Revealing the Effect of the Microstructure on Potassium Storage Behavior in a Two-Dimensional Mesoporous Carbon Anode

Hard carbon is considered as the most promising anode material for potassium-ion energy storage devices. Substantial progress has been made in exploring advanced hard carbons to solve the issues of sluggish kinetics and large volume changes caused by the large radius of K⁺. However, the relationship between their complicated microstructures and the K⁺ charge storage behavior is still not fully explored. Herein, a series of two-dimensional mesoporous carbon microcoins (2D-MCMs) with tunable microstructures in heteroatom content and graphitization degree are synthesized by a facile hard-template method and follow a temperature-controllable annealing process. It is found that high heteroatom content makes for surface-driven K⁺ storage behavior, which increases the capacity-contribution ratio from a high potential region, while a high graphitization degree makes for K⁺ intercalation behavior, which increases the capacity-contribution ratio from a low potential region. Electrochemical results from a three-electrode Swagelok cell demonstrate that a 2D-MCM anode with more capacity contribution from a low working region allows the porous carbon cathode to be operated in a much wider electrochemical window, thus storing more charge. As a result, potassium-ion capacitors based on the optimized 2D-MCM anode deliver a high energy density of 113 Wh kg^-1 and an exhilarating power density of 51,000 W kg^-1.