The influence of interfacial interactions on the conductivity and phase behaviour of organic ionic plastic crystal/polymer nanoparticle composite electrolytes

Nti, Frederick; Porcarelli, Luca; Greene, George W.; Zhu, Haijin; Makhlooghiazad, Faezeh; Mecerreyes, David; Howlett, Patrick C.; Forsyth, Maria; Wang, Xiaoen

doi:10.1039/c9ta12827a

Cited by 32 publications

(48 citation statements)

References 36 publications

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“…The addition of OIPC to a conducting polymer has been studied, providing promising results with an enhancement of ×9 for electronic conductivity (17.7 S cm –1 ) and ×180 for ionic conductivity in the 40/60 PEDOT–Cl/[C 2 mpyr][FSI] composite. Surprisingly, ionic conductivity values of around 10 –4 S cm –1 at room temperature were obtained, which might be due to the formation of highly conducting pathways through the interphase of PEDOT–Cl and [C 2 mpyr][FSI], as has been suggested for OIPC/PVdF composites. , It is important to note that these ionic conductivity values are really close to the desirable range of solid electrolytes (∼10 –3 S cm –1 ) in the field of ESSs . Furthermore, the activation energy for conduction in these composites was very low, as observed in the Arrhenius representation of ionic conductivity versus inverse temperature (Figure S3).…”

Section: Discussionmentioning

confidence: 74%

Tuning Electronic and Ionic Conductivities in Composite Materials for Electrochemical Devices

Casado

Zendegi

Olmo

et al. 2021

ACS Appl. Polym. Mater.

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Mixed conductors having both high ionic and electronic conductivities are needed in membrane electrode assemblies (MEAs) present in electrochemical devices from fuel cells to supercapacitors and all battery chemistries. Typically, carbon black, binders, and redox-active materials are combined to make an electrode assembly, into which a liquid electrolyte can impregnate. Solid-state devices require the ionic conduction built into the MEA. In this case, a material which can provide both electronic and ionic conduction as well as a redox functionality is described based on PEDOT−Cl as both the electronic conductor and the redox active component, while an organic ionic plastic crystal [C 2 mpyr][FSI] is present as both the binder and ionic conductor. Surprisingly, both the electronic and ionic conductivities of the composite are enhanced relative to the pure components by a factor of ×9 for electronic and ×180 for ionic conductivities. The mixed conducting composites are demonstrated to retain their redox activity in aqueous electrolytes, and in the optimum case, 103 F g −1 and 296 mF cm −2 capacitance values are obtained for low-and high-mass loading electrodes. These materials demonstrate an innovative approach to prepare electrode assemblies where all three functionalities are incorporated into the materials, that is, electronic, ionic, and redox activity for future energy devices.

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Section: Discussionmentioning

confidence: 74%

Tuning Electronic and Ionic Conductivities in Composite Materials for Electrochemical Devices

Casado

Zendegi

Olmo

et al. 2021

ACS Appl. Polym. Mater.

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“…The materials can possess plastic behavior and high ionic conductivities. In previous works, Nti et al [ 25 ] recently reported their study on the interactions between OIPCs and polymers, such as poly(vinylidene fluoride) (PVDF) and polystyrene (PS), which showed that the combination of OIPCs and polymer particles enhanced the ionic conductivity and resulted in good mechanical stability of the composites. Therefore, in this article the potential of organic ionic plastic crystals to enhance both the ionic conductivity and the mechanical properties of the PEDOT:PolyDADMA OMIECs was investigated.…”

Section: Introductionmentioning

confidence: 99%

Mixed Ionic-Electronic Conductors Based on PEDOT:PolyDADMA and Organic Ionic Plastic Crystals

et al. 2020

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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.

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“…As shown in Table S1, the peak wavenumbers for the spectra of the interlayer and [C 2 mpyr][FSI] composite are almost the same as those of [C 2 mpyr][FSI]. In contrast to the FTIR spectrum of the composite composed of PVdF nanoparticles and [C 2 mpyr][FSI], [25] no obvious peak shifts are observed for the spectrum of the interlayer. This is due to the low weight ratio of PVdF (10 wt %) in the interlayer.…”

Section: Resultsmentioning

confidence: 76%

“…To further analyze SEI formation at the first charging, FTIR spectroscopy was performed for the surfaces of the solid-state graphite-[C 2 mpyr][FSI] composite anodes (70 wt % graphite anode + 30 wt % [C 2 mpyr][FSI] composite). Figure 1c [25] no obvious peak shifts are observed for the spectrum of the interlayer. This is due to the low weight ratio of PVdF (10 wt %) in the interlayer.…”

Section: Initial Charge-discharge Profilementioning

confidence: 99%

Fast Charge and High Stability of Solid‐State Graphite Organic Ionic Plastic Crystal Composite Anodes

Ueda

Mizuno

Kerr

et al. 2022

Batteries & Supercaps

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All-solid-state batteries (ASSBs) using organic ionic plastic crystals (OIPCs) are promising candidates to overcome the inherent safety issues of lithium-ion batteries (LIBs). Although OIPCs have excellent process applicability in the roll-to-roll electrode fabrication process, their application as solid electrolytes incorporated in composite electrodes has yet to be demonstrated in detail. Herein, we denote the positive effect of the N-ethyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide ([C 2 mpyr][FSI]) incorporated within a composite graphite anode on the charge rate capability and cycle life. The highest charge capacity ratio (the charge capacity at 2C vs. that measured at 0.1C) was measured for the composite anode with an OIPC composite ratio of 50 wt % (89.5 %, 295.7 mAh/g at 2C charge), almost the same as that of the graphite anode with a liquid electrolyte (85.7 %, 295.9 mAh/g at 2C charge). More favorable lithium-ion conduction pathways were resolved for the anode with a higher OIPC composite ratio, whereas an excessive amount of OIPC reduced the long-term cyclability. The most stable discharge capacity retention was obtained for 30 wt % OIPC composite (257.4 mAh/g at the 100th discharge), which showed no signs of discharge capacity fading within 100 cycles. The lithiation/delithiation process of the solid-state graphite-[C 2 mpyr][FSI] composite anode was evaluated to be stable and reversible. In addition, the incorporated OIPC composite enhanced the electrolyte/electrode and electrode/current collector contacts. This work highlights multiple advantageous functions of the OIPC in a composite graphite anode, which will broaden our horizons for the use of OIPC composites in ASSBs.

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The influence of interfacial interactions on the conductivity and phase behaviour of organic ionic plastic crystal/polymer nanoparticle composite electrolytes

Abstract: The interactions between OIPCs and polymer nanoparticles create interfacial layers that control the ion mobility of the resulting composite.

Cited by 32 publications

References 36 publications

Tuning Electronic and Ionic Conductivities in Composite Materials for Electrochemical Devices

Tuning Electronic and Ionic Conductivities in Composite Materials for Electrochemical Devices

Mixed Ionic-Electronic Conductors Based on PEDOT:PolyDADMA and Organic Ionic Plastic Crystals

Fast Charge and High Stability of Solid‐State Graphite Organic Ionic Plastic Crystal Composite Anodes

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