A tricycloquinazoline based 2D conjugated metal–organic framework for robust sodium-ion batteries with co-storage of both cations and anions

Abstract

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 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 the p-type ligand and π–d hybridization center endows the 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.