Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity

Abstract

Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO2 supported Pt single atom catalysts with precisely controlled coordination environments are successfully fabricated. The joint experimental and theoretical analysis reveals that the Pt single atoms on Pt1/CeO2 prepared at 550 °C (Pt/CeO2-550) are mainly located at the edge sites of CeO2 with a Pt–O coordination number of ca. 5, while those prepared at 800 °C (Pt/CeO2-800) are predominantly located at distorted Ce substitution sites on CeO2 terrace with a Pt–O coordination number of ca. 4. Pt/CeO2-550 and Pt/CeO2-800 with different Pt1-CeO2 coordination environments exhibit a reversal of activity trend in CO oxidation and NH3 oxidation due to their different privileges in reactants activation and H2O desorption, suggesting that the catalytic performance of Pt single atom catalysts in different target reactions can be maximized by optimizing their local coordination structures.

Controllable Conversion of Platinum Nanoparticles to Single Atoms in Pt/CeO2 by Laser Ablation for Efficient CO Oxidation

“…CO oxidation is a reaction that possesses practical application value and can also be a catalytic model to investigate the structure–activity relationship of catalysts. , Different Pt 1 Pt NP /CeO 2 catalysts were evaluated for CO oxidation. The possible nitrate or chlorine residues on the sample were examined and removed before catalytic tests (Figure S24).…”

Regulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation

“…Thus, the coordination microenvironment of central atoms, including the types of coordination atoms, coordination numbers, and even peripheral coordination atoms in the second or higher shell, is crucial for determining their electronic and geometric structures, which in turn influence the absorption or desorption of reaction species and thus the catalytic properties of SACs 12 – 16 . The overwhelming of SACs research has been focused on this field, with remarkable achievements obtained in recent decades 17 – 19 . However, how to further tailor the electronic structure beyond the aforementioned strategy to enhance catalytic performance becomes a new frontier for SACs studies.…”

Boosting the Hydroformylation Activity of a Rh/CeO2 Single-Atom Catalyst by Tuning Surface Deficiencies

“…Atom trapping only occurs at high temperatures plausibly because the undesired surface species such as hydroxyls and carbonates are desorbed at high temperatures. 30 achieved fine-tuning of the local coordination environment of Pt single atoms by controlling the synthesis temperature. The Pt/CeO 2 catalyst calcined at high temperatures showed a lower O coordination number than the lower-temperature-calcined catalyst and exhibited distinct catalytic behaviors in CO oxidation and NH 3 oxidation.…”