Nitrogen and sulfur codoped micro-mesoporous carbon sheets derived from natural biomass for synergistic removal of chromium(VI): adsorption behavior and computing mechanism

We reported the effective removal of chromium(VI) (Cr(VI)) from wastewater with nitrogen and sulfur codoped micro-mesoporous carbon sheets (N,S-MMCSs), which were fabricated by pyrolysis of natural biomass (luffa sponge) followed by chemical activation and hydrothermal treatment. N,S-MMCSs possessed a hierarchical micro-mesoporous sheet-like framework, large specific surface area (1525.45 m2 g-1), high pore volume (1.21 cm3 g-1), and appropriate N (1.81 wt%) and S (1.01 wt%) co-doping. Batch adsorption experiments suggested that Cr(VI) adsorption by the N,S-MMCSs increased with increase the solution acidity, adsorbent dosage, Cr(VI) concentration, temperature, and time. The Cr(VI) adsorption was mainly controlled by the chemisorptions and could be well interpreted by the Langmuir isotherm and pseudo-second-order kinetic models. The maximum adsorption capacities of Cr(VI) were 217.39, 277.78, and 312.50 mg g-1 at 298, 308, and 318 K, respectively. The Cr(VI) adsorption procedure was spontaneous, endothermic, and randomness. The Cr(VI) adsorption mechanism followed the physical adsorption, electrostatic attraction, in situ reduction, and surface chelation. Besides, the density functional theory (DFT) calculation demonstrated that the N and S co-doping could decrease the adsorption energy and enhance the attractive interaction between N,S-MMCSs and Cr(VI) through the synergistic effect, and thus significantly improve the Cr(VI) adsorption property.