Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 130, Issue 6, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3063659
Keywords
dielectric polarisation; dielectric relaxation; electrodes; glass transition; ion mobility; ionic conductivity; lithium; permittivity; polymer blends
Funding
- Department of Energy, Office of Basic Energy Sciences [DE-FG02-07ER46409]
- U.S. Department of Energy (DOE) [DE-FG02-07ER46409] Funding Source: U.S. Department of Energy (DOE)
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We investigate the segmental and local dynamics as well as the transport of Li+ cations in a series of model poly(ethylene oxide)-based single-ion conductors with varying ion content, using dielectric relaxation spectroscopy. We observe a slowing down of segmental dynamics and an increase in glass transition temperature above a critical ion content, as well as the appearance of an additional relaxation process associated with rotation of ion pairs. Conductivity is strongly coupled to segmental relaxation. For a fixed segmental relaxation frequency, molar conductivity increases with increasing ion content. A physical model of electrode polarization is used to separate ionic conductivity into the contributions of mobile ion concentration and ion mobility, and a model for the conduction mechanism involving transient triple ions is proposed to rationalize the behavior of these quantities as a function of ion content and the measured dielectric constant.
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