TY - JOUR
T1 - Ultra-robust Single-Ion Conducting Composite Electrolytes for Stable Li-Metal Batteries
AU - Song, Zhaowei
AU - Zhao, Sheng
AU - Shan, Xinyuan
AU - Tian, Jia
AU - Muralidharan, Nitin
AU - Zhu, Jiadeng
AU - Zheng, Jackie
AU - Sokolov, Alexei P.
AU - Cao, Peng Fei
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025
Y1 - 2025
N2 - With significantly high lithium-ion (Li+) transport efficiency, single-ion conducting polymer electrolytes (SIPEs) often suffer from low ionic conductivity due to the covalently bonded anions to the polymer backbone. Adding plasticizers to SIPEs to improve ionic conductivity usually reduces the polymer matrix’s mechanical robustness, negatively affecting overall performance as solid electrolytes. Herein, to surpass such a trade-off relationship, we successfully designed a single-ion conducting composite membrane (c-SIPM60) with cross-linked linear SIPEs and incorporated glass-mesh substrate, which shows a cation transport number close to 1, ultrahigh tensile strength of 22 MPa (modulus of 547.3 MPa), and high ionic conductivity of 1.2 × 10-4 S/cm at 25 °C. The resultant Li/c-SIPM60/Li symmetric cell showed stable cycling performance up to 1200 h, and the LiFePO4/c-SIPM60/Li cell presented good reversibility at C/10. Meanwhile, with additional lithium salts, a high cationic-transport composite membrane (c-HTPM60) was designed to increase the ionic conductivity with retained high Li+ transport efficiency. The LiFePO4/c-HTPM60/Li cell exhibited a stable cycling performance with a capacity retention of >75.6% after 700 cycles at 25 °C. This work provides new insights into designing solid electrolytes with simultaneously high tLi+, ionic conductivity, and mechanical robustness, affording effective Li+ transport for energy storage systems.
AB - With significantly high lithium-ion (Li+) transport efficiency, single-ion conducting polymer electrolytes (SIPEs) often suffer from low ionic conductivity due to the covalently bonded anions to the polymer backbone. Adding plasticizers to SIPEs to improve ionic conductivity usually reduces the polymer matrix’s mechanical robustness, negatively affecting overall performance as solid electrolytes. Herein, to surpass such a trade-off relationship, we successfully designed a single-ion conducting composite membrane (c-SIPM60) with cross-linked linear SIPEs and incorporated glass-mesh substrate, which shows a cation transport number close to 1, ultrahigh tensile strength of 22 MPa (modulus of 547.3 MPa), and high ionic conductivity of 1.2 × 10-4 S/cm at 25 °C. The resultant Li/c-SIPM60/Li symmetric cell showed stable cycling performance up to 1200 h, and the LiFePO4/c-SIPM60/Li cell presented good reversibility at C/10. Meanwhile, with additional lithium salts, a high cationic-transport composite membrane (c-HTPM60) was designed to increase the ionic conductivity with retained high Li+ transport efficiency. The LiFePO4/c-HTPM60/Li cell exhibited a stable cycling performance with a capacity retention of >75.6% after 700 cycles at 25 °C. This work provides new insights into designing solid electrolytes with simultaneously high tLi+, ionic conductivity, and mechanical robustness, affording effective Li+ transport for energy storage systems.
KW - composite membrane
KW - lithium metal batteries
KW - mechanical robustness
KW - polymer electrolytes
KW - single-ion conducting polymers
UR - http://www.scopus.com/inward/record.url?scp=85214497528&partnerID=8YFLogxK
U2 - 10.1021/acsami.4c18659
DO - 10.1021/acsami.4c18659
M3 - Article
AN - SCOPUS:85214497528
SN - 1944-8244
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
ER -