Heterogeneous Doping of a Weak Covalent Electrolyte: Proton Conductivity Enhancement of Imidazole by Admixture of Oxide Particles

Beyazyildirim, Seniz; Kreuer, Klaus‐Dieter; Schuster, Michael; Bhattacharyya, Aninda J.; Maier, Joachim

doi:10.1002/adma.200701823

Cited by 29 publications

(25 citation statements)

References 14 publications

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“…Simultaneously, work by Kumar and Rodrigues 52 was published on (LiBF 4 + ethylene carbonate/propylene carbonate) doped with BaTiO 3 and Al 2 O 3 with, however, very weak conductivity effects. In this context also the later work of Beyazyildirim et al 53 is worth mentioning in which anion adsorption (imidazolate) at the surfaces of acidic oxides (TiO 2 , ZrO 2 ) led to increased proton conductivity of pure imidazolium. While in this case the ground state is the undissociated liquid, it is the undissociated ion pair in the solvent that is broken in the soggy-sand electrolytes.…”

Section: Introductionmentioning

confidence: 88%

Soggy-sand electrolytes: status and perspectives

Pfaffenhuber

Göbel

Popović

et al. 2013

Phys. Chem. Chem. Phys.

103

126

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Soggy-sand electrolytes (solid-liquid composites, typically gel electrolytes, with synergistic electrical properties) are reviewed as far as status and perspectives are concerned. Major emphasis is put on the understanding of the local mechanism as well as the long-range transport along the filler network. The beneficial property spectrum includes enhanced conductivity of one ion type and decreased conductivity of the counter ion, but also the exciting mechanical properties of the solid-liquid composites. Inherent but not insurmountable problems lie in the reproducibility and stationarity of the composites microstructure and morphology. Owing to the huge parameter complexity and hence to the multitude of adjusting screws, there are various strategies for materials optimization. The technological relevance is enormous, in particular for battery electrolytes as here all the above-mentioned electrical and mechanical benefits are welcome. The soggy-sand electrolytes combine high Li(+) conductivity, low anion conductivity and good wettability of electrode particles with the mechanical stability of semi-solids.

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Section: Introductionmentioning

confidence: 88%

Soggy-sand electrolytes: status and perspectives

Pfaffenhuber

Göbel

Popović

et al. 2013

Phys. Chem. Chem. Phys.

103

126

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“…Several models to explain such an interaction, all of which relying on electrostatic interactions between the surface of the particles and the various anionic or ionic species present in the polymer electrolyte have been put forward. In the Maier model [36][37][38][39][40][41], these adsorptive or desorptive interactions entail an increase of one ion species in the space charge layer in the interfacial regions of electrolyte and particle [41,42]. The electrostatic interactions between the ionic species and the particle surface may as well be viewed as Lewis acid/base interactions [43][44][45][46][47][48].…”

Section: Nanocompositesmentioning

confidence: 99%

Local Li Cation Coordination and Dynamics in Novel Solid Electrolytes

Wüllen¹,

Echelmeyer

Voigt

et al. 2010

Zeitschrift Für Physikalische Chemie

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Ionic TransportResearch on solid ionic conductors for use as electrolytes in all solid state batteries still constitutes a rather vivid branch of today's materials science. Despite enormous efforts, neither the development of a solid electrolyte fulfilling the key requirements such as mechanical stability and high ionic conductivity at ambient temperature has been successful nor has an extended understanding of the local Li coordination motifs in the often amorphous systems been obtained. In this contribution, recent progress both in the development of novel solid state electrolytes with high ionic conductivity and mechanical stability and in the characterization of the local Li coordination motifs in these electrolytes from our laboratory is presented. The work was performed as a project within the framework of the Collaborative Research Centre SFB 458 "Ionic Motion in Materials with Disordered Structures -From Elementary Steps to Macroscopic Transport". Results will be given for polymer electrolytes based on polyethylene oxide (PEO), polyphosphazene (PPZ) and polyacrylonitrile (PAN) with various Li salts, nano-composites of these polymer electrolytes and Al 2 O 3 as a ceramic filler, novel inorganic/organic hybrid electrolytes, in which a mixture of an ionic liquid and Li salt is confined within the pore system of a SiO 2 glass, and a crystalline electrolyte, Li 5 La 3 Nb 2 O 12 . Employing a range of advanced solid state NMR methodologies including dipolar based NMR techniques and pulsed field gradient (PFG) NMR and impedance spectroscopy we were able to obtain a detailed knowledge about the local Li cation coordination motifs and the mechanism of Li transport in these electrolytes. Especially the hybrid electrolytes and the salt rich PAN based polymer electrolytes were identified as rather promising materials which combine a high ionic conductivity and mechanical stability.

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“…Liquid–solid composites have also been investigated. Addition of the surface‐acidic oxides TiO 2 or sulfated ZrO 2 to liquid imidazole resulted in adsorption of the imidazolate anion accompanied by generation of free protons in the space charge zones 7. In all these cases, the undissociated ground state (regular ions or undissociated molecule) is broken up.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Investigations of Polyethylene Glycol‐Based “Soggy Sand” Electrolytes – From the Local Mechanism to the Overall Conduction

Jarosik

Pfaffenhuber

Bunde

et al. 2011

Adv Funct Materials

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Using the example of SiO 2 dispersions in LiClO 4 /polyethylene glycol electrolytes, the conduction mechanism of "soggy sand" electrolytes is discussed. The study is essentially based on zeta potential, impedance and transference number measurements as well as on modeling. All the results can be explained by anion adsorption by the oxide particles and increased concentration of free Li + in the double layer. The initially colloidal dispersion quickly forms fractal networks by cluster-cluster aggregation. Once they percolate, an interfacially dominated Li + conductance is observed. The subsequent coarsening of the network is self-decelerating leading to a steady state conductivity that is, for low volume fractions, enhanced compared to SiO 2 free electrolytes. At higher values, blocking and inhomogeneity effects (e.g., salt trapping) lead to decreased values of the overall conductivity.

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Heterogeneous Doping of a Weak Covalent Electrolyte: Proton Conductivity Enhancement of Imidazole by Admixture of Oxide Particles

Cited by 29 publications

References 14 publications

Soggy-sand electrolytes: status and perspectives

Soggy-sand electrolytes: status and perspectives

Local Li Cation Coordination and Dynamics in Novel Solid Electrolytes

Electrochemical Investigations of Polyethylene Glycol‐Based “Soggy Sand” Electrolytes – From the Local Mechanism to the Overall Conduction

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