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001     1029093
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100 1 _ |a Overhoff, Gerrit Michael
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245 _ _ |a Enhancing the Electrochemical Performance of Blended Single-Ion Conducting Polymers by Smart Modification of the Polymer Structure
260 _ _ |a Washington, DC
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520 _ _ |a Single lithium-ion conducting polymers represent a promisingclass of electrolytes that potentially enable the utilization of lithium metal anodes in next-generation batteries. The immobilization of anions within the polymer’s structure in principle mitigates issues related to localized ion depletion, resulting in decreased cell polarization when compared to common dual-ion conductors comprising poly(ethylene oxide) and lithium salt. However, the intrinsic rigidity of these materials often necessitates incorporation of flowable components and blending with other polymers, such as poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF-HFP), to enhance the mechanical flexibility of the resulting polymer membranes. Within polymer blends, distinct phases may be present, and the distribution of plasticizers among these phases is highly crucial as they act as carrier molecules for Li+ transport. In this study, we thus explored the impact of polymer chain modification from a rigid aromatic single-ion conducting polymer to a more flexible polymer by introducing ethylene glycol units into the backbone. Notably, this alteration yielded a substantial decrease of 100 °C of the glass transition temperature and a 6-fold increase in ionic conductivity (0.5 mS cm−1 @ 40 °C) after blending with PVdF-HFP and addition of ethylene carbonate/dimethyl carbonate. Atomistic molecular dynamics simulations suggest that this enhancement can be attributed to a high concentration of plasticizer within the Li+ containing phase. In symmetric Li||Li cells, exceptional performance was achieved, demonstrating operation at high limiting current density and successful plating/stripping for 1000 h at 0.2 mA cm−2. When paired with high-voltage NMC cathodes, the introduced polymer structures exhibited noteworthy capacity retention after 800 cycles, emphasizing advantages brought forth by flexible and adapted polymer architecture.
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700 1 _ |a Verweyen, Elisabeth
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700 1 _ |a Roering, Philipp
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700 1 _ |a Winter, Martin
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700 1 _ |a Brunklaus, Gunther
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773 _ _ |a 10.1021/acsaem.4c01117
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