Elucidation of Mass Transport Phenomena in Highly Concentrated Electrolytes during Current Cycling Using In-Situ Interferometry and Finite Difference Method

Go Kamesui; Kei Nishikawa; Mikito Ueda; Hisayoshi Matsushima

doi:10.1149/1945-7111/ad3ad1

Article Elucidation of Mass Transport Phenomena in Highly Concentrated Electrolytes during Current Cycling Using In-Situ Interferometry and Finite Difference Method

Go Kamesui ; Kei Nishikawa (National Institute for Materials Science) ; Mikito Ueda ; Hisayoshi Matsushima

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Go Kamesui, Kei Nishikawa, Mikito Ueda, Hisayoshi Matsushima. Elucidation of Mass Transport Phenomena in Highly Concentrated Electrolytes during Current Cycling Using In-Situ Interferometry and Finite Difference Method. Journal of The Electrochemical Society. 2024, 171 (4), 040519. https://doi.org/10.1149/1945-7111/ad3ad1

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Understanding electrolyte mass transfer during charge–discharge reactions is essential for developing next-generation storage batteries with high energy densities. In this study, we investigated Li+ transport in a highly concentrated electrolyte (HCE) consisting of an equimolar mixture of lithium bis(fluorosulfonyl)amide (LiFSA) and tetraglyme (G4) under current reversal and re-reversal. Concentration profiles of the electrolyte at a distance of 0–600 μm from the Li electrodes were obtained using in situ laser interferometry. The Li+ transference numbers and LiFSA diffusion coefficients were calculated from these profiles. Raman spectroscopy suggested that the coordination structure surrounding Li+ ions in the electrolytes mainly contributed to the transference number. A one-dimensional unsteady diffusion equation and the finite difference method were employed to simulate the concentration profiles. The maximum error percentage between the measured and simulated values was only 3%, confirming the accuracy and validity of the interferometric measurements. Our findings on Li-ion transfer in HCEs could promote the rational design of high-energy-density Li-ion batteries with higher cation transference numbers of electrolytes and charge–discharge rates.

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This is the Accepted Manuscript version of an article accepted for publication in Journal of The Electrochemical Society. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://dx.doi.org/10.1149/1945-7111/ad3ad1.