Understanding the Ion-Sorption Dynamics in Functionalized Porous Carbons for Enhanced Capacitive Energy Storage.

Heteroatom-functionalized porous carbon has long been regarded as a promising electrode material to construct high-performance capacitive energy storage devices. However, the development of this field is seriously limited due to the lack of an in-depth understanding of the ion-sorption dynamics. Herein, the component and structure controllable N, O, and Cl codoped bimodal (micro-to-meso) porous carbons were prepared and further used as the investigated object for exploring the intrinsic ion-sorption dynamics, which is the root of the enhanced electrochemical response in capacitive energy storage devices. Voltammetry response analysis is employed to quantify the charge storage contributions from both electrostatic adsorption effect (electrical double-layer capacitance) and highly reversible redox process (pseudocapacitance). The existence of electronic capacitance enables a positive correlation between surface capacitance and the ratio of micropores. Besides, an electron-dependent correlation between the electroactive functional groups and redox reaction induced capacitance is also explored. This work will advance the capacitive energy storage field by presenting a clear understanding of the ion-sorption dynamics in the functionalized porous carbons.