TY - JOUR
T1 - MOFs-induced robust interphase enriched in Li2O boosting Li plating/stripping coulombic efficiency of lithium metal anode in commercial carbonate electrolyte
AU - Wang, Ke
AU - Qian, Ji
AU - Chen, Yi
AU - Yu, Tianyang
AU - Zhang, Man
AU - Pan, Xinhui
AU - Chen, Renjie
N1 - Publisher Copyright:
© 2025
PY - 2025/9/1
Y1 - 2025/9/1
N2 - Lithium metal anodes face challenges of dendritic growth and unstable solid electrolyte interface (SEI) in carbonate electrolytes, leading to low Coulombic efficiency (CE<80%) and rapid capacity decay. Herein, we present a facile separator modification strategy utilizing functional Metal-organic framework (MOF) to catalyze the Li₂O-dominated SEI formation. The amine-functionalized MOF nanoparticles preferentially induce inorganic-rich SEI formation, yielding a mechanically robust interface with Li₂O crystallization and Young's modulus of 3.69 GPa, superior to that of conventional PP. Additionally, the porous structure of MOF nanoparticles endows the resulting separators with excellent electrolyte wettability and homogenizes ion transport. The functional separator with these synergistic effects reduces the decomposition of the electrolyte and facilitate the dense and uniform deposition of Li metal. As a result, exceptional Li plating/stripping stability is achieved in commercial carbonate electrolytes, delivering an average CE of 99.12% over 250 cycles at 1 mA cm−2/1 mAh cm−2 in Li/Cu cells. By implementing this functional separator, the Li/LiFePO4 full cells deliver a superior cycling lifespan that renders a high specific capacity of 130 mAh g−1 over 500 cycles at 1C with 90.9% capacity retention. This electrolyte-separator interfacial engineering strategy addresses critical challenges of Li metal anodes in carbonate electrolyte while demonstrating scalable potential for practical high-energy batteries.
AB - Lithium metal anodes face challenges of dendritic growth and unstable solid electrolyte interface (SEI) in carbonate electrolytes, leading to low Coulombic efficiency (CE<80%) and rapid capacity decay. Herein, we present a facile separator modification strategy utilizing functional Metal-organic framework (MOF) to catalyze the Li₂O-dominated SEI formation. The amine-functionalized MOF nanoparticles preferentially induce inorganic-rich SEI formation, yielding a mechanically robust interface with Li₂O crystallization and Young's modulus of 3.69 GPa, superior to that of conventional PP. Additionally, the porous structure of MOF nanoparticles endows the resulting separators with excellent electrolyte wettability and homogenizes ion transport. The functional separator with these synergistic effects reduces the decomposition of the electrolyte and facilitate the dense and uniform deposition of Li metal. As a result, exceptional Li plating/stripping stability is achieved in commercial carbonate electrolytes, delivering an average CE of 99.12% over 250 cycles at 1 mA cm−2/1 mAh cm−2 in Li/Cu cells. By implementing this functional separator, the Li/LiFePO4 full cells deliver a superior cycling lifespan that renders a high specific capacity of 130 mAh g−1 over 500 cycles at 1C with 90.9% capacity retention. This electrolyte-separator interfacial engineering strategy addresses critical challenges of Li metal anodes in carbonate electrolyte while demonstrating scalable potential for practical high-energy batteries.
KW - Carbonate electrolyte
KW - Coulombic efficiency
KW - Lithium metal anode
KW - Li₂O-rich solid electrolyte interphase
KW - MOFs
UR - http://www.scopus.com/inward/record.url?scp=105008503537&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2025.164928
DO - 10.1016/j.cej.2025.164928
M3 - Article
AN - SCOPUS:105008503537
SN - 1385-8947
VL - 519
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 164928
ER -