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Mesoscale dynamics of electrosorbed ions in fast-charging carbon-based nanoporous electrodes

Nature Nanotechnology volume 20, pages 1228–1236 (2025)Cite this article

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Abstract

Electrosorption, the accumulation of electrolyte ions at charged interfaces, is a common phenomenon across various electrochemical systems. Its impact is particularly pronounced in nanoporous electrodes owing to their high surface-to-volume ratios. Although electrosorption alters the ion distribution at the electrode–electrolyte interface through the formation of an electrical double layer, the effects of electrosorbed ions on the charge storage dynamics in nanoporous electrodes and their ability to improve charging processes have often been overlooked. Here we use a multilayered reduced graphene oxide-based membrane as a model nanoporous electrode material, integrating numerical simulations with experimental insights. We monitor the spatiotemporal distribution of electrosorbed ions and electrical potentials across the nanopore network during fast charging of symmetrical laboratory-scale cells using aqueous and non-aqueous electrolyte solutions. This method allowed us to quantitatively assess how features of the nanoporous electrode mesostructure, such as nanoslit size, the distribution of nanoslit sizes and electrode thickness, dynamically influence ion electrosorption and the local electrical and chemical potentials across the network. Our findings reveal that the mesostructure of nanoporous electrodes influences how migration and diffusion currents, mediated by electrosorbed ions, respond to charging rates.

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Fig. 1: Capacitance performance of symmetric MGM|electrolyte|MGM cells with varied electrode mass loadings and slit size distributions.
Fig. 2: Illustration of the spatiotemporal evolution of electrosorbed ions confined in a multilayered graphene nanoslit network.
Fig. 3: Electrosorption-mediated ion transport dynamics.
Fig. 4: Impact of the mesostructural electrode engineering strategy on the cell capacitance behaviour.

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All data needed to evaluate the conclusions are available in the Article or Supplementary Information. Source data are provided with this paper.

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Acknowledgements

We thank H. Zhan and Y. Wang for discussions. This work is supported by funding from the Australia Research Council (grant numbers FL180100029, IC180100049 and DP220103498 to D.L. and grant number FT220100149 to J.Z.L.).

Author information

Author notes

  1. Ke Zhang

    Present address: AI for Science Department, BYD Lithium Ions Battery Company Limited, Shenzhen, China

  2. Dan Li

    Present address: Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Hong Kong, China

  3. These authors contributed equally: Peiyao Wang, Ke Zhang.

Authors and Affiliations

  1. Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria, Australia

    Peiyao Wang, Jinsha Liao, Xiao Wang & Dan Li

  2. Department of Materials Science and Engineering, Monash University, Clayton, Victoria, Australia

    Ke Zhang, George P. Simon & Dan Li

  3. Department of Mechanical Engineering, The University of Melbourne, Parkville, Victoria, Australia

    Jefferson Zhe Liu

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  1. Peiyao Wang
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Contributions

Conceptualization: D.L., P.W. and K.Z. Methodology and data analysis: P.W., K.Z., J.L., D.L. and J.Z.L. Investigation: P.W. and K.Z. Visualization: P.W. and J.L. Funding acquisition: D.L. Project administration: D.L. Supervision: D.L., J.Z.L. and G.P.S. Writing—original draft: P.W., D.L. Writing—review and editing: P.W., J.L., D.L., J.Z.L., G.P.S., K.Z. and X.W.

Corresponding authors

Correspondence to Jefferson Zhe Liu or Dan Li.

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Nature Nanotechnology thanks Kangkang Ge and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Wang, P., Zhang, K., Liao, J. et al. Mesoscale dynamics of electrosorbed ions in fast-charging carbon-based nanoporous electrodes. Nat. Nanotechnol. 20, 1228–1236 (2025). https://doi.org/10.1038/s41565-025-01947-8

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