Zwitterion Doping to an Organic Ionic Plastic Crystal Electrolyte: A Strategy to Improve Ionic Conductivity without Compromising Melting Point
- 1Institute for Frontier Materials (IFM, Deakin University, 221 Burwood Highway, Burwood, Victoria, Australia, 3125
- 2Deakin University, 5/154 Highbury Road, Burwood, Victoria, Australia, 3125
- 3Innovation Strategy Division, Mitsubishi Chemical Corporation, 1000 Kamoshida-cho, Aobaku, Yokohama, Japan, 227-8502
Abstract
Li+-containing organic ionic plastic crystals (OIPCs) show great promise as solid electrolytes for solid-state batteries. However, their ongoing issue is a decrease in the melting point with an increase in the Li+ concentration, requiring a new strategy to improve ion-transport properties without compromising the operating temperature range of the electrolytes as a solid. Herein, we address this by incorporating a small portion of zwitterions into an OIPC matrix, N,Ndiethylpyrrolidinium bis(fluorosulfonyl)imide ([C2epyr][FSI]). The effect of zwitterion incorporation on physicochemical properties depends on the type of zwitterion. If its structure is similar to the host OIPC, it improves ionic conductivity without narrowing down the temperature range as a plastic crystal, which is supported by minimal destruction to the host crystalline lattice without obvious formation of new crystalline phases. The cycle test of solid-state Li | LiFePO4−[C2epyr][FSI] cells with various concentrations of the pyrrolidinium-based zwitterion in the cathode layer showed the most stable discharge capacity of 150 mAh/g at 0.1C, 50 °C for the cell with 8.70 mol% of the zwitterion, without any sign of capacity decay. Impedance analysis unveiled the positive effect of the zwitterion addition at this concentration regime, which stabilizes cathode-electrolyte interphase and charge transfer at the LFP interface.
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BibTeX
@misc{ueda2026zwitterion,
title = {{Zwitterion Doping to an Organic Ionic Plastic Crystal Electrolyte: A Strategy to Improve Ionic Conductivity without Compromising Melting Point}},
author = {Hiroyuki Ueda and Hiroki Sugisawa and Frederick Nti and Toshifumi Takahashi and Emi Nakatsuka and Hiroyuki Aikyo and Kaoru Fukii and Masahiko Kato and Kenichi Satake and Kazunori Mukunoki and Robert Kerr and Jennifer M. Pringle and Tomofumi Hamamura},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15009577/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009577/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Zwitterion Doping to an Organic Ionic Plastic Crystal Electrolyte: A Strategy to Improve Ionic Conductivity without Compromising Melting Point
AU - Hiroyuki Ueda
AU - Hiroki Sugisawa
AU - Frederick Nti
AU - Toshifumi Takahashi
AU - Emi Nakatsuka
AU - Hiroyuki Aikyo
AU - Kaoru Fukii
AU - Masahiko Kato
AU - Kenichi Satake
AU - Kazunori Mukunoki
AU - Robert Kerr
AU - Jennifer M. Pringle
AU - Tomofumi Hamamura
PY - 2026
DA - 2026/09/28
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009577/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009577/v1
AB - Li+-containing organic ionic plastic crystals (OIPCs) show great promise as solid electrolytes for solid-state batteries. However, their ongoing issue is a decrease in the melting point with an increase in the Li+ concentration, requiring a new strategy to improve ion-transport properties without compromising the operating temperature range of the electrolytes as a solid. Herein, we address this by incorporating a small portion of zwitterions into an OIPC matrix, N,Ndiethylpyrrolidinium bis(fluorosulfonyl)imide ([C2epyr][FSI]). The effect of zwitterion incorporation on physicochemical properties depends on the type of zwitterion. If its structure is similar to the host OIPC, it improves ionic conductivity without narrowing down the temperature range as a plastic crystal, which is supported by minimal destruction to the host crystalline lattice without obvious formation of new crystalline phases. The cycle test of solid-state Li | LiFePO4−[C2epyr][FSI] cells with various concentrations of the pyrrolidinium-based zwitterion in the cathode layer showed the most stable discharge capacity of 150 mAh/g at 0.1C, 50 °C for the cell with 8.70 mol% of the zwitterion, without any sign of capacity decay. Impedance analysis unveiled the positive effect of the zwitterion addition at this concentration regime, which stabilizes cathode-electrolyte interphase and charge transfer at the LFP interface.
ER -