Selective Conversion of CH ₄ by MAl ₂ O ₄ ⁻ (M = Au and Pd): A Theoretical Study

Abstract The catalytic reactions of individual noble metal atoms can offer theoretical guidance for the design of the relevant single‐atom catalysts. In this paper, from MD adsorption simulation, both Au and Pd atoms rather bond to Al than O atoms of the employed Al 2 O 3 (001) surface and display more active sites for the Au system with respect to the Pd system. Next, a detailed comparative study was conducted on the reactions of preferred MAl 2 O 4 − (M = Au and Pd) with CH 4 using the DFT‐B3LYP functional. The obtained results reveal that in the AuAl 2 O 4 − reaction, the CH 4 tends to be transformed into syngas, H 2 and CO. In contrast, the formaldehyde is generated in the reaction of PdAl 2 O 4 − + CH 4 . Additionally, our findings also suggest that the reactivity of AuAl 2 O 4 − is significantly higher than that of PdAl 2 O 4 − , indicating that the former can fully activate CH 4 four C─H bonds. This insight provides valuable guidance for the rational design of single‐atom catalysts aimed at selective CH 4 conversion.