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PreprintCC BY-NC-NDChemRxiv

Decoupling Nanofiller Dimensionality and Electronic Character in Gel Polymer Electrolytes for Supercapacitors

  1. 1William A. Brookshire Department of Chemical and Biomolecular Engineering, University of Houston, 4226 Martin Luther King Boulevard, Houston, TX, United States, 77204
  2. 2Materials Science and Engineering, University of Houston, 4226 Martin Luther King Boulevard, Houston, TX, United States, 77204

Abstract

Gel polymer electrolytes bridge the gap between the mechanical compliance needed for flexible supercapacitors and the ionic transport required for competitive rate performance, and nanofiller incorporation is a widely adopted route to improving both. However, because most studies examine individual nanofillers in different polymer hosts under varying conditions, the relative contributions of filler geometry and intrinsic electronic character remain entangled. Here, a chemically crosslinked poly(vinyl alcohol)-poly(ethylene glycol) gel electrolyte was used as a common matrix to compare four nanofillers at identical loading, spanning a 2 × 2 design of dimensionality (1D versus 2D) crossed with electronic character (insulative versus conductive): halloysite nanotubes (HNT), multiwalled carbon nanotubes (MWCNTs), hexagonal boron nitride (hBN), and reduced graphene oxide (rGO). The 1D-filled electrolytes reached ionic conductivities of approximately 39 mS cm −1 , compared with 26 mS cm −1 for the 2D-filled membranes and 15 mS cm −1 for the neat electrolyte. Thus, the 1D-filled electrolytes were approximately 50% more conductive than their 2D counterparts and this difference was largely independent of whether the filler was insulating or conductive. In symmetric supercapacitor cells, however, the capacitance ranking did not follow this conductivity trend. The MWCNT composite delivered the highest specific capacitance of 151 F g −1 and energy density of 13.5 Wh kg −1 , yet the insulating hexagonal boron nitride (94 F g −1 ) outperformed the conductive reduced graphene oxide (76 F g −1 ), demonstrating that cell-level charge storage is governed by the combined influence of ionic transport, filler-matrix interactions, and interfacial ion accessibility rather than any single filler descriptor. These findings provide a framework for rational nanofiller selection in gel polymer electrolytes based on both geometry and electronic classification.

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BibTeX
@misc{kanak2026decoupling,
  title = {{Decoupling Nanofiller Dimensionality and Electronic Character in Gel Polymer Electrolytes for Supercapacitors}},
  author = {Nishat Anzum Kanak and Hironmoy Chowdhury and Parisa Naji and Abrar Zadeed Ahmed and Alamgir Karim},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008965/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008965/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Decoupling Nanofiller Dimensionality and Electronic Character in Gel Polymer Electrolytes for Supercapacitors
AU  - Nishat Anzum Kanak
AU  - Hironmoy Chowdhury
AU  - Parisa Naji
AU  - Abrar Zadeed Ahmed
AU  - Alamgir Karim
PY  - 2026
DA  - 2026/09/17
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008965/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008965/v1
AB  - Gel polymer electrolytes bridge the gap between the mechanical compliance needed for flexible supercapacitors and the ionic transport required for competitive rate performance, and nanofiller incorporation is a widely adopted route to improving both. However, because most studies examine individual nanofillers in different polymer hosts under varying conditions, the relative contributions of filler geometry and intrinsic electronic character remain entangled. Here, a chemically crosslinked poly(vinyl alcohol)-poly(ethylene glycol) gel electrolyte was used as a common matrix to compare four nanofillers at identical loading, spanning a 2 × 2 design of dimensionality (1D versus 2D) crossed with electronic character (insulative versus conductive): halloysite nanotubes (HNT), multiwalled carbon nanotubes (MWCNTs), hexagonal boron nitride (hBN), and reduced graphene oxide (rGO). The 1D-filled electrolytes reached ionic conductivities of approximately 39 mS cm −1 , compared with 26 mS cm −1 for the 2D-filled membranes and 15 mS cm −1 for the neat electrolyte. Thus, the 1D-filled electrolytes were approximately 50% more conductive than their 2D counterparts and this difference was largely independent of whether the filler was insulating or conductive. In symmetric supercapacitor cells, however, the capacitance ranking did not follow this conductivity trend. The MWCNT composite delivered the highest specific capacitance of 151 F g −1 and energy density of 13.5 Wh kg −1 , yet the insulating hexagonal boron nitride (94 F g −1 ) outperformed the conductive reduced graphene oxide (76 F g −1 ), demonstrating that cell-level charge storage is governed by the combined influence of ionic transport, filler-matrix interactions, and interfacial ion accessibility rather than any single filler descriptor. These findings provide a framework for rational nanofiller selection in gel polymer electrolytes based on both geometry and electronic classification.
ER  -