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DOE OSTI · 2575314

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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BibTeXRIS

Uddin, Ain [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Lehmann, Michelle L. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000313239785), Agarwal, Tanya [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000155077708), Park, Heemin [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)], Gainaru, Catalin [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], He, Lilin [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000295608101), Sokolov, Alexei P. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000281879445), Kim, Yu Seung [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000254463890), Saito, Tomonori [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000245367530). 2025-07-16. Design of robust and versatile hydrocarbon-based single-ion-conducting polymer electrolytes. https://doi.org/10.1016/j.xcrp.2025.102712

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