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The traditional air cathode in microbial fuel cell (MFC) usually consists of catalyst layer (CL), supporting layer (SL) and conductive gas diffusion layer (GDL), the overall MFC performance is inevitably affected by the additional and expensive adhesives and conductive agents. Here, we developed an integrated air cathode in MFC without any additional SL, GDL or adhesives. The integrated air cathode was self-supporting nitrogen-doped reduced graphene oxide@carbon nanofiber (N-rGO@CNF) hybrid membranes fabricated by electrospinning with subsequent heat-treatment under ammonia atmosphere. The as-fabricated N-rGO@CNFs possessed far superior MFC performance and oxygen reduction reaction (ORR) activity to the pristine nitrogen-doped carbon nanofibers (NCNF) and commercial activated carbon (CAC). The amount of rGO embedded into CNF had prominent influence on their ORR activities and MFC performances. N-5-rGO@CNF had the lowest resistance and the maximal exchange current density, exhibiting desirable oxygen reduction performance via a four-electron pathway. The maximum power density of N-5-rGO@CNF can reach 826 mW m−2 in MFC, which is approximately 9, 2.53 and 1.82 times of pristine NCNF, CAC and Pt/C with values of 91, 327 and 454 mW m−2. The outstanding performance of the integrated air-cathodes originates from the integrality, brevity and hybrid composition of the electrospun nanofiber membrane. The appropriate embedded rGO not only improves the bulk conductivity of the rGO@CNF to promote ion adsorption, but also provides vacancies to accommodate ions, the doped nitrogen atoms facilitate O 2 adsorption and/or subsequent O–O bond breaking, thus improving the electrochemical performance of N-rGO@CNF in MFC. [Display omitted] • An integrated N-rGO@CNF air cathodes with high-efficiency were developed via electrospinning. • The integrated air cathodes showed excellent catalytic performance in Microbial Fuel Cells. • The optimal air cathode (N-5-rGO@CNF) had maximum power density of 20650 mW m−3. • N-5-rGO@CNF exhibited ideal oxygen reduction reaction via a four-electron pathway. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel electrode was fabricated by electrospinning PAN blended with ZIF-67. • The ZIF-67/CNFs electrode showed excellent electrocatalytic activities for ORR. • MFCs with ZIF-67/CNFs cathode had a maximum power density of 1.191±0.017 W m−2. • Geobacter was the highest proportion of microbial in ZIF-67/CNFs-MFC. In this study, the zeolitic imidazolate framework-67 (ZIF-67) and electrospinning polyacrylonitrile membrane were combined to prepare electrospinning carbon nanofibers composite cathode (ZIF-67/CNFs) which could enhance the oxygen reduction reaction (ORR) performance of microbial fuel cells (MFCs) cathode. The optimum electrode 3 wt% ZIF-67/CNFs revealed the excellent ORR performance with a half-wave potential of −0.03 V vs. Ag/AgCl, which was more positive than Pt/C-CC (-0.09 V vs. Ag/AgCl). The highest output voltage (607±9 mV) and maximum power density (1.191±0.017 W m−2) were obtained when the prepared ZIF-67/CNFs electrode was applied to the cathode of MFC (ZIF-67/CNFs-MFC). In addition, ZIF-67/CNFs-MFC showed the best pollutant removal effect. Geobacter was the highest proportion of microbial in ZIF-67/CNFs-MFC. The results have shown that the application of ZIF-67/CNFs electrode to MFC cathode is promising. [ABSTRACT FROM AUTHOR]