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Abstract:
Dendrite growth and high-voltage capacity fade conundrums persist as key barriers in lithium-metal batteries (LMBs). Although LiNO3 effectively optimizes interfacial chemistry as an electrolyte additive, its application remains hampered by limited carbonate-electrolyte solubility and self-depleting behavior during extended cycling. This study presents an innovative interfacial engineering strategy through the strategic incorporation of LiNO3-impregnated hollow mesoporous silica composites (HMS@LiNO3) onto separator surfaces to achieve dualinterface modulation. Capitalizing on the strong adsorption capability of HMS within the high-dielectric ethylene carbonate, a nitrate-rich solvation structure is lastingly established at the anode interface. The configuration facilitates the formation of a Li3N-enriched solid electrolyte interphase with superior ionic conductivity, effectively enhancing lithium deposition kinetics while inhibiting dendritic growth. Concurrently, the cathode interface benefits from a controlled nitrate-lean solvation sheath that preferentially undergoes oxidative decomposition, generating a robust protective layer to mitigate electrolyte decomposition under 4.5 V operation. As a result, the lifetime in Li plating/stripping exceeds 1800 h and the average Coulombic efficiency is as high as 98.25 % over 350 cycles. The matched NCM811//Li full cell exhibits a high-capacity retention rate of 80.38 % after 500 cycles at a cut-off voltage of 4.5 V, providing valuable guidance into the development of long-life highvoltage LMBs.
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NANO ENERGY
ISSN: 2211-2855
Year: 2025
Volume: 142
1 6 . 8 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 0
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