Microbial fuel cell (MFC) technology has become a novel and attractive method for generating renewable energy during wastewater treatment. In this study, researchers combined carbon felt (CF), metal oxide (NiO), and polyaniline (PANI) to prepare CF/NiO/PANI multilayer capacitive bioelectrodes. The MFC equipped with a CF/NiO/PANI bioanode has a peak power density of 1988.31 ± 50.96 mW/m2, which is 3.8 times higher than that of the MFC with a bare CF electrode, having a peak power density of 518.29 ± 27.07 mW/m2. Charge–discharge cycle tests show that the storage charge capacity of the CF/NiO/PANI bioanode is 3304.64 C/m2, which is 10.5 times greater than that of the bare CF anode. The electrochemical, morphological, and chemical properties of the prepared anodes are characterized using techniques such as SEM, EDS, FTIR, XPS, and XRD. Notably, high-throughput sequencing reveals that electrogenic bacteria account for 79.2% of the total microbial population on the CF/NiO/PANI multilayer capacitive bioelectrode. The synergistic effects of the composite materials result in the formation of a richer biofilm on the electrode surface, providing more active sites and enhancing capacitive characteristics. This innovative approach significantly improves the output power and peak current of MFCs, while also endowing the electrode with dual functions of simultaneous power generation and energy storage.
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