Pore-Engineering Enhances Low-Temperature Mixed Ionic-Electronic Conduction in Two-Dimensional Polymer Lithium Ion-Battery Electrodes
- 1Department of Chemistry
- 2Department of Materials Science and Engineering
- 3University of Florida
Abstract
Understanding the fundamental relationships between ionic and electronic charge transport in polymer systems is essential for the systematic development of bioelectronic, optoelectronic, and energy-storage devices that leverage these materials. A classic strategy to improve ionic conductivity in mixed conducting materials involves attaching ionophilic oligoethylene glycol (OEG) groups to charge-carrying polymers. However, installation of oxygen heteroatoms into the framework of mixed ionic-electronic conductors also induces unintended structural changes in both the native and operational states, thereby adding complexity to structure-property relationships. Two-dimensional polymers (2DPs) are crystalline, planar macromolecules with well-defined one-dimensional channels that can be functionalized without significantly disrupting the crystalline scaffold. We designed topologically equivalent 2DPs with either ionophobic or ionophilic pore structures and studied these materials as lithium-ion battery cathodes. We observed that OEG pore-functionalized 2DP electrodes exhibit higher redox potentials, lower charge-transfer resistances, and higher overall achievable capacities than ionophobic-functionalized 2DP electrodes. Additionally, we found that pore-functionalized 2DP electrodes have higher capacity retention at Arctic temperatures (-30 °C) than commercially available inorganic cathode materials. Our findings demonstrate that pore functionalization is a viable strategy for enhancing the performance of 2DP mixed ionic-electronic conductors and engineering them for extreme environment deployment.
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BibTeX
@misc{davis2026poreengineering,
title = {{Pore-Engineering Enhances Low-Temperature Mixed Ionic-Electronic Conduction in Two-Dimensional Polymer Lithium Ion-Battery Electrodes}},
author = {Ani N. Davis and Eva Vásquez-Barillas and Kiana A. Treaster and A M Mahmudul Hasan and John D. Langhout and Diana Graham and Kausturi Parui and Joshua D. Marquez and Megan M. Butala and Austin M. Evans},
howpublished = {ChemRxiv},
year = {2026},
month = oct,
doi = {10.26434/chemrxiv.15009754/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009754/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Pore-Engineering Enhances Low-Temperature Mixed Ionic-Electronic Conduction in Two-Dimensional Polymer Lithium Ion-Battery Electrodes
AU - Ani N. Davis
AU - Eva Vásquez-Barillas
AU - Kiana A. Treaster
AU - A M Mahmudul Hasan
AU - John D. Langhout
AU - Diana Graham
AU - Kausturi Parui
AU - Joshua D. Marquez
AU - Megan M. Butala
AU - Austin M. Evans
PY - 2026
DA - 2026/10/01
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009754/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009754/v1
AB - Understanding the fundamental relationships between ionic and electronic charge transport in polymer systems is essential for the systematic development of bioelectronic, optoelectronic, and energy-storage devices that leverage these materials. A classic strategy to improve ionic conductivity in mixed conducting materials involves attaching ionophilic oligoethylene glycol (OEG) groups to charge-carrying polymers. However, installation of oxygen heteroatoms into the framework of mixed ionic-electronic conductors also induces unintended structural changes in both the native and operational states, thereby adding complexity to structure-property relationships. Two-dimensional polymers (2DPs) are crystalline, planar macromolecules with well-defined one-dimensional channels that can be functionalized without significantly disrupting the crystalline scaffold. We designed topologically equivalent 2DPs with either ionophobic or ionophilic pore structures and studied these materials as lithium-ion battery cathodes. We observed that OEG pore-functionalized 2DP electrodes exhibit higher redox potentials, lower charge-transfer resistances, and higher overall achievable capacities than ionophobic-functionalized 2DP electrodes. Additionally, we found that pore-functionalized 2DP electrodes have higher capacity retention at Arctic temperatures (-30 °C) than commercially available inorganic cathode materials. Our findings demonstrate that pore functionalization is a viable strategy for enhancing the performance of 2DP mixed ionic-electronic conductors and engineering them for extreme environment deployment.
ER -