Nature Communications · 2024 · 174 citations · 75 references
Natural SciencesChemical EngineeringChemistryCatalysisSurface ScienceTheoretical ChemistryCatalyst CharacterizationCatalyst DesignCatalyst StabilityCatalytic MaterialsSupported CatalystsSurface CatalysisCatalyst MechanismsCatalyst Structure - Activity RelationshipsCatalytic Energy ConversionDry ReformingInterface StructureRate-determining StepSpectroscopic CharacterizationSyngas Production
Abstract The dry reforming of methane provides an attractive route to convert greenhouse gases (CH 4 and CO 2 ) into valuable syngas, so as to resolve the carbon cycle and environmental issues. However, the development of high-performance catalysts remains a huge challenge. Herein, we report a 0.6% Ir/CeO 2− x catalyst with a metal-support interface structure which exhibits high CH 4 (~72%) and CO 2 (~82%) conversion and a CH 4 reaction rate of ~973 μmol CH4 g cat −1 s −1 which is stable over 100 h at 700 °C. The performance of the catalyst is close to the state-of-the-art in this area of research. A combination of in situ spectroscopic characterization and theoretical calculations highlight the importance of the interfacial structure as an intrinsic active center to facilitate the CH 4 dissociation (the rate-determining step) and the CH 2 * oxidation to CH 2 O* without coke formation, which accounts for the long-term stability. The catalyst in this work has a potential application prospect in the field of high-value utilization of carbon resources.
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Projector augmented-wave method
Peter E. Blöchl · Physical review. B, Condensed matter · 1994 · 90.8K citations
Natural Sciences, Chemistry, Physics +17