Electrocapacitive desalination with nitrogen-doped hierarchically structured carbon prepared using a sustainable salt-template method

Porous carbon materials hold tremendous potential for capacitive deionization (CDI). However, realizing high specific surface area (SSA), suitable pore size distribution, and hierarchical porosity in carbons with facile and sustainable techniques is still challenging. In this work, we prepare hierarchical porous carbons (HPCs) with high SSA, abundant pore structures, and N-self doping via a versatile and sustainable modified salt-template approach. The optimized electrode gives a high SSA of 1639.9 m2/g, a large pore volume (2.7 cm3/g), and hierarchical porous structures (micro-meso-macro pores). For applications, the symmetric CDI electrode assembly delivers a salt adsorption capacity (SAC) of up to 17.67 mg/g in a 500 mg/L NaCl at 1.2 V together with ultrafast salt adsorption kinetics. We systematically study their associated desalination mechanism by combining several electrochemical experiments with the in-situ Raman spectroscopy technique, which revealed that the total salt storage is from the synergistic effect of both electrical double-layer (EDL) storage and pseudocapacitive mechanisms, with the EDL storage being dominant. This work paves the way to design economical and eco-friendly porous carbon materials for high-performance CDI desalination.