Pt/CeO2 single-atom catalysts are attractive materials for CO oxidation but normally show poor activity below 150 °C mainly due to the unicity of the originally symmetric Pt1O4 structure. In this work, a highly active and stable Pt1/CeO2 single-site catalyst with only 0.1 wt % Pt loading, achieving a satisfied complete conversion of CO at 150 °C, can be obtained through fabricating asymmetric Pt1O4-oxygen vacancies (Ov) dual-active sites induced by well-dispersed NbOx clusters. Specifically, the formation of new Ce-O-Nb interactions weakened the strength of the original Pt-O-Ce bond, thus transferring the originally near-perfect square-planar Pt1O4 into the distorted square-planar one, along with forming abundant Ov around the Pt site. Hence, the promoted CO activation on the asymmetric Pt1O4 structure and the facilitated dissociation of the O2 on the neighboring Ov site synergistically improved the CO catalytic oxidation performance. The fabrication of such asymmetric Pt1O4-Ov double-active sites was also active for the oxidation of other typical hydrocarbons pollutants such as C7H8 and C3H6 from exhaust gases, shedding light on engineering high-efficiency Pt-based oxidation catalysts for low-temperature environmental catalysis.
Keywords: Pt single-atom catalyst; Pt−O−Ce interaction; asymmetric Pt1O4−Ov double-active sites; catalytic oxidation; highly dispersed NbOx clusters.