Symmetrizing cathode-anode response to speed up charging of nanoporous supercapacitors

Abstract

Asymmetric behaviors of capacitance and charging dynamics in the cathode and anode are general for nanoporous supercapacitors. Understanding this behavior is essential for the optimal design of supercapacitors. Herein, we perform constant-potential molecular dynamics simulations to reveal asymmetric features of porous supercapacitors and their effects on capacitance and charging dynamics. Our simulations show that, counterintuitively, charging dynamics can be fast in pores providing slow ion diffusion and vice versa. Unlike electrodes with single-size pores, multi-pore electrodes show overcharging and accelerated co-ion desorption, which can be attributed to the subtle interplay between the dynamics and charging mechanisms. We find that capacitance and charging dynamics correlate with how the ions respond to an applied cell voltage in the cathode and anode. We demonstrate that symmetrizing this response can help boost power density, which may find practical applications in supercapacitor optimization.