Nano Research

Article Title

A systematic theoretical study on FeOx-supported single-atom catalysts: M1/FeOx for CO oxidation


single-atom catalyst, M1/FeOx, density functional theory, heterogeneous catalysis


ABSTRACT A single-atom catalyst (SAC) that was first proposed by us in 2011 has aroused significant recent interest. Among the various SACs, FeOx-based ones including Pt1/FeOx, Ir1/FeOx, Au1/FeOx, Ni1/FeOx, and Fe1/FeOx have been investigated either experimentally or theoretically for CO oxidation. However, a systematic study of FeO x-based SACs has not been conducted. For a comprehensive understanding of FeO x-supported single-metal-atom catalysts, extensive density functional theory calculations were carried out on the activities and catalytic mechanisms of SACs with the 3d, 4d, and 5d metals of group VIII to IB, i.e., M1/FeOx (M = Fe, Co, Ni, Cu; Ru, Rh, Pd, Ag; Os, Ir, Pt, Au) for CO oxidation. Remarkably, a new noble metal SAC, Pd1/FeOx, with high activity in CO oxidation was found and is predicted to be even better than the previously reported Pt1/FeOx and Ni1/FeOx. In comparison, other M1/FeOx SACs (M = Fe, Co, Cu; Ru, Rh, Ag; Os, Ir, Au) showed only low activities in CO oxidation. Moreover, the adsorption strength of CO on the single-atom active sites was found to be the key in determining the catalytic activity of these SACs for CO oxidation, because it governs the recoverability of oxygen vacancies on their surfaces in the formation of a second CO2 during CO oxidation. Our systematic studies of FeOx-supported SACs will help in understanding the fundamental mechanisms of the interactions between singly dispersed surface metal atoms and FeOx substrate and in designing highly active FeO x-supported SACs.

Graphical Abstract


Tsinghua University Press