Simulation-Supported Analysis of Calendering Impacts on the Performance of Lithium-Ion-Batteries. Lenze, G., Röder, F., Bockholt, H., Haselrieder, W., Kwade, A., & Krewer, U. Journal of The Electrochemical Society, 164(6):A1223–A1233, 2017.
Simulation-Supported Analysis of Calendering Impacts on the Performance of Lithium-Ion-Batteries [link]Paper  doi  abstract   bibtex   
A combination of experimental and model based analysis was performed to investigate calendering impacts on the performance of lithium-ion-batteries. When discharging, not only geometric parameters, such as electrode thicknesses and porosities are affecting performance. Calendering also impacts on other parameters, such as the effective ionic conductivity within the electrolyte, the effective electronic conductivity of solid active material and the effective solid-liquid interfacial area. The simulation supported method is shown to complement experimental analysis to understand correlations between calendering and these parameters; it enables to identify cell internal parameters which are hard to measure and to analyze how the lithium transport is affected. In experiments, cells containing non-calendered cathodes performed significantly worse than ones with 22%-calendered cathodes. Simulation indicated that this losses consist mainly of a deterioration of effective electronic conductivity leading to overpotentials close to the separator. Minor contributions to the losses in non-calendered cathodes caused by the geometric compaction and a reduction of effective solid-liquid interfacial area were found as well, whereas the impact of effective ionic conductivity turned out to be only insignificantly small. Calendering of electrodes is an important step within the manu-facturing process of lithium-ion-batteries as it affects energy density significantly. 1 An increase in energy density is crucial to achieve larger driving ranges for electric vehicles and thus to make them compet-itive on the market. Aim of this work is to establish an advanced model based method for the analysis of calendering impacts which gives additional insights into cell internal electrochemical correla-tions. Most studies about calendering impacts on battery electrodes are of experimental nature. 1–3 These investigations present mechanical and electrochemical characterization results of industrially produced and readily usable electrode samples. Usually mercury (Hg) porosime-try, scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), C-Rate, and cycling tests are performed. These methods are helpful to understand how calendering affects the ge-ometric and mechanical properties of particle-pore networks within electrodes. However, evaluation of correlations between structural changes and battery performance is rather phenomenological and empirical so that knowledge gained is limited. EIS measurements are commonly used for correlation between structural changes and performance determining physico-chemical processes and constants, such as electronic conductivity within the electrode; 4,5 to investigate calendering impacts on the aging behavior cycling experiments have been used 6 . However, it is still difficult to understand calendering im-pacts on performance entirely, as calendering affects several parame-ters simultaneously, making evaluations complex. Additional tools for analysis can improve this understanding and enable knowledge-driven optimization of manufacturing parameters. Physico-chemical battery models enable to simulate battery performance as a function of struc-tural parameters, such as electrode thickness and porosity, 7 as well as of parameters like solid-liquid interfacial area, electronic and ionic conductivities, which may be affected by calendering as well. 8 Fur-thermore, not only the resulting battery performance but underlying processes like lithium (Li) transport within electrolyte, electrodes and active material particles can be studied. 9 These features make simu-lation a promising complementary tool to experimental investigations for understanding calendering impacts in Li-ion-batteries and the re-lated structure-performance correlations. We see simulation therefore as essential to achieve an optimized battery production. Approaches of simulating structure-performance correlations in lithium-ion-batteries can be found in literature; they are rather theoretical, as they primarily
@article{lenze_simulation-supported_2017,
	title = {Simulation-{Supported} {Analysis} of {Calendering} {Impacts} on the {Performance} of {Lithium}-{Ion}-{Batteries}},
	volume = {164},
	copyright = {All rights reserved},
	issn = {0013-4651},
	url = {http://jes.ecsdl.org/lookup/doi/10.1149/2.1141706jes},
	doi = {10.1149/2.1141706jes},
	abstract = {A combination of experimental and model based analysis was performed to investigate calendering impacts on the performance of lithium-ion-batteries. When discharging, not only geometric parameters, such as electrode thicknesses and porosities are affecting performance. Calendering also impacts on other parameters, such as the effective ionic conductivity within the electrolyte, the effective electronic conductivity of solid active material and the effective solid-liquid interfacial area. The simulation supported method is shown to complement experimental analysis to understand correlations between calendering and these parameters; it enables to identify cell internal parameters which are hard to measure and to analyze how the lithium transport is affected. In experiments, cells containing non-calendered cathodes performed significantly worse than ones with 22\%-calendered cathodes. Simulation indicated that this losses consist mainly of a deterioration of effective electronic conductivity leading to overpotentials close to the separator. Minor contributions to the losses in non-calendered cathodes caused by the geometric compaction and a reduction of effective solid-liquid interfacial area were found as well, whereas the impact of effective ionic conductivity turned out to be only insignificantly small. Calendering of electrodes is an important step within the manu-facturing process of lithium-ion-batteries as it affects energy density significantly. 1 An increase in energy density is crucial to achieve larger driving ranges for electric vehicles and thus to make them compet-itive on the market. Aim of this work is to establish an advanced model based method for the analysis of calendering impacts which gives additional insights into cell internal electrochemical correla-tions. Most studies about calendering impacts on battery electrodes are of experimental nature. 1–3 These investigations present mechanical and electrochemical characterization results of industrially produced and readily usable electrode samples. Usually mercury (Hg) porosime-try, scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), C-Rate, and cycling tests are performed. These methods are helpful to understand how calendering affects the ge-ometric and mechanical properties of particle-pore networks within electrodes. However, evaluation of correlations between structural changes and battery performance is rather phenomenological and empirical so that knowledge gained is limited. EIS measurements are commonly used for correlation between structural changes and performance determining physico-chemical processes and constants, such as electronic conductivity within the electrode; 4,5 to investigate calendering impacts on the aging behavior cycling experiments have been used 6 . However, it is still difficult to understand calendering im-pacts on performance entirely, as calendering affects several parame-ters simultaneously, making evaluations complex. Additional tools for analysis can improve this understanding and enable knowledge-driven optimization of manufacturing parameters. Physico-chemical battery models enable to simulate battery performance as a function of struc-tural parameters, such as electrode thickness and porosity, 7 as well as of parameters like solid-liquid interfacial area, electronic and ionic conductivities, which may be affected by calendering as well. 8 Fur-thermore, not only the resulting battery performance but underlying processes like lithium (Li) transport within electrolyte, electrodes and active material particles can be studied. 9 These features make simu-lation a promising complementary tool to experimental investigations for understanding calendering impacts in Li-ion-batteries and the re-lated structure-performance correlations. We see simulation therefore as essential to achieve an optimized battery production. Approaches of simulating structure-performance correlations in lithium-ion-batteries can be found in literature; they are rather theoretical, as they primarily},
	number = {6},
	journal = {Journal of The Electrochemical Society},
	author = {Lenze, Georg and Röder, Fridolin and Bockholt, Henrike and Haselrieder, Wolfgang and Kwade, Arno and Krewer, Ulrike},
	year = {2017},
	pages = {A1223--A1233},
}
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