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Submicron Interfacial Layers for Nanoscale Control of Lithium Deposition in Surface-Engineered Current Collectors
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DOI：10.1039/D6NR01899H.png)
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Abstract
En 中文
Lithium metal batteries (LMBs) have garnered considerable attention owing to their high theoretical capacity and low electrochemical potential; however; their practical implementation is hindered by unstable Li plating/stripping and poor interfacial stability. Previous strategies have largely focused on enhancing lithiophilicity or wettability to regulate initial Li deposition; yet they do not necessarily ensure stable long-term cycling. In this study; an interfacial buffer layer was rationally designed for metal-based current collectors to elucidate the distinct contributions of lithiophilicity and wettability to Li deposition behavior. A comparison of representative material systems designed to decouple these effects revealed that interfacial stability; derived from mechanical robustness and adhesion; governs long-term electrochemical performance. Bare Cu induces localized Li nucleation and forms a compositionally heterogeneous and unstable solid electrolyte interphase (SEI); leading to dendritic growth and dead Li accumulation. Conversely; a graphene oxide–poly(vinylidene fluoride)-coated current collector enables uniform Li deposition and promotes the formation of a mechanically robust and chemically homogeneous SEI; improving plating/stripping reversibility. The submicron-thick coating enables effective interfacial control without compromising practical electrode configurations. The resulting system delivers a stable Coulombic efficiency of ~75% over 120 cycles; whereas other configurations exhibit rapid degradation due to interfacial instability. XPS depth profiling revealed the formation of a uniform and lithium fluoride(LiF)-rich SEI with minimal depth-dependent variation; indicating a stabilized interphase. These findings highlight that long-term stability in LMBs is governed by mechanically robust interfacial stability during repeated cycling rather than by initial nucleation behavior; providing clear design guidelines for interface-engineered current collectors.
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