Ultra-High Sulfur-Doped Hierarchical Porous Hollow Carbon Sphere Anodes Enabling Unprecedented Durable Potassium-Ion Hybrid Capacitors

Abstract

Sulfur doping is a promising path to ameliorate the kinetics of carbon-based anodes. However, the similar electronegativity of sulfur and carbon and the poor thermal stability of sulfur severely restrict the development of high-sulfur-content carbon-based anodes. In this work, ultra-high sulfur-doped hierarchical porous hollow carbon spheres (SHCS) with a sulfur content of 6.8 at % are synthesized via a direct high-temperature sulfur-doping strategy. An SHCS has sulfur bonded to the carbon framework including C-S-C and C-SO_<i>x</i>-C, which enlarges its interlayer distance (0.411 nm). In the K half-cell, benefiting from the considerable content and the reasonable architecture of sulfur, the SHCS exhibits significantly improved reversible specific capacity, initial Coulombic efficiency, and cyclability than hierarchical porous hollow carbon spheres without sulfur. Remarkably, the potassium ion hybrid capacitor device fabricated with the SHCS anode achieves excellent energy/power density (135.6 W h kg^-1/17.7 kW kg^-1) and unprecedented durability over 26,000 cycles at 2 A g^-1. This research provides a superior strategy to design high-sulfur-content carbon-based anodes with excellent potassium storage performance.