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Lamellar Ionenes with Highly Dissociative, Anionic Channels Provide Lower Barriers for Cation Transport
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DOI：10.1021/jacs.3c05053.png)
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Abstract
En 中文
Solidpolymer electrolytes have the potential to enable safer andmore energy-dense batteries; however, a deeper understanding of theirion conduction mechanisms, and how they can be optimized by moleculardesign, is needed to realize this goal. Here, we investigate the impactof anion dissociation energy on ion conduction in solid polymer electrolytesvia a novel class of ionenes prepared using acyclic diene metathesis(ADMET) polymerizationof highly dissociative, liquid crystalline fluorinated aryl sulfonimide-tagged(FAST) anion monomers. These ionenes with variouscations (Li+, Na+, K+, and Cs+) form well-ordered lamellae that are thermally stable upto 180 & DEG;C and feature domain spacings that correlate with cationsize, providing channels lined with dissociative FAST anions. Electrochemicalimpedance spectroscopy (EIS) and differential scanning calorimetry(DSC) experiments, along with nudged elastic band (NEB) calculations,suggest that cation motion in these materials operates via an ion-hoppingmechanism. The activation energy for Li+ conduction is59 kJ/mol, which is among the lowest for systems that are proposedto operate via an ion conduction mechanism that is decoupled frompolymer segmental motion. Moreover, the addition of a cation-coordinatingsolvent to these materials led to a >1000-fold increase in ionicconductivitywithout detectable disruption of the lamellar structure, suggestingselective solvation of the lamellar ion channels. This work demonstratesthat molecular design can facilitate controlled formation of dissociativeanionic channels that translate to significant enhancements in ionconduction in solid polymer electrolytes.
Keywords:
IONIC-CONDUCTIVITY
TRANSFERENCE NUMBER
ELECTROLYTES
LIQUID
POLYMERS
CRYSTALS
DESIGN
SALTS
Journal
IF:
15.6
Papers:
20.0W
Citations:
60.2W
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