Efficient CO oxidation at ambient or low temperatures
is essential
for environmental purification and selective CO oxidation in H2, yet achieving this remains a challenge with current methodologies.
In this research, we extensively evaluated the catalytic performance
of phosphotungstic acid (PTA)-supported 11 M1/PTA single-atom
catalysts (SACs) using density functional theory calculations across
both gas phase and 12 common solvents. The Rh1/PTA, Pd1/PTA, and Pt1/PTA systems exhibit moderate CO adsorption
energies, facilitating the feasibility of oxygen vacancy formation.
Remarkably, the Pd1/PTA and Pt1/PTA catalysts
exhibited negligible energy barriers and demonstrated exceptionally
high catalytic rates, with values reaching up to (1 × 1010)11, markedly exceeding the threshold for room
temperature reactions, set at 6.55 × 108. This phenomenon
is attributed to a transition from the high-energy barrier processes
of oxygen dissociation in O2 and N–O bond dissociation
in N2O to the more efficient dissociation of H2O2. Orbital analysis and charge variations at metal sites
throughout the reaction process provide deeper insights into the role
of the three metal catalytic sites in CO activation. Our findings
not only reveal key aspects of SACs in facilitating CO oxidation at
low temperatures but also provide valuable insights for future catalytic
reaction mechanism studies and environmental applications.