Relevance of solid electrolytes for lithium-based batteries: A realistic view

Lotsch, Bettina V.; Maier, Joachim

doi:10.1007/s10832-017-0091-0

Cited by 107 publications

(105 citation statements)

References 92 publications

(98 reference statements)

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“…In batteries and supercapacitors, liquid electrolytes are typically utilized, whereas fuel cells often use proton conducting or oxide‐ion conducting solid electrolytes . However, due to safety concerns, research efforts are now also aimed to building all‐solid‐state batteries and supercapacitors using solid electrolytes . As such, a thorough understanding of mass and charge transport in both solid and liquid electrolytes is of great importance and may have large implications in the development and optimization of novel energy storage and conversion devices.…”

Section: Introductionmentioning

confidence: 99%

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

2019

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Solid and liquid electrolytes for electrochemical energy storage and conversion cells, such as batteries, supercapacitors and fuel cells, contain often high concentrations of mobile ions. Therefore, the ion dynamics in these electrolytes is characterized by pronounced directional correlations between successive ion movements, which exert a strong influence on charge and mass transport. In this manuscript, we review the relevant transport properties of (i) single-ion conducting solid electrolytes and of (ii) liquid electrolytes with a single type of cations and a single type of anions. All transport quantities are based on Onsager's linear irreversible thermodynamics and are defined in the laboratory frame of reference, so that they can be easily related to correlations functions of the equilibrium ion dynamics by means of linear response theory. In the case of single-cation conducting solid electrolytes, we discuss how the complex interplay between cation-cation and cation-lattice interactions leads to a competition between cation self-correlations and distinct-cation correlations. In the case of liquid electrolytes, we describe how cation-cation, anion-anion, and cation-anions correlations influence the various transport quantities, such as total ionic conductivity, Haven ratio, salt diffusion coefficient and cation transference numbers. Moreover, we discuss how, in dilute liquid electrolytes, ion correlations can be governed by ion pair formation. Finally, the competition between cation/ anion and cation/polymer chain interactions can lead to negative cation transference numbers in polymer electrolytes, i. e. to cations migrating towards the positive electrode. Taken together, these case studies showcase how ion correlations in electrolyte systems can strongly influence the overall efficiency of energy storage and conversion devices due to transport limitations.[a] Dr.

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Section: Introductionmentioning

confidence: 99%

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

2019

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“…Fast lithium and sodium ion conductors composed of earth abundant elements as potential components of all solid‐state batteries attract immense interest . Recently, several phosphidosilicates with isolated or condensed SiP 4 tetrahedra have demonstrated lithium or sodium ion conductivity, for example Li 8 SiP 4 , Li 2 SiP 2 ,, LiSi 2 P 3 , and the series Na 23 Si 9 n +19 P 12 n +33 ( n = 0–3) .…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Structure of the Sodium Phosphidosilicate Na₂SiP₂

et al. 2020

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Ion conductors of light alkaline metals based on earth‐abundant elements are important components for all‐solid‐state batteries. The new sodium‐rich phosphidosilicate Na2SiP2 was synthesized by solid state reaction of stoichiometric amounts of the elements at 973 K and characterized by single‐crystal X‐ray diffraction (space group Pccn (no. 56), a = 12.7929(5) Å, b = 22.3109(9) Å, c = 6.0522(2) Å and Z = 16) and solid‐state NMR under MAS conditions. The compound forms dark‐red twinned crystals, and its crystal structure contains edge‐sharing SiP4 tetrahedra connected to infinite ∞1[SiP4/2] chains. The sodium ions between the chains are fairly mobile. Electrochemical impedance spectroscopy shows a total ionic conductivity of σ(Na+, 373 K) = 2.3 ? 10–6 Scm–1 with an activation energy of Ea = 0.43 eV, and the galvanostatic polarization reveals mixed conduction behavior with a transference number of 0.8.

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“…Solid state ion conductors are very promising candidates to replace current state‐of‐the‐art liquid electrolytes in next generation all‐solid‐state batteries (ASSB). The challenges involved with their application in all‐solid‐state batteries (ASSB) as well as recent progress in the field are summarized in a number of excellent publications and reviews …”

Section: Figurementioning

confidence: 99%

Stabilization of Highly Conductive Lithium Argyrodites by Means of Lithium Substitution: The Case of Li₆Fe_0.5PS₆

Schneider

Sedlmaier

et al. 2019

ChemistrySelect

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All‐solid‐state‐batteries (ASSB) are promising candidates for next generation lithium batteries providing high energy density and safety levels. Their success crucially depends on the properties of the available solid electrolyte materials, ideally offering sufficient conductivities in combination with stability against decomposition over a large electrochemical window. Therefore, the search for solid electrolytes with novel compositions remains of high interest. In this work we present a strategy to stabilize highly conductive lithium argyrodites by means of lithium substitution. This is different from the previously described possibilities to obtain stable structures by either substituting phosphorous or sulfide anions in the parent compound Li7PS6. This approach offers access to a new array of solid electrolyte candidates with an argyrodite‐type crystal structure. Conductivities of up to 1.4⋅10−4 S/cm can be obtained for Fe‐substituted materials of general composition Li7‐2xFexPS6.

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Relevance of solid electrolytes for lithium-based batteries: A realistic view

Cited by 107 publications

References 92 publications

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

Synthesis and Structure of the Sodium Phosphidosilicate Na₂SiP₂

Stabilization of Highly Conductive Lithium Argyrodites by Means of Lithium Substitution: The Case of Li₆Fe_0.5PS₆

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Relevance of solid electrolytes for lithium-based batteries: A realistic view

Cited by 107 publications

References 92 publications

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

Dynamic Ion Correlations in Solid and Liquid Electrolytes: How Do They Affect Charge and Mass Transport?

Synthesis and Structure of the Sodium Phosphidosilicate Na2SiP2

Stabilization of Highly Conductive Lithium Argyrodites by Means of Lithium Substitution: The Case of Li6Fe0.5PS6

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Synthesis and Structure of the Sodium Phosphidosilicate Na₂SiP₂

Stabilization of Highly Conductive Lithium Argyrodites by Means of Lithium Substitution: The Case of Li₆Fe_0.5PS₆