2021
DOI: 10.1021/acsami.1c16515
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Subtle Local Structural Details Influence Ion Transport in Glassy Li+ Thiophosphate Solid Electrolytes

Abstract: Many of the promising, high-performing solid electrolytes for lithium-ion batteries are amorphous or contain an amorphous component, particularly in the Li thiophosphate Li 2 S-P 2 S 5 compositional series (LPS). An explicit study of the local structure in four samples of ostensibly identically-prepared 70Li 2 S-30P 2 S 5 glass reveals substantial variation in the ratio between the two main local structural units in this system: PS 4 3− tetrahedra and P 2 S 7 4− corner-sharing tetrahedral pairs. Local structur… Show more

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Cited by 6 publications
(8 citation statements)
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“…20−22 These studies have shown that there are significant differences in the local structures (polyatomic anion) as a function of the glass compositions but also more surprisingly that glasses of the same composition feature different contents of local structures. 23 These structural differences not only occur in LiPS glasses and glass-ceramics prepared by different methods (such as melt-quenching, mechanical ball-milling or heattreatment), but even in the case of different samples from the same preparation method. The mechanism of the formation and transformation of the different polyatomic anions in LiPS systems is therefore still not well understood.…”
mentioning
confidence: 99%
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“…20−22 These studies have shown that there are significant differences in the local structures (polyatomic anion) as a function of the glass compositions but also more surprisingly that glasses of the same composition feature different contents of local structures. 23 These structural differences not only occur in LiPS glasses and glass-ceramics prepared by different methods (such as melt-quenching, mechanical ball-milling or heattreatment), but even in the case of different samples from the same preparation method. The mechanism of the formation and transformation of the different polyatomic anions in LiPS systems is therefore still not well understood.…”
mentioning
confidence: 99%
“…Figure A shows these three structures, highlighting the presence of a P–P bond in the P 2 S 6 4– ( hypo -thiophosphate) cluster, the corner-sharing P 2 S 7 4– ( pyro -thiophosphate) tetrahedral pairs, and the PS 4 3– ( ortho -thiophosphate) tetrahedral cluster. The structure of LiPS glasses and glass-ceramics has been characterized by, e.g., Raman and 31 P nuclear magnetic resonance spectroscopy. These studies have shown that there are significant differences in the local structures (polyatomic anion) as a function of the glass compositions but also more surprisingly that glasses of the same composition feature different contents of local structures . These structural differences not only occur in LiPS glasses and glass-ceramics prepared by different methods (such as melt-quenching, mechanical ball-milling or heat-treatment), but even in the case of different samples from the same preparation method.…”
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confidence: 99%
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“…It seems that the Raman peaks between 400.0 and 440.0 cm –1 show a clear shift toward lower wavenumbers for the Li 3 PS 4 - x % LiI ( x = 40 and 50) electrolytes. XRD results confirm that the thio-LISICON II phases are detected in those compositions, indicating that the above shift is associated with the formation of the thio-LISICON II phase and the P 2 S 7 4– unit in the structure. , During this structure evolution, a part of the PS 4 3– tetrahedrons breaks away from the constraints of the crystal lattice and transforms into P 2 S 7 4– and P 2 S 6 4– during the vitrification process . As demonstrated in Figure c, the content of PS 4 3– tetrahedron units in the structure shows a clear decrease with the increasing LiI content at the beginning and then increases with further increase in the LiI content, reaching the lowest value for Li 3 PS 4 - x % LiI ( x = 50).…”
Section: Resultsmentioning
confidence: 52%
“…49,50 During this structure evolution, a part of the PS 4 3− tetrahedrons breaks away from the constraints of the crystal lattice and transforms into P 2 S 7 4− and P 2 S 6 4− during the vitrification process. 51 As demonstrated in Figure 1c, the content of PS 4…”
Section: ■ Results and Discussionmentioning
confidence: 82%