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CO<sub>2</sub> Activation over Nanoshaped CeO<sub>2</sub> Decorated with Nickel for Low-Temperature Methane Dry Reforming

Kristijan Lorber, Janez Zavašnik, Iztok Arčon, Matej Huš, Janvit Teržan, Blaž Likozar, Petar Djinović

2022ACS Applied Materials & Interfaces77 citationsDOIOpen Access PDF

Abstract

Dry reforming of methane (DRM) is a promising way to convert methane and carbon dioxide into H 2 and CO (syngas). CeO 2 nanorods, nanocubes, and nanospheres were decorated with 1-4 wt % Ni. The materials were structurally characterized using TEM and in situ XANES/EXAFS. The CO 2 activation was analyzed by DFT and temperature-programmed techniques combined with MS-DRIFTS. Synthesized CeO 2 morphologies expose {111} and {100} terminating facets, varying the strength of the CO 2 interaction and redox properties, which influence the CO 2 activation. Temperature-programmed CO 2 DRIFTS analysis revealed that under hydrogen-lean conditions mono-and bidentate carbonates are hydrogenated to formate intermediates, which decompose to H 2 O and CO. In excess hydrogen, methane is the preferred reaction product. The CeO 2 cubes favor the formation of a polydentate carbonate species, which is an inert spectator during DRM at 500 C. Polydentate covers a considerable fraction of ceria's surface, resulting in less-abundant surface sites for CO 2 dissociation.

Topics & Concepts

Materials scienceCarbon dioxide reformingMethaneFormateSyngasDissociation (chemistry)HydrogenChemical engineeringXANESNanorodExtended X-ray absorption fine structureInert gasInorganic chemistryCatalysisNanotechnologyPhysical chemistryChemistryAbsorption spectroscopyOrganic chemistryEngineeringSpectroscopyComposite materialQuantum mechanicsPhysicsCatalytic Processes in Materials ScienceCatalysts for Methane ReformingCatalysis and Oxidation Reactions