset time, and then the pressurization module is controlled to reset. After the second electrode is inserted into the set second position of the sealing mold, the pressurization module is controlled to pressurize to the second specified pressure and maintain it for the second preset time. The pressurization module is then controlled to reset, and the solid electrolyte sample to be tested is obtained. The step of controlling the pressurization module to perform dynamic pressurization compensation based on the pressure value specifically includes: Set the allowable pressure deviation range and thickness fluctuation threshold; Read the values ​​of the pressure sensor and displacement sensor at a preset sampling frequency; If the pressure value is detected to decrease due to powder creep and exceed the pressure deviation range, and the thickness change does not exceed the thickness fluctuation threshold, then the servo mechanism of the pressurization module is controlled to feed downwards to perform active pressure compensation. The thickness change trajectory during the compensation process is recorded in real time, serving as a basis for determining the sample molding density.

2. The method according to claim 1, characterized in that, The step of determining the baseline data specifically includes: The pressurization module is controlled to compress the unloaded sealing mold at a first speed; When the pressure reaches the preset calibration pressure, the displacement value of the displacement sensor is recorded; The absolute zero point thickness is determined based on the displacement value; According to the preset pressure gradient, the displacement change of the absolute zero point thickness at different pressure points is recorded to generate the system stiffness compensation curve. Control the resetting of the pressurization module.

3. The method according to claim 1, characterized in that, The steps of correcting the thickness value based on the baseline data to obtain the true thickness of the solid electrolyte sample to be tested, and then calculating the ionic conductivity of the solid electrolyte sample to be tested by combining the true thickness and the impedance data, specifically include: The electrochemical impedance spectroscopy generated by the electrochemical workstation was obtained, and the bulk resistance of the solid electrolyte sample under test was determined by fitting a circuit model. ; Based on the system stiffness compensation curve, determine the system deformation under the current pressure; The real-time reading of the displacement sensor at the test moment is obtained as the thickness value. The absolute zero-point thickness, the thickness of the first electrode and the second electrode, and the system deformation corresponding to the baseline data are subtracted to obtain the true thickness of the sample. ; Obtain the inner diameter cross-sectional area of ​​the sealing mold. ; Calculate the ionic conductivity of the solid electrolyte sample to be tested. The specific formula is as follows: 。 4. The method according to claim 1, characterized in that, Also includes: Set a set of test stress sequences that increase in a gradient; The pressurization module is controlled to apply each pressure value in the test pressure sequence to the sealing mold in sequence. At each pressure value, the dynamic pressure compensation step is executed. After the pressure stabilizes within the preset deviation range, the electrochemical workstation is triggered to test and record the ionic conductivity at the current pressure. After traversing all pressure values, a correlation curve of the ionic conductivity of the solid electrolyte sample under test as a function of pressure is generated.

5. The method according to claim 1, characterized in that, After the step of calculating the ionic conductivity of the solid electrolyte sample to be tested, the method further includes: Control the pressurization module to pressurize to the third specified pressure input by the user; The screw-locking module is controlled to tighten the fastening screws of the sealing mold to a set torque.

6. A variable-pressure automated solid-state electrolyte testing device, characterized in that, The variable pressure automated solid electrolyte testing device includes: one or more processors and a memory; the memory is coupled to the one or more processors, the memory is used to store computer program code, the computer program code includes computer instructions, and the one or more processors call the computer instructions to cause the variable pressure automated solid electrolyte testing device to perform the method as described in any one of claims 1-5.

7. A computer-readable storage medium comprising instructions, characterized in that, When the instruction is executed on the variable pressure automated solid electrolyte test apparatus, the variable pressure automated solid electrolyte test apparatus performs the method as described in any one of claims 1-5.

8. A computer program product, comprising a computer program, characterized in that, When the computer program is run on the variable pressure automated solid electrolyte testing device, the variable pressure automated solid electrolyte testing device performs the method as described in any one of claims 1-5.

Images