Design of robust and versatile hydrocarbon-based single-ion-conducting polymer electrolytes

Ain Uddin; Michelle L. Lehmann; Tanya Agarwal; Heemin Park; Catalin Gainaru; Lilin He; Alexei P. Sokolov; Yu Seung Kim; Tomonori Saito

doi:10.1016/j.xcrp.2025.102712

Design of robust and versatile hydrocarbon-based single-ion-conducting polymer electrolytes

Ain Uddin, Michelle L. Lehmann, Tanya Agarwal, Heemin Park, Catalin Gainaru, Lilin He, Alexei P. Sokolov, Yu Seung Kim, Tomonori Saito

Research output: Contribution to journal › Article › peer-review

Abstract

Hydrocarbon-based polymers offer several advantages, including lower environmental impacts, cost effectiveness, and the ability to finely tune properties. Here, we have developed trifluoromethanesulfonimide (TFSI)-functionalized poly(norbornene) (PNB) polymers utilizing a specifically designed oxa-Michael addition of a vinyl TFSI anion to an alcohol. Our results reveal that PNB-TFSI derivatives exhibit superior thermal stability and mechanical robustness compared with Nafion. The optimized PNB-TFSI-H-48 polymer (IEC 1.86 mmol/g) exhibits equivalent performance to Nafion as an anode ionomer in a proton exchange membrane fuel cell. Exchanging the counter ion to Li⁺ enables PNB-TFSI to be used for Li-ion battery applications. Propylene carbonate plasticized PNB-TFSI derivatives achieve an Li-ion conductivity of over 10⁻⁵ S/cm at 30°C. This Li polymer electrolyte exhibits excellent electrochemical stability (5 V vs. Li⁺/Li) and good cycling in a Li symmetric cell. These results highlight the potential and rational design of PNB-TFSI polymers for next-generation energy storage and conversion technologies.

Original language	English
Article number	102712
Journal	Cell Reports Physical Science
Volume	6
Issue number	7
DOIs	https://doi.org/10.1016/j.xcrp.2025.102712
State	Published - Jul 16 2025

Funding

This work was supported as part of the Fast and Cooperative Ion Transport in Polymer-Based Materials (FaCT), an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences at Oak Ridge National Laboratory. Analysis for hydrogen fuel cell was supported by the US Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), and Hydrogen and Fuel Cell Technologies Office (HFTO) through the M2FCT (Million Mile Fuel Cell Truck) Consortium. This research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beam time was allocated to CG2 on proposal number IPTS-33565.1.

Keywords

TFSI
fuel cell
hydrocarbon
ion conductivity
membranes
polymer electrolytes
single-ion conductor

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10.1016/j.xcrp.2025.102712

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title = "Design of robust and versatile hydrocarbon-based single-ion-conducting polymer electrolytes",

abstract = "Hydrocarbon-based polymers offer several advantages, including lower environmental impacts, cost effectiveness, and the ability to finely tune properties. Here, we have developed trifluoromethanesulfonimide (TFSI)-functionalized poly(norbornene) (PNB) polymers utilizing a specifically designed oxa-Michael addition of a vinyl TFSI anion to an alcohol. Our results reveal that PNB-TFSI derivatives exhibit superior thermal stability and mechanical robustness compared with Nafion. The optimized PNB-TFSI-H-48 polymer (IEC 1.86 mmol/g) exhibits equivalent performance to Nafion as an anode ionomer in a proton exchange membrane fuel cell. Exchanging the counter ion to Li+ enables PNB-TFSI to be used for Li-ion battery applications. Propylene carbonate plasticized PNB-TFSI derivatives achieve an Li-ion conductivity of over 10−5 S/cm at 30°C. This Li polymer electrolyte exhibits excellent electrochemical stability (5 V vs. Li+/Li) and good cycling in a Li symmetric cell. These results highlight the potential and rational design of PNB-TFSI polymers for next-generation energy storage and conversion technologies.",

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author = "Ain Uddin and Lehmann, \{Michelle L.\} and Tanya Agarwal and Heemin Park and Catalin Gainaru and Lilin He and Sokolov, \{Alexei P.\} and Kim, \{Yu Seung\} and Tomonori Saito",

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AU - Uddin, Ain

AU - Lehmann, Michelle L.

AU - Agarwal, Tanya

AU - Park, Heemin

AU - Gainaru, Catalin

AU - He, Lilin

AU - Sokolov, Alexei P.

AU - Kim, Yu Seung

AU - Saito, Tomonori

PY - 2025/7/16

Y1 - 2025/7/16

N2 - Hydrocarbon-based polymers offer several advantages, including lower environmental impacts, cost effectiveness, and the ability to finely tune properties. Here, we have developed trifluoromethanesulfonimide (TFSI)-functionalized poly(norbornene) (PNB) polymers utilizing a specifically designed oxa-Michael addition of a vinyl TFSI anion to an alcohol. Our results reveal that PNB-TFSI derivatives exhibit superior thermal stability and mechanical robustness compared with Nafion. The optimized PNB-TFSI-H-48 polymer (IEC 1.86 mmol/g) exhibits equivalent performance to Nafion as an anode ionomer in a proton exchange membrane fuel cell. Exchanging the counter ion to Li+ enables PNB-TFSI to be used for Li-ion battery applications. Propylene carbonate plasticized PNB-TFSI derivatives achieve an Li-ion conductivity of over 10−5 S/cm at 30°C. This Li polymer electrolyte exhibits excellent electrochemical stability (5 V vs. Li+/Li) and good cycling in a Li symmetric cell. These results highlight the potential and rational design of PNB-TFSI polymers for next-generation energy storage and conversion technologies.

AB - Hydrocarbon-based polymers offer several advantages, including lower environmental impacts, cost effectiveness, and the ability to finely tune properties. Here, we have developed trifluoromethanesulfonimide (TFSI)-functionalized poly(norbornene) (PNB) polymers utilizing a specifically designed oxa-Michael addition of a vinyl TFSI anion to an alcohol. Our results reveal that PNB-TFSI derivatives exhibit superior thermal stability and mechanical robustness compared with Nafion. The optimized PNB-TFSI-H-48 polymer (IEC 1.86 mmol/g) exhibits equivalent performance to Nafion as an anode ionomer in a proton exchange membrane fuel cell. Exchanging the counter ion to Li+ enables PNB-TFSI to be used for Li-ion battery applications. Propylene carbonate plasticized PNB-TFSI derivatives achieve an Li-ion conductivity of over 10−5 S/cm at 30°C. This Li polymer electrolyte exhibits excellent electrochemical stability (5 V vs. Li+/Li) and good cycling in a Li symmetric cell. These results highlight the potential and rational design of PNB-TFSI polymers for next-generation energy storage and conversion technologies.

KW - TFSI

KW - fuel cell

KW - hydrocarbon

KW - ion conductivity

KW - membranes

KW - polymer electrolytes

KW - single-ion conductor

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DO - 10.1016/j.xcrp.2025.102712

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JO - Cell Reports Physical Science

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ER -

Design of robust and versatile hydrocarbon-based single-ion-conducting polymer electrolytes

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