TY - JOUR
T1 - High-Entropy Laminates with High Ion Conductivities for High-Power All-Solid-State Lithium Metal Batteries
AU - Zhao, Qi
AU - Cao, Zhenjiang
AU - Wang, Xingguo
AU - Chen, Hao
AU - Shi, Yu
AU - Cheng, Zongju
AU - Guo, Yu
AU - Li, Bin
AU - Gong, Yongji
AU - Du, Zhiguo
AU - Yang, Shubin
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/10/4
Y1 - 2023/10/4
N2 - Solid-state electrolytes (SSEs) are crucial to high-energy-density lithium metal batteries, but they commonly suffer from slow Li+ transfer kinetics and low mechanical strength, severely hampering the application for all-solid-state batteries. Here, we develop a two-dimensional (2D) high-entropy lithium-ion conductor, lithium-containing transition-metal phosphorus sulfide, HE-LixMPS3 (Lix(Fe1/5Co1/5Ni1/5Mn1/5Zn1/5)PS3) with five transition-metal atoms and lithium ions (Li+) dispersed into [P2S6]2- framework layers, exhibiting high lattice distortions and a large amount of cation vacancies. Such unique features enable to efficiently accelerate the migration of Li+ in 2D [P2S6]2- interlamination, delivering a high ionic conductivity of 5 × 10-4 S cm-1 at room temperature. Moreover, the HE-LixMPS3 laminate can be employed as a building block to construct an ultrathin SSE film (∼10 μm) based on strong C-S bonding between HE-LixMPS3 and nitrile-butadiene rubber. The SSE film delivers a strong mechanical robustness (6.0 MPa, 310% elongation) and a high ionic conductivity of 4 × 10-4 S cm-1, showing a long cycle stability of 800 h in lithium symmetric cells. Coupled with LiFePO4 cathode and lithium anode, the all-solid-state battery presents a high Coulombic efficiency of 99.8% within 2000 cycles at 5.0 C.
AB - Solid-state electrolytes (SSEs) are crucial to high-energy-density lithium metal batteries, but they commonly suffer from slow Li+ transfer kinetics and low mechanical strength, severely hampering the application for all-solid-state batteries. Here, we develop a two-dimensional (2D) high-entropy lithium-ion conductor, lithium-containing transition-metal phosphorus sulfide, HE-LixMPS3 (Lix(Fe1/5Co1/5Ni1/5Mn1/5Zn1/5)PS3) with five transition-metal atoms and lithium ions (Li+) dispersed into [P2S6]2- framework layers, exhibiting high lattice distortions and a large amount of cation vacancies. Such unique features enable to efficiently accelerate the migration of Li+ in 2D [P2S6]2- interlamination, delivering a high ionic conductivity of 5 × 10-4 S cm-1 at room temperature. Moreover, the HE-LixMPS3 laminate can be employed as a building block to construct an ultrathin SSE film (∼10 μm) based on strong C-S bonding between HE-LixMPS3 and nitrile-butadiene rubber. The SSE film delivers a strong mechanical robustness (6.0 MPa, 310% elongation) and a high ionic conductivity of 4 × 10-4 S cm-1, showing a long cycle stability of 800 h in lithium symmetric cells. Coupled with LiFePO4 cathode and lithium anode, the all-solid-state battery presents a high Coulombic efficiency of 99.8% within 2000 cycles at 5.0 C.
UR - https://www.scopus.com/pages/publications/85174080258
U2 - 10.1021/jacs.3c04279
DO - 10.1021/jacs.3c04279
M3 - 文章
C2 - 37751194
AN - SCOPUS:85174080258
SN - 0002-7863
VL - 145
SP - 21242
EP - 21252
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 39
ER -