Multimodal Operando Analysis of High-Capacity Electrodes with Neutrons and Photons
Authors: Risse Sebastian 
Published: December 2024

High-capacity electrodes like sulfur cathodes and silicon anodes are promising candidates for sustainable electrochemical energy storage in a post-lithium-ion era. While Lithium/sulfur (Li/S) batteries have a fivefold higher theoretical gravimetric energy density (ca. 2500 Wh/kg) than state-of-the-art lithium-ion batteries [1], silicon is an interesting anode material for lithium-ion batteries due to its ten times higher specific capacity than commercially used graphite anodes. However, despite decades of research, the strong capacity fading with increasing cycle numbers is still a significant obstacle to the broad technical utilization of both electrodes. Operando techniques [2] are very suitable tools for gaining a mechanistic understanding of degradation processes. Especially the simultaneous combination of several independent measurements (multimodal) while the electrodes are in operation allows deep insights into the degradation mechanisms and provides a further mechanistic understanding of both complex chemistries. Here, the results of novel setups are presented where several independent measurements are simultaneously performed. Electrochemical impedance spectroscopy (EIS) [3], temperature measurement, soft X-ray spectroscopy [4], and X-ray imaging [5-11] or neutron techniques like small-angle neutron scattering [12] and neutron reflectometry [13-16] were performed over several cycles. At the same time, the cell was galvanostatically or potentiostatically charged and discharged. Structural changes on the macroscopic and microscopic scale can be correlated to characteristic signals in the EIS and charge-discharge curves. Also, the advantages of molecular dynamics simulations for elucidating structures and processes in liquid electrolytes will be discussed [17-19].

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