Rational Design of Precious-Metal Single-Atom Catalysts for Methane Combustion

Supported precious-metal single-atom catalysts (PM SACs) have emerged as a new frontier of high-performance catalytic material with 100% atom utilization efficiency. However, the rational design of such material with guidance from fundamental understandings of the structure-activity relationship remains challenging. Here, we report the synthesis, characterizations, and mechanistic investigation of various PM SACs supported on nanoceria for CH₄ combustion. Using density functional theory, two descriptors as the d-band center of PMs and oxygen vacancy formation energy are established, which jointly govern the reactivity for CH₄ combustion. These descriptors are thus applied to predict a dual SAC consisting of proximate Pd and Rh sites, demonstrating a remarkable improvement versus Pd or Rh catalyst, respectively. Our results reveal the general strategy of integrating experimental and computational efforts for investigation of various PM SACs in methane combustion, thus paving the way for the next generation of advanced catalytic materials.