Ion transport in small-molecule and polymer electrolytes

Son, Chang Yun; Wang, Zhen‐Gang

doi:10.1063/5.0016163

Cited by 64 publications

(71 citation statements)

References 225 publications

(304 reference statements)

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“…We speculate that appropriately balanced vacant and occupied Li + coordinating sites are realized in samples lithiated with 1.5 equiv of Li + per macrocycle, leading to the observed peak in conductivity. 20,[41][42] This is consistent with previous reports that demonstrate optimal ionic conductivity upon establishing a [O]: [Li + ] ratio of 6 in triethylene glycol-based electrolytes. [43][44] Variable temperature EIS on lithiated STEG-NTs (1.5 equiv) demonstrated Arrhenius behavior with an activation energy (Ea) of 0.42 eV (Figures 4D and 4E), which is significantly lower than that of a framework material with similar functionality (0.87 eV).…”

Section: Resultssupporting

confidence: 91%

Lithium-Conducting Self-Assembled Organic Nanotubes

Strauss¹,

Hwang²,

Evans³

et al. 2021

Preprint

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Supramolecular polymers are compelling platforms for the design of stimuli-responsive materials with emergent functions. Here, we report the assembly of an amphiphilic nanotube for Li-ion conduction that exhibits high ionic conductivity, mechanical integrity, electrochemical stability, and solution processability. Imine condensation of a pyridine-containing diamine with a triethylene glycol functionalized isophthalaldehyde yields pore-functionalized macrocycles. Atomic force microscopy, scanning electron microscopy, and in solvo X-ray diffraction reveal that macrocycle protonation under their mild synthetic conditions drives assembly into high-aspect ratio (>103) nanotubes with three interior triethylene glycol groups. Electrochemical impedance spectroscopy demonstrates that lithiated nanotubes are efficient Li+ conductors, with an activation energy of 0.42 eV and a peak room temperature conductivity of 3.91 × 10-5 S cm-1. 7Li NMR and Raman spectroscopy demonstrate that lithiation occurs exclusively within the nanotube interior and implicates the glycol groups in facilitating efficient Li+ transduction. Linear sweep voltammetry and galvanostatic lithium plating-stripping tests reveal that this nanotube-based electrolyte is stable over a wide potential range and supports long-term cyclability. These findings demonstrate how coupling synthetic design and supramolecular structural control can yield high-performance ionic transporters that are amenable to device relevant fabrication. More broadly, these results demonstrate the technological potential of chemically designed self-assembled nanotubes.

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Section: Resultssupporting

confidence: 91%

Lithium-Conducting Self-Assembled Organic Nanotubes

Strauss¹,

Hwang²,

Evans³

et al. 2021

Preprint

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“…Research on proton-conducting solid polymer electrolytes (SPEs) over the past few decades has aimed to provide high-performance and stable electrochemical devices, such as electrochemical double-layer capacitors, light-emitting electrochemical cells, solid-state batteries, and fuel cells [1][2][3]. The proton transport in SPEs can be designated based on three mechanisms: hopping, diffusion, and transport associated with polymer chain segmental movement [4]. The ion hopping mechanism and ion transport by segmental motions are more favored at higher temperatures [5].…”

Section: Introductionmentioning

confidence: 99%

Effect of ZnO Nanoparticle Content on the Structural and Ionic Transport Parameters of Polyvinyl Alcohol Based Proton-Conducting Polymer Electrolyte Membranes

et al. 2021

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Proton conducting nanocomposite solid polymer electrolytes (NSPEs) based on polyvinyl alcohol/ammonium nitrate (PVA/NH4NO3) and different contents of zinc oxide nanoparticles (ZnO-NPs) have been prepared using the casting solution method. The XRD analysis revealed that the sample with 2 wt.% ZnO-NPs has a high amorphous content. The ionic conductivity analysis for the prepared membranes has been carried out over a wide range of frequencies at varying temperatures. Impedance analysis shows that sample with 2 wt.% ZnO-NPs has a smaller bulk resistance compared to that of undoped polymer electrolyte. A small amount of ZnO-NPs was found to enhance the proton-conduction significantly; the highest obtainable room-temperature ionic conductivity was 4.71 × 10−4 S/cm. The effect of ZnO-NP content on the transport parameters of the prepared proton-conducting NSPEs was investigated using the Rice–Roth model; the results reveal that the increase in ionic conductivity is due to an increment in the number of proton ions and their mobility.

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“…The mechanism of ionic conductivity would be what is often referred to as "vehicular motion" in electrolytes. [30] Charge hopping (of Li þ ) from these ionic structures is not likely as it would require leaving behind an anion with highly localized charge.…”

Section: Resultsmentioning

confidence: 99%

Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li

Liu

Counihan

Zhu

et al. 2021

Adv Energy and Sustain Res

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One of the most important technological advances in sustainable energy harvesting and storage is the development of the Liion battery technology. In recent years, increasing demand for energy has revived development of sustainable storage technologies with Li metal as the anode due to the high theoretical specific capacity of Li metal (3860 mA h g À1 ). [1][2][3][4] As a result, the focus of much research in the field of Li energy storage is centered on development of solid electrolyte materials that can replace flammable organic solvents and enable the use of Li metal anodes, required for high energy density batteries. [5,6] To fully implement solid-solid Li-ion technology, many challenges need to be resolved, namely the stability of electrode materials and electrolytes and selectivity of electrochemical interfaces. [7] Addressing these will minimize undesired side reactions at electrode surfaces and suppress Li dendrite formation on the anode to improve battery performance and lifetime.Polyethylene oxide (PEO), in particular, has attracted great interest as a polymer electrolyte for use in solid state Li batteries due to its low glass transition temperature (%À60 C), mechanical properties, low material cost, and good interfacial contact with the anode. [8][9][10] However, the ionic conductivity of pure PEO at room temperature is %10 À9 -10 À8 S cm À1 , five orders of magnitude lower than the practical threshold (10 À3 S cm À1 ) needed to achieve realistic charge-discharge rates. [11] This necessitates further doping with salts, e.g., LiTFSI. Even then, the best room temperature conductivity of simple LiTFSI-doped PEO is around 10 À5 S cm À1 , so high temperatures (≥60 C) are required to achieve sufficient ionic conductivity.When mixed with lithium salts, ether oxygens in the PEO backbone coordinate to Li þ , leading to salt dissociation and mobile charge carriers in the mixture. [12] The introduction of salt also suppresses polymer crystallization, leading to more amorphous content within PEO, which also improves conductivity. [9] However, the anion greatly contributes to the increased ionic conductivity of doped PEO. Strong coordination between ether oxygens and Li þ cations leads to low lithium transference

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Ion transport in small-molecule and polymer electrolytes

Cited by 64 publications

References 225 publications

Lithium-Conducting Self-Assembled Organic Nanotubes

Lithium-Conducting Self-Assembled Organic Nanotubes

Effect of ZnO Nanoparticle Content on the Structural and Ionic Transport Parameters of Polyvinyl Alcohol Based Proton-Conducting Polymer Electrolyte Membranes

Increasing Ionic Conductivity of Poly(ethylene oxide) by Reaction with Metallic Li

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