Abstract

AbstractThe activity of the Ni/ZrO2 catalyst for the dry reforming of methane was significantly enhanced by activation and regeneration in the presence of CO2. Exposure to CO2 maximized and dynamically restructured the Ni–ZrO2 interface, which was critical to obtain a stable catalyst. The ZrO2−x species at this interface was found to act catalytically by accepting and transferring one oxygen atom of CO2 to the Ni surface, which resulted in the release of CO in the decomposition of transiently formed carbonates. This was found to open a fast additional reaction pathway to convert CO2 that eclipsed direct CO2 dissociation on Ni. The kinetically controlled availability of atomic oxygen by this pathway reduced the carbon concentration on the surface, which led to less refractory carbon deposition and more facile regeneration.

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