In solid polymer electrolytes, the transference number ( ) is fundamental for performance as it defines the transport efficiency of the electrochemically active species. For systems "beyond Li", a lack of suitable methods to determine the is limiting the understanding of the ion transport in such systems. In this study, a method based on electrophoretic NMR (eNMR) and electrochemical impedance spectroscopy (EIS) is used to determine the for Na, K, and Mg in poly(ε-caprolactone) (PCL), comparing this to previous results in poly(ethylene oxide). In common for all cations, a distinct correlation between strong coordination and a low is observed. Paradoxically, however, the divalent Mg in PCL displayed a of 0.86 compared to ∼0.5 for the monovalent cations. Persistent clustering in this system suggests that it is better treated as a monovalent [MgTFSI] + TFSI system, resulting in a of the [MgTFSI] cation of 0.43. These results serve as a door opener for the wide applicability of the eNMR/EIS method in order to provide an understanding of charge transport in multivalent systems.
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| http://dx.doi.org/10.1021/acs.jpcc.4c04632 | DOI Listing |
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