Abstract

The kinetics of electrochemical intercalation and electrosorption processes are often limited by the solid-state diffusion of ions inside the lattice of the host material. While some of these limitations can be mitigated by nanostructuring of the electrode material, there is a large interest in the electrochemical energy storage community to find materials with structural motifs that allow for intrinsically fast ion diffusion, even in bulk-sized particles.In this presentation, it will be highlighted how interlayer properties, such as interlayer distance and interlayer chemistry, affect electrochemical ion intercalation and electrosorption processes in layered host materials. Using the examples of hydrogen titanates1 and Ti3C2Tx MXenes2, it is demonstrated that the presence of structural interlayer atoms or molecules can increase the accessibility of ions to the interlayer space. In the model layered host material TiS2, it is shown that increased interlayer spacing and reduced deformation during ion intercalation can lead to a change from diffusion-limited to non-diffusion limited (or pseudocapacitive) charge storage behavior,3 providing some of the most compelling experimental evidence of the intimate relationship between deformation, interlayer distance, and intercalation kinetics in layered host materials.This contribution will emphasize the importance of interlayer properties of layered and 2D materials for electrochemical ion intercalation and electrosorption processes and provide perspectives and design strategies for next generation ion insertion hosts with fast kinetics for high power energy storage. Fleischmann, S. et al. Interlayer separation in hydrogen titanates enables electrochemical proton intercalation. J. Mater. Chem. A 8, 412–421 (2020).Liang, K. et al. Engineering the Interlayer Spacing by Pre-Intercalation for High Performance Supercapacitor MXene Electrodes in Room Temperature Ionic Liquid. Adv. Funct. Mater. 31, 2104007 (2021).Fleischmann, S., Shao, H., Taberna, P.-L., Rozier, P. & Simon, P. Electrochemically Induced Deformation Determines the Rate of Lithium Intercalation in Bulk TiS2. ACS Energy Lett. 6, 4173–4178 (2021).

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