TY - JOUR
T1 - Deep Eutectic Interlayer Design for Stability Enhancement in LLZTO Solid-State Lithium Batteries
AU - Long, Sihong
AU - Gui, Boshun
AU - Li, Chengjie
AU - Yang, Binbin
AU - Sun, Lipu
AU - Zhan, Yu
AU - Huang, Chuhuai
AU - Tian, Jianing
AU - Wu, Feng
AU - Chen, Nan
AU - Chen, Renjie
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2026/1/26
Y1 - 2026/1/26
N2 - Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is a typical inorganic garnet-type ceramic solid electrolyte. By combining LLZTO with polyacrylonitrile (PAN), a homogeneous composite electrolyte film can be obtained, which is self-supporting and can be directly used as a solid-state electrolyte. However, PAN and its composite electrolyte exhibit low ionic conductivity at room temperature and suffer from poor solid-solid interface contact with the lithium metal anode. Herein, a method of using succinonitrile (SN) deep eutectic electrolyte is proposed to modify the solid-state electrolyte interface, thereby preventing corrosion reactions and improving the Li+ transference number of the composite solid electrolyte (PALS) to 0.66. The introduction of the interface modification layer enables the formation of a stable and dense solid-electrolyte interphase (SEI) layer at the interface between the lithium anode and the solid-state electrolyte, reducing interfacial impedance and improving the ionic conductivity of the solid-state electrolyte. The Li/PALS/lithium iron phosphate (LFP) full cell exhibits an initial specific capacity of 147 mAh·g−1 at a 0.5 C rate, with 97.3% capacity retention after 190 cycles at room temperature. This work presents a novel approach to improving the interfacial contact between LLZTO and lithium metal anode, offering new insights for the design of fast-rate, safe, and durable solid-state electrolytes.
AB - Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is a typical inorganic garnet-type ceramic solid electrolyte. By combining LLZTO with polyacrylonitrile (PAN), a homogeneous composite electrolyte film can be obtained, which is self-supporting and can be directly used as a solid-state electrolyte. However, PAN and its composite electrolyte exhibit low ionic conductivity at room temperature and suffer from poor solid-solid interface contact with the lithium metal anode. Herein, a method of using succinonitrile (SN) deep eutectic electrolyte is proposed to modify the solid-state electrolyte interface, thereby preventing corrosion reactions and improving the Li+ transference number of the composite solid electrolyte (PALS) to 0.66. The introduction of the interface modification layer enables the formation of a stable and dense solid-electrolyte interphase (SEI) layer at the interface between the lithium anode and the solid-state electrolyte, reducing interfacial impedance and improving the ionic conductivity of the solid-state electrolyte. The Li/PALS/lithium iron phosphate (LFP) full cell exhibits an initial specific capacity of 147 mAh·g−1 at a 0.5 C rate, with 97.3% capacity retention after 190 cycles at room temperature. This work presents a novel approach to improving the interfacial contact between LLZTO and lithium metal anode, offering new insights for the design of fast-rate, safe, and durable solid-state electrolytes.
KW - LLZTO/PAN composite solid electrolyte
KW - deep eutectic electrolyte
KW - interlayer design
KW - long cycling life
KW - solid-state lithium metal batteries
UR - https://www.scopus.com/pages/publications/105013779892
U2 - 10.1002/adfm.202513024
DO - 10.1002/adfm.202513024
M3 - Article
AN - SCOPUS:105013779892
SN - 1616-301X
VL - 36
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 8
M1 - e13024
ER -