Origin of the Outstanding Performance of Dual Halide Doped Li7P2S8X (X = I, Br) Solid Electrolytes for All-Solid-State Lithium Batteries

Bui, Anh Dinh; Choi, Sunhwa; Choi, Hae-Young; Lee, You-Jin; Doh, Chil‐Hoon; Park, Jun‐Woo; Kim, Byung Gon; Lee, Won–Jae; Lee, Sang‐Min; Ha, Yoon‐Cheol

doi:10.1021/acsaem.0c02321

Cited by 38 publications

(20 citation statements)

References 30 publications

(64 reference statements)

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“…These phases possess similar atomic arrangements and space groups to those of LGPS and are thus categorized as derivatives of LGPS (i.e., LGPS-type phases). Examination of these XRD patterns reveals that the pattern of LPSBr resembles that reported for Li 7 P 2 S 8 Br 0.5 I 0.5 , , whereas the pattern of LPSI resembles those reported for (100– x )(0.8Li 2 S·0.2P 2 S 5 )· x LiI and 70Li 3 PS 4 –30LiI . These previous studies propose that the obtained XRD patterns may be attributed to δ -Li 3 PS 4 in the space group P 4 2 mc (no.…”

Section: Resultssupporting

confidence: 72%

“…Moreover, the ionic conductivities were determined at 300 K for the densified samples as this form is closer to representing the bulk conductivity than the compressed powder form. Ionic conductivities of 5.8(1) and 9.1(2) mS cm –1 are obtained for the LPSBr and LPSI samples, respectively, which are the highest values of those currently reported for solid electrolytes in the Li–P–S– X ( X = Br, I) system. ,,, …”

Section: Resultsmentioning

confidence: 66%

“…Ionic conductivities of 5.8(1) and 9.1(2) mS cm −1 are obtained for the LPSBr and LPSI samples, respectively, which are the highest values of those currently reported for solid electrolytes in the Li−P−S−X (X = Br, I) system. 30,36,37,43 3.6. All-Solid-State Li Cell.…”

Section: Resultsmentioning

confidence: 99%

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Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Song

Hori

et al. 2022

Chem. Mater.

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All-solid-state Li-metal batteries require fast Li-ion conductors that are compatible with Li-metal electrodes. Herein, we aim to obtain such Liion conductors in Li 2 S−P 2 S 5 −LiX (X = Br, I) systems, where new tetragonal phases with P4 2 /nmc symmetry were formed at compositions of Li 10 P 3 S 12 Br (LPSBr) and Li 10.25 P 3 S 12.25 I 0.75 (LPSI). Rietveld refinement analyses indicated that both materials were structural analogues of a renowned superionic conductor, Li 10 GeP 2 S 12 (LGPS), with additional anions at 2a or 4c sites within LPSBr or LPSI, respectively. The LPSBr and LPSI phases exhibited ionic conductivities of 5.8(1) and 9.1(2) mS cm −1 at 300 K, respectively, with the latter having the highest conductivity among the reported Li−P−S−X (X = Br or I) systems. All-solid-state Li metal cells were prepared using LPSBr or LPSI as the separator to compare their charge−discharge cycle performances with those previously reported for Li cells using separator electrolytes with various chemical compositions. The most stable cyclability was observed for the Li cell using LPSBr, which exhibited a high ionic conductivity and phase purity, indicating that these two properties of the solid electrolyte are important for ensuring extended cycling of all-solid-state Li-metal batteries.

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Section: Resultssupporting

confidence: 72%

Section: Resultsmentioning

confidence: 66%

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Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Song

Hori

et al. 2022

Chem. Mater.

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“…After 50 cycles, larger S 2p peaks related to the decomposition products, such as Li 2 S, Li 2 S n , and P 2 S x , resulting from the side reactions, were detected on the LPSCl surface for the full cell with the Li–metal anode. [ 43–45 ] However, contrary to the Li cell case, the SE in contact with In showed almost similar peak intensities and shapes to those of the pristine one (Figure 3b–d), validating the decent interfacial stability between In and LPSCl. These consistent results show that the improved interfacial stability of LPSCl in contact with In contributed to the long‐term cycling stability of the ASSBs.…”

Section: Resultsmentioning

confidence: 61%

Stable Cycling of All‐Solid‐State Batteries with Sacrificial Cathode and Lithium‐Free Indium Layer

Choi

Yoo

Lim

et al. 2021

Adv Funct Materials

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All-solid-state batteries (ASSBs) comprising solidified cathodes, electrolytes, and Li-metal anodes have attracted notable attention as promising future batteries for electric vehicles owing to their exceptional stability and expectation of achieving high energy density. However, its permanent operation has been hindered by Li dendrite growth, chemo-mechanical degradation, and interfacial instability, leading to Li exhaustion, increased resistance, and internal short-circuiting. Herein, for the first time, the authors report the effects of a lithium nitride (Li 3 N) sacrificial cathode on the cycling performance of ASSBs combined with a Li-free In layer. Through in situ evolved gas and internal pressure change analyses of the cells, it is found that, as with the liquid electrolyte cell, the decomposed Li 3 N compensates for active Li consumed by side reactions in the cell. Moreover, it is demonstrated that the improved interparticle contact by volume expansion of In through additionally supplied Li as well as the interfacial stability at the anode side by the dendrite-free In layer, are strongly responsible for the improved cyclability of the ASSBs. The findings reveal the effectiveness of the Li compensation approach for the stable cycling of ASSBs based on the secured interfacial stability at the anode side.

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“…However, the ionic conductivity of LSPS and the stability to the anode need to be further improved. Li 6 PS 5 X (X = Cl, Br, I) and Li 7 P 2 S 8 X (X = I, Br) have halogens in these SSEs. ,, These indicate that halogen doping may be an effective method to improve ionic conductivity. , In addition, halogen elements such as F and I can also stabilize the interface between SSEs and lithium metal and enhance the interface stability.…”

Section: Introductionmentioning

confidence: 99%

Cl-Doped Li₁₀SnP₂S₁₂ with Enhanced Ionic Conductivity and Lower Li-Ion Migration Barrier

Wang

et al. 2022

ACS Appl. Mater. Interfaces

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All-solid-state lithium batteries based on sulfide solid electrolytes have attracted much attention because of their high ionic conductivity. Li10SnP2S12 (LSPS) has the same structure as Li10GeP2S12, and there is little difference in ionic conductivity between them, but the preparation cost of LSPS is lower. Here, Cl doping is used to improve the electrochemical stability of the LSPS to the anode and the Li-ion transport performance. Among them, Li9.9SnP2S11.9Cl0.1 had a high ion conductivity of 2.62 mS cm–1 after cold pressure. On the crystal structure, X-ray diffraction Rietveld refinement indicated that the Cl-substituted portion S is successfully incorporated into the lattice of the LSPS, increasing Li-ion vacancies and reducing the distance between adjacent Li-ion distributed along the c-axis, these are conducive to Li-ion transmission. The temperature-dependent AC impedance experiment and density functional theory calculation show that doping with Cl makes Li9.9SnP2S11.9Cl0.1 have a lower activation energy. The assembled lithium symmetric batteries show that the doping of Cl promotes the stability of the interface between LSPS and the lithium metal anode. The charge–discharge tests of all-solid-state batteries using Li9.9SnP2S11.9Cl0.1 as electrolyte have confirmed that Cl doping can improve the electrochemical performance of LSPS, which have a higher specific capacity and cycle life.

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Origin of the Outstanding Performance of Dual Halide Doped Li₇P₂S₈X (X = I, Br) Solid Electrolytes for All-Solid-State Lithium Batteries

Cited by 38 publications

References 30 publications

Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Stable Cycling of All‐Solid‐State Batteries with Sacrificial Cathode and Lithium‐Free Indium Layer

Cl-Doped Li₁₀SnP₂S₁₂ with Enhanced Ionic Conductivity and Lower Li-Ion Migration Barrier

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Origin of the Outstanding Performance of Dual Halide Doped Li7P2S8X (X = I, Br) Solid Electrolytes for All-Solid-State Lithium Batteries

Cited by 38 publications

References 30 publications

Material Search for a Li10GeP2S12-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Material Search for a Li10GeP2S12-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Stable Cycling of All‐Solid‐State Batteries with Sacrificial Cathode and Lithium‐Free Indium Layer

Cl-Doped Li10SnP2S12 with Enhanced Ionic Conductivity and Lower Li-Ion Migration Barrier

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Origin of the Outstanding Performance of Dual Halide Doped Li₇P₂S₈X (X = I, Br) Solid Electrolytes for All-Solid-State Lithium Batteries

Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Material Search for a Li₁₀GeP₂S₁₂-Type Solid Electrolyte in the Li–P–S–X (X = Br, I) System via Clarification of the Composition–Structure–Property Relationships

Cl-Doped Li₁₀SnP₂S₁₂ with Enhanced Ionic Conductivity and Lower Li-Ion Migration Barrier