Controlled fabrication of nitrogen-doped porous carbon foam with refined hierarchical architectures for desalination via capacitive deionization

Porous carbon materials have been regarded as a promising alternative to activated carbon for desalination via capacitive deionization (CDI) due to refined architectures and functionalities. However, it is still challenging to obtain a controlled hierarchical pore structure and considerable nitrogen-doped content by convenient method. Herein, nitrogen-doped hierarchical porous carbon foams (NHCFs) with different microstructural features, nitrogen contents and nitrogen species were successfully fabricated via a stepwise pyrolysis carbonization strategy using easily available melamine foam. Due to the synergistic effect of hierarchical porous structure and doped nitrogen, the optimized NHCF sample carbonized at 800℃ (NHCF-800) exhibited a maximum desalination capacity of 30.1 mg g-1 at the optimal operating parameters (500 mg/L NaCl solution, 1.2 V) and an excellent regeneration performance after 50 continuous adsorption-desorption cycles. Furthermore, density functional theory (DFT) was also conducted to elaborate the disparity of sodium adsorption energy among the nitrogen species for in-depth understanding, and it mainly benefits from the ascendency of the pyrrolic-N and pyridinic-N over the graphitic-N dopant. This work paves the way of rational regulation of nitrogen-doped process and hierarchical porous structure carbon as CDI electrode materials for desalination.