Study of Zinc Diffusion Based on S, N-Codoped Honeycomb Carbon Cathodes for High-Performance Zinc-Ion Capacitors

Capacitors with zinc ions, with excellent stabilities, low cost, and high energy density, are expected to be promising energy storage devices. However, the development of zinc-ion capacitors is quietly restricted by low specific capacity and cycling stability. Herein, to overcome these limitations, honeycomb-structured S, N-codoped carbon (SNPC) is constructed by one-pot calcination of waste corn bracts and thiourea. The honeycomb structure of SNPC is demonstrated to provide abundant active sites that can enhance the extron/ion transport, conductivity for high power export, and ion adsorption capacity in energy storage applications, leading to a higher electrochemical performance achieved. The electrolytes of zinc salt have also been studied. It reveals that the SNPC electrode presents the best electrochemical performance in a 2 M ZnSO₄ and 0.5 M ZnCl₂ electrolyte mixture because in the electrolyte mixture, Cl^- can replace the existing bound water in the solvation structure to form an anion-type water-free solvation structure ZnCl₄^2-. The SNPC-800 electrode with a highly improved surface area (∼909.0 m² g^-1) is proved to be more suitable as the electrode than other materials. Aqueous zinc-ion capacitors (ZICs) have been assembled by the honeycomb-structured SNPC-800 as the cathode, which can achieve a relatively wide working voltage range of 0.1-1.8 V. The SNPC-800 ZICs exhibit a superior specific capacity of 179.1 mA h g^-1 at 0.1 A g^-1. The energy density of SNPC-800 ZICs reaches an impressive value of 89.6 Wh kg^-1 at 53.8 W kg^-1, and it sustains 28.3 Wh kg^-1 at 1997.6 W kg^-1. In addition, there is 99.8% capacity retention in the SNPC-800 ZICs over 5000 cycles. The absorption energy in SPNC is much higher than that in undoped CPC, as confirmed by density functional theory, which reveals that introducing of heteroatoms (S, N) has a comparatively active advantage at increasing the Zn-ion storage capacity. This work proposes a practical strategy for the effective recycling of waste biomass materials into honeycomb carbon electrode materials. Moreover, the honeycomb carbon-based ZICs with excellent electrochemical performance and long-term cycling stability possess great potential to be a superior cathode in practical applications.