Abstract
Mixed ionic-electronic conductors, such as poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) are postulated to be the next generation materials in energy storage and electronic devices. Although many studies have aimed to enhance the electronic conductivity and mechanical properties of these materials, there has been little focus on ionic conductivity. In this work, blends based on PEDOT stabilized by the polyelectrolyte poly(diallyldimethylammonium) (PolyDADMA X) are reported, where the X anion is either chloride (Cl), bis(fluorosulfonyl)imide (FSI), bis(trifluoromethylsulfonyl)imide (TFSI), triflate (CF3SO3) or tosylate (Tos). Electronic conductivity values of 0.6 S cm−1 were achieved in films of PEDOT:PolyDADMA FSI (without any post-treatment), with an ionic conductivity of 5 × 10−6 S cm−1 at 70 °C. Organic ionic plastic crystals (OIPCs) based on the cation N-ethyl-N-methylpyrrolidinium (C2mpyr+) with similar anions were added to synergistically enhance both electronic and ionic conductivities. PEDOT:PolyDADMA X / [C2mpyr][X] composites (80/20 wt%) resulted in higher ionic conductivity values (e.g., 2 × 10−5 S cm−1 at 70 °C for PEDOT:PolyDADMA FSI/[C2mpyr][FSI]) and improved electrochemical performance versus the neat PEDOT:PolyDADMA X with no OIPC. Herein, new materials are presented and discussed including new PEDOT:PolyDADMA and organic ionic plastic crystal blends highlighting their promising properties for energy storage applications.
Highlights
Inorganic mixed ionic-electronic conductors (MIECs) have been well studied and applied in different fields [1,2], as they show excellent ionic conductivities and thermal stability
In this article we investigated the ternary system between PEDOT, PolyDADMA and pyrrolidonium
First we reported the synthesis and characterization of the individual systems, in the form of neat PolyDADMA X
Summary
Inorganic mixed ionic-electronic conductors (MIECs) have been well studied and applied in different fields [1,2], as they show excellent ionic conductivities and thermal stability. Many studies have aimed to enhance the properties such as the electronic conductivity, by adding high boiling point solvents [9], superacids [10] or ionic liquids [11], mechanical properties [12] or employing hybrid architectures [13], even showing metallic conductivities of 6259 ± 1468 S cm−1 for thin post-treated films [14] and totally flexible foils [12] These π-conjugated polymers can be either functionalized with polyelectrolytes and polymer electrolytes via pendant groups [15], or form copolymers and blends with other polymers (e.g., polyethylene oxide (PEO) [4] and polystyrene sulfonate (PSS) [12]), which provide the ionic conductivity. Very few studies have been carried out to enhance their weaker feature, that is the ionic conductivity in their dry state
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