Heterogeneously doped polyethylene glycol as nano-composite soft matter electrolyte

Jarosik, Anna; Hore, Sarminala; Kaskhedikar, N.; Pfaffenhuber, Christian; Maier, Joachim

doi:10.1016/j.electacta.2011.05.063

Cited by 17 publications

(50 citation statements)

References 61 publications

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“…5,6 To be precise, these oligomeric molecules are partly or fully CH 3 -terminated. We used PEG-150 (i.e.…”

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confidence: 99%

“…6 These phenomena find their explanations in the coarsening kinetics. Here we are not referring to the local mechanism of conductivity enhancement, 5 which we believe is the Heterogeneous Doping mechanism, 12 i.e. anion adsorption at the SiO 2 surfaces leading to breaking up ion pairs, thus increasing the concentration of free Li ions and hence the Li + surface conductivity.…”

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confidence: 99%

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Ion conducting particle networks in liquids: modeling of network percolation and stability

Jarosik

Traub

Maier

et al. 2011

Phys. Chem. Chem. Phys.

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Networks of inorganic particles (here SiO 2 ) formed within organic liquids play an important role in science. Recently they have been considered as 'soggy sand' electrolytes for Li-based batteries with a fascinating combination of mechanical and electrical properties. In this communication we model formation and stability of the networks by Cluster-Cluster Aggregation followed by coarsening on a different time scale. The comparison of computer simulations based on our model with experimental results obtained for LiClO 4 containing polyethylene glycol reveals (i) that the percolation threshold for interfacial conductivity is very small, (ii) that the networks once formed coarsen with a time constant that is roughly independent of volume fraction and size-to a denser aggregate which then stays stable under operating condition. (iii) Trapping of the conducting solvent at high packing is also revealed.Coherent networks of solids in liquids play an important role in colloid chemistry and physics and have a broad range of technological applications. Perhaps the most popular examples are dispersion paints that consist of inorganic particles dispersed in appropriate liquids. When a shear stress is applied, the network of the particles breaks up, and as a result the overall viscosity decreases. This thixotropy is beneficial for the process of painting. Brushing exerts shear stress and the resulting thinning facilitates applying the paint. Other examples are gels in which-unlike sols-colloidal particles form percolating networks.Here we will focus on the recently discovered ''soggy sand'' electrolytes in which by admixing fine insulating particles to salt containing liquids the overall ionic conductivity is pronouncedly increased.

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“…5,6 To be precise, these oligomeric molecules are partly or fully CH 3 -terminated. We used PEG-150 (i.e.…”

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confidence: 99%

mentioning

confidence: 99%

Ion conducting particle networks in liquids: modeling of network percolation and stability

Jarosik

Traub

Maier

et al. 2011

Phys. Chem. Chem. Phys.

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“…The ionic conductivity measurements is observed to have a one to one correlation with the measured effective Li + transference number ( ) versus silica volume fraction of freshly 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 free Li + ions [14]. heterogeneous doping [7], the effective measured transference number t eff can be expressed as t eff = ((1 -ϕ).t liquid σ liquid + ϕβσ sc t sc )/ ((1 -ϕ).σ liquid + ϕβσ sc )) [13,14] where t liquid= at ϕ= 0, σ liquid is the pure liquid ionic conductivity, β is the percolation efficiency, σ sc is the mean conductivity in the space charge layer and t sc is the transference number in the space charge layer.…”

Section: Vide Infra)mentioning

confidence: 85%

“…heterogeneous doping [7], the effective measured transference number t eff can be expressed as t eff = ((1 -ϕ).t liquid σ liquid + ϕβσ sc t sc )/ ((1 -ϕ).σ liquid + ϕβσ sc )) [13,14] where t liquid= at ϕ= 0, σ liquid is the pure liquid ionic conductivity, β is the percolation efficiency, σ sc is the mean conductivity in the space charge layer and t sc is the transference number in the space charge layer. On careful observation, Δσ≈ ϕβσ sc (σ eff = (1-ϕ)σ liquid + ϕβσ sc = (1-ϕ)σ liquid + Δσ; here σ eff = σ from figure 1) and assuming t sc = 1 (i.e.…”

Section: Vide Infra)mentioning

confidence: 99%

A Few Case Studies on the Correlation of Particle Network and Its Stability on the Ionic Conductivity of Solid–Liquid Composite Electrolytes

Santhosha

Bhattacharyya

2015

J. Phys. Chem. B

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We discuss here the crucial role of the particle network and its stability on the long-range ion transport in solid-liquid composite electrolytes. The solid-liquid composite electrolytes chosen for the study here comprise nanometer sized silica (SiO2) particles having various surface chemical functionalities dispersed in nonaqueous lithium salt solutions, viz. lithium perchlorate (LiClO4) in two different polyethylene glycol based solvents. These systems constitute representative examples of an independent class of soft matter electrolytes known as "soggy sand" electrolytes, which have tremendous potential in diverse electrochemical devices. The oxide additive acts as a heterogeneous dopant creating free charge carriers and enhancing the local ion transport. For long-range transport, however, a stable spanning particle network is needed. Systematic experimental investigations here reveal that the spatial and time dependent characteristics of the particle network in the liquid solution are nontrivial. The network characteristics are predominantly determined by the chemical makeup of the electrolyte components and the chemical interactions between them. It is noteworthy that in this study the steady state macroscopic ionic conductivity and viscosity of the solid-liquid composite electrolyte are observed to be greatly determined by the additive oxide surface chemical functionality, solvent chemical composition, and solvent dielectric constant.

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“…Electrochemical implications of ion pairing have been investigated in salt containing solid polyethylene oxide (PEO) electrolytes by Bruce [4,5] as well as more recently by Stolwijk et al [6][7][8], in oligoethers by Watanabe et al [9][10][11], and by Saito et al [12][13][14][15] employing electrophoretic NMR. This particular electrolyte (lithium salt containing poly(ethylene glycol) dimethyl ether) has been used for a variety of battery systems, most recently in Li-O 2 [16][17][18][19][20] and more generally as a component of "soggy sand" electrolytes [21][22][23][24][25].…”

Section: Introductionmentioning

confidence: 99%

Determination of individual contributions to the ionic conduction in liquid electrolytes: Case study of LiTf/PEGDME-150

Popović

Pfaffenhuber

Melchior

et al. 2015

Electrochemistry Communications

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Heterogeneously doped polyethylene glycol as nano-composite soft matter electrolyte

Cited by 17 publications

References 61 publications

Ion conducting particle networks in liquids: modeling of network percolation and stability

Ion conducting particle networks in liquids: modeling of network percolation and stability

A Few Case Studies on the Correlation of Particle Network and Its Stability on the Ionic Conductivity of Solid–Liquid Composite Electrolytes

Determination of individual contributions to the ionic conduction in liquid electrolytes: Case study of LiTf/PEGDME-150

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