Two-dimensional sp²-carbon-linked covalent organic framework for large-capacity and long-life Na metal batteries

Na metal batteries are regarded as an encouraging route for energy-dense and low-cost battery systems. However, the unstable and irreversible Na plating/stripping, caused by the uncontrolled dendritic Na growth, prevents their practical applications. Herein, a two-dimensional sp²-carbon-linked covalent organic framework (cyano-sp²c-COF) is adopted as seeding/hosting coating layer for a highly stable interface with long cycling life, large capacity, and high Na utilization. Benefit from the features of a fully π-conjugated structure and well-defined cyano groups, cyano-sp²c-COF with superior sodiophilicity and small interface resistance can reduce the nucleation barrier, enable Na ion flux uniformity, and enhance interface stability. Ultimately, the system achieves a low nucleation overpotential of only 10 mV, a remarkable average Coulombic efficiency of 99.7% maintained over 500 cycles in half cells, and exceptional interfacial durability of 8500 h with a high accumulated capacity of 8.5 Ah cm⁻² in symmetric cells. Furthermore, the symmetric cells also present a steady cycling, even increasing the depth of discharge up to 90%. As proof, full cells demonstrate a long lifespan enduring 2700 cycles with tiny capacity decay, providing valuable insights into the long-life Na batteries.