Solid-state impedance spectroscopy(SS-IS)was used to investigate the influence of structural modifications resulting from the addition of Nb2O5 on the dielectric properties and relaxation processes in the quaternary m...Solid-state impedance spectroscopy(SS-IS)was used to investigate the influence of structural modifications resulting from the addition of Nb2O5 on the dielectric properties and relaxation processes in the quaternary mixed glass former(MGF)system 35Na_(2)O–10V_(2)O_(5)–(55-x)P_(2)O_(5)–xNb_(2)O_(5)(x=0–40,mol%).The dielectric parameters,including the dielectric strength and dielectric loss,are determined from the frequency and temperature-dependent complex permittivity data,revealing a significant dependence on the Nb2O5 content.The transition from a predominantly phosphate glass network(x<10,region I)to a mixed niobate–phosphate glass net-work(10≤x≤20,region II)leads to an increase in the dielectric parameters,which correlates with the observed trend in the direct-cur-rent(DC)conductivity.In the predominantly niobate network(x≥25,region III),the highly polarizable nature of Nb5+ions leads to a fur-ther increase in the dielectric permittivity and dielectric strength.This is particularly evident in Nb-40 glass-ceramic,which contains Na_(13)Nb_(35)O_(94) crystalline phase with a tungsten bronze structure and exhibits the highest dielectric permittivity of 61.81 and the lowest loss factor of 0.032 at 303 K and 10 kHz.The relaxation studies,analyzed through modulus formalism and complex impedance data,show that DC conductivity and relaxation processes are governed by the same mechanism,attributed to ionic conductivity.In contrast to glasses with a single peak in frequency dependence of imaginary part of electrical modulus,M″(ω),Nb-40 glass-ceramic exhibits two distinct contributions with similar relaxation times.The high-frequency peak indicates bulk ionic conductivity,while the additional low-fre-quency peak is associated with the grain boundary effect,confirmed by the electrical equivalent circuit(EEC)modelling.The scaling characteristics of permittivity and conductivity spectra,along with the electrical modulus,validate time-temperature superposition and demonstrate a strong correlation with composition and modification of the glass structure upon Nb_(2)O_(5) incorporation.展开更多
Utilizing machine learning techniques for data-driven diagnosis of high temperature PEM fuel cells is beneficial and meaningful to the system durability. Nevertheless, ensuring the robustness of diagnosis remains a cr...Utilizing machine learning techniques for data-driven diagnosis of high temperature PEM fuel cells is beneficial and meaningful to the system durability. Nevertheless, ensuring the robustness of diagnosis remains a critical and challenging task in real application. To enhance the robustness of diagnosis and achieve a more thorough evaluation of diagnostic performance, a robust diagnostic procedure based on electrochemical impedance spectroscopy (EIS) and a new method for evaluation of the diagnosis robustness was proposed and investigated in this work. To improve the diagnosis robustness: (1) the degradation mechanism of different faults in the high temperature PEM fuel cell was first analyzed via the distribution of relaxation time of EIS to determine the equivalent circuit model (ECM) with better interpretability, simplicity and accuracy;(2) the feature extraction was implemented on the identified parameters of the ECM and extra attention was paid to distinguishing between the long-term normal degradation and other faults;(3) a Siamese Network was adopted to get features with higher robustness in a new embedding. The diagnosis was conducted using 6 classic classification algorithms—support vector machine (SVM), K-nearest neighbor (KNN), logistic regression (LR), decision tree (DT), random forest (RF), and Naive Bayes employing a dataset comprising a total of 1935 collected EIS. To evaluate the robustness of trained models: (1) different levels of errors were added to the features for performance evaluation;(2) a robustness coefficient (Roubust_C) was defined for a quantified and explicit evaluation of the diagnosis robustness. The diagnostic models employing the proposed feature extraction method can not only achieve the higher performance of around 100% but also higher robustness for diagnosis models. Despite the initial performance being similar, the KNN demonstrated a superior robustness after feature selection and re-embedding by triplet-loss method, which suggests the necessity of robustness evaluation for the machine learning models and the effectiveness of the defined robustness coefficient. This work hopes to give new insights to the robust diagnosis of high temperature PEM fuel cells and more comprehensive performance evaluation of the data-driven method for diagnostic application.展开更多
Machine learning-based methods have emerged as a promising solution to accurate battery capacity estimation for battery management systems.However,they are generally developed in a supervised manner which requires a c...Machine learning-based methods have emerged as a promising solution to accurate battery capacity estimation for battery management systems.However,they are generally developed in a supervised manner which requires a considerable number of input features and corresponding capacities,leading to prohibitive costs and efforts for data collection.In response to this issue,this study proposes a convolutional neural network(CNN)based method to perform end-to-end capacity estimation by taking only raw impedance spectra as input.More importantly,an input reconstruction module is devised to effectively exploit impedance spectra without corresponding capacities in the training process,thereby significantly alleviating the cost of collecting training data.Two large battery degradation datasets encompassing over 4700 impedance spectra are developed to validate the proposed method.The results show that accurate capacity estimation can be achieved when substantial training samples with measured capacities are given.However,the estimation performance of supervised machine learning algorithms sharply deteriorates when fewer samples with measured capacities are available.In this case,the proposed method outperforms supervised benchmarks and can reduce the root mean square error by up to 50.66%.A further validation under different current rates and states of charge confirms the effectiveness of the proposed method.Our method provides a flexible approach to take advantage of unlabelled samples for developing data-driven models and is promising to be generalised to other battery management tasks.展开更多
Accurate prediction of performance degradation in complex systems such as solid oxide fuel cells is crucial for expediting technological advancements.However,significant challenges still persist due to limited compreh...Accurate prediction of performance degradation in complex systems such as solid oxide fuel cells is crucial for expediting technological advancements.However,significant challenges still persist due to limited comprehension of degradation mechanisms and difficulties in acquiring in-situ features.In this study,we propose an effective approach that integrates long short-term memory(LSTM) neural network and dynamic electrochemical impedance spectroscopy(DEIS).This integrated approach enables precise prediction of future evolutions in both current-voltage and EIS features using historical testing data,without prior knowledge of degradation mechanisms.For short-term predictions spanning hundreds of hours,our approach achieves a prediction accuracy exceeding 0.99,showcasing promising prospects for diagnostic applications.Additionally,for long-term predictions spanning thousands of hours,we quantitatively determine the significance of each degradation mechanism,which is crucial for enhancing cell durability.Moreover,our proposed approach demonstrates satisfactory predictive ability in both time and frequency domains,offering the potential to reduce EIS testing time by more than half.展开更多
A novel method for detecting early damage at the steel-concrete interface due to external loading based on AC impedance spectroscopy technology was proposed.Firstly,alkali pretreatment was introduced to ensure the acc...A novel method for detecting early damage at the steel-concrete interface due to external loading based on AC impedance spectroscopy technology was proposed.Firstly,alkali pretreatment was introduced to ensure the accuracy and repeatability of the AC impedance test.Secondly,the AC impedance spectroscopy between the steel bar and concrete surface of different bonding positions was tested,and then the physical quantities reflecting the bonding damage condition were obtained by equivalent circuit fitting.Theoretical debonding position calculation and AC conductive structure analysis indicate that the change of interface resistance and interface capacitance can seize the development of bonding damage during the loading process.As the interface damage develops,obvious changes in interface resistance and interface capacitance are observed,and they cannot be recovered after unloading.展开更多
Impedance spectroscopy has been increasingly employed in quantum dot light-emitting diodes(QLEDs)to investigate the charge dynamics and device physics.In this review,we introduce the mathematical basics of impedance s...Impedance spectroscopy has been increasingly employed in quantum dot light-emitting diodes(QLEDs)to investigate the charge dynamics and device physics.In this review,we introduce the mathematical basics of impedance spectroscopy that applied to QLEDs.In particular,we focus on the Nyquist plot,Mott-Schottky analysis,capacitance-frequency and capacitance-voltage characteristics,and the d C/d V measurement of the QLEDs.These impedance measurements can provide critical information on electrical parameters such as equivalent circuit models,characteristic time constants,charge injection and recombination points,and trap distribution of the QLEDs.However,this paper will also discuss the disadvantages and limitations of these measurements.Fundamentally,this review provides a deeper understanding of the device physics of QLEDs through the application of impedance spectroscopy,offering valuable insights into the analysis of performance loss and degradation mechanisms of QLEDs.展开更多
With the increasing interest in highly concentrated electrolyte systems,correct determination of the cation transference number is important.Pulsed-field gradient NMR technique,which measures self-diffusion coefficien...With the increasing interest in highly concentrated electrolyte systems,correct determination of the cation transference number is important.Pulsed-field gradient NMR technique,which measures self-diffusion coefficients,is often applied on liquid electrolytes because of the wide accessibility and simple sample preparation.However,since the assumptions of this technique,that is,complete salt dissociation,all ions participating in motion,and all of them moving independently,no longer hold true in concentrated solutions,the transference numbers,thus obtained are often over-estimated.In the present work,impedance spectroscopy at a frequency range of 1 MHz to 0.1 mHz was used to examine the concentration effect on lithium-ion transference number under anion-blocking conditions T abc Liþfor two electrolytes:lithium bis(fluorosulfonyl)imide(LiFSI)in sulfolane(SL)and lithium bis(trifluorosulfonyl)imide(LiTFSI)in tetraglyme(G4).The T abc Liþof the former was almost an order of magnitude higher than that of the latter.It also appeared to increase with increasing concentration while the latter followed an opposite trend.The faster Li^(+)transport in the SL system is attributed to the formation of a liquid structure consisting of extended chains/bridges of SL molecules and the anions,which facilitate a cation-hopping/ligand-exchanged-typed diffusion mechanism by partially decoupling the cations from the anions and solvent molecules.The G4 system,in contrast,is dominated by the formation of long-lived,stable[Li(G4)]+solvation cages that results in a sluggish Li+transport.The difference between the two transport mechanisms is discussed via comparison of the bulk ionic conductivity,viscosity,ion self-diffusion coefficients,and the Onsager transport coefficients.展开更多
3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was...3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was investigated using impedance spectroscopy （IS） combined with scanning electron microscopy （SEM）, Raman spectroscopy and X-ray diffractometry （XRD）. Various electrical responses observed in the impedance spectra corresponding to GY-YSZ grains and grain boundaries were explained using circuit modeling. The change in the conduction mechanism of GY-YSZ was found to be related to the O^2- vacancy and lattice distortion due to the stabilizer diffusion during the oxidation. The results also suggested that the specific oxidation information about the GY-YSZ grains and grain boundaries should be acquired at a moderate measurement temperature, which was related to the resistance value in the impedance spectra. The resistance values of the GY-YSZ grains and grain boundaries should be measured at 200 ℃ and 300 ℃, respectively.展开更多
The passive film formed on 2205 duplex stainless steel（DSS） in 0.5 M NaHCO3＋0.5 M NaCl aqueous solution was characterized by electrochemical measurements,including potentiodynamic anodic polarization and dynamic el...The passive film formed on 2205 duplex stainless steel（DSS） in 0.5 M NaHCO3＋0.5 M NaCl aqueous solution was characterized by electrochemical measurements,including potentiodynamic anodic polarization and dynamic electrochemical impedance spectroscopy（DEIS）.The results demonstrate that there is a great difference between the passive film evolutions of ferrite and austenite.The impedance values of ferrite are higher than those of austenite.The impedance peaks of ferritic and austenitic phases correspond to the potential of 0.15 and 0.25 V in the low potential range and correspond to 0.8 and 0.75 V in the high potential range.The evolutions of the capacitance of both phases are reverse compared to the evolutions of impedance.The thickness variations obtained from capacitance agree well with those of impedance analysis.The results can be used to explain why pitting corrosion occurs more easily in austenite phase than in ferrite phase.展开更多
The degradation coefficient is proposed to evaluate the degradation degree of organic coatings by directly anaIyzing the Bode plots of the electrochemical impedance spectroscopy （EIS） data. This paper investigated t...The degradation coefficient is proposed to evaluate the degradation degree of organic coatings by directly anaIyzing the Bode plots of the electrochemical impedance spectroscopy （EIS） data. This paper investigated the degradation of phenolic epoxy coating/tinplate system by EIS and the degradation coefficient value, which correlates well with the results of breakpoint frequency and variation of phase angle at 10 Hz. Furthermore, the degradation process was confirmed by scanning electron microscope （SEM） and scanning probe microscopy （SPM）. It is concluded that degradation coefficient can be used for the fast evaluation of degradation degree of organic coatings in practical appli- cations.展开更多
The welded joints of 3Cr pipeline steel were fabricated with commercial welding wire using the gas tungsten arc welding （GTAW） technique. Potentiodynamic polarization curves, linear polarization resistance （LPR）, ...The welded joints of 3Cr pipeline steel were fabricated with commercial welding wire using the gas tungsten arc welding （GTAW） technique. Potentiodynamic polarization curves, linear polarization resistance （LPR）, electrochemical impedance spectroscopy （EIS）, scan- ning electron microscopy （SEM）, and energy-dispersive spectrometry （EDS） were used to investigate the corrosion resistance and the growth of a corrosion film on the weld zone （WZ）. The changes in electrochemical characteristics of the film were obtained through fitting of the EIS data. The results showed that the average corrosion rate of the WZ in CO2 environments first increased, then fluctuated, and finally de- creased gradually. The formation of the film on the WZ was divided into three stages： dynamic adsorption, incomplete-coverage layer forma- tion, and integral layer formation.展开更多
Pitting corrosion of 316L stainless steel in NaCl solution was investigated by means of staircase potential electrochemical impedance spectroscopy（SPEIS）.The investigation focused on the transition of stainless stee...Pitting corrosion of 316L stainless steel in NaCl solution was investigated by means of staircase potential electrochemical impedance spectroscopy（SPEIS）.The investigation focused on the transition of stainless steel from the passive state to pitting corrosion.Based on the evolution of electrical parameters of the equivalent electrical circuit,it is suggested that the most probable mechanism of pit creation is the film breaking model.The result demonstrates that staircase potential electrochemical impedance spectroscopy is an effective method for the investigation of pitting corrosion.展开更多
The corrosion inhibition for carbon steel in circulating cooling water by modified lignosulphonate has been investigated using electrochemical impedance spectroscopy technique. Results show that the inhibition efficie...The corrosion inhibition for carbon steel in circulating cooling water by modified lignosulphonate has been investigated using electrochemical impedance spectroscopy technique. Results show that the inhibition efficiency of modified lignosulphonate GCL2 is a great improvement on that of lignosulphonate. The maximum inhibition efficiency of GCL2 reaches 99.21% at the concentration of 400mg·L^-1 at 303K. The corrosion inhibition of GCL2 is attributed to forming adsorption film on the metal surface for the electrochemical impedance spectroscopy in GCL2 solution shows more than one time-constant.Moreover,results also indicate that it is more efficient in stirring solution than in still solution for GCL2 because the constant of adsorption in stirring solution is much larger than that in still solution. The adsorption of inhibitor GCL2 follows Langmuir＇s adsorption isotherm.展开更多
The corrosion behaviors of Fe-Cr alloy under three different pH values solutions with C1- and SO42- were investigated by localized electrochemical impedance spectroscopy （LEIS） measurements and the corrosion product...The corrosion behaviors of Fe-Cr alloy under three different pH values solutions with C1- and SO42- were investigated by localized electrochemical impedance spectroscopy （LEIS） measurements and the corrosion products were analyzed by laser Raman spectrometry. The results show that the high corrosion resistance of Fe-Cr Alloy is attributed to a passive film which is formed more easily when the alloy contains a large quantity of Cr element. However, its corrosion resistance varies in the solutions with different pH values, especially in the initial corrosion. The average impedance values in neutral and alkaline solution are much higher than that in acidic solution because the passive film is more likely to dissolve in the acidic condition. Moreover, the destructive effect of C1- and SO42 ions on the passive film is also demonstrated in corrosion process through the change of the impedance value with the steeping time.展开更多
BaBiO3-doped BaTiO3 （BB-BT） ceramic, as a candidate for lead-free positive temperature coefficient of resistivity （PTCR） materials with a higher Curie temperature, has been synthesized in air by a conventional sin...BaBiO3-doped BaTiO3 （BB-BT） ceramic, as a candidate for lead-free positive temperature coefficient of resistivity （PTCR） materials with a higher Curie temperature, has been synthesized in air by a conventional sintering technique. The temperature dependence of resistivity shows that the phase transition of the PTC thermistor ceramic occurs at the Curie temperature, Tc = 155℃, which is higher than that of BaTiO3 （≤ 130 ℃）. Analysis of ac impedance data using complex impedance spectroscopy gives the alternate current （AC） resistance of the PTCR ceramic. By additional use of the complex electric modulus formalism to analyse the same data, the inhomogeneous nature of the ceramic may be unveiled. The impedance spectra reveal that the grain resistance of the BB-BT sample is slightly influenced by the increase of temperature, indicating that the increase in overall resistivity is entirely due to a grain-boundary effect. Based on the dependence of the extent to which the peaks of the imaginary part of electric modulus and impedance are matched on frequency, the conduction mechanism is also discussed for a BB-BT ceramic system.展开更多
The electrochemical characteristics of 1Cr18Ni9Ti in sulphate-reducing bacteria （SRB） solutions and the biofilm of SRB on the surface of the 1Cr18Ni9Ti electrode were studied by electrochemical, microbiological, and...The electrochemical characteristics of 1Cr18Ni9Ti in sulphate-reducing bacteria （SRB） solutions and the biofilm of SRB on the surface of the 1Cr18Ni9Ti electrode were studied by electrochemical, microbiological, and surface analysis methods. Electrochemical impedance spectroscopy （EIS） of 1Cr18Ni9Ti was measured in the solutions with and without SRB at the culture time of 2, 4, 8 d, respectively. The measurement used two test methods, the nonimmersion electrode method and the immersion electrode method. It was found that the polarization resistance （Rp） of 1Cr18Ni9Ti in the solutions without SRB is the greatest for each test method. When using the nonimmersion electrode method, Rp shifts negatively at first and then positively, and the time constant is only one. Although using the immersion electrode method, the Rp shifts positively at first and then negatively, and the time constant also changes when the biofilm forms. The biofilm observed through SEM is with pores. It was demonstrated that SRB has accelerated corrosion action on 1Cr18Ni9Ti. The protection effect of the biofilm on the electrode depends on the compact degree of the film.展开更多
A microfabricated electrical impedance spectroscopy (EIS) chip with microelectrodes was developed.The substrate and the electrodes of the chip were made of glass and gold,respectively.The experimental results demonstr...A microfabricated electrical impedance spectroscopy (EIS) chip with microelectrodes was developed.The substrate and the electrodes of the chip were made of glass and gold,respectively.The experimental results demonstrated that the EIS-chip could distinguish different solutions (physiological saline,culture medium,living cell suspension etc.) by scanning from 10Hz to 45kHz.A 6-element circuit model was used for fitting the real part and the imaginary part admittance curves of the living cell suspension.An actual circuit was also built and tested to verify the 6-element circuit model proposed.The micro-EIS chip has several advantages including the use of small sample volumes,high resolution and ease of operation.It shows good application prospects in the areas of cellular electrophysioiogy,drug screening and bio-sensors etc.展开更多
A sinusoidal voltage wave generator is proposed based on the use of micro-processor digital signals with programmable duty-cycles, with application to real-time Electrical Cell-substrate Impedance Spectroscopy (ECIS) ...A sinusoidal voltage wave generator is proposed based on the use of micro-processor digital signals with programmable duty-cycles, with application to real-time Electrical Cell-substrate Impedance Spectroscopy (ECIS) assays in cell cultures. The working principle relies on the time convolution of the programmed microcontroller (μC) digital signals. The expected frequency is easily tuned on the bio-impedance spectroscopy range [100 Hz, 1 MHz] thanks to the μC clock frequency selection. This system has been simulated and tested on the 8 bits μC Arduino<sup>TM </sup>Uno with ATmega328 version. Results obtained prove that only three digital signals are required to fit the general specification in ECIS experiments, below 1% THD accuracy, and show the appropriateness of the system for the real-time monitoring of this type of biological experiments.展开更多
Despite great progress in lithium-sulfur(Li-S) batteries, the electrochemical reactions in the cell are not yet fully understood. Electrode processes, complex interfaces and internal resistance may be characterized by...Despite great progress in lithium-sulfur(Li-S) batteries, the electrochemical reactions in the cell are not yet fully understood. Electrode processes, complex interfaces and internal resistance may be characterized by electrochemical impedance spectroscopy(EIS). EIS is a non-destructive technique and easy to apply, though there are challenges in ensuring the reproducibility of measurements and the interpretation of impedance data. Here, we present the impedance behavior of a 3.4 Ah Li-S pouch cell characterized by EIS. The impedance changes were analyzed over the entire depth-of-discharge, depth-of-charge,and at various temperatures. Based on the formation of intermediates during(dis)charging, the changes of resistances are observed. Overall, the increase in temperature causes a decrease in electrolyte viscosity,lowering the surface energy which can improve the penetration of the electrolyte into the electrode pores. Moreover, the effect of superimposed AC current during EIS measurement was analyzed, and the results show the dependence of the charge transfer resistance on superimposed AC current which was lower compared to steady-state conditions and consents with theory.展开更多
The complex impedance spectroscopy and surface morphology of Mn1+xFe2-2xTixO4(0≤x≤0.5) system,prepared using a conventional solid state reaction technique,were investigated.The impedance spectroscopy measurements we...The complex impedance spectroscopy and surface morphology of Mn1+xFe2-2xTixO4(0≤x≤0.5) system,prepared using a conventional solid state reaction technique,were investigated.The impedance spectroscopy measurements were carried out at room temperature in the frequency range of 42-5 MHz.The electrical processes in the samples were modeled in the form of an equivalent circuit made up of a combination of two parallel RC circuits attributed to grain and grain boundaries.The DC conductivity obtained by extrapolation of AC data using impedance spectroscopy and four-probe method increases at 10% doping of Ti ions.The energy-dispersive X-ray(EDX) pattern confirmed the homogeneous mixing of the Mn,Fe,Ti and O atoms in pure and doped ferrite samples.展开更多
文摘Solid-state impedance spectroscopy(SS-IS)was used to investigate the influence of structural modifications resulting from the addition of Nb2O5 on the dielectric properties and relaxation processes in the quaternary mixed glass former(MGF)system 35Na_(2)O–10V_(2)O_(5)–(55-x)P_(2)O_(5)–xNb_(2)O_(5)(x=0–40,mol%).The dielectric parameters,including the dielectric strength and dielectric loss,are determined from the frequency and temperature-dependent complex permittivity data,revealing a significant dependence on the Nb2O5 content.The transition from a predominantly phosphate glass network(x<10,region I)to a mixed niobate–phosphate glass net-work(10≤x≤20,region II)leads to an increase in the dielectric parameters,which correlates with the observed trend in the direct-cur-rent(DC)conductivity.In the predominantly niobate network(x≥25,region III),the highly polarizable nature of Nb5+ions leads to a fur-ther increase in the dielectric permittivity and dielectric strength.This is particularly evident in Nb-40 glass-ceramic,which contains Na_(13)Nb_(35)O_(94) crystalline phase with a tungsten bronze structure and exhibits the highest dielectric permittivity of 61.81 and the lowest loss factor of 0.032 at 303 K and 10 kHz.The relaxation studies,analyzed through modulus formalism and complex impedance data,show that DC conductivity and relaxation processes are governed by the same mechanism,attributed to ionic conductivity.In contrast to glasses with a single peak in frequency dependence of imaginary part of electrical modulus,M″(ω),Nb-40 glass-ceramic exhibits two distinct contributions with similar relaxation times.The high-frequency peak indicates bulk ionic conductivity,while the additional low-fre-quency peak is associated with the grain boundary effect,confirmed by the electrical equivalent circuit(EEC)modelling.The scaling characteristics of permittivity and conductivity spectra,along with the electrical modulus,validate time-temperature superposition and demonstrate a strong correlation with composition and modification of the glass structure upon Nb_(2)O_(5) incorporation.
基金supported by the Chinese Scholarship Council(Nos.202208320055 and 202108320111)the support from the energy department of Aalborg University was acknowledged.
文摘Utilizing machine learning techniques for data-driven diagnosis of high temperature PEM fuel cells is beneficial and meaningful to the system durability. Nevertheless, ensuring the robustness of diagnosis remains a critical and challenging task in real application. To enhance the robustness of diagnosis and achieve a more thorough evaluation of diagnostic performance, a robust diagnostic procedure based on electrochemical impedance spectroscopy (EIS) and a new method for evaluation of the diagnosis robustness was proposed and investigated in this work. To improve the diagnosis robustness: (1) the degradation mechanism of different faults in the high temperature PEM fuel cell was first analyzed via the distribution of relaxation time of EIS to determine the equivalent circuit model (ECM) with better interpretability, simplicity and accuracy;(2) the feature extraction was implemented on the identified parameters of the ECM and extra attention was paid to distinguishing between the long-term normal degradation and other faults;(3) a Siamese Network was adopted to get features with higher robustness in a new embedding. The diagnosis was conducted using 6 classic classification algorithms—support vector machine (SVM), K-nearest neighbor (KNN), logistic regression (LR), decision tree (DT), random forest (RF), and Naive Bayes employing a dataset comprising a total of 1935 collected EIS. To evaluate the robustness of trained models: (1) different levels of errors were added to the features for performance evaluation;(2) a robustness coefficient (Roubust_C) was defined for a quantified and explicit evaluation of the diagnosis robustness. The diagnostic models employing the proposed feature extraction method can not only achieve the higher performance of around 100% but also higher robustness for diagnosis models. Despite the initial performance being similar, the KNN demonstrated a superior robustness after feature selection and re-embedding by triplet-loss method, which suggests the necessity of robustness evaluation for the machine learning models and the effectiveness of the defined robustness coefficient. This work hopes to give new insights to the robust diagnosis of high temperature PEM fuel cells and more comprehensive performance evaluation of the data-driven method for diagnostic application.
基金supported by the National Key R&D Program of China(2021YFB2402002)the National Natural Science Foundation of China(51922006 and 51877009)+1 种基金the China Postdoctoral Science Foundation(BX2021035 and 2022M710379)the Beijing Natural Science Foundation(Grant No.L223013)。
文摘Machine learning-based methods have emerged as a promising solution to accurate battery capacity estimation for battery management systems.However,they are generally developed in a supervised manner which requires a considerable number of input features and corresponding capacities,leading to prohibitive costs and efforts for data collection.In response to this issue,this study proposes a convolutional neural network(CNN)based method to perform end-to-end capacity estimation by taking only raw impedance spectra as input.More importantly,an input reconstruction module is devised to effectively exploit impedance spectra without corresponding capacities in the training process,thereby significantly alleviating the cost of collecting training data.Two large battery degradation datasets encompassing over 4700 impedance spectra are developed to validate the proposed method.The results show that accurate capacity estimation can be achieved when substantial training samples with measured capacities are given.However,the estimation performance of supervised machine learning algorithms sharply deteriorates when fewer samples with measured capacities are available.In this case,the proposed method outperforms supervised benchmarks and can reduce the root mean square error by up to 50.66%.A further validation under different current rates and states of charge confirms the effectiveness of the proposed method.Our method provides a flexible approach to take advantage of unlabelled samples for developing data-driven models and is promising to be generalised to other battery management tasks.
基金partly supported by Japan Society for the Promotion of Science (JSPS) Postdoctoral Fellowships for Research in Japan (P22370)by Key Project of Jiangsu Province (BE2022029) in China。
文摘Accurate prediction of performance degradation in complex systems such as solid oxide fuel cells is crucial for expediting technological advancements.However,significant challenges still persist due to limited comprehension of degradation mechanisms and difficulties in acquiring in-situ features.In this study,we propose an effective approach that integrates long short-term memory(LSTM) neural network and dynamic electrochemical impedance spectroscopy(DEIS).This integrated approach enables precise prediction of future evolutions in both current-voltage and EIS features using historical testing data,without prior knowledge of degradation mechanisms.For short-term predictions spanning hundreds of hours,our approach achieves a prediction accuracy exceeding 0.99,showcasing promising prospects for diagnostic applications.Additionally,for long-term predictions spanning thousands of hours,we quantitatively determine the significance of each degradation mechanism,which is crucial for enhancing cell durability.Moreover,our proposed approach demonstrates satisfactory predictive ability in both time and frequency domains,offering the potential to reduce EIS testing time by more than half.
基金Funded by the Opening Funds of State Key Laboratory of Building Safety and Built Environment and National Engineering Research Center of Building Technology (No.BSBE2019-07)the Young Talent Support Program of Hebei Institutions of Higher Learning (No.BJ2017019)the National Natural Science Foundation of China (No.51808357)。
文摘A novel method for detecting early damage at the steel-concrete interface due to external loading based on AC impedance spectroscopy technology was proposed.Firstly,alkali pretreatment was introduced to ensure the accuracy and repeatability of the AC impedance test.Secondly,the AC impedance spectroscopy between the steel bar and concrete surface of different bonding positions was tested,and then the physical quantities reflecting the bonding damage condition were obtained by equivalent circuit fitting.Theoretical debonding position calculation and AC conductive structure analysis indicate that the change of interface resistance and interface capacitance can seize the development of bonding damage during the loading process.As the interface damage develops,obvious changes in interface resistance and interface capacitance are observed,and they cannot be recovered after unloading.
基金supported by National Key Research and Development Program of China(Nos.2021YFB3602703,2022YFB3606504,and 2022YFB3602903)Shenzhen Key Laboratory for Advanced Quantum Dot Displays and Lighting(No.ZDSYS201707281632549)Shenzhen Science and Technology Program(No.JCYJ20220818100411025)。
文摘Impedance spectroscopy has been increasingly employed in quantum dot light-emitting diodes(QLEDs)to investigate the charge dynamics and device physics.In this review,we introduce the mathematical basics of impedance spectroscopy that applied to QLEDs.In particular,we focus on the Nyquist plot,Mott-Schottky analysis,capacitance-frequency and capacitance-voltage characteristics,and the d C/d V measurement of the QLEDs.These impedance measurements can provide critical information on electrical parameters such as equivalent circuit models,characteristic time constants,charge injection and recombination points,and trap distribution of the QLEDs.However,this paper will also discuss the disadvantages and limitations of these measurements.Fundamentally,this review provides a deeper understanding of the device physics of QLEDs through the application of impedance spectroscopy,offering valuable insights into the analysis of performance loss and degradation mechanisms of QLEDs.
基金This work was supported by US Department of Army and the Joint Center for Energy Storage Research(JCESR),an Energy Innovation Hub funded by Depart-ment of Energy,Basic Energy Science,under an Interagency Agreement No.IAA SN202095.
文摘With the increasing interest in highly concentrated electrolyte systems,correct determination of the cation transference number is important.Pulsed-field gradient NMR technique,which measures self-diffusion coefficients,is often applied on liquid electrolytes because of the wide accessibility and simple sample preparation.However,since the assumptions of this technique,that is,complete salt dissociation,all ions participating in motion,and all of them moving independently,no longer hold true in concentrated solutions,the transference numbers,thus obtained are often over-estimated.In the present work,impedance spectroscopy at a frequency range of 1 MHz to 0.1 mHz was used to examine the concentration effect on lithium-ion transference number under anion-blocking conditions T abc Liþfor two electrolytes:lithium bis(fluorosulfonyl)imide(LiFSI)in sulfolane(SL)and lithium bis(trifluorosulfonyl)imide(LiTFSI)in tetraglyme(G4).The T abc Liþof the former was almost an order of magnitude higher than that of the latter.It also appeared to increase with increasing concentration while the latter followed an opposite trend.The faster Li^(+)transport in the SL system is attributed to the formation of a liquid structure consisting of extended chains/bridges of SL molecules and the anions,which facilitate a cation-hopping/ligand-exchanged-typed diffusion mechanism by partially decoupling the cations from the anions and solvent molecules.The G4 system,in contrast,is dominated by the formation of long-lived,stable[Li(G4)]+solvation cages that results in a sluggish Li+transport.The difference between the two transport mechanisms is discussed via comparison of the bulk ionic conductivity,viscosity,ion self-diffusion coefficients,and the Onsager transport coefficients.
基金Projects (50771009, 50731001 and 51071013) supported by the National Natural Science Foundations of China Project (2010CB631200) supported by the National Basic Research Program of China
文摘3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was investigated using impedance spectroscopy （IS） combined with scanning electron microscopy （SEM）, Raman spectroscopy and X-ray diffractometry （XRD）. Various electrical responses observed in the impedance spectra corresponding to GY-YSZ grains and grain boundaries were explained using circuit modeling. The change in the conduction mechanism of GY-YSZ was found to be related to the O^2- vacancy and lattice distortion due to the stabilizer diffusion during the oxidation. The results also suggested that the specific oxidation information about the GY-YSZ grains and grain boundaries should be acquired at a moderate measurement temperature, which was related to the resistance value in the impedance spectra. The resistance values of the GY-YSZ grains and grain boundaries should be measured at 200 ℃ and 300 ℃, respectively.
基金supported by the National Natural Science Foundation of China(No.50871020)
文摘The passive film formed on 2205 duplex stainless steel（DSS） in 0.5 M NaHCO3＋0.5 M NaCl aqueous solution was characterized by electrochemical measurements,including potentiodynamic anodic polarization and dynamic electrochemical impedance spectroscopy（DEIS）.The results demonstrate that there is a great difference between the passive film evolutions of ferrite and austenite.The impedance values of ferrite are higher than those of austenite.The impedance peaks of ferritic and austenitic phases correspond to the potential of 0.15 and 0.25 V in the low potential range and correspond to 0.8 and 0.75 V in the high potential range.The evolutions of the capacitance of both phases are reverse compared to the evolutions of impedance.The thickness variations obtained from capacitance agree well with those of impedance analysis.The results can be used to explain why pitting corrosion occurs more easily in austenite phase than in ferrite phase.
基金Supported by Major State Basic Research Program of China ("973"Program,No. 2011CB610500)
文摘The degradation coefficient is proposed to evaluate the degradation degree of organic coatings by directly anaIyzing the Bode plots of the electrochemical impedance spectroscopy （EIS） data. This paper investigated the degradation of phenolic epoxy coating/tinplate system by EIS and the degradation coefficient value, which correlates well with the results of breakpoint frequency and variation of phase angle at 10 Hz. Furthermore, the degradation process was confirmed by scanning electron microscope （SEM） and scanning probe microscopy （SPM）. It is concluded that degradation coefficient can be used for the fast evaluation of degradation degree of organic coatings in practical appli- cations.
基金financial support from the Natural Science Foundation of China (No. 51371034)
文摘The welded joints of 3Cr pipeline steel were fabricated with commercial welding wire using the gas tungsten arc welding （GTAW） technique. Potentiodynamic polarization curves, linear polarization resistance （LPR）, electrochemical impedance spectroscopy （EIS）, scan- ning electron microscopy （SEM）, and energy-dispersive spectrometry （EDS） were used to investigate the corrosion resistance and the growth of a corrosion film on the weld zone （WZ）. The changes in electrochemical characteristics of the film were obtained through fitting of the EIS data. The results showed that the average corrosion rate of the WZ in CO2 environments first increased, then fluctuated, and finally de- creased gradually. The formation of the film on the WZ was divided into three stages： dynamic adsorption, incomplete-coverage layer forma- tion, and integral layer formation.
文摘Pitting corrosion of 316L stainless steel in NaCl solution was investigated by means of staircase potential electrochemical impedance spectroscopy（SPEIS）.The investigation focused on the transition of stainless steel from the passive state to pitting corrosion.Based on the evolution of electrical parameters of the equivalent electrical circuit,it is suggested that the most probable mechanism of pit creation is the film breaking model.The result demonstrates that staircase potential electrochemical impedance spectroscopy is an effective method for the investigation of pitting corrosion.
基金supported by the National Natural Science Foundation of China(No.20276024)the Guangdong Provincial Laboratory of Green Chemical Technology
文摘The corrosion inhibition for carbon steel in circulating cooling water by modified lignosulphonate has been investigated using electrochemical impedance spectroscopy technique. Results show that the inhibition efficiency of modified lignosulphonate GCL2 is a great improvement on that of lignosulphonate. The maximum inhibition efficiency of GCL2 reaches 99.21% at the concentration of 400mg·L^-1 at 303K. The corrosion inhibition of GCL2 is attributed to forming adsorption film on the metal surface for the electrochemical impedance spectroscopy in GCL2 solution shows more than one time-constant.Moreover,results also indicate that it is more efficient in stirring solution than in still solution for GCL2 because the constant of adsorption in stirring solution is much larger than that in still solution. The adsorption of inhibitor GCL2 follows Langmuir＇s adsorption isotherm.
基金National Natural Science Foundation of China (No. 50871021)
文摘The corrosion behaviors of Fe-Cr alloy under three different pH values solutions with C1- and SO42- were investigated by localized electrochemical impedance spectroscopy （LEIS） measurements and the corrosion products were analyzed by laser Raman spectrometry. The results show that the high corrosion resistance of Fe-Cr Alloy is attributed to a passive film which is formed more easily when the alloy contains a large quantity of Cr element. However, its corrosion resistance varies in the solutions with different pH values, especially in the initial corrosion. The average impedance values in neutral and alkaline solution are much higher than that in acidic solution because the passive film is more likely to dissolve in the acidic condition. Moreover, the destructive effect of C1- and SO42 ions on the passive film is also demonstrated in corrosion process through the change of the impedance value with the steeping time.
基金supported by the Research Funds of the Guangxi Key Laboratory of Information Materials at the School of Material Science and Engineering,China (Grant No. 0710908-07-Z)
文摘BaBiO3-doped BaTiO3 （BB-BT） ceramic, as a candidate for lead-free positive temperature coefficient of resistivity （PTCR） materials with a higher Curie temperature, has been synthesized in air by a conventional sintering technique. The temperature dependence of resistivity shows that the phase transition of the PTC thermistor ceramic occurs at the Curie temperature, Tc = 155℃, which is higher than that of BaTiO3 （≤ 130 ℃）. Analysis of ac impedance data using complex impedance spectroscopy gives the alternate current （AC） resistance of the PTCR ceramic. By additional use of the complex electric modulus formalism to analyse the same data, the inhomogeneous nature of the ceramic may be unveiled. The impedance spectra reveal that the grain resistance of the BB-BT sample is slightly influenced by the increase of temperature, indicating that the increase in overall resistivity is entirely due to a grain-boundary effect. Based on the dependence of the extent to which the peaks of the imaginary part of electric modulus and impedance are matched on frequency, the conduction mechanism is also discussed for a BB-BT ceramic system.
文摘The electrochemical characteristics of 1Cr18Ni9Ti in sulphate-reducing bacteria （SRB） solutions and the biofilm of SRB on the surface of the 1Cr18Ni9Ti electrode were studied by electrochemical, microbiological, and surface analysis methods. Electrochemical impedance spectroscopy （EIS） of 1Cr18Ni9Ti was measured in the solutions with and without SRB at the culture time of 2, 4, 8 d, respectively. The measurement used two test methods, the nonimmersion electrode method and the immersion electrode method. It was found that the polarization resistance （Rp） of 1Cr18Ni9Ti in the solutions without SRB is the greatest for each test method. When using the nonimmersion electrode method, Rp shifts negatively at first and then positively, and the time constant is only one. Although using the immersion electrode method, the Rp shifts positively at first and then negatively, and the time constant also changes when the biofilm forms. The biofilm observed through SEM is with pores. It was demonstrated that SRB has accelerated corrosion action on 1Cr18Ni9Ti. The protection effect of the biofilm on the electrode depends on the compact degree of the film.
文摘A microfabricated electrical impedance spectroscopy (EIS) chip with microelectrodes was developed.The substrate and the electrodes of the chip were made of glass and gold,respectively.The experimental results demonstrated that the EIS-chip could distinguish different solutions (physiological saline,culture medium,living cell suspension etc.) by scanning from 10Hz to 45kHz.A 6-element circuit model was used for fitting the real part and the imaginary part admittance curves of the living cell suspension.An actual circuit was also built and tested to verify the 6-element circuit model proposed.The micro-EIS chip has several advantages including the use of small sample volumes,high resolution and ease of operation.It shows good application prospects in the areas of cellular electrophysioiogy,drug screening and bio-sensors etc.
文摘A sinusoidal voltage wave generator is proposed based on the use of micro-processor digital signals with programmable duty-cycles, with application to real-time Electrical Cell-substrate Impedance Spectroscopy (ECIS) assays in cell cultures. The working principle relies on the time convolution of the programmed microcontroller (μC) digital signals. The expected frequency is easily tuned on the bio-impedance spectroscopy range [100 Hz, 1 MHz] thanks to the μC clock frequency selection. This system has been simulated and tested on the 8 bits μC Arduino<sup>TM </sup>Uno with ATmega328 version. Results obtained prove that only three digital signals are required to fit the general specification in ECIS experiments, below 1% THD accuracy, and show the appropriateness of the system for the real-time monitoring of this type of biological experiments.
基金supported by the Ministry of Education,Science,Research and Sport of the Slovak Republic under project No.313011V334,Innovative Solutions for Propulsion,Power and Safety Components of Transport Vehicles。
文摘Despite great progress in lithium-sulfur(Li-S) batteries, the electrochemical reactions in the cell are not yet fully understood. Electrode processes, complex interfaces and internal resistance may be characterized by electrochemical impedance spectroscopy(EIS). EIS is a non-destructive technique and easy to apply, though there are challenges in ensuring the reproducibility of measurements and the interpretation of impedance data. Here, we present the impedance behavior of a 3.4 Ah Li-S pouch cell characterized by EIS. The impedance changes were analyzed over the entire depth-of-discharge, depth-of-charge,and at various temperatures. Based on the formation of intermediates during(dis)charging, the changes of resistances are observed. Overall, the increase in temperature causes a decrease in electrolyte viscosity,lowering the surface energy which can improve the penetration of the electrolyte into the electrode pores. Moreover, the effect of superimposed AC current during EIS measurement was analyzed, and the results show the dependence of the charge transfer resistance on superimposed AC current which was lower compared to steady-state conditions and consents with theory.
基金Project supported by the Second Stage of Brain Korea 21 ProjectProject(RTI04-01-03) supported by the Regional Technology Innovation Program of the Ministry of Knowledge Economy (MKE),Korea
文摘The complex impedance spectroscopy and surface morphology of Mn1+xFe2-2xTixO4(0≤x≤0.5) system,prepared using a conventional solid state reaction technique,were investigated.The impedance spectroscopy measurements were carried out at room temperature in the frequency range of 42-5 MHz.The electrical processes in the samples were modeled in the form of an equivalent circuit made up of a combination of two parallel RC circuits attributed to grain and grain boundaries.The DC conductivity obtained by extrapolation of AC data using impedance spectroscopy and four-probe method increases at 10% doping of Ti ions.The energy-dispersive X-ray(EDX) pattern confirmed the homogeneous mixing of the Mn,Fe,Ti and O atoms in pure and doped ferrite samples.
