Enhancing oxidation reaction over Pt-MnO2 catalyst by activation of surface oxygen.

Formaldehyde (HCHO) and carbon monoxide (CO) are both common air pollutants and hazardous to human body. It is imperative to develop the catalyst that is able to efficiently remove these pollutants. In this work, we activated Pt-MnO2 under different conditions for highly active oxidation of HCHO and CO, and the catalyst activated under CO displayed superior performance. A suite of complementary characterizations revealed that the catalyst activated with CO created the highly dispersed Pt nanoparticles to maintain a more positively charged state of Pt, which appropriately weakens the Mn-O bonding strength in the adjacent region of Pt for efficient supply of active oxygen during the reaction. Compared with other catalysts activated under different conditions, the CO-activated Pt-MnO2 displays much higher activity for oxidation of HCHO and CO. This research contributes to elucidating the mechanism for regulating the oxidation activity of Pt-based catalyst.

Electronic Modification by Transitional Metal Dopants to Tune the Oxidation Activity of Pt-CeO2-Based Catalysts.

While utilization of transitional metals as a promoter has been extensively studied to enhance the activity of Pt-based catalysts for the oxidation of formaldehyde (HCHO), there is still a lack of well elucidated property-function relationship for the rational selection of a promoter in catalyst design. Herein, we modified a Pt/CeO2 catalyst with two transitional metal dopants (i.e., Mn and Cu) that showed negligible influence on the physical structure of the Pt-CeO2 matrix but distinct effects on the activity of the catalyst. Complementary characterizations combined with density functional theory modeling revealed that the transitional metal dopants significantly modified the electronic structure of the catalyst and shifted the d-band of Pt to higher energy with different extents, which may tune the bonding strength of HCHO/intermediates with the Pt-CeO2 interface domain. The catalyst with moderate bonding strength (i.e., Pt-Mn/CeO2) displayed the highest reactivity under the ambient condition, while Pt-Cu/CeO2 with the highest bonding strength showed a dramatically decreased activity. No correlation was observed between the abundancy of the active oxygen and catalytic activity, likely due to the oxygen supply having a much higher rate than the rate-determining step. This work contributes to the elucidation about the property-function relationship of a transitional metal dopant in Pt-based catalysts for the oxidation of HCHO.