Tricycloquinazoline Based 2D Conjugated Metal-Organic Framework for Robust Sodium-Ion Batteries with Ion Co-Storage of Both Cations and Anions

There is growing interest in 2D conjugated metal-organic frameworks (2D c-MOFs) for batteries due to their reversible redox chemistry. Nevertheless, currently reported 2D c-MOFs based on n-type ligands are mostly focused on the storage of cations for batteries. Herein, we successfully synthesize the nitrogen-rich and electron-deficient p-type ligand-based Ni3(HATQ)2 assembled from 2, 3, 7, 8, 12, 13-hexaaminotricycloquinazoline (HATQ), and the ion co-storage feature of cations and anions in sodium ion batteries (SIBs) is demonstrated for 2D c-MOFs for the first time. The redox chemistry from p-type ligand and π-d hybridization center endows Ni3(HATQ)2 cathode with high capacity and good rate performance, especially excellent capacity retention of 95% after 1000 cycles. These findings provide a promising avenue for the exploration of other p-type multidentate chelating ligands toward new 2D c-MOFs and expand the application of 2D c-MOFs in energy storage systems.