Synergetic interaction between neighboring platinum and ruthenium monomers boosts CO oxidation

Chem Sci. 2019 Apr 25;10(23):5898-5905. doi: 10.1039/c9sc00658c. eCollection 2019 Jun 21.

Abstract

Sub-nanometer noble metal catalysts, especially single atom (SA), are a new class of catalytic materials for boosting catalysis and possess unique catalytic properties and high atomic utilization efficiency. Exploring the interaction between two neighboring atom monomers has great potential to further improve the performance of SA catalysts and deepen the understanding on the catalytic mechanism of heterogeneous catalysis at the atomic level. Herein, we demonstrate that the synergetic effect between neighboring Pt and Ru monomers supported on N vacancy-rich g-C3N4 promotes the catalytic CO oxidation. The experimental observation and theoretical simulation reveal that the N vacancy in the g-C3N4 structure builds an optimized triangular sub-nanometer cavity for stabilizing the neighboring Pt-Ru monomers by forming Pt-C and Ru-N bonds. The mechanistic studies based on the in situ IR spectrum and theoretical simulation confirm that the neighboring Pt-Ru monomers possess a higher performance for optimizing O2 activation than Ru-Ru/Pt-Pt monomers or isolated Ru/Pt atoms by balancing the energy evolution of reaction steps in the catalytic CO oxidation. The discovery of the synergetic effect between neighboring monomers may create a new path for manipulating the catalytic properties of SA catalysts.