Abstract

Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions. However, producing thermally stable SACs, especially in a simple and scalable way, remains a formidable challenge. Here, we report the synthesis of Ru SACs from commercial RuO2 powders by physical mixing of sub-micron RuO2 aggregates with a MgAl1.2Fe0.8O4 spinel. Atomically dispersed Ru is confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy. Detailed studies reveal that the dispersion process does not arise from a gas atom trapping mechanism, but rather from anti-Ostwald ripening promoted by a strong covalent metal-support interaction. This synthetic strategy is simple and amenable to the large-scale manufacture of thermally stable SACs for industrial applications.

Highlights

  • Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions

  • Transformation of RuO2 powders into isolated Ru atoms is promoted by a strong covalent metal–support interaction (CMSI) with MgAl1.2Fe0.8O4

  • The resulting Ru SAC has excellent thermal stability and improved activity for N2O decomposition at low and high concentrations. This simple and low-cost synthesis paves a way for the large-scale production of thermally stable SACs with high metal loadings for industrial applications

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Summary

Introduction

Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions. Detailed studies reveal that the dispersion process does not arise from a gas atom trapping mechanism, but rather from anti-Ostwald ripening promoted by a strong covalent metalsupport interaction This synthetic strategy is simple and amenable to the large-scale manufacture of thermally stable SACs for industrial applications. Various strategies have been developed for the fabrication of SACs. Atomic layer deposition and mass-selected soft-landing methods offer precise and controllable synthesis of well-designed SACs30–32; their scale-up is hindered by high production costs and low catalyst yields[33,34]. The resulting Ru SAC has excellent thermal stability and improved activity for N2O decomposition at low and high concentrations This simple and low-cost synthesis paves a way for the large-scale production of thermally stable SACs with high metal loadings for industrial applications

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