Vapor-phase self-assembly for generating thermally stable single-atom catalysts

Preparation of thermally stable metal single-atom catalysts (SACs) is a challenge in heterogeneous catalysis, especially on conventional supports that provide a weak metal-support interaction. In this work, we report that a modified support MgAl2O4 can stabilize Pt single atoms by a mechanism of vapor-phase self-assembly in a high-temperature treatment (800 degrees C, air). The experimental results on the formation mechanism and the structure are validated by DFT and ab initio molecular dynamics simulations. We infer that stable triangular K3O3 structures help stabilize Pt single atoms at high temperatures in oxidizing conditions, exhibiting excellent reactivity for methane oxidation. The obtained Pt/K/MgAl2O4 SAC presents excellent stability in methane oxidation after steam treatment at elevated temperatures, whereas the Pt/MgAl2O4 nanocatalyst suffers from rapid deactivation due to Pt nanoparticle growth. This work paves the way for preparing thermally stable and highly active SACs using conventional high-surface-area supports, despite the weak metal-support interaction.

Automated summary

In this study, a modified support MgAl2O4 is used to stabilize Pt single atoms through a mechanism of vapor-phase self-assembly in high-temperature treatment. The formation mechanism and structure are validated through simulations. The obtained Pt/K/MgAl2O4 SAC shows excellent stability and reactivity in methane oxidation, providing a new approach for preparing thermally stable and highly active SACs using conventional high-surface-area supports.