TY - JOUR
T1 - Suppression of Dehydrofluorination Reactions of a Li0.33La0.557TiO3-Nanofiber-Dispersed Poly(vinylidene fluoride-co-hexafluoropropylene) Electrolyte for Quasi-Solid-State Lithium-Metal Batteries by a Fluorine-Rich Succinonitrile Interlayer
AU - Rath, Purna Chandra
AU - Liu, Ming Song
AU - Lo, Shih Ting
AU - Dhaka, Rajendra S.
AU - Bresser, Dominic
AU - Yang, Chun Chen
AU - Lee, Sheng Wei
AU - Chang, Jeng Kuei
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/3/29
Y1 - 2023/3/29
N2 - Solid-state lithium-metal batteries have great potential to simultaneously achieve high safety and high energy density for energy storage. However, the low ionic conductivity of the solid electrolyte and large electrode/electrolyte interfacial impedance are bottlenecks. A composite solid electrolyte (CSE) that integrates electrospun Li0.33La0.557TiO3 (LLTO) nanofibers, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is fabricated in this work. The effects of the LLTO filler fraction and morphology (spherical vs fibrous) on CSE conductivity are examined. Additionally, a fluorine-rich interlayer based on succinonitrile, fluoroethylene carbonate, and LiTFSI, denoted as succinonitrile interlayer (SNI), is developed to reduce the large interfacial impedance. The use of SNI rather than a conventional ester-based interlayer (EBI) effectively decreases the Li//CSE interfacial resistance and suppresses unfavorable interfacial side reactions. The LiF- and CFx-rich solid electrolyte interphase (SEI), derived from SNI, on the Li metal electrode, mitigates the accumulation of dead Li and excessive SEI. Importantly, dehydrofluorination reactions of PVDF-HFP are significantly reduced by the introduction of SNI. A symmetric Li//CSE//Li cell with SNI exhibits a much longer cycle life than that of an EBI counterpart. A Li//CSE@SNI//LiFePO4 cell shows specific capacities of 150 and 112 mAh g-1 at 0.1 and 2 C (based on LiFePO4), respectively. After 100 charge-discharge cycles, 98% of the initial capacity is retained.
AB - Solid-state lithium-metal batteries have great potential to simultaneously achieve high safety and high energy density for energy storage. However, the low ionic conductivity of the solid electrolyte and large electrode/electrolyte interfacial impedance are bottlenecks. A composite solid electrolyte (CSE) that integrates electrospun Li0.33La0.557TiO3 (LLTO) nanofibers, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is fabricated in this work. The effects of the LLTO filler fraction and morphology (spherical vs fibrous) on CSE conductivity are examined. Additionally, a fluorine-rich interlayer based on succinonitrile, fluoroethylene carbonate, and LiTFSI, denoted as succinonitrile interlayer (SNI), is developed to reduce the large interfacial impedance. The use of SNI rather than a conventional ester-based interlayer (EBI) effectively decreases the Li//CSE interfacial resistance and suppresses unfavorable interfacial side reactions. The LiF- and CFx-rich solid electrolyte interphase (SEI), derived from SNI, on the Li metal electrode, mitigates the accumulation of dead Li and excessive SEI. Importantly, dehydrofluorination reactions of PVDF-HFP are significantly reduced by the introduction of SNI. A symmetric Li//CSE//Li cell with SNI exhibits a much longer cycle life than that of an EBI counterpart. A Li//CSE@SNI//LiFePO4 cell shows specific capacities of 150 and 112 mAh g-1 at 0.1 and 2 C (based on LiFePO4), respectively. After 100 charge-discharge cycles, 98% of the initial capacity is retained.
KW - composite solid electrolyte
KW - electrospinning
KW - interface modification layer
KW - morphology effects
KW - polymer decomposition
UR - http://www.scopus.com/inward/record.url?scp=85150454020&partnerID=8YFLogxK
U2 - 10.1021/acsami.2c22268
DO - 10.1021/acsami.2c22268
M3 - 期刊論文
C2 - 36920173
AN - SCOPUS:85150454020
SN - 1944-8244
VL - 15
SP - 15429
EP - 15438
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 12
ER -