Atomic-scale Observation of the Generation and Dispersion of Iron Single Atoms

Abstract

Single-atom catalysts (SACs) have shown great potential in catalysis and energy-related applications. Among these, iron SACs stand out for their exceptional performance and environmental friendliness. In this study, we investigated the transformation of iron oxide nanoparticles into iron single atoms, exemplifying a top-down synthesis strategy. Using in-situ transmission electron microscopy (TEM), we directly observed the dynamic behaviors during the pyrolysis-induced atomization of Fe₃O₄ nanoparticles along the [110], [111], and [112] zone axes at atomic-scale resolution. Reducing gases were supposed to release during the thermal pyrolysis of an organic reducing agent and facilitate the generation of Fe single atoms. The rate-limiting step was the reaction of these gases with atoms at surface steps and vertices of Fe₃O₄ nanoparticles. Electron energy loss spectroscopy revealed a reduction in the Fe valence state and a transition in the Fe-O coordination environment after in-situ thermal treatment. The high-density dispersion of Fe single atoms was facilitated by the weak repulsive interactions between Fe atoms. This study enriches the understanding of the gas-assisted atomization mechanism and offers valuable insights for optimizing the production of high-density SACs. The methodology and findings can be extended to other material systems, broadening the scope of single-atom engineering and catalysis applications.

Keywords

Single atom recognition / In-situ heating / Atomic-scale dynamics / Nanoparticle decomposition / Gas-assisted solid-phase dissolution process / Technology / Nanotechnology / Chemical Sciences / Physical Chemistry (incl. Structural)

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RIGHTS & PERMISSIONS

Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH