Enhanced ion conduction by enforcing structural disorder in Li-deficient argyrodites Li6−xPS5−xCl1+x

Feng, Xuyong; Chien, Po‐Hsiu; Wang, Yan; Patel, Sawankumar; Wang, Pengbo; Liu, Haoyu; Immediato‐Scuotto, Marcello; Hu, Yan‐Yan

doi:10.1016/j.ensm.2020.04.042

Cited by 103 publications

(137 citation statements)

References 25 publications

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“…Zhang et al [205] reported the inter-and intracycle interfacial evolution of a LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NMC)|Li 6 PS 5 Cl|Li cell using impedance measurements, Raman spectroscopy, and scanning electron microscopy (SEM) studies. Furthermore, Zhou et al [206] studied the Li 6 PS 5 X (X = Cl, Br, I) and Li 6−y PS 5−y Cl 1+y argyrodites, while Feng et al [207] investigated Li 6−x PS 5−x Cl 1+x . Recently, Arnold et al [208] reported an improved conductivity of 0.53 × 10 −3 S cm −1 at RT for Li 6 PS 5 Cl doped with LiCl and they showed the enhanced electrochemical properties with cells assembled with Li||LTO (Li 4 Ti 5 O 12 ) using bare and doped electrolyte.…”

Section: Argyrodite Electrolytesmentioning

confidence: 99%

“…Owing to their high Li + ion conductivity at room temperature, sulfide-based materials are more promising electrolytes than oxide-based ones [ 159 , 160 , 161 , 162 , 163 , 164 , 165 , 166 , 167 , 168 , 169 , 170 , 171 , 172 , 173 , 174 , 175 , 176 , 177 , 178 , 179 , 180 , 181 , 182 , 183 , 184 , 185 , 186 , 187 , 188 , 189 , 190 , 191 , 192 , 193 , 194 , 195 , 196 , 197 , 198 , 199 , 200 , 201 , 202 , 203 , 204 , 205 , 206 , 207 , 208 ,…”

Section: Sulfide Solid Electrolytesmentioning

confidence: 99%

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Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

et al. 2020

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Energy storage materials are finding increasing applications in our daily lives, for devices such as mobile phones and electric vehicles. Current commercial batteries use flammable liquid electrolytes, which are unsafe, toxic, and environmentally unfriendly with low chemical stability. Recently, solid electrolytes have been extensively studied as alternative electrolytes to address these shortcomings. Herein, we report the early history, synthesis and characterization, mechanical properties, and Li+ ion transport mechanisms of inorganic sulfide and oxide electrolytes. Furthermore, we highlight the importance of the fabrication technology and experimental conditions, such as the effects of pressure and operating parameters, on the electrochemical performance of all-solid-state Li batteries. In particular, we emphasize promising electrolyte systems based on sulfides and argyrodites, such as LiPS5Cl and β-Li3PS4, oxide electrolytes, bare and doped Li7La3Zr2O12 garnet, NASICON-type structures, and perovskite electrolyte materials. Moreover, we discuss the present and future challenges that all-solid-state batteries face for large-scale industrial applications.

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Section: Argyrodite Electrolytesmentioning

confidence: 99%

Section: Sulfide Solid Electrolytesmentioning

confidence: 99%

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

et al. 2020

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“…[17][18][19][20][21][22][23] The synthetic Li6PS5X lithiumargyrodites are derived by replacing silver with lithium and substituting one chalcogen per formula unit with a halide ion. A large number of lithium-argyrodite compositions have previously been synthesized, [24][25][26][27][28][29][30][31] with some of the highest room temperature ionic conductivities reported for the Li6+xP1-xGexS5I and Li6+xSb1-xSixS5I series. 32,33 This classification follows the nomenclature proposed by Deiseroth et al with symmetry labels referring to the inverted setting 2.…”

Section: Introductionmentioning

confidence: 99%

“…(anion-ordered) is a poor Li-ion conductor compared to Li6PS5Cl and Li6PS5Br (both aniondisordered), which exhibit ×10 3 higher room-temperature ionic conductivities. 9,13,[38][39][40] While the correlation between anion disorder and fast lithium transport is well documented, 9,[24][25][26][27][28][29][30][31][32][33]36,41 the effect of anion site-disorder on the microscopic dynamics and local structure of the mobile lithium ions is less well understood. In Li6PS5X argyrodites, the anionic framework contains 132 tetrahedral voids per unit cell (4 formula units) that may accommodate the corresponding 24 lithium ions.…”

Section: Introductionmentioning

confidence: 99%

“…39 This three-jump model, in which the lithium diffusion mechanism is described entirely in terms of movement between type 5 sites, has been widely applied to explain experimental and theoretical trends in lithium transport in Li6PS5X and related lithium-argyrodites. 9,[24][25][26][27][28][29][30][31][32]41,43 This model, however, ignores the role of non-type 5 tetrahedra, and therefore gives an incomplete description of the lithium diffusion pathways in the argyrodite structure. The type 5 tetrahedra form face-sharing pairs, and pure 5 → 5 lithium motion is only possible for the doublet jump.…”

Section: Introductionmentioning

confidence: 99%

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On the Local Charge Inhomogeneity and Lithium Distribution in the Superionic Argyrodites Li6PS5X (X = Cl, Br, I)

Minafra¹,

Kraft²,

Bernges³

et al. 2020

Preprint

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The lithium-argyrodites Li6PS5X (X = Cl, Br, I) exhibit high lithium-ion conductivities, making them promising candidates for use in solid-state batteries. These solid electrolytes can show considerable substitutional X−/S2− anion-disorder, with greater disorder typically correlated with higher lithium-ion conductivities. The atomic-scale effects of this anion site-disorder within the host lattice—in particular how lattice disorder modulates the lithium substructure—are not well understood. Here, we characterize the lithium substructure in Li6PS5X (X = Cl, Br, I) as a function of temperature and anion site-disorder, using Rietveld refinements against temperature-dependent neutron diffraction data. Analysis of these high-resolution diffraction data reveals an additional lithium position previously unreported for Li6PS5Xargyrodites, suggesting that the lithium conduction pathway in these materials differs from the most common model proposed in earlier studies. Analysis of the Li+ positions and their radial distributions reveals that greater inhomogeneityof the local anionic charge, due to X−/S2− site-disorder, is associated with more spatially-diffuse lithium distributions. This observed coupling of site-disorder and lithium distribution provides a possible explanation for the enhanced lithium transport in anion-disordered lithium argyrodites, and highlights the complex interplay between anion configuration and lithium substructure in this family of superionic conductors.

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Revealing the Impact of Cl Substitution on the Crystallization Behavior and Interfacial Stability of Superionic Lithium Argyrodites

Liu

Zhong

et al. 2022

Adv Funct Materials

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All-solid-state batteries are believed to be the next-generation energy storage device that can meet the ever-growing market demand for high energy density and safety. The ionic conductivity and electrochemical stability of the solid electrolyte are two crucial properties that can affect battery performance. Herein, with an optimized crystallization process, the Cl-rich argyrodite possesses high ionic conductivity, good dendrite inhibition capability, as well as enhanced interfacial stability against decomposition. Ab initio molecular dynamics simulation and radial distribution function analysis are utilized to probe into the interfacial phenomenon between argyrodite electrolyte and lithium metal. LiNi 0.8 Co 0.1 Mn 0.1 O 2 -based all-solid-state battery using the Cl-rich argyrodite electrolyte also delivers more stable cyclic performance. This study shows the multiple enhancements of argyrodite electrolyte brought by Cl doping, which provides important guidance in selecting electrolytes for all-solid-state batteries.

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Enhanced ion conduction by enforcing structural disorder in Li-deficient argyrodites Li6−xPS5−xCl1+x

Cited by 103 publications

References 25 publications

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

On the Local Charge Inhomogeneity and Lithium Distribution in the Superionic Argyrodites Li6PS5X (X = Cl, Br, I)

Revealing the Impact of Cl Substitution on the Crystallization Behavior and Interfacial Stability of Superionic Lithium Argyrodites

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