Delong He

Based on the increasing application requirements for the efficient adsorption of wastewater pollutants, graphene oxide-carbon nanotube/activated carbon (GO-CNT/AC) composites are constructed from the optimal microstructure matching of GO, CNTs, and AC materials by solution impregnation and freeze-drying methods. Three-dimensional structures with nano-micro hierarchical pores are established, with GO and CNTs uniformly dispersed on the AC surface, effectively restrain the agglomeration. The added CNTs played a “spring” role, supporting the gap between the GO sheets and AC matrix. Meanwhile, stable links are formed between GO, CNTs, and AC, realizing the synergistic matching of the microstructure, which provides abundant active absorption sites beneficial for improving the adsorption performance. The influences of the CNT contents, adsorbent amounts, methylene blue (MB) concentrations, and pH values on the adsorption property of GO-CNT/AC composites are systematically investigated. The results show that when the pH value of the MB solution is 13, the CNT concentration is 3 mg/mL and the MB concentration is 200 mg/L, the adsorption property of the composite is the best, with an adsorption capacity of 190.8 mg/g and a removal percentage of 95.4%. Compared with the raw AC, the adsorption capacity and removal percentage of the composites are increased by 73.9% and 72.8%, respectively. The GO-CNT/AC composites exhibit excellent cyclic adsorption performance, with a cyclic stability of 91.8% after six rounds of adsorption–desorption cycles. The kinetic analysis shows that the adsorption process conforms to the PSO kinetic model. By fitting of the IPD model, the adsorption mechanisms of the GO-CNT/AC composites are divided into two adsorption stages and described respectively. This study provides a new way to achieve highly efficient adsorption of pollutants in wastewater.