Photothermal synergistic catalytic oxidation of toluene over single-atom Pt catalysts was investigated. Compared with the conventional thermocatalytic oxidation in the dark, toluene conversion and CO 2 yield over 0.39Pt 1 /CuO-CeO 2 under simulated solar irradiation (λ = 320−2500 nm, optical power density = 200 mW cm −2 ) at 180 °C could be increased about 48%. An amount of CuO was added to CeO 2 to disperse single-atom Pt with a maximal Pt loading of 0.83 wt %. The synergistic effect between photo-and thermocatalysis is very important for the development of new pollutant treatment technology with high efficiency and low energy consumption. Both light and heat played an important role in the present photothermal synergistic catalytic oxidation. 0.39Pt 1 /CuO-CeO 2 showed good redox performance and excellent optical properties and utilized the full-spectrum solar energy. Light illumination induced the generation of reactive oxygen species ( • OH and • O 2 − ), which accelerated the transformation of intermediates, promoted the release of active sites on the catalyst surface, and improved the oxidation reaction.
The controlled oxidation of alcohols to the corresponding ketones or aldehydes via selective cleavage of the β‐C−H bond of alcohols under mild conditions still remains a significant challenge. Although the metal/oxide interface is highly active and selective, the interfacial sites fall far behind the demand, due to the large and thick support. Herein, we successfully develop a unique Au−CuO Janus structure (average particle size=3.8 nm) with an ultrathin CuO layer (0.5 nm thickness) via a bimetal in situ activation and separation strategy. The resulting Au−CuO interfacial sites prominently enhance isopropanol adsorption and decrease the energy barrier of β‐C−H bond scission from 1.44 to 0.01 eV due to the strong affinity between the O atom of CuO and the H atom of isopropanol, compared with Au sites alone, thereby achieving ultrahigh acetone selectivity (99.3 %) over 1.1 wt % AuCu0.75/Al2O3 at 100 °C and atmospheric pressure with 97.5 % isopropanol conversion. Furthermore, Au−CuO Janus structures supported on SiO2, TiO2 or CeO2 exhibit remarkable catalytic performance, and great promotion in activity and acetone selectivity is achieved as well for other reducible oxides derived from Fe, Co, Ni and Mn. This study should help to develop strategies for maximized interfacial site construction and structure optimization for efficient β‐C−H bond activation.
Pt-based catalysts can be poisoned
by the chlorine formed during
the oxidation of multicomponent volatile organic compounds (VOCs)
containing chlorinated VOCs. Improving the low-temperature chlorine
resistance of catalysts is important for industrial applications,
although it is yet challenging. We hereby demonstrate the essential
catalytic roles of a bifunctional catalyst with an atomic-scale metal/oxide
interface constructed by an intermetallic compound nanocrystal. Introducing
trichloroethylene (TCE) exhibits a less negative effect on the catalytic
activity of the bimetallic catalyst for o-xylene
oxidation, and the partial deactivation caused by TCE addition is
reversible, suggesting that the bimetallic, HCl-etched Pt3Sn(E)/CeO2 catalyst possesses much stronger chlorine resistance
than the conventional Pt/CeO2 catalyst. On the site-isolated
Pt–Sn catalyst, the presence of aromatic hydrocarbon significantly
inhibits the adsorption strength of TCE, resulting in excellent catalytic
stability in the oxidation of the VOC mixture. Furthermore, the large
amount of surface-adsorbed oxygen species generated on the electronegative
Pt is highly effective for low-temperature C–Cl bond dissociation.
The adjacent promoter (Sn–O) possesses the functionality of
acid sites to provide sufficient protons for HCl formation over the
bifunctional catalyst, which is considered critical to maintaining
the reactivity of Pt by removing Cl and decreasing the polychlorinated
byproducts.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.