TY - JOUR
T1 - Rational design of a heterogeneous double-layered composite solid electrolyte via synergistic strategies of asymmetric polymer matrices and functional additives to enable 4.5 V all-solid-state lithium batteries with superior performance
AU - Li, Liansheng
AU - Wang, Jie
AU - Zhang, Leiting
AU - Duan, Huanhuan
AU - Deng, Yuanfu
AU - Chen, Guohua
N1 - Funding Information:
This work was supported by the National Natural Science Foundation of China (Grant Nos. 22178125 and 21875071 ), the Guangzhou Scientific and Technological Planning Project (Grant No. 201704030061 ), and the Guangdong key R&D Program of China (Grant No. 2019B090908001).
Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2022/3
Y1 - 2022/3
N2 - High-voltage all-solid-state lithium batteries (ASSLBs) are one of the very promising energy storage devices for future high performance energy storage and conversion, but their development faces multiple interfacial challenges at present. In this work, a novel strategy of asymmetric polymer matrices design combined with the using of functional additives is developed to meet the distinctive requirements on cathode and anode sides for high-voltage ASSLBs simultaneously. A composite solid electrolyte (CSE) consisting of blended polymer matrices (PEO + PVDF) is employed as the cathode side CSE (CSC) due to its high electrochemical stability, while PEO-based CSE with high stability against Li metal is used as the anode side CSE (ASC). Meanwhile, lithium bisoxalatodifluorophosphate (LiBODFP) is incorporated into the CSC to stabilize the cathode-electrolyte interface due to its ability to be oxidized to form the stable LiPxOyFz-rich cathode electrolyte interphase (CEI) film, and LiNO3 in the ASC as the solid electrolyte interphase (SEI) former to effectively suppress the lithium dendrites formation. The assembled high-voltage LiFe0.5Mn0.5PO4-based ASSLB using the as-prepared asymmetric CSE (CSC/ASC) exhibits superior electrochemical behaviors in the voltage range of 2.5 ∼ 4.5 V, with specific capacities of 161.7 and 103.5 mAh g−1 at 0.1 and 2 C, respectively, and a super high capacity retention of 90.6% after 1000 cycles at 1 C. Additionally, respective mechanisms of the addition of LiBODFP in the CSC and LiNO3 in the ASC to prolong the cycle stability of the ASSLB are systematically revealed through detailed characterization of the cycled electrodes.
AB - High-voltage all-solid-state lithium batteries (ASSLBs) are one of the very promising energy storage devices for future high performance energy storage and conversion, but their development faces multiple interfacial challenges at present. In this work, a novel strategy of asymmetric polymer matrices design combined with the using of functional additives is developed to meet the distinctive requirements on cathode and anode sides for high-voltage ASSLBs simultaneously. A composite solid electrolyte (CSE) consisting of blended polymer matrices (PEO + PVDF) is employed as the cathode side CSE (CSC) due to its high electrochemical stability, while PEO-based CSE with high stability against Li metal is used as the anode side CSE (ASC). Meanwhile, lithium bisoxalatodifluorophosphate (LiBODFP) is incorporated into the CSC to stabilize the cathode-electrolyte interface due to its ability to be oxidized to form the stable LiPxOyFz-rich cathode electrolyte interphase (CEI) film, and LiNO3 in the ASC as the solid electrolyte interphase (SEI) former to effectively suppress the lithium dendrites formation. The assembled high-voltage LiFe0.5Mn0.5PO4-based ASSLB using the as-prepared asymmetric CSE (CSC/ASC) exhibits superior electrochemical behaviors in the voltage range of 2.5 ∼ 4.5 V, with specific capacities of 161.7 and 103.5 mAh g−1 at 0.1 and 2 C, respectively, and a super high capacity retention of 90.6% after 1000 cycles at 1 C. Additionally, respective mechanisms of the addition of LiBODFP in the CSC and LiNO3 in the ASC to prolong the cycle stability of the ASSLB are systematically revealed through detailed characterization of the cycled electrodes.
KW - Asymmetric layered solid electrolyte
KW - High performance
KW - High-voltage cathode
KW - Lithium metal battery
KW - Lithium salt additive
UR - http://www.scopus.com/inward/record.url?scp=85119067628&partnerID=8YFLogxK
U2 - 10.1016/j.ensm.2021.10.047
DO - 10.1016/j.ensm.2021.10.047
M3 - Journal article
AN - SCOPUS:85119067628
SN - 2405-8297
VL - 45
SP - 1062
EP - 1073
JO - Energy Storage Materials
JF - Energy Storage Materials
ER -