Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal‐Oxide Interface Restructuring of Nickel/Zirconia

Abstract

The 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.

Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane

“…While the activation of metallic DRM catalysts by CO 2 treatment has been reported before 44 , in particular through the removal of deposited carbon by gasification 45 , the reactivation of carbide-based DRM catalysts by CO 2 is, to the best of our knowledge, unprecedented and remarkable given that Mo 2 C-based catalysts for DRM are typically oxidized by CO 2 yielding inactive MoO 2 11 , 15 . Note that the reference materials could not be reactivated in CO 2 , which is explained by the formation of MoO 2 layer covering the active phase (Supplementary Fig.…”

Catalytic Dry Reforming of Methane: Insights from Model Systems

“…Steib et al. proposes a complete cyclic catalyst regeneration scheme (Figure ) of activation‐reforming‐coking‐regeneration‐reforming‐steps …”

Kinetic study of the methane dry (CO2) reforming reaction over the Ce0.70La0.20Ni0.10O2−δcatalyst

“…[23][24][25] In addition, it has been evidenced that a fine-tuning and intensification of the interactions between Ni and support can induce better anticoke and anti-sintering performance of the catalysts. 26,27 The effect of interactions between the active metal and support, as a result of the formation of a solid solution, on the catalysts' performance during dry reforming reaction has been widely evaluated in literature. Excellent activity and stability have been reported by Hu for the NiO-MgO (or CoO-MgO) solid solution; 28 the carbon deposition is inhibited by the isolation effect of small nickel particles formed on the catalytic surface coupled with the surface basicity of MgO.…”