Realization of High Energy Density Sodium-Ion Hybrid Capacitors through Interface Engineering of Pseudocapacitive 3D-CoO-NrGO Hybrid Anodes

Sodium-ion hybrid capacitors (SHCs) have attracted great attention owing to the improved power density and cycling stability in comparison with sodium-ion batteries. Nevertheless, the energy density (<100 Wh·kg–1) is usually limited by low specific capacity anodes (<150 mAh·g–1) and “kinetics mismatch” between the electrodes. Hence, we report a high energy density (153 Wh·kg–1) SHC based on a highly pseudocapacitive interface-engineered 3D-CoO-NrGO anode. This high-performance anode (445 mAh·g–1 @0.025 A·g–1, 135 mAh·g–1 @5.0 A·g–1) consists of CoO (∼6 nm) nanoparticles chemically bonded to the NrGO network through Co–O–C bonds. Exceptional pseudocapacitive charge storage (up to ∼81%) and capacity retention (∼80% after 5000 cycles) are also identified for this SHC. Excellent performance of the 3D-CoO-NrGO anode and SHC is owing to the synergistic effect of the CoO conversion reaction and pseudocapacitive sodium-ion storage induced by numerous Na2O/Co/NrGO nanointerfaces. Co–O–C bonds and the 3D microstructure facilitating efficient strain relaxation and charge-transfer correspondingly are also identified as vital factors accountable for the excellent electrochemical performance. The interface-engineering strategy demonstrated provides opportunities to design high-performance transition metal oxide-based anodes for advanced SHCs.