Topography-confined dual-gradient 3D scaffold design for stable and dendrite-free sodium metal anodes
摘要
The rational design of a 3D scaffold with optimized electrical conductivity, sodiophilicity, and sufficient internal space is crucial for suppressing the growth of Na dendrites and accommodating the large volume changes of Na metal anodes during the plating/stripping process. Nevertheless, the uniform conductivity and sodiophilicity of conventional scaffolds often lead to Na metal deposition on the top of the scaffold, thereby hindering the complete functional capabilities of the scaffold. To tackle this challenge, we developed a novel imprinted dual-gradient 3D network skeleton that boasts gradients in both sodiophilicity and conductivity. Both theoretical and experimental analyses indicate that Na metal prefers to nucleate and deposit dendrite-free from the bottom of the 3D skeleton due to its superior conductivity and sodiophilicity. This dual-gradient design enables the electrode to achieve low nucleation overpotential of 11 mV and sustain stable operation for 1900 h at 1.5 mA cm−2/1.5 mAh cm−2 and 1000 h at 20 mA cm−2/20 mAh cm−2, far superior to the gradientless electrode. When paired with Na3V2(PO4)3 cathode, the full cell retains a capacity of 67.6 mAh g−1 after 1000 stable cycles with a capacity retention rate of 82.4% at a rate of 10 C. This advanced skeleton structure design is poised to advance the development of high-energy-density alkali metal batteries.