Hauptseite > Publikationsdatenbank > Understanding Lithium-Ion Transport in Selenophosphate-Based Lithium Argyrodites and Their Limitations in Solid-State Batteries > print

001     1008848
005     20240712113112.0
024 7 _ |a 10.1021/acs.chemmater.3c00658
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024 7 _ |a 0897-4756
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024 7 _ |a 1520-5002
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024 7 _ |a 10.34734/FZJ-2023-02508
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037 _ _ |a FZJ-2023-02508
082 _ _ |a 540
100 1 _ |a Hartel, Johannes
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245 _ _ |a Understanding Lithium-Ion Transport in Selenophosphate-Based Lithium Argyrodites and Their Limitations in Solid-State Batteries
260 _ _ |a Washington, DC
|c 2023
|b American Chemical Society
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520 _ _ |a To develop solid-state batteries with high power and energy densities, solid electrolytes with fast Li+ transport are required. Superionic lithium argyrodites have proven to be a versatile system, in which superior ionic conductivities can be achieved by elemental substitutions. Herein, we report the novel selenophosphate-based lithium argyrodites Li6–xPSe5–xBr1+x (0 ≤ x ≤ 0.2) exhibiting ionic conductivities up to 8.5 mS·cm–1 and uncover the origin of their fast Li+ transport. Rietveld refinement of neutron powder diffraction data reveals a better interconnection of the Li+ cages compared to the thiophosphate analogue Li6PS5Br, by the occupation of two additional Li+ sites, facilitating fast Li+ transport. Additionally, a larger unit cell volume, lattice softening, and higher structural disorder between halide and chalcogenide are unveiled. The application of Li5.85PSe4.85Br1.15 as the catholyte in In/LiIn|Li6PS5Br|LiNi0.83Co0.11Mn0.06O2:Li5.85PSe4.85Br1.15 solid-state batteries leads to severe degradation upon charging of the cell, revealing that selenophosphate-based lithium argyrodites are not suitable for applications in lithium nickel cobalt manganese oxide-based solid-state batteries from a performance perspective. This work further expands on the understanding of the structure–transport relationship in Li+ conducting argyrodites and re-emphasizes the necessity to consider chemical and electrochemical stability of solid electrolytes against the active materials when developing fast Li+ conductors.
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700 1 _ |a Banik, Ananya
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700 1 _ |a Gerdes, Josef Maximilian
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700 1 _ |a Wankmiller, Björn
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700 1 _ |a Helm, Bianca
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700 1 _ |a Li, Cheng
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700 1 _ |a Kraft, Marvin A.
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700 1 _ |a Hansen, Michael Ryan
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700 1 _ |a Zeier, Wolfgang G.
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773 _ _ |a 10.1021/acs.chemmater.3c00658
|g Vol. 35, no. 12, p. 4798 - 4809
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|t Chemistry of materials
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856 4 _ |u https://juser.fz-juelich.de/record/1008848/files/acs.chemmater.3c00658.pdf
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856 4 _ |y Published on 2023-06-12. Available in OpenAccess from 2024-06-12.
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