Abstract

The low catalytic activity of activated carbon (AC) toward oxygen reduction reaction (ORR) in air cathode severely limits the electricity production of microbial fuel cells (MFCs). In this work, a novel cobalt‑nitrogen‑carbon nanotube co-implanted activated carbon catalysts ([email protected]) were prepared by growth of Co/Zn-based metal organic frameworks on AC followed by thermal pyrolysis. The [email protected] catalyzed ORR via an efficient four-electron pathway in pH-neutral medium, and exhibited superb ORR catalytic activity comparable to commercial Pt/C. As compared with pristine AC, implantation of Co, N and carbon nanotubes into [email protected] improved the ORR current density and exchange current density of air cathodes by 120% and 73% respectively. The maximum power density of MFCs achieved 2045 ± 43 mW m−2 by using the optimized [email protected] pyrolyzed at 850 °C, which was 65% higher than that of pristine AC. The superb ORR performance of [email protected] originated from the synergistic effect of abundant Co-Nx, Pyridinic-N and Graphitic-N active sites, high graphitization degree, well dispersed Co nanoparticles and improved micro-mesoporous coexistence structure, which enabled high ORR catalytic activity and rapid mass transfer at the three-phase boundary. This work provides a new routine for large-scale synthesis of highly-efficient ORR electrocatalysts based on AC and metal organic frameworks, which has promising potential for the application in practical MFCs.

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