The distribution of relaxation times as basis for generalized time-domain models for Li-ion batteries

Schmidt, Jan Philipp; Berg, Philipp; Schönleber, Michael; Weber, André; Ivers-Tiffée, Ellen

doi:10.1016/j.jpowsour.2012.07.100

Cited by 162 publications

(88 citation statements)

References 37 publications

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“…For both SEIs, the DRT peaks are rather broad. On porous electrodes, such peak broadening is caused by through‐plane distributions, whereas on a flat electrode like HOPG we tentatively assign it laterally inhomogeneous surface layer properties.…”

Section: Resultsmentioning

confidence: 79%

“…This underlines the “step” characteristics of the changes between the two regimes. Figure shows the Nyquist plots and the Distribution of Relaxation Times (DRT) g(f), the latter calculated following the scheme from refs and g(f) is presented only in the regions where both real and imaginary residuals are reasonably small. The DRT plots of all temperatures, DRT residuals and Bode phase plots can be found in the SI.…”

Section: Resultsmentioning

confidence: 99%

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Formation of the Solid Electrolyte Interphase at Constant Potentials: A Model Study on Highly Oriented Pyrolytic Graphite

Antonopoulos

Maglia

Schmidt-Stein

et al. 2018

Batteries & Supercaps

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The solid electrolyte interphase (SEI) on graphite anodes is a key enabler for rechargeable lithium-ion batteries (LIBs). It ensures that only Li + ions and no damaging electrolyte components enter the anode and hinders electrolyte decomposition. Its growth should be confined to the initial SEI formation process and stop once the battery is in operation to avoid capacity/ power loss. In technical LIB cells, the SEI is formed at constant current, with the potential of the graphite anode slowly drifting from higher to lower voltages. SEI formation rate, composition, and structure depend on the potential and on the chemical properties of the anode surface. Here, we characterize SEIs formed at constant potentials on the chemically inactive basal plane of highly oriented pyrolytic graphite (HOPG). X-ray photoemission spectroscopy (XPS) detects carbonate species only at lower formation potentials. Cyclic voltammetry (CV) and Electrochemical Impedance Spectroscopy (EIS) with Fc/Fc + as an electrochemical probe demonstrate how the formation potential influences ion transport and electrochemical kinetics to and at the anode surface, respectively. Breaking the EIS data down to a Distribution of Relaxation Times (DRT) reveals distinct kinetics and transport related peaks with varying Arrhenius-type temperature dependencies. We discuss our findings in the context of previous electrochemical studies and existing SEI models and of SEI formation protocols suitable for industry.

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Section: Resultsmentioning

confidence: 79%

Section: Resultsmentioning

confidence: 99%

Formation of the Solid Electrolyte Interphase at Constant Potentials: A Model Study on Highly Oriented Pyrolytic Graphite

Antonopoulos

Maglia

Schmidt-Stein

et al. 2018

Batteries & Supercaps

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“…[9,10] Using this method, the high-intensity characteristic frequencieso fameasured impedance spectrum are determined to derive the number of RCelements.Asimplified version to determine the equivalent circuit configuration is curve sketching to identify the minima, maxima, and inflection points in the Nyquistp lot. [11] Thef requencieso ft he distinctive points are also called process frequenciesa st hey show in which frequency range of This work is an overviewo fv arious equivalent circuits (ECs) containingv ariousd egrees of detail.…”

Section: Introductionmentioning

confidence: 99%

Analysis of Lithium‐Ion Battery Models Based on Electrochemical Impedance Spectroscopy

et al. 2016

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This work is an overview of various equivalent circuits (ECs) containing various degrees of detail. The ECs are evaluated in terms of model accuracy and parameterization time for the systematic assignment of an equivalent circuit to application fields. For this purpose, impedance spectra were measured using electrochemical impedance spectroscopy at different states of charge, health and temperatures. Then the parameters of the EC were extracted using the least‐squares method and the Levenberg–Marquardt algorithm. After comparing the simulated to the measured impedance spectrum, a review and assignment of equivalent circuits for potential applications is given. Simple equivalent circuits with a series resistor and a maximum of two resistance–capacitance (RC) elements are ideal for simulations with lower dynamics. Equivalent circuits with up to five RC elements or even a constant‐phase element (CPE) are promising for simulating highly dynamic processes. By using RCPE elements the impedance spectrum can be modeled with the highest accuracy, which is why this type of model should be used for diagnostic purposes.

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“…The fact that the Nyquist plots in fig.2 and 3 show depressed semi-circles in the high to medium frequency domain suggested that the inclusion of CPE's in the modified Randles circuit would be appropriate, and this differentiates our model from the DP approach; our model may be considered as one consisting of multiple time constants [31] as opposed to only two. A process of iteration using these elements at the anode and cathode resulted in the proposed model assuming a finite length diffusion component (W a and W c ) at both electrodes.…”

Section: Resultsmentioning

confidence: 99%

A study of 40 Ah lithium ion batteries at zero percent state of charge as a function of temperature

Attidekou

Lambert

Armstrong

et al. 2014

Journal of Power Sources

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A theoretical equivalent circuit model of two 40Ah commercial batteries supplied by Saft was formulated to interpret electrochemical impedance spectra as a function of temperature at zero state-of-charge. The batteries were chosen to represent viable and non-viable products from the Saft production line. This paper is the first contribution from a project in Newcastle to develop a rapid, non-destructive analytical method for quality control on the battery production line. Using the model, it proved straightforward to discriminate between viable and non-viable batteries based on the temperature dependence of the electrochemical reaction kinetics at the electrodes, the average diffusion coefficients and the charge transfer resistances. Furthermore, as well as marked differences, for example, between the time constants, activation energies, polarisation resistances of the viable and non-viable batteries, the individual contributions of the anodes and cathodes in the batteries were de-convoluted and interpreted through the model framework.5

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The distribution of relaxation times as basis for generalized time-domain models for Li-ion batteries

Cited by 162 publications

References 37 publications

Formation of the Solid Electrolyte Interphase at Constant Potentials: A Model Study on Highly Oriented Pyrolytic Graphite

Formation of the Solid Electrolyte Interphase at Constant Potentials: A Model Study on Highly Oriented Pyrolytic Graphite

Analysis of Lithium‐Ion Battery Models Based on Electrochemical Impedance Spectroscopy

A study of 40 Ah lithium ion batteries at zero percent state of charge as a function of temperature

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