Iron Single Atoms Anchored on Carbon Matrix/g-C3N4 Hybrid Supports by Single-Atom Migration-Trapping Based on MOF Pyrolysis.

Abstract

Numerous efforts have been devoted to realizing the high loading and full utilization of single-atom catalysts (SACs). As one of the representative methods, atom migration-trapping (AMT) is a top-down strategy that converts a certain volume of metal nanoparticles (NPs) or metal-based precursors into mobile metal species at high temperature, which can then be trapped by suitable supports. In this study, high-loading iron single atoms anchored onto carbon matrix/g-C3N4 hybrid supports were obtained through a single-atom migration-trapping method based on metal–organic framework (MOF) pyrolysis. It is confirmed, by high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS), that the Fe(acac)3 precursor is reduced to Fe single atoms (SAs), which are not only anchored onto the original N-doped carbon (NC), but also onto g-C3N4, with an Fe-N coordination bond. Further electrochemical results reveal that Fe-C3N4-0.075 possesses a better half-wave potential of 0.846 V and onset potential of 0.96 V compared to Fe-N-C, the product obtained after pyrolysis of Fe(acac)3@ZIF-8. As opposed to SAs prepared by the pyrolysis process only, SAs prepared by AMT are commonly anchored onto the surface of the supports, which is a simple and effective way to make full use of the source metal and prepare SACs with higher exposing active sites.