Al homogeneous deposition induced by N-containing functional groups for enhanced cycling stability of Al-ion battery negative electrode

Rechargeable Al-ion batteries (AIBs) are considered as one of the most fascinating energy storage systems due to abundant Al resource and low cost. However, the cycling stability is subjected to critical problems for using Al foil as negative electrode, including Al dendrites, corrosion and pulverization. For addressing these problems, here a lightweight self-supporting N-doped carbon rod array (NCRA) is demonstrated for a long-life negative electrode in AIBs. Experimental analysis and first-principle calculations reveal the storage mechanism involving the induced deposition of N-containing function groups to Al as well as the ideal skeleton of the NCRA matrix for Al plating/stripping, which is favorable for regulating Al nucleation and suppressing dendrites growth. Compared with the Al foil, the NCRA exhibits lower areal mass density (∼ 72% of Al foil), smaller thickness (40% of Al foil), but much longer cycle life (> 4 times of Al foil). Benefiting from the remarkable stability of the array structure, symmetric cells show excellent cycling stability with small voltage hysteresis (∼ 80 mV) and meanwhile there are no corrosion and pulverization problems even after cycled for 120 hours. Besides, full cells also manifest long lifespan (1,500 cycles) and increased Coulombic efficiency (100±1%).