Abstract
Excellent catalysts for the catalytic oxidation of benzene (C6H6) require active sites with robust oxidation capabilities. Heteronuclear dual-single atom catalysts can exhibit enhanced catalytic activity through synergistic interactions between the dual single atoms (SAs). Herein, we successfully engineered a bimetallic single-atom catalyst, Pt1-Ni1/TiO2-NW, which demonstrates exceptional performance in C6H6 oxidation. Various technologies, including X-ray absorption fine structure and Z-type spherical aberration-corrected transmission electron microscopy, were used to identify the bimetallic single atoms within the catalyst. The catalytic oxidation of C6H6 by Pt1-Ni1/TiO2-NW was comprehensively investigated. Finally, in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) were employed to reveal the underlying mechanism for the synergetic effect of the bimetallic single atoms. The results indicate that the introduction of Ni SA favors the formation of Pt SA. The T90% of Pt1-Ni1/TiO2-NW reached 185 °C, a remarkable 40 °C lower than that of the single-atom catalyst Pt1/TiO2-NW. More importantly, the active center of Pt-O-Ni, formed by the collaboration of Pt SA and Ni SA with bridging oxygen, plays a crucial role in reducing the energy barrier during the conversion of C6H6 to phenol and further to benzoquinones. This research provides a valuable methodology for constructing heteronuclear bimetallic single-atom catalysts tailed specifically for C6H6 oxidation.
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