Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration

Metal-support interaction predominately determines the electronic structure of metal atoms in single-atom catalysts (SACs), largely affecting their catalytic performance. However, directly tuning the metal-support interaction in oxide supported SACs remains challenging. Here, we report a new strategy to subtly regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFe2O4 SACs by a simple water soaking treatment. Detailed studies reveal that the CMSI is weakened by the bonding of H+, generated from water dissociation, onto the interface of Pt-O-Fe, resulting in reduced charge transfer from metal to support and leading to an increase of C-H bond activation in CH4 combustion by more than 50 folds. This strategy is general and can be extended to other CMSI-existed metal-supported catalysts, providing a powerful tool to modulating the catalytic performance of SACs. A simple water soaking treatment significantly weakened the strong covalent metal-support interaction between the atomically dispersed Pt and CoFe2O4, which leads to an enhanced activity towards methane combustions by 55 times. This work highlights the critical role of altering the coordination structure of single-atom active sites and provides a new strategy to modulate metal-support interaction regulation.

Automated summary

A new strategy to regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFe2O4 single-atom catalysts (SACs) by water soaking treatment is reported. This strategy provides a powerful tool to modulate the catalytic performance of SACs.