Optimizing graphene oxide membranes for effective removal of dyes by modulating the reduction degree and doped nitrogen.

The excellent mechanical and chemical characteristics of graphene oxide (GO) enable their potential application in the realm of membrane separation. However, the expansion and instability of GO nanosheets in water limit its application. In this work, nitrogen-doped GO (NGO) was obtained by a harmless hydrothermal reduction method. The obtained NGO films were attached to a polyvinylidene fluoride support membrane by vacuum filtration. By changing the hydrothermal reaction temperature, the reduction degree of GO and doping amount of nitrogen was adjusted to control the inter-layer structure and permeability of NGO. The defect of NGO nanosheets and the reduction of oxygen-containing functional groups could accelerate the transportation of water molecules through the inter-layer space of the hydrophobic graphene sheets. Significantly, the polarization and high adsorption energy of pyridine-N serve as a supplement to the exclusion mechanism of the inter-layer spacing. NGO membranes have better permeability than the initial GO membranes without sacrificing the rejection rate. The optimized NGO film has a significant rejection rate of above 99% for various dyes, such as methylene blue, Congo red and methyl blue.