Amorphous Modulation of Atomic Nb‐O/N Clusters with Asymmetric Coordination in Carbon Shells for Advanced Sodium‐Ion Hybrid Capacitors

Anode materials with excellent properties have become the key to develop sodium‐ion hybrid capacitors (SIHCs) that combine the advantages of both batteries and capacitors. Amorphous modulation is an effective strategy to realize high energy/power density in SIHCs. Herein, atomically amorphous Nb‐O/N clusters with asymmetric coordination are in situ created in N‐doped hollow carbon shells (Nb‐O/N@C). The amorphous clusters with asymmetric Nb‐O3/N1 configurations have abundant charge density and low diffusion energy barriers, which effectively modulate the charge transport paths and improve the reaction kinetics. The clusters are also enriched with unsaturated vacancy defects and isotropic ion‐transport channels, and their atomic disordering exhibits high structural stress buffering, which are strong impetuses for realizing bulk‐phase‐indifferent ion storage and enhancing the storage properties of the composite. Based on these features, Nb‐O/N@C achieves notably improved sodium‐ion storage properties (reversible capacity of 240.1 mAh g−1 at 10.0 A g−1 after 8000 cycles), and has great potential for SIHCs (230 Wh Kg−1 at 4001.5 W Kg−1). This study sheds new light on developing high‐performance electrodes for sodium‐ion batteries and SIHCs by designing amorphous clusters and asymmetric coordination. Atomically amorphous Nb‐O/N clusters are in situ created in N‐doped hollow carbon shells (Nb‐O/N@C). The clusters with Nb‐O3/N1 configurations have abundant charge densities and low diffusion energy barriers, which can effectively improve the reaction kinetics. The clusters are also enriched with unsaturated vacancy defects and isotropic transport channels, and their atomic disordering exhibits high structural stress buffering. These characteristics are strong impetuses for enhancing the storage properties of the composite.