Enhancement of high-efficiency potassium ion hybrid supercapacitors utilizing oxygen-deficient Co2NiO4@nitrogen-doped carbon nanoflower

Abstract

Transition metal oxides represent a promising category of pseudocapacitive materials for potassium-ion hybrid supercapacitors (PIHCs) characterized by high energy density. Nevertheless, their utility is hindered by intrinsic low conductivity, restricted electrochemical sites, and notable volume expansion, all of which directly contribute to the degradation of their electrochemical performance, thereby limiting their practical applicability in supercapacitor systems. In this study, we present a facile synthesis approach to fabricate nitrogen-doped carbon-supported oxygen vacancy-rich Co2NiO4 nanoflowers (Ov-Co2NiO4/NC NFs) featuring tunable surface layering and electron distribution. The nanoflower structure augments the contact area between the material and the electrolyte. Density functional theory (DFT) calculations reveal oxygen vacancies could bring an enhanced charge density across the entire Fermi level in Co2NiO4 and expand the interatomic distances between adjacent cobalt and nickel atoms to 3.370 Å. N-doped carbon carriers further accelerate charge transfer, increase the electrostatic energy storage and inhibit the structural collapse of Co2NiO4. These structural modifications serve to improve electrochemical reaction kinetics, augment the binding energy of K+ (−2.87 eV), and mitigate structural variations during K+ storage. In a 6 M KOH electrolyte, Ov-Co2NiO4/NC NF exhibits a specific capacitance of 1104 F g−1 at a current density of 0.5 A g−1, with a remarkable capacitance retention rate of 91.48 % after 6500 cycles. Furthermore, the assembled PIHCs demonstrate an energy density of 47.8 Wh kg−1 and an ultra-high power density of 376 W kg−1, alongside notable cycle stability, retaining 90.13 % of its capacitance after 8000 cycles in a 6 M KOH electrolyte.