Trifunctional Synergy of Host-Catalysis-Interface Engineering for Ultrastable Lithium Metal Batteries.

Utilizing ultrathin lithium metal batteries (LMBs) is highly promising for next-generation energy storage, offering exceptional energy density and enhanced safety. However, their widespread adoption is severely hindered by poor Li plating/stripping reversibility and unstable electrode/electrolyte interfaces. In this study, an architectured current collector (CC) is designed by integrating a three-dimensional (3D) conductive host co-functionalized with single-atomic Zn sites and Ag nano-clusters (Zn1-Agn@CP) dual active sites in conjunction with a prelithiation protocol. Advanced in situ/operando characterizations combined with density functional theory (DFT) calculations reveal that single-atom Zn and Ag clusters effectively modulate charge distribution within the CP matrix, thereby promoting uniform Li-ion flux and fast reaction kinetics. Specifically, Zn1-Agn@CP induces the formation of an inorganic-rich solid-electrolyte interphase (SEI) that suppresses dendrite growth, while the Ag clusters catalyze solvent decomposition to generate a compact cathode-electrolyte interphase (CEI) that limits transition metal (TM) ion migration and reinforces cathode structural stability. Consequently, the well-orchestrated Zn1-Agn@CP achieves reversible Li deposition with a high Coulombic efficiency (CE) of 99.91% over 900 cycles. When paired with a LiNi0.8Co0.1Mn0.1O2 cathode, the system retains substantial reversible capacity after 1000 cycles at 5 C with a high CE of 99.58%, highlighting the efficacy of the integrated "host-catalysis-interface" synergistic strategy for high-rate LMBs.