Operando imaging of intercalation memory in MXenes
Abstract
Ion intercalation enables reversible control of charge, structure and function in layered solids. Yet layered materials contain nanosheets with different thicknesses and stacking, whose intercalation pathways are averaged out in ensemble measurements. This becomes critical under Angstrom-scale confinement, where ion transport couples to solvent reorganization and host deformation, leaving the origins of kinetics, reversibility and activation unresolved. Here we combine operando interferometric scattering and interference reflection microscopy to resolve proton-driven dynamics in individual single- and multilayer Ti3C2Tx MXene flakes and show that even a few stacked layers introduce a significant kinetic barrier. Cycling then separates nanosheets into three persistent behaviors: reversible monolayers, restacked multilayers with incomplete recovery and delayed deintercalation, and coherently stacked multilayers that self-stabilize through reversible folding. Operando synchrotron X-ray diffraction shows this memory at electrode scale, where the interlayer structure converges towards a reproducible state. Our findings reveal cycling-induced structural memory that governs subsequent intercalation in layered MXenes.
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BibTeX
@misc{groebmeyer2026operando,
title = {{Operando imaging of intercalation memory in MXenes}},
author = {Franz Groebmeyer and Mohsen Beladi and Christoph G. Gruber and Ruocun Wang and Pol Salles and Nhu Quynh Nguyen and Jakub Drnec and Yury Gogotsi and Emiliano Cortes},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.04977},
eprint = {2609.04977},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.04977},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Operando imaging of intercalation memory in MXenes
AU - Franz Groebmeyer
AU - Mohsen Beladi
AU - Christoph G. Gruber
AU - Ruocun Wang
AU - Pol Salles
AU - Nhu Quynh Nguyen
AU - Jakub Drnec
AU - Yury Gogotsi
AU - Emiliano Cortes
PY - 2026
DA - 2026/09/04
PB - arXiv
DO - 10.48550/arxiv.2609.04977
UR - https://arxiv.org/abs/2609.04977
AB - Ion intercalation enables reversible control of charge, structure and function in layered solids. Yet layered materials contain nanosheets with different thicknesses and stacking, whose intercalation pathways are averaged out in ensemble measurements. This becomes critical under Angstrom-scale confinement, where ion transport couples to solvent reorganization and host deformation, leaving the origins of kinetics, reversibility and activation unresolved. Here we combine operando interferometric scattering and interference reflection microscopy to resolve proton-driven dynamics in individual single- and multilayer Ti3C2Tx MXene flakes and show that even a few stacked layers introduce a significant kinetic barrier. Cycling then separates nanosheets into three persistent behaviors: reversible monolayers, restacked multilayers with incomplete recovery and delayed deintercalation, and coherently stacked multilayers that self-stabilize through reversible folding. Operando synchrotron X-ray diffraction shows this memory at electrode scale, where the interlayer structure converges towards a reproducible state. Our findings reveal cycling-induced structural memory that governs subsequent intercalation in layered MXenes.
ER -