Abstract
The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. Traditional approaches focus on oxygen-activating oxides as support which provides the oxygen activation at the catalyst-support peripheral interface. Here we report a new approach to oxidation catalysts for total oxidation of hydrocarbons (e.g., propane) by surface oxygenation of platinum (Pt)-alloyed multicomponent nanoparticles (e.g., platinum-nickel cobalt (Pt–NiCo)). The in-situ/operando time-resolved studies, including high-energy synchrotron X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy, demonstrate the formation of oxygenated Pt–NiOCoO surface layer and disordered ternary alloy core. The results reveal largely-irregular oscillatory kinetics associated with the dynamic lattice expansion/shrinking, ordering/disordering, and formation of surface-oxygenated sites and intermediates. The catalytic synergy is responsible for reduction of the oxidation temperature by ~100 °C and the high stability under 800 °C hydrothermal aging in comparison with Pt, and may represent a paradigm shift in the design of self-supported catalysts.
Highlights
The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability
The catalytic performance of such catalysts heavily relies on the oxygen-activation activity at the peripheral interface between the active component and the oxide support, which is not efficient by design and poses difficulty in preparing the oxide supported catalysts in order to achieve the full controllability over activity and stability
The surface oxygenation of the multimetallic alloy nanoparticles creates oxygenated active sites on the catalyst, which differs from traditional metal/metal oxide support catalysts where the catalytic reaction occurs on metal/support perimeter zone[6,7,8,9,10,11,12,13]
Summary
The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. The oscillatory depletion of surface-oxygenated intermediate species played an important role in introducing lattice oxygen and structural disordering on the NA–SONA catalyst (Fig. 3d).
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