An Integrated Structural Air Electrode Based on Parallel Porous Nitrogen-Doped Carbon Nanotube Arrays for Rechargeable Li–Air Batteries

The poor discharge and charge capacities, and the cycle performance of current Li–air batteries represent critical obstacles to their practical application. The fabrication of an integrated structural air electrode with stable parallel micropore channels and excellent electrocatalytic activity is an efficient strategy for solving these problems. Herein, a novel approach involving the synthesis of nitrogen-doped carbon nanotube (N-CNT) arrays on a carbon paper substrate with a conductive carbon-black layer for use as the air electrode is presented. This design achieves faster oxygen, lithium ion, and electron transfer, which allows higher oxygen reduction/evolution reaction activities. As a result, the N-CNT arrays (N/C = 1:20) deliver distinctly higher discharge and charge capacities, 2203 and 186 mAh g(−1), than those of active carbons with capacities of 497 and 71 mAh g(−1) at 0.05 mA cm(−2), respectively. A theoretical analysis of the experimental results shows that the parallel micropore channels of the air electrode decrease oxygen diffusion resistance and lithium ion transfer resistance, enhancing the discharge and charge capacities and cycle performance of Li–air batteries. Additionally, the N-CNT arrays with a high pyridinic nitrogen content can decompose the lithium peroxide product and recover the electrode morphology, thereby further improving the discharge–charge performance of Li–air batteries.