In Situ Transformation of Isolated Pt ₁ to Oligomeric PtO _x Clusters via H ₂ Plasma Restructuring

ABSTRACT

Two‐dimensional monolayer PtO _x catalysts exhibit attractive properties in heterogeneous catalytic reactions due to their synergistic effect of adjacent metals and high activation potential of lattice oxygen. However, traditional preparation methods are extremely complex and not environmentally friendly, and their simple and rapid directional synthesis remains a huge challenge. Here, we found that the H ₂ plasma treating is an efficacious strategy for the facile synthesis of single‐layer oligomeric PtO _x cluster catalyst with nearly 100% metal dispersion of Pt via single atom Pt ₁ /CeO ₂ precursor. The obtained monolayer oligomeric PtO _x cluster catalyst exhibits excellent low‐temperature activity with CH ₄ totally oxidized at just 260°C, and the reaction rates in 100°C–260°C are 2‐3 orders of magnitude comparing to that of Pt ₁ /CeO ₂ . Different from isolated Pt atoms, the hybridization of Pt and O in oligomeric PtO _x promotes the charge transfer of Pt→O and activates the surrounding Pt lattice oxygen (O _lat ), boosting the cleavage of C─H bonds. The rapid activation and release of O _lat accelerates the desorption of intermediates formed on the catalyst surface. The present work demonstrates a promising and scalable low‐temperature plasma treatment strategy for fabricating highly active supported noble metal catalysts with regulable nanostructure and metal‐support interaction.