Matches in SemOpenAlex for { <https://semopenalex.org/work/W3202314816> ?p ?o ?g. }
Showing items 1 to 74 of
74
with 100 items per page.
- W3202314816 abstract "The rational development of fast–ion-conducting solid electrolytes for all-solid-state lithium-ion batteries requires understanding the key structural and chemical principles that give some materials their exceptional ionic conductivities. For the lithium argyrodites Li 6 PS 5 X ( X = Cl,Br,I), the choice of the halide, X , strongly affects the ionic conductivity, with room-temperature ionic conductivities for X = {Cl, Br} ×10 3 higher than for X = I. This variation has been attributed to differing degrees of S/ X anion disorder. For X = {Cl, Br} the S/ X anions are substitutionally disordered, while for X = I the anion sublattice is fully ordered. To better understand the role of substitutional anion disorder in enabling fast lithium-ion transport, we have performed a first-principles molecular dynamics study of Li 6 PS 5 I and Li 6 PS 5 Cl, with varying amounts of S/ X anion-site disorder. Considering the S/ X substructure as a tetrahedrally close-packed lattice, we identify three partially occupied lithium sites that form a contiguous three-dimensional network of face-sharing tetrahedra. The active lithium-ion diffusion pathways within this network, however, depend on the S/ X anion configuration. For anion-disordered systems, the active site–site pathways give a percolating three-dimensional diffusion network; whereas for anion-ordered systems, critical site–site pathways are inactive, giving a disconnected diffusion network with lithium motion restricted to local orbits around S positions. Analysis of the lithium substructure and dynamics in terms of the lithium coordination around each sulfur site shows a mechanistic link between substitutional anion disorder and lithium disorder, which enables fast lithium diffusion. In anion-ordered systems the Li-ions are pseudo-ordered, with preferential 6-fold coordination of sulfur sites. Long-ranged lithium diffusion disrupts this SLi 6 pseudo-ordering, and is therefore disfavoured. In anion-disordered systems, a uniform 6-fold S–Li coordination is frustrated due to Li–Li Coulombic repulsion. Lithium positions become disordered, giving a range of S–Li coordination environments. Long-ranged Li diffusion is now possible with no net change in S–Li coordination numbers. This gives rise to superionic lithium transport in the anion-disordered systems, which is effected by a concerted string-like diffusion mechanism." @default.
- W3202314816 created "2021-10-11" @default.
- W3202314816 creator A5070797735 @default.
- W3202314816 date "2021-02-11" @default.
- W3202314816 modified "2023-10-14" @default.
- W3202314816 title "Mechanistic Origin of Superionic Lithium Diffusion in Anion-Disordered Li6PS5X Argyrodites" @default.
- W3202314816 doi "https://doi.org/10.26434/chemrxiv.12349703.v3" @default.
- W3202314816 hasPublicationYear "2021" @default.
- W3202314816 type Work @default.
- W3202314816 sameAs 3202314816 @default.
- W3202314816 citedByCount "0" @default.
- W3202314816 crossrefType "posted-content" @default.
- W3202314816 hasAuthorship W3202314816A5070797735 @default.
- W3202314816 hasBestOaLocation W32023148161 @default.
- W3202314816 hasConcept C109883240 @default.
- W3202314816 hasConcept C121332964 @default.
- W3202314816 hasConcept C127413603 @default.
- W3202314816 hasConcept C134018914 @default.
- W3202314816 hasConcept C138679309 @default.
- W3202314816 hasConcept C145148216 @default.
- W3202314816 hasConcept C147789679 @default.
- W3202314816 hasConcept C159467904 @default.
- W3202314816 hasConcept C17525397 @default.
- W3202314816 hasConcept C178790620 @default.
- W3202314816 hasConcept C179104552 @default.
- W3202314816 hasConcept C185592680 @default.
- W3202314816 hasConcept C2182769 @default.
- W3202314816 hasConcept C2778541603 @default.
- W3202314816 hasConcept C66938386 @default.
- W3202314816 hasConcept C68801617 @default.
- W3202314816 hasConcept C69357855 @default.
- W3202314816 hasConcept C71924100 @default.
- W3202314816 hasConcept C8010536 @default.
- W3202314816 hasConcept C97355855 @default.
- W3202314816 hasConcept C99679407 @default.
- W3202314816 hasConceptScore W3202314816C109883240 @default.
- W3202314816 hasConceptScore W3202314816C121332964 @default.
- W3202314816 hasConceptScore W3202314816C127413603 @default.
- W3202314816 hasConceptScore W3202314816C134018914 @default.
- W3202314816 hasConceptScore W3202314816C138679309 @default.
- W3202314816 hasConceptScore W3202314816C145148216 @default.
- W3202314816 hasConceptScore W3202314816C147789679 @default.
- W3202314816 hasConceptScore W3202314816C159467904 @default.
- W3202314816 hasConceptScore W3202314816C17525397 @default.
- W3202314816 hasConceptScore W3202314816C178790620 @default.
- W3202314816 hasConceptScore W3202314816C179104552 @default.
- W3202314816 hasConceptScore W3202314816C185592680 @default.
- W3202314816 hasConceptScore W3202314816C2182769 @default.
- W3202314816 hasConceptScore W3202314816C2778541603 @default.
- W3202314816 hasConceptScore W3202314816C66938386 @default.
- W3202314816 hasConceptScore W3202314816C68801617 @default.
- W3202314816 hasConceptScore W3202314816C69357855 @default.
- W3202314816 hasConceptScore W3202314816C71924100 @default.
- W3202314816 hasConceptScore W3202314816C8010536 @default.
- W3202314816 hasConceptScore W3202314816C97355855 @default.
- W3202314816 hasConceptScore W3202314816C99679407 @default.
- W3202314816 hasLocation W32023148161 @default.
- W3202314816 hasLocation W32023148162 @default.
- W3202314816 hasOpenAccess W3202314816 @default.
- W3202314816 hasPrimaryLocation W32023148161 @default.
- W3202314816 hasRelatedWork W1981868170 @default.
- W3202314816 hasRelatedWork W2008380130 @default.
- W3202314816 hasRelatedWork W2095365526 @default.
- W3202314816 hasRelatedWork W2250550751 @default.
- W3202314816 hasRelatedWork W2949726110 @default.
- W3202314816 hasRelatedWork W3039994028 @default.
- W3202314816 hasRelatedWork W3093008345 @default.
- W3202314816 hasRelatedWork W3115899579 @default.
- W3202314816 hasRelatedWork W4230026538 @default.
- W3202314816 hasRelatedWork W4281786392 @default.
- W3202314816 isParatext "false" @default.
- W3202314816 isRetracted "false" @default.
- W3202314816 magId "3202314816" @default.
- W3202314816 workType "article" @default.