Nitrogen-doped graphene oxide with enhanced bioelectricity generation from microbial fuel cells for marine sewage treatment

With the increasing demand for clean water and energy, microbial fuel cell (MFC) as a promising technology for obtaining energy from wastewater has attracted great research interest in the last two decades. The performance of the anode electrode is the most critical factor limiting the large-scale application of MFC. Graphene materials as a suitable candidate have been successfully used as the anode due to their excellent biocompatibility and efficient extracellular electron transfer (EET) ability. Here, nitrogen-doped graphene oxide (NGO) was prepared by a simple one-step hydrothermal method. X-ray photoelectron spectroscopy (XPS) was used to analyse the valence states of the surface chemical elements and their associated molecular species. Fourier transform infrared spectroscopy (FTIR) was used to identify the surface functional groups, and Raman spectroscopy was used to analyse the information about surface defects. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) revealed the increased electrochemical activity and rapid EET ability from the NGO electrodes. Scanning electron microscopy demonstrated the two-dimensional layered structure of the NGO with some wrinkled texture. MFCs equipped with the modified NGO anode achieved the highest power density of 708.3 mW/m2 with an output voltage of 498.6 mV in comparison with the other graphene-based electrodes, i.e., graphene and graphene oxide. Moreover, the chemical oxygen demand (COD) removal rate increased significantly from 18.1% to 45.6%. The analysis of the bacterial community using a high-throughput sequencing indicated that the relative abundance of the electricigens increased on the NGO electrode biofilim, and the relative expression of ccoN gene coding cytochrome-c oxidase (Cco) was markedly up-regulated. These results demonstrated that NGO modification effectively enhanced the bio-electrocatalytic activity of MFC with improved wastewater treatment capacity. [Display omitted] •The annealing time and temperature can effectively tune the N doping degree.•The NGO induces the enrichment of Proteobacteria in anode biofilm.•The relative expression of cooN gene enhances the performance of MFCs.•The nitrogen doped graphene surface boosts interfacial electron transfer.