Dual Vertically Aligned Electrode-Inspired High-Capacity Lithium Batteries

Abstract

Lithium (Li) dendrite formation and poor Li⁺ transport kinetics under high-charging current densities and capacities inhibit the capabilities of Li metal batteries (LMBs). This study proposes a 3D conductive multichannel carbon framework (MCF) with homogeneously distributed vertical graphene nanowalls (VGWs@MCF) as a multifunctional host to efficiently regulate Li deposition and accelerate Li⁺ transport. A novel electrode for both Li|VGWs@MCF anode and LFP|VGWs@MCF (NCM₈₁₁ |VGWs@MCF) cathode is designed and fabricated using a dual vertically aligned architecture. This unique hierarchical structure provides ultrafast, continuous, and smooth electron transport channels; furthermore, it furnishes outstanding mechanical strength to support massive Li deposition at ultrahigh rates. As a result, the Li|VGWs@MCF anode exhibits outstanding cycling stability at ultrahigh currents and capacities (1000 h at 10 mA cm^-2 and 10 mAh cm^-2 , and 1000 h at 30 mA cm^-2 and 60 mAh cm^-2 ). Moreover, full cells made of such 3D anodes and freestanding LFP|VGWs@MCF (NCM₈₁₁ |VGWs@MCF) cathodes with conspicuous mass loading (45 mg cm^-2 for LFP and 35 mg cm^-2 for NCM₈₁₁ ) demonstrate excellent areal capacities (6.98 mAh cm^-2 for LFP and 5.6 mAh cm^-2 for NCM₈₁₁ ). This strategy proposes a promising direction for the development of high-energy-density practical Li batteries that combine safety, performance, and sustainability.

Keywords: dual vertically aligned architectures; lithium metal batteries (LMBs); ultrahigh currents and capacities; vertical graphene nanowalls.