Nitrogen-doped carbon (NC) materials have been proposed as next-generation oxygen reduction reaction (ORR) catalysts to significantly improve scalability and reduce costs, but these alternatives usually exhibit low activity and/or gradual deactivation during use. Here, we develop new 2D sandwich-like zeolitic imidazolate framework (ZIF) derived graphene-based nitrogen-doped porous carbon sheets (GNPCSs) obtained by in situ growing ZIF on graphene oxide (GO). Compared to commercial Pt/C catalyst, the GNPCSs show comparable onset potential, higher current density, and especially an excellent tolerance to methanol and superior durability in the ORR. Those properties might be attributed to a synergistic effect between NC and graphene with regard to structure and composition. Furthermore, higher open-circuit voltage and power density are obtained in direct methanol fuel cells.

Oxygen evolution: A 3D nickel foam/porous carbon/anodized nickel electrode was designed for the oxygen evolution reaction (see picture). The conductive porous carbon membrane, which is derived from a zeolite imidazolate framework, plays a key role as an interlayer to both protect the inner instable Ni foam and support the outermost oxygen‐evolving Ni catalyst layer.