Sodiophilically Graded Gold Coating on Carbon Skeletons for Highly Stable Sodium Metal Anodes

Metallic sodium (Na) is an appealing anode material for high-energy Na batteries. However, Na metal suffers from low coulombic efficiencies and severe dendrite growth during plating/stripping cycles, causing short circuits. As an effective strategy to improve the deposition behavior of Na metal, a 3D carbon foam is developed that is sputter-coated with gold nanoparticles (Au/CF), forming a functional gradient through its thickness. The highly porous Au/CF host is proven to have gradually varying sodiophilicity, which in turn facilitates initially preferential Na deposition on the gold-rich, sodiophilic region in a "bottom-up growth" mode, leading to uniform plating over the entire Au/CF host. This finding contrasts with dendrite formation in the pristine CF host, as proven by in situ microscopy. The Na-predeposited Au/CF (Na@Au/CF) composite anode operates steadily for 1000 h at a low overpotential of ≈20 mV at 2 mA cm^-2 in a symmetric cell. When the composite anode is coupled with a Na₃ V₂ (PO₄ )₂ F₃ cathode, the full cell has a high capacity of 102.1 mAh g^-1 after 500 cycles at 2 C. The sodiophilicity gradient design that is explored in this study offers new insight into developing porous Na metal hosts with highly stable plating/stripping performance for next-generation Na batteries.