TY - JOUR
T1 - Triple-Layered Noncombustible PEO-Based Solid Electrolyte for Highly Safe Lithium-Metal Batteries
AU - Lim, Heesoo
AU - Chae, Munseok S.
AU - Jamal, Hasan
AU - Khan, Firoz
AU - Jeon, Injun
AU - Kim, Jongmin
AU - Kim, Jae Hyun
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/11/3
Y1 - 2024/11/3
N2 - Lithium-metal batteries are currently recognized as promising next-generation technologies owing to their high energy density. Solid polymer electrolytes, particularly those based on polyethylene oxide (PEO), are lauded for their leakage resistance, safety, and flexible design. Despite the ongoing fire safety- and ionic conductivity-related concerns, a novel noncombustible solid polymer electrolytes with superior ionic conductivities are introduced here with additive decabromodiphenyl ethane and zeolite. To enhance the mechanical strength and ensure soft interactions at the electrode interface, a triple-layer structure with self-extinguishing properties and robust ionic conductivity is proposed. Notably, the softness at the electrode interface intensifies as the LiTFSI concentration increases; this higher concentration negatively impacts PEO crystallinity, enhancing the ionic conductivity owing to the presence of free Li+ and TFSI− ions. This novel electrolyte can achieve a conductivity of 1.5 mS cm−1 at 60 °C, maintain anodic stability up to 4.8 V, and exhibit flame retardancy. Furthermore, adding LiTFSI at 60% relative to PEO is shown to reduce LiF formation on the surface, enhancing anode stability. The [LiFePO4/triple-layered electrolyte/Li] lithium-metal batteries are capable of an initial capacity of 153 mAh g−1, sustained superior capacity retention of 87.9%, and high Coulombic efficiency (99.6%) over 1000 cycles at a 1C rate.
AB - Lithium-metal batteries are currently recognized as promising next-generation technologies owing to their high energy density. Solid polymer electrolytes, particularly those based on polyethylene oxide (PEO), are lauded for their leakage resistance, safety, and flexible design. Despite the ongoing fire safety- and ionic conductivity-related concerns, a novel noncombustible solid polymer electrolytes with superior ionic conductivities are introduced here with additive decabromodiphenyl ethane and zeolite. To enhance the mechanical strength and ensure soft interactions at the electrode interface, a triple-layer structure with self-extinguishing properties and robust ionic conductivity is proposed. Notably, the softness at the electrode interface intensifies as the LiTFSI concentration increases; this higher concentration negatively impacts PEO crystallinity, enhancing the ionic conductivity owing to the presence of free Li+ and TFSI− ions. This novel electrolyte can achieve a conductivity of 1.5 mS cm−1 at 60 °C, maintain anodic stability up to 4.8 V, and exhibit flame retardancy. Furthermore, adding LiTFSI at 60% relative to PEO is shown to reduce LiF formation on the surface, enhancing anode stability. The [LiFePO4/triple-layered electrolyte/Li] lithium-metal batteries are capable of an initial capacity of 153 mAh g−1, sustained superior capacity retention of 87.9%, and high Coulombic efficiency (99.6%) over 1000 cycles at a 1C rate.
KW - flame retardant
KW - lithium metal batteries
KW - multi-layered electrolyte
KW - polyethylene oxide
KW - polymer electrolyte
UR - http://www.scopus.com/inward/record.url?scp=85207935280&partnerID=8YFLogxK
U2 - 10.1002/smll.202406200
DO - 10.1002/smll.202406200
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C2 - 39491500
AN - SCOPUS:85207935280
SN - 1613-6810
JO - Small
JF - Small
ER -