All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid...All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.展开更多
High-voltage pulse discharge(HVPD)rock fragmentation controls a plasma channel forming inside the rock by adjusting the electrical parameters,electrode type,etc.In this work,an HVPD rock fragmentation test platform wa...High-voltage pulse discharge(HVPD)rock fragmentation controls a plasma channel forming inside the rock by adjusting the electrical parameters,electrode type,etc.In this work,an HVPD rock fragmentation test platform was built and the test waveforms were measured.Considering the effects of temperature,channel expansion and electromagnetic radiation,the impedance model of the plasma channel in the rock was established.The parameters and initial values of the model were determined by an iterative computational process.The model calculation results can reasonably characterize the development of the plasma channel in the rock and estimate the shock wave characteristics.Based on the plasma channel impedance model,the temporal and spatial distribution characteristics of the radial stress and tangential stress in the rock were calculated,and the rock fragmentation effect of the HVPD was analyzed.展开更多
Seismic impedance inversion is an important technique for structure identification and reservoir prediction.Model-based and data-driven impedance inversion are the commonly used inversion methods.In practice,the geoph...Seismic impedance inversion is an important technique for structure identification and reservoir prediction.Model-based and data-driven impedance inversion are the commonly used inversion methods.In practice,the geophysical inversion problem is essentially an ill-posedness problem,which means that there are many solutions corresponding to the same seismic data.Therefore,regularization schemes,which can provide stable and unique inversion results to some extent,have been introduced into the objective function as constrain terms.Among them,given a low-frequency initial impedance model is the most commonly used regularization method,which can provide a smooth and stable solution.However,this model-based inversion method relies heavily on the initial model and the inversion result is band limited to the effective frequency bandwidth of seismic data,which cannot effectively improve the seismic vertical resolution and is difficult to be applied to complex structural regions.Therefore,we propose a data-driven approach for high-resolution impedance inversion based on the bidirectional long short-term memory recurrent neural network,which regards seismic data as time-series rather than image-like patches.Compared with the model-based inversion method,the data-driven approach provides higher resolution inversion results,which demonstrates the effectiveness of the data-driven method for recovering the high-frequency components.However,judging from the inversion results for characterization the spatial distribution of thin-layer sands,the accuracy of high-frequency components is difficult to guarantee.Therefore,we add the model constraint to the objective function to overcome the shortages of relying only on the data-driven schemes.First,constructing the supervisor1 based on the bidirectional long short-term memory recurrent neural network,which provides the predicted impedance with higher resolution.Then,convolution constraint as supervisor2 is introduced into the objective function to guarantee the reliability and accuracy of the inversion results,which makes the synthetic seismic data obtained from the inversion result consistent with the input data.Finally,we test the proposed scheme based on the synthetic and field seismic data.Compared to model-based and purely data-driven impedance inversion methods,the proposed approach provides more accurate and reliable inversion results while with higher vertical resolution and better spatial continuity.The inversion results accurately characterize the spatial distribution relationship of thin sands.The model tests demonstrate that the model-constrained and data-driven impedance inversion scheme can effectively improve the thin-layer structure characterization based on the seismic data.Moreover,tests on the oil field data indicate the practicality and adaptability of the proposed method.展开更多
In the electrochemical conversion of carbon dioxide, high currents need to be employed to obtain large production rates, thus implying that mass transport of reactants and products is of crucial importance.This aspect...In the electrochemical conversion of carbon dioxide, high currents need to be employed to obtain large production rates, thus implying that mass transport of reactants and products is of crucial importance.This aspect can be investigated by employing a model that depicts the local environment for the reduction reactions. Simultaneously, electrochemical impedance spectroscopy, despite being a versatile technique, has rarely been adopted for studying the mass transport features during the carbon dioxide(CO_(2))electroreduction. In this work, this aspect is deeply analyzed by correlating the results of impedance spectroscopy characterization with those obtained by a bubble-induced mass transport modeling under controlled diffusion conditions on a gold rotating disk electrode. The effects of potential and rotation rate on the local environment are also clarified. In particular, it has been found that CO_(2) depletion occurs at high kinetics when the rotation is absent, giving rise to an increment of the competing hydrogen evolution reaction. This feature reflects in an enlargement of the diffusion resistance, which overcomes the charge transport one.展开更多
Electrochemical impedance spectroscopy(EIS)is a robust characterization method to probe prevalent(electro)chemical processes in an electrochemical system.Despite its extensive utilization in fuel cell research,the app...Electrochemical impedance spectroscopy(EIS)is a robust characterization method to probe prevalent(electro)chemical processes in an electrochemical system.Despite its extensive utilization in fuel cell research,the application of EIS in redox flow battery systems particularly for simplified two-electrode full-cell configurations is more limited.Herein we attempt to strengthen the understa nding of cha racteristic EIS data of vanadium redox flow batteries by a combination of equivalent circuit modeling with a validated Multiphysics model analyzed under hydrodynamic conditions in frequency domain.Following a highlight of system linearity and stability concerns for EIS in redox flow batteries,we specifically use our combinatory approach to investigate the effects of different cell component properties on observed galva nostatic EIS spectra and accompanying fitted equivalent circuit element parameters.For the investigated two-electrode full-cell flow battery configuration with the same electrode material on both sides,the EIS spectral data is observed to be dominated by different mass or cha rge transport processes at different ends of the spectrum.Sensitivity analyses of both obtained EIS spectral data and fitted circuit elements parameters show that electrode morphological properties,membrane porosity,and electrolyte inflow conditions predominantly define the EIS spectral data.Insights from the type of analyses performed herein can facilitate flow battery cell/stack diagnostics and targeted performance improvement efforts.展开更多
Mixed ionic electronic conductors(MIECs)have attracted increasing attention as anode materials for solid oxide fuel cells(SOFCs)and they hold great promise for lowering the operation temperature of SOFCs.However,there...Mixed ionic electronic conductors(MIECs)have attracted increasing attention as anode materials for solid oxide fuel cells(SOFCs)and they hold great promise for lowering the operation temperature of SOFCs.However,there has been a lack of understanding of the performance-limiting factors and guidelines for rational design of composite metal-MIEC electrodes.Using a newly-developed approach based on 3 D-tomography and electrochemical impedance spectroscopy,here for the first time we quantify the contribution of the dual-phase boundary(DPB)relative to the three-phase boundary(TPB)reaction pathway on real MIEC electrodes.A new design strategy is developed for Ni/gadolinium doped ceria(CGO)electrodes(a typical MIEC electrode)based on the quantitative analyses and a novel Ni/CGO fiber-matrix structure is proposed and fabricated by combining electrospinning and tape-casting methods using commercial powders.With only 11.5 vol%nickel,the designer Ni/CGO fiber-matrix electrode shows 32%and 67%lower polarization resistance than a nano-Ni impregnated CGO scaffold electrode and conventional cermet electrode respectively.The results in this paper demonstrate quantitatively using real electrode structures that enhancing DPB and hydrogen kinetics are more efficient strategies to enhance electrode performance than simply increasing TPB.展开更多
The dielectric properties of nucleated erythrocytes from bullfrogs were measured in a frequency range of 10 kHz–110 MHz.The complex permittivity(ε*),complex conductivity(κ*),and complex resistivity(ρ*)were analyze...The dielectric properties of nucleated erythrocytes from bullfrogs were measured in a frequency range of 10 kHz–110 MHz.The complex permittivity(ε*),complex conductivity(κ*),and complex resistivity(ρ*)were analyzed and compared in the 10.63%to 37.58%haematocrit(Hct)range.The relaxation behavior,the passive electrical properties,and the cellular structure parameters,including the cell membrane,the cytoplasm,the nuclear membrane,and the nucleoplasm of the nucleated erythrocyte suspensions were investigated.The method used is based on the binomial Cole–Cole equation and the double spherical-shell physical models.Upon the elimination of the electrode polarization effect,two definite relaxations related to the interfacial polarization are observed on low-and high-frequency dispersions.The permittivity values and the characteristic frequency values differ by one order of magnitude:the low-frequency relaxation increments[?ε1=(5.63±1.43)×103]and the characteristic frequency[fc1=(297.06±14.48)kHz]derived from the cell membrane,the high-frequency relaxation increments[?ε2=(5.21±1.20)×102]and the characteristic frequency[fc2=(3.73±0.06)MHz]derived from the dielectric response to the external electric field of the nuclear membrane,respectively.Moreover,the other core dielectric parameters,such as the relative permittivity of the cell membrane[εm=(7.57±0.38)]and the nuclear envelope[εne=(23.59±4.39)],the conductivity of the cytoplasm(hemoglobin,κHb=(0.50±0.13)S/m]and the nuclear endoplasm[κnp=(2.56±0.75)S/m],and the capacitance of the bilayer membranes[Cm:(0.84±0.04)μF/cm2],and Cne:(0.52±0.10)μF/cm2]were also accurately and reliably measured.This work presents a feasible method to evaluate the dielectric parameters and the cellular structure of the erythrocytes of bullfrogs.Moreover,it paves the way for new studies on the haematology of frogs and the detection of nucleated cells via dielectric impedance spectroscopy.展开更多
基金supported by the Beijing Natural Science Foundation(Z200011,L233004)the National Key Research and Development Program(2021YFB2500300)+3 种基金the National Natural Science Foundation of China(52394170,52394171,22109011,22393900,and 22108151)the Tsinghua-Jiangyin Innovation Special Fund(TJISF)(2022JYTH0101)the S&T Program of Hebei(22344402D)the Tsinghua University Initiative Scientific Research Program.
文摘All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.
基金support of National Natural Science Foundation of China(No.52177144)。
文摘High-voltage pulse discharge(HVPD)rock fragmentation controls a plasma channel forming inside the rock by adjusting the electrical parameters,electrode type,etc.In this work,an HVPD rock fragmentation test platform was built and the test waveforms were measured.Considering the effects of temperature,channel expansion and electromagnetic radiation,the impedance model of the plasma channel in the rock was established.The parameters and initial values of the model were determined by an iterative computational process.The model calculation results can reasonably characterize the development of the plasma channel in the rock and estimate the shock wave characteristics.Based on the plasma channel impedance model,the temporal and spatial distribution characteristics of the radial stress and tangential stress in the rock were calculated,and the rock fragmentation effect of the HVPD was analyzed.
基金funded by R&D Department of China National Petroleum Corporation(2022DQ0604-04)the Strategic Cooperation Technology Projects of CNPC and CUPB(ZLZX2020-03)the Science Research and Technology Development of PetroChina(2021DJ1206).
文摘Seismic impedance inversion is an important technique for structure identification and reservoir prediction.Model-based and data-driven impedance inversion are the commonly used inversion methods.In practice,the geophysical inversion problem is essentially an ill-posedness problem,which means that there are many solutions corresponding to the same seismic data.Therefore,regularization schemes,which can provide stable and unique inversion results to some extent,have been introduced into the objective function as constrain terms.Among them,given a low-frequency initial impedance model is the most commonly used regularization method,which can provide a smooth and stable solution.However,this model-based inversion method relies heavily on the initial model and the inversion result is band limited to the effective frequency bandwidth of seismic data,which cannot effectively improve the seismic vertical resolution and is difficult to be applied to complex structural regions.Therefore,we propose a data-driven approach for high-resolution impedance inversion based on the bidirectional long short-term memory recurrent neural network,which regards seismic data as time-series rather than image-like patches.Compared with the model-based inversion method,the data-driven approach provides higher resolution inversion results,which demonstrates the effectiveness of the data-driven method for recovering the high-frequency components.However,judging from the inversion results for characterization the spatial distribution of thin-layer sands,the accuracy of high-frequency components is difficult to guarantee.Therefore,we add the model constraint to the objective function to overcome the shortages of relying only on the data-driven schemes.First,constructing the supervisor1 based on the bidirectional long short-term memory recurrent neural network,which provides the predicted impedance with higher resolution.Then,convolution constraint as supervisor2 is introduced into the objective function to guarantee the reliability and accuracy of the inversion results,which makes the synthetic seismic data obtained from the inversion result consistent with the input data.Finally,we test the proposed scheme based on the synthetic and field seismic data.Compared to model-based and purely data-driven impedance inversion methods,the proposed approach provides more accurate and reliable inversion results while with higher vertical resolution and better spatial continuity.The inversion results accurately characterize the spatial distribution relationship of thin sands.The model tests demonstrate that the model-constrained and data-driven impedance inversion scheme can effectively improve the thin-layer structure characterization based on the seismic data.Moreover,tests on the oil field data indicate the practicality and adaptability of the proposed method.
文摘In the electrochemical conversion of carbon dioxide, high currents need to be employed to obtain large production rates, thus implying that mass transport of reactants and products is of crucial importance.This aspect can be investigated by employing a model that depicts the local environment for the reduction reactions. Simultaneously, electrochemical impedance spectroscopy, despite being a versatile technique, has rarely been adopted for studying the mass transport features during the carbon dioxide(CO_(2))electroreduction. In this work, this aspect is deeply analyzed by correlating the results of impedance spectroscopy characterization with those obtained by a bubble-induced mass transport modeling under controlled diffusion conditions on a gold rotating disk electrode. The effects of potential and rotation rate on the local environment are also clarified. In particular, it has been found that CO_(2) depletion occurs at high kinetics when the rotation is absent, giving rise to an increment of the competing hydrogen evolution reaction. This feature reflects in an enlargement of the diffusion resistance, which overcomes the charge transport one.
基金sponsored by the Dubai Electricity and Water Authority(DEWA)R&D centre,Dubai,United Arab Emirates。
文摘Electrochemical impedance spectroscopy(EIS)is a robust characterization method to probe prevalent(electro)chemical processes in an electrochemical system.Despite its extensive utilization in fuel cell research,the application of EIS in redox flow battery systems particularly for simplified two-electrode full-cell configurations is more limited.Herein we attempt to strengthen the understa nding of cha racteristic EIS data of vanadium redox flow batteries by a combination of equivalent circuit modeling with a validated Multiphysics model analyzed under hydrodynamic conditions in frequency domain.Following a highlight of system linearity and stability concerns for EIS in redox flow batteries,we specifically use our combinatory approach to investigate the effects of different cell component properties on observed galva nostatic EIS spectra and accompanying fitted equivalent circuit element parameters.For the investigated two-electrode full-cell flow battery configuration with the same electrode material on both sides,the EIS spectral data is observed to be dominated by different mass or cha rge transport processes at different ends of the spectrum.Sensitivity analyses of both obtained EIS spectral data and fitted circuit elements parameters show that electrode morphological properties,membrane porosity,and electrolyte inflow conditions predominantly define the EIS spectral data.Insights from the type of analyses performed herein can facilitate flow battery cell/stack diagnostics and targeted performance improvement efforts.
基金the financial support from EPSRC(EP/P024807/1,EP/M014045/1,EP/S000933/1 and EP/N009924/1)by the EPSRC energy storage for low carbon grids project(EP/K002252/1)+3 种基金the EPSRC Joint UK-India Clean Energy center(JUICE)(EP/P003605/1)the Integrated Development of Low-Carbon Energy Systems(IDLES)project(EP/R045518/1)the Innovate UK BAFTA project,the Innovate UK for Advanced Battery Lifetime Extension(ABLE)project for funding underthe China Scholarship Council。
文摘Mixed ionic electronic conductors(MIECs)have attracted increasing attention as anode materials for solid oxide fuel cells(SOFCs)and they hold great promise for lowering the operation temperature of SOFCs.However,there has been a lack of understanding of the performance-limiting factors and guidelines for rational design of composite metal-MIEC electrodes.Using a newly-developed approach based on 3 D-tomography and electrochemical impedance spectroscopy,here for the first time we quantify the contribution of the dual-phase boundary(DPB)relative to the three-phase boundary(TPB)reaction pathway on real MIEC electrodes.A new design strategy is developed for Ni/gadolinium doped ceria(CGO)electrodes(a typical MIEC electrode)based on the quantitative analyses and a novel Ni/CGO fiber-matrix structure is proposed and fabricated by combining electrospinning and tape-casting methods using commercial powders.With only 11.5 vol%nickel,the designer Ni/CGO fiber-matrix electrode shows 32%and 67%lower polarization resistance than a nano-Ni impregnated CGO scaffold electrode and conventional cermet electrode respectively.The results in this paper demonstrate quantitatively using real electrode structures that enhancing DPB and hydrogen kinetics are more efficient strategies to enhance electrode performance than simply increasing TPB.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.51277099 and 52007087)the Natural Science Foundation of Zhejiang Province,China(Grant Nos.LY20C110001 and LSY19A010002)+2 种基金the Natural Science Foundation of Ningbo City,China(Grant Nos.2019A610349 and 202003N4116)the Fund from the Educational Commission of Zhejiang Province,China(Grant No.Y202044047)the Fundamental Research Funds for the Provincial Universities of Zhejiang Province,China.
文摘The dielectric properties of nucleated erythrocytes from bullfrogs were measured in a frequency range of 10 kHz–110 MHz.The complex permittivity(ε*),complex conductivity(κ*),and complex resistivity(ρ*)were analyzed and compared in the 10.63%to 37.58%haematocrit(Hct)range.The relaxation behavior,the passive electrical properties,and the cellular structure parameters,including the cell membrane,the cytoplasm,the nuclear membrane,and the nucleoplasm of the nucleated erythrocyte suspensions were investigated.The method used is based on the binomial Cole–Cole equation and the double spherical-shell physical models.Upon the elimination of the electrode polarization effect,two definite relaxations related to the interfacial polarization are observed on low-and high-frequency dispersions.The permittivity values and the characteristic frequency values differ by one order of magnitude:the low-frequency relaxation increments[?ε1=(5.63±1.43)×103]and the characteristic frequency[fc1=(297.06±14.48)kHz]derived from the cell membrane,the high-frequency relaxation increments[?ε2=(5.21±1.20)×102]and the characteristic frequency[fc2=(3.73±0.06)MHz]derived from the dielectric response to the external electric field of the nuclear membrane,respectively.Moreover,the other core dielectric parameters,such as the relative permittivity of the cell membrane[εm=(7.57±0.38)]and the nuclear envelope[εne=(23.59±4.39)],the conductivity of the cytoplasm(hemoglobin,κHb=(0.50±0.13)S/m]and the nuclear endoplasm[κnp=(2.56±0.75)S/m],and the capacitance of the bilayer membranes[Cm:(0.84±0.04)μF/cm2],and Cne:(0.52±0.10)μF/cm2]were also accurately and reliably measured.This work presents a feasible method to evaluate the dielectric parameters and the cellular structure of the erythrocytes of bullfrogs.Moreover,it paves the way for new studies on the haematology of frogs and the detection of nucleated cells via dielectric impedance spectroscopy.
