Micelles of Mesoporous Silica with Inserted Iron Complexes as a Platform for Constructing Efficient Electrocatalysts for Oxygen Reduction.

Iron, N-codoped carbon materials (Fe-N-C) are promising electrocatalysts toward oxygen reduction reactions due to their high atom utilization efficiency and intrinsic activity. Nanostructuring of the Fe-N-C materials, such as introducing porosity into the carbon structure, would be conducive to further increasing the exposure of active sites as well as improving the mass transfer. Herein, we explore the potential of iron complex-functionalized micelles of mesoporous SiO2 as a platform for constructing porous Fe-N-C materials. The classical three-dimensional MCM-48 was selected as a proof-of-concept example, which was utilized as the hard template, and cetyltrimethylammonium bromide micelles inside it played the role of the main carbon source. Fe-Nx sites were derived from Fe-1,10-phenanthroline complexes in the micelles introduced by in situ incorporation of 1,10-phenanthroline and post Fe2+ insertion in an aqueous solution. After thermal annealing in a nitrogen atmosphere and subsequent removal of the MCM-48 framework, a carbon material that possesses porous structural features with uniformly dispersed Fe-Nx sites (MPC@PhFe) was obtained, which shows superior ORR activity in a 0.1 M KOH solution and great potential for Zn-air battery applications as well. This work demonstrates the feasibility as well as the effectiveness of turning micelles of mesoporous SiO2 into porous carbon structures and might offer a universal strategy for manufacturing carbon materials for future application in energy storage and conversion.