Journal
ACS CENTRAL SCIENCE
Volume 8, Issue 2, Pages 169-175Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.1c01260
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Funding
- National Science Foundation (NSF) through the Materials Research Science and Engineering Center at UC Santa Barbara [DMR-1720256 (IRG-2)]
- Mitsubishi Chemical Center for Advanced Materials (MC-CAM)
- UCSB MRSEC [NSF DMR 1720256]
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By self-assembling into superionically conductive domains, the ion electrolyte overcomes the limitation of limited conductivity and achieves excellent performance in lithium-ion batteries.
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(+) approximate to 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.
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