Synergetic Catalysis of Magnetic Single-Atom Catalysts Confined in Graphitic-C3N4/CeO2(111) Heterojunction for CO Oxidization

Magnetic single-atom catalysts (MSAC), due to the intrinsic spin degree of freedom, are of particular importance relative to other conventional SAC for applications in various catalytic processes, especially in those cases that involve spin-triplet O-2. However, the bottleneck issue in this field is the clustering of the SAC during the processes. Here using first-principles calculations we predict that Mn atoms can be readily confined in the interface of the porous g-C3N4/CeO2(111) heterostructure, forming high-performance MSAC for O-2 activation via a delicate synergetic mechanism of charge transfer, mainly provided by the p-block g-C3N4 overlayer mediated by the d-block Mn active site, and spin selection, preserved mainly through active participation of the f-block Ce atoms and/or g-C3N4, which effectively promotes the CO oxidization. Such a recipe is also demonstrated to be valid for V- and Nb-MSACs, which may shed new light on the design of highly efficient MSACs for various important chemical processes wherein spin-selection matters.

Automated summary

Magnetic single-atom catalysts (MSAC) play a crucial role in catalytic processes, especially in cases involving spin selection. By utilizing the interface of the porous g-C3N4/CeO2(111) heterostructure, high-performance MSAC for O-2 activation and CO oxidation can be achieved through a delicate synergistic mechanism of charge transfer and spin selection.