Progress toward durable and energy-dense lithium-ion batteries has been hindered by instabilities at electrolyte–electrode interfaces, leading to poor cycling stability, and by safety concerns associated with energy-dense lithium metal anodes. Solid polymeric electrolytes (SPEs) can help mitigate these issues; however, the SPE conductivity is limited by sluggish polymer segmental dynamics. We overcome this limitation via zwitterionic SPEs that self-assemble into superionically conductive domains, permitting decoupling of ion motion and polymer segmental rearrangement. Although crystalline domains are conventionally detrimental to ion conduction in SPEs, we demonstrate that semicrystalline polymer electrolytes with labile ion–ion interactions and tailored ion sizes exhibit excellent lithium conductivity (1.6 mS/cm) and selectivity ( t + ≈ 0.6–0.8). This new design paradigm for SPEs allows for simultaneous optimization of previously orthogonal properties, including conductivity, Li selectivity, mechanics, and processability.
Rechargeable batteries generate current through the transfer of electrons between paramagnetic and/or metallic electrode materials. Electron spin probes, such as electron paramagnetic resonance (EPR) and magnetometry, can therefore provide detailed insight into the underlying energy storage mechanisms. These techniques have been applied ex situ, and more recently operando, to both intercalation-and conversion-type batteries. After briefly reviewing the principles of EPR and magnetometry, this perspective provides a critical discussion of recent studies that leverage these tools to understand the local structure, defect chemistry and charge/discharge and failure mechanisms of rechargeable batteries. Challenges in data collection and interpretation are addressed and strategies to facilitate EPR spectral assignment and expand the scope of EPR and magnetometry studies of battery systems are suggested.
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