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Binder-free Ultra-thin Graphene Oxide as an Artificial Solid Electrolyte Interphase for Anode-free Rechargeable Lithium Metal Batteries
Z. T. Wondimkun, T. T. Beyene, M. A. Weret, N. A. Sahalie, C.-J. Huang, B. Thirumalraj, B. A. Jote, D. Wang, W.-N. Su*, C.-H. Wang, G. Brunklaus, M. Winter, and B.-J. Hwang*
The unregulated growth of lithium dendrite upon cycling is hampering the applications of lithium metal batteries. The inherent artificial solid electrolyte interphase (SEI) formed during the first few cycles cannot provide the desired stability of lithium deposition. In the anode free battery (AFB) configuration, uncontrolled lithium plating on bare copper imposes a more serious lithium dendrite growth. Herein, we modify the copper current collector with a binder-free ultra-thin spin-coated graphene oxide (GO). The synchronize smooth and conductive GO-coated artificial SEI with lithium fluoride derived from fluoroethylene carbonate (FEC) electrolyte additive greatly control the lithium deposition. Accordingly, the synergistic effect enables smooth, uniform, and dendrite-free lithium plating. Moreover, the AFB with GO film and 5% FEC in the carbonate-based electrolyte is capable of achieving high coulombic efficiency of an average 98% and attains ~44% of its initial capacity after 50 cycles. In contrast, the full cell with bare Cu//LiNi1/3Mn1/3Co1/3O2 (NMC) has a coulombic efficiency of 89% and retains 26.9% after 20 cycles. Our results demonstrate that the synergy of GO-coated artificial SEI with FEC additive can be a promising approach to impede lithium dendrites growth and result in enhanced electrochemical performance in an AFB.