Introduction of nitrogen doped graphene nanosheets as efficient adsorbents for nitrate removal from aqueous samples

PURPOSE: Introducing and developing new kinds of adsorbents are always a significant challenge in water treatments. In this work, for the first time, graphene oxide (GO), nitrogen-doped graphene oxide (ND-GO), highly nitrogen-doped graphene oxide (HND-GO), and 3D high nitrogen-doped graphene oxide (3D-HND-GO) were synthesized and comparatively evaluated in the removal of nitrate content of tap and underground waters. METHODS: The removal of the target analyte was performed through a batch adsorption approach, and the factors influencing its removal efficiency (i.e., initial pH of the sample, primary concentrations of nitrate, amount of adsorbent, and contact time) were evaluated through a central composite design (CCD) and response surface methodology (RSM). RESULTS: Based on the results, 3D-HND-GO showed the highest removal efficiency in comparison with the other mentioned nanoparticles. The nitrate removal using this adsorbent was modeled successfully so that R(2), adjusted R(2), and predicted R(2) values were 0.9717, 0.9508, and 0.9010, respectively. In addition, the optimal removal condition was achieved using the Nelder-Mead non-linear optimization algorithm as follow: the initial concentrations of nitrate (expressed as nitrogen): 15.0 mg/mL, the amount of the adsorbent: 2.0 mg/mL; pH of the sample: 3.0; and the contact time: 20.0 min. Under this optimal condition, the actual removal result (92.5 ± 4.0%) was in good agreement with the expected value (94.8 ± 5.1%). Additional studies were also performed to comprehensibly evaluate the adsorption activity of the adsorbent (e.g., kinetic, isotherm, and desorption parameters). The adsorption isotherm complied with the Langmuir model illustrating the considerable mono-layer adsorption capacities for the target ions with q(m) of 8.7 mg/g. The adsorption process was indicated to obey a pseudo 2nd order kinetic model, with the rate-limiting step for the adsorption phase. CONCLUSIONS: This study revealed which 3D-HND-G leads to improved yield in the nitrate ions elimination, particularly at acidic media, which was related to the enhanced dispersibility and larger surface area. The adsorbent was further successfully used for treating tap and underground water samples. At the present moment, research as grown to modify 3D-HND-G in orders to increase the potentiality for industrial applications. SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40201-021-00741-7.