Polyethylenimine functionalized graphene oxide and cellulose nanofibril composite hydrogels: Synthesis, characterization and water pollutants adsorption

A stable 2,2,6,6-tetramethylpiperidine-1-yl)oxyl (TEMPO)-oxidized cellulose nanofibril (TCNF)/graphene oxide (GO)/polyethylenimine (PEI) composite hydrogel was synthesized by self-assembly instead of chemical crosslinking. Their chemical, morphology, surface, and mechanical properties were characterized and adsorption behavior for methyl blue (–) was systematically investigated in terms of the optimal GO content, pH effect, kinetics, and isotherm models. Additionally, to assess the adsorption capability of the TCNF/GO/PEI hydrogel for various contaminants, its effectiveness was also tested for methylene blue (+), Cu (II), and soybean oils. The maximum adsorption capability for the methyl blue (−) dyes increased from 3125 to 3962 mg/g when 13.3 % of GO was added. The adsorption capability for Cu (II) and soybean oils rose from 205.3 to 218.5 and 2.1 to 7.2 mg/g, respectively. The adsorption capability of optimized TCNF/GO/PEI hydrogel for a variety of contaminants was improved overall based on the increase of surface area, electrostatic interactions, and hydrophobic domains. Moreover, adding GO did not impact the adsorption mechanism but increased the external diffusion rate in the intraparticle diffusion model. This work provides a self-assembling route to TCNF/GO/PEI hydrogels with great potential for the removal of multiple water pollutants.